The extensive application of lithium-ion batteries in electric vehicles has led to a torrential surge of endof-life batteries.As the dominant anode material,graphite's environmental and resource costs in productio...The extensive application of lithium-ion batteries in electric vehicles has led to a torrential surge of endof-life batteries.As the dominant anode material,graphite's environmental and resource costs in production highlight the necessity of recycling spent graphite(SG).However,SG recycling technologies remain markedly underdeveloped compared to the cathode recovery status,due to perceived lower economic value.This review provides an in-depth analysis of the current SG growth trend and highlights the cost accounting for graphite recycling and the significant importance of advanced recycling technologies.By examining the failure mechanisms of graphite,various recycling and upcycling technologies in both practical application and fundamental research are fully discussed,in terms of the regeneration principle,recycling effect,strengths,and limitations of each method.Furthermore,the multi-purpose applications of recycled graphite beyond LIB anodes are explored to enhance its high-value properties.Finally,the prospects of SG recycling and large-scale application challenges are presented,including economic feasibility,process optimization,and regulatory restrictions.This review provides a comprehensive overview of developments in SG recycling strategies,offering valuable insights for narrowing the gap between fundamental research and practical applications.展开更多
The impurities and structural cracks within spent graphite(SG)in lithium-ion battery anodes hamper lithium-ion intercalation and extraction after successive charge-discharge operations,thereby yielding poor lithium st...The impurities and structural cracks within spent graphite(SG)in lithium-ion battery anodes hamper lithium-ion intercalation and extraction after successive charge-discharge operations,thereby yielding poor lithium storage behavior.Herein,low-viscosity natural deep eutectic solvent(NDES)composed of citric acid(CA)and betaine hydrochloride was employed to remove the organic impurities in SG via a one-step benign process involving hydrogen bonds and electrostatic interactions at mild conditions of 80℃ for only 30 min.After NDES leaching under optimal conditions(molar ratio of CA to betaine hydrochloride=3:1,80℃,30 min),the as-obtained sample(denoted as BG-3)exhibited an extremely clean surface,moderately enlarged interlayer distance,and more structural defects at the edge of graphite lamellae.These features facilitated lithium-ion intercalation and withdrawal,bestowing BG-3 with remarkable activity in lithium-ion battery(LIB)recycling.For instance,BG-3 delivered a capacity of 438.6 mAh g^(-1) at a current density of 0.1 A g^(-1).Its capacity retention reached 97.9%,accompanied by a Coulombic efficiency of 99.1%,upon completing 100 cycles.A molecular dynamics simulation was employed to illuminate the regeneration mechanism for anode graphite from a theoretical perspective.It revealed that NDES exhibits lower binding energy with all contaminants compared to graphite,which is favorable for NDES to eliminate impurities from graphite surfaces.This study unveils a method of recycling SG from retired LIBs by a short eco-friendly process,providing a competitive blueprint to address the shortage of battery-grade anode graphite and to achieve carbon neutrality.展开更多
Recycling spent lithium-ion(Li+)batteries is critical for achieving environmental conservation and the strategic recovery of essential resources.Compared with conventional methods for recovering cathode materials,whic...Recycling spent lithium-ion(Li+)batteries is critical for achieving environmental conservation and the strategic recovery of essential resources.Compared with conventional methods for recovering cathode materials,which are energy-intensive and prone to secondary pollution,the direct regeneration approach has emerged as a rapid and highly efficient method,gaining widespread attention in recent years.However,this approach faces major challenges,including degraded electrochemical performances and limited economic value.This study,therefore,proposes a high-value direct regeneration strategy to convert degraded spent LiFePO_(4)(S-LFP)into a gradient manganese(Mn)-doped regenerated LiFe_(0.7)Mn_(0.3)PO_(4)/C(R-LFMP)composite.This method leverages the inherent microcracks and Li vacancies present in S-LFP,likely acting as diffusion channels for the Mn^(2+)/Li^(+)ions.Through a two-step mechanochemical ball-milling and carbothermal reduction process,this approach achieves simultaneous Li replenishment and surface-localised Mn gradient doping with enhanced structural control.Notably,the R-LFMP exhibits an exceptional electrochemical performance.At 0.1 C,it delivers a discharge capacity of 161.4 mA h g^(−1)and an energy density of 563.5 Wh kg^(−1)(representing a 60.5%improvement over S-LFP).Additionally,it maintains 83%capacity retention after 900 cycles at 0.5C,a considerable enhancement compared to commercial LFMP(62%).Furthermore,the regenerated cathode material generates a net profit of$7.102 kg^(−1),surpassing the profitability of conventional recycling methods by 90%.Overall,this study introduces a transformative and sustainable LFP regeneration technology,achieving breakthroughs in electrochemical restoration and high-value recycling,while paving the way for the closed-loop utilisation of LFP-based energy storage systems.展开更多
The rapid accumulation of spent LiFePO_(4)(LFP)cathodes from retired lithium-ion batteries necessitates the development of effective and environmental-friendly recycling strategies.In this context,direct regeneration ...The rapid accumulation of spent LiFePO_(4)(LFP)cathodes from retired lithium-ion batteries necessitates the development of effective and environmental-friendly recycling strategies.In this context,direct regeneration has emerged as a promising approach for reclaiming LFP cathode materials,offering a streamlined pathway to restore their electrochemical functionality.We report an integrated regeneration protocol that simultaneously repairs the degraded crystal structure and reconstructs the damaged carbon coating in spent LFP.The regenerated cathode material had superfast lithium-ion diffusion kinetics and a stable cathode-electrolyte interface,giving a remarkable rate capability with specific capacities of 122 m Ah g^(-1)at 5C and 106 m Ah g^(-1)at 10C(1C=170 m A g^(-1)).It also maintained capacities of 110.7 m Ah g^(-1)(5C)and 84.1 m Ah g^(-1)(10C)after 400 cycles.It could be used in harsh environments and could be stably cycled at subzero temperatures(-10 and-20°C)and in solid-state electrolyte batteries.Life cycle assessment combined with economic evaluation using the Ever Batt model reveals that this direct regeneration approach has high economic and environmental benefits.展开更多
The pyrometallurgy combined with hydrometallurgy process is commonly used for recovering valuable elements from spent lithium-ion batteries.To improve the corrosion resistance of heat treatment furnace lining material...The pyrometallurgy combined with hydrometallurgy process is commonly used for recovering valuable elements from spent lithium-ion batteries.To improve the corrosion resistance of heat treatment furnace lining materials in this process,SiC-Si_(3)N_(4)-C composite refractories were prepared by heat-treating at 800-1400℃ for 3 h,using fine particles of spent iron ladle bricks(1-0.5 and<0.5 mm),silicon carbide(2-1,1-0.5,and<0.5 mm),silicon nitride(<0.045 mm),and graphite as raw materials.The fine particles of spent iron ladle bricks were used to replace silicon nitride with the same particle size.The effects of the spent iron ladle brick fine particles additions(0,12.12%,26.25%,36.38%and 48.5%,by mass)and the heat treatment temperatures(800,1000,1200 and 1400℃)on the properties of the composite refractories were studied.The results show that:(1)with the<1 mm spent iron ladle brick fine particles addition increasing,the bulk density of the samples changes slightly,the apparent porosity gradually decreases,the cold modulus of rupture(CMOR)increases,and the cold compressive strength(CCS)first decreases,then increases and finally decreases slightly;(2)with the heat treatment temperature rising,the bulk density of the samples first increases and then decreases,the apparent porosity gradually decreases,and the CCS and the CMOR increase;(3)when the temperature is 1400℃ and the spent iron ladle brick fine particles completely replace the silicon nitride fine particles with the same particle size,the sample exhibits the best comprehensive performance,with the bulk density of 2.37 g·cm^(-3),apparent porosity of 14.3%,CCS of 31.6 MPa,and CMOR of 9.0 MPa,and it has a good resistance to the corrosion of crushed spent lithium-ion battery materials at 1000℃.展开更多
