The growing volume of end-of-life lithium-ion batteries(LIBs)represents both an urgent environmental challenge and a critical resource opportunity,especially for cathode materials.Among commercial cathodes,LiFePO4(LFP...The growing volume of end-of-life lithium-ion batteries(LIBs)represents both an urgent environmental challenge and a critical resource opportunity,especially for cathode materials.Among commercial cathodes,LiFePO4(LFP)dominates the market due to its favorable properties;thus,a substantial amount of LFP cathode materials is expected to retire in the near future.The conventional hydrometallurgical method suffers from high costs and serious pollution.Direct regeneration technologies,especially solid-state sintering,provide a more efficient and environmentally benign alternative by repairing cathode structures through high-temperature solid-phase reactions without extra chemical reagents.Traditional solid-state sintering faces challenges in processing spent LFP from diverse sources,struggling to achieve the homogenization of physical–chemical properties and electrochemical performance.To address the limitations above,phase homogenization with a lattice reconstruction strategy has been investigated,which can enable effective lattice reconstruction and microstructural homogenization,demonstrating robust adaptability to spent samples from variable sources.This review systematically summarizes the mechanisms,detailed steps,characterization techniques,and advances in pre-oxidation optimization(including ion-doping and coated carbon layer modification),as well as future research directions for sustainable LFP recycling.Given this,this review is expected to offer theoretical guidance for achieving homogeneous regeneration of LFP cathode.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
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
With the approaching of large-scale retirement of power lithium-ion batteries(LIBs),their urgent handling is required for environmental protection and resource reutilization.However,at present,substantial spent power ...With the approaching of large-scale retirement of power lithium-ion batteries(LIBs),their urgent handling is required for environmental protection and resource reutilization.However,at present,substantial spent power batteries,especially for those high recovery value cathode materials,have not been greenly,sustainably,and efficiently recycled.Compared to the traditional recovery method for cathode materials with high energy consumption and severe secondary pollution,the direct repair regeneration,as a new type of short-process and efficient treatment methods,has attracted widespread attention.However,it still faces challenges in homogenization repair,electrochemical performance decline,and scaling-up production.To promote the direct regeneration technology development of failed NCM materials,herein we deeply discuss the failure mechanism of nickel-cobalt-manganese(NCM)ternary cathode materials,including element loss,Li/Ni mixing,phase transformation,structural defects,oxygen release,and surface degradation and reconstruction.Based on this,the detailed analysis and summary of the direct regeneration method embracing solid-phase sintering,eutectic salt assistance,solvothermal synthesis,sol-gel process,spray drying,and redox mediation are provided.Further,the upcycling strategy for regeneration materials,such as single-crystallization and high-nickelization,structural regulation,ion doping,and surface engineering,are discussed in deep.Finally,the challenges faced by the direct regeneration and corresponding countermeasures are pointed out.Undoubtedly,this review provides valuable guidance for the efficient and high-value recovery of failed cathode materials.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
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
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
Lithium iron phosphate(LiFePO_(4),LFP)batteries have shown extensive adoption in power applications in recent years for their reliable safety,high theoretical capability and low cost.Nevertheless,the finite lifespan o...Lithium iron phosphate(LiFePO_(4),LFP)batteries have shown extensive adoption in power applications in recent years for their reliable safety,high theoretical capability and low cost.Nevertheless,the finite lifespan of these batteries necessitates the future processing of a significant number of spent LFP batteries,underscoring the urgent need for the development of both efficient and eco-friendly recycling methods.This study combines the advantages of wet leaching and direct regeneration methods,leveraging citric acid's multifaceted role to streamline the combined leaching and hydrothermal processes.Results indicate that citric acid efficiently leaches all elements from spent LFP batteries.Furthermore,through its unique structure,it enhances hydrothermal regeneration by stabilizing metal ions and controlling crystal growth,and also acts as a carbon source for the surface carbon coating of regenerated LFP(RLFP).The R-LFP shows outstanding electrochemical stability,achieving a discharge capacity of 155.1 mAh.g^(-1)at 0.1C,with a capacity retention rate of 93.2%after 300 cycles at 1C.Furthermore,economic and environmental analyses demonstrate this method's superior cost-effectiveness and sustainability.Therefore,the method proposed in this study is efficient,simple and avoids the complex process of element separation,innovatively using a single reagent to achieve closed-loop recycling of LFP batteries,providing a novel and effective solution for the resource sustainability application.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
