Materials Today Sustainability 24 (2023) 100483

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CO2 capture materials: a review of current trends and future

challenges
Bartosz Dziejarski a, b, *, Jarosław Serafin c, Klas Andersson b, Renata Krzyzy
_ n ska a
a
Faculty of Environmental Engineering, Wroclaw University of Science and Technology, 50-370 Wroclaw, Poland
b
Department of Space, Earth and Environment, Division of Energy Technology, Chalmers University of Technology, SE-412 96 Gothenburg, Sweden
c
Department of Inorganic and Organic Chemistry, University of Barcelona, Martí i Franqu
es, 1-11, 08028 Barcelona, Spain

a r t i c l e i n f o a b s t r a c t

Article history: Over the last decade, CO2 adsorption technology has quickly gained popularity and is now widely applied
Received 15 April 2023 in global CCUS projects due to playing an important role in achieving net-zero emissions by 2050. As a
Accepted 20 July 2023 result, novel materials, or post-modification methods of those already available have been successively
Available online 28 July 2023
reported to enhance the efficiency of CO2 capture from flue gases. This paper discusses a systematic
understanding of fundamental aspects of current research trends in terms of developing selected solid
Keywords:
CO2 adsorbent, with a particular emphasis on the upcoming challenges. The candidates are reviewed
CO2 adsorption
considering the practical drawbacks of imposed by industrial scale and economics, including carbon-
Sorption
Adsorbents
based materials, metal-organic frameworks (MOFs), polymers, zeolites, silica, alumina, metal oxides,
Greenhouse gases amine-based adsorbents, and other composite porous materials. Sustainable sorbents derived from
CO2 emission biomass and industrial residues are also studied due to the high need for cost-effective raw materials and
Climate change mitigation their crucial role in the circular economy. Lastly, a techno-economic analysis (TEA) is included to provide
the most important criteria that should be considered when adsorbents are implemented on an in-
dustrial scale. Consequently, the review is summarized, and recommendations are offered for future
research in the advancement of CO2 capture materials. The paper aims to establish a comprehensive
theoretical basis of adsorption technologies currently progressed to reduce CO2 emissions, along with
highlighting the identification and precise articulation of the most important future research paths that
could be beneficial to address over the next years.
© 2023 The Author(s). Published by Elsevier Ltd. This is an open access article under the CC BY license
([Link]

1. Introduction the constant rise in average temperatures throughout the world

and the associated frequency with greater intensity of the emer-
1.1. The impact of industrialization on CO2 emissions and climate gence of severe extreme weather events (heat waves, droughts,
change blizzards, and rainstorms) are among the most direct and imme-
diately apparent effects that have resulted from this phenomenon
Since the beginning of the industrial revolution, there has been [2,3]. It is anticipated that human activities have contributed to an
an exceptional boost in the amount of heavy pollution released escalation of global temperature of around 1
C surpassing those of
from industrial facilities, mainly as a result of the burning of fossil the pre-industrial period of time, with a probable range of
fuels (coal, crude oil, and natural gas). Today, one of the most 0.8e1.2
C [4]. In 2020, CO2 average annual level in the atmosphere
challenging and urgent environmental issues facing the world is was approximately 50% higher than in the 60's 18th century and
the reduction of CO2 concentration in the atmosphere, which is has attained their greatest value recorded in the history of
widely reported to be the main anthropogenic greenhouse gas that 412.5 ppm [5].
leads to global warming and climate changes [1]. For this reason, Unfortunately, the rapid development of the world's economic,
and accelerating industrialization, with a soaring world population,
will definitely cause a gradual growth of CO2 emissions and will
affect global warming to reach 1.5
C in the next 30 years at the
* Corresponding author.
current state [1]. According to the Intergovernmental Panel on
E-mail addresses: [Link]@[Link], bartoszd@[Link]
(B. Dziejarski). Climate Change (IPCC) latest report from 2022, to prevent this

[Link]
2589-2347/© 2023 The Author(s). Published by Elsevier Ltd. This is an open access article under the CC BY license ([Link]
B. Dziejarski et al. Materials Today Sustainability 24 (2023) 100483

scenario, climate change mitigation efforts should be executed contains specific materials that are commonly called physical and
immediately. IPCC estimation indicates that the peak of GHG chemical adsorbents.
emissions must take place in 2025 at the latest, so by 2030 a 43% Generally, the most widely used solid materials for CO2 capture
reduction of it will possibly be achieved. Otherwise, by the end of are silica, zeolites, alumina, amine-based materials, metal oxides,
2100 the average temperature on Earth and atmospheric concen- metal-organic frameworks (MOFs), polymers, and carbon materials
tration of CO2 will increase by 3.2
C and to 570 ppm, respectively (activated carbon, graphite, graphene, fullerene, carbon nanotubes,
[6]. In order to prevent this occurrence and meet the Paris Agree- biochar, and hydrochar). Moreover, it is crucial to elucidate the
ment climate ambition, specific system changes for energy man- differentiation between amorphous and crystalline solids in terms
agement should be adopted. In particular, innovative of sorbents due to their substantial impact on CO2 uptake perfor-
transformation concerns industry, which is responsible for 25% of mance, related strictly with their distinct physical and chemical
CO2 emissions from energy and industrial processes, such as the characteristics. Crystalline materials exhibit distinct pore structures
cement, chemicals, iron and steel sectors [7]. Furthermore, it is and surface areas, thus demonstrating the potential for significant
associated with widespread electrification, better energy efficiency, CO2 adsorption capacity. Their high stability under harsh process
aiming at rational supervision of fossil fuel exploitation, and conditions and precise regulation of pore size and distribution can
intensification of the share of renewable energy sources (hydrogen, be optimized for practical purposes in CCUS projects. In contrast,
biomass-based fuels, solar energy, or nuclear power) in global en- materials characterized by the absence of a definite lattice pattern
ergy consumption. Although the above long-term plans have in the arrangement of its constituent atoms and molecules
enormous potential, they are currently unable to lessen the carbon demonstrate an amorphous structure. The lack of a defined
footprint of humanity simply by mitigation of CO2 emissions, arrangement often results in elevated surface areas and porosities,
burning fossil fuels, and R&D on total commercialization of clean making them highly suitable for CO2 capture. However, it could also
energy requires large financial outlays and investments, and above potentially lead to inadequate stability and diminished selectivity.
all time. Therefore, it is imperative to understand the properties while
In view of this, over the course of the last several decades, a choosing and formulating CO2 capture materials for particular uses.
concerted initiative has been launched all over the world to create The optimal CO2 adsorption efficiency can be achieved by utilizing
new methods for point source carbon capture aiming to stop CO2 either amorphous or crystalline materials, or a combination of both,
emissions from entering the atmosphere. Especially one receives depending on the specific requirements of the application. The
the most interest and is predicted to play a crucial part in the number of publications since 2013 that have concerned solid ma-
evolution toward the use of low-carbon energy, which is called terials for CO2 capture is shown in Fig. 1.
carbon capture, utilization and storage (CCUS). The CCUS system As can be observed, over the last several years, there has been a
specifies a group of technologies, such as carbon capture and substantial increase in the number of researchers interested in CO2
storage (CCS), carbon capture and utilization (CCU), or bioenergy capture by adsorption. This results directly in the publication of
with carbon capture and storage (BECCS). Among the CCUS value scientific articles related to the synthesis of different new materials
chain, the CO2 capture stage roughly represented around 70e90% of or post-modification methods to optimize the efficiency of the CO2
total operating expenditures, making it one of the key research adsorption capacity. However, a generic overview that focuses on
areas for maturing the entire technologies and contributing to the summarizing the current knowledge for beginner scientist in this
achievement of net zero emissions [8]. Depending on the specific field in sense of critical limitations, opportunities, or research trend
CO2 manufacturing method, operating conditions, composition of for a specific adsorbent group, is not something that has been re-
flue gas and process parameters, there are three main capture ap- ported very often in the recent years.
proaches: pre-combustion capture, post-combustion capture, and In general, the aim of this review is to provide a comprehensive
oxy-fuel combustion [9]. Each of the above uses various CO2 sep- summary of advances that have been accomplished in in the
aration process, which are the most vital part of CO2 capture, development of solid CO2 capture materials with highly insightful
including: absorption, membranes, cryogenic method, chemical current and future research directions. Furthermore, our work in-
looping combustion (CLC), calcium looping (CaL), and adsorption. cludes a compilation of up-to-date data on physicochemical mea-
surements along with modification strategies to improve CO2
1.2. A wide spectrum of CO2 capture materials adsorption capacity. Moreover, we also discuss the details of the
techno-economic analysis (TEA), which is an essential procedure
The application of solid adsorbent materials is widely regarded for introducing novel materials on an industrial level. Ultimately,
as one of the most promising research directions and has garnered several concluding perspectives are provided with proposed solu-
a high amount of attention for carbon capture in CCUS [10]. It de- tions for the existing challenges and upcoming barriers in com-
livers benefits such as, amongst others: considerably high CO2 mercial facilitation of discussed sorbents.
uptake efficiency, easy regeneration, simple handling, wide process
operability range, material stability, the possibility of using broadly 2. Desired properties and criteria for selecting CO2 capture
understood waste to produce materials [11]. Important definitions materials
that should be used for the correct CO2 adsorption characteristics
are the formulations of the individuals participating in the process: To efficiently removing CO2 from the flue gas mixture, the
adsorbent e a solid on which gas molecules from inside the gas synthesized adsorbents should possess stringently specified good
phase are adsorbed, and adsorbate e a gas that has finally been characteristics and satisfy technical and economic requirements
adsorbed on the surface of the adsorbent [12]. There are two main that are favorable for CO2 adsorption (Fig. 2). First and foremost, the
types of gas molecule adsorption on the surface of a solid. If the material must be characterized by a high capacity to efficiently
accumulation of the adsorbate on the surface of the solid occurs adsorb CO2 under a variety of process conditions. Additionally, it is
due to weak intermolecular van der Waals interactions, then essential that the materials have superior application capability for
adsorption is termed physisorption or physical adsorption [12,13]. commercial purposes. Regrettably, it is quite unusual to satisfy all
When gas molecules accumulate on the surface of the adsorbent by crucial requirements. In this section, an evaluation of the most
chemical bonds, the phenomenon occurring is called chemical important adsorbent properties and criteria are listed below
adsorption or chemisorption [14]. Each of these two groups [12,14].
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B. Dziejarski et al. Materials Today Sustainability 24 (2023) 100483

Fig. 1. Number of publications on CO2 capture with various solid materials since 2013 (based on Scopus with keywords “CO2 adsorption” or “CO2 capture”).

Fig. 2. The most important properties and criteria for selecting CO2 capture materials.

 Equilibrium adsorption capacity is directly related to the specific  Mechanical properties, the adsorbent should be mechanically
surface, pore size, and surface chemistry of the adsorbent. The strong, i.e., perfectly resistant to abrasion and crushing during
capacity value indicates the maximum amount of adsorbate its operation in process equipment (adsorption and chromato-
related to the adsorbent mass unit that can be adsorbed at graphic columns under various process conditions). These
equilibrium (phase equilibrium at the solidegas interface, properties directly affect the efficiency of the process and the
where the adsorption rate is equal to the desorption rate) for a generation of additional costs.
given temperature and pressure.  Chemical nature of surface is also an important determinant.
 CO2 selectivity parameter serves as a theoretical metric for The adsorption capacity of adsorbent may be enhanced by the
evaluating the practical effectiveness of an adsorbent, especially presence of heteroatomic functional groups in the form of
in scenarios involving the adsorption of multicomponent carboneoxygen, carbonenitrogen, or carbonesulfur on its sur-
gaseous mixtures. It mainly depends on the size, shape, and face. The most significant functional groups contain oxygen
distribution of pore network. The selectivity has a direct impact atoms, so conferring a hydrophilic (polar) character to the outer
on the degree of purity of the obtained product, which in turn surface, in addition to the hydrophobic (nonpolar) nature shown
affects the economics of the adsorption installation. This crite- by the internal structure of the material. The dual nature of the
rion is the most important for physical adsorbents. adsorbent surface allows it to effectively adsorb a diverse range
 Kinetics of adsorption and desorption are influenced by several of gases, with a particular emphasis on CO2 from flue gas
factors, including the size of adsorbate molecules, the porosity streams containing moisture.
of sorbent material, the concentration of adsorbate in the flue  Pores characteristics, there is a one-to-one correlation between
gas stream, and even the type of chemical bonding formed the presence of micropores and the effectiveness of material in
during the process, which also exerts a significant impact. Ki- the adsorption process. Their widths are comparable to those of
netics during CO2 sorption should exhibit favorable and signif- the CO2 molecules that are capable of being adsorbed, falling
icantly fast behaviour, indicating that a short time is required to within the range of <2 nm. Mesopores and macropores, which
attain the equilibrium state between the adsorbateeadsorbent serve secondary functions, have the responsibility of trans-
complex or to facilitate expedited regeneration of the adsor- porting the adsorbed gaseous medium via a network of
bent bed. channels.

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B. Dziejarski et al. Materials Today Sustainability 24 (2023) 100483

 Chemical and thermal stability, adsorbents are often exposed to [19]. Additional complications encompass equipment corrosion
harsh chemical conditions (the flue gas stream mainly contains and amine solvent degradation due to the presence of oxygen in the
water vapor and other impurities, such as CO, trace elements, aqueous solution [20]. Therefore, to minimize these issues and
particulates, NOx, and SOx), as well as high pressure and potential elevated costs, research efforts are concentrated on the
elevated temperature. Robust stability and exceptional development of amine-functionalized solid materials, referred to as
tolerance under these conditions ensure their proper lifetime, N-functionalized solid adsorbents (NFSAs). This approach aims to
high equilibrium sorption capacity, and the possibility of improve the CO2 capture capacity of amine groups by increasing
subsequent regeneration and reuse in a greater number of functional group availability and adsorption kinetics, concurrently
adsorptionedesorption cycles. The lack of an appropriate degree ensuring stability and high porosity. Moreover, when compared to
of chemical and thermal stability of the sorbent directly affects unmodified porous adsorbents, NFSAs exhibit improved CO2 af-
the economics of the entire CO2 separation process. finity and superior moisture tolerance. Thus, they have garnered
 Regeneration capacity, adsorbents undergo a regeneration pro- attention as highly promising candidates for CO2 adsorption from
cess after their adsorption capacity is exhausted, as a result of flue gas mixtures [21,22]. The excellent affinity of N-functionalized
the maximum filling of the pore volume and occupying their solid adsorbents towards CO2 and their enhanced resistance to
surface with CO2 molecules. The process of regeneration in- moisture can be attributed to the existence of nitrogen-containing
volves removal of the adsorbed CO2 molecules from both the functional groups on their surface. These functional groups possess
pores and the surface of adsorbent by desorption. This fully al- the capability to interact with CO2 molecules via diverse mecha-
lows the restoration of the sorption capabilities of the material. nisms such as electrostatic interactions, hydrogen bonding, and
Furthermore, the investigation of optimal sorbent regeneration Lewis acid-base interactions. Furthermore, the nitrogen-containing
conditions is now a key subject of current research in the se- functional groups confer hydrophobic characteristics to NFSAs,
lection of the suitable materials. Depending on their structure enabling them to withstand moisture and maintain CO2 uptake
and physicochemical properties, the adsorption/desorption cy- efficiency even in high-humidity conditions.
cles are carried out considering parameters, such as tempera- The amine-based adsorbents are typically synthesized in two
ture, pressure, and applying a specific adsorption technology or independent steps: initial preparation of solid supports and the
as a combination of several types: pressure swing adsorption subsequent integration of N-source sorbents with these supports.
(PSA), vacuum swing adsorption (VSA), vacuum pressure swing For the creation of high-performance NFSAs, a variety of different
adsorption (VPSA), temperature swing adsorption (TSA), tem- amine types can be employed, as listed in Table 1.
perature pressure swing adsorption (TPSA), and electric swing Further, numerous porous solid materials have also been
adsorption (ESA). investigated and documented for their ability to adsorb CO2 from
 Stability in adsorption/desorption cycles and the lifetime of flue gas streams. These materials involve the functionalization of
adsorbents play a crucial role in determining the frequency of amines onto supports like activated carbons (ACs), carbon-based
material replacement, hence directly influencing the economic nanoadsorbents, mesoporous silica, zeolites, porous organic poly-
viability of industrial-scale installations. mers, metal oxides, and others, all of which are extensively covered
 Production costs are another crucial parameter that is consid- in this review. To date, three distinct classes of amine-based sor-
ered obligatorily in terms of the development of adsorbent bent have been identified, based on the combination of the amine
production technology and the analysis of prospective research species/support material (bond structures), and nitrogen sources
directions for materials suited to CO2 sorption processes. (types of amines) [23,24].
 Environmental implications, it is essential to appropriately These classes are categorized as follows: Class 1 (impregnation
dispose of adsorbents that are incapable of undergoing further method), Class 2 (grafting method), and a combination of the
regeneration. Therefore, they cannot possess a significant impregnation and grafting approaches, often referred to as Class 3
adverse influence on the environment. (direct synthesis method) [25,26]. Each of these classes offers
unique synthesis paths, which are described below:
The evaluation of the described criteria and attributes of ad-
sorbent's effectiveness to capture CO2 is based on an analysis of the  Class I materials are prepared through the physically loading
initial characteristics of synthesized materials, as well as experi- monomeric or polymeric amine species, amino acid, amino-
mental investigations into CO2 adsorption isotherms, breakthrough containing ionic liquid, into accessible pores and on the sur-
curves of adsorbent bed, and mass transport kinetics. The entire face of porous support [27,28]. This process involves the use of a
procedure is shown schematically Fig. 3. solvent, typically water or organic solvents like methanol or
ethanol, to combine the amine with the support. The solvent
3. CO2 capture materials aids in dispersing amine molecules into the pores of the support
material [27]. Within the pores and on the support surface,
3.1. Amine-based adsorbents amine molecules that have formed bonds with each other serve
as active adsorption sites for capturing CO2. Notably, the amine
One prevalent method used in the industrial sector so far in- groups do not interact with the support in a chemical manner,
volves the utilization of aqueous amine solutions with a concen- meaning there is no substantial chemical bond or reaction be-
tration ranging from 20 to 30 wt% for the purpose of capturing post- tween the loaded amines and the surface of the support. The
combustion carbon dioxide [15e17]. This approach is primarily total pore volume of the porous material, along with the amine
favored owing to the notable affinity shown by amines towards density, plays a key role in determining the amount of amine
CO2. Nevertheless, the practicality of using amine is limited due to that can be effectively dispersed into the porous structure [29].
many drawbacks. One of these disadvantages is the high heat ca- Ideally, the support material should possess a larger pore vol-
pacity of the liquid phase, which results in substantial energy ume, as this increases the potential capacity for impregnated
consumption and increased costs during the regeneration process amine. Once the impregnation step is complete, excess solvent is
[18]. Another significant difficulty connected with aqueous amine removed through filtration, followed by drying of the solution.
absorption lies in its limited technological scalability, confining its The resulting amine-loaded adsorbent is then further dried in an
applicability to CO2 capture from coal or natural gas power plants oven at a temperature of around 40
C [30].
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B. Dziejarski et al. Materials Today Sustainability 24 (2023) 100483

Fig. 3. The examination path to evaluate the suitability of materials for CO2 capture application.

 In class II, materials are synthesized by dissolving the amine- presence of CeO interface bonds [31]. Compared to the
containing organosilanes in a volatile solvent. The adsorbent is impregnation and grafting methods, the direct synthesis
introduced into the solution and heated to facilitate covalent process is accomplished in a single step, reducing the
tethering. During this covalent bonding process, the amines of complexity of the operation. Furthermore, the distribution of
the silane group become attached to the surface functional amino groups in the amine-based solid adsorbent is more
groups of the support material. More specifically, hydroxyl uniform compared to the other methods [29]. This class of
groups (OHe) at the target interface form bonds with the central supported materials can be considered as a cross-over be-
region of the organosilanes, leading to adhesion [31,32]. tween the other two methods.
Therefore, it's crucial that the support material's surface con-
tains a high concentration of these hydroxyl functional groups. Considering the three major techniques mentioned above. Two
Once the grafting process is complete, the primary solvent is different types of adsorbents can be synthesized, such as amine-
replaced with a second volatile solvent. This step serves to loaded adsorbents (obtained by impregnation and grafting) and
activate the adsorbent by removing any remaining unreacted N-doped adsorbents (prepared by direct synthesis). In addition, a
amine molecules [31,33]. Consequently, the number of active novel synthesis approach called double functionalization has been
groups present on the substrate surface is critical in determining developed for the preparation of amine-based materials. This
the quantity of loaded amine and the resulting adsorption per- approach involves two functionalization steps, namely impregna-
formance [34]. This synthesis approach results in a stronger tion and grafting, combining the benefits of these two single syn-
linkage between the support and the amine compared to the thesis techniques.
impregnation method. In conjunction with the numerous successes in the creation of
 Class III materials are created through in situ polymerizations NFSAs for increased CO2 capture in recent years, several reviews
of the amine-containing precursor, which is the amine poly- have been compiled to provide the most up-to-date and relevant
mer monomer in the porous material. The direct synthesis insights into their development. Therefore, the focus is particu-
method also relies on chemical bonding, resulting in materials larly on review papers reported in 2020e2022. In 2020, Hu et al.
featuring a single covalent bond for each amine molecule. [27] published a review that explored future research and devel-
Additionally, these materials are characterized by the opment directions, as well as potential commercialization routes

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B. Dziejarski et al. Materials Today Sustainability 24 (2023) 100483

Table 1
Commonly used types of amines in I, II, and III class.

Amine type Abbreviation Structure Class

Monoethanolamine MEA I

Diethanolamine DEA II

Ethylenediamine EDA I

Diethylenetriamine DETA I

Tetraethylenepentamine TEPA III

Triethylenetetramine TETA I

Pentaethylenehexamine PEHA III

Polyethyleneimine PEI II

Isopropanol amine IPA III

2-Amino-2-methyl-1,3-propanediol AMPD III

2-Amino-2-methyl-1-propanol AMP III

(3-Aminopropyl)trimethoxysilane APTMS III

for amine-based adsorbents. The researchers emphasized two  Developing support features by increasing the pore diameters
probable aspects of NFSAs development. The first objective is to with specific reagents or selecting appropriate additives and
overcome their disadvantages, making them more competitive solvents, using the most suitable treatment techniques.
with aqueous amines. The second objective is to investigate their  In the case of amine-impregnated adsorbents, it's preferable to
practical applications, including the design of test equipment and choose supports with greater pore volumes and pore sizes, such
technological methods applicable to current power plant systems as hierarchical pore structures or multilayered structures.
and cost reduction. For amine-loaded adsorbents, one inherent Alternatively, for amine-grafted adsorbents, surfaces with a high
drawback is their limited range of uses due to reduced adsorption concentration of hydroxyl groups are more convenient.
capacity caused by factors, including as ammonia loss during  Utilizing distinctive and well-structured supports, such as cage-
extended adsorption operations, oxidative degradation of amines, structured zeolites, is recommended.
and degradation of porous supports due to irreversible adsorption  Supports made of inexpensive materials that are abundant in
of flue gas impurities like SO2, NO2, and O2. Regarding N-doped nature, such as clay, are favored over more expensive
adsorbents, a fundamental challenge is controlling their adsorp- alternatives.
tion capacity, either through the selection of materials or by
improving the synthesis process. MOFs and polymers have been In the same year, Gelles et al. [31] discussed the latest de-
highlighted as the most promising options for the future. In velopments in the production and assessment of different kinds of
conclusion, the authors point out the most important strategies amine functionalized materials, with the goal of presenting a
for enhancing the adsorption performances of amine-loaded ad- thorough overview of current work and future trends in materials
sorbents, such as the following: research and process implementation. The authors concluded that
to adequately evaluate the potential of amine-based adsorbents for
 The selection of appropriate amines for the synthesis of adsor- CO2 capture, a comprehensive view must be employed, considering
bents with improved adsorption capacity or lower desorption a variety of measurements that take both material and process
temperatures (materials containing a mixture of two different performance into account. These data should be optimized as much
amines often exhibit superior performance). as possible and can be categorized into main utilization criteria,

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B. Dziejarski et al. Materials Today Sustainability 24 (2023) 100483

including CO2 working capacity, adsorbent kinetics, regeneration related to pore control, problematic functionalization, and inef-
requirements, cost, long-term stability, and formulation. In terms of fective binding of CO2 molecules.
future research, recent years have seen the development of class I-II A significant breakthrough in utilizing silica for sorption pur-
and class I-III hybridized amine-materials. These hybrids have poses occurred in the 1990s, marking a crucial moment in materials
demonstrated superior working capability and cycle stability chemistry. Yanagisawa et al. [35,36] successfully synthesized mes-
compared to their individual class counterparts. In consequence, it oporous silica based on layered kanemite, which is a hydrated so-
is highly likely that further advancements will be made in the dium silicate with the chemical formula NaHSi2O5$3H2O. This
development of hybridized materials. Additionally, it has been specific silicate showed a high ion exchange capacity, and its
emphasized that, although VSA and TSA systems have demon- interlayer space was easily modifiable. The key innovation lay in the
strated commercial viability, future research efforts should be introduction of surface-active cationic organic compounds, often
directed towards conducting TEA. This analysis is essential for referred to as surfactants, between the layers of kanemite. This
determining the costs associated with scaling up and ensuring the process enabled the creation of porous silica with remarkable
stability of amine-based adsorbents on an industrial scale. Over the characteristics, including a highly regular structure featuring a
years, various types of amines and adsorbent supports have been hexagonally ordered pore system. Moreover, this material boasted
extensively investigated. In the future, the primary focus of an exceptionally large specific surface area, reaching up to 900 m2/
research will be on identifying the optimal amine-adsorbent g, and pores with an average size of about 3 nm.
combination. This blend should be easy to synthesize and seam- In 1992, the Mobile Research and Development Corporation
lessly integrate into process operations with minimal loss of CO2 achieved a notable advancement in creating materials similar to
capture capacity. those developed by Japanese scientists [37,38]. This material family
Recently, in 2021, Zhao et al. [29] conducted a comprehensive was named the M41S and comprised MCM-type materials (Mobil
review of the latest advancements in amine-functionalized solid Composition of Matter), which were classified as MCM-41 (hex-
adsorbents for post-combustion capture. Their recommendations agonal), MCM-48 (cubic), and MCM-50 (lamellar, with surfactant
for the development of NFSAs align with those proposed by Hu molecules present between the lamellae). They showed variations
et al. [27] and Gelles et al. [31]. The authors highlighted the need in pore ordering. Especially, MCM-41 possesses a unidirectional
to reduce preparatory costs and simplify the synthesis process, pore system, featuring a regularly arranged hexagonal array of
aiming to design a highly efficient and eco-friendly production tubes. On the other hand, MCM-48 exhibits a three-dimensional
method. They also stressed the importance of finding effective pore system characterized by two non-intersecting gyroid pores.
methods for introducing amines into practical support structures. Among these, MCM-41 garnered the most attention due to its or-
Hence, the review noted that certain impurity gases, such as dered and periodically repeating structure, even though it had an
water vapor, can enhance CO2 capture. Furthermore, most of the amorphous wall structure [39]. It was further distinguished by a
amine-based adsorbents studied so far exist in powder form, specific surface area exceeding 1000 m2/g and relatively large pore
which can lead to challenges related to heat and mass transfer sizes, some of which reached up to 10 nm. The development of
during CO2 adsorption. Consequently, there is growing interest in M41S materials paved the way for the creation of new ordered
monolithic adsorbents, which can improve heat and mass transfer mesoporous silicas, including SBA (Santa Barbara Amorphous) [40],
rates and eliminate the need for the molding process. Finally, the MSU (Michigan State University), HMS (Hexagonal Mesoporous
review also mentioned the pressing need for research into the Silica), KIL (Kemijski Institut Ljubljana), FSM (Folded Sheet Mate-
stability of these adsorbents on the commercial scale. Addition- rials), FDU (Fudan University), and KIT (Korean Advanced Institute
ally, it's worth noting that amines are commonly employed as a of Science and Technology). These materials mainly differed in the
post-modification method for solid CO2 adsorbents, which are arrangement of mesopores [41]. Fig. 5 summarizes the collective
treated as supports. This category includes materials like gra- efforts made in developing silica materials over the past few years,
phene, graphite, activated carbons, and metal-organic frame- with their primary textural properties are presented in Table 2.
works. Among these materials, silica stands out as it represents The unique properties of ordered mesoporous silica materials
the dominant research direction for amine functionalization have broadened potential applications as solid sorbents for CO2
[80,87]. Therefore, this review begins by focusing on this type of capture in various scientific and technological disciplines. They
CO2 capture materials. offer several advantages, including high adsorption capacity under
Fig. 4 illustrates the modification strategies, challenges, and dry, high-pressure conditions (approximately 45 bar) and at
current research directions of amine-based adsorbents. The size ambient temperature, large surface area and pore volumes, tunable
and color of the block sets change along the specialized investiga- pore size, low production cost, superior regeneration stability with
tion path, indicating that more specific areas of research are smaller low regeneration energy requirements, good selectivity over CH4
in size compared to those representing broader ones. The order is and N2, fast kinetics, or strong thermal and mechanical stability
consistently maintained: green > blue > purple > crimson. The [45e47]. However, a distinct barrier associated with these mate-
same principle has been applied to other CO2 capture materials as rials, and an ongoing research focus to overcome it, is their limited
well. hydrothermal stability, which involves the hydrolysis of SieOeSi
bonds. This limitation can affect their economic feasibility [48].
3.1.1. Silica-based adsorbents The final textural characteristics, including specific surface area,
Silica is the collective term for a group of minerals found in pore volume, pore size, and their distribution, can be modified by
various forms in the environment, typically as a crystalline solid adjusting the synthesis process. This offers significant potential for
with high hardness. It comprises silicon and oxygen, two of the increasing CO2 adsorption capacity and addressing specific defects,
most abundant elements in the Earth's crust. One of its most particularly through surface modification [49]. Moreover, silica
common forms is quartz, which is the planet's most prevalent materials possess morphological flexibility and porosity, making
mineral, constituting around 12% of its composition. The potential them amenable to the integration of a wide range of organic and
use of silica as an adsorbent for CO2 capture lies in the synthesis of inorganic groups through the functionalization process [50,51].
ordered mesoporous materials derived from it, possessing a pre- Another avenue of research involves the development of compos-
cisely defined structure. However, amorphous silica presents ite/hybrid materials by dispersing nanoparticles of different metals
challenges in supporting CO2 adsorption. This is due to issues within the porous structure of silica. This approach is advantageous
7
B. Dziejarski et al. Materials Today Sustainability 24 (2023) 100483

Fig. 4. The modification strategies and research directions of amine-based adsorbents.

when these materials are used as catalysts [52e54]. Additionally, silica materials, including silica nanoparticles, silica hollow
silica can be combined with various adsorbents, such as carbon spheres, silica nanotubes, silica fumes, mesocellular silica foams,
nanotubes (CNTs) [270], or MOFs [380], as discussed later in this macroporous silica, and aerogels [296]. Researchers investigate the
review. selection of suitable amine functionalities. The modification of
According to the literature, silica is mainly exploited as a sup- silica surfaces can be achieved through post-synthetic methods,
port material for amine aimed at enhancing CO2 capture, which is such as chemical grafting or physical impregnation, which have
a strategy for designing new adsorbents. Numerous studies have been extensively discussed before [55e57]. On the other hand,
also investigated the impact of moisture on CO2 adsorption amine functionalization can be accomplished by combining the
revealing that its content in the feed gas is beneficial for CO2 above methods. This involves impregnating amine onto silica that
uptake. As a result, a significant portion of research activity related has previously undergone grafting with amine-containing orga-
to silica-based adsorbents focuses on developing various types of nosilanes [58].

8
B. Dziejarski et al. Materials Today Sustainability 24 (2023) 100483

as new advanced materials that show excellent CO2 adsorption

properties. Fatima et al. [55] collected data on the development and
progress of silica functionalized with ILs, the mechanism of inter-
action, and the kinetics of CO2 adsorption. The authors stated that
traditional amines may readily be replaced with ionic liquids,
which offer tunable physicochemical features such as cation/anion
pairing, viscosity, and vapor pressure, among other properties.
Some crucial topics that should be addressed were also identified,
including the inability of ILs to be recycled along with the lack of life
cycle assessment, limited knowledge of the adsorption mechanism,
and the design of equipment for use on an industrial scale.
Fig. 6 illustrates current and future research directions of silica-
based adsorbents. Tables 3 and 4 summarize the CO2 uptake and
textural properties of silica-based materials with specific amine
functionalization methods.

3.2. Carbon-based adsorbents

The success of the CO2 adsorption process essentially depends

on the adsorbent material used. The rising levels of CO2 emissions
into the atmosphere have spurred significant interest among sci-
entists and researchers in developing technologically advanced
materials for gaseous media storage. Carbon-based materials have
gained a wide interest due to their rather unusual physical and
Fig. 5. Comparative overview of silica-based materials for CO2 capture. chemical properties highly related with the CO2 uptake abilities.

