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Environmental Research: Dechen Jiang, Zhilong Cao, Bochao Zhou, Guanyu Gong, Zeying Huang, Chao Wang

This study evaluates the environmental impact of incorporating waste plastics into asphalt mixtures, focusing on VOCs emissions and health risks. It finds that while waste plastics can enhance road performance and reduce total VOC emissions, certain types and dosages can also increase hazardous emissions. The research highlights the need for careful selection and optimization of waste plastic types to balance performance and environmental safety in road engineering.

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0% found this document useful (0 votes)
15 views10 pages

Environmental Research: Dechen Jiang, Zhilong Cao, Bochao Zhou, Guanyu Gong, Zeying Huang, Chao Wang

This study evaluates the environmental impact of incorporating waste plastics into asphalt mixtures, focusing on VOCs emissions and health risks. It finds that while waste plastics can enhance road performance and reduce total VOC emissions, certain types and dosages can also increase hazardous emissions. The research highlights the need for careful selection and optimization of waste plastic types to balance performance and environmental safety in road engineering.

Uploaded by

nasir khan
Copyright
© All Rights Reserved
We take content rights seriously. If you suspect this is your content, claim it here.
Available Formats
Download as PDF, TXT or read online on Scribd

Environmental Research 279 (2025) 121642

Contents lists available at ScienceDirect

Environmental Research
journal homepage: [Link]/locate/envres

Environmental impact assessment of waste plastic modified asphalt


mixtures: VOCs emission characteristics, environmental-health risks, and
underlying mechanism
Dechen Jiang , Zhilong Cao *, Bochao Zhou , Guanyu Gong , Zeying Huang , Chao Wang
Department of Road & Railway Engineering, Beijing University of Technology, Beijing, 100124, China

A R T I C L E I N F O A B S T R A C T

Keywords: Incorporating waste plastics into asphalt mixtures offers dual benefits of enhancing performance and reducing
Asphalt mixture white pollution, while also necessitating consideration of their environmental impact. This work quantitatively
Waste plastic investigated the effects of waste high-density polyethylene (wHDPE), polyvinyl chloride (wPVC), and poly­
VOCs emissions characteristics
propylene (wPP) plastics on volatile organic compounds (VOCs) emissions and associated environmental-health
Environmental and health impact
Road performance
risks of asphalt mixtures prepared via the dry method under simulated paving conditions, with mechanistic
insights into the impacts. Results revealed that waste plastics could improve high-temperature and water sta­
bility. Meanwhile, these selected waste plastics can effectively reduce the total VOCs concentrations of asphalt
mixture, with a maximum inhibition rate of 36.72 % by wPP. Alkanes and aldehydes (81.41 % of total VOCs)
were decreased by over 30 %. Meanwhile, wPP was the most effective in reducing environmental and health
impacts, achieving up to 39.7 %, 33 %, and 27.7 % inhibition of ozone formation potential, secondary organic
aerosol formation potential, and cancer risk, respectively. However, the addition of wPVC and high-dose wHDPE
increased hazardous emissions such as benzene series and halogenated hydrocarbons due to thermal degradation
under high temperature. These findings underscore the importance of waste plastic type/dosage optimization to
address performance-environmental trade-offs, providing valuable guidance for sustainable waste plastic reuse in
road engineering.

1. Introduction the compatibility between the plastic and asphalt (Chavez et al., 2019;
Xu et al., 2021). Waste plastic is added directly to the mixture either as a
Plastic products have brought numerous conveniences to people’s substitute aggregate or a modifier to enhance the performance of the
daily lives. However, the widespread use of plastic products has caused a mixture in the dry process method (Angelone et al., 2016). This method
series of environmental pollution (Khoaele et al., 2023). The plastic can facilitate the application and promotion of waste plastic in road
crisis has become a pressing subject requiring urgent resolution (Pan engineering applications due to its straightforward procedure (Li et al.,
et al., 2020; Sharma and Bansal, 2016). Against this backdrop, the 2021; Ashish et al., 2023).
technology of waste plastic modified asphalt material has garnered Polypropylene (PE) was used as a modifier in asphalt mixtures,
significant attention in the field of road engineering (Dawodu et al., achieving fatigue and rutting resistance comparable to SBS modified
2023; Abdy et al., 2022). There are generally two methods for incor­ asphalt mixture (Cardone et al., 2022). Recycled polyvinyl chloride
porating waste plastic into asphalt materials: the wet process and the dry (PVC) from drainage pipes was widely used to increase the viscosity and
process (Biswas et al., 2020). In the wet process, waste plastic is added stiffness of the asphalt, which improved its rutting resistance (Cheng
directly to the asphalt before mixing with aggregates. It undergoes et al., 2019). Polyethylene terephthalate (PET) has a significant recy­
physical and chemical interactions with asphalt at elevated tempera­ cling volume, primarily from beverage bottles. Various dosages of PET
tures for a period of time (Costa et al., 2013). Asphalt mixtures prepared (2 %, 4 %, 6 %) were added to reclaimed asphalt mixtures at the level of
using the wet method typically require higher mixing temperatures and 20 %, 30 %, and 40 %. Among these, a combination of 4 % PET com­
greater energy consumption, while also necessitating consideration of bined with 30 % reclaimed asphalt achieved optimal Marshall stability

* Corresponding author.
E-mail address: zhilongcao@[Link] (Z. Cao).

