Metal organic framework(MOF) assembled with coordination bonds has the disadvantage of poor stability that limits its application in the field of stationary phase,while covalent organic framework(COF)assembled through...Metal organic framework(MOF) assembled with coordination bonds has the disadvantage of poor stability that limits its application in the field of stationary phase,while covalent organic framework(COF)assembled through covalent bonds exhibits excellent structural stability.It has been shown that the stationary phases prepared by combining MOF and COF can make up for the poor stability of MOF@SiO_(2),and the MOF/COF composites have superior chromatographic separation performance.However,the traditional methods for preparing COF/MOF based stationary phases are generally solvent thermal synthesis.In this study,a green and low-cost synthesis method was proposed for the preparation of MOF/COF@SiO_(2) stationary phase.Firstly,COF@SiO_(2) was prepared in a choline chloride/ethylene glycol based deep eutectic solvent(DES).Secondly,another acid-base tunable DES prepared by mixing p-toluenesulfonic acid(PTSA)and 2-methylimidazole in different proportions was introduced as the reaction solvent and reactant for rapid synthesis of MOF/COF@SiO_(2).Compared with the toxic transition metal-based MOFs selected in most previous studies,a lightweight and non-toxic S-zone metal(calcium) based MOF was employed in this study.PTSA and calcium will form the calcium/oxygen-containing organic acid framework in acidic DES,which assembles with terephthalic acid dissolved in basic DES to form MOF.The strong hydrogen bonding effect of DES can facilitate rapid assembly of Ca-MOF.The obtained Ca-MOF/COF@SiO_(2) can be used for multi-mode chromatography to efficiently separate multiple isomeric/hydrophilic/hydrophobic analytes.The synthesis method of Ca-MOF/COF@SiO_(2) is green and mild,especially the use of acid-base tunable DES promotes the rapid synthesis of non-toxic Ca-MOF/COF@silica composites,which offers an innovative approach of greenly synthesizing novel MOF/COF stationary phases and extends their applications in the field of chromatography.展开更多
Solvent extraction,a separation and purification technology,is crucial in critical metal metallurgy.Organic solvents commonly used in solvent extraction exhibit disadvantages,such as high volatility,high toxicity,and ...Solvent extraction,a separation and purification technology,is crucial in critical metal metallurgy.Organic solvents commonly used in solvent extraction exhibit disadvantages,such as high volatility,high toxicity,and flammability,causing a spectrum of hazards to human health and environmental safety.Neoteric solvents have been recognized as potential alternatives to these harmful organic solvents.In the past two decades,several neoteric solvents have been proposed,including ionic liquids(ILs)and deep eutectic solvents(DESs).DESs have gradually become the focus of green solvents owing to several advantages,namely,low toxicity,degradability,and low cost.In this critical review,their classification,formation mechanisms,preparation methods,characterization technologies,and special physicochemical properties based on the most recent advancements in research have been systematically described.Subsequently,the major separation and purification applications of DESs in critical metal metallurgy were comprehensively summarized.Finally,future opportunities and challenges of DESs were explored in the current research area.In conclusion,this review provides valuable insights for improving our overall understanding of DESs,and it holds important potential for expanding separation and purification applications in critical metal metallurgy.展开更多
This study explores green and low-viscosity deep eutectic solvents(DESs) for the efficient extraction of quinoline(QUI) from wash oil.The hydrogen bond donors and acceptors constituting DESs were initially screened ba...This study explores green and low-viscosity deep eutectic solvents(DESs) for the efficient extraction of quinoline(QUI) from wash oil.The hydrogen bond donors and acceptors constituting DESs were initially screened based on thermodynamic properties predicted by the conductor-like screening model for real solvents(COSMO-RS),followed by further selection considering the viscosity and cost of the formed DESs.Phase equilibrium experiments showed that the DES composed of triethylmethylammonium chloride and formic acid exhibited the best extraction performance among the selected candidates.Key extraction parameters were optimized experimentally,achieving a maximum QUI extraction efficiency of 97.18% under mild conditions.Molecular dynamics simulations revealed that the interactions between quaternary ammonium cations and QUI play a crucial role in the extraction mechanism.This study provides insights into the use of DESs for QUI extraction and demonstrates their potential for application to other coal tar derivatives.展开更多
Green Analytical Chemistry attempts to develop analytical procedures that reduce the environmental impact of the reagents and processes while also ensuring efficiency and cost-effectiveness.This Green Chemistry philos...Green Analytical Chemistry attempts to develop analytical procedures that reduce the environmental impact of the reagents and processes while also ensuring efficiency and cost-effectiveness.This Green Chemistry philosophy impacts the analysis of contaminants in foodstuffs,a global concern due to their harmful effects on human health.Most contaminant extraction methods are based on organic solvents,which are toxic to humans and hazardous to the environment.Thus,using novel green extraction solvents to replace the current ones is a huge challenge.In this sense,Natural Deep Eutectic Solvents(NADESs)are a great alternative.These solvents have been proven to behave similarly to traditional solvents(i.e.,organic solvents and ionic liquids)in extracting and removing different contaminants from food samples.The synthesis of NADESs is simple and involves low-cost,environmentally friendly,and natural-origin constituents.Moreover,NADES-based extraction methods require fewer steps and reduce the risk for workers as milder experimental procedures are needed.Here,we review a critical gap in the literature:the application of NADESs in the extraction of food chemical contaminants.This review is relevant given the frequent combination of NADESs with organic solvents involved in sample preparation,a practice that confuses future users of this methodology and contradicts the basic principles of green chemistry.Following sustainable development objectives,avoiding these inconsistencies,and highlighting ecological methods to control contaminant residues in food samples are necessary.We believe this review will be a starting point for facilitating the implementation and commercialization of 100%green analytical methodologies applied to the food sector.展开更多
Copper nanosheets and sulfur particles were synthesized synchronously by electrolysis,after dissolving Cu_(2)S in ChCl-thiourea(TU)deep eutectic solvent(DES)system.The optimized electrolysis conditions of 0.9 V,80℃,a...Copper nanosheets and sulfur particles were synthesized synchronously by electrolysis,after dissolving Cu_(2)S in ChCl-thiourea(TU)deep eutectic solvent(DES)system.The optimized electrolysis conditions of 0.9 V,80℃,and 2 h resulted in the deposition of pure nano-sized copper sheets with a length of approximately 500 nm and a thickness of approximately 30 nm,and the production of sulfur particles with an average size of approximately 10μm.The morphology of the cathodic products was significantly influenced by the electrolysis voltage.When Cu_(2)S was introduced into ChCl-TU,it dissolved[CuCl_(2)]^(-)without disrupting the structure of the choline ion(Ch^(+)).As the electrolysis time increased,the copper deposition changed from wire to sheet growth,with the growth direction from radial to epitaxial along the substrate and back to radial.展开更多