Table 2
Textural properties of different types of mesoporous silica-based materials [42e44].

Silica-based material BET surface area, m2/g Total pore volume, cm3/g Pore diameter, nm

MCM-41 1229 1.15 2.7

SBA-15 950 1.31 6.6
MSU-1 1021 0.40 e
HMS 561 1.44 9.8
KIT-6 895 1.22 6.0
FDU-15 660 0.44 10.2
KIL-2 702 1.61 9.55

Zhang et al. [57] summarized recent advances between 2017 and They are characterized by low-cost precursor materials, low den-
2019 in amine-functionalized silica for CO2 capture. In their sys- sity, diverse carbon structural forms (powder, fibers, aerogels,
tematic review of the literature, the authors found few issues which composites, sheets, monoliths, tubes), high surface area, tailored
need to be addressed for future practical applications. In the case of surface chemistry (O, N, S, P, F, or other heteroatom doping),
the amine-impregnated silica, while functionalization with high extensive pore morphology, large pore volumes, and very high
concentrations of amines is advantageous for easy sorbent prepa- resistance to rapid changes in temperature and pressure [94e96].
ration, a significant problem with these materials is their stability Among other attributes, they are distinguished by fine reproduc-
during many adsorption-desorption cycles. This matter is related to ibility and electronic properties [97,98]. Additionally, they possess
the leaching and degradation of amines, which can potentially be the following unique features, which are especially highly relevant
solved by introducing amines with higher boiling points or by for CO2 capture, as follows: (1) excellent stability, particularly in
reducing the operating temperature. In contrast, amine-grafted sil- high and humid environments; (2) a hydrophobic surface, where
ica is stable throughout the cycles, but the amine loading is limited, CO2 sorption on their surface is not affected by moisture; (3) a
and the synthesis method is more rigorous, resulting in lower CO2 reversible nature of physical adsorption, where regeneration con-
adsorption capacity. In addition, the authors noted that there is an sumes less energy (weak van der Waals forces); (4) effectively
insufficient number of research results on one-pot synthesis, which suitable for adsorption usage under atmospheric pressure [94].
should receive more attention as a research direction. Chen et al. [56] Carbon-based adsorbents comprise a diverse range of materials
drawn similar conclusions in their paper, which focused on with varying morphologies, structures, and precursor sources.
contemporary progress in amineesilica composites, including the These materials can be broadly categorized into several basic
preparation and characterization of adsorbents, CO2 capture under groups, such as activated carbons, hydrochar, biochar, graphene,
dry and moisture conditions, and stability after many cyclic fullerenes, graphite, and carbon nanotubes (Fig. 7).
adsorptiondesorption runs. Furthermore, it was shown that
although there are several successful methods for immobilizing 3.2.1. Biochar and hydrochar
amine species on a silica surface through a chemical grafting process, There has been a notable rise in demand for biomass-derived
innovative procedures capable of achieving larger amine loadings products along with industrial waste containing char across
are still required. various economic sectors. This response stems from the pressing
Future research paths should also consider the potential effects environmental challenges we currently face, encompassing CO2
of silica functionalization by an amine moiety in ionic liquids (ILs), emissions, the climate crisis, and industrial contamination.
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B. Dziejarski et al. Materials Today Sustainability 24 (2023) 100483

Fig. 6. The modification strategies and research directions of silica-based adsorbents.

Nowadays, scientists are concentrating their efforts on developing relies on thermochemical decomposition of organic matter present
biochar and hydrochar, mainly due to the cost-effectiveness and in waste biomass into structural carbons within a high pressure and
sustainability merits [99]. temperature water environment [103]. HTC is typically performed
Therefore, the focus has been highly diverted from other at temperatures ranging from 180 to 260
C. During this step,
carbonaceous materials for the purpose of CO2 capture. The clas- biomass and water are combined, then subjected to high pressures
sification of feedstock employed in the synthesis of biochar and of around 2e6 MPa for a duration of 5e240 min [104,105]. Among
hydrochar is one of the greatest paramount importance in deter- the specific parameters of HTC, process water exhibits character-
mining the most optimal production method for the conversion istics akin to those of organic solvents and function as a catalyst in
process. In view of this, there are many different types of carbon- the biomass transformation through decarboxylation, condensa-
rich biomass that can serve as perspective, abundant and sustain- tion, aromatization, hydrolysis, and dehydration [106]. The result-
able sources. These sources include residues from agriculture or ing product based on converting organic material consists of
forestry, food and energy crops, animal by-products, wood resi- carbonized material (hydrochar), liquid bio-oil, and gaseous vola-
dues, as well as municipal wastes (Fig. 8) [99,100]. tile vapors. The final solid product preserves a considerable per-
Many studies have explored thermal conversion as an alterna- centage of the original biomass structure, making it particularly
tive path to biomass processing, aiming to generate value-added valuable for carbon dioxide storage applications [107]. HTC char
products for CO2 applications. This approach can break the chem- generally retains between 55 and 90% of the original mass of the
ical bonds in organic matter and directly convert its intermediates feedstock while possessing 80e95% of its energy content [108].
into char, bio-oil, and syngas [101]. Consequently, the biomass Recently, a few reviews related to this research scope were
processing procedure strives to obtain char as a potential adsor- published between 2018 and 2021. Goel et al. [103] examined fac-
bent, increasing the carbon content within the solid product [102]. tors necessary for achieving higher yields of biochar and hydrochar
The most common ways to produce biochar and hydrochar, suitable for CO2 capture. The authors highlighted several crucial
respectively, are through the processes of pyrolysis and hydro- process parameters affecting the sorption properties of the final
thermal carbonization (HTC). HTC product, including the type of feedstock, temperature, pres-
sure, residence time, biomass-to-process water ratio, and the use of
[Link]. Hydrochar. Hydrochar is synthesized through hydrother- a catalyst. Fang et al. [109] presented a concise summary of the
mal carbonization, abbreviated as HTC, which may be used to potential applications of hydrochar and outlined the primary steps
produce low-cost CO2 capture materials. This conversion process involved in the hydrothermal carbonization of biomass. They
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B. Dziejarski et al. Materials Today Sustainability 24 (2023) 100483

Table 3
Influence of amine functionalization on textural properties and CO2 uptake of silica-based adsorbents.

Silica-based adsorbents Functionalization agent Amine loadings BET surface Total pore CO2 uptake, CO2, Adsorption Pressure, Reference
(Nitrogen) area, m2/g volume, mmol/g vol% temperature, bar


cm3/g C

Physical impregnation method

SiO2-NS Polyethyleneimine 50 wt% 463.5 1.3 4.01 100 75 1 [59]
SBA-15 Polyethyleneimine 50 wt% 49.0 0.09 0.83 100 25 1 [60]
1.70 45
2.04 75
SBA-15 Polyethyleneimine 50 wt% e e 3.94 100 75 1 [61]
MCM-41 Polyethyleneimine 50 wt% 1254 2.44 3.19 100 75 1 [62]
Si-MCM-41 Polyethyleneimine 50 wt% 6 0.00 2.26 e 100 1 [63]
Silica monoliths Tetraethylenepentamine 11.5 mmol N/g 13 0.07 2.23 10 25 1 [64]
Silica powder Tetraethylenepentamine 12.8 mmol N/g 35 0.17 2.56 10 25 1 [64]
KIT-6 Polyethyleneimine 50 wt% e e 3.07 100 75 e [65]
KIL-2 Tetraethylenepentamine 50 wt% 177 0.46 3.37 e 25 1 [44]
4.35 95
KIL-2 Polyethyleneimine 50 wt% 127 0.35 2.19 e 25 1 [44]
3.60 95
MSU-J Tetraethylenepentamine 50 wt% 185 0.54 3.73 100 25 1 [66]
Platelet mesoporous silica Branched polyethyleneimine 50 wt% 29.2 0.115 5.65 10 75 e [67]
Granular silica Polyethyleneimine 50 wt% 44 0.41 2.39 95 25 1 [68]
3.06 55
3.11 85
Microspherical silica Polyethyleneimine 50 wt% 29 0.22 2.27 95 25 1 [68]
3.07 55
3.26 85
Silica Tetraethylenepentamine; e 5.9 0.0 2.00 15 30 e [69]
1,2-epoxybutane
Mesoporous silica Polyethyleneimine/diethanolamine 7.4 mmol N/g 74 0.46 2.93 100 35 e [70]
~
(PEI/DEA50:50)
ILs-SBA-15 Tetraethylenepentamine ([TEPA] 66 wt% 21.90 0.008 2.15 15 60 0.15 [71]
[NO3])
Chemical grafting method
MCM-41 N1-(3-trimethoxysilylpropyl) 6.39 mmol N/g 38.75 0.4096 2.10 10 75 0.2 [72]
diethylenetriamine
Silica monolith 3-aminopropyltrimethoxysilane 4.83 62 0.22 1.13 10 25 1 [64]
Silica powder 3-aminopropyltrimethoxysilane 4.95 103 0.32 1.14 10 25 1 [64]
SBA-15 N1-(3-trimethoxysilylpropyl) 3.14 mmol N/g 434 1.13 1.88 5 25 1 [73]
diethylenetriamine
SBA-15 Diethylenetriamine alkoxysilane e 81 0.15 2.00 100 45 1 [74]
Spherical silica gel 3-Aminopropyltriethoxysilane e 203.59 0.49 1.56 1 35 e [75]
Silica gel, dry grafted N1-(3-trimethoxysilylpropyl) 3.39 mmol N/g 152 0.62 1.35 100 25 1 [76]
diethylenetriamine
Silica gel, wet grafted N1-(3-trimethoxysilylpropyl) 5.12 mmol N/g 73.1 0.31 1.97 100 25 1 [76]
diethylenetriamine 2.3 75
KIT-6 (3-Aminopropyl)triethoxysilane 2.44 mmol N/g 90 0.22 1.56 e 30 1 [77]
HMS “as made” Polyethyleneimine 50 wt% 11 0.02 2.40 100 45 1 [78]
HMS “calcined” Polyethyleneimine 70 wt% 2.1 <0.01 2.19 100 45 1 [78]
Hierarchical bimodal silica, Diethylenetriamine alkoxysilane 28 wt% 203 0.96 1.72 70 25 1 [79]
dry grafted
Hierarchical bimodal silica, Diethylenetriamine alkoxysilane 49 wt% 28 0.19 2.31 70 25 1 [79]
wet grafted
MCM-41 Aminopropyl organosilanes e 544 0.74 0.87 100 45 1 [80]
MCM-41 Ethylenediamino organosilanes e 421 0.60 1.51 100 45 1 [80]
MCM-41 Diethylenetriamino organosilanes e 373 0.54 1.75 100 45 1 [80]
SBA-15 Diethylenetriamine e 204 0.36 1.90 100 45 1 [81]
Silica particles (0.5e1.5 nm) Si-[P8883]TFSI e 263.9 0.1208 0.99 100 40 1 [82]
One-pot synthesis
ILs-Silica aerogels (3-Aminopropyl)triethoxysilane e 6.37 e 5.53 50 e 1 [83]
Precipitated silica (3-Aminopropyl)triethoxysilane 30 wt% 7.34 0.12 1.025 100 50 1 [84]
Silsesquioxane aerogel (3-Aminopropyl)triethoxysilane e 146.3 1.52 3.04 1 50 1 [85]
Mesoporous silica powder Polyethyleneimine 54.09 wt% 413.9 0.27 2.82 15 75 1 [86]
Double functionalization
Pore expanded Aminopropyl/ 50 wt% 169 0.20 2.37 100 45 1 [80]
MCM-41 Tetraethylenepentamine
Pore expanded Diethylenetriamino/ 50 wt% 162 0.18 2.13 100 45 1 [80]
MCM-41 Tetraethylenepentamine
Pore expanded Aminopropyl/ 30 wt% 88 0.16 1.53 100 45 1 [80]
MCM-41 Pentaethylenehexamine
MCM-41 3-aminopropyltrimethoxysilane/ 30/40 wt% 33.7 0.05 3.50 15 70 1 [87]
Tetraethylenepentamine

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 B. Dziejarski et al. Materials Today Sustainability 24 (2023) 100483

brought attention to the necessity for unique syntheses and crea-

Reference

tive manufacturing techniques that are crucial for the development

[88] of value-added tailored carbon products from hydrochar. Moreover,
[89]

[64]
[64]
[90]

[91]
[92]
[93]
[85]
to promote the practical implementation of hydrochar on an in-
dustrial scale, support for the concept of engineered hydrochar is
Pressure,

also necessary in the research field. Unfortunately, there is still a

0.15

noticeable lack of a critical literature review closely related to

bar

1
1
1

1
1
1
1 hydrochar for CO2 capture and its utilization in cyclic regeneration
systems at different scale. Precise systematization of current
temperature,
Adsorption

knowledge would significantly improve the scaling process of using

these materials and increase their technological maturity.
Hydrochar itself obtained exclusively from the HTC process
25

75
75
70
50
40
75

25
25
C

often exhibits a poorly developed microporosity and a low specific

surface area, posing challenges for its use in CO2 sorption purposes
vol%
CO2,

0.15
10

15
10
15
15

10
15

[110]. To improve the above properties, physical or chemical acti-

1

vation is widely reported as essential step to synthesize biomass-

Humid CO2

derived activated carbons (Fig. 9). As section 3.2.2 is devoted to

CO2 uptake, mmol/g

ACs and the activation processes, the most important theoretic

3.12

4.02
4.28
2.27
3.84
4.97

1.96
5.05

3.84

aspects of this material will be covered there.

[Link]. Biochar. Biochar is a carbonaceous material obtained by

Dry CO2

pyrolysis, which involves the thermal decomposition of biomass

2.23

3.52
3.45
2.44
4.07

1.21
1.63

3.04
2.2

under the influence of elevated temperature (ranging from 300 to

650
C) in the absence of oxygen or other oxidizing agents.
Total pore

Following the completion of this process, three distinct groupings

volume,
cm3/g

of products are created: gaseous (volatile parts), liquid (polycyclic

0.07

0.28
0.02
1.80

0.03
0.01

1.52

aromatic hydrocarbons and water, the so-called bio-oil), and solid

e

(high-carbon solid residue as well as ash, termed as biochar) [111].

BET surface
area, m2/g

A solid char, as in the case of hydrothermal carbonization, due to its

porous structure, the prospect for a large storage capacity, and the
146.3
Comparison of CO2 adsorption capacity of several functionalized silica-based adsorbents in dry and humid feed streams.

0.09
261

existence of fundamental functional groups, has been recognized as

13

90
16

e
3
8

an ecologically favorable and sustainable material in terms of CO2

capture [112]. Considering a supply of biomass, it is approximately
Amine loadings

11.5 mmol N/g

13.2 mmol N/g

10 times less expensive than other CO2 adsorbents on the market

(Nitrogen)

and the cost of production is approximately one-sixth of that of ACs

63.8 wt%
50 wt%
50 wt%
60 wt%

30 wt%

[113]. First and foremost, biochar is stable and does not degrade
easily, its carbon half-life is between 100 and 107 years during
e
e

exposition to ambient oxidation [114]. The ability of biochar to

adsorb CO2 is largely determined by its physicochemical charac-
teristics, such as specific surface area, pore sizes, total pore volume,
Tetraethylenepentamine

Tetraethylenepentamine
Tetraethylenepentamine

basicity of biochar surface, presence and type of surface functional

Functionalization agent

groups, appearance of alkali and alkali earth metals, hydrophobic-

Polyethyleneimine
Polyethyleneimine

Polyethyleneimine
Polyethyleneimine

Polyethyleneimine

ity, polarity, and aromaticity [115]. The aforementioned properties

(3-Aminopropyl)
triethoxysilane

are inherently interconnected with the composition of the feed-

stock used in its formation as well as the thermochemical condi-
tions. Biochar main component is obviously carbon, but there is
also hydrogen, oxygen, nitrogen, a mineral substance, and trace
amounts of sulfur [116]. Low-mineral biochars with a high content
of carbon element are used for energy applications and the pro-
duction of ACs. Consequently, the substantial concentration of
mineral substances in biochars may potentially provide a beneficial
Physical impregnation
Physical impregnation

Physical impregnation
Physical impregnation
Physical impregnation

Physical impregnation
Physical impregnation
Physical impregnation

effect on fertilizer and sorption utilization [117].

Type of the surface

One-pot synthesis

Many review articles have described the current state of

knowledge on biochar between 2019 and 2022, with a particular
modification

emphasis on its use in CO2 adsorption, as opposed to hydrochar.

Jung et al. [118] devoted significant attention to advancing current
research on activated biochars for CO2 adsorption, derived from
various biomass sources. According to the final findings of authors,
the production of activated biochars from biomass holds promise as
5A@mesoporous

Mesoporous silicas
Macroporous silica

Fibrous nanosilica

Mesoporous silica

a viable approach for creating the required CO2 capture materials.

multilamellar

Silica monoliths
Silica monoliths
silica vesicle

Silsesquioxane

However, consideration needs to be given to the optimization of

Mesoporous
Silica-based

pyrolysis and activation parameters to enhance energy efficiency,

Core-shell
adsorbent

aerogel
silica

reduce chemical usage, and minimize reaction time. This can be

Table 4

achieved through methods such as microwave-assisted pyrolysis or

combining pyrolysis and activation into one step. Other aspects that
12
B. Dziejarski et al. Materials Today Sustainability 24 (2023) 100483

alkalinity to enhance the CO2 adsorption capacity. Additionally,

biochar can undergo various post-treatment modifications,
including chemical activation (NaOH, KOH) [119], physical activation
(CO2, steam) [119,120], amine functionalization [121], high-
temperature treatment with chemical mixtures of CO2 with
ammonia [120,122], ammonification with ammonia (NH3)
[120,122], and metal incorporation [123,124] (Fig. 10). Shafawi et al.
[125] provided an overview of current research directions on the
production of engineered biochar by various modifications to in-
crease its CO2 capture capacity. The present study evaluated and
discussed the influence of several modification strategies involving
physical, chemical, and physicochemical treatments, on the modi-
fied biochar. Authors suggested that future studies aimed at
improving CO2 uptake, by significantly increasing surface area,
micropore volume, and surface chemistry, could benefit from
combining multiple modifications. These could consist of function-
alization with alkali and amines or doping with metal or metal oxide,
which can be empirically and conceptually proven to be significant.
Moreover, density functional theory (DFT) was identified as a
feasible way to uncover relevant details associated with biochar
modifications and the CO2 adsorption mechanism. In conclusion, it
was recommended that further research be conducted to investigate
the stability and regeneration of spent biochar, expanding its role in
green chemistry and climate change mitigation. Dissanayake et al.
[126] also summarized an assessment of the potential use of both
Fig. 7. Applicable carbon-based materials for CO2 capture.
pristine and tailored biochar as CO2 adsorbent. In particular, they
discussed the variables affecting CO2 adsorption capacity and the
deserve future exploration include in-depth practical research on challenges connected with biochar synthesis. The final conclusions
CO2 separation from flue gas mixtures under varying conditions, emphasized the importance of future research in creating cost-
and the discovery of appropriate examination methods for poten- effective and environmentally friendly biochar-based composites
tially abundant biomass to lower sorbent production costs (natu- (incorporating metal-organic frameworks, and carbon-based
rally heteroatom-doped and metal-impregnated biomass nanomaterials) for extensive implementation in large-scale CO2
precursors can reduce the need for surface treatment processes). capture technologies. On top of that, the primary importance should
The regulation of thermochemical process parameters and the be placed on the development of innovative techniques for regen-
implementation of specific modification strategies are also crucial erating and recycling captured CO2.
considerations for biochars. The main objective is to modify surface Among the research on modification of biochars, several
characteristics such as mesoporosity, microporosity, basicity, and important studies can be identified. Lahijani et al. [123] studied

Fig. 8. Suitable types of biomass for the production of biochar and hydrochar.

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B. Dziejarski et al. Materials Today Sustainability 24 (2023) 100483

Fig. 9. The modification strategies and research directions of hydrochar.

Fig. 10. The modification strategies and research directions of biochar.

14
B. Dziejarski et al. Materials Today Sustainability 24 (2023) 100483

the development of metal incorporated biochar as an inexpen- the presence of nitrogen functional groups, become more promi-
sive and durable adsorbent for CO2 capture at ambient temper- nent. The same author conducted additional research on the effect
atures. Biochars were created from walnut shell using a simple of the same modification at different temperatures on CO2
one-step pyrolysis procedure, and then different metals were adsorption [120].
introduced into the biochar skeleton using a simple impregna- Madzaki et al. [121] examined the properties of raw sawdust
tion approach followed by heat treatment to increase the CO2 biochar and amine treated sawdust biochar. The highest CO2 cap-
adsorption capacity. The Mg-loaded biochar exhibited the ture capacity of amine treated biochar was 1.09 mol/g, at temper-
greatest CO2 uptake of 1.82 mmol/g when compared to the other ature of 30
C. The incorporation of nitrogen functionalities into the
metalized biochars. carbon surface of the treated biochar resulted in lower CO2
Creamer et al. [124] synthesized and described aluminum hy- adsorption than that of untreated biochar. In addition, the incor-
droxide, magnesium hydroxide, and iron oxideebiochar compos- poration of nitrogen functionalities onto the carbon surface may
ites, as well as evaluated their capacity to capture CO2 at ambient lead to a reduction in the exposed surface area of the biochar.
temperature and atmospheric pressure. They subjected biomass Table 5 presents a comparative analysis of modification strate-
feedstocks to pretreatment with various metal ions and subse- gies impact on the CO2 adsorption capacity and textural properties
quently pyrolyzed them at 600
C. This resulted in a greater CO2 of biochar. The following data presents a concise overview of the
uptake in the composites, especially in those with optimum metal- principal results obtained from current research using modified
to-biomass ratios, when compared to unmodified biochar. Each biochar for the purpose of carbon dioxide adsorption. The scope of
composite possessed a reasonably high surface area and primarily biochar activation is presented in section 3.2.2 on activated car-
absorbed CO2 by physical adsorption. While Fe2O3ebiochar com- bons, so it will not be present here deeply.
posites showed the maximum surface area, AlOOHebiochar com-
posites demonstrated the highest adsorption capacity, reaching 3.2.2. Activated carbons (ACs)
1.61 mmol/g at 25
C, equivalent to that of commercial adsorbents. Activated carbons are indisputably the most thoroughly
Zhang et al. [122] used soybean straw as a raw material to researched, extremely effective, and attractive material among
synthesize highly efficient adsorbents, specifically nitrogen-doped carbon materials for capturing CO2 from the flue gas stream [129].
porous modified biochars. The authors evaluated three distinct Their main advantages as adsorbent include cost-effectiveness, low
modification methods for manufacturing these materials, namely temperature required for desorption, straightforward regeneration
CO2 activation, ammonification with ammonia, and high temper- process, low energy consumption, fast CO2 sorption kinetics, high
ature treatment with a combination of carbon dioxide and thermal and chemical stability, mechanical strength, or exceptional
ammonia. Combining the CO2 activation and NH3 ammonification thermal conductivity [130e132].
processes not only enhanced the formation of micropore structures The production of activated carbons (Fig. 11) is based on the use
in soybean straw-modified biochar but also increased the intro- of large amounts of waste biomass or industrial waste rich in high
duction of nitrogen functional groups onto the surface. The carbon concentration and low inorganic content [133,134]. ACs can
micropore structure of modified biochars was found to be the most also be manufactured from natural charcoal resources such as coal
critical attribute influencing their CO2 capture capability at lower and lignite [135,136]. Moreover, the synthesis method may also use
adsorption temperatures, when comparing the physicochemical synthetic polymers, although at a notable rise in manufacturing
parameters of modified biochars. In contrast, as the adsorption costs. These synthetic polymers may include mixes of cellulose
temperature increases, the influence of the micropore structure with polystyrene, waste resins, or polyvinylidene chloride. There-
gradually diminishes, and the chemical characteristics, particularly fore, the low price and widespread availability of carbon-rich raw

Table 5
The effect of biochar modification strategies on textural properties and CO2 uptake of biochar.

Biochar precursor Temperature Residence BET surface Total pore CO2 CO2 CO2 adsorption Adsorption Reported treatment Purpose of Reference
of pyrolysis, time, h area, m2/g volume, selectivity uptake, temperature,
C pressure, sources/chemicals modification


C cm3/g at 1 bar mmol/g bar method

Walnut shell 900 1.5 292 0.157 e 1.86 25 1 Metal incorporation Improving the [123]
(Mg) surface
Cottonwood 600 3 275 0.01 e 1.45 25 1 Metal incorporation properties and [124]
(Mg:biochar ¼ 0.01) enhancing the
Cottonwood 600 3 367 0.37 e 1.61 25 1 Metal incorporation interaction [124]
(Al:biochar ¼ 4) with CO2
Cottonwood 600 3 654 0.19 e 1.48 25 1 Metal incorporation [124]
(Fe:biochar ¼ 4)
Rambutan peel 900 1.5 505 0.28 e 1.72 25 1 Metal incorporation [127]
(Mg)
Soybean straw 500 e 365 e e ~1.80 30 1 High temperature Increasing [122]
NH3 treatment basicity and
level-up N-
contents
Soybean straw 500 e 491 e e ~2.02 30 1 High temperature Developing [122]
Cotton stalk 600 e 627 e e ~2.16 e 1 NH3 and CO2 porosity, [122]
treatment increasing
Cotton stalk 600 e 436 e e ~1.77 e 1 High temperature basicity along [122]
NH3 treatment with level-up
Chicken manure 450 1 302 0.22 79.1 10.15 20 1 HNO3 and NH3 N-contents [128]
treatment
Sawdust 750 e 0.61 e e 0.90 30 1 Amine [121]
Sawdust 850 e 3.17 e e 1.02 70 1 functionalization [121]
(monoethanolamine)

15
B. Dziejarski et al. Materials Today Sustainability 24 (2023) 100483

Fig. 11. Schematic diagram of activated carbons pre-treatment steps.

material sources, along with the production on an industrial scale, Among the activating gases, CO2 is considered one of the most
offer a significant competitive edge to ACs compared to other ad- advantageous factors due to its ability to create narrow micropores
sorbents. However, due to the quite diverse properties of raw ma- of large volume, suitable for the kinematic diameter of the CO2
terials, activated carbons are characterized by a different structure molecule [143]. In the case of AC activation with steam, the existing
(porosity and specific surface area), implying that the overall course pores are enlarged [140]. In the case of activation with steam, the
of the CO2 adsorption process is changeable [131]. existing pores are enlarged [140]. On the other hand, using a gas
Activated carbons offer a wide distribution of an extensive porous mixture of H2O þ O2 as an activating agent leads to rapid reaction
structure, mainly microporous and mesoporous, where the size of kinetics, resulting in an active carbon structure with random
the specific surface ranges from 500 to about 3000 m2/g [137]. The porosity and substantial char losses. Consequently, its use is not
pores within the ACs structure may have different shapes depending recommended [144e146]. The effect of activation gases is also
on the type of hysteresis loop present in the multilayer range of chemical in nature and involves the elemental carbon oxidation of
physisorption isotherms. In most cases, they correspond to H1 material. For activation with CO2, the general reaction, also known
(nearly vertical and parallel adsorption and desorption branches) as the Boudouard reaction, may be described as follows [140]:
and H2 (sloping adsorption branch and nearly vertical desorption
branch) types, defining the shape of the pores as cylinders open on kJ
C þ CO2 /2CO DH ¼ þ171 (1)
both sides, or alternatively, as ink bottle-shaped pore. mol
The CO2 adsorption capacity of ACs can also be increased by the The above reaction can be written in more details by separating
presence of heteroatomic functional groups in the form of con- it into two distinct phases, i.e., dissociative chemisorption
nections: carboneoxygen, carbonenitrogen or carbonesulfur on its (involving the dissociation of CO2 on the surface of carbon material
surface. They can be categorized into acidic, such as carboxyl, along with the formation of an oxide on its surface) and desorption
lactone, or phenolic groups, and basic, including chromene, ketone, of the surface oxide (in which the oxide is desorbed from the sur-
or pyrone groups [138]. The most important functional groups face, and CO is produced) [147]:
contain oxygen atoms, which contribute the outer surface a hy-
drophilic (polar) nature, in addition to the hydrophobic (nonpolar)  Dissociative chemisorption
character shown by the internal structure. The inherent duality of
ACs surfaces enables them to effectively adsorb a diverse array of C þ CO2 /CO þ CðOÞ (2)
gases, with a particular emphasis on greenhouse gases (GHGs),
therefore mitigating their release into the atmosphere.
 Surface oxide desorption
[Link]. Physical activation. Thermochemical conversion (hydro-
thermal carbonization, or pyrolysis) and activation are the two CðOÞ/CO (3)
basic steps in the preparation of ACs. The char structure with un-
For activation using H2O, the general reaction can be presented
developed porosity (especially microporosity) and a small specific
as follows [148]:
surface, which for a significant useful applications of CO2 adsorp-
tion, are unsatisfactory, as highlighted before [131,139]. To improve kJ
the above parameters, the activation process (physical or chemical) C þ H2 O/CO þ H2 DH ¼ þ117 (4)
mol
is performed, by using a specific thermal treatment, which ulti-
mately facilitates the improvement of carbon dioxide storage effi- In the physical activation mechanism of O2, it runs according to
ciency. Specifically, this treatment leads to the expansion or the following reactions [149,150]:
creation of new pores at both the micro and meso sizes.
Physical activation entails the partial gasification of raw mate-  Chemisorption
rials in the presence of oxidizing gases at a temperature of 800
C-
1000
C, such as water vapor, CO2, air, or their mixtures [140]. The kJ
2C þ O2 /2CðOÞ DH ¼ 395 (5)
process can be classified into two distinct ways, either in combi- mol
nation with thermochemical conversion or as an independent
operation, i.e., the direct approach and the two-step approach. In  Carbon gasification
the direct way, thermochemical conversion is performed in the
presence of nitrogen flow until the reaction is complete. The N2 kJ
flow is then stopped, and the activation gas is immediately intro- C þ O2 /CO2 DH ¼ 395 (6)
mol
duced at the temperature. In the case of the second method, the
activation process is divided into two steps. During it, the conver-
sion of feedstock is carried out while maintaining a continuous  Oxide gasification on the surface of carbon material
supply of nitrogen flow. The process mentioned continues until an
adequate amount of carbonaceous material is generated and kJ
CðOÞ þ O2 /CO2 þ CO DH ¼ 111 (7)
collected afterward, then the activation is processed [141,142]. mol

16
B. Dziejarski et al. Materials Today Sustainability 24 (2023) 100483

The development of char porosity, specifically the capillary

Reference
structure, as a direct outcome of physical activation occurs

[153]
[154]
[154]
[155]
[156]
[157]
[150]
[158]
[159]
[159]
[160]
[161]
[162]
[163]
[164]
[165]
[158]
[150]
[166]
[167]
[168]
[169]
through the reaction of oxidizing gases with amorphous carbon.
These activating gases penetrate the internal structure of the
precursor surface, resulting in the opening and widening of pre-

pressure, bar
Adsorption
viously inaccessible pores and the creation of new ones [151]. This
process is the effect of complex mechanisms, including the

1.30
diffusion of reactants to the surface of the carbon material and

1.3

10
10
1
1
1

1
1
1
1

1
1
1
1
1
1
1
1
1
1
1
into the pores, their chemisorption on the surface, chemical re-
actions, and the subsequent desorption of reaction products.

CO2 uptake, mmol/g

~2.95
25
C
Additionally, physical activation promotes the presence of func-

1.88
2.13

2.94
1.66
2.02

3.90

2.20
1.58
3.48

2.11
4.38
3.1

1.7

3.1

1.8

2.7

3.2
tional groups containing oxygen atoms, such as phenolic, ketone,

e
4.28 (30
C)
4.66 (30 C)

1.58 (20
C)
and carboxyl groups [152].

To date, CO2 capture has been achieved using various of

2.945

~3.28
3.10

5.60

3.50
4.07

3.11
0
C
physically activated carbon adsorbents from char, as given in

6.1
e
e
e
e
e
e

e
e

e
Table 6. The majority of research findings highlight the potential of

CO2 selectivity
biomass as a viable and sustainable raw material for AC synthesis
through physical activation. Currently, laboratory-scale research

at 1 bar

~ 42.00
primarily concentrates on identifying new precursors and opti-

~73.00
18.00

24.20

13.00
68.50
12.30

15.00
36.10
7.60
7.00
mizing activation parameters to enhance CO2 uptake.

e
e
e
e

e
e

e
e

e
Li et al. [153] synthesized AC from rice husk that was leached

volume, cm3/g
with potassium carbonate after being activated with CO2. The
resulting material was then examined for its CO2 adsorption ca-

Mesopore
pacity, kinetics, and regeneration. The studies revealed that the

0.014

0.049
0.49

0.17
0.04

0.10
activated carbon possessed a dual pore structure comprising mi-

e
e
e
e
e
e
e

e
e

e
e
e
e
e
e
e
cropores and mesopores. The BET specific surface area, mesopores
volume, and micropores volume were 1097 m2/g, 0.49 cm3/g, and volume, cm3/g
0.34 cm3/g, respectively. The developed AC demonstrated both a
Micropore

high CO2 adsorption capacity, reaching 3.1 mmol/g, and excellent

0.373

0.245
0.34

0.28
0.08
0.27

0.52
0.40

0.55
0.11
0.24

0.21
0.34
0.53
0.18
CO2 selectivity of 7.6 at 25
C and 1 bar, respectively. These values
Influence of precursors, physical activation process conditions on textural properties and CO2 uptake of activated carbons.

e
e
e

e
e

e
were comparable to those of AC produced by chemical activation
volume, cm3/g

with KOH serving as the activator.