[Link]
Received 28 December 2024; Received in revised form 4 April 2025; Accepted 16 April 2025
Available online 8 May 2025
0013-9351/© 2025 Elsevier Inc. All rights are reserved, including those for text and data mining, AI training, and similar technologies.
D. Jiang et al. Environmental Research 279 (2025) 121642

(Hayat et al., 2020). However, the enhancement effect of waste plastics themselves at elevated temperatures. Thus, analyzing the variations in
on asphalt mixture performance exhibits dose dependency. Although a VOCs emissions from asphalt mixtures solely based on total concentra­
certain dosage of HDPE effectively improves Marshall stability, exces­ tions may not be appropriate, and more refined analytical methods are
sive plastic content induces detrimental consequences. The plastic oc­ required. Additionally, the incorporation of waste plastics significantly
cupies aggregate voids and forms surface coatings after melting, thereby influences the emission characteristics of VOCs from asphalt mixtures.
reducing the mixture’s optimal binder content and compromising The relationship between the VOCs emissions from waste plastics
Marshall stability (Heydari et al., 2021). It is reported that increasing themselves and the abrupt changes in the concentration of certain VOCs
polyethylene content reduces the maximum flexural tensile strain of from waste plastic modified asphalt mixture needs to be thoroughly
modified asphalt mixtures, correlating with diminished investigated. It is crucial to assess the environmental friendliness of their
low-temperature crack resistance. To address this performance limita­ applications in road engineering.
tion, the introduction of waste rubber as a composite modifier has The objective of this study is to investigate the implications of
proven effective. The PE/CR modified system achieves maximum various waste plastics on the emission characteristics of asphalt mixture
bending strain values comparable to conventional SBS-modified asphalt, VOCs, considering both environmental and health impacts while
demonstrating successful mitigation of low-temperature performance ensuring road performance. The relationship and influence mechanisms
degradation (Zhang et al., 2019). Therefore, meticulous optimization of between waste plastics and the VOC emission characteristics of modified
both waste plastic dosage and material type selection is imperative for asphalt mixtures were also elucidated in this paper. First, the influence
achieving enhanced road performance in asphalt mixtures. of varying dosages of different waste plastics on the road performance of
Waste plastics can indeed enhance mixture performance, while their asphalt mixtures was discussed to optimize their dosages. Then, the
impact on VOCs emissions behaviors and the associated environmental compositional structure before and after high-temperature treatment
and health risks of asphalt mixture VOCs also require careful attention and VOCs emissions characteristics of waste plastics at high tempera­
(Li et al., 2020). Recent studies have demonstrated that the addition of tures were examined. The goal was to elucidate the correlation and
waste plastics to asphalt could reduce the total concentration of VOCs. underlying mechanisms between the structural composition of waste
Gas emissions from waste plastic-modified asphalt mixtures were plastics and their VOCs emission behaviors under elevated thermal
investigated under different temperatures and plastic contents. Waste conditions. Finally, the impact of waste plastics on VOCs emissions from
LDPE (low-density polyethylene), PP, and HDPE showed the ability to asphalt mixture was investigated at multiple levels. A range of indicators
absorb VOCs, with adsorption efficiencies up to 78 % (Boom et al., was also used to assess the environmental and health benefits of
2022a). The mechanism by which plastics reduce VOCs was briefly different waste plastic modified asphalt mixtures. This study provides
explored in some studies. The low crystallinity and hydrophobicity of insights into the selection of waste plastic modifiers for asphalt mixtures
plastics contributed to their ability to reduce VOCs emissions. The in terms of both pavement performance and environmental and health
presence of amorphous regions resulted in a higher specific surface area. impacts, thereby providing a basis for the design of eco-friendly waste
Consequently, these provided more adsorption sites for VOCs (Wang plastic asphalt mixtures.
et al., 2020; Sojitra et al., 1995). However, some studies indicated that
the concentration of specific VOCs increased following the addition of 2. Materials and methods
certain types of waste plastics. For instance, an increase in the content of
waste ABS (acrylonitrile butadiene styrene) in binder led to higher 2.1. Materials
benzene concentrations (Boom et al., 2022b). This also suggests that the
suppression of total VOCs concentration of asphalt mixture VOCs by 2.1.1. Waste plastics
waste plastics does not necessarily imply that they effectively inhibit all Three different types of waste plastics were utilized in this study. All
VOC groups. Other studies have found that in VOCs produced from rABS three plastics were purchased from waste plastic treatment plants, with
modified asphalt mixture, components such as tetrachloroethylene and a particle size of 200 mesh. The known information for three waste
styrene posed negligible non-carcinogenic health risks to workers. plastics is presented in Table 1.
However, benzo[a]pyrene and dibenz[a,h]anthracene would cause
serious risks to workers exposed to asphalt fumes (Boom et al., 2023). 2.1.2. Asphalt and aggregates
This indicated that the inhibitory effects of waste plastics on the envi­ SK-90 asphalt was selected as the raw asphalt binder in this study. Its
ronmental health risks posed by VOCs components are markedly basic physical properties are listed in Table 2. AC-16 was chosen as the
different. Therefore, asphalt mixture VOCs represent a complex system. target grading for the asphalt mixture. The grading curve is shown in
The reduction of the total VOCs concentration due to waste plastics does Fig. 1.
not imply the reduction in the concentration of all gaseous components
and their associated environmental health hazards. It is necessary to
conduct a multi-level and detailed study on the concentration of VOCs 2.2. Preparation of waste plastic modified asphalt mixture
released from waste plastic modified asphalt mixtures.
Previous studies have found the polymer chains of plastics could The dry method was used to prepare asphalt mixtures. Aggregates
undergo thermal degradation under high temperatures, resulting in the were weighted according to the mix design, they were preheated to
production of low molecular weight hydrocarbons and gaseous 175 ◦ C and held for 2h. The raw asphalt binder was heated to a molten
byproducts (Yamashita et al., 2009). Due to the varying compositions of state at 160 ◦ C. Initially, aggregates and a specified proportion of waste
different plastics, the gaseous by-products they released at high tem­ plastic were introduced into a preheated mixing bowl and stirred for 90s
peratures also differed (Pajaro-Castro et al., 2014). High-density poly­
ethylene released higher amounts of aldehydes and alkanes during Table 1
heating, whereas polyvinyl chloride emitted benzene series and chlori­ Basic information on waste plastics.
nated hydrocarbons (Lomonaco et al., 2020). Additionally, plastics that Types of plastics Samples Density (g/ Source
have been used for extended periods release higher and more complex ID cm3)
concentrations of VOCs compared to their original state (Cabanes et al., Waste high-density wHDPE 0.97 Fuel tank
2020). Toxic and harmful compounds such as toluene, ethylbenzene, polyethylene
and benzaldehyde were generated during the artificial use of plastics Waste polyvinyl chloride wPVC 1.12 Sewer pipe
(Moghe et al., 2015). Overall, waste plastics have the ability to reduce Waste polypropylene wPP 0.90 Food insurance
box
asphalt mixture VOCs. However, they also release some VOCs