Reaction crystallization method is a common cocrystal synthesis approach attributed to the advantage of avoiding individual crystallization of insoluble components,but faces the defects of soluble components precipita...Reaction crystallization method is a common cocrystal synthesis approach attributed to the advantage of avoiding individual crystallization of insoluble components,but faces the defects of soluble components precipitated due to organic solvent volatilization and the formation of unwanted solvates.Our group recently proposed a slurry method based on deep eutectic solvents(DESs)for cocrystal synthesis,which is green,safe and can avoid solvate formation.However,some reactions only produce insoluble raw materials rather than cocrystals due to insufficient activity of the soluble cocrystal co-formers in DESs.Herein,combining the dual benefits of the two methods,a novel reaction crystallization method based on DESs was proposed and employed for cocrystal synthesis of nicotinamide,carbamazepine and theophylline,which can prevent individual crystallization,unwanted solvate formation,and soluble component precipitation,providing a promising alternative for green and efficient synthesis of cocrystals.展开更多
Two-and three-component deep eutectic solvents(DES)based on acrylic acid(AA),acrylamide(AAm),and choline chloride(ChCl)were used to disintegrate bacterial cellulose into cellulose nanofibers(CNF).As a result,polymeriz...Two-and three-component deep eutectic solvents(DES)based on acrylic acid(AA),acrylamide(AAm),and choline chloride(ChCl)were used to disintegrate bacterial cellulose into cellulose nanofibers(CNF).As a result,polymerizable precursors suitable for 3D printing with CNF as a rheology modifier and reinforcer with formation of interpenetrating double polymer network were obtained after UV curing.Composite hydrogels were formed by replacing ChCl with water.It was found that the introduction of amide groups into the acrylate polymer matrix resulted in an increase in compressive strength.The layered architecture of the 3D printed products provides greater mechanical strength compared to molded products.The structure of the composites was investigated using wide-angle X-ray scattering(WAXS),small-angle X-ray scattering(SAXS),atomic force microscopy(AFM)and polarized light microscopy.These studies suggest that the enhanced mechanical properties of the 3D printed hydrogels are associated with swelling and branching of CNF in the DES,as well as alignment of the filler during extrusion.For comparative analysis,composite hydrogels were also prepared using aqueous solutions of AA and AA/AAm with dispersed CNF.However,the 3D printing process was hampered in this case due to cellulose agglomeration.Mechanical testing revealed the formation of premature microcracks in these samples,which were not observed in composites produced using DES.Cytotoxicity of the composite hydrogels was also tested.The results provide valuable insights into the production of strong(up to 3.4 MPa)homogeneous composite hydrogels using 3D printing with nanocellulose filler.展开更多
Green extraction of bioactive components from natural sources has been a hot topic in the field of chemistry and biology.As a kind of green solvents,deep eutectic solvents(DESs)have unique advantages in the extraction...Green extraction of bioactive components from natural sources has been a hot topic in the field of chemistry and biology.As a kind of green solvents,deep eutectic solvents(DESs)have unique advantages in the extraction of bioactive substances.In recent years,as a new subgroup of DESs,the switchable deep eutectic solvents(SDESs)can realize reversible phase switching between hydrophobic and hydrophilic by external driving forces(CO_(2)/p H/temperature),allowing for the extraction of different polar components while avoiding the problem of difficult recovery of DESs.The application of SDESs reduces the consumption of large amounts of organic solvents during the extraction process,thereby promoting sustainability.In the meanwhile,it presents an advantage over traditional extraction methods in preserving product activity.Based on the recent researches on SDESs,this work summarized the composition,driving factors,and conversion mechanism of SDESs.The applications of SDESs in the extraction of natural products were primarily highlighted to provide a reference for future research.展开更多
Candida albicans is one of the most common pathogens causing invasive fungal infections,with a mortality rate of up to 20%-50%.Amphotericin B(AmB),a biopharmaceutics classification system(BCS)IV drug,significantly inh...Candida albicans is one of the most common pathogens causing invasive fungal infections,with a mortality rate of up to 20%-50%.Amphotericin B(AmB),a biopharmaceutics classification system(BCS)IV drug,significantly inhibits Candida albicans.AmB is primarily administered via oral and intravenous infusion,but severe infusion adverse effects,nephrotoxicity,and potential hepatotoxicity limit its clinical application.Deep eutectic solvents(DESs),with excellent solubilization ability and skin permeability,are attractive for transdermal delivery.Herein,we used DESs to deliver AmB for antifungal therapy transdermally.We first prepared and characterized DESs with different stoichiometric ratios of choline(Ch)and geranate(Ge).DESs increased the solubility of AmB by a thousand-fold.In vitro and in vivo,skin permeation studies indicated that DES_(1:2)(Ch and Ge in 1:2 ratio)had the most outstanding penetration and delivered fluorescence dye to the dermis layer.Then,DES_(1:2)-AmB was prepared and in vitro antifungal tests demonstrated that DES_(1:2)-AmB had superior antifungal effects compared to AmB and DES_(1:2).Furthermore,DES_(1:2)-AmB was skin-irritating and biocompatible.In conclusion,DES-AmB provides a new and effective therapeutic solution for fungal infections.展开更多
The development of low-energy consumption and environmentally friendly electrodeposition of metal/alloy films or coatings is presently one of the primary topics for the research community.For this purpose,deep eutecti...The development of low-energy consumption and environmentally friendly electrodeposition of metal/alloy films or coatings is presently one of the primary topics for the research community.For this purpose,deep eutectic solvents(DESs)are valued as electrolytes for their advantages of low operating temperature and wide electrochemical windows.At present,there is large amount of literature on this emerging field,but there are no specialized reviews of these studies.Here,after a brief introduction of DESs’concept and history,we comprehensively reviewed the lastest progress on the metal/alloy electrodeposition in DESs.Additionally,we discussed the key influence factors of the electrodeposition process and analyzed the corresponding mechanisms.Based on these,we emphasized the importance of the establishment of predictive models for dealing with the challenges in large-scale applications.展开更多
In recent years,flexible ionic conductors have made remarkable progress in the fields of energy storage devices and flexible sensors.However,most of these materials still face challenges such as the difficult trade-of...In recent years,flexible ionic conductors have made remarkable progress in the fields of energy storage devices and flexible sensors.However,most of these materials still face challenges such as the difficult trade-off between stretchability and high mechanical strength,as well as insufficient ionic conductivity.Among them,polymerizable deep eutectic solvents(PDES),which possess both hydrogen bond network construction capabilities and ionic conduction properties,have demonstrated great advantages in the synthesis of flexible ionic conductors.Herein,we report an ionic conductive elastomer(ICE)named PCHS-X based on PDES composed of 2-(methacryloyloxy)-N,N,N-trimethylammonium methyl sulfate(MA-MS),choline chloride(ChCl),and 2-hydroxyethyl acrylate(HEA).The introduction of MA-MS enabled the polymer network to form abundant hydrogen bonds,endowing PCHS-X with excellent mechanical strength,high transparency,favorable ionic conductivity,self-adhesiveness,and self-healing efficiency.When used as a strain sensor,the PCHS-X exhibits highly sensitive strain response,along with good stability and durability,allowing it to accurately monitor the movement of human body parts such as fingers,wrists,elbows,and knees.Additionally,owing to the enhanced ionic mobility at higher temperatures,this material also possesses excellent temperature sensing performance,enabling the fabrication of simple temperature sensors that can sensitively respond to temperature changes.This research provides new strategies for the practical applications of flexible electronic devices in fields such as wearable health monitoring and intelligent human-machine interaction.展开更多