Total pore

Rashidi et al. [154] conducted research on the volumetric CO2

adsorption utilizing AC made from palm kernel shells. The carbon

0.476

0.374
0.171
0.67
0.22
0.45

0.09

0.51
0.69
0.44

0.65
0.15
0.24

0.36

0.39
0.63
0.34
0.34
was directly activated at 850
C for 1 h. The obtained AC
e

e
demonstrated a satisfactory CO2 adsorption capacity of
BET surface
area, m2/g

2.13 mmol/g along with excellent regeneration performance of 7.0

1190.65
798.38
167.08

955.06

810.85
and stability after many cycles.
660.7
367.8
821.7
1097

1215

1327

1296
697

424

371
593
767
573
862
557
858

424
Ogungbenro et al. [156] investigated the preparation of AC
from date fruits as a promising adsorbent material. The AC syn-
Activation temperature,

thesis involved pyrolysis in a furnace, followed by activation in a

carbon dioxide environment at temperatures ranging from 600 to
900
C. Among the samples, the one pyrolyzed at 800
C and
activated at 900
C for 1 h exhibited the highest CO2 adsorption
capacity, reaching 3.21 mmol/g. This can be attributed to its su-
perior textural properties, including a BET specific surface area of
1000
900
850
850
600
900
800
650
800
900

850
800
800
700
800
900
750
650
900
880
700
500

798.38 m2/g, a micropore area of 712.87 m2/g, and a micropore

C

volume of 0.28 cm3/g.

Activation

Two-step
Two-step
Two-step

Two-step

Two-step
Two-step
Two-step

Two-step
Two-step
Two-step
approach

Puig-Gamero et al. [159] studied the influence of physical

Direct
Direct
Direct

Direct
Direct
Direct
Direct

Direct
Direct

Direct
Direct

Direct

activation parameters involving CO2 and steam on the production

of AC derived from olive stones and its CO2 adsorption capabilities.
For H2O activation, the determined conditions were 900
C,
Activating agent

30 min, 0.15 ml/min, and 1 bar. In the case of CO2 activation, the
Steam (H2O)

optimal conditions were found to be 900
C, 30 min, 300 ml/min,

O2 (3%)

O2 (3%)
Steam

Steam

and 1 bar. Furthermore, the ACs demonstrated respectable CO2

CO2

CO2
CO2
CO2
CO2

CO2

CO2
CO2
CO2
CO2
CO2
CO2
CO2
CO2

CO2
CO2

CO2

adsorption capacity of 4.28 and 4.66 mmol/g at 30
C and 10 bar,

with BET specific surface area of 955.06 and 1190.65 m2/g, and
Amazonian andiroba shell

total pore volumes of 0.44 and 0.69 cm3/g for CO2 and H2O acti-
vation, respectively.
To sum up, several comparative studies have been conducted in
Palm kernel shell

Palm kernel shell

Olive mill waste

Palm date seeds

Coffee grounds
Rice husk char

recent years to evaluate various activating agents for physical

Coconut shell
Coconut shell

Almond shell
Almond shell

Walnut shell
Olive stones
Olive stones
Olive stones
Olive stones

Vine shoots
Date seeds
Date stone

Pine cones

activation. The physical activation method of steam activation is

Precursor

Nutshell

widely utilized, yielding activated carbon possessing a substantial

Table 6

Peat

surface area and micropore volume. However, the process neces-

sitates elevated temperatures and prolonged activation periods,
17
B. Dziejarski et al. Materials Today Sustainability 24 (2023) 100483

resulting in a high demand for energy and a prolonged duration. On Generally, CO2 adsorption mechanism depends on the type and
the other hand, the use of CO2 as an activating agent requires less volume of pores in the ACs structure. Carbon materials with mi-
energy and can be carried out at lower temperatures compared to cropores, especially pores with diameters less than 1 nm, were
steam activation. The process yields activated carbon that exhibits found to show a high capacity to adsorb CO2 [188,189]. In addition,
substantial surface area and pore volume, albeit potentially leading these pore sizes favor the diffusion of CO2 in the materials, which
to a reduced micropore volume relative to steam-activated carbon. makes the adsorption kinetics very fast [190]. For several years, the
Further, air activation has the capability to generate activated carbon interest of researchers has focused on the use of waste residues and
featuring diverse pore sizes and surface areas. Its application is not as biomass as a precursor to produce activated carbons. Among the
frequent owing to the potential hazard of oxidation and combustion works published between 2010 and 2022, there are several that
of the precursor material. In general, the selection of physical acti- have contributed in particular to this field of research.
vating agent is contingent upon the intended characteristics of the Hu et al. [191] obtained activated carbons for CO2 adsorption
resultant activated carbon. Although steam activation remains the using petroleum coke as a precursor. The authors employed various
predominant technique, CO2 activation is increasingly being adopted ratios of KOH to carbon, and the most favorable CO2 adsorption
owing to its reduced energy demands. Although less frequently results were achieved when the ratio of KOH to the carbon pre-
employed, air activation has the potential to provide a broader cursor was 3. Under these conditions, the material adsorbed
spectrum of pore sizes and surface areas. 3.5 mmol/g of CO2 at a temperature of 25
C and a pressure of 1 bar.
This carbon was shown to be characterized by a significant
[Link]. Chemical activation. Chemical activation concerns the re- advantage in micropore volume with diameters less than 1 nm
action of char with chemical reagents, followed by subjecting it to compared to other pores.
heat treatment under neutral conditions. This method leads to the Ouzzine et al. [192] prepared activated carbon from pome-
production of ACs within a temperature range of 450e900
C [170]. granate peel (PP). Optimal conditions for CO2 adsorption were
The two most common chemical activation procedures are a single evaluated by controlling the activation temperature. KOH was used
step approach, known as dry mixing, and a two step approach as an activating agent in a KOH/PP activating ratio of 1:1. Four
referred to as wet impregnation [171]. The difference between the activated carbons were synthesized at activation temperatures in
two is related to the environment for carrying out the activation the range of 600e900
C, and their surface and pore characteristics
reaction and the number of sequential steps required in achieving were examined along with CO2 adsorption. The results showed that
the final product. The wet impregnation method involves the with the increase of the activation temperature from 600 to 800
C,
addition of an AC precursor to a saturated solution of an activating the total pore volume and the specific surface area increased
agent, followed by heating and drying. The dried mixture is then considerably from 0.78 to 1.28 cm3/g and from 1311 to 2141 m2/g,
activated under a nitrogen gas atmosphere in a furnace. Subse- respectively. However, the values of these two parameters
quently, the activated material undergoes a washing process prior decreased at temperatures above 900
C. The best CO2 adsorption
to a further drying step. On the other hand, the dry mixing capacity of 4.44 mmol/g and 5.53 mmol/g was obtained for acti-
approach is characterized by its simplicity, involving mixing of a vated carbon prepared at 800
C at 25 and 0
C at 1 bar, respectively.
solid activating agent with the particular raw material. Then, the This result highlights the importance of the structural and textural
mixture also is directly subjected to carbonization and activation in characteristics of activated carbons, prepared at different activation
a single step, maintaining an atmosphere of N2 gas [172]. temperatures, on the CO2 adsorption behavior.
The development of porous structure through chemical activa- Acevedo et al. [193] investigated the preparation of porous
tion is influenced by several factors, including the content of activated carbon from the chemical activation of African palm shells
organic or synthetic raw material, activation temperature, resi- sourced from crops in the Guajira region, Colombia. They utilized
dence time, heating rate, type of activating agent, and the weight solutions of Fe(NO3)3 and Cu(NO3)2 with varying concentrations
ratio between AC precursor and activating agent [173e175]. and conducted the activation process at two different temperatures
Chemical activation provides a number of benefits over physical of 700
C and 800
C. The obtained material presented micro-
activation, such as a reduction in temperature and activation time mesoporosity with surface area between 5 and 1300 m2/g. The
[176,177], higher carbon yield, more porous structure of activated fixed carbon content ranged from 47.1% to 78.4%. These results
carbon, low energy and operating cost, or easier development of indicated that the activation process had notable effects on the
microporosity [132,178]. It has also been observed that chemically textural parameters, elemental composition, and proximal
activated chars have higher carbon yields and surface areas than composition of the obtained solids. Additionally, the CO2 uptake
physically activated ones [179]. Conversely, the chemical activation values at low pressures were between from 1.82 to 5.68 mmol/g.
has several drawbacks, including an additional rinse step to remove Ello et al. [194] prepared microporous activated carbon from
excess chemical agent, and secondary contamination issues along palm shells for CO2 capture. The volume of micropores and the
with their ecological disposal [180]. specific surface area of the obtained carbons varied depending on
Commercially available ACs have a relatively low CO2 adsorption the ratio of KOH to the carbon precursor, ranging from 0.16 cm3/g
capacity due to the wide pore size distribution [181,182]. In order to (365 m2/g) to 0.82 cm3/g (1890 m2/g). Among these carbons, the
achieve high CO2 adsorption, various chemicals are utilized in the one with a specific surface area of 1250 m2/g and an ultramicropore
chemical activation to regulate the pore network, which fall into volume (diameter less than 0.7 nm) of 0.29 cm3/g proved to be the
three main classes, namely alkaline (KOH, NaOH, K2CO3, Na2CO3 most effective CO2 capture material. At 1 bar and 0
C, it exhibited
and K3PO4), which are most commonly used, acidic (H3PO4, H2SO4, CO2 adsorption capacity of 6.3 mmol/g. Interestingly, activated
HNO3) and neutral (FeCl3, ZnCl2, K2SO4, NaNH2, NH4Cl) [183,184]. carbon with a higher specific surface area (1890 m2/g) showed
Their main goal is to serve as a hydrating agent, affecting the lower CO2 uptake and a reduced ultramicropore volume.
breakdown process and preventing the formation of tar to restrict it Similar research results were presented by Zhu et al. [197], who
to a minimum [185,186]. Cao et al. [187] recommended the use of tested the carbon obtained from sawdust in the CO2 adsorption
chemical activation instead of physical activation using the steam process. They noted that the carbon material with the highest
method because it consumes less energy. Among the activators, specific surface area of 2435 m2/g was not characterized by the best
they proposed the utilization of KOH for its less harmful influence CO2 adsorption capacity. The authors concluded that the reason
on the environment than ZnCl2 or H3PO4. was the relatively low volume of the micropores, which
18
B. Dziejarski et al. Materials Today Sustainability 24 (2023) 100483

represented only 29% of the total pore volume. On the other hand, may render some sites inaccessible to adsorption, resulting in
the maximum CO2 uptake of 8.0 mmol/g at a pressure of 1 bar at a reduced CO2 uptake.
temperature of 0
C was obtained on activated carbon with a much In summary, the utilization of KOH is frequently favored over
lower specific surface, but with a high volume of micropores, alternative chemical agents owing to its capacity to generate
constituting 73% of the pore volume. Therefore, the proper micro- structures that are highly porous and possess extensive specific
pore fraction in the carbon structure was found to be the main surface areas. The heightened chemical reactivity of KOH facilitates
factor contributing to CO2 adsorption. a more efficient reaction with the precursor material at lower
Sevilla et al. [222] used eucalyptus sawdust, cellulose, and po- temperatures, ultimately resulting in the generation of a greater
tato starch as precursors to produce KOH-activated carbons. They quantity of micropores and mesopores. Furthermore, potassium
prepared several series of activated carbons that differed in the hydroxide is a cost-effective and easily accessible option, rendering
ratio of KOH to the carbon precursor and in the activation tem- it a feasible alternative for mass manufacturing.
perature. The carbon samples obtained at the activation tempera-
ture of 600
C showed the highest CO2 capture capacity at room [Link]. Modification strategies of activated carbons. By applying
temperature (4.8 mmol/g, 250
C and 1 bar). The authors associated specific strategy methods, the key disadvantages of ACs merit
the high adsorption of CO2 with the presence of narrow micropores attention, i.e., susceptibility to SOx, NOx, and H2O impurities in the
(diameter <1 nm). The specific surface area was found to play a less flue gas stream, low balance, less effective adsorption capacity at
significant role. In addition, there was an observation made that the low partial CO2 pressures, and a decrease in adsorption efficiency
obtained carbons under mild activation conditions at temperatures with increasing process temperature [131]. Therefore, to eliminate
of 600e800
C, are characterized by higher CO2 uptake. It was the influence of the above drawbacks on CO2 adsorption, many
found that using the ratio of KOH to precursor equal to 2 led to the studies described in the scientific literature focused primarily on:
formation of materials characterized by an increased number of (1) modification of the synthesis condition (thermochemical con-
pores with widths below 0.8 nm. version, or activation process), which were previously discussed;
The increase in pore diameters causes a decrease in CO2 uptake, (2) surface modifications (high temperature NH3 treatment
in line with the previously discussed concept that pores with vol- [224,225], amine functionalization [226,227]); (3) development of
umes less than 1 nm play a predominant role in CO2 adsorption activated carbon composites (carbon-based nanomaterials [228],
under ambient conditions. Presser et al. [195] found that the vol- polymers [229e231], metal oxides/metal impregnation [232,233],
ume of pores with diameters less than 0.8 nm correlated with the zeolites [234e237], metal-organic frameworks [238,239]) (Fig. 12).
amount of CO2 adsorbed at 0
C and a pressure of 1 bar. Therefore, The combinations of the above modification strategies have also
the authors stated that micropores smaller than 0.8 nm play a been reported in the literature and seems to be a very promising
dominant role in CO2 adsorption under these conditions. solution for increasing CO2 capture. They are closely related to the
Wei et al. [196] also conducted studies on activated carbons optimization of the synthesis conditions with high temperature
derived from biomass for CO2 adsorption and arrived at similar NH3 treatment [205], amine functionalization [240], or metal
conclusions. Activated carbons with a high CO2 adsorption capacity impregnation.
were produced from bamboo using KOH as the activator. The Zhang et al. [205] improved CO2 adsorption by biochar synthesis
maximum amount of CO2 adsorbed at the temperature of 0
C and modification (chemical activation of KOH) in conjunction with
the pressure of 1 bar was 7.0 mmol/g. The study aimed to identify surface modification by heat treatment of NH3 resulted in the
the pores responsible for CO2 adsorption, revealing a strong linear development of microporosity and the introduction of basic
correlation between the amount of CO2 uptake and the size of pores nitrogen-containing groups into biomass-based carbon material.
with diameters less than 0.82 nm. The authors found that pores in The high CO2 uptake of 7.19 mmol/g and 5.05 mmol/g at 0 and 25
C
the range of 0.33e0.82 nm were mainly responsible for CO2 were achieved due to the development of the micropore structure
adsorption at 0
C and 1 bar pressure. and the abundance of basic nitrogen-containing functionalities,
Based on the literature review and the findings presented in which enhanced CO2 adsorption at higher adsorption tempera-
Table 7, KOH emerges as the most frequently used reagent in tures. According to the findings, the modified activated carbon
chemical activation for CO2 adsorption compared to the others. It is contained a high surface area, measuring 2511 m2/g, as well as a
widely considered as one of the chemicals for improving CO2 significant micropore volume, reaching 1.16 cm3/g.
adsorption capacity and selectivity, enhancing the microporosity, Liu et al. [240] reported an effective synthesis of hierarchical
increasing surface area, and subduing the generation of tar. How- ultra-micro/mesoporous biocarbons by chemical activation and
ever, an excess of KOH blocks pores and reduces the surface area amine functionalization (MEA). At ambient temperature and low
[197e200]. The superior performance of KOH is evident in the CO2 partial pressure, the biocarbons displayed high adsorption
research examples carried out with the utilization of other acti- capacities (1.90 mmol/g) at 25
C and 15 kPa CO2 and record high
vating agents. For example, Shen et al. [201] used coal pitch as a Henry's law CO2/N2 selectivity up to 212. The final results estab-
precursor of activated carbons, activated with steam. The ACs lished that the unique surface textural features high mesoporosity
showed low CO2 uptake at the level of 1.9 mmol/g at a temperature and ultra-microporosity of 0.175 cm3/g with a restricted pore size
of 30
C and a pressure of 1 bar. Plaza et al. [202] produced a series distribution, large specific surface are of 1190 m2/g and increased
of ACs by the activation of olive pits with carbon dioxide. The surface chemistry. These factors combined to provide favorable
maximum CO2 adsorption capacity value that could be obtained on conditions for CO2 adsorption with strong selectivity for CO2/N2 at
these carbons was 2.4 mmol/g at a temperature of 25
C and a low partial pressures of CO2, while the presence of mesoporosity
pressure of 1 bar. The use of carbon dioxide as activating agent significantly enhanced CO2 adsorption kinetics.
resulted in ACs with lower CO2 adsorption performance compared In recent years, researchers have been more interested in pro-
to KOH-ACs. Lastly, Goel et al. [103] in their review identified the ducing AC composites, which are very effective path for increasing
ideal synthesis and process working conditions for chemical acti- CO2 uptake and selectivity. The utilization of AC composites is
vation via KOH, such as a KOH/char ratio of 2e3, an activation principally noteworthy due to their synergistic impact on the CO2
temperature of 700
C, and an optimal CO2 adsorption temperature adsorption efficiency of the constituent materials.
of below 50
C. They also emphasized that increasing the KOH/char Othman et al. [241] combined activated carbon nanofibers
ratio beyond 3 may enhance the surface area, but larger pore sizes (ACNFs) with four different types of metal oxides, including
19
 Table 7

B. Dziejarski et al.
Influence of precursors, chemical activation process conditions on textural properties and CO2 uptake of activated carbons.

Precursor Activating Activation Residence Activation approach Weight ratio BET surface Total pore CO2 selectivity CO2 uptake, mmol/g Adsorption Reference
agent temperature, time, h (precursor:agent) area, volume, at 1 bar pressure, bar

0
C 25
C
C m2/g cm3/g

Urea and tobacco stem KOH 600 1 Dry mixing 1:2 3839 2.30 e e 29.5 30 [203]
Pomegranate peels KOH 700 1 Wet impregnation 1:1 585 0.28 15.10 6.03 4.11 1 [204]
Carrot peels KOH 700 1 Wet impregnation 1:1 1379 0.58 8.10 5.64 4.18 1 [204]
Fern leaves KOH 700 1 Wet impregnation 1:1 1593 0.74 6.50 4.52 4.12 1 [204]
Black locust KOH 830 1.5 Wet impregnation 1:6 2064 0.98 e 5.86 3.75 1 [205]
Rice husk char KOH 780 1 Wet impregnation 1:3 2965 1.14 e 6.24 3.71 1 [206]
Jujun grass KOH 700 1 Dry mixing 1:2 3144 1.56 e e 4.10 1 [207]
Camellia japonica KOH 600 1 Dry mixing 1:2 1353 0.67 e e 5.00 1 [207]
Pristine gelatin KOH 700 0.17 Dry mixing 1:4 1294 0.63 e 4.25 3.30 1 [208]
Starch KOH 700 0.17 Dry mixing 1:4 714 0.40 e 3.02 2.81 1 [208]
Pristine gelatin and starch KOH 700 0.17 Dry mixing 1:4 1636 0.51 e 7.49 3.84 1 [208]
Slash pine KOH 580 2 Wet impregnation 1:4 906 0.35 e 4.93 e 1 [209]
Slash pine ZnCl2 580 2 Wet impregnation 1:1 1384 0.37 e 4.32 e 1 [209]
Longan shell KOH 800 2 Wet impregnation 1:2 3139 2.5 ~40.61 4.5 3.4 1 [210]
Paulownia sawdust KOH 700 1 Wet impregnation 1:4 1643 0.857 e 8.00 5.80 1 [197]
Bituminous coal NaOH 800 2 Wet impregnation 1:4 1511 0.75 e 8.25 e 1 [211]
Bituminous coal KOH 800 2 Wet impregnation 1:4 2599 1.16 e 9.09 e 1 [211]
Bituminous coal ZnCl2 700 2 Wet impregnation 1:4 1568 1.06 e 5.54 e 1 [211]
Argan hard shells NaOH 850 1 Wet impregnation 1:4 1827 0.96 e e 3.73 1 [212]
Argan hard shells NaOH 850 1 Dry mixing 1:4 1463 0.74 e e 3.64 1 [212]
Argan hard shells KOH 850 1 Dry mixing 1:4 1890 0.87 e e 5.63 1 [212]
Argan hard shells KOH 850 1 Wet impregnation 1:4 2251 1.04 e e 5.51 1 [212]
Vine shoots KOH 700 1 Dry mixing 1:5 1439 0.674 56.80 6.08 e 1 [164]
Vine shoots KOH 700 1 Wet impregnation 1:2 1671 0.67 8.50 5.40 e 1 [164]
20

Coffee grounds KOH 600 1 Dry mixing 1:2 876 0.40 18.00 4.40 3.00 1 [163]
Coffee grounds KOH 700 1 Dry mixing 1:4 2785 1.36 e 4.00 6.89 1 [213]
Wooden chopstick KOH 700 1.5 Wet impregnation 1:1.5 e e 17.60 e 2.63 1 [214]
Assai seeds KOH 600 2 Dry mixing 1:2 1857 0.75 e 7.13 4.38 1 [215]
Brazilian nutshell KOH 600 2 Dry mixing 1:2 1824 0.68 e 6.99 4.79 1 [215]
Andiroba seeds KOH 600 2 Dry mixing 1:2 1894 0.79 e 7.18 4.80 1 [215]
Cupuassu nutshell KOH 600 2 Dry mixing 1:2 2004 0.68 e 6.51 4.18 1 [215]
Polypodium vulgare KOH 800 1 Wet impregnation 1:1 1994 0.998 66.30 9.05 5.67 1 [216]
Common oak leader KOH 700 1 Wet impregnation 1:1 1842 0.91 74.36 6.17 5.44 1 [217]
Walnut shell KOH 800 1 Wet impregnation 1:1 1868 1.06 163.00 9.54 5.17 1 [218]
Corn stover KOH 800 2 Dry mixing 1:2 2442 1.56 15.50 7.14 e 1 [219]
Corn stover KOH 800 4 Dry mixing 1:2 1862 0.81 e 6.32 e 1 [219]
Corn stover KOH 600 2 Dry mixing 1:2 955 0.43 e 4.93 e 1 [219]
Corn stover KOH 700 2 Dry mixing 1:2 1539 0.72 e 6.80 e 1 [219]
Corn stover KOH 800 2 Dry mixing 1:1 1543 0.71 e 5.06 e 1 [219]

Materials Today Sustainability 24 (2023) 100483

Corn stover KOH 800 2 Dry mixing 1:3 2201 1.31 e 6.22 e 1 [219]
Sugarcane bagasse KOH 800 0.75 Wet impregnation 1:6.25 2080 1.316 12.00 2.00 e 1 [220]
Lignin waste KOH 700 1 Dry mixing 1:2 1551 0.77 e 7.40 4.60 1 [221]
Lignin waste KOH 800 1 Dry mixing 1:2 1924 0.95 e e 6.5 1 [221]
Lignin waste KOH 700 1 Dry mixing 1:4 2038 1.00 e e 3.2 1 [221]
Lignin waste KOH 900 1 Dry mixing 1:4 2750 1.66 e e 2.4 1 [221]
Palm date seeds KOH 900 2 Wet impregnation 1:1 1906 1.06 e e 5.44 1 [166]
Palm date seeds KOH 900 2 Wet impregnation 1:2 2335 1.54 e e 4.67 1 [166]
Palm date seeds H3PO4 900 2 Wet impregnation 1:2 1439 0.60 e e 4.40 1 [166]
Palm date seeds H3PO4 900 2 Wet impregnation 1:1 1218 0.50 e e 4.00 1 [166]
Starch, cellulose and sawdust KOH 800 1 Dry mixing 1:2 1940 0.82 5.80 3.90 1 [222]
Starch, cellulose and sawdust KOH 600 1 Dry mixing 1:2 1260 0.55 5.40 6.10 4.80 1 [222]
Starch, cellulose and sawdust KOH 600 1 Dry mixing 1:4 2370 0.91 e 5.20 2.90 1 [222]
Garlic peel KOH 800 1 Dry mixing 1:2 1206 0.70 e 4.33 2.82 1 [223]
Garlic peel KOH 600 1 Dry mixing 1:2 947 0.51 e 6.25 4.22 1 [223]
B. Dziejarski et al. Materials Today Sustainability 24 (2023) 100483

Fig. 12. The modification strategies and research directions of activated carbons.

magnesium oxide (MgO), manganese dioxide (MnO2), zinc oxide the highest BET surface area (1368 m2/g) and micropore volume
(ZnO), and calcium oxide (CaO). Among the composites tested, it (0.60 cm3/g) were observed for the AC sample. Additionally, the CO2
was discovered that ACNFs with MgO had the highest specific adsorption capacity were shown to have a correlation with the
surface area (413 m2/g) and micropore volume (0.1777 cm3/g), specific surface area, the volume of micropores (less than 2 nm),
when compared to pristine material and other composites. It also and the volume of ultra-micropores (less than 0.7 nm).
exhibited the maximum CO2 adsorption at 25
C, with a capacity of From recent reviews on ACs for CO2 capture, in 2021 Abd et al.
2.08 mmol/g. According to these findings, the integration of MgO [138] made attempts to examine the adsorption characteristics of
into ACNFs led to the greatest improvement in the physicochemical carbon dioxide on activated carbons produced from a variety of
qualities of all treatments. Metal impregnation mainly increased sources. They drew attention to the current performance, prepa-
CO2 adsorption capacity due to the high affinity between metals ration, and surface modification of ACs for future research progress
and CO2 molecules, especially at elevated temperatures. or improvement. They outlined several important directions that
Liu et al. [242] created innovative composites by combining Cu- future research should focus on, including: novel structures of AC
BTC with porous carbon materials, including ordered mesoporous materials that are resistant to harsh process environment condi-
activated carbon. All composites formed were recognized as tions (high temperatures and moisture level in flue gas stream);
microporous materials having an adsorption isotherm of type I. necessary academic cooperation for the manufacturing, character-
Additional micropores that were created during the synthesis of ization, and performance modeling of AC; more investigation on
these composites, significantly increasing their specific surface area the price of producing AC at a larger scale, since it is crucial to
and porosity. These unique porous carbon/MOF composites had a evaluate their potential applications in the commercial level;
significant application of CO2 adsorption. In particular, the analysis of the life environmental cycle impact as well as the
nitrogen-containing microporous carbon composite demonstrated financial implications of AC manufacturing; or more in-depth
the highest CO2 capacity, with 8.24 and 4.51 mmol/g under 1 research on AC stability and the regeneration requirements for
pressure at 0 and 25
C, respectively. In the case of the AC com- flue gas mixtures that may contain not only N2 or CH4, but also
posite, the CO2 uptake was equal to 8.03 and 4.49 mmol/g. Further, different impurities.
21
B. Dziejarski et al. Materials Today Sustainability 24 (2023) 100483

Table 8 summarizes the modification strategies applied to 2.11 mmol/g at 20 wt% was observed, respectively. On the other
improve textural properties and the CO2 capture capabilities of hand, higher amounts of PEI (>20 wt%) caused decreasing the ef-
activated carbons. ficiency of CO2 adsorption. Lee et al. [264] also used MWCNTs to
impregnate them with PEI. They reached the same conclusions,
3.2.3. Carbon nanotubes (CNTs) finding that attaching amino groups to the carbon surface in the
Carbon dioxide adsorption on carbon nanotubes is receiving a impregnation process leaves oxygen affinity sites, which increases
growing experimental and theoretical focus due to their structure sorption efficiency. Rahimi et al. [256] instead, used diamine pre-
similar to activated carbons, favorable surface properties, topo- cursor (1,3-diaminopropane) for the modification of multi-walled
logical hollow tube structures, high mechanical strength, very low carbon nanotubes, which improved the CO2 adsorption capacity
weight, thermal and chemical stability, and beneficial pore size of MWCNTs from 1.10 to 2.11 mmol/g.
distribution [254e256]. The cross-sectional diameter of CNTs may Additionally, Keller et al. [270] noticed the high potential use-
reach magnitudes of tens of nanometers, although their length can fulness of a composite based on CNTs and silica, due to the reduced
extend to several thousand times more. Their internal structure pressure drop, lower energy consumption, higher CO2 recovery,
focuses on the interactions between graphene layers, rolled up into and thermal and chemical stability. Silica particles were dispersed
a uniform cylinder, which is empty inside. This tubular geometry in the CNTs network, and polyethyleneimine was immobilized in
enables the gas distribution and residence time to be controlled. the hollow fibers to increase the efficiency of CO2 sorption. The
The amount of adsorbed CO2 in carbon nanotubes is determined by application of silica particles improved the specific surface area of
gas pressure, temperature, their diameter in the entire volume of the composite to 283.2 m2/g. Nevertheless, the impact of the in-
the material, and the distance between adjacent layers graphene crease in PEI loading was more pronounced, resulting in a higher
[257]. CO2 uptake of 1.92 mmol/g.
The main possibility of the systematic division of carbon nano- Another interesting direction is the development of composite
tubes can be based on the number of graphene layers present in materials is a synthesis of hierarchically porous MWCNTs/carbon
their spatial structure (walls), therefore the following are distin- foam (CF) nanocomposites based on biomass. The results obtained
guished: single walled carbon nanotubes (SWCNTs), double walled by Zhang et al. [272], which determined the influence of the
carbon nanotubes (DWCNTs), multi walled carbon nanotubes amount of MWCNTs on the mechanical properties, the pore
(MWCNTs). The three-dimensional representations of SWCNTs, structure of CF and the composite, showed a unique potential both
DWCNTs, MWCNTs, are given in Fig. 13. Each of the above forms has in terms of CO2 capture and energy storage of these materials. Due
been found to be an effective adsorbent material for specific to a more developed hierarchical porosity, in particular ultra-
gaseous media. The number of graphene layers additionally affects microporosity with a pore size from 0.50 to 0.80 nm and meso-
the properties of nanotubes, i.e., mechanical (tensile strength) and pores with an average size of about 3.70e3.90 nm. The MWCNTs
thermal parameters. Moreover, single-walled carbon nanotubes contained in the foam significantly increased the compressive
(SWCNTs) are distinguished by a large specific surface area, usually strength of CF (by 113%), and also improved the thermal stability
between 400 and 3000 m2/g, which is comparable to the activated and the degree of graphitization. The CO2 adsorption capacity of the
carbons [258]. Nonetheless, MWCNTs are considered to be a su- nanocomposite reached a high value of 4.58 and 3.19 mmol/g at
perior CO2 capture materials than SWCNTs [259,260]. 0 and 25
C, respectively.
The CNTs also offer the possibility of modifying their surface by Table 9 outlines the modification strategies used to enhance CO2
adding chemical groups [261,262]. All ways of functionalizing car- uptake and optimize the textural properties of carbon nanotubes.
bon nanotubes fall into one of two categories: internal function-
alization and external chemical functionalization (based on the 3.2.4. Fullerenes
mechanism of attaching compounds and groups). Chemical func- Fullerenes are also one of the allotropic forms of carbon that has
tionalization can be further divided into three subgroups as fol- been shown to be effective in separation and storage of a wide
lows: (1) adding functional groups to defects or ends of carbon range of gases from simple monoatomic to polyatomic, including
nanotubes for covalent functionalization, (2) “side wall function- H2, and CO2 [283e286]. They possess interesting physicochemical
alization” for covalent functionalization, and 3) non-covalent properties, considering their carbon atom bonding structure, which
functionalization, such as the use of surfactants to wrap carbon is uniform and demonstrates sp2 hybridization. The structure of
nanotubes in polymers [256]. fullerenes can additionally be illustrated as a twisted layer of a
Many studies on modification strategies to enhance CO2 graphene sheet, in which the carbon atoms form pentagonal or
adsorption capacity of CNTs, have focused on the nitrogen doping hexagonal configurations, resulting in a three-dimensional spatial
via amines on the surface of CNTs [263e266]; treatment methods architecture [287]. The most frequently considered as a potential
by chemical agents [267,268]; synthesis of hybrid materials with adsorbent is icosahedral fullerene, composed of 60 carbon atoms
MOFs (creation of hierarchical structures composed of functional- (C60), due to its exceptional chemical stability [288]. However,
ized MWCNTs and zeolitic imidazolate frameworks) [269], silica other forms of fullerenes are also being explored in the context of
[270], deposition of layered double hydroxides (LDHs) [271], and improving CO2 capture, such as B40 [289e292], B80 [293], or C24N24
carbon foams [272]; or the combination of approaches listed above. [294].
The generic CNTs modification strategies and research paths are Studies with fullerene primarily concern the utilization of DFT
presented in Fig. 14. approaches (Fig. 15). The methodology for investigating fullerenes
Based on the review, the amine functionalized CNTs are sug- via DFT entails the optimization of geometry, selection of a suitable
gested to be very suitable, non-toxic, materials for further devel- level of theory and basis set, computation of electronic structure
opment of CO2 capture processes from flue gas streams. Keller et al. and properties, and examination of vibrational modes, electron
[263] functionalized highly porous multi-walled carbon nanotube density, and charge distribution. Upon completion of the DFT cal-
based microtubes with polyethyleneimine. In the case of low PEI culations, a range of properties pertaining to the fullerene structure
fractions in the impregnating solution, the carbon material was can be computed, including but not limited to the electronic den-
characterized by a large specific surface and porosity of the sity of states, the HOMO-LUMO gap, and the vibrational spectra.
microtubes, and the sorption of CO2 increased with the increase in Recently, that method was used in few research regarding fullerene
the amount of PEI. Thus, a CO2 uptake maximum value of to investigate the potential of them to capture and store CO2
22
 Table 8