2
D. Jiang et al. Environmental Research 279 (2025) 121642

Table 2 180 ◦ C for 30min. Powdered samples were mixed with potassium bro­
Fundamental physical properties of raw asphalt binder. mide (KBr) and pressed into transparent KBr pellets, the sample surface
Item Penetration (25 ◦ C, 0.1 Softening point Ductility (15 ◦ C, was pressed against the ATR crystal to collect the infrared spectrum.
mm) (◦ C) cm) Spectra were collected in the range of 4000-400 cm− 1, with 32 scans per
Test 89 48 120 sample at a resolution of 4 cm− 1.
value Quantitative analysis was performed using the peak areas within the
range of 4000 -400 cm− 1 (the total spectrum peak area) as a reference to
compare the peak area ratios of characteristic functional groups in this
study. The ratio of the peak area of characteristic functional groups,
defined as the functional group index, is given by Eq (1).
/∑
Ix = Ax A (1)

where, Ix represents the functional group index of a specific functional


group. Ax denotes the peak area of that functional group measured in the
infrared spectrum. ΣA is the sum of the peak areas within the 4000 to
400 cm− 1 range.

2.3.3. Collection of waste plastics VOCs


The setup for collecting VOCs from waste plastics is shown in Fig. 2.
10g of waste plastic was placed in a three-neck flask, which was then
heated to 180 ◦ C using an electric heating mantle and maintained at this
temperature for 30min. Subsequently, VOCs were collected at a constant
Fig. 1. The grading curve of asphalt mixture.
flow rate of 1.2 L/min until the Teflon airbag was filled. During this
process, a thermometer was placed on the surface of the waste plastic to
at 180 ◦ C. Subsequently, molten base asphalt was gradually added and
monitor the temperature.
mixed for another 90s. Finally, mineral filler was added and stirred for
90s, then waste plastic modified asphalt mixture could be obtained. The
2.3.4. Collection of asphalt mixture VOCs
composition and label of each waste plastic modified asphalt mixture are
Different types of prepared asphalt mixtures in a loose state were
shown in Table 3.
placed into the VOCs collection apparatus at 180 ◦ C. A 30-min timer was
started upon achieving equipment temperature stabilization. VOCs were
2.3. Testing and characterization methods collected using Teflon bags at a constant rate of 1.2 L/min after the 30-
min timer ended. The VOCs collection device for asphalt mixture is
2.3.1. Road performance test of waste plastic modified asphalt mixture shown in Fig. 3.
The water stability of the waste plastic modified asphalt mixture was
evaluated by the immersion Marshall residual stability (MS0) and the 2.3.5. VOCs monitoring method
tensile strength ratio (TSR) obtained by the water immersion Marshall Gas Chromatography-Mass Spectrometry (GC-MS) was employed to
test and freeze-thaw splitting test. High-temperature stability was monitor and analyze VOCs from asphalt mixtures and plastics in this
assessed through the dynamic stability (DS) obtained by the rutting test, study. The parameter settings for the pre-concentration system were as
while low-temperature cracking resistance was evaluated by the follows: the cold trap adsorption temperature was − 20 ◦ C, the cold trap
maximum flexural strain (εB) obtained by the low-temperature bending desorption temperature was 260 ◦ C, the transfer line temperature was
test. The preparation and performance testing of asphalt mixtures 150 ◦ C, and the injection valve temperature was 120 ◦ C. The ion source
strictly adhered to the standard test methods for asphalt and bituminous temperature was set at 240 ◦ C. The temperature program started with an
mixtures in highway engineering. (JTG-E20-2011) (Ministry of Trans­ initial isothermal hold at 40 ◦ C for 10 min, followed by a ramp of 10 ◦ C/
port of the People’s Republic of China, 2011). The road performance of min to 290 ◦ C, and then held for 5 min. The gas sampling flow rate was
the waste plastic modified asphalt mixtures was evaluated through 50 mL/min. Certified calibration standards were used for the qualitative
parallel testing in accordance with standard specifications, and the re­
sults met all normative requirements.