Lithium-ion batteries(LIBs)are the most popular energy storage devices due to their high energy density,high operating voltage,and long cycle life.However,green and effective recycling methods are needed because LIBs ...Lithium-ion batteries(LIBs)are the most popular energy storage devices due to their high energy density,high operating voltage,and long cycle life.However,green and effective recycling methods are needed because LIBs contain heavy metals such as Co,Ni,and Mn and organic compounds inside,which seriously threaten human health and the environment.In this work,we review the current status of spent LIB recycling,discuss the traditional pyrometallurgical and hydrometallurgical recovery processes,and summarize the existing short-process recovery technologies such as salt-assisted roasting,flotation processes,and direct recycling.Finally,we analyze the problems and potential research prospects of the current recycling process,and point out that the multidisciplinary integration of recycling will become the mainstream technology for the development of spent LIBs.展开更多
Background Meat originating from the spent hen is an important source of poultry meat production;however,multiple factors cause the decline in the meat quality of spent hens.Chinese herbs have been widely used as medi...Background Meat originating from the spent hen is an important source of poultry meat production;however,multiple factors cause the decline in the meat quality of spent hens.Chinese herbs have been widely used as medi-cine for a long time to prevent diseases and as nutrient supplements to improve the product quality.This experi-ment explored the effects of adding 1.0%Chinese herbal formula(CHF,including 0.30%Leonurus japonicus Houtt.,0.20%Salvia miltiorrhiza Bge.,0.25%Ligustrum lucidum Ait.,and 0.25%Taraxacum mongolicum Hand.-Mazz.)for 120 d to the spent hens’diet through metabolomics,network pharmacology,and microbiome strategies.Results The results indicated that CHF supplementation improved the meat quality by reducing drip loss(P<0.05),b*value(P=0.058),and shear force(P=0.099)and increasing cooked meat percentage(P=0.054)and dry matter(P<0.05)of breast muscle.The addition of CHF improved the nutritional value of breast muscle by increasing(P<0.05)the content of C18:2n-6,n-6/n-3 polyunsaturated fatty acids(PUFA),total PUFA,PUFA-to-saturated fatty acids(SFA)ratio,and hypocholesterolemic-to-hypercholesterolemic ratio,and tending to increase serine content(P=0.069).The targeted metabolomics analysis revealed that the biosynthesis of SFA,linoleic acid metabolism,fatty acid degradation,fatty acid elongation,and fatty acid biosynthesis pathways were enriched by CHF supplementation.Furthermore,the network pharmacology analysis indicated that CHF was closely associated with oxidative stress and lipid metabo-lism.The CHF supplementation increased the glutathione peroxidase level(P<0.05)and upregulated gene expres-sion related to the Nrf2 pathway(including HO-1,P<0.05;Nrf2,P=0.098;CAT,P=0.060;GPX1,P=0.063;and SOD2,P=0.052)and lipid metabolism(including PPARγ,P<0.05;SREBP1,P=0.059;and CPT1A,P=0.058).Additionally,CHF supplementation increased Firmicutes and decreased Bacteroidetes,Spirochaetes,and Synergistetes abundances(P<0.05),which may contribute to better meat quality.Conclusions Our results suggest that CHF supplementation improved the quality and nutritional value of meat,which will provide a theoretical basis for the utilization of CHF as a feed additive in spent hens’diets.展开更多
Lithium-ion batteries(LIBs)are critical for the rapid growth of electric vehicles(EVs),but their inherent lifespan leads to numerous retirements and resource challenges.The efficacy of conventional recycling technique...Lithium-ion batteries(LIBs)are critical for the rapid growth of electric vehicles(EVs),but their inherent lifespan leads to numerous retirements and resource challenges.The efficacy of conventional recycling techniques is increasingly compromised by their high energy consumption and secondary pollution,rendering them less responsive to greener and more sustainable requirement of rapid development.Thus,the direct recycling process emerged and was considered as a more expedient and convenient method of recycling compared to the conventional recycling modes that are currently in study.However,due to the reliance on the indispensable sintering process,direct recycling still faces considerable challenges,motivating researchers to explore faster,greener,and more cost-effective strategies for LIBs recycling,Inspiringly,Joule heating recycling(JHR),an emerging technique,offers rapid,efficient impurity removal and material regeneration with minimal environmental impact,addressing limitations of existing methods.This method reduces the time for direct recycling of spent LIBs by a factor of at least three orders of magnitude and exhibits significant potential for future industrial production.Unfortunately,due to the lack of systematic organization and reporting,this next generation approach to direct recycling of spent LIBs has not yet gained much interest.To facilitate a more profound comprehension of rising flash recycling strategy,in this study,JHR is distinguished into two distinctive implementation pathways(including flash Joule heating and carbon thermal shock),designed to accommodate varying pretreatment stages and diverse spent LIBs materials.Subsequently,the advantages of the recently developed JHR of spent LIBs in terms of material performance,environmental friendliness,and economic viability are discussed in detail.Ultimately,with the goal of achieving more attractive society effects,the future direction of JHR of spent LIBs and its potential for practical application are proposed and envisaged.展开更多
The efficient recycling of spent lithium iron phosphate(LiFePO_(4),also referred to as LFP)should convert Fe(Ⅱ)to Fe(Ⅲ),which is key to the extraction of Li and separation of Fe and is not well understood.Herein,we ...The efficient recycling of spent lithium iron phosphate(LiFePO_(4),also referred to as LFP)should convert Fe(Ⅱ)to Fe(Ⅲ),which is key to the extraction of Li and separation of Fe and is not well understood.Herein,we systematically study the oxidation of LiFePO_(4)in the air and in the solution containing oxidants such as H_(2)O_(2)and the effect of oxidation on the leaching behaviors of LFP.In the air,O_(2)breaks down the LFP olivine structure at 550℃for 1 h by oxidizing Fe(Ⅱ)to Fe(Ⅲ)in terms of converting LFP to Li_(3)Fe_(2)(PO_(4))_(3)and Fe_(2)O_(3).After that,Li is leached in 0.5 M sulfuric acid solution and is further recycled as Li_(3)PO_(4)with a Li recovery efficiency of 97.48%.Meanwhile,Fe is recovered as FePO_(4)and Fe_(2)O_(3).Compared with H_(2)SO_(4)-H_(2)O_(2),the air oxidation saves H_(2)O_(2)but increases the leaching efficiency of Fe and H_(2)SO_(4)consumption.The discrepancy of Fe leaching efficiency can be attributed to the different leaching mechanisms involving the solid-to-solid and solid-to-liquid-to-solid conversions.Furthermore,the results of the Everbatt model analysis show that the air roasting-H_(2)SO_(4)leaching method has low emission and potentially high income,which is simple and safe.Overall,this work will deepen the understanding of acid leaching of LFP and favorably stimulate the maturation of the LFP recycling technique.展开更多
A tunable oxidization and reduction strategy was proposed to directly regenerate spent LiFePO_(4)/C cathode materials by oxidizing excessive carbon powders with the addition of FePO_(4).Experimental results indicate t...A tunable oxidization and reduction strategy was proposed to directly regenerate spent LiFePO_(4)/C cathode materials by oxidizing excessive carbon powders with the addition of FePO_(4).Experimental results indicate that spent LiFePO_(4)/C cathode materials with good performance can be regenerated by roasting at 650℃ for 11 h with the addition ofLi_(2)CO_(3),FePO_(4),V_(2)O_(5),and glucose.V_(2)O_(5) is added to improve the cycle performance of regenerated cathode materials.Glucose is used to revitalize the carbon layers on the surface of spent LiFePO_(4)/C particles for improving their conductivity.The regenerated V-doped LiFePO_(4)/C shows an excellent electrochemical performance with the discharge specific capacity of 161.36 mA·h/g at 0.2C,under which the capacity retention is 97.85%after 100 cycles.展开更多