B. Dziejarski et al.
Influence of modification strategies on textural properties and CO2 uptake of activated carbons.

Activated carbon BET surface Total pore Micropore Average pore CO2 selectivity CO2 uptake, Adsorption Adsorption Reported treatment sources/ Purpose of modification Reference
area, m2/g volume, cm3/g volume, cm3/g diameter, nm at 1 bar mmol/g temperature, pressure, bar chemicals method


C

NH3-AC (biomass residue) 788 0.369 0.305 0.9 e 2.23 25 1 High temperature NH3 Increasing basicity, [224]
treatment at 400
C affinity between CO2
NH3-AC (palm shell) 889 0.474 0.442 e e 1.67 30 1 High temperature NH3 molecules-adsorbent [225]
treatment at 800
C surface and level-up N-
NH3-AC (black locust) 2511 1.35 1.16 2.15 30.75 5.05 25 1 High temperature NH3 contents [205]
treatment at 600
C
NH3-AC (cane or beet sugar) 611 0.890 e 4.7 e 1.41 35 1 High temperature NH3 [243]
treatment at 600
C
NH3-AC (biomass corncob) 1154 0.57 e e e 2.8 25 1 High temperature NH3 [244]
treatment at 800
C
MEA-AC (dried rice husk) 1190 0.777 0.422 e 115.00 1.90 25 1 Amine functionalization [240]
(Monoethanolamine)
TETA-AC (broom sorghum stalks) 1098 0.642 0.525 2.33 e 3.2 25 1 Amine functionalization [226]
(Triethylenetetramine)
Urea-AC (broom sorghum stalks) 614 0.383 0.274 2.49 e 2.33 25 1 Amine functionalization (Urea) [226]
PEI-AC (bagasse) 483.86 0.280 0.258 2.18 e 0.20 75 1 Amine functionalization [227]
(Polyethylenimine)
DEA-AC (palm shell) 652.6 0.38 e 2.34 e 5.3 70 4 Amine functionalization [245]
(Diethanolamine)
PEI-AC (biomass derived waste) e e e e e 2.0 30 1 Amine functionalization [246]
(Polyethylenimine)
AC/MgOeCaO 331 e e e e 0.15 30 1 Loading of metal oxides (MgO, Improving the surface [232]
CaO) properties and
AC/MgO 615 0.496 0.147 e e 1.11 25 1 Loading of metal oxide (MgO) promoting the [233]
23

AC/CueZn 599.41 e 0.399 e e 2.26 30 1 Loading of metals (Cu, Zn) interaction with CO2; [247]
AC/Cu 638 0.30 0.24 e e 4.93 0 1 Loading of metal (Cu) Composite formation [248]
AC/Ni 595.97 0.33 0.22 2.20 e 2.36 25 1 Loading of metal (Ni) [249]
AC nanofibers/MgO 413 0.22 e e e 2.08 25 1 Loading of metal oxides (MgO) [241]
AC/CuOeMgO 727.7 0.50 0.26 2.8 e 1.91 30 1 Loading of metal oxides (CuO, [250]
MgO)
AC/CuO 1954 1.63 1.60 1.56 e 6.78 30 1 Loading of metal oxide (CuO) [251]
AC/NiO 1945 1.63 1.59 1.79 e 6.48 30 1 Loading of metal oxide (NiO) [251]
PEI-K2CO3/AC 160.34 0.105 e 2.62 e 3.60 60 e Amine functionalization Improving the surface [252]
(Polyethylenimine); Alkali properties and
metal loading (K2CO3) promoting the
interaction with CO2;
Increasing basicity and
level-up N-contents
AC/Zeolite 13X 656 0.315 0.267 e e 5.31 30 0.05 Zeolite 13X Composite formation [234]

Materials Today Sustainability 24 (2023) 100483

AC/Na-A zeolite 182 0.047 e e e 1.14 25 1 Na-A zeolite [235]
AC/hydrotalcite 441 0.21 e 1.95 e 1.638 200 3 Hydrotalcite [253]
AC/expanded graphite 523 0.205 e e 18.10 2.89 25 1 Expanded graphite [228]
AC/HKUST-1 (MOF) 1,1456 e 0.4363 e e 3.52 25 1 HKUST-1 (MOF) [238]
AC/Cu-BTC (MOF) 1368 0.66 0.60 e 16.80 4.49 25 1 Cu-BTC (MOF) [242]
Pd-AC/MOF-74(Ni) 1115 0.78 e 0.823 14.60 12.24 25 32 MOF-74(Ni) [239]
Pd-AC/MOF-74(Co) 1088 0.75 e 0.815 12.40 11.42 25 32 MOF-74(Co) [239]
AC/polydopamine 1841 0.74 e e 25.10 4.05 25 1 Polydopamine [230]
AC/molecularly imprinted polymer 3010 1.506 1.289 2.6 22.60 3.00 25 1 Molecularly imprinted polymer [229]
AC/phenolic resin/carbon fibers 79.83 0.148 e e 12.30 3.578 25 1 Phenolic resin, carbon fibers [165]
B. Dziejarski et al. Materials Today Sustainability 24 (2023) 100483

Fig. 13. Spatial models of single-walled (a), double-walled (b), and multi-walled (c) carbon nanotubes.

molecules. One of the newest directions of research on fullerene as polarization and charge transfer processes governing the adsorp-
adsorbents is the simultaneous sorption and reduction of CO2 to tion of CO2 on the Ca-coated B40. In this way, each coated Ca atom
compounds that can be reused in industry (MOFs materials are could adsorb up to four CO2 molecules with an average adsorption
applied in a similar strategy). Qu et al. [293] sought to produce energy of 0.54 eV, which is within the range proposed for an ideal
photocatalysts for CO2 reduction with high efficiency and selec- CO2 adsorbent. Furthermore, because to the considerable difference
tivity, which is important from both an energy and environmental in adsorption energy between CO2 and H2, CH4, or N2, Ca-coated B40
standpoint. They discovered through comprehensive density has proven to be effective in separating CO2 from CH4/H2 in natural
functional theory calculations that fullerene B80 is an excellent gas or from N2 in flue gas mixture (high selectivity towards CO2).
metal-free photocatalyst for CO2 reduction to HCOOH (the activa- DFT approach was also implemented in research regarding electric
tion and reduction mechanisms have been thoroughly investi- field in CO2 adsorption, where it consisted in achieving a specific
gated). Formic acid, which is frequently used in organic synthesis, process mechanism in order to facilitate the uptake and regener-
beekeeping, and as a strong fungicidal preservative, can be reused ation of CO2 capture material. Khan et al. [295] used an electric field
in this manner. Their work provided significant insight into to study the behavior of carbon dioxide storage by phosphorus-
adsorption of CO2 and its possible reduction products on B80. doped fullerene (P-doped C60-fullerene). They demonstrated that
Further, the adsorption behavior of the calcium coated fullerene CO2 is physisorbed without the application of an electric field by
B40 by DFT method was studied by Esrafili et al. [292]. The Ca atom using the predicted adsorption energy. However, when it is
has been discovered to be able to stably adsorb CO2 molecules, with employed, it induced a change from physical to chemisorption of

Fig. 14. The modification strategies and research directions of carbon nanotubes.

24
B. Dziejarski et al. Materials Today Sustainability 24 (2023) 100483

carbon dioxide as a stronger chemical bond is formed between the compared to the pristine material. Conversely, the samples with 10
P atom and the CO2 molecule. Consequently, by eliminating the and 50 wt% of TEPA shown worse performance in terms of CO2
electric field, the adsorbent may be easily regenerated for reuse. uptake. In this particular scenario, it was observed that an optimal
Moreover, P-doped fullerene has been discovered to be an excellent quantity of TEPA loading resulted in an enhanced CO2 adsorption
adsorbent for CO2 removal from a N2/CO2 mixture. Khan et al. [294] capacity. However, excessive TEPA loading yielded a contrary
conducted the same research for P-decorated C24N24 fullerene for outcome, mostly owing to the decrease in the specific surface area
selective separation of CO2 from N2/CO2 mixture in the presence of of the adsorbent and the reduced accessibility of the amine groups.
an electric field. The estimated geometric parameters revealed that It is noteworthy that research has also been undertaken on the
under the electric field, bond lengths and angles (O¼C¼O) modification of the graphite surface using other chemical com-
(O¼C¼O) are vastly reduced, converting physisorption to chemi- pounds than amines as an alternative. Espinosa-Jime nez and
sorption by raising the electric field. This research discovered that Domínguez [309] used an anionic surfactant, sodium dodecyl sul-
P-decorated C24N24 was a selective adsorbent and can aid in the fate to promote CO2 adsorption on a graphite surface. The results
development of a controlled, and regenerable sorption for the CO2 showed that the addition of surfactants increased confinement of
separation from a gas mixture in the presence of an electric field. CO2 and the amount of gas retention on adsorbent. Other studies
also concern an investigation of sulfur doping effects and humidity
3.2.5. Graphite-based adsorbents influence on the adsorption performance of graphite. Li et al. [310]
Graphite in light of its internal structure, properties similar to demonstrated that sulfur doping significantly increased the
those of carbonaceous adsorbents, and the economic advantage of adsorption of pure CO2 (graphite split graphite pore showed a
being low cost is also considered a unique material for CO2 capture 39.85% growth in the adsorption capacity by the impregnation with
[296]. Its structure is characterized by a multilayer arrangement 33.12% sulfur at 27
C and 1 bar). Significantly, it was observed that
whereby carbon atoms exhibit sp2 hybridization and occur in the split graphite pores demonstrated a notably greater CO2 uptake
configuration of closed six-membered rings [297]. These rings are compared to sorbents without sulfur admixture, particularly in the
composed of graphene layers that form a complex spatial structure presence of water.
connected by relatively weak intermolecular interactions known as As previously mentioned, graphite oxides have been utilized in
van der Waals forces. The strength of these forces may be precisely the synthesis of composites, especially with MOFs. Policicchio et al.
represented by appropriate modeling techniques (Fig. 16). There- [307] studied CO2 adsorption on the parent MOFs and their com-
fore, the storage of gas molecules between the graphene layers is posites with graphite oxide and amine-based versions. The com-
possible by adjusting their mutual distances. However, graphite has posite of metal-organic frameworks and amine-based graphite
a weak affinity towards CO2 and a low surface area, limiting its CO2 oxide with the highest content of nitrogen, showed the best per-
adsorption capacity [298]. formance, in terms of both adsorption capacity and process
The formation of new graphite structures is one of method to reversibility. The CO2 capacity on this material reached 4.65 and
overcome these limitations, apart from graphite exfoliation (con- 7.27 mmol/g at 25 and 4
C at 0.1 MPa, which is competitive with
version to graphene oxide), chemical/physical activation, surface many best performing adsorbents addressed in the literature. In the
functionalization, or composites synthesis (Fig. 17). Several exam- case of promising strategy for designing and fabricating composites
ples of them have been reported in the literature, e.g., graphite using copper-based MOF, Zhao et al. [308] examined graphite oxide
nanofibers (Yuan et al. [299] studied the effect of KOH activation on modified with urea. The composite with the highest nitrogen
its surface), graphite nanoplatelets (Mishra et al. [300] proved that content exhibited an excellent CO2 uptake (4.23 mmol/g) at 25
C.
this particular structure has the potential as an effective CO2 cap- The results indicated that CO2 was mainly physisorbed on the
ture material under high pressure conditions, such as fumes from composites under dry conditions and the primary adsorption sites
thermal power plants, or the cement industry sector). were the open Cu centers. Then the small micropores on the
The most commonly form of graphite utilized in CO2 adsorption interface between MOF units and the modified graphene layers,
is graphite oxide, which is a product by applying the Hummer were occupied by the adsorbate molecules. The analysis of the
method [301]. This approach introduces oxygen-containing func- adsorption heats suggested that the unsaturated copper sites were
tional groups, namely epoxide and hydroxyl groups, into the crystal stronger adsorption centers than the small micropores and the
structure of graphite. To date, researchers have successfully syn- interactions between copper and CO2 were highly specific. In
thesized several types of adsorbents, including amine-based ad- addition, a prominent research direction in composite synthesis is
sorbents [302e305] and hybrid materials [306e308], by employing the application of graphite electrode waste together with cerium
graphite oxide as an initial component. Shin et al. [302] developed oxide or iron oxide as adsorbents. These materials exhibit stability
CO2 adsorbents based on graphite oxide modified with poly- and selectivity towards carbon dioxide, hence minimizing the
ethyleneimine. The study showed that the CO2 adsorption capacity negative impacts on the environment [311,312].
and CO2/N2 selectivity increased with increasing poly- Table 10 summarizes the modification strategies employed to
ethyleneimine content (enhanced acid-base interaction between improve CO2 uptake and textural properties of graphite-based ad-
CO2 gases with nitrogen functional groups) and exceeded pristine sorbents. So far, there has been no review closely related to
graphite oxide. The results obtained indicated that the maximum graphite, fullerene, the same as for carbon nanotubes. Therefore, a
CO2 uptake and selectivity were 0.75 mmol/g and 37.13, respec- critical review of the literature is recommended, which would
tively, with a polyethyleneimine content of 60% by weight. Hong contribute to the organization of current knowledge on a laboratory
et al. [305] modified the graphite oxide with 3-aminopropyl-trie- scale to facilitate the technological maturity of these carbon-based
thoxysilane, which ensured the enhancement of the affinity for CO2 materials.
and increased its adsorption capacity. The aminated material also
showed high stability during the adsorption/desorption cycles. 3.2.6. Graphene-based adsorbents
Zhang et al. [304] achieved noteworthy findings of their research Graphene is a carbon allotrope in the form of a single-layer two-
involving the modification of graphite oxide by 3, 5, 10, and 50 wt% dimensional honeycomb lattice (a 2D structure composed of car-
TEPA, where CO2 adsorption experiments were carried out over a bon atoms connected in hexagons with sp2 hybridization) [315]. In
wide range of pressures and temperatures. The graphite oxide the pursuit for a highly efficient sorption materials, graphene-
samples with 3 and 5 wt% of TEPA exhibited superior CO2 uptake based adsorbents have been discovered to offer amazing
25
 Table 9

B. Dziejarski et al.
Influence of modification strategies on textural properties and CO2 uptake of carbon nanotubes.

Carbon nanotube- BET surface Total pore Micropore Average pore CO2 selectivity CO2 uptake, Adsorption Adsorption Reported treatment sources/chemicals Purpose of modification Reference
based adsorbent area, m2/g volume, volume, diameter, nm at 1 bar mmol/g temperature,
C pressure, method
cm3/g cm3/g bar

TEPA-CNT 2.20 0.03 e e e 5.00 60 e Amine functionalization Increasing basicity, affinity [267]
(Tetraethylenepentamine); between CO2 molecules-
Chemical activation (KOH) adsorbent surface and level-up
K2CO3-APF-CNT 1005 0.61 0.45 0.92 8.80 4.50 0 1 Amine functionalization (3- N-contents; Increasing surface [273]
aminophenol/formaldehyde resin); area and porosities
Chemical activation (K2CO3)
TEPA-CNT 8.94 0.0565 e 19.04 e 3.56 40 e Amine functionalization Increasing basicity, affinity [254]
(Tetraethylenepentamine) between CO2 molecules-
PEI-MWCNT 34.7 23.4 e e 196.00 2.11 25 1 Amine functionalization adsorbent surface and level-up [263]
(Polyethylenimine) N-contents
PEI-MWCNT 174 1.646 0.015 e e 2.14 25 0.15 HNO3/H2SO4 pre-treatment; Carboxylation, oxidation of [264]
Amine functionalization MCNT; Increasing basicity,
(Polyethylenimine) affinity between CO2
molecules-adsorbent surface
and level-up N-contents
BPEI-CNT 14.1 0.10 e e e 2.43 70 e Amine functionalization Increasing basicity, affinity [274]
(Polyethylenimine) between CO2 molecules-
adsorbent surface and level-up
N-contents
PEI-purine-CNT e e e e e 3.875 50 1 Amine functionalization Increasing specific area of CNTs, [266]
(Polyethylenimine); Purine basicity, affinity towards CO2
and level-up N-contents
APS-CNT 198 0.63 e 12.2 e 2.19 25 1 Amine functionalization (3- Increasing basicity, affinity [275]
aminopropyltriethoxysilane) between CO2 molecules-
adsorbent surface and level-up
26

N-contents
PAA-MWCNT 60.44 0.40 e 13.76 e 1.59 25 1 Amine functionalization Building bonding between [276]
(Polyaspartamide) amino-containing compound
and substrate material to
enhance the surface area and
pore volume
HNO3/H2SO4-DAP- 112.8 0.65 e 11.6 e 2.11 30 17.3 HNO3/H2SO4 pre-treatment; Amine Carboxylation, oxidation of [256]
MCNT functionalization (1,3-diaminopropane) MCNT; Increasing basicity,
HNO3/H2SO4-PDA- 90.7 0.53 e 23.80 e 0.54 25 2 HNO3/H2SO4 pre-treatment; Diamine affinity between CO2 [277]
MCNT functionalization (phenylenediamine) molecules-adsorbent surface
and level-up N-contents
HNO3/H2SO4-MCNT 100.93 0.05 1.59 2.73 ~12.00 0.32 25 1 HNO3/H2SO4 pre-treatment Carboxylation, oxidation of [268]
MCNT
PEI-CNT/Silica 283.2 e e e 217.00 1.92 25 0.15 Amine functionalization Composite formation [270]
(Polyethylenimine); Silica

Materials Today Sustainability 24 (2023) 100483

PAN-CNT/Carbon 390 0.40 0.33 e 78.00 6.3 25 1 Amine functionalization [278]
nanofibers (CNF) (Polyacrylonitrile as amine source);
Carbon nanofibers
CNT/N-doped AHPC 561 e e e 18.04 3.91 25 1 N-doped acicular hollow porous carbon [279]
MWCNT/Carbon foam 805.91 0.35 0.31 e 8.44 3.19 25 1 Carbon foam [272]
N-doped CNT/PAN-ACF 709 0.3577 0.2312 2.019 e 1.75 25 1 Amine functionalization; Polyamide- Increasing basicity, affinity [280]
based activated carbon fibers between CO2 molecules-
adsorbent surface and level-up
N-contents;
Composite formation
PEI-MWCNT/Cd- 365 0.39 e 2.65 e 5.70 25 20 Amine functionalization Composite formation [281]
nanozeolite (Polyethylenimine); Nanozeolite
modified with Cd2þ
MWCNT/MIL-101 e e e e e 0.003 25 1 MIL-101 (MOF) [282]
(MOF)
B. Dziejarski et al. Materials Today Sustainability 24 (2023) 100483

However, because of the highly strong intermolecular interac-

tion and the limited number of functional groups, pristine gra-
phene has poor dispersibility and compatibility [321]. In this sense,
graphene oxide (GO), an alternative form of graphene, exhibits
remarkable characteristics attributed to the abundance of hydro-
philic oxygenated functional groups. These groups offer numerous
active sites for the joining of additional functional groups or mol-
ecules, thereby enabling functionalization through both covalent
and non-covalent bonding mechanisms [322,323]. In addition to
that, the adaptability of surface modification allows the use of
graphene-based materials for CO2 capture [324]. Another form of
graphene used in CO2 adsorption application, inter alia, for the
synthesis of composites, is reduced graphene oxide (rGO). rGO is
produced by the chemical or thermal reduction of graphene oxide.
It is considered to possess a structure that is between that of a
graphene sheet and highly oxidized graphene oxide [325]. The
three structures of graphene are schematically shown in Fig. 18.
Currently, research on graphene as a CO2 capture material
concerns similar modifications as in the case of graphite, such as
synthesis of hybrid materials/composites (MOFs [326e328],
carbon-based materials [329], polymers [330,331], incorporation of
metal oxides [332,333], clays [334]), creating new material struc-
tures based on graphene (aerogels [335], cryogels [336,337]), and
treatment methods related to the improvement of the surface
morphology (oxidation [338], physical and chemical activation
[339e341]) (Fig. 19). Xia et al. [339] tuned the pore structure and
surface chemistry of porous graphene materials (PGMs) for CO2
capture, which was achieved by activating CO2 and KOH in ther-
Fig. 15. The modification strategies and research directions of fullerenes. mally exfoliated graphite oxide. CO2-activated PGMs (CPGM) had a
three-dimensional morphology with a hierarchical pore structure,
while KOH-activated PGMs (KPGM) had a two-dimensional
attributes, including large specific surface area, high proclivity for morphology with large number of micropores and small meso-
gas adsorption, extraordinary electrical conductivity, good me- pores. Specifically, CPGM exhibited a substantial presence of
chanical stability, and easy surface modification [316e318]. quinone and carbonyl functional groups, while KPGM demon-
Furthermore, it is well acknowledged as a powerful adsorbent, strated a significant concentration of hydroxyl groups. These dis-
particularly in terms of its ability to demonstrate a high adsorption tinctions in surface chemistry were confirmed through pore
capacity for carbon dioxide, surpassing that of methane and ni- structure analysis and gas adsorption experiments. Additionally,
trogen [319]. The intimate relationship between graphene and its the CO2 adsorption by PGM was influenced by both the pore
dense single-atom structure contributes to its ability to serve as a structure and the surface chemistry. At 0
C and 1 bar, the highest
high-speed transport channel with exceptional gas selectivity adsorption value reached 4.06 mmol/g.
[320]. Another popular modification of graphene-based adsorbents is
attaching organic functional groups to the graphene surface. Ni-
trogen doping [342e344] has been found to be a promising strat-
egy to improve CO2 adsorption capability. The developed materials
were characterized by excellent stability and recyclability, high
selectivity of CO2 in relation to N2, suitable heat of adsorption, high
dynamic adsorption, as well as fast CO2 adsorption kinetics. As a
result of their exceptional characteristic, GO has been fully exploi-
ted as a suitable framework for the fabrication of an amine-
functionalized adsorbents for selective CO2 capture. Moreover,
there are many advantages associated with this specific research
path, which are as follows: (1) reduced energy consumption during
regeneration, (2) no corrosion susceptibility of instruments, (3) low
creation of harmful byproducts due to amine groups incorporated
in the solid matrix. Hosseini et al. [342] modified the surfaces of
graphene oxide with 3 different amines, including triethylenetetr-
amine (TETA), pentaethylenehexamine (PEHA) and meta-phenyl-
enediamine (MPD). At 298 K and 1 bar, CO2 adsorption improved
dramatically from 0.39 mmol/g for graphene oxide (GO) to 0.61,
0.74, and 0.91 mmol/g for GO-PEHA, GO-TETA, and GO-MPD sam-
ples, respectively. Furthermore, based on the ideal adsorbed solu-
tion theory (IAST), the predicted CO2/N2 selectivity of the
investigated solid sorbents revealed an outstanding value, partic-
ularly for the GO/MPD, reaching around 21.21 under ambient
Fig. 16. Schematic structure of graphite. conditions. An et al. [345] examined graphene-derived N-enriched
27
B. Dziejarski et al. Materials Today Sustainability 24 (2023) 100483

Fig. 17. The modification strategies and research directions of graphite-based adsorbents.

carbonaceous materials as well, although with an alternative and functionalizing carbon-based adsorbents, with the aim of
nitriding agent, namely urea. The experimental setup included the fostering a beneficial influence on the circular economy. Additional
usage of GO as the precursor and KOH as the activator. Subse- barriers that should be taken into consideration refer to the de-
quently, the samples were exposed to a thermal shock treatment, mand for more extensive research and an in-depth analysis of the
which aimed to enhance the structural features of the adsorbent. CO2 adsorption mechanism. Furthermore, it is crucial to place
The results demonstrated that thermal expansion of the GO pre- greater emphasis on conducting CO2 sorption tests in both wet and
cursor improved the porosity and nitrogen enrichment of the dry environments to enhance the diffusion of CO2 molecules into
porous carbons. At atmospheric pressure, the produced adsorbents the porous structure of the material. Additionally, there is a ne-
demonstrated good CO2 adsorption, with 2.40 and 3.24 mmol/g at cessity for further advancement in hybrid materials incorporating
25 and 0
C, respectively. Furthermore, investigations have shown graphene-based adsorbents to enhance CO2 uptake, while also
that under ambient conditions, both narrow microporosity and N- considering other criteria for the selection and optimization of CO2
doping are favorable for CO2 capture. capture materials.
In summary, this type of CO2 capture materials must exhibit a The previously published review in 2015 by Balasubramanian
range of desired properties in order to be considered economically and Chowdhury [347] also presented an in-depth evaluation of the
viable and ecologically sustainable for sorption applications. These emerging field of graphene-based adsorbents, highlighting notable
include a substantial surface area and pore volume, the presence of areas for future research. Its primary objective was to compile the
a porous structure (specifically microporosity), and the effective latest advancements in this rapidly evolving field. In particular, the
modification of surface chemistry through the incorporation of authors highlighted the importance of defining the work path
functional groups or heteroatoms. Lately, Ruhaimi et al. [346] sys- development on a laboratory scale and their practical transfer to a
tematically provided a comprehensive overview of the most recent commercial application. Due to this, there is an unavoidable need
scientific research concerning the utilization of graphene-based for an expansive research endeavor that is both multidisciplinary
adsorbents in CO2 adsorption technologies, as well as a discussion and interconnected. Further future perspectives and recommen-
of that investigation. The authors highlighted several significant dations have been proposed in relation to the measurement of CO2
challenges that must be addressed in order to fully harness the uptake on a volumetric basis, assessment of working capacity,
promise of graphene-based adsorbents in the present moment. determination of multicomponent gas adsorption isotherms,
First, most of the current fabrication techniques, apparatus, investigation of the impact of water vapor, in situ characterization
and supplies are both expensive and time consuming, which limits of adsorbed CO2, and the development of molecular models along
their usefulness in the industrial sector. The significance of with force fields that accurately simulate realistic conditions.
manufacturing costs in the context of large CO2 capture systems The CO2 capture performance and textural properties of
cannot be overstated. Consequently, it is imperative to explore graphene-based adsorbents associated with specific modification
alternative recyclable waste residues for the purpose of processing strategies are compared in Table 11.

28
 Table 10

B. Dziejarski et al.
Influence of modification method on textural properties and CO2 uptake graphite-based adsorbents.

Graphite-based adsorbent BET surface Total pore Micropore CO2 selectivity CO2 uptake, Adsorption Adsorption Reported treatment sources/chemicals Purpose of modification Reference
area, m2/g volume, cm3/g volume, cm3/g at 1 bar mmol/g temperature, pressure, bar method


C

PEI-graphite oxide 16 0.051 0.004 37.13 0.75 25 1 Amine functionalization Increasing basicity, [302]
(Polyethyleneimine) affinity between CO2
APTS-graphite oxide 19 e e e 1.16 30 1 Amine functionalization (3- molecules-adsorbent [305]
Aminopropyl-Triethoxysilane) surface and level-up N-
EDA-graphite oxide 2.73 e e e 1.22 30 e Amine functionalization contents [303]
(Ethylenediamine)
TEPA-graphite oxide 42.68 e e e 2.08 25 30 Amine functionalization [304]
(Tetraethylenepentamine)
Graphite nanoplatelets (GNP) e e e e 4.9 25 12 Acid intercalation (HNO3/H2SO4 pre- Graphite oxidation; [300]
treatment); Thermal exfoliation; HNO3 Introducing hydrophilic
post-treatment functional groups
(eCOOH, eC¼O, and
eOH)
Graphite nanoplatelets (GNP)/ 102.35 0.1509 e e 8.5 25 11.5 Acid intercalation (HNO3/H2SO4 pre- Graphite oxidation; [312]
Fe3O4 treatment); Thermal exfoliation; HNO3 Introducing hydrophilic
post-treatment; Loading of metal oxide functional groups
(Fe3O4) (eCOOH, eC¼O, and
eOH); Composite
formation
Graphite waste/Fe3O4 18.48 0.07 e e 5.36 30 8 Loading of metal oxide (Fe3O4) Composite formation [312]
Graphite waste/CeO2 20.03 e e e 3.58 30 20 Loading of metal oxide (CeO2) [311]
S-doped graphite oxide/Porous 831 0.589 0.38 e 5.00 0 1.2 Porous carbon; Sulfur doping Composite formation; [313]
carbon Enhancing the
interaction strength
29

between CO2 and

composite surface.
Graphite oxide/Cu3(BTC)2 837 0.19 e e 3.30 25 1 Cu3(BTC)2 (MOF); Presence of humidity Composite formation [306]
(MOF)
Aminated graphite oxide/Cu- 1367 0.663 0.572 24.77 4.65 25 1 Amine functionalization by urea Increasing basicity, [307]
BTC (MOF) treatment; Cu-BTC (MOF) affinity between CO2
molecules-adsorbent
surface and level-up N-
contents; Composite
formation
KOH-activated graphite 919 1.057 0.226 e 1.61 25 1 Chemical activation with KOH Improving the [299]
nanofibers development of
KOH-activated graphite 567 0.708 0.274 e 1.35 25 1 Chemical activation with KOH microporous structures [314]
nanofibers and increasing surface
area

Materials Today Sustainability 24 (2023) 100483

B. Dziejarski et al. Materials Today Sustainability 24 (2023) 100483

Fig. 18. Schematic representation of structures of graphene sheet (a), graphene oxide (GO) (b), and reduced graphene oxide (rGO) (c).

Fig. 19. The modification strategies and research directions of graphene-based adsorbents.

30
 Table 11

B. Dziejarski et al.
Influence of modification method on textural properties and CO2 uptake of graphene-based adsorbents.