Efficient recognition and selective capture of NH_(3)is not only beneficial for increasing the productivity of the synthetic NH_(3)industry but also for reducing air pollution.For this purpose,a group of deep eutectic...Efficient recognition and selective capture of NH_(3)is not only beneficial for increasing the productivity of the synthetic NH_(3)industry but also for reducing air pollution.For this purpose,a group of deep eutectic solvents(DESs)consisting of glycolic acid(GA)and phenol(PhOH)with low viscosities and multiple active sites was rationally designed in this work.Experimental results show that the GA^(+)PhOH DESs display extremely fast NH_(3)absorption rates(within 51 s for equilibrium)and high NH_(3)solubility.At 313.2 K,the NH_(3)absorption capacities of GA^(+)PhOH(1:1)reach 6.75 mol/kg(at 10.7 kPa)and 14.72 mol/kg(at 201.0 kPa).The NH_(3)solubility of GA^(+)PhOH DESs at low pressures were minimally changed after more than 100 days of air exposure.In addition,the NH_(3)solubility of GA^(+)PhOH DESs remain highly stable in 10 consecutive absorption-desorption cycles.More importantly,NH_(3)can be selectively captured by GA^(+)PhOH DESs from NH_(3)/CO_(2)/N_(2)and NH_(3)/N_(2)/H_(2)mixtures.1H-NMR,Fourier transform infrared and theoretical calculations were performed to reveal the intrinsic mechanism for the efficient recognition of NH_(3)by GA^(+)PhOH DESs.展开更多
H_(2)S in natural gas and other industrial gas is seriously harmful to human health,environmental protection and the downstream industries.Efficient purification of H_(2)S containing gas is the basic process in the ch...H_(2)S in natural gas and other industrial gas is seriously harmful to human health,environmental protection and the downstream industries.Efficient purification of H_(2)S containing gas is the basic process in the chemical industry.Benefiting from multiple advantages,deep eutectic solvents(DES)can be used as tailor-made green solvents,and have been booming in the fields of harmful gas removal and fuel oil desulfurization.Furthermore,significant scientific research of DES in desulfurization and purification of natural gas has accelerated the process of its practical application.This paper systematically summarizes and analyzes the removal mechanism,impact factors and challenges of DES as emerging green solvent in H_(2)S absorption and conversion.Strategies on H_(2)S removal by DES generally fall into two categories:physical absorption and chemical conversion.Although the chemical conversion of H_(2)S by DES has been less studied compared with the physical absorption,it presents great application potential.At present,the research on H_(2)S removal by DES is still in the initial stage.Therefore,it is necessary to further study the mechanism of H_(2)S removal and construct the relationship between structural properties and desulfurization performance of DES,thereby to solve the issues of sulfur blockage and low quality of sulfur paste which is suffered by conventional liquid redox desulfurization solvent system.Additionally,the methods for efficient solvent regeneration and recycling remain to be explored out to promote the practical application of iron-based DES in the field of gas desulfurization.展开更多
Recently, deep eutectic solvents (DES) have received great attention in assisting water flooding and surfactant flooding to improve oil recovery because they can reduce the interfacial tension (IFT) between oil and wa...Recently, deep eutectic solvents (DES) have received great attention in assisting water flooding and surfactant flooding to improve oil recovery because they can reduce the interfacial tension (IFT) between oil and water, inhibit surfactant adsorption, and change the wettability of rock. However, the effects of DES on the wettability of rock surface have not been thoroughly investigated in the reported studies. In this study, the effects of various DES samples on the wettability of sandstone samples are investigated using the Amott wettability measurement method. Three DES samples and several DES solutions and DES-surfactant solutions are firstly synthesized. Then, the wettability of the sandstone samples is measured using pure saline water, DES solutions, and DES-surfactant solutions, respectively. The effects of the DES samples on the wettability of the sandstone samples are investigated by comparing the measured wettability parameters, including oil displacement ratio (I_(o)), water displacement ratio (I_(w)), and wettability index (I_(A)). The Berea rock sample used in this study is weakly hydrophilic with I_(o), I_(w), and I_(A) of 0.318, 0.032, and 0.286, respectively. Being processed by the prepared DES samples, the wettability of the Berea sandstone samples is altered to hydrophilic (0.7 > I_(A) > 0.3) by increasing I_(w) but lowering Io. Similarly, DES-surfactant solutions can also modify the wettability of the Berea sandstone samples from weakly hydrophilic to hydrophilic. However, some DES-surfactant solutions can not only increase I_(w) but also increase I_(o), suggesting that the lipophilicity of those sandstone samples will be improved by the DES-surfactant solutions. In addition, micromodel flooding tests confirm the promising performance of a DES-surfactant solution in improving oil recovery and altering wettability. Moreover, the possible mechanisms of DES and DES-surfactant solutions in altering the wettability of the Berea sandstone samples are proposed. DES samples may improve the hydrophilicity by forming hydrogen bonds between rock surface and water molecules. For DES-surfactant solutions, surfactant micelles can capture oil molecules to improve the lipophilicity of those sandstone samples.展开更多
Ionic liquids (ILs) and deep eutectic solvents (DESs) as green solvents have attracted dramatic attention recently due to their highly tunable properties. However, traditional experimental screening methods are ineffi...Ionic liquids (ILs) and deep eutectic solvents (DESs) as green solvents have attracted dramatic attention recently due to their highly tunable properties. However, traditional experimental screening methods are inefficient and resource-intensive. The article provides a comprehensive overview of various ML algorithms, including artificial neural network (ANN), support vector machine (SVM), random forest (RF), and gradient boosting trees (GBT), etc., which have demonstrated exceptional performance in handling complex and high-dimensional data. Furthermore, the integration of ML with quantum chemical calculations and conductor-like screening model-real solvent (COSMO-RS) has significantly enhanced predictive accuracy, enabling the rapid screening and design of novel solvents. Besides, recent ML applications in the prediction and design of ILs and DESs focused on solubility, melting point, electrical conductivity, and other physicochemical properties become more and more. This paper emphasizes the potential of ML in solvent design, overviewing an efficient approach to accelerate the development of sustainable and high-performance materials, providing guidance for their widespread application in a variety of industrial processes.展开更多
Hydrogels based on Deep Eutectic Solvents(DES)demonstrate remarkable anti-freezing,resilience,and toughness,presenting a promising avenue to the operation of aqueous zincion batteries under extreme conditions.A gel el...Hydrogels based on Deep Eutectic Solvents(DES)demonstrate remarkable anti-freezing,resilience,and toughness,presenting a promising avenue to the operation of aqueous zincion batteries under extreme conditions.A gel electrolyte capable of operating over a wide temperature range is developed based on a DES comprising 1 mol/kg(m)Zn(ClO_(4))_(2)+3.5 m Mg(ClO_(4))_(2).Spectral characterization confirms the synergistic influence of both anions and cations on the freezing point of the DES.With four hydrogen bond(HB)acceptors,Mg^(2+) exhibits strong electrostatic attraction towards the O atoms of H_(2)O,while ClO_(4)^(-)forms numerous HBs with H_(2)O molecules.This dual interaction allows for precise adjustment of the chemical environment around the H and O atoms of H_(2)O,resulting in an exceptionally low freezing point of-116.92℃for the DES.The gel electrolyte derived from this DES demonstrates an impressive ionic conductivity of 0.285 mS/cm at-70℃.Leveraging its excellent low-temperature performance and compatibility with a zinc anode,the flexible Zn-Mn battery constructed with this electrolyte exhibits robust electrochemical performance at low temperatures.Specifically,at-70℃,it achieves a high specific capacity of 76.83 mAh/g,displays excellent rate capability,andmaintains stable cycling performance.Moreover,the Zn-Mn battery operates reliably across a broad temperature range from-70 to 80℃.This study presents innovative insights for advancing Zn-Mn batteries capable of efficient operation across diverse environmental conditions,thereby opening new avenues for their development.展开更多
