9.

Room Temperature Gold Leaching: A Sustainable Approach

Gold extraction method at room temperature can offer several advantages by eliminating the

need for additional heating and reducing energy costs. A combination of NBS and Py was

reported to have effectively leached Au(0) from gold ore and electronic waste at room

temperature, converting it to Au(III) with high efficiency and minimal byproducts. It also

lowered the overall chemical waste generated during gold extraction. This method uses readily

available and relatively non-toxic reagents, minimizing environmental impact. It also provides a

straightforward and practical approach for gold leaching, reducing the complexity and cost of the

process. Overall, this method presents a significant advancement in gold recovery, offering a

sustainable and efficient alternative to traditional techniques [134].

Several factors or conditions can impact the temperature dependence of a gold extraction

process. A study using thiourea solution with a concentration of 15.96 kg/t at pH 1.35 and at

room temperature revealed that it was possible to achieve 80.5% gold extraction from a 100%,

106 μm feed within 6 hours. Even higher extraction efficiencies of 92.5% were attainable with a

finer feed and lower pH values [135].

Three key factors (e.g., ore type, iodide/iodine concentration, oxygen presence) were

examined to investigate the effectiveness of iodide/iodine leaching for gold extraction from two

different types of gold ores at room temperature. The results revealed significant differences in

gold extraction efficiency between the two ore types. The carbonaceous ore exhibited a low

extraction of only 20% due to the strong adsorption of gold-iodide complexes onto the organic

matter present in the ore. In contrast, the oxide ore displayed a much higher gold extraction rate,

reaching 77% in 6 hours and 89% in 24 hours when leached with a solution containing 20 g/L

iodide and 4 g/L iodine [136].

developing the optimal combination for gold extraction methods. Interestingly, using iodate as

the oxidant in the leaching solution resulted in no gold extraction even after 48 hours. However,

when a portion of the iodate was converted to iodine by adding HCl to the solution, gold

leaching commenced. This suggests that the presence of iodine is crucial for the oxidation and

complexation of gold, while the initial presence of iodate might hinder the process. Furthermore,

the study observed that the iodine in the solution was gradually consumed within 48 hours due to

its reactions with sulfide and ferrous minerals present in the oxide ore [137].

The specific mechanism of gold leaching also plays a crucial role (i.e., oxidation,

complexation, kinetics) in determining the efficiency and effectiveness of the room temperature

extraction process. A feasibility study of the thiourea process for gold recovery from Kaymaz ore

at a laboratory scale was demonstrated. The results revealed that at room temperature, using a

thiourea solution with a concentration of 16.04 kg/t at pH 1.35, it was possible to achieve an

85.8% gold extraction from a 53 μm feed size within 6 hours. The consumption of thiourea is

directly proportional to the Fe2(SO4)3/thiourea molar ratio and inversely proportional to both pH

and solution temperature. While higher temperatures (e.g., 60 °C) are expected to increase the

gold extraction rate due to enhanced reaction kinetics, the observed decrease in thiourea

consumption at higher temperatures requires further investigation [138].

9.1. Gold Extraction from Ores and Wastes Using Ionic Liquids at Room Temperature

Room temperature ionic liquids (RTILs) are a class of salts with melting points below room

temperature, making them liquid at ambient conditions. Their potential as catalysts and catalytic

supports has been extensively explored in various fields [139].

research has been conducted on diverse RTIL compositions. Specific combinations of organic

cations, such as imidazolium and pyridinium derivatives, with bulky and soft anions like PF6-,

BF4-, CF3SO3-, and (CF3SO2)2N-, have been found to form RTILs at near room temperature.

These RTILs exhibit a range of advantageous properties that make them attractive for various

applications. They demonstrate remarkable chemical and thermal stability, allowing them to

resist degradation and operate effectively at high temperatures. Additionally, their negligible

vapor pressure and nonflammability characteristics contribute to their safety in handling.

Furthermore, their high ionic conductivity facilitates their use in diverse electrochemical

applications, while their wide electrochemical potential window allows for a broad range of

potential values at which electrochemical reactions can occur [140] [141] [142].