For realizing the goals of“carbon peak”and“carbon neutrality”,lithium-ion batteries(LIB)with LiFePO_(4)as the cathode material have been widely applied.However,this has also led to a large number of spent lithium-...For realizing the goals of“carbon peak”and“carbon neutrality”,lithium-ion batteries(LIB)with LiFePO_(4)as the cathode material have been widely applied.However,this has also led to a large number of spent lithium-ion batteries,and the safe disposal of spent lithium-ion batteries is an urgent issue.Currently,the main reason for the capacity decay of LiFePO_(4)materials is the Li deficiency and the formation of the Fe^(3+)phase.In order to address this issue,we performed high-temperature calcination of the discarded lithium iron phosphate cathode material in a carbon dioxide environment to reduce or partially remove the carbon coating on its surface.Subsequently,mechanical grinding was conducted to ensure thorough mixing of the lithium source with the discarded lithium iron phosphate.The reaction between CO_(2)and the carbon coating produced a reducing atmosphere,reducing Fe^(3+)to Fe^(2+)and thereby reducing the content of Fe^(3+).The Fe^(3+)content in the repaired LiFePO_(4)material is reduced.The crystal structure of spent LiFePO_(4)cathode materials was repaired more completely compare with the traditional pretreatment method,and the repaired LiFePO_(4)material shows good electrochemical performance and cycling stability.Under 0.1 C conditions,the initial capacity can reach 149.1 m Ah/g.It can be reintroduced for commercial use.展开更多
With the continuous increase in the disposal volume of spent lithium-ion batteries(LIBs),properly recycling spent LIBs has become essential for the advancement of the circular economy.This study presents a systematic ...With the continuous increase in the disposal volume of spent lithium-ion batteries(LIBs),properly recycling spent LIBs has become essential for the advancement of the circular economy.This study presents a systematic analysis of the chlorination roasting kinetics and proposes a new two-step chlorination roasting process that integrates thermodynamics for the recycling of LIB cathode materials.The activation energy for the chloride reaction was 88.41 kJ/mol according to thermogravimetric analysis–derivative thermogravimetry data obtained by using model-free,model-fitting,and Z(α)function(αis conversion rate).Results indicated that the reaction was dominated by the first-order(F1)model when the conversion rate was less than or equal to 0.5 and shifted to the second-order(F2)model when the conversion rate exceeded 0.5.Optimal conditions were determined by thoroughly investigating the effects of roasting temperature,roasting time,and the mass ratio of NH_(4)Cl to LiCoO_(2).Under the optimal conditions,namely 400℃,20 min,and NH_(4)Cl/LiCoO_(2)mass ratio of 3:1,the leaching efficiency of Li and Co reached 99.43% and 99.05%,respectively.Analysis of the roasted products revealed that valuable metals in LiCoO_(2)transformed into CoCl_(2) and LiCl.Furthermore,the reaction mechanism was elucidated,providing insights for the establishment of a novel low-temperature chlorination roasting technology based on a crystal structure perspective.This technology can guide the development of LIB recycling processes with low energy consumption,low secondary pollution,high recovery efficiency,and high added value.展开更多
Hazardous wastes from the production of cleaner fuels,spent hydrodesulfurization(HDS)catalysts,pose a threat to the environment and the sustainability of rare metal resources.However,conventional recovery approaches a...Hazardous wastes from the production of cleaner fuels,spent hydrodesulfurization(HDS)catalysts,pose a threat to the environment and the sustainability of rare metal resources.However,conventional recovery approaches are limited by long processes,easy generation of waste liquids,and difficult reuse of recovery products.Herein,a SiO_(2)-Na_(2)O-B_(2)O_(3)-MgO-TiO_(2)glass phase extraction system was proposed for the full-component recycle from spent MoNi/γ-Al_(2)O_(3)catalysts to the materials,including the individual recovery of Mo and the synthesis of Ni^(2+)-doped glass–ceramics.96.7%of Ni and 99.8%of Al were extracted into the loaded glass in one step,while 95.3%of Mo was precipitated as molybdate and directly recovered with high separation factors(SF_(Mo/Ni)594.8,SF_(Mo/Al)8718.2)in one step.Moreover,the broadband near-infrared luminescence(1150-1700 nm)of glass–ceramics was triggered by Ni^(2+)in the octahedral crystal structure of Me_(3)O_(5)(Me=Mg,Al,Ti)by meltingannealing-crystallization processes,which provided it the potential to be applied in tunable lasers and broadband optical amplifiers for the wavelength-division-multiplexing transmission systems.The Ni^(2+)-doping mechanism was calculated using molecular dynamics simulations.This work emphasized the maximization of the reuse value for each metal resource from hazardous wastes while reducing the burden on the environment and achieving the recycling of rare metal resources with re-valorization.展开更多
PbS quantum dot(QD)image sensors have emerged as promising chips for a wide range of infrared(IR)imaging applications due to their monolithic integration with silicon-based readout integrated circuits.However,avoiding...PbS quantum dot(QD)image sensors have emerged as promising chips for a wide range of infrared(IR)imaging applications due to their monolithic integration with silicon-based readout integrated circuits.However,avoiding primary toxic Pb usage and reducing the cost of PbS QDs remains crucial for widespread application.We present a novel cost-effective and environmentally friendly hydrometallurgical process for recovering PbCl_(2)from spent lead-acid battery paste to synthesize high-quality PbS QDs.The method recovers PbCl_(2)with a production ratio of 97%and a purity of 99.99%.PbS QDs and photodetectors synthesized from recycled PbCl_(2)(R-PbCl_(2))have comparable performance and quality to those made using commercial PbCl_(2).R-PbCl_(2)-derived photodetectors exhibit a high external quantum efficiency of 49.6%and a high specific detectivity of 6.95×10^(12)Jones compared to published studies.Additionally,based on R-PbCl_(2),a PbS QD image sensor with 640×512 resolution successfully discriminated common solvents.Moreover,through life-cycle assessment and economic cost analysis,this novel synthesis route offers great advantages in the environmentally friendly use of chemical reagents and reduces the production cost of PbS QDs by 23.2%compared to commercial PbCl_(2).Thus,this work not only contributes to the green recycling of spent lead paste but also provides a low-cost strategy for synthesizing PbS QDs and their optoelectronic application.展开更多
This paper presented a novel and environmentally friendly approach for recovering platinum group metals(PGMs)from spent automotive exhaust catalysts.The study employed lead slag and waste graphite electrodes as raw ma...This paper presented a novel and environmentally friendly approach for recovering platinum group metals(PGMs)from spent automotive exhaust catalysts.The study employed lead slag and waste graphite electrodes as raw materials,incorporating CaO as an additive to fine-tune the slag's viscosity and density.By reducing FeO in the lead slag using waste graphite electrodes,pure Fe was obtained,effectively trapping the PGMs from the exhausted catalysts.The study explored the effects of reductant addition,trapping duration,slag basicity,and trapping temperature on the recovery rate of PGMs.The results indicated that a maximum recovery rate of 97.86%was achieved when the reductant was added at 1.5 times the theoretical amount,with a trapping duration of 60 minutes,a slag basicity of 0.7,and a trapping temperature of 1600℃.This research offered a greener pathway for the recovery of PGMs from spent automotive exhaust catalysts.展开更多
The industrial-grade black mass of LiFePO_(4)/LiNixMnyO_(4)/C from spent lithium-ion battery is difficult to be recovered because of its complex composition.In this study,a recycling of graphite and comprehensive reco...The industrial-grade black mass of LiFePO_(4)/LiNixMnyO_(4)/C from spent lithium-ion battery is difficult to be recovered because of its complex composition.In this study,a recycling of graphite and comprehensive recovery of valuable metals from industrial-grade black mass of spent lithium-ion battery was proposed.Acid leaching can separate graphite and cathode materials well.The separated graphite was purified by roasting,and its electrochemical properties were tested.The specific discharge capacity of graphite purified at 600◦are the best,which reach 342.46 mA·h·g^(-1)at 0.1 C.After 50 cycles at 0.1 C,the capacity retention rate was 98.26%.The charge-discharge cycle stability was improved at high rates.Nearly 100%of copper can be recovered from leaching solution by electrodeposition.FePO_(4)·2H_(2)O is recovered by adjusting the pH of the solution to 2,andα-FePO_(4) is obtained by roasting.Ni,Mn and Li can be recovered by precipitation separation.The optimum conditions for the recovery process was determined,and the mechanisms of the leaching and electrodeposition process were characterized by XRD,XPS,SEM-EDS.展开更多