2.3.2. Fourier Transform Infrared Spectroscopy (FT-IR) analysis method


Fourier Transform Infrared Spectroscopy (FT-IR) was used to analyze
the chemical composition of the samples. This study conducted infrared
spectroscopy tests on waste plastic samples before and after heating at

Table 3
The composition and code of each waste plastic modified asphalt mixture.
Composition Label Composition Label

Raw asphalt mixture SK-M Asphalt mixture with wPVC0.3


0.3 %wPVC %-M
Asphalt mixture with wHDPE0.25 Asphalt mixture with wPVC0.35
0.25 %wHDPE %-M 0.35 %wPVC %-M
Asphalt mixture with wHDPE0.3 Asphalt mixture with wPP0.25
0.3 %wHDPE %-M 0.25 %wPP %-M
Asphalt mixture with wHDPE0.35 Asphalt mixture with wPP0.3 %-M
0.35 %wHDPE %-M 0.3 %wPP
Asphalt mixture with wPVC0.25 Asphalt mixture with wPP0.35
0.25 %wPVC %-M 0.35 %wPP %-M
Fig. 2. The waste plastic VOCs collection apparatus.

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D. Jiang et al. Environmental Research 279 (2025) 121642

shows the opposite trend. All modified mixtures exceed the 75 % tech­
nical requirement, where 0.25 % wHDPE provides a notable increase in
TSR by 26.9 %. Adding waste plastics to asphalt mixtures initially in­
creases their dynamic stability (DS), but further increases in plastic
content reduce stability. The DS of wHDPE0.35 %-M and wPVC0.35
%-M is lower than that of the raw asphalt mixture. The optimal per­
formance is observed with 0.25 % wHDPE, which boosts the DS by 29.5
%. All modified mixtures meet the minimum standard of 1000 times/
mm. For low temperature performance, lower dosages of wHDPE
improve the maximum flexural strain (εB) substantially by 57.2 %,
showcasing the best deformation resistance. However, this beneficial
effect decreases with increasing dosage, and while higher dosages of
wPVC and wPP increase the flexural strain, the enhancement is less
significant.

Fig. 3. The asphalt mixture VOCs collection apparatus.


3.2. Characteristics of VOCs emissions from waste plastics

and quantitative analysis of VOCs, establishing a VOCs database that 3.2.1. FT-IR of waste plastics
includes 85 different components (Gong et al., 2024). These components The infrared spectra and functional group indices of the three waste
were divided into the following groups according to their chemical plastics before and after high temperature treatment are shown in Figs. 5
properties.: alkanes, alkenes, aldehydes, ketones, benzene series, halo­ and 6, respectively. Except for the peak around 3400 cm− 1 and 1600
genated hydrocarbons, and others. For asphalt mixture VOCs emission cm− 1, the relative intensity of other characteristic peaks in the infrared
testing, each waste plastic-modified asphalt mixture sample was spectra of waste plastics decreases after high-temperature treatment.
analyzed in duplicate, each test was conducted independently, to avoid This trend indicates that the associated chemical bonds are degraded
cross-contamination. The coefficient of variation for VOCs measure­ during heating. A characteristic peak appears at 3400 cm− 1, indicating
ments was maintained below 15 %, ensuring data reliability. the presence of the hydroxyl groups in the samples. The increased
relative intensity of the O-H bond is typically attributed to oxidative
2.3.6. Environmental health impact assessment method of waste plastic reactions. The peak around 1600 cm− 1 associates with C=C stretching
modified asphalt mixtures VOCs vibrations. Its appearance likely arises from the rupture and rear­
The ozone formation potential (OFP) and secondary organic aerosol rangement of polymer chains. It results in the formation of unsaturated
formation potential (SOAFP) were used to assess the environmental bonds. The peak at 872 cm− 1 for wHDPE and wPVC is due to C-Cl bond
impact of VOCs from asphalt mixtures. Hazard index (HI) and cancer vibrations, while for wPP, it is due to C-H vibrations. Halogenated
risk (R) were employed to evaluate health risks. The calculation for­ compounds typically exhibit stronger peak than C-H in their infrared
mulas for these four indicators are provided in Eq (2)–(5) in Table 4. spectra (Wu et al., 2023). This peak is more pronounced in the spectra of
Where VOCsi represents the concentration of the ith VOCs compo­ wHDPE and wPVC compared to wPP, and there is a notable shift in the
nents. MIRi is the maximum incremental reactivity of that component. intensity of these peaks after high temperature treatment. The peaks
SOAPi is the secondary organic aerosol potential of that component. RfDi around 2920 cm− 1 of all three plastics are attributed to C-H stretching
is the reference dose of that component. SFi is the slope factor for that vibrations. A peak near 1425 cm− 1 is typically associated with CH2
component. bending vibrations. The peak observed around 1750 cm− 1 in all three
plastics is attributed to C=O stretching vibrations.
3. Results and discussions
3.2.2. Concentration of waste plastics VOCs
3.1. Road performance of waste plastic modified asphalt mixtures A total of 49 components are detected in the VOCs generated by
wHDPE after high-temperature treatment, while wPVC and wPP yield
The integration of waste plastics into asphalt mixtures affects their 43 and 42 components, respectively. The total concentration and group
road durability, but the impact varies depending on the type and amount proportion of VOCs released by three waste plastics are shown in Fig. 7.
of plastic used. The basic road performance of waste plastic-modified Under identical experimental conditions, wHDPE generates the widest
asphalt mixtures is illustrated in Fig. 4. The road performance values variety of VOCs components and the highest VOCs concentration at 1.14
are shown in Table 5. In terms of water stability, the immersion Marshall mg/m3 under high temperatures known in Fig. 8, primarily consisting of
residual stability (MS0) decreases with increasing contents of wHDPE alkanes, olefins and aldehydes, which together account for over 85 % of
and wPP, whereas an opposite trend is seen with wPVC. Notably, 0.25 % its total concentration. The concentration of VOCs released by wPVC is
wPP enhances the immersion residual stability of the asphalt mixture by the second highest at 1.10 mg/m3, predominantly composed of benzene
33.5 %. The inclusion of waste plastics increases the tensile strength series and halogenated hydrocarbons, which collectively account for
ratio (TSR) of the asphalt mixtures. However, this improvement trend over 85 % of the total concentration. In contrast, wPP emits the lowest
diminishes with increasing addition of wPVC and wPP, while wHDPE total VOCs concentration at 0.38 mg/m3. Benzene series, ketones, and
aldehydes each comprise about 25 %, yet due to the overall lower
concentration, their absolute levels are relatively modest. It is note­
Table 4 worthy that the monomers for HDPE, PVC, and PP are ethylene, vinyl
Calculation method of environmental health impact assessment index.
chloride, and propylene, respectively. It has been found through analysis
Evaluation indicators Calculation formula that various types of waste plastics release the gaseous derivatives of the
OFP OFP =