A wide range of established electrochemical methods have been successfully employed

for in-depth investigations of the physical and chemical properties of RTILs. Beyond the

traditional approach of cyclic voltammetry on millimeter-sized electrodes, more sophisticated

techniques have also proven to be highly effective in RTIL environments. These advanced

methods, including fast microsecond timescale transient electrochemistry, steady-state

voltammetry at microdisk electrodes, and scanning electrochemical microscopy, provide

powerful tools for studying various processes occurring within RTILs. This diverse toolbox of

electrochemical techniques allows researchers to gain deeper insights into the fundamental

behavior and characteristics of these unique liquid electrolytes [143].

The bmim+HSO42/thiourea/Fe2(SO4)3 leaching system demonstrates efficient extraction

of gold and silver from Perseverance ore at a high solid-to-liquid ratio of 1:4. Notably, the

bmim+HSO42 leaching system achieves comparable gold extraction (86%) to the aqueous
system (85%). This result is also attainable with the ionic liquid alone, without the addition of

sulfuric acid. However, the rate of gold extraction into the bmim+HSO42 leach liquor is slightly

slower, likely due to the increased viscosity of the ionic liquid at room temperature, which

hinders efficient mixing of the sample [144].

Understanding the thermodynamic properties of ILs is crucial for developing and

optimizing efficient and sustainable gold leaching processes at room temperature. By analyzing

the influence of temperature, concentration, and other factors on the system's thermodynamics,

researchers can select the most suitable IL and optimize the leaching conditions for maximizing

gold extraction while minimizing environmental impact. However, it is important to

acknowledge that while RTILs offer several advantages, they also have limitations such as high

cost, limited biodegradability, and potential toxicity [145].

9.2. The Potential of Deep Eutectic Solvents for Efficient Gold Extraction at Ambient

Conditions

The thermal stability of deep eutectic solvents (DESs) differs significantly from that of ionic

liquids. Unlike ionic liquids, DESs exhibit progressive decomposition when subjected to rapid

thermal analysis (TGA). This behavior is attributed to the crucial role of hydrogen bonding in

DESs. Hydrogen bonds create strong interactions between molecules, hindering their "escape"

and influencing the overall thermal decomposition process. This research investigated the

influence of hydrogen bond acceptors (HBAs), hydrogen bond donors (HBDs), and their molar

ratio on DES stability, leading to the identification of specific rules. By carefully selecting

appropriate HBDs and HBAs, particularly the HBDs, DESs with desired thermal stability can be

designed and prepared [146].

salt (e.g., choline chloride (ChCl), N,N-diethylammonium chloride, tetrapropylammonium

bromide, methyltriphenylphosphonium bromide) with a hydrogen bond donor (HBD) (e.g.,

alcohols, carboxylic acids, carbolic acids, amides, esters, ethers, and hydrated metal salts of

halides, nitrates, and acetates). These mixtures form eutectics through hydrogen bonding,

resulting in a significantly lower melting point compared to the individual components [147].

Investigations using solvatochromic probes dissolved in three choline chloride-based

DESs demonstrate that key physicochemical properties of DESs can be effectively modulated by

altering temperature or introducing water. This work specifically examines the impact of

temperature and water addition on the behavior of solvatochromic probes within three DESs

formed by combining choline chloride with 1,2-ethanediol, glycerol, and urea, respectively, in a

1:2 molar ratio. These DESs are named ethaline, glyceline, and reline. The study reveals that

increasing temperature leads to a decrease in the hydrogen bond donating acidity of the DESs.

However, the dipolarity/polarizability and hydrogen bond accepting basicity remain unaffected

by temperature changes. Furthermore, the fluorescence response of the probe pyrene also

suggests a decrease in the polarity of the DESs as temperature is increased [148]. This gives an

insight into the temperature dependence of hydrogen bonding activity, specifically highlighting

its increased strength and prevalence at lower temperatures, starting from room temperature.

For industrial applications, DESs with melting points close to room temperature are

highly desirable. A study investigated the relationship between hydrogen bonding network

features, as analyzed through the Atoms in Molecules (AIM) approach and melting points for a

set of 45 DESs. The electronic density at the cage critical points, representing the entire

interacting network, was identified as the most suitable indicator for inferring molecular-level
characteristics that influence DES melting points. This was confirmed by the observed linear

correlation between the electronic density and melting points. The results demonstrate that low

electronic density at the cage critical points corresponds to lower melting points. This behavior

can be attributed to the high charge delocalization within the hydrogen bonding network, leading

to a low charge concentration at the cage critical points. Consequently, the melting point

depression observed upon mixing DES components is primarily driven by the charge

delocalization process associated with the development of the entire hydrogen bonding network

[149].