This study addresses the global problem of the detoxification of cadmium(Cd)-containing solid waste by developing an eco-friendly thiosulfate system for extracting the negative electrode materials from spent Ni–Cd ba...This study addresses the global problem of the detoxification of cadmium(Cd)-containing solid waste by developing an eco-friendly thiosulfate system for extracting the negative electrode materials from spent Ni–Cd batteries and proposing an ultraviolet(UV)photolysis technology for the green recycling of the Cd in the resultant leached solution.Cd extraction is performed using both simple thiosulfate and cuprous thiosulfate systems,with the cuprous thiosulfate system exhibiting a superior leaching performance(80%),as compared with that of the simple thiosulfate system(36%).X-ray diffraction(XRD)and X-ray photoelectron spectroscopy(XPS)analyses reveal the formation of copper sulfide on the surface of the Ni–Cd batteries leaching residue,which is confirmed by Cdleaching kinetics fitting using the shrinking-core model.Following UV exposure,95%of the Cd precipitates from the leaching solution to form CdS.Transmission electron microscopy(TEM)characterization and particle size distribution reveal that the CdS contains 100–150 nm-diameter spherical particles with compact surface structures.Electrochemical performance tests and UV–visible diffuse reflectance spectra(UV–Vis DRS)analyses demonstrate that the UV-photolysis product exhibits excellent photoelectric conversion characteristics.Photocatalytic activity tests of the recovered CdS confirm that the photocatalytic degradation ratio of methyl orange is 87%,indicating the successful green recycling of Cd from spent Ni–Cd batteries,which improves its potential application in the field of photocatalysis.展开更多
With large-scale commercial applications of lithium-ion batteries(LIBs),lots of spent LIBs will be produced and cause huge waste of resources and greatly increased environmental problems.Thus,recycling spent LIB mater...With large-scale commercial applications of lithium-ion batteries(LIBs),lots of spent LIBs will be produced and cause huge waste of resources and greatly increased environmental problems.Thus,recycling spent LIB materials is inevitable.Due to high added-value features,converting spent LIB cathode materials into catalysts exhibits broad application prospects.Inspired by this,we review the high-added-value reutilization of spent LIB materials toward catalysts of energy conversion.First,the failure mechanism of spent LIB cathode materials are discussed,and then the transformation and modification strategies are summarized and analyzed to improve the transformation efficiency of failed cathode materials and the catalytic performance of catalysts,respectively.Moreover,the electrochemical applications of failed cathode material derived catalysts are introduced,and the key problems and countermeasures are analyzed and proposed.Finally,the future development trend and prospect of high-added-value reutilization for spent LIB cathode materials toward catalysts are also given.This review will predictably advance the awareness of valorizing spent lithium-ion battery cathode materials for catalysis.展开更多
Lithium iron phosphate(LFP)batteries,boasting significant advantages in cost-effectiveness,safety,and longevity,are extensively utilized as the core components for electric vehicles.However,with the increasing end-ofl...Lithium iron phosphate(LFP)batteries,boasting significant advantages in cost-effectiveness,safety,and longevity,are extensively utilized as the core components for electric vehicles.However,with the increasing end-oflife of LFP batteries,the recycling of these spent batteries has become a crucial and urgent matter.Given the relatively short process and high-value-added recycled products,the direct regeneration of cathode materials from spent LFP batteries has become a highly preferred approach.This paper provides a comprehensive review of the research status and technical challenges of direct regeneration technologies(i.e.,solid-phase sintering,hydrothermal repair and electrochemical repair technology)applicable to spent LFP cathode materials.The failure mechanisms of LFP,as well as the detailed processes and recent advancements in recycling pretreatment are elaborated and summarized.Additionally,this paper extends to introduce the research advancements in innovative upgrading regeneration of cathode materials.Finally,a comparative analysis of the three direct regeneration strategies is conducted,emphasizing their respective advantages,limitations,and target application fields.It is anticipated to establish a comprehensive reference framework for the efficient regeneration and reuse of cathode materials from spent LFP batteries,thus promoting the green and sustainable development of the new energy vehicle industry.展开更多
In view of the difference in coordination capacity of the glycine ion(Gly−),a selective leaching process for treating with spent lithium-ion batteries(LIBs)in the alkaline glycinate system was proposed.The effects of ...In view of the difference in coordination capacity of the glycine ion(Gly−),a selective leaching process for treating with spent lithium-ion batteries(LIBs)in the alkaline glycinate system was proposed.The effects of retention time,leaching temperature,concentration of glycine ligand,liquid-solid ratio(L/S),pH,stirring speed,and H_(2)O_(2) dosage on the leaching efficiency of valuable metals and the dissolution of impurities were investigated.When the spent LIBs were leached in 3 mol/L glycine aqueous solution with pH of 8,L/S of 5 mL:1 g and H_(2)O_(2) dosage of 5 vol.%at 90℃and stirring speed of 400 r/min for 3 h,lithium,cobalt,nickel,and manganese recoveries were 96.31%,83.18%,91.56%,and 31.16%,respectively,but Ca,Al,Fe,and Cu were almost insoluble.Meanwhile,the kinetic study showed that the activation energies for the leaching of Li,Co,Ni,and Mn were all in the range of 45−61 kJ/mol.The results indicate that the leaching process is all controlled by chemical reactions.展开更多
基金funded by the National Key Research and Development Program of China(grant no.2023YFB3809300)Longzhong Laboratory Research Project(grant no.2024KF-20)+4 种基金the National Science Foundation of China(grant no.52373306)the Key Research and Development Program Project of Hubei Province(grant no.2023BAB140,2024BAA013)the Natural Science Foundation of Hubei Province(grant no.2023AFA053)the Key Research and Development Program of Henan Province(grant no.251111240100)the Postdoctoral Fellowship Program of CPSF(grant no.GZB20230553)。
文摘The extensive application of lithium-ion batteries in electric vehicles has led to a torrential surge of endof-life batteries.As the dominant anode material,graphite's environmental and resource costs in production highlight the necessity of recycling spent graphite(SG).However,SG recycling technologies remain markedly underdeveloped compared to the cathode recovery status,due to perceived lower economic value.This review provides an in-depth analysis of the current SG growth trend and highlights the cost accounting for graphite recycling and the significant importance of advanced recycling technologies.By examining the failure mechanisms of graphite,various recycling and upcycling technologies in both practical application and fundamental research are fully discussed,in terms of the regeneration principle,recycling effect,strengths,and limitations of each method.Furthermore,the multi-purpose applications of recycled graphite beyond LIB anodes are explored to enhance its high-value properties.Finally,the prospects of SG recycling and large-scale application challenges are presented,including economic feasibility,process optimization,and regulatory restrictions.This review provides a comprehensive overview of developments in SG recycling strategies,offering valuable insights for narrowing the gap between fundamental research and practical applications.