(VOCsi ×MIRi ) (Wang et al., 2023) (2) above chemical compositions under high temperature conditions. For
SOAFP SOAFP =

(VOCsi ×SOAPi ) (Chen et al., 2023) (3) instance, wPVC exhibits detectable levels of components such as 1,1-
HI HI =

VOCsi /RfDi (Tong et al., 2019) (4) dichloroethylene and 1,2-dichloroethylene in their emitted VOCs.
R

(5)
Components like acrolein and cis-1,3-dichloro-1-propene are presented
R= (VOCsi ×SFi ) (Khoshakhlagh et al., 2023)
in VOCs emitted from wPP.

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D. Jiang et al. Environmental Research 279 (2025) 121642

Fig. 4. Road performance of waste plastic modified asphalt mixtures.

Table 5
Results of road performance tests of waste plastic modified asphalt mixtures.
MS0/% TSR/% DS/times/mm εB/με
SK-M 85.6 84.6 1532.8 2477
wHDPE0.25 %-M 87.6 107.3 1985.3 3894.8
wHDPE0.3 %-M 79.8 96.4 1611.4 2786.1
wHDPE0.35 %-M 76.9 94.3 1433.2 2511.2
wPVC0.25 %-M 93.8 91.3 1852.1 2489.9
wPVC0.3 %-M 96.4 105.2 1752.3 2527.5
wPVC0.35 %-M 99.7 108.5 1287.3 2896.3
wPP0.25 %-M 114.3 92.4 1843.6 2663.3
wPP0.3 %-M 99 103.5 1628.3 2819.4
wPP0.35 %-M 89.5 104.9 1611.7 3300

Fig. 6. Characteristic peak functional group index of different waste plastics


before and after high temperature treatment.

waste plastics’ chemical structure, the release of certain VOCs can be


attributed to oxidative degradation and chemical structural changes
during high-temperature treatment.

1) C=C bond

The appearance of the C=C bond at 1600 cm− 1 after high tempera­
ture treatment in the infrared spectra of all waste plastics indicates the
emergence and reaction residue of unsaturated hydrocarbons. The
presence of C=C bonds provides an implication for the formation of
VOCs belonging to the benzene series.

2) C=O bond

The formation of ketones and aldehydes after high-temperature


treatment of plastics is closely related to the intensity change of C=O
Fig. 5. The infrared spectra of the three waste plastics before and after high bonds during heating. The oxidation and decomposition of the material
temperature treatment. during high-temperature processing lead to the emission of these two
types of groups. Additionally, it is likely that all three types of plastics
3.2.3. Correlation analysis between the chemical structure of waste plastics contain plasticizers, such as dioctyl phthalate (DOP), which has a sig­
and their VOCs emission characteristics nificant amount of C=O groups in its chemical structure.
Combined with the analysis of VOCs and the characterization of

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D. Jiang et al. Environmental Research 279 (2025) 121642

Fig. 7. The total concentration and group proportion of VOCs released by three waste plastics.

chain. These double bonds can further react to conjugated double-bond


systems, which would extend into long-chain conjugated systems with
the effect of continued heating. This process leads to the darkening of
the material and may ultimately result in the formation of the benzene
series.
Reaction of dehydrochlorination.

[-CH2-CH(Cl)-]n → CH2=CH-CH=CH2 + nHCl

Aromatization of unsaturated intermediates.

CH2=CH-CH=CH2 → C6H6

CH2=CH-CH=CH2 + CH3Cl → C6H5CH3 + HCl

C6H6 + CH2=CH2 → C6H5CH2CH3 + HCl


Fig. 8. Components concentrations of different waste plastics VOCs.