In current spent nuclear fuel reprocessing,the predominant method involves chemical extraction,leveraging the differing distribution ratios of elements to achieve separation and purification.Effective separation of ur...In current spent nuclear fuel reprocessing,the predominant method involves chemical extraction,leveraging the differing distribution ratios of elements to achieve separation and purification.Effective separation of uranium(U),plutonium(Pu),and neptunium(Np) typically relies on redox processes that alter their oxidation states during extraction.Therefore,reductants play a critical role in reprocessing processes.An important shift in the advanced reprocessing process is the use of salt-free reagents in the actinide separation process.In addition,the salt content in the reprocessing stream is often indicative of the overall technological sophistication of the process,and it is critical to reform the reductants used in the main process stream.Salt-free reductants have attracted much attention in recent years for basic and applied research in reprocessing processes because of their advantages such as being easily destroyed,not introducing salts,reacting quickly,simplifying the process,and reducing the amount of waste.This study summarizes emerging salt-free reagents with potential applications in reprocessing,and outlines their kinetic and chemical reaction mechanism properties in reducing Pu(Ⅳ) and Np(Ⅵ).The conclusion discusses the future potential of salt-free reagents in reprocessing.This study summarizes the currently well-studied salt-free reductants and offers recommendations and future research directions in salt-free alternatives.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
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
Within the framework of carbon neutrality,lithium-ion batteries(LIBs)are progressively booming along with the growing utilization of green and clean energy.However,the extensive application of LIBs with limited lifesp...Within the framework of carbon neutrality,lithium-ion batteries(LIBs)are progressively booming along with the growing utilization of green and clean energy.However,the extensive application of LIBs with limited lifespan has brought about a significant recycling dilemma.The traditional hydrometallurgical or pyrometallurgical strategies are not capable to maximize the output value of spent LIBs and minimize the potential environmental hazards.Herein,to alternate the tedious and polluting treatment processes,we propose a high-temperature molten-salt strategy to directly regenerate spent cathodes of LIBs,which can also overcome the barrier of the incomplete defects'restoration with previous low-temperature molten salts.The high-energy and stable medium environment ensures a more thorough and efficient relithiation reaction,and simultaneously provides sufficient driving force for atomic rearrangement and grains secondary growth.In consequence,the regenerated ternary cathode(R-NCM)exhibits significantly enhanced structural stability that effectively suppresses the occurrence of cracks and harmful side reactions.The R-NCM delivers excellent cycling stability,retaining 81.2%of its capacity after 200 cycles at 1 C.This technique further optimizes the traditional eutectic molten-salt approach,broadening its applicability and improving regenerated cathode performance across a wider range of conditions.展开更多
基金financially supported by National Natural Science Key Foundation of China(52534010)National Natural Science Foundation of China(52374288,52204298)+2 种基金Young Elite Scientists Sponsorship Program by China Association for Science and Technology(2022QNRC001)National Key Research and Development Program of China(2022YFC3900805-4/7)Collaborative Innovation Centre for Clean and Efficient Utilization of Strategic Metal Mineral Resources,Found of State Key Laboratory of Mineral Processing(BGRIMM-KJSKL-2017-13).
文摘The growing volume of end-of-life lithium-ion batteries(LIBs)represents both an urgent environmental challenge and a critical resource opportunity,especially for cathode materials.Among commercial cathodes,LiFePO4(LFP)dominates the market due to its favorable properties;thus,a substantial amount of LFP cathode materials is expected to retire in the near future.The conventional hydrometallurgical method suffers from high costs and serious pollution.Direct regeneration technologies,especially solid-state sintering,provide a more efficient and environmentally benign alternative by repairing cathode structures through high-temperature solid-phase reactions without extra chemical reagents.Traditional solid-state sintering faces challenges in processing spent LFP from diverse sources,struggling to achieve the homogenization of physical–chemical properties and electrochemical performance.To address the limitations above,phase homogenization with a lattice reconstruction strategy has been investigated,which can enable effective lattice reconstruction and microstructural homogenization,demonstrating robust adaptability to spent samples from variable sources.This review systematically summarizes the mechanisms,detailed steps,characterization techniques,and advances in pre-oxidation optimization(including ion-doping and coated carbon layer modification),as well as future research directions for sustainable LFP recycling.Given this,this review is expected to offer theoretical guidance for achieving homogeneous regeneration of LFP cathode.
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financially supported by the National Key Research and Development Program of China(2023YFB3809300)。
文摘With the approaching of large-scale retirement of power lithium-ion batteries(LIBs),their urgent handling is required for environmental protection and resource reutilization.However,at present,substantial spent power batteries,especially for those high recovery value cathode materials,have not been greenly,sustainably,and efficiently recycled.Compared to the traditional recovery method for cathode materials with high energy consumption and severe secondary pollution,the direct repair regeneration,as a new type of short-process and efficient treatment methods,has attracted widespread attention.However,it still faces challenges in homogenization repair,electrochemical performance decline,and scaling-up production.To promote the direct regeneration technology development of failed NCM materials,herein we deeply discuss the failure mechanism of nickel-cobalt-manganese(NCM)ternary cathode materials,including element loss,Li/Ni mixing,phase transformation,structural defects,oxygen release,and surface degradation and reconstruction.Based on this,the detailed analysis and summary of the direct regeneration method embracing solid-phase sintering,eutectic salt assistance,solvothermal synthesis,sol-gel process,spray drying,and redox mediation are provided.Further,the upcycling strategy for regeneration materials,such as single-crystallization and high-nickelization,structural regulation,ion doping,and surface engineering,are discussed in deep.Finally,the challenges faced by the direct regeneration and corresponding countermeasures are pointed out.Undoubtedly,this review provides valuable guidance for the efficient and high-value recovery of failed cathode materials.