基金supported by the National Natural Science Foundation of China(Project Nos.22372051 and 21406044)Australian Research Council/Discovery Early Career Researcher Award(DECRA)funding scheme(DE230100180).
文摘The impurities and structural cracks within spent graphite(SG)in lithium-ion battery anodes hamper lithium-ion intercalation and extraction after successive charge-discharge operations,thereby yielding poor lithium storage behavior.Herein,low-viscosity natural deep eutectic solvent(NDES)composed of citric acid(CA)and betaine hydrochloride was employed to remove the organic impurities in SG via a one-step benign process involving hydrogen bonds and electrostatic interactions at mild conditions of 80℃ for only 30 min.After NDES leaching under optimal conditions(molar ratio of CA to betaine hydrochloride=3:1,80℃,30 min),the as-obtained sample(denoted as BG-3)exhibited an extremely clean surface,moderately enlarged interlayer distance,and more structural defects at the edge of graphite lamellae.These features facilitated lithium-ion intercalation and withdrawal,bestowing BG-3 with remarkable activity in lithium-ion battery(LIB)recycling.For instance,BG-3 delivered a capacity of 438.6 mAh g^(-1) at a current density of 0.1 A g^(-1).Its capacity retention reached 97.9%,accompanied by a Coulombic efficiency of 99.1%,upon completing 100 cycles.A molecular dynamics simulation was employed to illuminate the regeneration mechanism for anode graphite from a theoretical perspective.It revealed that NDES exhibits lower binding energy with all contaminants compared to graphite,which is favorable for NDES to eliminate impurities from graphite surfaces.This study unveils a method of recycling SG from retired LIBs by a short eco-friendly process,providing a competitive blueprint to address the shortage of battery-grade anode graphite and to achieve carbon neutrality.
基金supported by the National Key Research and Development Program of China(2023YFB3809300).
文摘Recycling spent lithium-ion(Li+)batteries is critical for achieving environmental conservation and the strategic recovery of essential resources.Compared with conventional methods for recovering cathode materials,which are energy-intensive and prone to secondary pollution,the direct regeneration approach has emerged as a rapid and highly efficient method,gaining widespread attention in recent years.However,this approach faces major challenges,including degraded electrochemical performances and limited economic value.This study,therefore,proposes a high-value direct regeneration strategy to convert degraded spent LiFePO_(4)(S-LFP)into a gradient manganese(Mn)-doped regenerated LiFe_(0.7)Mn_(0.3)PO_(4)/C(R-LFMP)composite.This method leverages the inherent microcracks and Li vacancies present in S-LFP,likely acting as diffusion channels for the Mn^(2+)/Li^(+)ions.Through a two-step mechanochemical ball-milling and carbothermal reduction process,this approach achieves simultaneous Li replenishment and surface-localised Mn gradient doping with enhanced structural control.Notably,the R-LFMP exhibits an exceptional electrochemical performance.At 0.1 C,it delivers a discharge capacity of 161.4 mA h g^(−1)and an energy density of 563.5 Wh kg^(−1)(representing a 60.5%improvement over S-LFP).Additionally,it maintains 83%capacity retention after 900 cycles at 0.5C,a considerable enhancement compared to commercial LFMP(62%).Furthermore,the regenerated cathode material generates a net profit of$7.102 kg^(−1),surpassing the profitability of conventional recycling methods by 90%.Overall,this study introduces a transformative and sustainable LFP regeneration technology,achieving breakthroughs in electrochemical restoration and high-value recycling,while paving the way for the closed-loop utilisation of LFP-based energy storage systems.
基金financial support from the National Key R&D Program of China(2022YFB2402600)the National Natural Science Foundation of China(52372250,52125105,52173242)+1 种基金Shenzhen Science and Technology Planning Project(RCYX20221008092850072,JSGG20220831104004008,KJZD20230923113859006,JCYJ20220531100405012,KJZD20241122161900001)Science and Technology Planning Project of Guangdong Province(2024A1515030076)。
文摘The rapid accumulation of spent LiFePO_(4)(LFP)cathodes from retired lithium-ion batteries necessitates the development of effective and environmental-friendly recycling strategies.In this context,direct regeneration has emerged as a promising approach for reclaiming LFP cathode materials,offering a streamlined pathway to restore their electrochemical functionality.We report an integrated regeneration protocol that simultaneously repairs the degraded crystal structure and reconstructs the damaged carbon coating in spent LFP.The regenerated cathode material had superfast lithium-ion diffusion kinetics and a stable cathode-electrolyte interface,giving a remarkable rate capability with specific capacities of 122 m Ah g^(-1)at 5C and 106 m Ah g^(-1)at 10C(1C=170 m A g^(-1)).It also maintained capacities of 110.7 m Ah g^(-1)(5C)and 84.1 m Ah g^(-1)(10C)after 400 cycles.It could be used in harsh environments and could be stably cycled at subzero temperatures(-10 and-20°C)and in solid-state electrolyte batteries.Life cycle assessment combined with economic evaluation using the Ever Batt model reveals that this direct regeneration approach has high economic and environmental benefits.
基金funded by the National Natural Science Foundation of China Youth Fund Project(52002371 and 52204425)National Key Research and Development Program Solid Waste Resource Utilization Project(2018YFC1901504).
文摘The pyrometallurgy combined with hydrometallurgy process is commonly used for recovering valuable elements from spent lithium-ion batteries.To improve the corrosion resistance of heat treatment furnace lining materials in this process,SiC-Si_(3)N_(4)-C composite refractories were prepared by heat-treating at 800-1400℃ for 3 h,using fine particles of spent iron ladle bricks(1-0.5 and<0.5 mm),silicon carbide(2-1,1-0.5,and<0.5 mm),silicon nitride(<0.045 mm),and graphite as raw materials.The fine particles of spent iron ladle bricks were used to replace silicon nitride with the same particle size.The effects of the spent iron ladle brick fine particles additions(0,12.12%,26.25%,36.38%and 48.5%,by mass)and the heat treatment temperatures(800,1000,1200 and 1400℃)on the properties of the composite refractories were studied.The results show that:(1)with the<1 mm spent iron ladle brick fine particles addition increasing,the bulk density of the samples changes slightly,the apparent porosity gradually decreases,the cold modulus of rupture(CMOR)increases,and the cold compressive strength(CCS)first decreases,then increases and finally decreases slightly;(2)with the heat treatment temperature rising,the bulk density of the samples first increases and then decreases,the apparent porosity gradually decreases,and the CCS and the CMOR increase;(3)when the temperature is 1400℃ and the spent iron ladle brick fine particles completely replace the silicon nitride fine particles with the same particle size,the sample exhibits the best comprehensive performance,with the bulk density of 2.37 g·cm^(-3),apparent porosity of 14.3%,CCS of 31.6 MPa,and CMOR of 9.0 MPa,and it has a good resistance to the corrosion of crushed spent lithium-ion battery materials at 1000℃.
基金financial support by the National Natural Science Foundation of China(No.52374293)Zhongyuan Science and Technology Innovation Leading Talent Project,China(No.224200510025)+1 种基金the Science and Technology Innovation Program of Hunan Province,China(No.2022RC1123)One of the authors,Hong-bo ZENG,gratefully acknowledges the support from the Natural Sciences and Engineering Research Council of Canada(NSERC)and the Canada Research Chairs Program.