Graphene-based BET surface Total pore Micropore Average pore CO2 selectivity CO2 uptake, Adsorption Adsorption Reported treatment sources/chemicals Purpose of modification Reference
adsorbents area, m2/g volume, cm3/g volume, cm3/g diameter, nm at 1 bar mmol/g temperature, pressure, bar method


C

MPD-graphene oxide 44.33 0.046 0.031 4.23 21.21 0.91 25 1 Amine functionalization (Meta- Increasing basicity, [342]
phenylenediamine) affinity between CO2
TETA-graphene oxide 14.40 0.016 0.011 4.65 16.37 0.74 25 1 Amine functionalization molecules-adsorbent [342]
(Triethylenetetramine) surface and level-up
PEHA-graphene oxide 9.39 0.012 0.008 5.27 9.54 0.61 25 1 Amine functionalization N-contents [342]
(Pentaethylenehexamine)
PEI-graphene oxide e 1.822 e e e 2.91 75 1 Amine functionalization [343]
(Polyethylenimine)
EDA-graphene oxide 21.37 e e e e 2.0 25 1 Amine functionalization [336]
cryogels (Ethylenediamine)
EDA-graphene oxide 167.66 e e e e 1.18 25 1 Peroxidation step; Improving adsorption [337]
cryogels Amine functionalization property; Increasing
(Ethylenediamine) basicity, affinity
between CO2
molecules-adsorbent
surface and level-up
N-contents
Chitosan- graphene 33.32 0.129 e e e 0.257 25 1 Chitosan grafting Providing the large [348]
oxide cryogels surface area, high
porosity, and a large
number of amine group
Urea-KOH-graphene 1032 0.82 e e 12.00 2.40 25 1 Thermal shocking; Urea modification (a Improving porosity and [345]
oxide source of amines); KOH activation nitrogen enrichment of
the ultimately
31

synthesized porous
carbon
CO2-activated porous 2518 1.65 1.32 e e 4.06 0 1 KOH activation Improving the [339]
graphene development of
NaOH-activated porous 843 2.71 0.12 e e 1.74 0 1 CO2 activation microporous structures [339]
graphene and increasing surface
3D crumpled graphene- 1.316 1.07 0.21 e 162.00 2.45 25 1 CO2 activation of reduced graphene area [340]
based porous oxide
adsorbent
Monolithic reduced 1622 7.15 e e e 6.31 25 10 Steam activation of reduced graphene [335]
graphene oxide- oxide
based aerogels
Triply oxidized e e e e e 3.54 30 9 Multiple oxidations Tuning the composition [338]
graphene oxide of GO functionalities
(increasing the amount

Materials Today Sustainability 24 (2023) 100483

of oxygen containing
groups)
Graphene oxide/MOF- 3359 e e e 18.37 1.34 25 1 MOF-200 Composite formation [326]
200
Graphene oxide/Cu- 1820 0.88 0.88 e 21.00 9.05 0 1 Cu-BTC (MOF) [327]
BTC
Graphene oxide/Cu- 1772 0.718 0.593 e 43.80 8.90 0 1 Cu-BTC (MOF) [328]
BTC
Graphene oxide/Cu- 1015 0.4996 e e e 2.50 32 5 Cu-BTC (MOF) [349]
BTC
UV-irradiated graphene 1324 0.777 0.676 2.304 14.35 5.14 25 1 UV-irradiation of GO; Enhancing critical [350]
oxide/Cu3(BTC)2 Cu3(BTC)2 (MOF) parameters of GO
adsorbents associated
(continued on next page)
 B. Dziejarski et al. Materials Today Sustainability 24 (2023) 100483

3.3. Metal-organic frameworks (MOFs)

Purpose of modification Reference

[350]

[351]
[330]

[331]

[332]
[333]

[334]
Organic-inorganic hybrid porous materials, such as metal-
organic frameworks, are solid CO2 adsorbents with benefits
including excellent thermodynamic stability, customizable chemi-
Composite formation
Composite formation

cal functionality, extra high porosity, easily programmable pore

characteristics, high purity, well-defined crystallographic geo-
to CO2 capture;

metric properties, and large-scale production capability, among

other materials [352e354]. Generally, MOFs are composed of
method

metal-containing nodes that are connected together by organic

linking groups (organic ligand bridges) principally through strong
covalent bonds (coordination bonds) that form a one-, two- or
Reported treatment sources/chemicals

three-dimensional coordination network [355e357]. MOFs can be

Incorporation of metal oxide (TiO2)

Polyphosphoric acid modified clay

classified into different groups based on their structural properties,

such as rigid MOFs, dynamic/flexible MOFs, surface functionalized
Polymer monolithic material

Incorporation of metal oxide

MOFs, open metal sites MOFs, Lewis basic sites MOFs, both open
metal and Lewis basic sites MOFs, microporous MOFs, post-
nanoparticles (MgO)

synthetically modified MOFs, and MOF composites [356]. Addi-

Cu3(BTC)2 (MOF)

tionally, a combination of the above groups can be distinguished,

UiO-66 (MOF)

i.e., MOFs with micropores and a functionalized surface, or micro-

Polyaniline

pores and open metal sites. The generic classification is shown in

(PMMT)

Fig. 20.
To date, a significant number of publications have been dedi-
temperature, pressure, bar

cated to the improvement of CO2 capture by MOFs. Modifying the

Adsorption

type and quantity of organic linkers or changing the connectivity of

metal ions (both of the two fundamental building components)
1.18
60

may be used to continuously improve a CO2 adsorption perfor-

1

1
1

mance and quality of MOFs structures [358,359]. As a result, various

Average pore CO2 selectivity CO2 uptake, Adsorption

modifications of MOFs synthesis and their influence on the effi-

ciency of carbon dioxide uptake were investigated, including the
selection of organic linker [360], activating and removing the sol-
25

25
25

30

25
60

25


C

vent molecule [361], and altering the open metal sites and Lewis
basic sites [362,363]. Therefore, those materials possess a high
mmol/g

degree of simplicity in terms of their production and adaptability

2.53

3.37
3.85

1.31

1.88
3.34

0.49

for CO2 capture application. The schematic illustration of CO2

storage mechanism in MOFs structure is given in Fig. 21 By
comparing metal-organic frameworks with other porous materials
diameter, nm at 1 bar

like zeolites and activated carbons, it becomes transparent that

~19.00
12.00

22.00

MOFs exhibit the ability to readily optimize their porosity, surface

e

characteristics, and other properties. This versatility renders them

highly suitable for a diverse range of specific and precise applica-
tions as solid material for CO2 adsorption [364]. Nevertheless, the
30.856
2.336

main challenge in achieving a high degree of crystallinity in the

13.6

6.7

synthesis of MOFs lies in the optimization of multiple reaction

e

parameters. These parameters include the concentration of re-

area, m2/g volume, cm3/g volume, cm3/g

actants, the ratio of metal to ligand, the concentration of co-

Micropore

solvents, the pH of the solution, as well as the temperature and

<0.01
0.524

0.304
0.036

time of the reaction [356,365].

e

The amount of CO2 captured by porous MOF materials is

dependent on a number of parameters, including adsorption ca-
pacity, surface morphology, selectivity, and the amount of energy
BET surface Total pore

used during adsorption. Generally, the robust ability of MOFs to

0.0788
0.632

0.384
0.197

0.382
0.10

capture CO2 can be attributed to their unique chemical and

e

physical properties of frameworks, which are appropriately

changed and adjusted to increase the interaction forces between
the material surface and the CO2 molecules [357]. These dis-
99.54

50.77
1097

1184
110

<5

tinguishing characteristics primarily include pore size, porosity,

12

specific surface area, unsaturated or open metal sites, and inte-

Graphene oxide/UiO-66

Graphene oxide/MgO
Graphene oxide/TiO2
Polyaniline (PANI)

gration of polar functional groups into the pore channels (eNH2,

Table 11 (continued )

Reduced graphene

Reduced graphene

eOH, eNO2, and eCOOH) [366,367]. In order to modify these

oxide/Polymer
Graphene oxide/

Graphene oxide/
Graphene-based

nanoparticles

oxide/PMMT

parameters, extensive research has been performed in recent

Cu3(BTC)2
adsorbents

decades. As an instance, Furukawa et al. [366] developed ultrahigh

porosity in MOFs by synthesizing crystalline solids with extended
non-interpenetrating three-dimensional crystal structures sup-
ported well-defined pores. Series of MOFs showed exceptional
32
B. Dziejarski et al. Materials Today Sustainability 24 (2023) 100483

linkers may be selectively added to MOFs, the pores within these

materials can be tuned more precisely than standard porous zeo-
lites. Wu et al. [372] presented flexible MMOFs as remarkable
adsorbent with high CO2 selectivity of over other gaseous mole-
cules at relative low pressure and high temperature, which are
comparable to those present in flue gas mixtures.
However, developing MMOFs with exceptionally high CO2 cap-
ture capacity and gas selectivity while still simultaneously
requiring low regeneration energy, remains a formidable obstacle
to overcome. Recently, Wen et al. [373] designed and synthesized a
MMOF with suitable pore size and dual functionalities. That ma-
terial displayed excellent CO2 capture capacity (3.56 mmol/g at
0.15 bar and 23
C) as well as strong CO2/N2 selectivity (600), both
of these values were considerably higher than those observed in
most other MMOFs previously reported. The research findings
further indicated that the outstanding CO2 uptake at low pressure
and mild heat of CO2 adsorption may be related to the appropriate
pore size and dual functionalities, which not only interact with CO2
molecules but also enable them to dense pack inside the
framework. Other studies on MMOFs concern pore environment
modifications to enhance CO2 adsorption. Fan et al. [374] alter
multifunctional ligands with eF, eCl, eNH2, eCH3, eOCH3, and
organic secondary building units with bipy-N ligands (dimethyl-
Fig. 20. Classification of metal-organic frameworks for CO2 capture. amine, pyridine, 4-aminopyridine, and isonicotinic acid) based on

Fig. 21. Adsorption process of CO2 molecules within the structure of MOFs.

porosities and CO2 uptake with the maximum BET surface area microporous Ni-MOFs. Fluorine modified MOFs showed the highest
reaching of almost 6240 m2/g. Further, Farha et al. [367] focused CO2 uptake of 3.81 mmol/g at 0
C and 1 atm. The conclusive
on combining MOFs featuring ultrahigh surface via de novo findings indicated successful synthesis of innovative porous ma-
approach entailing computational design and simulations before terials that offer significant efficacy as CO2 adsorbent, hence
experimentation. The obtained adsorbent had a high BET surface contributing to the development of a systematic approach for
(6143 m2/g) with high CO2 storage capacity. enhancing gas adsorption and separation abilities.
Currently, R&D projects on MOFs mainly focus on investigating Several research have been conducted to investigate the rational
the impact of process conditions and flue gas composition on CO2 modification of open metal sites and Lewis nitrogen sites, aiming to
adsorption. This research mainly concentrates on the influence of enhance the CO2 sorption performance. These studies provide vital
moisture, as well as pollutants. Other areas of interest include insights for the design and synthesis of novel materials in the field
altering and fixing pore shape and size, modifying metal sites and of MOFs. Song et al. [375] conceived and produced three diisoph-
Lewis basic bases, doping with metal ions, creating novel struc- thalate organic ligands containing nitrogen and utilized them to
tures, optimizing regeneration and recycling procedures, exploring synthesize three isostructural NbO-type MOFs with varying
various methods of functionalizing the pore surfaces of MOFs, and numbers and orientations of nitrogen sites. The results of the
synthesizing MOF composites (Fig. 22) [296,355,356]. The main investigation established that the CO2 adsorption characteristics of
objective of the above modifications is to further enhance the CO2 MOFs are influenced not only by the amount of Lewis basic nitrogen
uptake, selectivity towards CO2, and stability of the framework it- sites but also by their accessibility. Additionally, the introduction of
self, according to the researchers [368]. Therefore, the majority of functional groups does not have a restricted impact on improving
studies concern the evaluation of CO2 adsorption capacity by CO2 uptake.
determining the adsorption equilibrium [369]. Accordingly, ligand functionalization or post-synthetic modifi-
A large number of microporous metaleorganic frameworks cation has been explored by many researchers. Xu et al. [376]
(MMOFs) have been developed as CO2 capture materials. Chen et al. developed two N-oxide functionalized linear diisophthalate ligands
[370,371] emphasized that the tuning of micropores inside MOFs is and used them to create their corresponding NbO-type MOFs under
critical for their application in the separation of small molecules. acceptable solvothermal conditions. Their CO2 adsorption capac-
Since metal-containing secondary building units and organic ities and selectivity towards CO2 shown considerable levels of

33
B. Dziejarski et al. Materials Today Sustainability 24 (2023) 100483

Fig. 22. The modification strategies and research directions of metal-organic frameworks.

effectiveness for NbO-type MOF counterparts. Furthermore, Recently, the ordered mesoporous silica has also been selected
structureeproperty relationship investigations demonstrated that for use in the fabrication of MOF-based composite materials, ac-
the N-oxide functionality is highly critical for increasing CO2 cording to the researchers [380e383]. The introduction of ordered
adsorption efficiency. mesoporous structure, in addition to providing functional attri-
As previously stated, metal-organic frameworks are typically butes that are comparable to those of carbon-based materials, also
utilized together with other materials to form composite struc- offers the reduction of mass transfer resistance of guest molecules
tures. Typically, the production of these MOF-based composites and boosts the diffusion efficiency [379]. Chen et al. [380]
requires the dissolution of the raw components or as-processed attempted to create hybrid composites based on mesoporous silica
materials in the precursor solutions of MOFs prior to initiating and MOFs that exhibited both high CO2 adsorption capacity and
the reactions. As a consequence of the synergistic effects, the rapid adsorption kinetics. The composite was constituted of MIL-
resulting multi-component composites not only exhibit the 101(Cr) and mesoporous silica through an in-situ hydrothermal
inherent strength of the original materials, but also possess unique method. The synthesis led to reduced particle size, enhanced
physicochemical characteristics and functional properties. In recent micropore volume, and increased specific surface area of the
years, carbon-based materials have been extensively used to composite, resulting in a considerable improvement in its CO2
fabricate such composites. The addition of these components has uptake (2.09 mmol/g at 0
C and 1 bar), about 79% higher than that
the potential to regulate particle sizes and drive the formation of of parent MOF. Further, the application of MCM-41 contributed to a
MOF crystals in a certain direction, hence leading to improved decrease in the mass transfer resistance and facilitated the CO2
adsorption capacity [377]. Kayal and Chakraborty [378] designed diffusion. Consequently, there was an apparent reduction in
and developed carbon-based MOF composite, which was synthe- the time required to achieve adsorption equilibrium and an in-
sized by in situ incorporation of activated carbon powder (type crease in the adsorption rate. Moreover, the synergistic impact of
Maxsorb-III) in MOF (MIL-101(Cr)). In comparison to the parent mesoporous silica and MOFs strengthened the interactions be-
MOF, it was seen that the composite exhibited greater CO2 tween CO2 molecules and the composite, as indicated by the isos-
adsorption capacity. Specifically, the composite demonstrated a 10% teric heats of CO2 adsorption and desorption activation energy.
and 15% increase in CO2 uptake on a volumetric and gravimetric Further, the chemical composition of the flue gases, which are
basis, respectively. Qian et al. [379] aimed to improve the structural separated for the purpose of carbon dioxide capture, is a crucial
features of hierarchical porous carbon monolith (HCM) by incor- factor to consider in relation to MOFs. Especially, the presence of
porating the advantages of metaleorganic frameworks (Cu3(BTC)2) moisture can substantially impact on the CO2 adsorption capacity of
to optimize the CO2 capture on a volumetric basis. The obtained MOFs. Llewellyn et al. [384] highlighted the difference in the
composite was characterized by a significant CO2 adsorption ca- adsorption behavior between the polar and nonpolar nature of the
pacity value, notable CO2-over-N2 selectivity and a good regener- molecules that are being adsorbed on MOFs. In general, different
ation capability. molecules with various degrees of polarity need to be investigated

34
B. Dziejarski et al. Materials Today Sustainability 24 (2023) 100483

to productively recover CO2 in mixed-gas streams, particularly which stand as crystalline materials featuring ordered structures
those with a substantial water content. Yu and Balbuena [385] formed under thermodynamic control, all other POPs show an
evaluated water effects on post-combustion CO2 capture in MOFs amorphous nature [417,418].
by using a combination of grand canonical Monte Carlo (GCMC) and Until recently, considerable endeavors have been dedicated to
DFT simulations. Their findings indicated that the presence of water formulating and creating high-performance POPs adsorbents,
molecules linked to coordinatively unsaturated metal sites (CUMs) yielding promising outcomes. According to the latest reviews
reduces the CO2 adsorption capacity of MOFs. This resulted from a published between 2017 and 2022 by Mohamed et al. [416], Gao
decrease in the binding energy between CO2 and the water- et al. [421], Bhanja et al. [422], and Wang et al. [423], the key
coordinated MOFs. Simultaneously, it was revealed that the CUMs research fields for improving the CO2 capture properties of POPs
in MOFs are critical for their CO2 uptake in realistic streams that can be characterized as follows: (1) increasing the CO2 adsorption
incorporate water and other contaminants. Nevertheless, these capacity of materials, (2) enhancing CO2/N2 selectivity, and (3)
data are especially noteworthy in light of the recovery of carbon considerations the real application conditions. The all authors
dioxide in multicomponent gas mixtures. highlighted that mainly, due to the micropore filling process, large
In summary, MOFs are potentially extremely interesting inno- specific surface areas [424,425] and appropriate micropore sizes
vation for large-scale commercialization of CO2 adsorbent mate- [426,427] are considered as influential factors with regard to CO2
rials. Unfortunately, there are several drawbacks associated with uptake and selectivity. Alternatively, the metal sites [428,429] and
MOFs that need to be addressed in order to facilitate their scal- the morphology of POPs have been reported to be important de-
ability and enhance technological maturity. Aniruddha et al. [386] terminants that impact CO2 storage process. Therefore, some as-
in their review on utilization of MOFs in CO2 capture, highlighted pects of the above properties should be investigated further. The
several important aspects, including difficulty in large-scale syn- creation of 3D POPs with a large surface is one of them [426]. This
thesis (majority of synthesis techniques are suitable for small-scale strategy could allow modification of POPs to occur while still
and laboratory experiments), lack of thermal stability (enhancing it retaining a part of the BET surface area. Secondly, it's advisable to
through manipulation of MOFs morphology is crucial), excessive employ post-synthesis conditions that are milder and more effi-
attraction of moisture (total disintegration of the crystalline cient. This approach can incorporate the functional moiety while
structure), further study to increase the desorption temperature preserving the porous structure of POPs. Furthermore, enhancing
and the spontaneity of the CO2 adsorption, or development of pa- the affinity between CO2 and the material surface can be achieved
rameters for screening MOFs. The other barriers are related to high through the introduction of heteroatoms (N, O, S, F) or the inte-
cost on an industrial scale, low selectivity of CO2/N2, poor chemical, gration of functional groups (eNH2, eOH) within POPs. This can be
mechanical, and hydrothermal stability, These challenges still realized by using diverse monomers or implementing post-
persist for their application under humid conditions [387]. functionalization techniques. Unfortunately, the insertion of func-
Furthermore, to assess their virtues and demerits, metrics such as tional groups could potentially diminish the CO2 capture efficiency
cyclic stability, regenerability, and kinetics must be evaluated under of POPs. This could occur due to the added volume of functional
real/harsh operating conditions. Therefore, as stated by Youmas groups obstructing the available pore space or leading to an in-
et al. [355], integrating the economics of the manufacturing process crease in the density of porous polymers, among other possible
with the molecular-level properties of MOFs is essential path to factors. Diverse strategies can be applied to address these chal-
create materials that are technically viable as well as commercially lenges. These include utilizing low-density functional groups,
successful. controlling pore sizes to enhance CO2 surface interaction, and
Table 12 provides a comprehensive analysis of the impact of expanding the specific surface area of polymers [416,421e423].
modification strategies on the textural properties and CO2 uptake of In the case of industrial application, the subsequent aspects
various metal-organic frameworks. have been examined and continue to pose challenges, especially
within post-combustion capture technology. Those issues involve
3.4. Polymers CO2 capture performance at high temperatures and low pressures
(developing POPs with multiple adsorption sites for binding CO2
3.4.1. Porous organic polymers (POPs) molecules), material stability in the presence of moisture and at
Porous organic polymers (POPs) constitute an emerging class of high temperatures, cost-effectiveness and scalability (investigating
porous materials, composed of lightweight components linked by novel synthesis techniques that use non-noble metal catalysts, low-
robust covalent bonds. They have showcased significant potential cost monomers, and mild reactions) [421,423].
across various applications, including gas storage and separation Fig. 25 illustrates a comparison of modification strategies
[409,410]. Several classes of POPs have been developed, including applied to POPs in relation to various ongoing research trends.
conjugated microporous polymers (CMPs), covalent organic
frameworks (COFs), hyper-crosslinked polymers (HCPs), covalent [Link]. Conjugated microporous polymers (CMPs). Conjugated
triazine frameworks (CTFs), porous aromatic frameworks (PAFs), microporous polymers are three-dimensional semiconducting
and polymers of intrinsic microporosity (PIMs), presented sche- polymers in which rigid aromatic groups are connected together,
matically in Fig. 23. In the context of widespread utilization for CO2 either through direct bonds or double or triple bonds, to form p-
capture, three fundamental groups of POPs can be highlighted, such conjugated microporous structure [430]. Due to molecular rigidity
as CMPs, COFs, and HCPs. and expansion of their conjugated parts, creating the inherent
POPs exhibit a combination of advantageous characteristics, porous characteristics, they aroused great interest [431]. The CMPs
including low density, extensive surface areas, adjustable pore sizes can be synthesized by a wide range of synthetic building blocks and
with numerous channels, and abundant active sites available for enormously different synthesis routes, such as Sonogashira-
chemical reactions. They also offer easily customizable function- Hagihara coupling reaction, Suzuki-Miyaura reaction, Yamamoto
ality, exceptional physicochemical stability, and a wide array of reaction or Heck reaction [432]. This diversity results in CMPs
design options and synthetic approaches (Fig. 24). Hence, POPs having distinctive properties, different structures with unique
have arisen as highly promising CO2 capture materials [411e416]. skeleton, and highly modifiable nature.
Typically, diverse network reactions are employed in the prepara- Numerous CMPs have been developed in recent years to opti-
tion of each type of POPs. With the sole exception of CTFs and COFs, mize CO2 capture by various research approaches, e.g., tailoring
35
 Table 12

B. Dziejarski et al.
Influence of modification strategies on textural properties and CO2 uptake of metal-organic frameworks.

Metal-organic frameworks (MOFs) BET surface Total pore CO2 selectivity CO2 uptake, Adsorption Adsorption Reported modification Purpose of modification method Reference
area, m2/g volume, cm3/g at 1 bar mmol/g temperature, pressure, bar


C

Zn(ADC)(4,40 -Bpe)0.5‘xG 100 e e 5.8 78.15 1 Novel structures Tuning the micropores by triple- [370]
Cu(FMA)(4,40 -Bpe)0.5 e e e 4.41 78.15 1.0 Novel structures framework interpenetration [371]
PCN-5 225 (Langmuir) 0.13 e 4.80 78.15 1.0 Novel structures [388]
Flexible microporous MOF e e 116.00 1.11 25 1 Novel structures Increasing high selectivity in capturing [372]
and separating CO2 from a gas mixture
3D MOF (UPC-21) 1117 e 34.30 3.87 0 1 Novel structures Improving CO2 adsorption selectivity [389]
UTSA-120 [Cu(dpt)2(SiF6)]n 638 e ~600.00 3.56 23 0.15 Novel structures; Tuning the pore size; Enhancing the [373]
Functionalizing pore surface interaction strength between CO2 and
MOFs surface
2D MOF 340.8 e e 1.9 25 1 Novel structures; Obtaining thermal stability and [390]
Functionalizing pore surface moisture resistance; Increasing CO2
affinity
Dehydrated-MIL-53 (Cr) e e e 8.5 30.85 20 Adsorption conditions Influence of hydration on the [384]
Hydrated-MIL-53(Cr) e e e 7.7 30.85 20 (moisture effect) adsorption capacity and selectivity [384]
Hydrated 6.5 wt%-Mg-MOF-74 e e ~110 6.18 25 1 [385]
Hydrated 13 wt%-Mg-MOF-74 e e ~130 4.73 25 1 [385]
MOF-177 [Zn4O(BTB)2] 4508 e e 33.5 25 35 Adsorption conditions Influence of room temperature and high [391]
IRMOF-1 [Zn4O(BDC)3] 2833 e e 21.79 25 30 (temperature and pressure pressure on CO2 capacity (isotherms [391]
IRMOF-6 [Zn4O(C2H4;BDC)3] 2516 e e 19.45 25 30 effect) analysis) [391]
IRMOF-3 [Zn4O(NH2BDC)3] 2160 e e 18.70 25 30 [391]
IRMOF-11 [Zn4O(HPDC)3] 2096 e e 14.73 25 30 [391]
Cu3(BTC)2 [Zn4O(HPDC)3] 1781 e e 10.62 25 30 [391]
MOF-74 [Zn2(DHBDC)] 816 e e 10.41 25 30 [391]
MOF-505 [Cu2(BPTC)] 1547 e e 10.21 25 30 [391]
36

MOF-2 [Zn2(BDC)2] 345 e e 3.22 25 30 [391]

MIL-53(Al) e e e 10.53 30.85 30 Metal ions doping Improving the surface area, pore [392]
MIL-53(Cr) e e e 10.04 30.85 25 volume; Creating rich adsorptive sites [392]
[Ni6(OH)4(BTB)8/3(H2O)6]$ 819.3 e e 1.3 25 1 for CO2 adsorption [393]
4H2O$9DMF}n
Li-HKUST-1 985.8 0.46 e 7.89 25 18 [394]
Na-HKUST-1 1006 0.45 e 8.11 25 18 [394]
K-HKUST-1 1189 0.52 e 8.64 25 18 [394]
Cu3(BTC)2 1734 e e 2.94 42 1.1 Metal ions doping; Improving Improving the surface area, pore [395]
Cr3(BTC)2 1689 e e 1.82 42 1.1 activation procedures and volume, and CO2 affinity towards MOFs [395]
Ni3(BTC)2(DMF)2(H2O) 847 e e 2.32 42 1.1 syntheses surface [395]
Mo3(BTC)2(DMF)0.5 1689 e e 1.82 42 1.1 [395]
[Ru3(BTC)2][BTC]0.5 1180 e e 2.46 42 1.1 [395]
SNU-1100 411 0.248 35.00 0.58 25 1 Synthesis modification Improving the selectivity over H2, N2, [396]
(selecting or modifying organic CH4

Materials Today Sustainability 24 (2023) 100483

Noninterpenetrated-SNU-700 5290 2.17 e 0.80 25 1 linker) Improving a pore size, surface area, and [397]
Interpenetrated-SNU-710 1770 0.709 e 1.05 25 1 CO2 uptake [397]
MOF-505 [JNU-Bai12] 3038 e 24.60 19.85 25 20 Improving the specific surface area and [398]
pore volume
MOF-177 4500 1.89 e 35.23 25 50 Developing ultrahigh porosity [366]
MOF-210 6240 3.60 e 65.23 25 80 [366]
NU-100 6143 2.82 e 52.61 25 40 Improving surface area [367]
PCN-68 5109 2.13 e 41.00 25 100 [399]
ZNJU-43a 2243 0.8943 e 4.60 25 1 Synthesis modification Increasing basicity, affinity between [375]
(selecting or modifying organic CO2 molecules-adsorbent surface
linker); Creating Lewis basic
sites
PCN-124 1372 0.579 e 5.01 22 1 Synthesis modification Improving the micro-porosity, and the [400]
(selecting or modifying organic selectivity over CH4
linker); Metal site modification;
Functionalizing pore surface
 B. Dziejarski et al.
SNU-310 704 0.28 e 0.59 25 1.0 Synthesis modification Improving the selectivity over H2, O2, [401]
(selecting or modifying organic N2, CH4
UPC-105 2082 e 2.50 2.37 25 1 linker); Functionalizing pore Optimization of the pore environment [374]
UPC-106 1984 2.49 2.42 25 1 surface for enhanced C2H2/CO2 storage and [374]
UPC-107 1865 2.56 2.06 25 1 separation performances [374]
UPC-108 1837 e 2.84 2.04 25 1 [374]
UPC-109 1601 e 2.71 1.08 25 1 [374]
UPC-110 1384 e 5.10 1.08 25 1 [374]
UPC-111 1732 e 2.56 1.88 25 1 [374]
UPC-112 1559 e 2.76 1.83 25 1 [374]
pt-UiO-66(Zr)(OH)2 1230 e 105.00 5.63 25 1 New synthesis approach Improving a pore size, surface area, CO2 [402]
uptake, selectivity over H2, N2, CH4
amino-MIL-53 400 1.03 42.30 2.16 0 1 Amine functionalization Increasing basicity, affinity between [403]
1.88 23 CO2 molecules-adsorbent surface and
level-up N-contents
amino-MIL-53-dimethylformamide/ 356 0.71 637.00 2.98 0 1 Amine functionalization; Increasing basicity, affinity between [403]
ethanol 2.01 23 New synthesis approach CO2 molecules-adsorbent surface;
amino-MIL-53-dimethylformamide/ 321 0.65 637.00 2.42 0 1 Enhancing CO2 adsorption and [403]
ethanol/acetic acid 1.81 23 selectivity of CO2/N2
amino-MIL-53-dimethylformamide/ 348 0.51 153.00 3.17 0 1 [403]
methanol 2.10 23
amino-MIL-53-dimethylformamide/ 632 0.33 42.30 3.35 0 1 [403]
methanol/acetic acid
TEPA-HKUST-1 327 0.25 e 0.225 45 0.15 Amine functionalization Increasing basicity, affinity between [404]
TEPA- MIL-53 (Al) 286 0.30 e 0.159 45 0.15 (Tetraethylenepentamine) CO2 molecules-adsorbent surface and [404]
TEPA- ZIF-8 9 0.01 e 1.52 45 0.15 level-up N-contents [404]
ZJNU-13 1352 0.502 5.76 3.92 25 1 Oxygen atoms functionalization Increasing separation and purification [405]
with high adsorptivity and impressive
selectivity
dmpn-Mg2(dobpdc) 948 e e 2.42 40 1 Diamine functionalization (2,2- Increasing basicity, and affinity [406]
37

dimethyl-1,3- between CO2 molecules-adsorbent

diaminopropane)(dmpn) surface
ZNJU-19 2165 0.882 6.40 4.75 25 1 N-oxide groups Increasing affinity between CO2 [376]
ZNJU-20 2154 0.902 6.20 4.63 25 1 functionalization molecules-adsorbent surface; [376]
Enhancing CO2/CH4 separations
SNU-77H 3670 1.52 e 0.89 25 1 Different activation method Discarding unreacted precursors and [407]
approaches (high temperature solvents from synthesized MOFs
evacuation)
HCM-Cu3(BTC)2/Hierarchical porous 516 0.26 10.60 2.75 25 1 MOF incorporation in Composite/hybrid materials formation [379]
carbon monoliths hierarchical porous carbon
monoliths
MIL-101(Cr)/Activated carbon (type 2670 1.27 e 7.14 27 5 Activated carbon incorporated [378]
Maxsorb-III) in MOF
MIL-101(Cr)/MCM-41 2843 1.30 8.53 2.09 25 1 MCM-41 as the structure- [380]
directing agent for MOF

Materials Today Sustainability 24 (2023) 100483

MIL-101(Cr)/MIL-53(Al) 1746 0.80 59.34 16 25 40 Hybrids of nanoporous MOFs [408]
synthetization
B. Dziejarski et al. Materials Today Sustainability 24 (2023) 100483

remains an ongoing obstacle in synthetic chemistry because of the

complicated creation process of the porous morphology. Newly, Liu
et al. [444] improved CO2 adsorption capacity by developing a
simple post-knitting process to enhance the surface area. The ob-
tained CMPs had a high BrunauereEmmetteTeller surface area and
total pore volume up to 2267 m2/g and 3.27 cm3/g, respectively,
which was 2.3 and 8.8 times greater than that of the precursors.
These CMPs demonstrated significant CO2 uptake improvements,
achieving 3.98 mmol/g at 1 bar and 0
C. Moreover, it has been
reported that non-functionalized microporous organic polymers
(MOPs) typically exhibit a significantly low CO2 uptake at ambient
temperatures and pressures. This is due to their low CO2 adsorption
enthalpies resulting from the absence of robust CO2 binding sites.
To accomplish high-performance CO2 capture, novel MOPs with
rationally modified skeletons and varied functionalities are desir-
able. Zhang et al. [445] used sulfone and hydroxyl groups as func-
tionalities in a synthesis of biofunctionalized CMPs via palladium-
catalyzed Sonogashira-Hagihara cross-coupling reaction. The syn-
thesized polymers showed a significant BET surface area up to
1470 m2/g, along with a carbon dioxide uptake of 2.77 mmol/g at
0
C and 1.13 bar. Likewise, Wang et al. [446] proposed to use
thiophene as a base for two novel CMPs. The obtained adsorbents
displayed good physicochemical stability and outstanding CO2
adsorption capacity (14.73 mmol/g at 50 bar and 44.85
C).
Fig. 23. Classification of different types of porous organic polymers for CO2 capture Fig. 26 provides a current overview of the recent modification
application. strategies and research trends for CMPs. The CO2 uptake and
textural properties of CMPs associated with distinct methodologies
size and shape of the pores [433e436], incorporation of functional are summarized in Table 13, providing a comprehensive overview
groups [437e440], introduction of heteroatoms into the skeleton of the data.
[441,442], and metal functionalization [413]. Due to that, CMPs can
be customized for utilization across a diverse spectrum of CO2 [Link]. Covalent organic frameworks (COFs). Covalent organic
capture applications, owing to the wide range of variability in the frameworks are synthesized based on the principles of reticular
selection and design of components, as well as the control over chemistry, where organic building blocks with pre-designed ge-
other characteristics. Jiang et al. [443] showed that, the surface area ometries and radicals are connected through the formation of co-
and pore size can be regulated by the monomer structure of the valent bonds to produce extended networks [451]. Fine regulation
network. In addition, these features may be fine-tuned in a pore sizes, shapes with specific distribution, alongside achieving
continuous way by copolymerization of monomers with varying low density and precise control of skeleton structure, emerge as the
lengths. This provides an unparalleled level of direct synthetic most attractive characteristics of COFs for CO2 adsorption. This
control over micropore characteristics in an organic network. distinction is particularly apparent when comparing COFs with
CMPs also encounter many challenges that need resolutions, crystalline structures to their amorphous counterparts [452].
Gao et al. [421] in their review highlighted that one of the most Recent findings suggested that materials featuring pore sizes close
significant considerations for the future involves discovering cost- to the kinetic radius of CO2 tend to exhibit notable CO2 uptake
effective synthesis methods, attributed to the difficulties of scal- [423], emphasizing the effectiveness of COFs with precisely
ability. Other issues relate achieving a high surface area, which controlled pore sizes as promising CO2 capture materials [453].