Deep eutectic solvents(DESs)are a kind of potential lixiviant for selective metal processing due to their versatile complexation properties.In this study,we investigated the recovery of zinc from zinc oxide dust using...Deep eutectic solvents(DESs)are a kind of potential lixiviant for selective metal processing due to their versatile complexation properties.In this study,we investigated the recovery of zinc from zinc oxide dust using choline chloride-ureaethylene glycol(ChCl-urea-EG)DESs.The zinc extraction efficiency can be up to 85.2%when the slurry concentration is 50 g/L,leaching temperature is 80°C and stirring speed is 600 r/min.The leaching process is controlled by the diffusion and the corresponding activation energy is 32.1 k J/mol.The resultant solution was directly used for the electrodeposition of zinc.The pure zinc deposit is obtained with a current efficiency of 82.6%.Furthermore,the ChCl-urea-EG DESs can be recycled.This approach is shown to be promising for the recycling of zinc from the zinc-containing dust.展开更多
Efficient recycling technology for the rapid growth of spent lithium-ion batteries(LIBs)is essential to tackle the resources and environmental crisis.Hydrometallurgical approach has attracted extensive research due to...Efficient recycling technology for the rapid growth of spent lithium-ion batteries(LIBs)is essential to tackle the resources and environmental crisis.Hydrometallurgical approach has attracted extensive research due to its potential to reduce the consumption of energy and threat to the environment.However,the simultaneous realization of green,efficient and closed-loop recycling is still challenging.Herein,we report a closed-loop and highly efficient approach to recycle lithium cobalt oxide from spent LIBs based on a choline chloride:oxalic acid(ChCl:OA)type deep eutectic solvent(DES).An ultrafast leaching process is observed at 180°C for 10 s with no observable residues.The energy barrier during leaching is calculated to be 113.9 kJ/mol.Noteworthy,the solubility of cobalt ions can be reversibly tuned by simply adding/evaporating deionized water,thus avoiding the addition of precipitant and enabling the easy recovery of the leaching solvent for realizing a closed-loop recycling process.The simultaneous realization of high efficiency,green and closed-loop process is expected to push the DES into practical application for recycling the electrodes of LIBs.展开更多
This review divides the acidic deep eutectic solvents(ADES) into Br?nsted and Lewis DES according to their diversity of acidic character.The hydrogen bond donors and halide salts for formulating an ADES are classified...This review divides the acidic deep eutectic solvents(ADES) into Br?nsted and Lewis DES according to their diversity of acidic character.The hydrogen bond donors and halide salts for formulating an ADES are classified, the synthesis methods are described, and the physicochemical properties including freezing point, acidity, density, viscosity and conductivity are presented. Furthermore, the applications of Br?nsted acidic deep eutectic solvents(BADES) and Lewis acidic deep eutectic solvents(LADES) are overviewed, respectively, covering the fields in dissolution, extraction, organic reaction and metal electrodeposition. It is expected that the ADES has great potential to replace the pollutional mineral acid, expensive and unstable solid acid, and costly ionic liquid in many acid-employed chemical processes, thus meeting the demands of green chemistry.展开更多
The CO_(2)solubilities(including CO_(2)Henry’s constant)in physical-and chemical-based ILs/DESs and the COSMO-RS models describing these properties were comprehensively collected and summarized.The summarized results...The CO_(2)solubilities(including CO_(2)Henry’s constant)in physical-and chemical-based ILs/DESs and the COSMO-RS models describing these properties were comprehensively collected and summarized.The summarized results indicate that chemical-based ILs/DESs are superior to physical-based ILs/DESs for CO_(2)capture,especially those ILs have functionalized cation and anion,and superbase DESs;some of the superbase DESs have higher CO_(2)solubilities than those of ILs;the best physical-and chemical-based ILs,as well as physical-and chemicalbased DESs are[BMIM][BF4](4.20 mol kg^(-1)),[DETAH][Im](11.91 mol kg^(-1)),[L-Arg]-Gly 1:6(4.92 mol kg^(-1))and TBD-EG 1:4(12.90 mol kg^(-1)),respectively.Besides the original COSMO-RS mainly providing qualitative predictions,six corrected COSMO-RS models have been proposed to improve the prediction performance based on the experimental data,but only one model is with universal parameters.The newly determined experimental results were further used to verify the perditions of original and corrected COSMO-RS models.The comparison indicates that the original COSMO-RS qualitatively predicts CO_(2)solubility for some but not all ILs/DESs,while the quantitative prediction is incapable at all.The original COSMO-RS is capable to predict CO_(2)Henry’s constant qualitatively for both physical-based ILs and DESs,and quantitative prediction is only available for DESs.For the corrected COSMO-RS models,only the model with universal parameters provides quantitative predictions for CO_(2)solubility in physical-based DESs,while other corrected models always show large deviations(>83%)compared with the experimental CO_(2)Henry’s constants.展开更多
基金supported by National Natural Science Foundation of China (Nos.21906124,32302202)Natural Science Foundation of Hubei Province (No.2017CFB220)Natural Science Foundation of Shandong Province (No.ZR2023MH278)。
文摘Metal organic framework(MOF) assembled with coordination bonds has the disadvantage of poor stability that limits its application in the field of stationary phase,while covalent organic framework(COF)assembled through covalent bonds exhibits excellent structural stability.It has been shown that the stationary phases prepared by combining MOF and COF can make up for the poor stability of MOF@SiO_(2),and the MOF/COF composites have superior chromatographic separation performance.However,the traditional methods for preparing COF/MOF based stationary phases are generally solvent thermal synthesis.In this study,a green and low-cost synthesis method was proposed for the preparation of MOF/COF@SiO_(2) stationary phase.Firstly,COF@SiO_(2) was prepared in a choline chloride/ethylene glycol based deep eutectic solvent(DES).Secondly,another acid-base tunable DES prepared by mixing p-toluenesulfonic acid(PTSA)and 2-methylimidazole in different proportions was introduced as the reaction solvent and reactant for rapid synthesis of MOF/COF@SiO_(2).Compared with the toxic transition metal-based MOFs selected in most previous studies,a lightweight and non-toxic S-zone metal(calcium) based MOF was employed in this study.PTSA and calcium will form the calcium/oxygen-containing organic acid framework in acidic DES,which assembles with terephthalic acid dissolved in basic DES to form MOF.The strong hydrogen bonding effect of DES can facilitate rapid assembly of Ca-MOF.The obtained Ca-MOF/COF@SiO_(2) can be used for multi-mode chromatography to efficiently separate multiple isomeric/hydrophilic/hydrophobic analytes.The synthesis method of Ca-MOF/COF@SiO_(2) is green and mild,especially the use of acid-base tunable DES promotes the rapid synthesis of non-toxic Ca-MOF/COF@silica composites,which offers an innovative approach of greenly synthesizing novel MOF/COF stationary phases and extends their applications in the field of chromatography.