文摘Lithium-ion batteries(LIBs)are the most popular energy storage devices due to their high energy density,high operating voltage,and long cycle life.However,green and effective recycling methods are needed because LIBs contain heavy metals such as Co,Ni,and Mn and organic compounds inside,which seriously threaten human health and the environment.In this work,we review the current status of spent LIB recycling,discuss the traditional pyrometallurgical and hydrometallurgical recovery processes,and summarize the existing short-process recovery technologies such as salt-assisted roasting,flotation processes,and direct recycling.Finally,we analyze the problems and potential research prospects of the current recycling process,and point out that the multidisciplinary integration of recycling will become the mainstream technology for the development of spent LIBs.
基金supported by the National Key Research and Development Project(2022YFC3400700)the City-School Cooperation Project of the Fuyang Science and Technology Special Fund undertaken by Fuyang Normal University(SXHZ2020007)+1 种基金the Basic Research Program of Shenzhen Municipal Government(JCYJ20200109114242138)the Special Commissioner for Rural Science and Technology of Guangdong Province(KTP20210345).
文摘Background Meat originating from the spent hen is an important source of poultry meat production;however,multiple factors cause the decline in the meat quality of spent hens.Chinese herbs have been widely used as medi-cine for a long time to prevent diseases and as nutrient supplements to improve the product quality.This experi-ment explored the effects of adding 1.0%Chinese herbal formula(CHF,including 0.30%Leonurus japonicus Houtt.,0.20%Salvia miltiorrhiza Bge.,0.25%Ligustrum lucidum Ait.,and 0.25%Taraxacum mongolicum Hand.-Mazz.)for 120 d to the spent hens’diet through metabolomics,network pharmacology,and microbiome strategies.Results The results indicated that CHF supplementation improved the meat quality by reducing drip loss(P<0.05),b*value(P=0.058),and shear force(P=0.099)and increasing cooked meat percentage(P=0.054)and dry matter(P<0.05)of breast muscle.The addition of CHF improved the nutritional value of breast muscle by increasing(P<0.05)the content of C18:2n-6,n-6/n-3 polyunsaturated fatty acids(PUFA),total PUFA,PUFA-to-saturated fatty acids(SFA)ratio,and hypocholesterolemic-to-hypercholesterolemic ratio,and tending to increase serine content(P=0.069).The targeted metabolomics analysis revealed that the biosynthesis of SFA,linoleic acid metabolism,fatty acid degradation,fatty acid elongation,and fatty acid biosynthesis pathways were enriched by CHF supplementation.Furthermore,the network pharmacology analysis indicated that CHF was closely associated with oxidative stress and lipid metabo-lism.The CHF supplementation increased the glutathione peroxidase level(P<0.05)and upregulated gene expres-sion related to the Nrf2 pathway(including HO-1,P<0.05;Nrf2,P=0.098;CAT,P=0.060;GPX1,P=0.063;and SOD2,P=0.052)and lipid metabolism(including PPARγ,P<0.05;SREBP1,P=0.059;and CPT1A,P=0.058).Additionally,CHF supplementation increased Firmicutes and decreased Bacteroidetes,Spirochaetes,and Synergistetes abundances(P<0.05),which may contribute to better meat quality.Conclusions Our results suggest that CHF supplementation improved the quality and nutritional value of meat,which will provide a theoretical basis for the utilization of CHF as a feed additive in spent hens’diets.
基金financially supported by the National Key Research and Development Program of China(No.2023YFC3904800)the National Outstanding Young Scientists Fund(No.5a2125002)+7 种基金the National Science Foundation of China(No.22476073)the Key Project of Jiangxi Provincial Research and Development Program(Nos.20223BBG74006 and 20243BBI91001)the China Postdoctoral Science Foundation(No.2024M751282)the “Thousand Talents Program”of Jiangxi Province(S_(2)021GDQN2161)the Key Project of Ganzhou City Research and Development Program(No.2023PGX17350)the Science&Technology Talent Lifting Project of Hunan Province(No.2022TJ-N16)the Natural Science Foundation of Hunan Province China(No.2024JJ4022,2023JJ30277)the Open-End Fund for National-Local Joint Engineering Research Center of Heavy Metals Pollutants Control and Resource Utilization(ES_(2)02480184)。
文摘Lithium-ion batteries(LIBs)are critical for the rapid growth of electric vehicles(EVs),but their inherent lifespan leads to numerous retirements and resource challenges.The efficacy of conventional recycling techniques is increasingly compromised by their high energy consumption and secondary pollution,rendering them less responsive to greener and more sustainable requirement of rapid development.Thus,the direct recycling process emerged and was considered as a more expedient and convenient method of recycling compared to the conventional recycling modes that are currently in study.However,due to the reliance on the indispensable sintering process,direct recycling still faces considerable challenges,motivating researchers to explore faster,greener,and more cost-effective strategies for LIBs recycling,Inspiringly,Joule heating recycling(JHR),an emerging technique,offers rapid,efficient impurity removal and material regeneration with minimal environmental impact,addressing limitations of existing methods.This method reduces the time for direct recycling of spent LIBs by a factor of at least three orders of magnitude and exhibits significant potential for future industrial production.Unfortunately,due to the lack of systematic organization and reporting,this next generation approach to direct recycling of spent LIBs has not yet gained much interest.To facilitate a more profound comprehension of rising flash recycling strategy,in this study,JHR is distinguished into two distinctive implementation pathways(including flash Joule heating and carbon thermal shock),designed to accommodate varying pretreatment stages and diverse spent LIBs materials.Subsequently,the advantages of the recently developed JHR of spent LIBs in terms of material performance,environmental friendliness,and economic viability are discussed in detail.Ultimately,with the goal of achieving more attractive society effects,the future direction of JHR of spent LIBs and its potential for practical application are proposed and envisaged.
基金supported by the Chilwee Group(No.CWDY-ZH-YJY-202101-001)the Fundamental Research Funds for the Central Universities(No.2042023kf0214)the Starting Funding from Wuhan University.
文摘The efficient recycling of spent lithium iron phosphate(LiFePO_(4),also referred to as LFP)should convert Fe(Ⅱ)to Fe(Ⅲ),which is key to the extraction of Li and separation of Fe and is not well understood.Herein,we systematically study the oxidation of LiFePO_(4)in the air and in the solution containing oxidants such as H_(2)O_(2)and the effect of oxidation on the leaching behaviors of LFP.In the air,O_(2)breaks down the LFP olivine structure at 550℃for 1 h by oxidizing Fe(Ⅱ)to Fe(Ⅲ)in terms of converting LFP to Li_(3)Fe_(2)(PO_(4))_(3)and Fe_(2)O_(3).After that,Li is leached in 0.5 M sulfuric acid solution and is further recycled as Li_(3)PO_(4)with a Li recovery efficiency of 97.48%.Meanwhile,Fe is recovered as FePO_(4)and Fe_(2)O_(3).Compared with H_(2)SO_(4)-H_(2)O_(2),the air oxidation saves H_(2)O_(2)but increases the leaching efficiency of Fe and H_(2)SO_(4)consumption.The discrepancy of Fe leaching efficiency can be attributed to the different leaching mechanisms involving the solid-to-solid and solid-to-liquid-to-solid conversions.Furthermore,the results of the Everbatt model analysis show that the air roasting-H_(2)SO_(4)leaching method has low emission and potentially high income,which is simple and safe.Overall,this work will deepen the understanding of acid leaching of LFP and favorably stimulate the maturation of the LFP recycling technique.