3) C-H bond
3.3. Characteristics of VOCs emissions from waste plastic modified
Contacting sections 3.2.1 and 3.2.2, the generation of alkanes and asphalt mixtures
benzene series under high temperature conditions may be closely
related to the intensity reduction of C-H bonds from waste plastics. Based on the above discussion, the detected VOCs in different waste
During high-temperature pyrolysis, plastics decompose into lower mo­ plastics show significant differences, which would impact the compo­
lecular weight hydrocarbons, including alkenes and alkanes. Long-chain sition of VOCs in waste plastic modified asphalt mixtures. The influence
alkanes may undergo cracking and rearrangement, resulting in the for­ of various waste plastics on the VOCs emission characteristics of asphalt
mation of benzene series. mixtures is investigated in this chapter.
For example, the dimerization reaction to generate butene.
3.3.1. Concentration of total VOCs
2 CH2=CH2 → C4H8
The total VOCs concentration and the inhibition rates of various
The cyclization reaction generates benzene. asphalt mixtures are shown in Fig. 9. The total VOCs concentration of
the raw asphalt mixture is 2.56 mg/m3. Each type of waste plastic ex­
6 CH2=CH2 → C6H6 + 3H2 hibits a certain inhibitory effect on the total VOCs concentration. It is
attributed to the low crystallinity and hydrophobicity of the plastics, as
4) C-Cl bond well as their large specific surface area (Barletta et al., 2019). The VOCs

The significant presence of halogenated hydrocarbons is observed in


the VOCs released from wHDPE and wPVC, its concentration is not high
in the VOCs released by wPP. This also corroborates the hypothesis that
the presence of C-Cl bonds exists in wHDPE and wPVC. The degradation
or pyrolysis of wHDPE and wPVC at high temperatures may result in the
formation of halogenated hydrocarbons from partial chloride ions and
organic compounds.
For example, considering chlorinated hydrocarbons, the reaction
path for their formation is as follows.

R-CH2-CH2Cl → R-CH(Cl)-CH2R’ + HCl

Additionally, the substantial release of the benzene series may be


related to the relative intensity change of the C-Cl and C-H bonds before
and after high temperature treatment. At high temperatures, the C-Cl
bonds break first, generating hydrogen chloride gas. After the loss of
HCl, unsaturated double bonds (-CH=CH-) are formed in the polymer Fig. 9. Total VOCs concentration of asphalt mixtures and inhibition efficiency
of waste plastics.

6
D. Jiang et al. Environmental Research 279 (2025) 121642

concentration decreases with the increasing content of wPVC and wPP.


Although the addition of wHDPE could reduce the VOCs concentration,
0.35 % wHDPE shows a weaker inhibitory effect compared to 0.25 %
wHDPE. This may be related to the higher concentration and complexity
of VOCs released by wHDPE at elevated temperatures. The 0.35 % wPP
shows the best inhibitory effect on VOCs, with an inhibition efficiency of
36.72 %.

3.3.2. Concentration of asphalt mixture VOCs groups


Alkanes and aldehydes are the predominant groups of the raw
asphalt mixture VOCs, accounting for over 80 % of the total VOCs from
Fig. 10. The changes in VOCs groups concentrations caused by waste
plastics and their inhibition rates are shown in Fig. 11. The different
types and dosages of the plastics show remarkable selectivity in the
suppression of different VOCs groups. Specifically, 0.35 % wPP shows
the highest suppression effect on all groups except halogenated hydro­
carbons and others, the emission reduction efficiency is more than 30 %.
The addition of 0.25 % wHDPE is the most effective technique in
reducing halogenated hydrocarbons, with an inhibition efficiency of
11.6 %. 0.35 % wPVC is the most effective material among them in
inhibiting the other category by 41.6 %.
For wHDPE, 0.25 % wHDPE exhibits better suppression of VOCs
groups compared to 0.35 % wHDPE, except for the benzene series and
the other categories. Additionally, 0.35 % wHDPE has a negative effect
on the suppression of halogenated hydrocarbons, its concentration is
increased by 11.7 %. For wPVC, the concentrations of other VOCs groups
decrease with increasing wPVC content except for benzene series and
halogenated hydrocarbons. The inclusion of wPVC has a significant
negative impact on the concentration of halogenated hydrocarbons,
with 0.25 % and 0.35 % wPVC increasing its concentration by 69.2 % Fig. 11. The changes of VOC group concentrations caused by waste plastics.
and 123.7 %, respectively. Additionally, 0.35 % wPVC substantially
increases the concentration of the benzene series by 64.8 %. 0.25 %
wPVC has a slightly smaller effect, increasing the concentration by 11.9
%. wPP demonstrates the most effective suppression of asphalt mixture
VOCs groups. It is consistent with the finding on the total VOCs con­
centration. Moreover, the suppressive effect on each VOCs group be­
comes more pronounced with increasing wPP content. These results can
be related to the discussion of waste plastic VOCs in Section 3.2. The
poor suppression effect of wHDPE and wPVC on certain VOC compo­
nents can be attributed to the VOCs released from the waste plastics
themselves.

3.3.3. Concentration of asphalt mixture VOCs components


The component concentrations of VOCs from different asphalt mix­
tures are illustrated in Fig. 12. Waste plastics can inhibit most asphalt
mixture VOCs components in varying degrees. Except for 0.35 % Fig. 12. Components concentrations of different waste plastic modified asphalt
mixtures VOCs.

wHDPE, all other waste plastics can suppress more than 85 % of the
asphalt mixture VOCs components. 0.25 % and 0.35 % wPP demonstrate
the highest efficacy by 96.47 %. In contrast, 0.35 % wHDPE only ach­
ieves a VOCs components inhibition coverage rate of 74.12 %.
The utilization of 0.35 % wHDPE and wPVC deserves attention. As
shown in Table 6, the incorporation of 0.35 % wHDPE shows negative
impact on the concentration inhibition of 21 types of VOCs components.
0.35 % wHDPE provides a certain reduction in the total concentration of
the asphalt mixture VOCs. There are still 20 types of VOCs components
whose concentrations, while lower compared to the raw asphalt
mixture, are higher than those found from wHDPE0.25 %-M. Two po­
tential reasons for this phenomenon are conjectured. First, the waste
plastics may not have been adequately mixed within the asphalt
mixture, thus failing to fully exhibit its inhibiting properties. More
importantly, the experiments in Section 3.2 also show that wHDPE re­
leases a rich variety of VOCs with high concentration at high tempera­
Fig. 10. The concentration and proportion of the raw asphalt mixture tures. 0.35 % wPVC shows a significant negative effect on the inhibition
VOCs groups.