Fig. 24. Synthetic methodologies widely used for the preparation of POPs [419,420].

38
B. Dziejarski et al. Materials Today Sustainability 24 (2023) 100483

Fig. 25. The modification strategies and research directions of porous organic polymers.

Similar conclusions were drawn by Furukawa and Yaghi [454], heteropores possessed two kinds of micropores characterized by
demonstrating that COFs hold an advantageous standing in com- varying shapes and sizes, with one being a quadrangle and the
parison to common carbon-based materials, zeolites, and MOFs. other an inequilateral hexagon. They exhibited favorable adsorp-
This positions COFs firmly within the category of valuable porous tion capacities for CO2 and H2, with CO2 uptake reaching up to
materials and highlights their efficacy as effective CO2 adsorbents. 19.8 wt% (0
C, 1 bar), positioning them as one of the top-
A significant number of ongoing research concern the explora- performing COFs for CO2 capture.
tion for innovative COFs through diverse different synthetic An alternative approach for developing COFs is the functional-
methods, aiming to capture CO2 from a variety of sources and ization of pore surfaces, specifically through channel wall func-
transform it to valuable products. These applications involve CO2 tionalization. This can be achieved by incorporating chemical
fixation to epoxides for cyclic carbonate synthesis and CO2 reduc- moieties, such as polar functional groups [457], immobilizing ionic
tion to CO [455]. Additionally, it is very desirable to combine the liquids or introducing specific special active sites into polymer
criteria for high crystallinity, robust stability, and increasing networks [458], such as heteroatoms [459], charged units [460] and
porosity with the requirements for high specific surface area and unsaturated metal sites [461]. The objective of these modifications
small pore size for gas storage. In consequences, the precise regu- is to enhance the affinity between the material surface and CO2.
lation of control of internal pore structure becomes crucial for COFs. Huang et al. [457] reported a strategy for converting a conven-
Considering these trends, Tian et al. [456] managed to develop a tional 2D COF into an outstanding platform for carbon dioxide
strategy to construct heteropores COFs. These COFs with capture through channel-wall functionalization. Through the

39
B. Dziejarski et al. Materials Today Sustainability 24 (2023) 100483

Fig. 26. The modification strategies and research directions of conjugated microporous polymers.

adoption of a dense layer structure, the integration of carboxylic- and 0.97 cm3/g, respectively. The resulting COF demonstrated a
acid groups onto the channel walls was successfully achieved, selectivity value of 19, indicating its ability for moderately selective
leading to the emergence of an advanced version of COF with CO2/N2 adsorption, with a CO2 uptake of 1.71 mmol/g.
enhanced CO2 uptake, reusability, selectivity, and separation pro- Collectively, these data indicate that it is imperative to dedicate
ductivity for flue gas treatment. The results indicated that channel- substantial resources towards investigating the synthesis and
wall functionalization effectively transformed typical COFs into CO2 characterization of COFs. This research should aim to integrate the
adsorption materials with exceptional performance. desirable attributes of stability, crystallinity, and porosity in COFs,
Dong et al. [458] presented immobilization of ionic liquid on the with the ultimate goal of optimizing their efficacy as CO2 capture
channel walls of COF using a post-synthetic strategy. According to materials. Furthermore, considering the analysis of various reviews
authors, the ionic COF exhibited an excellent CO2 adsorption ca- about COFs, it is possible to provide supplementary objectives for
pacity of 3.74 mmol/g (1 bar, 0
C) and was very stable. Further- enhancing this category of POPs. Olajire et al. [463] used a wide
more, it has been established as an efficient heterogeneous catalyst range of sources to present an in-depth look of potential research
for the transformation of CO2 into high-value-added formamides paths for COFs. According to the author, research endeavors should
under ambient conditions. be concentrated on the following areas, such as the exploration of
Buyukcakir et al. [460] developed and synthesized the first novel synthetic methodologies, 3D COFs construction, improving
charged covalent triazine frameworks (CTFs) with temperature- the synthesis parameters of COFs and scaling them for commercial
dependent surface area and hierarchical porosity by incorpora- applications, constructing hybrid membranes based on COFs, and
tion of ionic functional moieties. The ionic character of CTFs, in conducting experiments on separation of CO2 from other gases in
addition to their large surface area, thermal and chemical dura- flue gas streams. In addition, Gao et al. [421] highlighted an addi-
bility, resulted in considerable increases in CO2 adsorption capacity, tional significant challenge, which involves synthesizing COFs with
due to the extra electrostatic interactions between CO2 molecules high CO2 uptake under humid conditions.
and charge centers of viologen units. The resulting CTFs showed Fig. 27 presents the current status of modification strategies and
high BET surface area up to 1247 m2/g and CO2 uptake approxi- research directions for COFs. Table 14 offers an overview of CO2
mately around 3.02 mmol/g at 1 bar and 0
C. uptake and textural properties exhibited by COFs in relation to
Liu et al. [462] constructed the triazine-based COF (highly specific modification strategies.
heteroatom-functionalized COF) with a 2D structure by the
condensation reaction. The adsorbent exhibited a notable level of [Link]. Hyper-crosslinked polymers (HCPs). Hyper-crosslinked
crystallinity, along with remarkable chemical and thermal stabil- polymers are commonly synthesized from a wide range of low-cost
ities. The BET surface area and a pore volume measured 1407 m2/g monomers and electrophiles that serve as cross-linking agents. The
40
 Table 13
Influence of modification strategies on textural properties and CO2 uptake of conjugated microporous polymers.

B. Dziejarski et al.
Conjugated BET surface Average pore Total pore Micropore Vmic/Vtot, % CO2 selectivity CO2 uptake, Adsorption Pressure, Reported modification Purpose of modification Reference
microporous area, m2/g size, nm volume, volume, cm3/g at 1 bar mmol/g temperature,
C bar method
polymer cm3/g

CMP@1 346 e 0.22 e e e 1.52 0 1 New synthetic methodologies Novel structures [447]
1.03 25 of synthesis (imidization
CMP@2 325 e 0.60 e e e 2.28 0 1 reaction) [447]
1.47 25
CMP@3 343 e 0.70 e e e 1.43 0 1 [447]
0.71 25
BTCMP-1 4.37 e 0.0046 e e e 14.73 44.85 50 New synthetic methodologies [446]
BTCMP-2 5.13 e 0.0019 e e 6.57 44.85 50 of synthesis (cross-coupling [446]
polycondensation)
CMP 772 e 1.21 0.117 9.7 e 1.61 25 1 Metal functionalization (Co, Al) Creating rich adsorptive sites [413]
Co-CMP 965 e 2.81 0.419 14.9 e 1.80 25 1 for CO2 adsorption [413]
Al-CMP 798 e 1.41 0.298 21.1 e 1.74 25 1 [413]
ZnPe50%F-CMPs 240 e 0.376 e e e 2.05 25 1 Introduction of chemical Increasing affinity between CO2 [448]
functionalities (fluoride molecules-adsorbent surface
functionalization)
BFCMP-1 1316 e 1.20 0.31 25.83 31.90 2.45 0 1.13 Introduction of chemical [445]
1.39 25 functionalities (sulfone and
BFCMP-2 1470 e 1.35 0.29 21.48 29.60 2.77 0 1.13 eOH groups) [445]
1.64 25
CMP-1 837 e 0.45 0.32 71 e 1.18 25 1 Introduction of chemical [438]
CMP-1 COOH 522 e 0.30 0.22 73 e 1.60 25 1 functionalities (carboxylic [438]
CMP-1-NH2 710 e 0.39 0.27 69 e e e e acids, amines, hydroxyl groups, [438]
CMP-1-(CH3)2 899 e 0.75 0.34 45 e 0.94 25 1 and methyl groups) [438]
CMP-1-(OH)2 1043 e 0.71 0.40 56 e 1.07 25 1 [438]
NCMP-2 900 e 0.55 0.32 58.18 10.50 2.10 0 1 Introduction of heteroatoms [449,450]
1.15 25 (N)
41

TPA-BD-CMP 543 e 1.11 e e e 3.25 0 1 [441]

TCMP-0 963 e 0.98 0.38 39 9.60 2.38 0 1 Synthetic control of the Improving the pore and surface [450]
1.34 25 micropore size and surface properties; Increasing affinity
TNCMP-2 995 e 0.55 0.30 73 7.60 2.62 0 1 area; between CO2 molecules- [450]
1.45 25 Introduction of chemical adsorbent surface
TCMP-3 961 e 0.36 0.28 78 25.20 2.25 0 1 functionalities into CMPs [450]
1.26 25 skeleton (nitrogen-rich triazine
TCMP-5 494 e 0.51 0.19 37 17.00 0.37 0 1 units) [450]
1.22 25
CMP-0 1018 e 0.56 0.38 67.86 e 2.10 0 1 Synthetic control of the Improving the pore and surface [443]
1.21 25 micropore size and surface area properties to promote the
CMP-3 522 e 0.26 0.18 69 e 1.22 0 1 interaction with CO2 [443]
0.68 25
CMP-5 512 e 0.47 0.16 34 e 1.11 0 1 [443]

Materials Today Sustainability 24 (2023) 100483

0.63 25
KCMP-F1 1433 2.9 1.04 0.32 30.8 e 0.58 0 0.15 Synthetic control of the [444]
2.70 1 micropore size and surface area
KCMP-M1 1845 3.6 1.66 0.35 21.1 e 0.88 0 0.15 [444]
3.77 1
KCMP-F2 1632 5.1 2.08 0.34 16.3 e 0.86 0 0.15 [444]
3.51 1
KCMP-M2 2267 5.3 3.00 0.31 10.3 e 0.80 0 0.15 [444]
3.69 1
KCMP-F3 494 5.1 0.64 0.12 18.8 e 0.42 0 0.15 [444]
1.59 1
KCMP-M3 1321 3.6 1.20 0.30 25.0 29.10 0.97 0 0.15 [444]
3.61 1
KCMP-F4 1245 6.9 2.16 0.20 9.3 e 0.46 0 0.15 [444]
2.14 1
KCMP-M4 2157 6.1 3.27 0.34 10.4 e 0.90 0 0.15 [444]
B. Dziejarski et al. Materials Today Sustainability 24 (2023) 100483

Fig. 27. The modification strategies and research directions of covalent organic frameworks.

Friedel-Crafts alkylation reaction, employed in the production of other characteristics, HCPs exhibit robustness and scalability,
HCPs, allows the attainment of desired properties without neces- exceptional thermal stability, outstanding chemical resistance (e.g.,
sitating the use of precious metal coupling catalysts [467]. More- to strong acids and bases), and exceptionally facile manufacturing
over, a variety of precursors has been used in the synthesis process process on a large scale. Nevertheless, a significant challenge
of HCPs. A noticeable trend is observed in repurposing waste ma- encountered by HCPs is associated with their molecular design-
terials [468], including biomass-based aromatic compounds [469]. based synthesis, requiring carefully control over pore structure
That is closely related to the broad adaptability of monomers, and [421].
the processability of their structures. For example, Fu et al. [468] A considerable body of literature has focused on the exploration
proposed a facile strategy for synthesizing HCPs using expanded of strategies to improve CO2 capture by COFs. The conventional
polystyrene foam. The HCPs that were produced exhibited high approach adopted to enhance the CO2 adsorption capacity of these
specific surface areas and excellent thermal stability. At 0
C and materials involves increasing the specific surface area and modi-
1.13 bar, HCP demonstrated the maximum CO2 adsorption capacity, fying the pore size through various synthetic methods. In recent
reaching 1.987 mmol/g, along with the highest adsorption selec- years, studies have shown that HCPs containing active sites can
tivity ratio (CO2 over N2) of 23.4. Additionally, Fayemiwo et al. [470] achieve higher CO2 adsorption capacity while having a smaller
used monomers for the environmentally friendly fabrication of specific surface area compared to traditional HCPs. For this reason,
HCPs using hydrocarbons sourced from fossil fuels. several endeavors have been undertaken with the aim of increasing
Compared to other types of microporous polymers, HCPs offer a the CO2 uptake and selectivity of HCPs by the introduction of polar
straightforward synthesis procedure, a diverse selection of mono- functional groups or heteroatoms (N, O, Si). Fayemiwo et al. [472]
mer sources, and a relatively inexpensive and widely accessible synthesized a series of nitrogen-rich, hyper-crosslinked polymers
catalyst [471]. One of the most significant advantages of these (HCP-MAAMs) through bulk co-polymerization. The polymers were
organic polymers for CO2 capture is the substantial surface area initially functionalized with amide groups and demonstrated a
created through the interconnected aromatic structures. Among remarkable CO2/N2 selectivity of 104 at ultra-low CO2 partial
42
 Table 14

B. Dziejarski et al.
Influence of modification strategies on textural properties and CO2 uptake of covalent organic frameworks.

Covalent organic frameworks Covalent BET surface Total pore CO2 selectivity CO2 uptake, Adsorption Pressure, Reported modification Purpose of modification Reference
bond type area, m2/g volume, cm3/g at 1 bar mmol/g temperature, bar method


C

SIOCeCOF-5 Imine 707 0.59 e 4.5 0 1 Synthetic control of new Novel structures [456]
SIOCeCOF-6 Imine 1617 0.92 e 3.2 0 1 topological structure
TPEeCOFeII Imine 2168 2.14 e 5.27 0 1 Novel synthetic methodologies Broadening the synthetic [464]
scope for making tunable
framework structures
COF-JLU2 Azine 410 0.56 77.0 4.93 0 1 Tuning the porosity, pore [459]
volume/size, surface area
and increasing number of
heteroatom active sites
COF-JLU6 Imine 1450 0.96 e 2.93 0 1 Tuning the porosity, pore [465]
COF-JLU7 Imine 1392 1.78 e 3.43 0 1 volume/size, surface area, [465]
and functionalization of
COFs frameworks
ACOF-1 Azine 1176 0.91 e 4.02 0 1 Tuning the porosity, pore [452]
TDCOF-5 Boronate 2497 e e 2.1 0 1 volume/size, surface area [466]
[Et4NBr]50%-Py-COF Imine 700 e e 3.74 0 1 Functionalization of COFs Tuning the pore size, [458]
frameworks (immobilization of surface area, and increasing
ionic liquids) affinity between CO2
molecules-adsorbent
surface
cCTF-500 Triazine 1247 1.04 e 3.02 0 1 Functionalization of COFs Tuning the porosity, and [460]
1.82 25 frameworks (incorporation of surface area to promote the
cCTF-450 Triazine 861 0.59 e 2.25 0 1 charged units) interaction with CO2 [460]
1.41 25
43

cCTF-400 Triazine 744 0.36 e 2.86 0 1 [460]

1.89 25
[HO]25%- H2PeCOF Imine 1054 0.89 e 54 0 1 Functionalization of COFs Tuning the porosity, and [457]
31 25 frameworks (introduction of increasing affinity between
[HO]50%- H2PeCOF Imine 1089 0.91 e 46 0 1 polar functional group) CO2 molecules-adsorbent [457]
32 25 surface
[HO]75%- H2PeCOF Imine 1153 0.96 e 52 0 1 [457]
32 25
[HO]100%- H2P -COF Imine 1284 1.02 8.00 63 0 1 [457]
35 25
[HO2C]25%- H2PeCOF Imine 786 0.78 e 96 0 1 [457]
58 25
[HO2C]50%- H2PeCOF Imine 673 0.66 e 134 0 1 [457]
67 25
[HO2C]75%- H2PeCOF Imine 482 0.54 e 157 0 1 [457]

Materials Today Sustainability 24 (2023) 100483

72 25
[HO2C]100%-H2PeCOF Imine 364 0.43 77.00 174 0 1 [457]
76 25
TMFPT-COF Triazine 1407 0.97 17.00 1.71 0 1 Functionalization of COFs [462]
0.86 25 frameworks (introduction of
heteroatoms)
MCTF@500 Triazine 1510 2.674 e 3.16 0 1 Functionalization of COFs [461]
frameworks (introduction of
unsaturated metal sites)
COF-1 Boronate 750 0.30 e 5.23 0 55 e e [454]
COF-5 Boronate 1670 1.07 e 19.17 0 55 [454]
COF-6 Boronate 750 0.32 e 7.05 0 55 [454]
COF-8 Boronate 1350 0.69 e 14.32 0 55 [454]
COF-10 Boronate 2080 1.44 e 22.95 0 55 [454]
COF-102 Boronate 4650 1.55 e 27.27 0 55 [454]
COF-103 Boronate 4630 1.54 e 27.05 0 55 [454]
B. Dziejarski et al. Materials Today Sustainability 24 (2023) 100483

pressures. At 0
C, the maximum CO2 adsorption capacity was Shao et al. [478] developed a series of NDPC with tunable porosity
1.56 mmol/g, while the corresponding isosteric heat of adsorption and polarity derived from the N-containing HCPs, prepared from 4-
ranged from 28 to 35 kJ/mol, respectively. vinylbenzyl chloride and 4-vinyl pyridine by the suspension poly-
Another extensively reported nitrogen-containing functional merization and Friedel-Crafts reaction. It was found that the cur-
group used in HCP synthesis is carbazole [473e477]. Chang et al. rent NDPC could be good candidates for CO2 capture, and a new
[475] created two distinct types of indolo[3,2-b] carbazole-based idea was proposed for the design of porous carbons e the ultra-
building blocks, differing in the different number of reactive sites. micropore walls modified with plentiful heteroatoms. The volume
The synthesized nitrogen-rich polymers demonstrated a substan- of ultramicropores was shown to be a critical element in CO2
tial BET surface area of up to 1421 m2/g, coupled with a CO2 uptake adsorption. The developed material exhibited satisfactory CO2 up-
of 3.58 mmol/g at 0
C and 1.13 bar. These values are comparable to take (6.11 mmol/g at 0
C and 1 bar) and CO2/N2 selectivity (11.2) of
those seen in several other POPs, indicating their competitive na- the developed material were satisfactory. Similar outcomes were
ture. Ramezanipour Penchah et al. [477] investigated the influence achieved in the experiment using imidazole-based HCPs. In the
of operating parameters (crosslinker ratio, synthesis time, and other study, Shao et al. [479] observed that the NDPCs exhibited a
catalyst type) on CO2 adsorption capacity of carbazole-based HCP, large BET surface area (1248e2059 m2/g) and pore volume
synthesized through a FriedeleCrafts reaction. At a temperature of (0.80e1.12 cm3/g). At low pressure, these NPCs adsorbed a large
25
C and a pressure of 5 bars, the CO2 uptake reached its optimum amount of CO2 (4.09e5.86 mmol/g at 0
C and 1 bar,
value of approximately 4.35 mmol/g. 0.93e1.66 mmol/g at 0
C and 0.15 bar). In conclusion, it was
HCPs can also serve as precursors for producing porous carbons. determined that in comparison to porosity, the nitrogen concen-
The wide variety of aromatic compounds available as raw materials tration has a minor impact on CO2 uptake.
makes it appealing to synthesize porous carbons from HCPs, A comprehensive overview of the paths for modifying HCPs
especially those that are highly porous or entirely microporous and the direction of ongoing research is presented in Fig. 28.

Fig. 28. The modification strategies and research directions of hyper-crosslinked polymers.

44
B. Dziejarski et al. Materials Today Sustainability 24 (2023) 100483

Table 15 presents a thorough analysis of how various strategies crystallinity that are not achievable in nature. On the contrary, in
have impacted the textural properties and CO2 adsorption capa- terms of CO2 capture, synthetic zeolites tend to be more expensive
bilities of hyper-crosslinked polymers, showcasing their potential compared to more affordable natural zeolites, which, despite their
for advancing carbon capture technologies. lower cost, often display inferior sorption properties, varying
composition, and reduced purity [497].
3.5. Zeolites Over the last few decades, waste management and the reduction
of costs in the synthesis process of zeolites have gained importance
Since the seminal discovery made by Cronstedt in 1756, zeolites in many sectors of the industry. A substantial amount of research
have attracted significant scholarly interest, leading to several has been dedicated to both the reuse of fly ash as a raw material and
practical applications in recent decades. Zeolites offer several ad- the exploitation of natural material. Garshasbi et al. [498] prepared
vantages, including cyclic stability, high surface area, and extremely zeolite 13X synthesized by hydrothermal treatment using natural
fast kinetics of CO2 adsorption compared to other solid sorbents clays. The zeolite 13X demonstrated a superior BET surface area
[483,484]. They additionally possess robust adsorption sites and (591.22 m2/g), CO2 uptake (6.9 mmol/g) and micropore volume
show favorable mechanical properties, including high abrasion (0.250 cm3/g) compared to the other materials studied. Chen et al.
resistance, density, and mechanical strength, enabling their for- [499] prepared zeolite 13X using bentonite as raw material by
mation into granules, spheres, and extrudates [485e487]. alkaline fusion followed by hydrothermal treatment. It was deter-
Furthermore, these CO2 capture materials have an immense mined that the newly synthesized zeolite 13X had high BET surface
adsorption capacity under moderate operating conditions area of 688 m2/g, a large micropore volume of 0.30 cm3/g, and
(0e100
C, 0.1e1 bar) [488], which is strongly influenced by tem- exhibited substantial CO2 capture capacity (4.80 mmol/g) along
perature and is positively correlated with their pore size [489]. with selectivity (CO2/N2 ¼ 37) at 25
C and 1 bar. Considering these
Unfortunately, if the temperature approaches 100
C, the CO2 up- details, the variety of natural and synthetic zeolites makes them
take of zeolites drops dramatically. According to lately review of appealing for use in the CO2 adsorption process due to their un-
Kumar et al. [489], it was indicated that the optimal temperature for usual versatility.
CO2 adsorption on zeolites is 70
C, which is lower than the typical Zeolites are a class of highly porous crystalline aluminosilicates,
flue gas temperature (normally 90
C). Therefore, either cooling the composed of tetrahedrons formed by shared oxygen atoms of
flue gas or modifying the adsorbents to render them suitable for alumina and silica, characterized by the formula TO4 (T ¼ Si or Al)
high-temperature adsorption is necessary before their industrial- [500]. Such a substitution leads to the accumulation of negative
scale implementation. On the other hand, introduction an addi- charge in their pore structure, leading to an increase in basicity
tional process, such as cooling, could lead to increased energy when incorporating a higher concentration of aluminum atoms in
consumption and higher costs in CO2 capture technology. Hence, the framework [501]. This is owing to the weaker electronegativity
addressing this aspect effectively in the future is crucial. Fig. 29 of aluminum compared to silica, which causes this effect. Further-
provides a schematic representation of the zeolites most more, cations (Liþ, Naþ, Ca2þ, etc.) are present in the zeolite's
frequently mentioned in the literature for applications in CO2 channels and chamber systems, with strictly defined molecular
adsorption. sizes to compensate for this negative charge. This gives rise to
In last years, more publications have been published in zeolite another key aspect of zeolites, namely, ion exchange [502].
discipline, and it is apparent that researchers are concentrating their Consequently, the alteration of the Si/Al ratio is of significant
efforts on a few key areas, including: (1) searching for new raw importance, as higher basicity corresponds to greater CO2 adsorp-
materials, (2) new synthetic methodologies of synthesis, (3) tion capacity of zeolites [503]. The different Si/Al ratios in zeolites
designing of textural properties and material composition (by determine their properties. Low-silica zeolites (Si/Al < 2) exhibit
changing the Si/Al ratio, development of porosity), (4) cation ex- considerable acid resistance and thermal stability, as well as hy-
change, (5) amine functionalization, (6) reduction of adverse drophilic properties. Conversely, high-silica zeolites (Si/Al > 50) are
moisture-related impacts, and (7) developing composite/hybrid characterized by an increased degree of ion exchange, and hydro-
materials. Furthermore, regarding the latest first-principles phobicity [504]. Overall, this parameter signifies the focus of
modeling for the design of materials in CO2 capture technologies, research endeavors concerning zeolite-based adsorbents, specif-
Yuan et al. [490] stated that utilizing DFT fundamentals to analyze ically centered around optimizing material composition through
CO2 adsorption behavior on zeolites can be applied to predict mul- diverse synthesis approaches. Further, due to the defined crystal
tiple factors, such as adsorption capacity, preferred sites, and selec- structure, zeolites show a very narrow pore size range from 0.5 to
tive adsorption between different gaseous mixtures. The same 1.2 nm [505]. As a direct consequence of possessing that property,
quantum-mechanical method for modeling non-covalent in- zeolites can effectively separate CO2 molecules through a molecular
teractions and thermochemistry, has been reported in many other sieving process, because of their tailorable cavities and tunable
papers [491e495]. Currently, molecular simulations play a crucial pore sizes. The presence of microporosity in zeolites classifies them
role in advancing understanding of the correlation between micro- as molecular sieves, enabling pore size-dependent adsorption
scopic and macroscopic characteristics within zeolites. Gaining in- selectivity (Fig. 30) [506]. In this case, only gas molecules with a
sights into the adsorption characteristics of zeolites could enhance kinetic diameter smaller than the pore size of the zeolite can be
knowledge of the underlying processes of adsorption and diffusion adsorbed. Hence, the topologies and pore diameters within the
phenomena. Also, it can contribute to identifying further potential crystal lattice are important criteria in the research for developing
applications of zeolites as CO2 adsorbents. The generic methodology CO2 capture materials based on zeolites. Introducing mesopores
was comprehensively described by García-Pe rez et al. [496]. into microporous zeolites, achieved through the synthesis of hier-
Zeolites can be categorized into natural and synthetic. Natural archical porous materials, stands as one of the most promising
ones are used as dryers, deodorants, for air separation, ion ex- approaches for creating novel structures with tailored chemical and
change (in water treatment, especially heavy metal ions), and soil textural attributes [507e510]. It offers the combined benefits of
improvement. Synthetics are exploited primarily for research and improved CO2 adsorption properties and enhanced mass transfer
industry and possess several distinct advantages over those that through the mesoporous channels, due to adaptable porous struc-
occur in nature. One of them is the possibility of achieving un- ture that effectively addresses limitations in molecule diffusion
precedented levels of control over the material porosity and [511,512].
45
 B. Dziejarski et al.
Table 15
Influence of modification strategies on textural properties and CO2 uptake of hyper-crosslinked polymers.

Hyper-crosslinked BET surface Total pore volume, cm3/g Micropore CO2 selectivity CO2 uptake, Adsorption temperature, Pressure, Reported modification Purpose of modification Reference


polymers area, m2/g volume, cm3/g at 1 bar mmol/g C bar method

HCPs-5% 1165 0.98 0.37 32.30 2.25 0 1 Novel synthetic Tuning the porosity, and [480]
0.56 0.15 methodologies (new surface area to promote the
synthesis strategy) interaction with CO2
HC-Pcz-8 1688 1.11 0.37 17.00 3.50 25 1 Novel synthetic [476]
methodologies (new
synthesis strategy)
HCTPP 582 0.32 e e ~1.65 25 1 Novel synthetic [481]
HCTPA 921 0.53 e e ~2.13 25 1 methodologies (selecting [481]
HCTPM 670 0.37 e e ~1.70 25 1 external crosslinker) [481]
InCz-HCP2 1421 1.48 0.42 29.00 3.58 0 1.13 Heteroatoms Enhancing adsorbent [475]
functionalization (N) surface binding affinity to
46

HCP 992 1.06 0.1188 49.00 3.55 0 1 Heteroatoms CO2 molecules [471]
2.72 25 functionalization (N, O)
HCP-MAAM 142 0.87 e 53.00 1.45 0 1 Introduction of chemical [470]
HCP-MAAMs 1 856 1.00 0.25 ~20.00 1.56 0 1 functionalities (amide [472]
groups)
BAHCP 1101 e e 42.00 3.03 0 1 Introduction of chemical [482]
functionalities (-OH
groups)
HCP-1 434 0.25 0.19 56.60 1.95 25 1 HCP as precursor N-doped Providing the possibility to [479]
0.61 0.1 porous carbon large-scale production;
NPC-700-KOH 2616 1.37 1.14 14.20 5.45 25 1 Employing the large [479]
0.80 0.1 number of containing N
NDPC-10% 1226 0.70 0.57 20.20 6.11 0 1 aromatic compounds [478]
3.89 25
NPC-700-ZnCl2 1105 0.58 0.50 42.60 4.02 25 1 [479]

Materials Today Sustainability 24 (2023) 100483

1.09 0.15
B. Dziejarski et al. Materials Today Sustainability 24 (2023) 100483

Fig. 29. Classification of zeolites for CO2 capture application.

Panda et al. [513] created hierarchical zeolites 4A (HZ4A) by (Co(II), Ni(II), Zn(II), Fe(III), Cu(II), Ag(I), La(III), and Ce(III)) exchanged
introducing mesoporosity into zeolites Z4A bodies using a urea SSZ-13, Co(II)/SSZ-13 and Ni(II)/SSZ-13 demonstrated the greatest
treatment under hydrothermal conditions. The obtained CO2 uptake (4.49 and 4.45 mmol/g, respectively) and the best CO2
zeolites showed adjustable physicochemical properties, including selectivity over N2 (52.55 and 42.61, respectively) at 0
C and 1 bar.
expanded surface area (126 m2/g), increased mesopore volume The findings revealed a significant difference between performance
(0.44 cm3/g), and coexistence of micropores (about 0.4 nm) with of alkali metal-form. The exceptional CO2 capture capacity was
mesopores (5.5 nm). Moreover, compared to Z4A bodies, the attributed to the pi-complexation effect.
presence of mesopores increased the rapid gas diffusion within the As previously observed in other material types, the influence of
pores during both adsorption and desorption. As an outcome, the moisture also poses an added challenge for zeolite-based adsor-
CO2 adsorption efficiency was improved, while maintaining an bents in real-world applications. The presence of another gas,
acceptable regeneration energy requirement. Dabbawala et al. [514] which potentially competes with CO2 molecules for active
designed the synthesis of hierarchical porous zeolite-Y by adsorption sites along with exposure to water vapor, can consid-
employing cationic polymer polydiallyldimethylammonium chlo- erably diminish the adsorption capacity and stability in an adverse
ride (PDDA) as a bifunctional mesopore directing template. It was manner [516,518]. Under acidic conditions that arise from contact
reported that the hierarchical zeolite-Y had a higher CO2 adsorption with water and carbon dioxide, there can be alterations in the
capacity (ranging from 5.4 to 5.9 mmol/g) and better selectivity
(reaching up to 160) than microporous zeolite-Y. Liu et al. [515]
prepared hierarchical porous zeolite (HP-ZSM-5) combining both
micro and mesoporous structures using organosilanes. The syn-
thesized material showed an improved CO2 adsorption capacity,
achieving a maximum value of up to 2.6 g/mol at 0
C and 1 bar. The
HP-ZSM-5 also demonstrated a faster physical adsorption process
compared to the pristine zeolite (ZSM-5). Further, it was deter-
mined that the microstructure and morphology of the hierarchical
zeolite were the most important parameters influencing the CO2
adsorption performance.
CO2 separation on zeolites can also occur through a mechanism of
selective adsorption, where CO2 molecules interact with the electric
field generated by the presence of ions within the zeolite framework.
This interaction creates a strong affinity between the acidic adsor-
bate and the adsorbent surface [516]. Thus, the coordination and
distribution of exchangeable cations within the zeolite framework
can influence the adsorption equilibrium and gas diffusion, directly
impacting the strength of the electric field they create. Sun et al. [517]
verified the CO2 capture efficiency of transition metal cation-
exchanged SSZ-13 zeolites. Among the tested transition metals Fig. 30. Schematic mechanism of CO2 adsorption in the zeolite Y structure.