9.3. Thermodynamic Computations and Modelling

Understanding and improving the gold dissolution processes in ethaline DES requires the

data visualization and representation tools, and the application of computational approaches for

exploratory modeling and analysis (EMA) to create an integrative framework [150] [151].

During the anodic dissolution of gold, ethaline causes a more intense reaction than an

aqueous ionic liquid-chlorine electrolyte. This discrepancy is probably caused by ethaline's high

chloride ion concentration. Moreover, the anodic dissolution of gold is accelerated by the

addition of water, supporting the observed variations in reaction rates. Because the Au-Cl bond

was defined, the results were utilized to create a potential chemical equation that would explain

the electrochemical oxidation process of the gold electrodes in ethaline, whereby gold-chloride

(AuCl) ions were most likely to form [152].

Under basic pH settings, the diol component EG (CH2OH-CH2OH or 1,2-ethanediol) in

an ethaline solution can deprotonate at each end by its two hydroxyl groups, releasing possibly

the doubly charged dianion [C2H4O2]2- or the singly charged anion (-OCH2-CH2O-). The
complex would result from a contact between the electrophile, a chemical species whose purpose

is to accept a pair of electrons, and the EG anion [153].

Density functional theory (DFT) was utilized in this work to comprehend and create

ligand-metal complexes (based on the previously mentioned mechanisms). DFT sheds light on

the structure and stability of different complexes. For example, the Gibbs free energy (ΔG) can

be used to determine whether the suggested coordination complexes can form or not [20]. In the

framework of investigating gold complexes, the Becke, 3-parameter, Lee–Yang–Parr (B3LYP)

hybrid functional and the Los Alamos National Laboratory 2-Double Zeta (LANL2DZ) basis set

can be utilized. In particular, LANL2DZ functions as a reliable core potential (ECP), facilitating

core electron treatment and properly representing valence electrons, while B3LYP integrates

Hartree-Fock exchange with DFT exchange-correlation functionals [154].

Thermochemical data are computed through DFT, which is provided in the resulting

output file. Additional calculations are required to obtain the gibbs energy and ethalpy of the

proposed mechanisms. In the context of gold dissolution using ethaline, a negative ΔG value is

favorable. It signifies an exothermic process; energy being released in this case translates to a

higher thermodynamic stability for the formed complexes compared to the initial reactants. The

magnitude of the negative ΔG value directly correlates to the strength of the thermodynamic

driving force for complex formation. The negative ΔG values quantify the inherent tendency of

these complex formation reactions to proceed without the need for external energy input [155].

The energy gap that differentiates a gold complex's lowest unoccupied molecular orbital

(LUMO) from its highest occupied molecular orbital (HOMO) is another factor contributing to

its thermodynamic stability. A large energy gap is advantageous since it shows that the complex

is the least reactive and most stable [156].

reaction. It shows that the complex requires energy from external sources to develop under

specific circumstances [157]. The enthalpy of a system is another measure of thermodynamic

favorability. When the enthalpy is negative, the gold dissolving process releases heat into the

surrounding area. This breakdown process produces spontaneity, which is generally considered

advantageous for gold. The heat produced not only aids in dissolving but also maintains the

reaction temperature [158].

A positive ΔS value indicates that systemic disorder or randomness increases as the

system disintegrates. Higher unpredictability has thermodynamic benefits, which generally

encourage the dissolution of gold [159]. A system possessing a high heat capacity can absorb or

release a significant amount of heat without causing a discernible shift in temperature. This helps

maintain a constant reaction temperature during the gold dissolving process, especially in

exothermic reactions (where heat is released) [160].

9.4. Existing Room-Temperature Applications for Gold Extraction and Recovery

Another study employing ammoniacal leaching solution containing 2 M thiosulfate, 4 M

ammonia, and 0.1 M copper sulfate for gold extraction, stated that the temperature did not exert a

positive influence on gold dissolution. The initial hour of leaching exhibited a rapid gold

dissolution rate, reaching approximately 90% of the maximum achievable recovery. However,

further increases in leaching time only resulted in modest gains, with recoveries reaching 80% at

25°C. Increasing the temperature from 25°C to 60°C also led to a decrease in gold recovery, with

78.84% Au leaching compared to 55.74% Au after 3 hours. This decrease in gold recovery at

higher temperatures is likely attributed to the passivation caused by cupric sulfide. The thermal
reaction between Cu(II) ions and thiosulfate leads to the formation of cupric sulfide, and at 60°C,

the kinetics of this film formation are significantly accelerated, hindering gold dissolution [161].