基金financially supported by the Original Exploration Project of the National Natural Science Foundation of China(No.52150079)the National Natural Science Foundation of China(Nos.U22A20130,U2004215,and 51974280)+1 种基金the Natural Science Foundation of Henan Province of China(No.232300421196)the Project of Zhongyuan Critical Metals Laboratory of China(Nos.GJJSGFYQ202304,GJJSGFJQ202306,GJJSGFYQ202323,GJJSGFYQ202308,and GJJSGFYQ202307)。
文摘Solvent extraction,a separation and purification technology,is crucial in critical metal metallurgy.Organic solvents commonly used in solvent extraction exhibit disadvantages,such as high volatility,high toxicity,and flammability,causing a spectrum of hazards to human health and environmental safety.Neoteric solvents have been recognized as potential alternatives to these harmful organic solvents.In the past two decades,several neoteric solvents have been proposed,including ionic liquids(ILs)and deep eutectic solvents(DESs).DESs have gradually become the focus of green solvents owing to several advantages,namely,low toxicity,degradability,and low cost.In this critical review,their classification,formation mechanisms,preparation methods,characterization technologies,and special physicochemical properties based on the most recent advancements in research have been systematically described.Subsequently,the major separation and purification applications of DESs in critical metal metallurgy were comprehensively summarized.Finally,future opportunities and challenges of DESs were explored in the current research area.In conclusion,this review provides valuable insights for improving our overall understanding of DESs,and it holds important potential for expanding separation and purification applications in critical metal metallurgy.
基金financially supported by the Natural Science Foundation of Shanxi Province (20210302123167)National Key Research and Development Program (2022YFC3902505)。
文摘This study explores green and low-viscosity deep eutectic solvents(DESs) for the efficient extraction of quinoline(QUI) from wash oil.The hydrogen bond donors and acceptors constituting DESs were initially screened based on thermodynamic properties predicted by the conductor-like screening model for real solvents(COSMO-RS),followed by further selection considering the viscosity and cost of the formed DESs.Phase equilibrium experiments showed that the DES composed of triethylmethylammonium chloride and formic acid exhibited the best extraction performance among the selected candidates.Key extraction parameters were optimized experimentally,achieving a maximum QUI extraction efficiency of 97.18% under mild conditions.Molecular dynamics simulations revealed that the interactions between quaternary ammonium cations and QUI play a crucial role in the extraction mechanism.This study provides insights into the use of DESs for QUI extraction and demonstrates their potential for application to other coal tar derivatives.
基金funded by the Spanish Ministry of Science and Innovation(MICIN,ref.PID2021-127457OB-C21/22)。
文摘Green Analytical Chemistry attempts to develop analytical procedures that reduce the environmental impact of the reagents and processes while also ensuring efficiency and cost-effectiveness.This Green Chemistry philosophy impacts the analysis of contaminants in foodstuffs,a global concern due to their harmful effects on human health.Most contaminant extraction methods are based on organic solvents,which are toxic to humans and hazardous to the environment.Thus,using novel green extraction solvents to replace the current ones is a huge challenge.In this sense,Natural Deep Eutectic Solvents(NADESs)are a great alternative.These solvents have been proven to behave similarly to traditional solvents(i.e.,organic solvents and ionic liquids)in extracting and removing different contaminants from food samples.The synthesis of NADESs is simple and involves low-cost,environmentally friendly,and natural-origin constituents.Moreover,NADES-based extraction methods require fewer steps and reduce the risk for workers as milder experimental procedures are needed.Here,we review a critical gap in the literature:the application of NADESs in the extraction of food chemical contaminants.This review is relevant given the frequent combination of NADESs with organic solvents involved in sample preparation,a practice that confuses future users of this methodology and contradicts the basic principles of green chemistry.Following sustainable development objectives,avoiding these inconsistencies,and highlighting ecological methods to control contaminant residues in food samples are necessary.We believe this review will be a starting point for facilitating the implementation and commercialization of 100%green analytical methodologies applied to the food sector.
基金the financial support from the National Natural Science Foundation of China(Nos.51904005,52304362)the Key Research Foundation of University in Anhui Province,China(No.2023AH051113)+1 种基金the Key Laboratory of Ionic Rare Earth Resources and Environment,Ministry of Natural Resources,China(No.2022IRERE203)the Distinguished Young Research Project of Anhui Higher Education Institution,China(No.2023AH020017)。
文摘Copper nanosheets and sulfur particles were synthesized synchronously by electrolysis,after dissolving Cu_(2)S in ChCl-thiourea(TU)deep eutectic solvent(DES)system.The optimized electrolysis conditions of 0.9 V,80℃,and 2 h resulted in the deposition of pure nano-sized copper sheets with a length of approximately 500 nm and a thickness of approximately 30 nm,and the production of sulfur particles with an average size of approximately 10μm.The morphology of the cathodic products was significantly influenced by the electrolysis voltage.When Cu_(2)S was introduced into ChCl-TU,it dissolved[CuCl_(2)]^(-)without disrupting the structure of the choline ion(Ch^(+)).As the electrolysis time increased,the copper deposition changed from wire to sheet growth,with the growth direction from radial to epitaxial along the substrate and back to radial.