7
D. Jiang et al. Environmental Research 279 (2025) 121642

of certain components. For instance, the concentration of benzene in­


creases from 6.5 × 10− 4 to 1.3 × 10− 2, 1,2-dichloroethane increases

Trans-1,3-dichloro-

dichloro-1-propene
1-propene, Cis-1,3-
from 8.1 × 10-4 to 8.5 × 10− 3, and chlorobenzene increases from 1.5 ×

wPP0.35 %-M

Methacrolein
10− 3 to 5.5 × 10− 3 after the addition of 0.35 % wPVC. The underlying
cause of these issues may be attributed to the release of benzene series
and halogenated hydrocarbons from wPVC itself at sustained elevated
– temperatures. Additionally, PVC exhibits lower thermal stability



compared to PP and PE due to the presence of chlorine atoms. The study

Trans-1,3-dichloro-

dichloro-1-propene
1-propene, Cis-1,3-
of Section 3.2 indicates that waste plastics release gaseous derivatives of
their own at elevated temperatures. At the same time, these specific
wPP0.25 %-M

Methacrolein components have also been observed in the detection of waste plastics
VOCs. Combined with the above analysis, conducting component anal­
ysis of VOCs at the components level suggests that the anomalous un­



dulation of VOCs concentration is attributable to the inherent
composition of the waste plastics themselves.
1,1-dichloroethylene, Dichloromethane, 1,2-

Monobromodichloromethane, 1,2-Dibromo­
3.4. Environmental and health risks of waste plastic modified asphalt
Benzene, O-ethyltoluene, Diethylbenzene

mixtures VOCs
dichloroethylene, 1,2-dichloroethane,

Two environmental risk indicators (OFP and SOAFP), along with two
health risk indicators (HI and R) are utilized to quantify the environ­
mental and health benefits of waste plastic modified asphalt mixtures.
ethane, Chlorobenzene
Methyl tert butyl ether

The environmental and health impact indicators of asphalt mixtures are


depicted in Fig. 13. The incorporation of waste plastics in asphalt mix­
wPVC0.35 %-M

tures shows the inhibitory effect on OFP, SOAFP and HI. The inhibition
efficiency of wPVC and wPP for OFP, SOAFP, and HI increases with
higher dosages, whereas it decreases with an increasing amount of



wHDPE. The inclusion of wHDPE and wPVC negatively affects the R-


value of asphalt mixture VOCs. This negative impact becomes more
ethylene, 1,2-dichloroethane, 1,2-

pronounced as the plastic content increases. In contrast, PP can reduce


Dibromoethane, Chlorobenzene
Dichloromethane, 1,2-dichloro­

the carcinogenic risk of VOCs from asphalt mixtures. 0.35 % wPP shows
Benzene, O-ethyltoluene,

the most effective in reducing the environmental risk of asphalt mixture


Methyl tert butyl ether
1,1-dichloroethylene,

VOCs among the waste plastics, achieving inhibition rates of 39.7 % for
OFP and 33 % for SOAFP. Meanwhile, 0.25 % wHDPE is the most
wPVC0.25 %-M

Diethylbenzene

optimal material for inhibiting HI, with an inhibition rate of 58.5 %. This
Asphalt mixture VOCs components with increased concentration due to the addition of waste plastics.

effectiveness is attributed to the ability of wPP to better suppress the


components like pentanal and undecane that significantly contribute to
OFP and SOAP, wHDPE has a better inhibitory effect on components



that contribute significantly to HI, such as acetaldehyde. At the same


methylheptane, Undecane, 2,3-dimethylbu­

1,1,2-trichloroethane, Tetrachloroethylene,

time, the concentrations of these components released by themselves are


Trans-2-pentene, 1-hexene, Trans-2-butene
2-methylpentane, Methyl cyclopentane, 2-
methylhexane, 2,3,4-trimethylpentane, 2-

Dichloromethane, 1,1,1-TrichloroEthane,

very low at high temperatures.


Dibromochloromethane, 1,2-Dibromo­

The most notable aspect is the carcinogenic risk posed by VOCs from
Benzene, 1,2,3-trimethylbenzene

waste plastic modified asphalt mixtures. This is a crucial indicator in


health risk assessments. The addition of 0.35 % wPP can reduce the R-
value of asphalt mixture VOCs by 27.7 %, and 0.25 % wPP also shows a
ethane, Chlorobenzene

certain control over this indicator. However, the inclusion of wHDPE


Pentanal, Hexanal
wHDPE0.35 %-M

and wPVC has a negative impact on this metric, with the adverse effect
tane, Isobutane

increasing as their content rises, particularly evident with wPVC. The


incorporation of 0.25 % and 0.35 % wPVC increases the carcinogenic
risk of asphalt mixture VOCs by 20.7 % and 107.8 %, respectively. 0.25
% and 0.35 % wHDPE increases the risk by 18.8 % and 31.4 %,

respectively. This is because the carcinogenic risk of asphalt mixture


VOCs is mainly caused by halogenated hydrocarbons. According to the
Dibromochloromethane, 1,2-

study in Section 3.2, these two types of waste plastics undergo a series of
chemical reactions at high temperatures, potentially releasing large
amounts of halogenated hydrocarbons. Additionally, the incorporation
Dichloromethane,
wHDPE0.25 %-M

2-methylheptane

Dibromoethane

of wPVC and 0.35 % wHDPE significantly increases the concentration of


halogenated hydrocarbons as discussed in Section 3.3.