Increasing the temperature from 25°C to 60°C also led to a decrease in gold recovery,

with 78.84% Au leaching compared to 55.74% Au after 3 hours. This decrease in gold recovery

at higher temperatures is likely attributed to the passivation caused by cupric sulfide. The

thermal reaction between Cu(II) ions and thiosulfate leads to the formation of cupric sulfide, and

at 60°C, the kinetics of this film formation are significantly accelerated, hindering gold

dissolution. Furthermore, the increased temperature from 25°C to 60°C facilitates the

decomposition of thiosulfate to sulfur compounds, leading to a significant loss. Under these

conditions, only a small fraction of the added thiosulfate remains available for gold

complexation, further limiting the leaching efficiency [161].

While temperature often plays a significant role in gold leaching processes, there are

some instances where its impact might be minimal. A study investigated the influence of solution

temperature on gold extraction and ore mass loss during gold leaching using a solution

containing thiourea and ammonium thiocyanate. The results revealed that the solution

temperature did not significantly impact either the gold extraction efficiency or the mass loss

percentage of the ore. Notably, the maximum gold extraction of 95% was achieved at near room

temperature of 21°C. This finding suggests that the leaching process in this specific case is

relatively insignificant to temperature changes within the studied range [162].

By carefully selecting the right leaching and oxidizing conditions and agents, it is

possible to achieve efficient and environmentally friendly gold extraction at room temperature.

This can contribute to more sustainable and responsible gold processing practices.
 While DESs offer several advantages, It is critcal to consider the drawbacks when

selecting and using DESs at higher temperatures over lower temperatures close to or at room

temperature. The observed changes in DES behavior with increasing temperature are attributed

to the enhanced ion-pair segregation, leading to increased nanoscale heterogeneity within the

DESs. This study highlights the formation of Li+/ClO4- domains or a general increase in

heterogeneity at elevated temperatures as a key finding. Molecular dynamics (MD) simulations

further reveal that while hydrogen bonding between the amide hydrogens of alkylamides and the

perchlorate ion oxygens diminishes with increasing temperature, hydrogen bonding between the

amide group hydrogens and carbonyl oxygen exhibits a slight increase. These observations

suggest the DES structure is influenced by electrostatic interactions and significant hydrogen

bonding [163].

The viscosity and conductivity of pure DESs can be significantly affected by increasing

temperature, which resulted in an exponential decrease in viscosity and a corresponding

exponential increase in conductivity. Additionally, all the pure DESs are formed tightly packed

ion pairs with similar packing efficiency and temperature dependence. Additionally, structural

investigations using NMR spectroscopy confirmed the presence of a strong interaction network

between the HBA choline chloride and the HBD glycols at all investigated temperatures.

Notably, the temperature did not significantly alter the supramolecular structure of these DESs

up to 353 K [164][165]. Therefore, understanding the molecular interactions involved in gold

leaching at room temperature is essential for developing efficient and selective processes.

Conventionally, cyanide solutions have been employed to achieve efficient gold

dissolution at room temperature. However, due to the environmental and safety concerns

associated with cyanide, alternative leaching agents are being explored. One promising
alternative is DES, with iodine as oxidizing agent. Studies have shown that gold can dissolve in

iodide solutions even at room temperature, making it a viable option for environmentally friendly

gold leaching. Additionally, the rate of gold dissolution is expected to increase proportionally

with the concentration of iodine, offering a potential means to further enhance the efficiency of

the process [166].

A thorough understanding of temperature's influence on DESs is crucial for their

implementation within industrial settings characterized by fluctuating thermal conditions. The

studies underscore the importance of designing DES systems that exhibit resilience to

temperature variations, thus supporting their application in scenarios where environmental

temperatures can significantly impact chemical processes. Situationally, some ChCl-based DES

and their vulnerability to thermal decomposition at high temperatures, not only compromises

their physical and chemical integrity but also raises safety and environmental concerns. Critical

and meticulous selection of operating temperatures when employing DESs is emphasized. This

ensures optimal efficiency and minimizes the risk of degradation, safeguarding both process

safety and environmental well-being [167].

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