基金financially supported by National Natural Science Foundation of China(Nos.22101204 and 22271220)the project grant from the Innovation and Strengthening Project of Guangdong Pharmaceutical University-Special Project of the Guangdong Education Commission(No.2020KZDZX1128)+1 种基金the Research Projects of the Chinese Medicine Council of Guangdong Province(No.20231209)the Key Laboratory of Tropical Medicinal Resource Chemistry of the Ministry of Education at Hainan Normal University(No.RDZH2023001)。
文摘Reaction crystallization method is a common cocrystal synthesis approach attributed to the advantage of avoiding individual crystallization of insoluble components,but faces the defects of soluble components precipitated due to organic solvent volatilization and the formation of unwanted solvates.Our group recently proposed a slurry method based on deep eutectic solvents(DESs)for cocrystal synthesis,which is green,safe and can avoid solvate formation.However,some reactions only produce insoluble raw materials rather than cocrystals due to insufficient activity of the soluble cocrystal co-formers in DESs.Herein,combining the dual benefits of the two methods,a novel reaction crystallization method based on DESs was proposed and employed for cocrystal synthesis of nicotinamide,carbamazepine and theophylline,which can prevent individual crystallization,unwanted solvate formation,and soluble component precipitation,providing a promising alternative for green and efficient synthesis of cocrystals.
基金financially supported by part of the state assignment(No.1023031700043-2-1.4.4)。
文摘Two-and three-component deep eutectic solvents(DES)based on acrylic acid(AA),acrylamide(AAm),and choline chloride(ChCl)were used to disintegrate bacterial cellulose into cellulose nanofibers(CNF).As a result,polymerizable precursors suitable for 3D printing with CNF as a rheology modifier and reinforcer with formation of interpenetrating double polymer network were obtained after UV curing.Composite hydrogels were formed by replacing ChCl with water.It was found that the introduction of amide groups into the acrylate polymer matrix resulted in an increase in compressive strength.The layered architecture of the 3D printed products provides greater mechanical strength compared to molded products.The structure of the composites was investigated using wide-angle X-ray scattering(WAXS),small-angle X-ray scattering(SAXS),atomic force microscopy(AFM)and polarized light microscopy.These studies suggest that the enhanced mechanical properties of the 3D printed hydrogels are associated with swelling and branching of CNF in the DES,as well as alignment of the filler during extrusion.For comparative analysis,composite hydrogels were also prepared using aqueous solutions of AA and AA/AAm with dispersed CNF.However,the 3D printing process was hampered in this case due to cellulose agglomeration.Mechanical testing revealed the formation of premature microcracks in these samples,which were not observed in composites produced using DES.Cytotoxicity of the composite hydrogels was also tested.The results provide valuable insights into the production of strong(up to 3.4 MPa)homogeneous composite hydrogels using 3D printing with nanocellulose filler.
基金financially supported by National Natural Science Foundation of China(No.22174129)the Natural Science Foundation of Zhejiang Province(No.LZY21E030001)the Xin-Miao Talents Program of Zhejiang Province(No.2024R403B064)。
文摘Green extraction of bioactive components from natural sources has been a hot topic in the field of chemistry and biology.As a kind of green solvents,deep eutectic solvents(DESs)have unique advantages in the extraction of bioactive substances.In recent years,as a new subgroup of DESs,the switchable deep eutectic solvents(SDESs)can realize reversible phase switching between hydrophobic and hydrophilic by external driving forces(CO_(2)/p H/temperature),allowing for the extraction of different polar components while avoiding the problem of difficult recovery of DESs.The application of SDESs reduces the consumption of large amounts of organic solvents during the extraction process,thereby promoting sustainability.In the meanwhile,it presents an advantage over traditional extraction methods in preserving product activity.Based on the recent researches on SDESs,this work summarized the composition,driving factors,and conversion mechanism of SDESs.The applications of SDESs in the extraction of natural products were primarily highlighted to provide a reference for future research.
基金supported by the National Natural Science Foundation of China(Nos.81872823,82073782,and 82241002)the Key R&D Plan of Ganjiang New District of Jiangxi(No.2023010).
文摘Candida albicans is one of the most common pathogens causing invasive fungal infections,with a mortality rate of up to 20%-50%.Amphotericin B(AmB),a biopharmaceutics classification system(BCS)IV drug,significantly inhibits Candida albicans.AmB is primarily administered via oral and intravenous infusion,but severe infusion adverse effects,nephrotoxicity,and potential hepatotoxicity limit its clinical application.Deep eutectic solvents(DESs),with excellent solubilization ability and skin permeability,are attractive for transdermal delivery.Herein,we used DESs to deliver AmB for antifungal therapy transdermally.We first prepared and characterized DESs with different stoichiometric ratios of choline(Ch)and geranate(Ge).DESs increased the solubility of AmB by a thousand-fold.In vitro and in vivo,skin permeation studies indicated that DES_(1:2)(Ch and Ge in 1:2 ratio)had the most outstanding penetration and delivered fluorescence dye to the dermis layer.Then,DES_(1:2)-AmB was prepared and in vitro antifungal tests demonstrated that DES_(1:2)-AmB had superior antifungal effects compared to AmB and DES_(1:2).Furthermore,DES_(1:2)-AmB was skin-irritating and biocompatible.In conclusion,DES-AmB provides a new and effective therapeutic solution for fungal infections.
基金financially supported from the National Natural Science Foundation of China(Nos.52274291,52204305)Beijing Institute of Technology Research Fund Program for Young Scholars,China(No.1740011182102).
文摘The development of low-energy consumption and environmentally friendly electrodeposition of metal/alloy films or coatings is presently one of the primary topics for the research community.For this purpose,deep eutectic solvents(DESs)are valued as electrolytes for their advantages of low operating temperature and wide electrochemical windows.At present,there is large amount of literature on this emerging field,but there are no specialized reviews of these studies.Here,after a brief introduction of DESs’concept and history,we comprehensively reviewed the lastest progress on the metal/alloy electrodeposition in DESs.Additionally,we discussed the key influence factors of the electrodeposition process and analyzed the corresponding mechanisms.Based on these,we emphasized the importance of the establishment of predictive models for dealing with the challenges in large-scale applications.
基金financially supported by the Natural Science Foundation of the Jiangsu Higher Education Institutions of China(No.20KJA150009)a Project Funded by the Priority Academic Program Development(PAPD)of Jiangsu Higher Education Institutions。
文摘In recent years,flexible ionic conductors have made remarkable progress in the fields of energy storage devices and flexible sensors.However,most of these materials still face challenges such as the difficult trade-off between stretchability and high mechanical strength,as well as insufficient ionic conductivity.Among them,polymerizable deep eutectic solvents(PDES),which possess both hydrogen bond network construction capabilities and ionic conduction properties,have demonstrated great advantages in the synthesis of flexible ionic conductors.Herein,we report an ionic conductive elastomer(ICE)named PCHS-X based on PDES composed of 2-(methacryloyloxy)-N,N,N-trimethylammonium methyl sulfate(MA-MS),choline chloride(ChCl),and 2-hydroxyethyl acrylate(HEA).The introduction of MA-MS enabled the polymer network to form abundant hydrogen bonds,endowing PCHS-X with excellent mechanical strength,high transparency,favorable ionic conductivity,self-adhesiveness,and self-healing efficiency.When used as a strain sensor,the PCHS-X exhibits highly sensitive strain response,along with good stability and durability,allowing it to accurately monitor the movement of human body parts such as fingers,wrists,elbows,and knees.Additionally,owing to the enhanced ionic mobility at higher temperatures,this material also possesses excellent temperature sensing performance,enabling the fabrication of simple temperature sensors that can sensitively respond to temperature changes.This research provides new strategies for the practical applications of flexible electronic devices in fields such as wearable health monitoring and intelligent human-machine interaction.