4. Conclusions



The road performance and VOCs emissions characteristics of waste


hydrocarbon
Benzene series

Halogenated

plastic modified asphalt mixtures were examined in this study. Emis­


Aldehyde

sions of VOCs from various waste plastics at high temperatures have also
Alkane

Ketone
Table 6

Others
Olefin

been explored. The utilization of different types of waste plastics is a


significant factor contributing to the increased concentrations of certain

8
D. Jiang et al. Environmental Research 279 (2025) 121642

Fig. 13. Environmental and health impact indicators of asphalt mixtures VOCs.

VOCs groups and components released from asphalt mixtures. The 5. Different waste plastic modified asphalt mixtures VOCs have
environmental and health impacts of VOCs from various waste plastics different environmental and health impacts. The addition of 0.35 %
modified asphalt mixtures are also being quantified subsequently. The wPP shows certain inhibition rates for OFP, SOAFP, and R, by 39.7
primary findings are summarized as follows. %, 33 %, and 27.7 %, respectively. The optimal choice for reducing
HI is 0.25 % wHDPE, by 58.5 %. The inclusion of wHDPE and wPVC
1. Waste plastics can enhance the high and low-temperature perfor­ increases the R-value, especially at higher dosages. The incorpora­
mance of asphalt mixtures and improve their water stability, with tion of 0.35 % wPVC can increase the index by 107.8 %. The carci­
wHDPE0.25 %-M demonstrating the best overall road performance. nogenic risk of wPVC-M warrants significant attention and scholarly
All waste plastics modified mixtures can meet the performance consideration.
standards. The negative effect of using highly doped wHDPE on MS0
needs to be noted. In conclusion, while the incorporation of waste plastics into asphalt
2. Different types of waste plastics exhibit significant variations in mixtures can improve road performance and reduce the total concen­
VOCs emissions. The reduction in the absorption peak intensity of C- tration of VOC emissions, the type and dosage of waste plastics must be
H bonds on the plastic surface means the release of alkanes, alkenes, carefully considered. This is due to the highly selective nature of waste
and benzene series. The changes in oxygen-containing functional plastics in inhibiting VOCs from asphalt mixtures. This selectivity is
groups of waste plastics at elevated temperatures signify the for­ largely related to the different types of VOCs released by the waste
mation of ketones and aldehydes. Additionally, the degradation and plastics at high temperatures. 0.35 % wPP is identified as the most
rearrangement of halogen-containing structures during the process effective modifier to balance road performance improvements and
are the primary mechanisms responsible for the generation of ben­ environmental health benefits. The ecological impacts should also be
zene series and halogenated hydrocarbons from waste plastics. taken into consideration seriously when using wPVC and high doses of
3. Alkanes and aldehydes are the primary groups of asphalt mixture wHDPE as modifiers in asphalt mixtures. Future research should focus
VOCs. Different plastics have varying effects on these emissions. on optimizing the selection process of waste plastics from different
Notably, 0.35 % wPP effectively suppresses most VOC groups, sources and further investigating the mechanisms behind the suppres­
achieving over 30 % inhibition. In contrast, 0.25 % wHDPE and 0.35 sion of VOCs by waste plastics.
% wPVC are most effective for inhibiting halogenated hydrocarbons
and other groups, with inhibition rates of 14.6 % and 41.6 %, CRediT authorship contribution statement
respectively. However, 0.35 % wPVC increases the concentrations of
benzene series and halogenated hydrocarbons by 64.8 % and 123.7 Dechen Jiang: Writing – original draft, Visualization, Software,
%. Similarly, 0.35 % wHDPE raises halogenated hydrocarbon con­ Investigation, Formal analysis, Data curation. Zhilong Cao: Writing –
centration by 11.7 %. These increases in specific VOCs groups are review & editing, Supervision, Project administration. Bochao Zhou:
attributed to the emissions from the waste plastics themselves at Supervision, Methodology, Funding acquisition. Guanyu Gong: Vali­
elevated temperatures. dation, Supervision. Zeying Huang: Validation. Chao Wang: Re­
4. Different types and dosages of waste plastics impact specific VOCs sources, Funding acquisition, Conceptualization.
components differently. wPP offers the best overall inhibition, with
an inhibition coverage of 96.47 %. Notably, wPVC raises the con­ Declaration of competing interest
centration of specific components deeply, such as benzene and
chlorobenzene. The incorporation of 0.35 % wHDPE affects the The authors declare that they have no known competing financial
greatest number of components, negatively impacting 41 compo­ interests or personal relationships that could have appeared to influence
nents. Waste plastics release gaseous derivatives of their own at the work reported in this paper.
elevated temperatures, and the affected VOCs are closely related to
the compositional constituents of the added waste plastics.

9
D. Jiang et al. Environmental Research 279 (2025) 121642

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