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 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 Natural Science Foundation of China(No.22162007)the Science and Technology Supporting Project of Guizhou Province(Nos.[2021]480 and[2023]379)+1 种基金Wengfu(Group)Co.,Ltd.Technology Development Project(No.WH-220787(YF))the project from Guizhou Institute of Innovation and development of dual-carbon and new energy technologies(No.DCRE-2023-05)。
文摘Lithium iron phosphate(LiFePO_(4),LFP)batteries have shown extensive adoption in power applications in recent years for their reliable safety,high theoretical capability and low cost.Nevertheless,the finite lifespan of these batteries necessitates the future processing of a significant number of spent LFP batteries,underscoring the urgent need for the development of both efficient and eco-friendly recycling methods.This study combines the advantages of wet leaching and direct regeneration methods,leveraging citric acid's multifaceted role to streamline the combined leaching and hydrothermal processes.Results indicate that citric acid efficiently leaches all elements from spent LFP batteries.Furthermore,through its unique structure,it enhances hydrothermal regeneration by stabilizing metal ions and controlling crystal growth,and also acts as a carbon source for the surface carbon coating of regenerated LFP(RLFP).The R-LFP shows outstanding electrochemical stability,achieving a discharge capacity of 155.1 mAh.g^(-1)at 0.1C,with a capacity retention rate of 93.2%after 300 cycles at 1C.Furthermore,economic and environmental analyses demonstrate this method's superior cost-effectiveness and sustainability.Therefore,the method proposed in this study is efficient,simple and avoids the complex process of element separation,innovatively using a single reagent to achieve closed-loop recycling of LFP batteries,providing a novel and effective solution for the resource sustainability application.
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.
文摘In current spent nuclear fuel reprocessing,the predominant method involves chemical extraction,leveraging the differing distribution ratios of elements to achieve separation and purification.Effective separation of uranium(U),plutonium(Pu),and neptunium(Np) typically relies on redox processes that alter their oxidation states during extraction.Therefore,reductants play a critical role in reprocessing processes.An important shift in the advanced reprocessing process is the use of salt-free reagents in the actinide separation process.In addition,the salt content in the reprocessing stream is often indicative of the overall technological sophistication of the process,and it is critical to reform the reductants used in the main process stream.Salt-free reductants have attracted much attention in recent years for basic and applied research in reprocessing processes because of their advantages such as being easily destroyed,not introducing salts,reacting quickly,simplifying the process,and reducing the amount of waste.This study summarizes emerging salt-free reagents with potential applications in reprocessing,and outlines their kinetic and chemical reaction mechanism properties in reducing Pu(Ⅳ) and Np(Ⅵ).The conclusion discusses the future potential of salt-free reagents in reprocessing.This study summarizes the currently well-studied salt-free reductants and offers recommendations and future research directions in salt-free alternatives.
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support by National Natural Science Foundation of China(22379166)Natural Science Foundation for Distinguished Young Scholars of Hunan Province(2022JJ10089)Central South University Innovation-Driven Research Programme(2023CXQD034).
文摘Within the framework of carbon neutrality,lithium-ion batteries(LIBs)are progressively booming along with the growing utilization of green and clean energy.However,the extensive application of LIBs with limited lifespan has brought about a significant recycling dilemma.The traditional hydrometallurgical or pyrometallurgical strategies are not capable to maximize the output value of spent LIBs and minimize the potential environmental hazards.Herein,to alternate the tedious and polluting treatment processes,we propose a high-temperature molten-salt strategy to directly regenerate spent cathodes of LIBs,which can also overcome the barrier of the incomplete defects'restoration with previous low-temperature molten salts.The high-energy and stable medium environment ensures a more thorough and efficient relithiation reaction,and simultaneously provides sufficient driving force for atomic rearrangement and grains secondary growth.In consequence,the regenerated ternary cathode(R-NCM)exhibits significantly enhanced structural stability that effectively suppresses the occurrence of cracks and harmful side reactions.The R-NCM delivers excellent cycling stability,retaining 81.2%of its capacity after 200 cycles at 1 C.This technique further optimizes the traditional eutectic molten-salt approach,broadening its applicability and improving regenerated cathode performance across a wider range of conditions.