基金National Natural Science Foundation of China(Nos.52174269,52374293)Science and Technology Innovation Program of Hunan Province,China(Nos.2024CK1009,2022RC1123)。
文摘A tunable oxidization and reduction strategy was proposed to directly regenerate spent LiFePO_(4)/C cathode materials by oxidizing excessive carbon powders with the addition of FePO_(4).Experimental results indicate that spent LiFePO_(4)/C cathode materials with good performance can be regenerated by roasting at 650℃ for 11 h with the addition ofLi_(2)CO_(3),FePO_(4),V_(2)O_(5),and glucose.V_(2)O_(5) is added to improve the cycle performance of regenerated cathode materials.Glucose is used to revitalize the carbon layers on the surface of spent LiFePO_(4)/C particles for improving their conductivity.The regenerated V-doped LiFePO_(4)/C shows an excellent electrochemical performance with the discharge specific capacity of 161.36 mA·h/g at 0.2C,under which the capacity retention is 97.85%after 100 cycles.
基金supported by Heilongjiang Province Key R&D Program(No.GA22A014)。
文摘For realizing the goals of“carbon peak”and“carbon neutrality”,lithium-ion batteries(LIB)with LiFePO_(4)as the cathode material have been widely applied.However,this has also led to a large number of spent lithium-ion batteries,and the safe disposal of spent lithium-ion batteries is an urgent issue.Currently,the main reason for the capacity decay of LiFePO_(4)materials is the Li deficiency and the formation of the Fe^(3+)phase.In order to address this issue,we performed high-temperature calcination of the discarded lithium iron phosphate cathode material in a carbon dioxide environment to reduce or partially remove the carbon coating on its surface.Subsequently,mechanical grinding was conducted to ensure thorough mixing of the lithium source with the discarded lithium iron phosphate.The reaction between CO_(2)and the carbon coating produced a reducing atmosphere,reducing Fe^(3+)to Fe^(2+)and thereby reducing the content of Fe^(3+).The Fe^(3+)content in the repaired LiFePO_(4)material is reduced.The crystal structure of spent LiFePO_(4)cathode materials was repaired more completely compare with the traditional pretreatment method,and the repaired LiFePO_(4)material shows good electrochemical performance and cycling stability.Under 0.1 C conditions,the initial capacity can reach 149.1 m Ah/g.It can be reintroduced for commercial use.
基金financially supported by the National Natural Science Foundation of China(No.52204310)the Guizhou Provincial Key Laboratory of Coal Clean Utilization(No.[2020]2001)+5 种基金the China Postdoctoral Science Foundation(Nos.2020TQ0059 and 2020M570967)the Natural Science Foundation of Liaoning Province(No.2021–MS–083)the Fundamental Research Funds for the Central Universities,China(No.N2125010)the Open Project Program of Key Laboratory of Metallurgical Emission Reduction&Resources Recycling(Anhui University of Technology),Ministry of Education(No.JKF22–02)the Foundation of Liupanshui Normal University(No.LPSSYZDZK202205)the Key Laboratory for Anisotropy and Texture of Materials,Ministry of Education,China。
文摘With the continuous increase in the disposal volume of spent lithium-ion batteries(LIBs),properly recycling spent LIBs has become essential for the advancement of the circular economy.This study presents a systematic analysis of the chlorination roasting kinetics and proposes a new two-step chlorination roasting process that integrates thermodynamics for the recycling of LIB cathode materials.The activation energy for the chloride reaction was 88.41 kJ/mol according to thermogravimetric analysis–derivative thermogravimetry data obtained by using model-free,model-fitting,and Z(α)function(αis conversion rate).Results indicated that the reaction was dominated by the first-order(F1)model when the conversion rate was less than or equal to 0.5 and shifted to the second-order(F2)model when the conversion rate exceeded 0.5.Optimal conditions were determined by thoroughly investigating the effects of roasting temperature,roasting time,and the mass ratio of NH_(4)Cl to LiCoO_(2).Under the optimal conditions,namely 400℃,20 min,and NH_(4)Cl/LiCoO_(2)mass ratio of 3:1,the leaching efficiency of Li and Co reached 99.43% and 99.05%,respectively.Analysis of the roasted products revealed that valuable metals in LiCoO_(2)transformed into CoCl_(2) and LiCl.Furthermore,the reaction mechanism was elucidated,providing insights for the establishment of a novel low-temperature chlorination roasting technology based on a crystal structure perspective.This technology can guide the development of LIB recycling processes with low energy consumption,low secondary pollution,high recovery efficiency,and high added value.
基金financially supported by the National Natural Science Foundation of China for Distinguished Young Scholar(No.52025042)。
文摘Hazardous wastes from the production of cleaner fuels,spent hydrodesulfurization(HDS)catalysts,pose a threat to the environment and the sustainability of rare metal resources.However,conventional recovery approaches are limited by long processes,easy generation of waste liquids,and difficult reuse of recovery products.Herein,a SiO_(2)-Na_(2)O-B_(2)O_(3)-MgO-TiO_(2)glass phase extraction system was proposed for the full-component recycle from spent MoNi/γ-Al_(2)O_(3)catalysts to the materials,including the individual recovery of Mo and the synthesis of Ni^(2+)-doped glass–ceramics.96.7%of Ni and 99.8%of Al were extracted into the loaded glass in one step,while 95.3%of Mo was precipitated as molybdate and directly recovered with high separation factors(SF_(Mo/Ni)594.8,SF_(Mo/Al)8718.2)in one step.Moreover,the broadband near-infrared luminescence(1150-1700 nm)of glass–ceramics was triggered by Ni^(2+)in the octahedral crystal structure of Me_(3)O_(5)(Me=Mg,Al,Ti)by meltingannealing-crystallization processes,which provided it the potential to be applied in tunable lasers and broadband optical amplifiers for the wavelength-division-multiplexing transmission systems.The Ni^(2+)-doping mechanism was calculated using molecular dynamics simulations.This work emphasized the maximization of the reuse value for each metal resource from hazardous wastes while reducing the burden on the environment and achieving the recycling of rare metal resources with re-valorization.
基金supported by Key program of National Natural Science Foundation of China(52330004)National Natural Science Foundation of China General Project(51978301)National Key Research and Development Program of China(2023YFC3902802)。
文摘PbS quantum dot(QD)image sensors have emerged as promising chips for a wide range of infrared(IR)imaging applications due to their monolithic integration with silicon-based readout integrated circuits.However,avoiding primary toxic Pb usage and reducing the cost of PbS QDs remains crucial for widespread application.We present a novel cost-effective and environmentally friendly hydrometallurgical process for recovering PbCl_(2)from spent lead-acid battery paste to synthesize high-quality PbS QDs.The method recovers PbCl_(2)with a production ratio of 97%and a purity of 99.99%.PbS QDs and photodetectors synthesized from recycled PbCl_(2)(R-PbCl_(2))have comparable performance and quality to those made using commercial PbCl_(2).R-PbCl_(2)-derived photodetectors exhibit a high external quantum efficiency of 49.6%and a high specific detectivity of 6.95×10^(12)Jones compared to published studies.Additionally,based on R-PbCl_(2),a PbS QD image sensor with 640×512 resolution successfully discriminated common solvents.Moreover,through life-cycle assessment and economic cost analysis,this novel synthesis route offers great advantages in the environmentally friendly use of chemical reagents and reduces the production cost of PbS QDs by 23.2%compared to commercial PbCl_(2).Thus,this work not only contributes to the green recycling of spent lead paste but also provides a low-cost strategy for synthesizing PbS QDs and their optoelectronic application.