47
B. Dziejarski et al. Materials Today Sustainability 24 (2023) 100483

dealumination of zeolite structures, leading to the disintegration of between 2018 and 2021, these improvements can be achieved by
the framework [519]. Other impurities within the flue gas stream creating composites/hybrid materials, and more specifically
can also negatively affect CO2 capture. Panda et al. [513] investi- through [542e554]:
gated the CO2 adsorption performance of HZ4A under humid con-
ditions, with HZ4A-13 exhibiting a CO2 uptake of 1.36 mmol/g at  new synthesis approaches and modification of the process
40
C and retaining 34.67% of CO2 adsorption (0.61 mmol/g) in conditions;
comparison to the dry state at 0.15 bar. Significantly, HZ4A-13  functionalization by ionic liquids;
shown superior performance in mitigating the negative effects of  functionalization by metal oxides/carbonates;
moisture within the low flue gas pressure range. Furthermore, the  impregnation with metal hydroxides;
authors highlighted that the CO2 adsorption capacity of HZ4A-13  impregnation or grafting with amines;
surpassed that of other tested adsorbents, including zeolite 13X,  use of different structure of Al2O3-based supports;
amine-functionalized LTA-125-NH2, and zeolite 5A, providing a  use carbon waste for aluminum extraction as an adsorbent.
distinct advantage. Consequently, HZ4A-13 holds promise for CO2
capture in humid flue gas environments within extensive coal-fired By combining an alumina-aerogel support with K2CO3, Bar-
power plant operations. arpour et al. [542] developed a unique process for the production of
Zeolites act as an excellent case in which intricate research can solid sorbents in the post-combustion CO2 capture process with
be succinctly outlined through a list of research requirements and very high CO2 capture capacity and stability. Compared to previous
potential development pathways as CO2 capture materials. Given investigations on alumina-based materials, the alumina-aerogel
this perspective, they establish the groundwork for a comprehen- support showed a significantly higher BET surface area of
sive methodological overview of the current advancements in 2019 m2/g, an achievement that had not been attained in previous
novel adsorbent production. The comparison of modification stra- studies for this specific type of material. Under optimal conditions,
tegies reported for zeolite-based adsorbents regarding their impact the sorbent achieved a notable CO2 capture capacity of 7.2 mmol/g
on CO2 adsorption performance and textural properties is pre- at 56.1
C, which was statistically significant. In another research,
sented in Table 16. Fig. 31 provides a broad overview of the modi- Bararpour et al. [546] investigated the influence of textural qualities
fication strategies and their associated research directions for on the performance of the mesoporous alumina supported K2CO3.
zeolites in CO2 capture. Al2O3 was synthesized using a surfactant-assisted technique. The
support constructed with a surfactant-to-Al ratio of 0.5 possessed
3.6. Alumina the highest CO2 uptake of 5.7 mmol/g and stayed stable during 15
cycles of carbonation/regeneration. This increase was related to the
Basic alumina, also referred to as aluminum oxide, is a well- existence of numerous active sites for carbonation reactions, lead-
recognized support material utilized in CO2 adsorption applica- ing to an enhanced CO2 capture capacity. Studies on the function-
tions, existing in multiple crystallographic forms (with approxi- alization of aluminum support with ionic liquids have also been
mately 27 forms reported to date). Substrates associated with the reported by Sun et al. [552].
synthesis of Al2O3 encompass aluminum-containing minerals, such Hiremath et al. [553] presented a facile, green, and template-free
as aluminum hydroxide and oxyhydroxide, the most known are synthesis of mesoporous Al2O3 for effective insertion of MgO to
bayerite (a-Al(OH)3 or b-Al(OH)3), gibbsite (Al2O3$3H2O or generate strong basicity. Significantly, the material was endowed
Al(OH)3), boehmite (g-AlO$OH), diaspore (a-AlO$OH), and pseu- with strong basicity, thereby eliminating the loss of active surface
doboehmite [536]. These chemical compounds differ in the area. The approach showed a scalable mesoporous structure with an
arrangement sequence of atomic layers and the distance between excellent surface area of 315 m2/g, characterized by a narrow pore
them. Subsequently, they are subjected to the Bayer process as raw size distribution (PSD). Furthermore, the incorporation of MgO as a
materials for alumina production. This procedure can be catego- heteroatom into the mesoporous alumina framework resulted in an
rized into three steps: extraction, precipitation, and calcination improved surface area of 357 m2/g, while maintaining PSD. An ad-
[537]. The various metastable phases of Al2O3 obtained through this vantageous aspect of the developed material was its improvement in
method are primarily influenced by the temperature of thermal basicity, increasing from 1.13 to 2.73 mmol/g. This improvement
treatment, the type of natural ore, and the pH of solution during the increased the affinity of the adsorbent surface for CO2 molecules.
neutralization process of aluminum salt [538]. The most recogniz- Zhou et al. [549] synthesized and immobilized polymeric ionic
able crystal types of alumina are alpha (a), rho (r), gamma (g), eta liquids (PILs) on mesoporous g- Al2O3 (MA) using the ultrasonic
(h), chi (c), theta (q), delta (ð), and kappa (8). The g-, r- and a-types immersion method. The experimental results showed that P[VCIm]
are the most frequently observed on an industrial scale [539]. Cl/MA demonstrated the highest CO2 adsorption capacity among all
Fig. 32 presents an overview of the commonly utilized alumina adsorbents. The maximum value reached 0.562 mmol/g and
phases in CO2 adsorption applications. occurred under optimal working conditions, including a loading
The use of an all-alumina support for CO2 adsorption offers ratio of 1:1, a temperature of 40
C, a pressure of 5 bar, and a CO2
many prominent benefits. These advantages include cost- flow rate of 10 mL/min.
effectiveness, exceptional crystallinity, high specific surface area, Another noteworthy research direction is the extraction of
well-tailored mesoporosity, large pore volumes, as well as superior alumina from coal-based solid waste, which serves as a means to
chemical, mechanical, and thermal stability [319,540,541]. Current mitigate environmental hazards. Li et al. [550] prepared amine-
research trends mainly focus on enhancing the physicochemical functionalized CO2 adsorbents by grafting APTES with the
properties of Al2O3-based supports to improve CO2 adsorption ca- alumina residue and the alumina-extracted residue. The findings
pacity, stabilize adsorption-desorption cycles, and increase CO2 indicated that under conditions of 25
C and 100 vol% CO2 feed flow,
selectivity over CH4/N2 in flue gas streams. These covers optimizing the sample treated with 12 mmol of APTES exhibited a peak CO2
texture characteristics, periodicity, long-range order, the distribu- adsorption capacity of 1.23 mmol/g. The sorbent was successfully
tion, or number of active sites, as well as adjusting basicity to regenerated at 110
C and maintained a stable uptake over 5
strengthen the interaction between the adsorbent surface and CO2 repeated adsorption-desorption cycles. Fig. 33 highlights related to
molecules. According to the modifications reported in the literature alumina that have been published in the literature.

48
 Table 16
Influence of modification strategies on textural properties and CO2 uptake of zeolites.

B. Dziejarski et al.
Zeolite BET surface Total pore Micropore Mesopore Si/Al ratio CO2 selectivity CO2 uptake, Adsorption Pressure, Reported modification Purpose of modification Reference
area, m2/g volume, volume, volume, at 1 bar mmol/g temperature, bar method


cm3/g cm3/g cm3/g C

Zeolite 4A e e e e 0.74 e 4.8 25 20.7 e e [181]

Zeolite 13X e e e e 1.08 e 5.2 25 20.7 e e [181]
Zeolite 13X 164.3 0.21 e e e e 4.54 25 30 e e [485]
Zeolite 5A e e e e e e 4.5 25 1 e e [520]
NaY 723 e 0.35 e e e 4.8 30 1 e e [521]
Nano-zeolite 698.19 0.369 e e e 18.65 4.81 20 1 Novel synthetic methodologies Enhancement of CO2 capture [419]
Silicalite-1 (CON) 390.14 0.24 e e e ~2.75 2.36 30 0.8 of synthesis [420]
Silicalite-1 (SON) 382.83 0.31 e e e ~3.20 2.12 30 0.8 [420]
A5 Zeolite 179.44 e e e 11.9 e 5.2 0 30 [522]
Z4A 39 0.14 e 0.13 e e 3.77 0 1 Novel synthetic methodologies Implementation of [513]
3.39 25 1 of synthesis; Textural mesoporosity into zeolite
3.00 40 1 properties adjustment; structure
Humid-Z4A e e e e e 1.56 40 1 Moisture effect
HZ4A-1-3 126 0.45 e 0.44 e e 3.41 0 1 [513]
3.09 25 1
2.86 40 1
Humid-HZ4A-1-3 e e e e e e 1.36 40 1 [513]
HZ4A-1-1 112 0.42 e 0.41 e e 2.72 0 1 [513]
2.38 25 1
2.05 40 1
HZ4A-3-1 65 0.53 e 0.52 e e 0.47 0 1 [513]
0.45 25 1
0.38 40 1
ZY 662 0.30 0.28 0.02 2.2 e 4.5 25 1 Novel synthetic methodologies Improving structural properties [514]
PDY-3 699 0.36 0.27 0.09 2.3 e 5.1 25 1 of synthesis; Textural (increasing the pore volume [514]
PDY-6 705 0.38 0.26 0.12 2.1 ~100.00 5.2 25 1 properties adjustment and surface area) [514]
49

PDY-7 773 0.39 0.26 0.13 2.0 160.00 5.9 0 1 [514]

5.4 25 1
ZSM-5 383 0.21 0.19 0.02 25 ~72.50 2.37 0 1 Novel synthetic methodologies Improving structural properties [515]
1.81 25 1 of synthesis; Textural (combining micro- and
Cl-HP-ZSM-5 438 0.29 0.17 0.12 26 ~67.50 2.60 0 1 properties adjustment; mesoporous structures) [515]
1.95 25 1 Moisture effect
Humid-Cl-HP-ZSM-5 e e e e e e 0.26 50 1 [515]
N-HP-ZSM-5 405 0.25 0.18 0.07 25.5 ~65.00 2.53 0 1 [515]
1.91 25 1
LTA-000 656 0.35 0.29 e e e e e e Textural properties Implementation of [523]
APTMS-LTA-050 708 0.64 0.23 e e e 1.4 60 0.15 adjustment; mesoporosity into zeolite [523]
APTMS-LTA-100 708 0.58 0.14 e e e 1.9 60 0.15 Amine functionalization (3- structure; Increasing basicity, [523]
APTMS-LTA-125 499 1.02 0.11 e e e 2.3 60 0.15 aminopropyl)trimethoxysilane) affinity between CO2 [523]
molecules-adsorbent surface
and level-up N-contents

Materials Today Sustainability 24 (2023) 100483

TEPA-ZSM-5 19.045 e 0.049 e e e 1.80 100 1 Amine functionalization Increasing basicity, affinity [524]
(Tetraethylenepentamine) between CO2 molecules-
Meso-13X 728 0.46 0.25 0.21 e e e 100 1 Amine functionalization adsorbent surface and level-up [525]
PEI-Meso-13X 1 0.001 e e e e 1.82 100 1 (Polyethylenimine) N-contents [525]
Ag(I)-SSZ-13 770.88 0.33 0.26 e 11.9 18.80 3.14 25 1 Cation exchange (Agþ, Co2þ, Increasing basicity, affinity [517]
Co(II)-SSZ-13 786.75 0.44 0.23 e 9.92 52.55 4.49 25 1 Niþ) between CO2 molecules- [517]
Ni(I)-SSZ-13 836.01 0.44 0.23 e 10.04 42.61 4.45 25 1 adsorbent surface [517]
Li-LSX 662 0.32 0.31 e 1.00 128.00 400 60 0.15 Cation exchange (Liþ) [526]
LiX 560.25 0.30 e e e 103.00 e e e Cation exchange (Liþ, Agþ, [527]
LiPdAgX 549.19 0.29 e e e 128.00 e e e Pd2þ) [527]
Clino 37 0.14 0.005 e 4.79 e 2.25 10 1 Cation exchange (Naþ); Increasing basicity, affinity [528]
2.16 30 Natural materials as zeolite between CO2 molecules-
Na-Clino 32 0.14 0.004 e 5.75 e 2.17 10 1 precursor adsorbent surface; Reduction of [528]
2.00 30 production costs
Na-Zeolite b 508 0.52 e e 7.4 16.80 3.45 0 1 Cation exchange (Naþ, Kþ, Liþ) [529]
(continued on next page)
 Table 16 (continued )

B. Dziejarski et al.
Zeolite BET surface Total pore Micropore Mesopore Si/Al ratio CO2 selectivity CO2 uptake, Adsorption Pressure, Reported modification Purpose of modification Reference
area, m2/g volume, volume, volume, at 1 bar mmol/g temperature, bar method


cm3/g cm3/g cm3/g C

2.96 25 Increasing basicity, affinity

K-Zeolite b 446 0.41 e e 7.4 14.70 3.57 0 1 between CO2 molecules- [529]
2.70 25 adsorbent surface
Li-Zeolite b 474 0.45 e e 7.4 20.00 3.08 0 1 [529]
2.39 25
Z-Y-3 819 0.33 0.32 e 2.25 e 2.59 30 1 Solid wastes as zeolite Reduction of production costs [530]
precursor (gasified rice husk)
Coal fly ash zeolites (CFAZ) 486 0.31 0.13 0.17 e e 3.02 0 1 Solid wastes as zeolite [531]
precursor
Zeolite 13X 643 e 0.35 e 3.0e5.0 e 5.07 25 1 Solid wastes as zeolite [532]
precursor (fly ash)
Fly ash zeolite (F) 414 0.251 0.188 e e e 4.16 50 e Solid wastes as zeolite Reduction of production costs; [533]
Fly ash zeolite (H) 39 0.138 0.016 e e e 1.2 50 e precursor; Enhancement of CO2 capture [533]
Fly ash zeolite (TS) 34 0.069 0.013 e e e 0.24 50 e Novel synthetic methodologies [533]
of synthesis
Zeolite 13X (13X-C) 588 e 0.240 e e e 6.9 25 1 Natural materials as zeolite Reduction of production costs [498]
6.3 35 precursor (kaolin, bentonite,
Zeolite 13X (13X-K) 591 e 0.250 e e 6.88 5.5 25 1 feldspar) [498]
6.2 35
Zeolite 13X (13X-B) 505 e 0.160 e e e 4.9 25 1 [498]
4.2 35
Zeolite 13X (13X-F) 472 e 0.140 e e e 3.9 25 1 [498]
3.2 35
C-13X 876 0.35 0.35 e e 26.00 6.18 25 1 Natural materials as zeolite [499]
B-13X 688 0.38 0.30 e e 37.00 4.80 25 1 precursor (bentonite) [499]
50

Silicalite-1/TOCNF/gelatin ~272 ~0.22 e e e e ~1.24 25 1 Materials based on the gelatin/ Composite/hybrid materials [534]
nanocellulose formation
Zeolite-Y/Chitosan 795 e e e e e 1.64 25 1 Chitosan biopolymer [535]
ZSM-5/Chitosan 444 e e e e e 2.39 25 1 [535]

Materials Today Sustainability 24 (2023) 100483

B. Dziejarski et al. Materials Today Sustainability 24 (2023) 100483

Fig. 31. The modification strategies and research directions of zeolites.

The CO2 uptake and textural properties of alumina-supported ad-

sorbents resulting from various modification approaches are sum-
marized in Table 17.

3.7. Metal oxides

One of the strategies for CO2 capture involves the utilization of

metal oxides as adsorbents. These materials, including calcium
oxide (CaO), magnesium oxide (MgO), titanium dioxide (TiO2), iron
oxides (FxOx), and their various combinations, can be directly
applied in a CO2-solid reaction to form metal carbonates (Fig. 34).
The choice of these particular metal oxides is deeply interrelated by
the objective of producing a thermodynamically stable carbonized
material as the end product [555]. Consequently, it is feasible to
thermally desorb CO2 molecules that have been adsorbed and then
regenerate the adsorbent. Carbonation reactions generally release
heat (exothermic), whereas carbonate breakdown reactions require
heat input (endothermic), enabling the establishment of a cyclic
process [556e559].

3.7.1. Titanium dioxide

Titanium dioxide has attracted considerable interest among
researchers due to its efficacy as an adsorbent, with distinctive
characteristics making it suited to a range of industrial and envi-
ronmental applications. Remarkably, it demonstrates a strong af-
finity towards CO2 [560], high adsorption capacity, and selective
adsorptions based on the size of absorbate molecules due to its
Fig. 32. Alumina phases used as support materials for CO2 adsorption. unsaturated surface atoms [332]. Hence, TiO2 has also been widely
51
B. Dziejarski et al. Materials Today Sustainability 24 (2023) 100483

utilized in the separation of CO2 from flue gas streams. Further- Regarding a potential CO2 composite adsorbent, Chowdhury
more, its significant surface area and tight range of pore sizes result et al. [332] studied mesoporous titanium dioxide/graphene oxide
in a shorter time period required to achieve adsorption equilibrium (TiO2/GO) nanocomposites using varying ratios of GO to TiO2 mass.
[561]. It is closely related to the high regularity in mesopore The material with the lowest GO to TiO2 mass ratio, due to its wide
channels with access to active sites, which significantly improves specific surface area (99.536 m2/g) and total pore volume
the diffusion rate, ensuring the rapid uptake of gas molecules (0.382 cm3/g), displayed the highest adsorption rate. The achieved
during adsorption [562]. maximum CO2 adsorption capacity was 1.88 mmol/g at 25
C and
Currently, titanium dioxide is primarily exploited as a catalyst, 1 bar, a value significantly surpassing that of various other CO2
giving rise to the development of new hybrid materials for CO2 adsorbents, including zeolite, activated carbon, and specific MOFs,
conversion processes. Research in this field mainly centers on the among others. Furthermore, the TiO2/GO composite exhibited rapid
photocatalytic reduction of CO2 into valuable chemical compounds, CO2 uptake kinetics and excellent CO2/N2 selectivity, suggesting its
such as solar fuels [563e569]. The literature has documented in- potential for further exploration in CO2 capture applications.
vestigations into the direct implementation of TiO2 for CO2 capture. Mixed oxides represent an alternative option for CO2 adsorption
These studies concern optimizing amine functionalization performance enhancement. Jeon et al. [556] synthesized
[332,570e575], incorporating phosphorus [576], and developing mixed oxides of mesoporous MgO/TiO2 containing spherical nano-
composite materials with other solid adsorbents. This leads to particles through a solegel process. Nitrogen adsorption/desorption
increased adsorption capacity and improved cyclic stability research demonstrated an increase in the surface area and total pore
compared to the parent materials [556,577,578]. volume of mixed MgO/TiO2 oxide, as well as the formation of
According to Ota et al. [575], while the wide variety of TiO2 bimodal pores. Because of this, the CO2 adsorption capacity of the
structures exist, including particulate, tube, rod, sheet, and MgO/TiO2 was found to be substantially higher (0.477 mmol/g at
sponge, there is relatively limited research comparing amine 25
C and 1 bar) compared to the individual pure oxides. Wu et al.
functionalization to other porous materials. This is due to a low [578] focused on the preparation of TiO2 coated nano CaO-based
concentration of OH groups on the surface of TiO2, which makes adsorbent. The results revealed a considerable increase in the
it challenging to achieve significant modifications with high endurance of the adsorption capacity. After 40 cycles of carbonation-
levels of amines. Consequently, the authors developed a tech- calcination, nano CaO-based adsorbent with an optimal TiO2 con-
nique to synthesize new amorphous TiO2 nanoparticles with a centration of 10% exhibited considerably more stable CO2 adsorption
diameter of 3 nm, a large surface area of 617 m2/g, and a higher capacity (5.3 mmol/g) than CaO without TiO2 coating (3.7 mmol/g).
concentration of OH groups. Compared to conventional TiO2, Fig. 35 compares the reported modification strategies and their
amorphous TiO2 nanoparticles treated with ethylenediamine related research directions for TiO2 in CO2 capture.
demonstrated a higher CO2 adsorption capacity (2.90 mmol/g at
0
C and 1 bar). The tuning of the ethylenediamine quantity 3.7.2. Iron oxides
bound to the particles enhanced their CO2 uptake without Iron oxides have been shown to possess exposed active sites on
impeding pore accessibility. their surfaces, capable of interacting with gaseous CO2 molecules

Fig. 33. The modification strategies and research directions of alumina-supported adsorbents.

52
 B. Dziejarski et al.
Table 17
Influence of modification strategies on textural properties and CO2 uptake of alumina-based adsorbents.

Alumina-based adsorbent Alumina support BET surface Total pore Average pore CO2 uptake, CO2 vol% Adsorption Pressure, Reported modification Reference
area, m2/g volume, diameter/width, nm mmol/g temperature, bar


cm3/g C

Alumina-aerogel/K2CO3 Alumina-aerogel 2019 6.3 8.3e9.5 7.20 e 56.1 e New synthesis approach and [542]
g-Alumina/K2CO3 g-Alumina 49.6 0.173 11.9e13.9 e e e e modification of the process [542]
conditions; Carbonates
functionalization
g-Alumina/K2CO3 g-Alumina 90 0.27 8.7 0.66 5 60 e Carbonates functionalization [545]
g-Alumina/K2CO3 g-Alumina 62.61 0.200 e 5.5 e e Comparison of the synthesis [543]
Boehmite/K2CO3 Boehmite 88.03 0.130 e e e e e approach; Carbonates [543]
Alumina-aerogel/K2CO3 Alumina-aerogel 188.66 0.212 e e e e e functionalization [543]
Activated alumina/K2CO3 Activated alumina 6.23 0.003 e 2.29 10 60 1 New synthesis approach; [544]
Activated alumina/K2CO3/15 wt% urea Activated alumina 10.62 0.004 e 3.10 10 60 1 Carbonates functionalization [544]
Mesoporous alumina/K2CO3 Mesoporous 87 0.11 6.7 2.82 2.33 e e New synthesis approach and [546]
alumina modification of the process
53

conditions; Carbonates
functionalization
Ordered mesoporous Al2O3 Mesoporous 305 0.33 e 1.69 e 0 1 New synthesis approach [547]
alumina
Mesoporous alumina/sodium Mesoporous 448.6 0.46 5.59 6.34 5 50 1 [548]
tripolyphosphate/chitosan alumina
Mesoporous alumina/Polymeric ionic Mesoporous g- 171.87 0.87 22.26 0.562 e 40 5 Ionic liquids functionalization [549]
liquids Al2O3
Mesoporous alumina/Bi-functionalized Mesoporous 91 0.16 5.85 2.02 e 25 1 [552]
ionic liquid alumina
Mesoporous alumina/Bi-functionalized Mesoporous 0.03 ~0 e 3.27 e 40 1 [554]
ionic liquid alumina
Mesoporous alumina/MgO Mesoporous 357 0.6 7.1 0.82 e 150 e Metal oxide functionalization [553]
alumina
Alumina-extracted residue/APTES Alumina-extracted 151.73 0.26 1.23 100 25 1 Amine functionalization ((3- [550]

Materials Today Sustainability 24 (2023) 100483

e
residue aminopropyl)triethoxysilane)
Activated alumina/NaOH Activated alumina 92.40 0.24 10.31 3.33 e 20 6 Metal hydroxide [551]
Activated alumina/KOH Activated alumina 103.02 0.25 9.83 2.97 e 20 6 functionalization [551]
B. Dziejarski et al. Materials Today Sustainability 24 (2023) 100483

this sector consumes a substantial quantity of fossil fuels and ac-

counts for approximately 7% of global CO2 emissions [581].
Unfortunately, the catalytic role of iron oxide in CO2 adsorption
and desorption has not been conclusively proved yet. The surface
interaction of iron oxide gradually revealed various carbonate
species, including monodentate carbonate, bidentate carbonate,
bicarbonate, and carboxylate [582]. In order to gain a deeper un-
derstanding of the CO2 adsorption mechanism, it is essential to
provide detailed explanations. Hakim et al. [582] studied CO2
adsorption and desorption properties using FeO, Fe2O3, and Fe3O4,
as absorbents, mainly due to the basicity and porosity of the
morphology. In the case of Fe2O3, the study revealed the presence
of various basic sites, including weak, medium, strong, and very
strong phases. Fe3O4, despite its potential for use in CO2 capture,
showed instability in adsorbing higher concentrations of carbon
dioxide, resulting in its oxidation to form Fe2O3. On the other hand,
among the other oxides, Fe2O3 exhibited the most significant in-
crease in BET specific surface area and the highest CO2 adsorption
capacity after undergoing four cycles of adsorption-desorption
(0.50 mmol/g). The authors concluded that enhancing CO2 cap-
ture efficiency can be achieved through chemical modification of
the Fe2O3 surface, either by increasing its basicity through the
addition of basic metal oxides or by optimizing the surface through
the use of appropriate support materials.
Fig. 34. Metal oxides explored as materials for CO2 adsorption in the literature. Recently, Mendoza et al. [583] presented a novel method for
capturing CO2 by mixtures of raw materials used in the steel in-
[579]. Iron-based solid sorbents offer several key advantages, dustry (Fe3O4 þ Fe and Fe2O3 þ Fe). Based on CO2 pressure and
including their accessibility, favorable thermodynamics, cost- planetary ball mill process parameters, they examined the kinetics
effectiveness, straightforward synthesis, abundance, and sus- of mechanically stimulated chemical reactions between iron oxides
tained adsorption capacity with slow degradation over time [580]. and CO2. By applying increased CO2 pressure (10e30 bar) and room
Iron oxides, especially, present an attractive option for CO2 capture temperature, it was assumed that total carbonation of iron oxides
in iron mills due to the potential for multiple cycles of carbonation may be accomplished. Under the same pressure, temperature, and
and regeneration within the same ironmaking facility, allowing for reaction time as the Fe2O3 and Fe system, the CO2 capture capacity
seamless integration with steel production processes. Furthermore, of Fe3O4 and Fe was 13.87 mmol/g, which was comparatively lower.

Fig. 35. The modification strategies and research directions of titanium dioxide-based adsorbents.

54
B. Dziejarski et al. Materials Today Sustainability 24 (2023) 100483

As a result of these findings, iron oxides are considered to be po-

tential and efficient reversible solid sorbents for CO2 capture.
The current research directions and modification strategies of
iron oxides are given in Fig. 36.

3.7.3. Magnesium oxide

The general adsorption mechanism on MgO is based on the
reversible interaction between CO2 molecules and O2 sites of
magnesium oxide, as presented in equation (8):

Mg  O þ CO2 /Mg  O$$$CO2ðadsÞ (8)

As a result, depending on the adsorption conditions and the

structure of solid surface, several types of complexes are formed,
such as bicarbonate, unidentate carbonate, and bidentate carbonate
[584e586]. Fast physisorption occurs at low temperatures, whereas
slower chemisorption takes place at high temperatures.
Initially, MgO was deemed unsuitable for high temperature CO2
capture applications due to its inherent drawbacks. They partly
include a limited practical CO2 adsorption capacity at elevated
temperatures due to restricted CO2 access to the internal cavities,
which is constrained by a small specific surface area and very
sluggish kinetics [587]. Furthermore, MgO-based adsorbents
frequently raise concerns about thermal stability since they require
very high temperatures during the desorption stage [588,589]. This
phenomenon is related to sintering processes taking place within
the adsorbent, leading to the formation of a carbonate termination
layer on the surface when the temperature surpasses a specific
threshold. Consequently, this leads to a decrease in surface area and
a decline in both CO2 capture performance and recyclability. Due to
these limitations, MgO-based materials are less cost-effective for
industrial applications [519,590].
Nonetheless, there is a growing interest in reevaluating the
suitability of MgO for CO2 adsorption, owing to its lower energy
consumption (<500
C) in comparison to alternatives like Li2O and
CaO [584,587], its affordability, abundant precursors, and ad- Fig. 36. The modification strategies and research directions of iron oxides-based
vancements in materials science. Furthermore, magnesium oxide adsorbents.
presents itself as a promising option for CO2 capture applications
owing to its distinctive attributes, such as appropriate surface ba-
sicity leading to the creation of oxygen vacancies that directly Fig. 37 illustrates the current status of modification strategies for
impact adsorption performance [591e595]. As a result, several in- MgO-based adsorbents, as well as future research directions.
vestigations have been conducted to improve efficient CO2 Further, the CO2 capture performance is summarized in Table 18
adsorption by MgO-based adsorbents, including their distribution and Table 19.
on porous supports, metal doping, using different synthesis
methods (precipitation method, double-replicate, aerogel method, 3.7.4. Calcium oxide
sol-gel method, and many others), influence of surfactants, effect of Calcium oxide has been widely investigated for CO2 adsorption
the magnesium precursors, amine functionalization, synthesizing due to its superior thermodynamic and chemical properties,
molten salt-modified MgO (alkali metal nitrate/carbonate), and enhanced regeneration capabilities, as well as its affordability and
mixed metal oxides. natural abundance in the form of carbonates like limestone and
Recently, Ruhaimi et al. [596] provided the most in-depth dolomite [628]. Furthermore, CaO offers durability, low toxicity,
analysis to date of the review on MgO-based adsorbents prepared recyclability of spent materials, environmental friendliness, the
through diverse modification strategies using different approaches potential for CO2 removal from flue gases in hydrogen generation
of synthesis and promoters. The authors suggested that merging processes, high reactivity towards CO2 across a broad temperature
innovative concepts and trends from other separation processes range of 500e900
C (allowing for heat recovery possibilities), and
could enhance the economic viability and optimization of pro- versatility in fluidized bed applications. Consequently, CaO has
moters in the adsorbent preparation. One approach could involve been a subject of research for many years [629e634]. The adsorp-
creating adsorbents with distinct morphological characteristics tion capacity of calcium oxide is affected by several parameters,
derived from biomass, along with the application of promoter including partial pressure of CO2, particle size, material
optimization techniques like spray coating and aerosol impaction- morphology, and precursor nature [519,635].
driven assembly. Moreover, inclusion of promoters, hybrid adsor- Upon exposure to elevated temperatures, CaO undergoes a re-
bents, and amine functionalization with the aid of a stabilizer may action with CO2 on its surface, involving the nucleation and growth
help to increase the cycle stability even further. It is also crucial to of CaCO3. The carbonation process of CaO can be divided into two
consider real-world industrial conditions, which often involve stages: a rapid phase controlled by kinetics, followed by a slower
gaseous impurities like NOx and SOx in the flue gas stream, as well phase controlled by diffusion [636]. Carbonation of CaO concludes
as the presence of moisture. once a layer of CaCO3 accumulates and forms over the unreacted
55
B. Dziejarski et al. Materials Today Sustainability 24 (2023) 100483

adsorbent. The carbonated sorbent can be regenerated through entrainment, and material attrition in some cases [630]. Extensive
calcination, leading to the restoration of CaO, which can be reused for research efforts have aimed to address these challenges related to
subsequent CO2 sorption. This approach, known as calcium looping, CaO as a CO2 adsorbent, focusing on improving its stability and
involves the cyclic utilization of CaO. The underlying chemisorption recyclability through a variety of techniques.
mechanisms during CO2 adsorption (carbonation) and desorption In 2018, Sun et al. [640] reviewed the progress in the develop-
(decarbonation/calcination) by CaO are shown below: ment and application of CaO-based adsorbents for CO2 capture and
Carbonation: provided an understanding of the basic elements of cyclic carbon-
ation/calcium in a systematic way. The authors identified four main
kJ strategies for enhancing CO2 uptake of CaO-based materials, which
CaOðSÞ þ CO2 4CaCO3ðSÞ DH ¼ 177:8 (9) include producing synthetic CaO with high surface area (employing
mol
diverse CaO precursors and refining synthesis techniques),
Decarbonation/calcination: dispersing CaO on inert supports (utilizing bimetallic metal oxides,
other metal oxides), applying surface modifications (using organic
kJ acids, mineral acids), and improving CO2 capture during rigorous
CaCO3ðSÞ 4CaOðSÞ þ CO2 DH ¼ þ177:8 (10)
mol calcination conditions. Furthermore, they identified several issues
Regrettably, the utilization of calcium oxide as a CO2 capture that need to be thoroughly addressed during the creation of novel
material presents several challenges, including the need for a high adsorbents. In terms of material stability, nanoparticles with a stable
energy input during regeneration (typically exceeding 800
C for framework and porous structure are critical. Additionally, new CaO-
CaCO3 decomposition), leading to sintering and mechanical based adsorbents are rarely evaluated under exceptional conditions,
degradation over successive cycles of CaO carbonation and calci- such as regeneration at 100% CO2, and the challenge of their attrition
nation [637]. Additionally, there is a decrease in carbonation ki- is infrequently reported. Another consideration is also whether the
netics after the initial layer of calcium carbonate forms on the oxide synthesis is both cost-effective and environmentally friendly.
surface, attributed to restricted CO2 diffusion (a rate-determining In the same year, Salaudeen et al. [628] discussed current ad-
step) [638,639]. Ultimately, complications also arise from the vances in metal-based solid sorbents with a particular focus on
structure of high-specific surface area CaO powder during calcium oxide and presented the use of biomass as competitive
adsorption processes, resulting in increased pressure drop, flow sources of CaCO3. This review showed that adsorbent hydration is

Fig. 37. The modification strategies and research directions of magnesium oxide-based adsorbents.