基金supported by the National Natural Science Foundation of China(22008033)the Major Program of Qingyuan Innovation Laboratory.
文摘Efficient recognition and selective capture of NH_(3)is not only beneficial for increasing the productivity of the synthetic NH_(3)industry but also for reducing air pollution.For this purpose,a group of deep eutectic solvents(DESs)consisting of glycolic acid(GA)and phenol(PhOH)with low viscosities and multiple active sites was rationally designed in this work.Experimental results show that the GA^(+)PhOH DESs display extremely fast NH_(3)absorption rates(within 51 s for equilibrium)and high NH_(3)solubility.At 313.2 K,the NH_(3)absorption capacities of GA^(+)PhOH(1:1)reach 6.75 mol/kg(at 10.7 kPa)and 14.72 mol/kg(at 201.0 kPa).The NH_(3)solubility of GA^(+)PhOH DESs at low pressures were minimally changed after more than 100 days of air exposure.In addition,the NH_(3)solubility of GA^(+)PhOH DESs remain highly stable in 10 consecutive absorption-desorption cycles.More importantly,NH_(3)can be selectively captured by GA^(+)PhOH DESs from NH_(3)/CO_(2)/N_(2)and NH_(3)/N_(2)/H_(2)mixtures.1H-NMR,Fourier transform infrared and theoretical calculations were performed to reveal the intrinsic mechanism for the efficient recognition of NH_(3)by GA^(+)PhOH DESs.
基金supported by Research Project of Petro-China Southwest Oil&Gas Field Company,China(No.2024D106-03-02).
文摘H_(2)S in natural gas and other industrial gas is seriously harmful to human health,environmental protection and the downstream industries.Efficient purification of H_(2)S containing gas is the basic process in the chemical industry.Benefiting from multiple advantages,deep eutectic solvents(DES)can be used as tailor-made green solvents,and have been booming in the fields of harmful gas removal and fuel oil desulfurization.Furthermore,significant scientific research of DES in desulfurization and purification of natural gas has accelerated the process of its practical application.This paper systematically summarizes and analyzes the removal mechanism,impact factors and challenges of DES as emerging green solvent in H_(2)S absorption and conversion.Strategies on H_(2)S removal by DES generally fall into two categories:physical absorption and chemical conversion.Although the chemical conversion of H_(2)S by DES has been less studied compared with the physical absorption,it presents great application potential.At present,the research on H_(2)S removal by DES is still in the initial stage.Therefore,it is necessary to further study the mechanism of H_(2)S removal and construct the relationship between structural properties and desulfurization performance of DES,thereby to solve the issues of sulfur blockage and low quality of sulfur paste which is suffered by conventional liquid redox desulfurization solvent system.Additionally,the methods for efficient solvent regeneration and recycling remain to be explored out to promote the practical application of iron-based DES in the field of gas desulfurization.
基金supported by the Scientific Research and Technology Development Projects of PetroChina(2023ZZ22-02)the Local Efficient Reform and Development Funds for Personnel Training Projectsthe China Scholarship Council(CSC)via a Ph.D.Scholarship(No.202008510128).
文摘Recently, deep eutectic solvents (DES) have received great attention in assisting water flooding and surfactant flooding to improve oil recovery because they can reduce the interfacial tension (IFT) between oil and water, inhibit surfactant adsorption, and change the wettability of rock. However, the effects of DES on the wettability of rock surface have not been thoroughly investigated in the reported studies. In this study, the effects of various DES samples on the wettability of sandstone samples are investigated using the Amott wettability measurement method. Three DES samples and several DES solutions and DES-surfactant solutions are firstly synthesized. Then, the wettability of the sandstone samples is measured using pure saline water, DES solutions, and DES-surfactant solutions, respectively. The effects of the DES samples on the wettability of the sandstone samples are investigated by comparing the measured wettability parameters, including oil displacement ratio (I_(o)), water displacement ratio (I_(w)), and wettability index (I_(A)). The Berea rock sample used in this study is weakly hydrophilic with I_(o), I_(w), and I_(A) of 0.318, 0.032, and 0.286, respectively. Being processed by the prepared DES samples, the wettability of the Berea sandstone samples is altered to hydrophilic (0.7 > I_(A) > 0.3) by increasing I_(w) but lowering Io. Similarly, DES-surfactant solutions can also modify the wettability of the Berea sandstone samples from weakly hydrophilic to hydrophilic. However, some DES-surfactant solutions can not only increase I_(w) but also increase I_(o), suggesting that the lipophilicity of those sandstone samples will be improved by the DES-surfactant solutions. In addition, micromodel flooding tests confirm the promising performance of a DES-surfactant solution in improving oil recovery and altering wettability. Moreover, the possible mechanisms of DES and DES-surfactant solutions in altering the wettability of the Berea sandstone samples are proposed. DES samples may improve the hydrophilicity by forming hydrogen bonds between rock surface and water molecules. For DES-surfactant solutions, surfactant micelles can capture oil molecules to improve the lipophilicity of those sandstone samples.
基金supported by the National Key Research and Development Program of China(2022YFB3504702)support from Horizon-EIC,Pathfinder challenges(101070976)+3 种基金support from the National Natural Science Foundation of China(22278402,22478389)the Key Research and Development Program of Henan Province(231111241800)State Key Laboratory of Mesoscience and Engineering(MESO-23-A08)the Frontier Basic Research Projects of Institute of Process Engineering,CAS(QYJC-2023-03).
文摘Ionic liquids (ILs) and deep eutectic solvents (DESs) as green solvents have attracted dramatic attention recently due to their highly tunable properties. However, traditional experimental screening methods are inefficient and resource-intensive. The article provides a comprehensive overview of various ML algorithms, including artificial neural network (ANN), support vector machine (SVM), random forest (RF), and gradient boosting trees (GBT), etc., which have demonstrated exceptional performance in handling complex and high-dimensional data. Furthermore, the integration of ML with quantum chemical calculations and conductor-like screening model-real solvent (COSMO-RS) has significantly enhanced predictive accuracy, enabling the rapid screening and design of novel solvents. Besides, recent ML applications in the prediction and design of ILs and DESs focused on solubility, melting point, electrical conductivity, and other physicochemical properties become more and more. This paper emphasizes the potential of ML in solvent design, overviewing an efficient approach to accelerate the development of sustainable and high-performance materials, providing guidance for their widespread application in a variety of industrial processes.