基金Funded by the Natural Science Foundation of Henan(No.252300421563)the Key Research Projects of Henan Provincial Colleges and Universities(No.25B450001)+3 种基金the Basic and Frontier Research Project of Nanyang(No.24JCQY032)National Natural Science Foundation of China(No.52201044)the Key Specialized Research&Development and Promotion Project(Scientific and Technological Project)of Henan Province(No.232102221022)the Basic and Frontier Technology Research Project of Nanyang(No.23JCQY1001)。
文摘This paper presented a novel and environmentally friendly approach for recovering platinum group metals(PGMs)from spent automotive exhaust catalysts.The study employed lead slag and waste graphite electrodes as raw materials,incorporating CaO as an additive to fine-tune the slag's viscosity and density.By reducing FeO in the lead slag using waste graphite electrodes,pure Fe was obtained,effectively trapping the PGMs from the exhausted catalysts.The study explored the effects of reductant addition,trapping duration,slag basicity,and trapping temperature on the recovery rate of PGMs.The results indicated that a maximum recovery rate of 97.86%was achieved when the reductant was added at 1.5 times the theoretical amount,with a trapping duration of 60 minutes,a slag basicity of 0.7,and a trapping temperature of 1600℃.This research offered a greener pathway for the recovery of PGMs from spent automotive exhaust catalysts.
基金the Shandong Provincial Natural Science Foundation,China(ZR2022MB129)for the financial support。
文摘The industrial-grade black mass of LiFePO_(4)/LiNixMnyO_(4)/C from spent lithium-ion battery is difficult to be recovered because of its complex composition.In this study,a recycling of graphite and comprehensive recovery of valuable metals from industrial-grade black mass of spent lithium-ion battery was proposed.Acid leaching can separate graphite and cathode materials well.The separated graphite was purified by roasting,and its electrochemical properties were tested.The specific discharge capacity of graphite purified at 600◦are the best,which reach 342.46 mA·h·g^(-1)at 0.1 C.After 50 cycles at 0.1 C,the capacity retention rate was 98.26%.The charge-discharge cycle stability was improved at high rates.Nearly 100%of copper can be recovered from leaching solution by electrodeposition.FePO_(4)·2H_(2)O is recovered by adjusting the pH of the solution to 2,andα-FePO_(4) is obtained by roasting.Ni,Mn and Li can be recovered by precipitation separation.The optimum conditions for the recovery process was determined,and the mechanisms of the leaching and electrodeposition process were characterized by XRD,XPS,SEM-EDS.
基金financially supported by the National Natural Science Foundation of China(No.52104349)Henan Provincial Science and Technology R&D Plan Joint Fund Project(No.232103810032)+1 种基金the Funds for HAUST Young Cadre Teacher(No.400213450022)supporting by China Postdoctoral Science Foundation(No.2022M721031)。
文摘This study addresses the global problem of the detoxification of cadmium(Cd)-containing solid waste by developing an eco-friendly thiosulfate system for extracting the negative electrode materials from spent Ni–Cd batteries and proposing an ultraviolet(UV)photolysis technology for the green recycling of the Cd in the resultant leached solution.Cd extraction is performed using both simple thiosulfate and cuprous thiosulfate systems,with the cuprous thiosulfate system exhibiting a superior leaching performance(80%),as compared with that of the simple thiosulfate system(36%).X-ray diffraction(XRD)and X-ray photoelectron spectroscopy(XPS)analyses reveal the formation of copper sulfide on the surface of the Ni–Cd batteries leaching residue,which is confirmed by Cdleaching kinetics fitting using the shrinking-core model.Following UV exposure,95%of the Cd precipitates from the leaching solution to form CdS.Transmission electron microscopy(TEM)characterization and particle size distribution reveal that the CdS contains 100–150 nm-diameter spherical particles with compact surface structures.Electrochemical performance tests and UV–visible diffuse reflectance spectra(UV–Vis DRS)analyses demonstrate that the UV-photolysis product exhibits excellent photoelectric conversion characteristics.Photocatalytic activity tests of the recovered CdS confirm that the photocatalytic degradation ratio of methyl orange is 87%,indicating the successful green recycling of Cd from spent Ni–Cd batteries,which improves its potential application in the field of photocatalysis.
基金supported by the National Key Research and Development Program of China(No.2023YFB3809300).
文摘With large-scale commercial applications of lithium-ion batteries(LIBs),lots of spent LIBs will be produced and cause huge waste of resources and greatly increased environmental problems.Thus,recycling spent LIB materials is inevitable.Due to high added-value features,converting spent LIB cathode materials into catalysts exhibits broad application prospects.Inspired by this,we review the high-added-value reutilization of spent LIB materials toward catalysts of energy conversion.First,the failure mechanism of spent LIB cathode materials are discussed,and then the transformation and modification strategies are summarized and analyzed to improve the transformation efficiency of failed cathode materials and the catalytic performance of catalysts,respectively.Moreover,the electrochemical applications of failed cathode material derived catalysts are introduced,and the key problems and countermeasures are analyzed and proposed.Finally,the future development trend and prospect of high-added-value reutilization for spent LIB cathode materials toward catalysts are also given.This review will predictably advance the awareness of valorizing spent lithium-ion battery cathode materials for catalysis.
基金financially supported by the National Natural Science Foundation of China(Nos.52374281,52204287,92475001)the National Key Research and Development Program of China(No.2023YFC2908301)+4 种基金the National Major Science and Technology Projects of China(No.2024ZD1004007)the Postdoctoral Fellowship Program of CPSF(No.GZC20232398)the China Postdoctoral Science Foundation(No.2023TQ0302)the Research Startup Fund of Zhengzhou University(No.32213512)the Project of Zhongyuan Critical Metals Laboratory(Nos.GJJSGFYQ202316 and GJJSGFYQ202322)
文摘Lithium iron phosphate(LFP)batteries,boasting significant advantages in cost-effectiveness,safety,and longevity,are extensively utilized as the core components for electric vehicles.However,with the increasing end-oflife of LFP batteries,the recycling of these spent batteries has become a crucial and urgent matter.Given the relatively short process and high-value-added recycled products,the direct regeneration of cathode materials from spent LFP batteries has become a highly preferred approach.This paper provides a comprehensive review of the research status and technical challenges of direct regeneration technologies(i.e.,solid-phase sintering,hydrothermal repair and electrochemical repair technology)applicable to spent LFP cathode materials.The failure mechanisms of LFP,as well as the detailed processes and recent advancements in recycling pretreatment are elaborated and summarized.Additionally,this paper extends to introduce the research advancements in innovative upgrading regeneration of cathode materials.Finally,a comparative analysis of the three direct regeneration strategies is conducted,emphasizing their respective advantages,limitations,and target application fields.It is anticipated to establish a comprehensive reference framework for the efficient regeneration and reuse of cathode materials from spent LFP batteries,thus promoting the green and sustainable development of the new energy vehicle industry.
基金Projects(51974137,52274299)supported by the National Natural Science Foundation of ChinaProject(2023M733190)supported by the China Postdoctoral Science Foundation。
文摘In view of the difference in coordination capacity of the glycine ion(Gly−),a selective leaching process for treating with spent lithium-ion batteries(LIBs)in the alkaline glycinate system was proposed.The effects of retention time,leaching temperature,concentration of glycine ligand,liquid-solid ratio(L/S),pH,stirring speed,and H_(2)O_(2) dosage on the leaching efficiency of valuable metals and the dissolution of impurities were investigated.When the spent LIBs were leached in 3 mol/L glycine aqueous solution with pH of 8,L/S of 5 mL:1 g and H_(2)O_(2) dosage of 5 vol.%at 90℃and stirring speed of 400 r/min for 3 h,lithium,cobalt,nickel,and manganese recoveries were 96.31%,83.18%,91.56%,and 31.16%,respectively,but Ca,Al,Fe,and Cu were almost insoluble.Meanwhile,the kinetic study showed that the activation energies for the leaching of Li,Co,Ni,and Mn were all in the range of 45−61 kJ/mol.The results indicate that the leaching process is all controlled by chemical reactions.