56
B. Dziejarski et al. Materials Today Sustainability 24 (2023) 100483

an efficient method for regenerating and optimizing multiple re-

Reference
action cycles. Furthermore, while the stability of CaO-based solid

[597]
[598]
[599]
[600]
[601]
[602]
[603]
[604]

[605]
[606]
[607]
[608]
sorbents has been described in literature in the presence of various
inert supports or dopants, the fundamental mechanisms of this
phenomenon are not yet fully comprehended. To gain a deeper
understanding of the principles and potential factors that impact

Direct calcination (effect of moisture)

Extrusion-spheronisation technique
the relationship between sorbent performance and inert support,
Description of synthesis method

Hydrothermal method (effect of

further research is needed. Concerning the utilization of biomass as

One-pot hydrothermal method

Solution-combustion method
Solid state chemical reaction
a precursor for calcium oxide production, animal shell waste
emerges as a potential source. However, conflicting results exist
Flame aerosol method
regarding the comparative advantages of calcined shells versus
Precipitation method

calcined limestone. Addressing this discrepancy might require

Double-replicate
Aerogel method

Urea hydrolysis
Sol-gel method

further experimentation and the application of kinetic modeling.

surfactants) Numerous other studies have also highlighted the potential value of
waste biomass. Recently, Nawar et al. [641] exploited waste egg-
shells to synthesize modified structure CaO through the use of
organic acids, demonstrating that eggshells could serve as a cost-
effective option for CO2 adsorption.
Pressure,

In the field of novel research directions in CaO-based materials,

there is a discernible increase in the attention being given to the
bar

1
1
1
1
1
1
1
1

1
1
1
1

wide exploration of biomass and industrial residues as potential

sources for CaCO3 and support materials. Moreover, the addition of
temperature,
Adsorption

anionic surfactants, or the amine functionalization during synthe-

sis, appears to be a promising approach for enhancing the charac-
teristics. Finally, the impact of process conditions, particularly the
120
100
300

200
200
232
25
25
30
30
60

25
C
An overview of textural properties and CO2 capture performance of magnesium oxide-based adsorbents synthesized via various methods.

influence of moisture on the CO2 capture efficiency, is being

extensively investigated.
CO2, vol %

10þH2O

Fig. 38 illustrates the existing improvement strategies and

ongoing research pathways for CaO-based adsorbents for CO2
100
100
100
100

100
100

100
30

10
40
e

adsorption. Table 20 provides an overview of the performance of

CaO-based adsorbents in CO2 capture applications, categorized
CO2 uptake, mmol/g

based on the main modification strategies employed.

3.7.5. Cerium oxide

Cerium oxide, also referred to as ceria, has been extensively
0.681

0.602

studied and has garnered significant attention within the field of

1.56
1.82
2.34

1.49
0.73
2.61
0.83

1.18
2.39

0.39

catalysts and catalytic supports [658]. Ceria demonstrates distinc-

tive attributes in relation to its structural and thermal properties.
Average pore size (nm)

These characteristics encompass extensive accessible surface area,

rigid frameworks, notable interaction with CO2 molecules at
ambient conditions (exhibiting Lewis-base active site properties),
orderly distribution of pore sizes, substantial capacity for oxygen
storage, and straightforward redox reaction [659e663].
12.12

Numerous efforts have been made to enhance the catalytic ac-

7.06

4.90

4.11

2.19

1.84
5.2

9.9
e

e
e

tivity of ceria by increasing its thermal stability and surface area

5

through the use of organized porous structures. The interaction of

volume, cm3/g

cerium oxide with carbon dioxide has also been thoroughly char-
Total pore

acterized [664e667]. However, despite ceria's ability to adsorb and

0.0289

desorb CO2 under ambient conditions, its practical application in

0.575

0.414
0.823
0.53
2.11

0.32
0.36

0.38
0.67

CO2 capture hasn't been adequately investigated, particularly in

0.3

terms of adsorption capacity and the influencing factors.

In 2014, Yoshikawa et al. [668] detailed the synthesis and
BET surface
area, m2/g

analysis of cerium oxide-based adsorbents, providing the first

coherent measurement of CO2 uptake. The authors investigated CO2
5.71
331
250
686
350
177
123
130
321

372
100
33

capture materials derived from various single metal oxides (SiO2,

Al2O3, ZrO2). CeO2 exhibited the highest CO2 adsorption capacity,
achieving 0.132 mmol/g at 50
C, along with its specific surface area
Irregular plateletlike MgO-A

Mesoporous leaf like MgO

of 166 m2/g. Furthermore, the experimental results have revealed

MgO-based adsorbent

Lamellar shaped MgO

essential insights into the factors that play a significant role in

Thin sheet-like MgO
MgO nanoparticles

influencing the number of available CO2 adsorption sites as well as

Foam-like MgO
Leaf-like MgO

the overall CO2 uptake of metal oxide materials. It was emphasized

Rod-like MgO

Nanosheets

Pellet-MgO
Meso-MgO

that these encompass synthesis conditions, precursor choices that

MgO-SC

could introduce surface contaminants hindering CO2 adsorption,

Table 18

MgO

and material attributes including morphology, particle sizes,

porosity, and surface area.
57
 B. Dziejarski et al.
Table 19
A summary of the modification strategies applied to magnesium oxide-based adsorbents and their impact on textural properties and CO2 adsorption uptake.

MgO adsorbent BET surface Total pore Average pore CO2 uptake, CO2, vol % Adsorption Pressure, Description of promoter used in Reported modification Reference
area, m2/g volume, cm3/g size (nm) mmol/g temperature, bar modification


C

Mesoporous MgO 95.8 0.22 9.09 6.25 100 350 10 e e [609]

Mesoporous MgO 250 0.53 4.3 1.81 100 25 1 Mesoporous carbon obtained from Effect of the magnesium [598]
mesoporous SBA-15 precursor
MgOeFe 15.85 0.1387 9.20 0.90 e 25 1 Fe Metal doping [608]
MgOeNi 30.83 0.1588 4.20 1.50 e 25 1 Ni [608]
MgO-mPC 306 0.156 2.03 5.45 100 80 e Mesoporous carbon Distribution on porous supports [610]
MgO-OMC 598.9 0.58 2.20 2.09 100 25 1 Mesoporous carbon [611]
MgO (20 wt%)-RHA 39.5 0.12 e 4.56 10 200 e Biomass wastes (rice husk ash) [612]
MgO (20 wt%)/MCM-41 390 0.27 2.24 1.06 100 25 1 Mesoporous silica [613]
Mesoporous carbon supported MgO 421 0.40 3.8 1.68 e 25 1 Mesoporous carbon derived from [614]
biomass
MgO/g-Al2O3 225.5 0.52 3.41 2.10 10 60 1 g-Al2O3 [615]
MgO/Al2O3 200.91 0.60 17.3 0.97 13 60 1 Al2O3 [557]
PAC4/15%MgO 1623 1.43 3.53 3.86 10 25 1 Biomass-derived activated carbon [616]
58

MgO/Al2O3 200.91 0.60 17.3 1.36 13 60 1 Al2O3 Distribution on porous [557]

supports; Moisture effect
PAC4/10%MgOe5%Al2O3 1605 1.33 3.31 4.50 10 25 1 Biomass-derived activated carbon; Distribution on porous [616]
Al2O3 supports; Mixed metal oxides
formation
Ordered mesoporous MgO/carbon 355.6 0.22 2.7 3.08 e 0 1.2 Carbon spheres Composite formation [617]
spheres composites
MgOeZrO2 180 e 5e10 1.15 100 300 1 ZrO2 Mixed metal oxides formation [618]
MgO/CaO 21.4 0.173 38.4 9.49 20 650 1 CaO [619]
MgO/FeO 177 0.20 3.0 0.795 14 200 1 FeO [620]
MgeNa double salts 1.26 e e 3.48 100 375 1 Na2CO3 Synthesis of molten salt- [621]
(Li0.3Na0.6K0.1)NO3$MgO 65.8 0.438 e 16.8 100 300 1 LiNO3, NaNO3, KNO3 modified MgO [622]
MgO-[(Li0.44K0.56)NO3]2[(Na0.5K0.5)CO3] e e e 19.06 100 325 1 KNO3, LiNO3, K2CO3, Na2CO3 [623]
MgOeNaNO2 16 e e 15.7 100 350 1 NaNO2 [624]
MgOeNaNO3 67 0.29 11.2 10 260 1 NaNO3 [625]

Materials Today Sustainability 24 (2023) 100483

e
MgOeCaCO3 29.9 0.16 26.1 13.18 100 350 1 CaCO3 [626]
TEPA-MgO 19 0.22 1.9 4.98 40 30 1 Tetraethylenepentamine Amine functionalization [627]
APTES-MgO 134 0.301 9 1.49 100 30 1 (3-Aminopropyl)triethoxysilane [600]
DETA-MgO 91 0.203 9 1.08 100 30 1 Diethylenetriamine [600]
PEI-MgO 72 0.178 10 0.54 100 30 1 Polyethylenimine [600]
B. Dziejarski et al. Materials Today Sustainability 24 (2023) 100483

Fig. 38. The modification strategies and research directions of calcium oxide-based adsorbents.

In 2015, Li et al. [669] studied mesostructured ceria and ceria Fig. 39 presents an up-to-date overview of the current modifi-
doped with Mg, Zr, La, and Cu for CO2 adsorption prepared using a cation strategies and research trends of CeO2-based adsorbents.
surfactant-templated method and tested at room temperature. The
findings indicated that the adsorption characteristics of the mate- 4. Techno-economic analysis (TEA) of CO2 capture materials
rials are influenced not only by their textural properties but also by
their surface chemistry, including acidebase sites and oxygen va- A CO2 sorption-based process utilizing the efficient and cost-
cancies. These aspects are affected by the type and content of effective adsorbents has the potential to yield significant techno-
dopants in the CeO2. logical and economic advantages. In line with ongoing theoretical
In 2017, Slostowski et al. [670] investigated the potential of CeO2 and practical research, there appear to be distinct categories of
nanoparticles as CO2 adsorbents in the form of nanopowders, materials exhibiting remarkable CO2 capture capabilities. Primarily,
focusing on their specific surface area. This method resulted in a newly synthesized materials intended for industrial applications
solid sorbent with a specific surface area of 199 m2/g. Additionally, must demonstrate efficacy within specific technological regenera-
it showed a maximum CO2 adsorption capacity of approximately tion configurations (in terms of pressure, temperature, electricity,
1.13 mmol/g at 25
C and 1 pressure. The possibility of cycling CO2 or combined cycles) and in various gasesolid contactors (such as
adsorption/desorption was also explored. Initial research indicated fixed, fluidized, moving, or rotating beds). This assessment is
the feasibility of adsorbing CO2 at 25
C and nearly completely pivotal, as it ultimately determines whether a technology based on
regenerating the material at 150
C in an inert gas environment a particular adsorbent type can be economically viable for CO2
without compromising the CO2 capture capability. Therefore, CeO2 capture from flue gas in power plants. Integrated capture and
with substantial specific surface areas hold great promise as po- separation processes incur the most costs, making careful analysis
tential candidates for low-temperature reversible CO2 capture imperative prior to scaling up and introducing the technology at
materials in the future. manufacturing scale. Consequently, in order to facilitate a system-
In 2020, Azmi et al. [671] further elaborated on the amine func- atic and equitable comparison of CO2 separation technologies, and
tionalization (APTMS) of mesoporous ceria nanoparticles (MCN) for to comprehensively understand the techno-economic impacts
CO2 capture. The introduction of APTMS functional groups onto MCN associated with implementing CO2 capture systems across diverse
enhanced the availability of CO2 binding sites, evident through the industries, techno-economic analysis is extremely essential.
formation of carbamate species upon CO2 interaction with the NH In many cases of TEA, it's important to adopt a real model of a
groups. As a result, the adsorption capacity increased by up to tenfold coal-fired power plant at a specific scale, proportionally reflecting
compared to the pristine oxide. However, the addition of APTMS to the electricity generation rate. This is closely associated with the
the MCNs led to a reduction in their textural properties. This amount of fossil fuel consumption and, consequently, the resulting
decrease is attributed to the functionalization and blocking effect of CO2 emissions into the atmosphere. The Emissions and Generation
APTMS molecules within the MCN support. Resource Integrated Database (eGRID) of U.S. EPA (Environmental
59
 Table 20
A summary of the modification strategies applied to calcium oxide-based adsorbents and their impact on textural properties and CO2 adsorption capacity.

B. Dziejarski et al.
Calcium oxide-based Methods BET surface Total pore Average Carbonation conditions Calcination conditions Number of CO2 uptake Material Improvement Reference
adsorbents. area, m2/g volume, pore (adsorption) (desorption) implemented mmol/g strategy
cm3/g size cycles to test
T,
C Atmosphere t, min T,
C Atmosphere t, min
(nm) adsorbent

CaO-based pellets e 15.6 0.063 e 650 15% CO2 (N2 balance) 20 850 100% N2 120 e 11.4 Powdered Introduction of [642]
limestone various CaO
CaO-based carbide Bubbling methods ~11.3 e e 750 100% CO2 60 900 100% He 90 15 14.09 Carbide slag precursor [643]
sledge
Eggshell-Ca(OH)2eCaO Calcination 84.37 0.25 7.6 700 100% CO2 10 900 100% CO2 5 10 14.32 Eggshell waste [644]
CaO Sol-gel method e e e 650 15% CO2 (N2 balance) 15 800 100% N2 10 20 11.59 CaO by solegel Improvement [645]
process of synthesis
CaO-gemini surfactant Precipitation 16.3 0.059 14.5 600 15% CO2 (N2 balance) e 850 e e 5 6.59 Sodium dodecyl method [646]
method sulfate (SDS)
surfactant
CaO-SDS surfactant Precipitation 9.4 0.036 15.0 600 15% CO2 (N2 balance) e 850 e e 5 6.14 Gemini surfactant [646]
method
Mn-promoted CaO Sol-gel method 17.72 0.0222 4.88 600 100% CO2 60 700 100% H2 60 10 15.43 Mn Dispersing CaO [647]
CaO/Y2O3 Solegel 25 0.115 e 650 20% CO2 (N2 balance) 30 900 100% N2 5 10 11.1 Y2O3 on inert [648]
combustion supports
method
CaO/Ca9Al6O18 Citric acid method 958 0.85 5 600 20% CO2 (N2 balance) 20 850 100% N2 10 100 13.64 Al2O3 [649]
Mesocellular siliceous e 12.9 0.06 e 700 100% CO2 30 900 100% N2 15 5 4.00 Mesocellular [650]
foam (MCF)- siliceous foam
supported CaO
CaO/KIT-6 Non-ionic 2.9 0.007 e 600 15% CO2 (N2 balance) 30 800 100% N2 10 10 7.6 Mesoporous silica Dispersing CaO [651]
surfactant (KIT-6) on inert
templating method supports
CaO/Ca12Al14O33 Hydrothermal 9.2 0.08 e 500 15% CO2, 47% H2O (N2 10 920 21% CO2, 3 40 4.77 Al2O3 [652]
method balance) 78% H2O (N2
60

balance)
CaO/Ca12Al14O33 Sol-gel method 13 0.09 e 750 50% CO2 (N2 balance) 6 750 100% N2 e 30 7.05 Al2O3 [653]
nanoCaO/CaTiO3 Coating method 6.13 e 10.15 600 20% CO2 (N2 balance) 10 750 100% N2 10 40 5.3 TiO2 [578]
CaO/MgO Wet mixing e e e 650 15% CO2 (N2 balance) 15 850 100% N2 10 50 9.09 MgO [633]
combustion
synthesis
CaO/Ca12Al14O33- Precipitation 17 0.0035 8.42 600 15% CO2 (N2 balance) e 850 e e 5 7.05 Al2O3 [646]
gemini surfactant method
Charcoal-supported Sol-gel method 63.6 0.166 10.45 600 15% CO2 (N2 balance) 25 650 100% N2 30 10e30 15.1 Charcoal [654]
CaO (1:4 mass ratio)
Charcoal-supported Wet impregnation 18.0 0.044 9.88 600 15% CO2 (N2 balance) 25 650 100% N2 30 10e30 5.7 Charcoal [654]
CaO (1:4 mass ratio) method
Al-doped CaO Precipitation 12 0.066 e 650 14.9% CO2, 3.6% O2, 20 900 100% N2 5 30 5.4 Al2O3 [655]
method 8.8% H2O (N2 balance)
CaO/NiO Sol-gel combustion 12.8 0.11 750 15% CO2 (N2 balance) 25 5% H2 (N2 20 15.0 NiO [656]

Materials Today Sustainability 24 (2023) 100483

e e e
method balance)
Ca1Ni0.1Ce0.017 Sol-gel combustion 22.5 0.20 e 750 15% CO2 (N2 balance) 25 e 5% H2 (N2 e 20 14.2 NiO, CeO Dispersing CaO [656]
(molar ratio) method balance) on inert
Ca1Ni0.1Ce0.033 Sol-gel combustion 20.7 0.14 e 750 15% CO2 (N2 balance) 25 e 5% H2 (N2 e 20 14.1 NiO, CeO supports [656]
(molar ratio) method balance)
Formic acid-modified e 2.91 0.0071 6.82 650 15% CO2 (N2 balance) 20 850 100% N2 5 20 13.63 Formic acid Surface [657]
(10 vol%) CaO-based modification
adsorbent
Citric acid-modified e 5.23 0.022 2.134 650 15% CO2 (N2 balance) 5 850 100% N2 5 20 8.64 Citric acid [641]
(10 vol%) CaO
Acetic acid -modified e 4.45 0.021 6.126 650 15% CO2 (N2 balance) 5 850 100% N2 5 20 ~8.41 Acetic acid [641]
(10 vol%) CaO
Formic acid -modified e 9.38 0.023 2.368 650 15% CO2 (N2 balance) 5 850 100% N2 5 20 ~8.41 Formic acid [641]
(10 vol%) CaO
PDA-CaO Calcination 62.56 0.40 12.6 700 100% CO2 10 900 100% CO2 5 10 14.09 Pyridine [644]
dithioethylamine
B. Dziejarski et al. Materials Today Sustainability 24 (2023) 100483

the size and shape of adsorption columns. Finally, optimization of

the Pareto front demonstrated that the productivity index is
affected by factors such as the volume of zeolite 13X and the metal
used in forming the adsorption columns.
Subraveti et al. [675] also conducted a TEA analysis for post-
combustion CO2 capture with cyclic process. Their goal was to
determine the cost limitations of PVSA cycles assuming the creation
of a 'perfect' cost-free adsorbent. Employing various carbon dioxide
compositions and industrial flue gas flow rates as inputs, the re-
searchers enhanced adsorbent characteristics (such as adsorption
isotherms and particle morphology) and process design parame-
ters. The objective aimed to examine the lowest possible CO2
avoidance cost, excluding CO2 conditioning, transport, and storage
expenses. The obtained results revealed insights into the CO2
concentration in the flue gas significantly influencing the cost
limitations of PVSA. The lowest potential CO2 avoidance costs
decrease as the CO2 concentration increases. By applying a four-
step PVSA cycle and altering the pelletized adsorbent's
morphology, CO2 avoidance costs can be reduced by 9e22%. Opti-
mization highlighted that 'ideal' adsorbents for achieving the
lowest CO2 avoidance costs have reasonably linear CO2 adsorption
isotherms and minimal N2 adsorption. The flue gas flow rate
notably impacts the complexity of the PVSA plant in terms of train
Fig. 39. The modification strategies and research directions of cerium oxide-based numbers, equipment, piping, and space requirements. The ultimate
adsorbents. cost of CO2 avoided for PVSA varied from 87.1 to 10.4 V/tonne,
corresponding to CO2 feed concentration of 3.5e30 mol%. When
Protection Agency) released in 2018, revealed that natural gas units compared with a monoethanolamine-based absorption method,
have an average CO2 emission rate of 407 kg/MWh, while coal units the findings indicated that PVSA could be a potentially
have an average CO2 emission rate of 989 kg/MWh [672]. Hanak favorable separation technique for flue gas streams with high CO2
and Manovic [673] determined the technical and economic feasi- concentrations.
bility of a CO2 capture system utilizing a molecularly imprinted PSA technique has also been explored to assess its viability for
polymer sorbent based on acrylamide (MIP) within the context of recovering CO2 from post-combustion power plant flue gases. In
retrofitting a 580 MW coal-fired power plant. The cost of CO2 2008, Ho et al. [676] used commercial adsorbents, including zeolite
avoided was calculated to be 29.3 £/ton of CO2. This performance, 13X with a working capacity of 2.2 mol/kg and a CO2/N2 selectivity
compared to a CO2 capture system employing chemical solvents, of 54, to evaluate high-pressure feed and vacuum desorption in
exhibited superior techno-economic viability. Parametric studies their analysis. By utilizing vacuum desorption, the capture cost was
indicated that the sorbent capacity had the most significant impact reduced from 57 to 51 $/tonne of CO2 avoided. With this method,
on the thermodynamic performance of the polymer. Furthermore, both an 85% CO2 recovery rate and a product that was 46% CO2
the economic performance was influenced not only by the sorbent enriched were achievable. Moreover, the authors found that when
capacity but also significantly by its cyclic performance. The anal- combining the novel adsorbent with enhanced processing cycles
ysis findings demonstrated a linear relationship between the cost of like depressurization, adsorber bed equalization, and product
CO2 avoided and increasing MIP sorbent makeup, at a rate of 6.8 purging, a CO2 avoidance cost as low as 30 $/tonne could be
£/tCO2 for each one-tenth percent increase in sorbent makeup. attainable.
As mentioned earlier in this review, there are several regener-
ation technologies that are commonly employed during the CO2
capture process, including PSA, VSA, VPSA, TSA, TPSA, and ESA. 4.1. Techno-economic analysis (TEA): principles and procedures
Zanco et al. [674] prepared a comparative techno-economic
evaluation for the post-combustion CO2 capture process based on Given the technological solutions discussed, a solid grasp of
mature technology for CO2 separation, such as adsorption using key engineering data is imperative for multiple aspects, including
zeolite 13X in conventional fixed beds (either VSA or TSA). The the development of CO2 capture materials, designing installations
analysis assumed a carbon dioxide source emitting 12% CO2 v/v for CO2 removal from flue gas at pilot or industrial scales (through
(with 95% relative humidity at the inlet conditions of 30
C and computer simulations and numerical methods), and especially
1.3 bar) to produce a CO2 stream with 96% purity. Techno-economic conducting techno-economic analyses. As briefly mentioned
assessment revealed that while the studied adsorption process earlier regarding the future prospects of CO2 adsorbents, these
might achieve cost competitiveness on a small scale, particularly include the working and equilibrium capacity of beds within a
for very low recovery rates and small plant sizes, overcoming a specific temperature, pressure, and absorbate concentration range
significant cost gap is necessary to establish the adsorption process in flue gas mixtures. Isothermal and kinetic data derived from
as economically viable. Notably, cost components related to flue gas mathematical models analyzing experimental points are relevant.
pre-drying contribute significantly to this disparity. In this context, Mass transfer considerations during the process, along with
innovative water-resistant adsorbents combined with more com- identification of diffusion mechanisms that govern the adsorption
plex process configurations could potentially reverse the observed process (surface diffusion, boundary layer effects, and adsorbate
cost trends. Furthermore, the research highlighted that the unit diffusion within the internal porous structure of material), are
cost of the commercial adsorbent has a considerably lower impact crucial. Additionally, the thermodynamics of adsorption and
on investment costs compared to geometric constraints related to characteristics of the adsorbent particles within the bed, as well as

61
B. Dziejarski et al. Materials Today Sustainability 24 (2023) 100483

the impact of impurities (such as NO2, SO2, H2S) or moisture in the  Cycle time of the CO2 capture process, which defines the time
flue gas undergoing separation, should be considered. When these required for effective CO2 adsorption and desorption to enable
details are verified as integral components of the overall pro- efficient adsorbent reuse. This factor has an immediate impact
cedure, the technical and economic phase of the analysis can on productivity.
commence. The most crucial engineering data for conducting TEA  Cycle scheduling, given that adsorption cycles often employ
are depicted in Fig. 40. multiple beds for CO2 capture and separation. This parameter
In addition to carbon dioxide capture technologies and cyclic involves effectively managing the cycle of each bed within the
adsorption methods, the choice of bed is also pivotal within TEA. installation to meet process requirements.
When selecting a bed for a specific technology, its functionality  Vacuum pump curves, vital for adsorption processes involving
must be carefully analyzed. The utilization of a fluidized bed vacuum regeneration stages like VPSA. Vacuum pump perfor-
intensifies mass exchange between the gas mixture flowing mance can vary across changing operating conditions.
through its structure and the solid particles, owing to a sub-  Mechanical design considerations, where determining funda-
stantial interface and effective mixing of the material with the mental mechanical aspects of the process equipment design,
gas phase. This acceleration enhances the adsorption process particularly the thickness of the adsorption columns, is neces-
[677,678]. However, the efficacy of gas mixture contact with the sary during the TEA stage.
bed during fluidization can be compromised, especially by the  Evaluation of energy requirements, noting that in
agglomeration of bed solids at higher temperatures, resulting adsorption processes, heat input is noticeable during thermal
from van der Waals intermolecular forces for physical adsorption regeneration steps in processes like TSA. Additionally, blowers,
[679,680]. This phenomenon leads to material heterogeneity, compressors, and vacuum pumps demand energy for processes
characterized by crack and channel formation in the structure. like VPSA.
These channels allow the gas phase to bypass adsorbent parti-  Emphasis on the understanding that scaling and equilibrium
cles, rendering the equilibrium of CO2 adsorption ineffective models should not be used for detailed process design or cost
[681,682]. In contrast, an adsorbent in the form of a fixed bed estimation. Instead, they are more aptly suited for deliberate
possesses a compact structure with specific internal and external selection to identify the most promising adsorbents.
surfaces and consistent pore morphology. This directly impacts
the material's adsorption capacity during the process, resulting In terms of process economics, the authors emphasized the
in a higher concentration of adsorbent solids compared to a importance of several key aspects. These include IBL costing
fluidized bed. However, adsorption on a fixed bed also presents methods (Inside Battery Limits), which focus on the primary pro-
challenges, including undesirable heat gradients, process control cess equipment items involved in converting the feed into the final
complexities, and, crucially, difficulties in regeneration during product. The authors also highlighted the significance of novel
CO2 desorption. technologies. For instance, fluidized beds for moving bed TSA and
In 2021, Danaci et al. [683] published guidelines for TEA on rotary adsorbers for continuous TSA are being explored for
adsorption processes, categorizing them into two main sections: adsorption processes. Additionally, estimating the cost of the
technical and economic issues. The aforementioned engineering adsorbent, particularly when it's not yet commercialized, can be
data forms an integral part of this determination. In each section, contentious, underscoring the importance of concentrating on
the authors presented key factors with substantial influence, along scale-up considerations. Lastly, the concern of other capital costs
with the consequences of decisions made during the TEA phase and completes the spectrum of factors.
recommended practices. Among these factors, parameters of the Overall, a significant objective of TEA studies is to develop cost-
bed type were highlighted for comprehensive consideration effective process equipment designs tailored to the physical and
throughout the procedure and as a reference point for the covered chemical properties of the adsorbent. Moreover, the wide array of
topics. Regarding technical considerations, they highlighted regeneration technologies available in different modes, process con-
essential aspects that demand attention, as follows: ditions, reactor configurations, and types of adsorbents offers sub-
stantial potential for process enhancement. In a broader sense, given
 Feed flow rates of CO2 must be accurately determined for their affordability, widespread availability, and versatility across
appropriate sizing and calculation of process equipment com- various applications, CO2 capture materials emerge as an intriguing
ponents, process design, and economic assessment. These cal- choice for CCUS technologies. Furthermore, key aspects related to
culations should reflect the actual flow rate in the specific scaling up and the barriers that require addressing for the successful
application. commercialization of a given adsorbent have been highlighted.

Fig. 40. Essential engineering data for techno-economic analysis.

62
B. Dziejarski et al. Materials Today Sustainability 24 (2023) 100483

5. Summary and future directions  Emphasize materials with highly developed specific surface
area, mesoporosity, and microporosity to improve CO2 adsorp-
This review thoroughly addresses the latest modification tion kinetics and equilibrium working capacity.
strategies, scientific advancements, and future research di-  Select the most suitable adsorbent type for specific industrial
rections concerning selected CO2 capture materials under applications, considering synthesis approach, material cost,
investigation at various scales. These solid CO2 adsorbents production process, life cycle evaluation, and modification
exhibit considerable potential for CO2 removal from flue gas, strategies.
offering advantages over traditional liquid amine absorption  Improve resistance of materials to moisture, NOx, and SOx in flue
methods in terms of regeneration energy efficiency and cost- gas by investigating long-term effects and concentrations of these
effectiveness. However, they also confront certain limitations factors, especially for zeolites,silica-based adsorbents, and MOFs.
and challenges that need to be overcome before they can be  Study the close interaction and influence of water vapor and
scaled up for diverse industrial applications, defining the specific impurities on CO2 uptake, essential for optimizing CO2 removal
knowledge gaps for each material type. Among the existing ad- from flue gases.
sorbents, critical parameters for improvement include working  Develop a research reference path for mature adsorbent types,
adsorption capacity, reduced production costs, cycle longevity, covering process conditions, preparation, and chemical charac-
thermal stability, resistance to moisture and impurities, and teristics, applicable to novel and innovative materials.
durability across multiple cycles. To achieve technologically and  Focus on reducing textural degradation during adsorption and
economically viable systems, novel porous materials with desorption operations, particularly for metal oxides, to enhance
modified strategies have been developed to enhance CO2 capture thermal stability.
capabilities significantly. This emphasizes the importance of  Conduct CO2 capture tests under real flue gas conditions, such as
collecting data on factors influencing effective adsorption system low pressure, high temperature, certain moisture levels, or us-
design, an aspect warranting special attention. In-depth analysis ing different types of adsorbent beds.
of these factors enables a more accurate portrayal of carbon di-  Research well-known and new materials for composite syn-
oxide adsorption behavior on individual materials, identifying thesis, contributing to a comprehensive database and selection
parameters impacting performance such as temperature, CO2 of modification strategies.
concentration or partial pressure in the flue gas, thermodynamic  Investigate natural materials, biomass residues, and industrial
attributes of the process, controlling mass transport rates, waste as raw materials for cost-effective CO2 capture material
textural properties of the adsorbent bed (specific surface area, synthesis, aligning with waste management and circular econ-
chemical properties, porosity, pore volume), moisture and im- omy principles.
purity levels in the flue gas stream, and thorough theoretical  Explore biomass as a support material for enhancing the
evaluations. Furthermore, scrutinizing these criteria for a specific dispersion of metal oxides in modification processes.
adsorbent application can yield cost reductions in CO2 capture.  Create a comprehensive engineering data database for specific
Additionally, adsorbents are routinely evaluated for their capac- material groups to enhance TEA analysis.
ity, selectivity, and regenerability across multiple cycles. Under-  Develop general guidelines for CO2 capture materials within
standing their mechanisms, which precisely elucidate the suitable process condition ranges (temperature, pressure, gas
interactions between adsorbent and adsorbate, as well as CO2 concentration, desired CO2 purity), application types (pre-
storage within their structures, is crucial. An approach to address combustion capture, post-combustion capture, and oxy-fuel
this involves integrating structural, sorption equilibrium, ki- combustion), textural properties, and performance criteria.
netics, spectroscopic, and thermodynamic studies with molecu-  Utilize techno-economic analysis to compare promising adsor-
lar simulations and modeling of adsorption equations. This bents for industrial purposes, outlining criteria specific to
combination validates theoretical assumptions and offers valu- different material groups, technological variants, scalability, and
able insights for facilitating their scalable implementation. stability costs.
Another crucial aspect of this review lies in the techno-economic
analysis of various CO2 capture materials in practical applica- In summary, the considerations presented in this review
tions, a topic extensively discussed. The results unequivocally demonstrate clear trends in CO2 capture materials research and
highlight the promise and necessity of such analyses in assessing modifications, evident from the substantial number of published
the actual viability of adsorbent use across industries. Within papers between 2017 and 2021. Various types of CO2 adsorbents,
each section of the TEA, specific criteria are essential consider- including carbon-based materials, amine-based materials, MOFs,
ations during its execution. silica, zeolites, alumina, and polymers, have been developed to
In conclusion, this paper highlights several performance in- varying degrees. When comparing their developmental paths and
dicators and outlines directions for future research activities in the research trends, certain commonalities and patterns emerge, sug-
field of CO2 capture materials, as follows: gesting the relevance of a generic approach to sorbent develop-
ment. The general approach for creating novel CO2 capture
 Simplify the synthesis process to reduce production costs, materials is shown in Fig. 41. A prominent research trend involves
shorten preparation time, and facilitate parameter analysis the utilization of waste biomass and industrial residues as raw
affecting adsorbent characteristics. materials, aligning with green synthesis principles. This calls for a
 Explore existing synthesis methods to identify optimal condi- detailed analysis of their thermochemical conversion to obtain in-
tions, parameters specific to adsorbent groups, and innovative termediates like biochar or hydrochar, characterized by specific
material structures for enhanced CO2 uptake. elemental composition and solid phase percentages. Furthermore,
 Enhance new synthesis methods that utilize affordable raw the activation process plays a crucial role in enhancing specific
materials and chemicals, significantly lowering production costs surface area and porosity. Another notable research avenue is the
(e.g., waste biomass, industrial byproducts). functionalization of amines, a widely adopted technique exten-
 Focus on environmentally friendly synthesis approaches using sively documented in literature. Adsorbents modified through this
ecologically safe solvents to minimize ecological impact and approach exhibit comparable CO2 uptake values to materials with
energy consumption. more time-consuming and costly synthesis procedures. Another
63
B. Dziejarski et al. Materials Today Sustainability 24 (2023) 100483

Fig. 41. The generic research paths for the development of novel CO2 capture materials.

research direction involves the creation of hybrid materials based Data availability
on diverse adsorbents, yielding unique properties for CO2 adsorp-
tion from flue gases. In conclusion, a key recommendation and No data was used for the research described in the article.
knowledge gap in CO2 capture materials research is the combina-
tion of the aforementioned methodologies. References

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