基金supported by the National Natural Science Foundation of China(Nos.52072136,51972257,51872104,and 52172229)Hubei Key Laboratory of Biomass Fibers&Eco-Dyeing&Finishing(Wuhan Textile University)(Nos.STRZ202225,and STRZ202406).
文摘Hydrogels based on Deep Eutectic Solvents(DES)demonstrate remarkable anti-freezing,resilience,and toughness,presenting a promising avenue to the operation of aqueous zincion batteries under extreme conditions.A gel electrolyte capable of operating over a wide temperature range is developed based on a DES comprising 1 mol/kg(m)Zn(ClO_(4))_(2)+3.5 m Mg(ClO_(4))_(2).Spectral characterization confirms the synergistic influence of both anions and cations on the freezing point of the DES.With four hydrogen bond(HB)acceptors,Mg^(2+) exhibits strong electrostatic attraction towards the O atoms of H_(2)O,while ClO_(4)^(-)forms numerous HBs with H_(2)O molecules.This dual interaction allows for precise adjustment of the chemical environment around the H and O atoms of H_(2)O,resulting in an exceptionally low freezing point of-116.92℃for the DES.The gel electrolyte derived from this DES demonstrates an impressive ionic conductivity of 0.285 mS/cm at-70℃.Leveraging its excellent low-temperature performance and compatibility with a zinc anode,the flexible Zn-Mn battery constructed with this electrolyte exhibits robust electrochemical performance at low temperatures.Specifically,at-70℃,it achieves a high specific capacity of 76.83 mAh/g,displays excellent rate capability,andmaintains stable cycling performance.Moreover,the Zn-Mn battery operates reliably across a broad temperature range from-70 to 80℃.This study presents innovative insights for advancing Zn-Mn batteries capable of efficient operation across diverse environmental conditions,thereby opening new avenues for their development.
基金Project(51764027)supported by the National Natural Science Foundation of ChinaProject(2014CB643404)supported by the National Basic Research Program of China
文摘Deep eutectic solvents(DESs)are a kind of potential lixiviant for selective metal processing due to their versatile complexation properties.In this study,we investigated the recovery of zinc from zinc oxide dust using choline chloride-ureaethylene glycol(ChCl-urea-EG)DESs.The zinc extraction efficiency can be up to 85.2%when the slurry concentration is 50 g/L,leaching temperature is 80°C and stirring speed is 600 r/min.The leaching process is controlled by the diffusion and the corresponding activation energy is 32.1 k J/mol.The resultant solution was directly used for the electrodeposition of zinc.The pure zinc deposit is obtained with a current efficiency of 82.6%.Furthermore,the ChCl-urea-EG DESs can be recycled.This approach is shown to be promising for the recycling of zinc from the zinc-containing dust.
基金supported by the Talented Program of Guizhou University(702759203301)the Natural Science Foundation of Guizhou Science and Technology Department(QKHJC-ZK[2021]-YB257)。
文摘Efficient recycling technology for the rapid growth of spent lithium-ion batteries(LIBs)is essential to tackle the resources and environmental crisis.Hydrometallurgical approach has attracted extensive research due to its potential to reduce the consumption of energy and threat to the environment.However,the simultaneous realization of green,efficient and closed-loop recycling is still challenging.Herein,we report a closed-loop and highly efficient approach to recycle lithium cobalt oxide from spent LIBs based on a choline chloride:oxalic acid(ChCl:OA)type deep eutectic solvent(DES).An ultrafast leaching process is observed at 180°C for 10 s with no observable residues.The energy barrier during leaching is calculated to be 113.9 kJ/mol.Noteworthy,the solubility of cobalt ions can be reversibly tuned by simply adding/evaporating deionized water,thus avoiding the addition of precipitant and enabling the easy recovery of the leaching solvent for realizing a closed-loop recycling process.The simultaneous realization of high efficiency,green and closed-loop process is expected to push the DES into practical application for recycling the electrodes of LIBs.
基金The financial support from National Natural Science Foundation of China(21776074,21576081,and 2181101120)is greatly acknowledged
文摘This review divides the acidic deep eutectic solvents(ADES) into Br?nsted and Lewis DES according to their diversity of acidic character.The hydrogen bond donors and halide salts for formulating an ADES are classified, the synthesis methods are described, and the physicochemical properties including freezing point, acidity, density, viscosity and conductivity are presented. Furthermore, the applications of Br?nsted acidic deep eutectic solvents(BADES) and Lewis acidic deep eutectic solvents(LADES) are overviewed, respectively, covering the fields in dissolution, extraction, organic reaction and metal electrodeposition. It is expected that the ADES has great potential to replace the pollutional mineral acid, expensive and unstable solid acid, and costly ionic liquid in many acid-employed chemical processes, thus meeting the demands of green chemistry.
基金financially supported by Carl Tryggers Stiftelse foundation(No.18:175)the financial support from the Swedish Energy Agency(P47500-1)+5 种基金K.C.Wang Education Foundation(No.GJTD-201804)the financial support from the National Natural Science Foundation of China(No.21890764)the financial supports from the National Natural Science Foundation of China(No.21838010)the financial support from the National Natural Science Foundation of China(No.21776276)the National Natural Science Foundation of China(21701024)the Foundation for Distinguished Young Talents in Higher Education of Fujian Province(GY-Z17067)
文摘The CO_(2)solubilities(including CO_(2)Henry’s constant)in physical-and chemical-based ILs/DESs and the COSMO-RS models describing these properties were comprehensively collected and summarized.The summarized results indicate that chemical-based ILs/DESs are superior to physical-based ILs/DESs for CO_(2)capture,especially those ILs have functionalized cation and anion,and superbase DESs;some of the superbase DESs have higher CO_(2)solubilities than those of ILs;the best physical-and chemical-based ILs,as well as physical-and chemicalbased DESs are[BMIM][BF4](4.20 mol kg^(-1)),[DETAH][Im](11.91 mol kg^(-1)),[L-Arg]-Gly 1:6(4.92 mol kg^(-1))and TBD-EG 1:4(12.90 mol kg^(-1)),respectively.Besides the original COSMO-RS mainly providing qualitative predictions,six corrected COSMO-RS models have been proposed to improve the prediction performance based on the experimental data,but only one model is with universal parameters.The newly determined experimental results were further used to verify the perditions of original and corrected COSMO-RS models.The comparison indicates that the original COSMO-RS qualitatively predicts CO_(2)solubility for some but not all ILs/DESs,while the quantitative prediction is incapable at all.The original COSMO-RS is capable to predict CO_(2)Henry’s constant qualitatively for both physical-based ILs and DESs,and quantitative prediction is only available for DESs.For the corrected COSMO-RS models,only the model with universal parameters provides quantitative predictions for CO_(2)solubility in physical-based DESs,while other corrected models always show large deviations(>83%)compared with the experimental CO_(2)Henry’s constants.
