Progress,challenges,and prospects of spent lithium-ion batteries recycling:A review

The recycling and reutilization of spent lithium-ion batteries(LIBs)have become an important measure to alleviate problems like resource scarcity and environmental pollution.Although some progress has been made,battery recycling technology still faces challenges in terms of efficiency,effectiveness and environmental sustainability.This review aims to systematically review and analyze the current status of spent LIB recycling,and conduct a detailed comparison and evaluation of different recycling processes.In addition,this review introduces emerging recycling techniques,including deep eutectic solvents,molten salt roasting,and direct regeneration,with the intent of enhancing recycling efficiency and diminishing environmental repercussions.Furthermore,to increase the added value of recycled materials,this review proposes the concept of upgrading recycled materials into high value-added functional materials,such as catalysts,adsorbents,and graphene.Through life cycle assessment,the paper also explores the economic and environmental impacts of current battery recycling and highlights the importance that future recycling technologies should achieve a balance between recycling efficiency,economics and environmental benefits.Finally,this review outlines the opportunities and challenges of recycling key materials for next-generation batteries,and proposes relevant policy recommendations to promote the green and sustainable development of batteries,circular economy,and ecological civilization.

Managing the surge:A comprehensive review of the entire disposal framework for retired lithium-ion batteries from electric vehicles

Anticipating the imminent surge of retired lithium-ion batteries(R-LIBs)from electric vehicles,the need for safe,cost-effective and environmentally friendly disposal technologies has escalated.This paper seeks to offer a comprehensive overview of the entire disposal framework for R-LIBs,encompassing a broad spectrum of activities,including screening,repurposing and recycling.Firstly,we delve deeply into a thorough examination of current screening technologies,shifting the focus from a mere enumeration of screening methods to the exploration of the strategies for enhancing screening efficiency.Secondly,we outline battery repurposing with associated key factors,summarizing stationary applications and sizing methods for R-LIBs in their second life.A particular light is shed on available reconditioning solutions,demonstrating their great potential in facilitating battery safety and lifetime in repurposing scenarios and identifying their techno-economic issues.In the realm of battery recycling,we present an extensive survey of pre-treatment options and subsequent material recovery technologies.Particularly,we introduce several global leading recyclers to illustrate their industrial processes and technical intricacies.Furthermore,relevant challenges and evolving trends are investigated in pursuit of a sustainable end-of-life management and disposal framework.We hope that this study can serve as a valuable resource for researchers,industry professionals and policymakers in this field,ultimately facilitating the adoption of proper disposal practices.

Facile synthesis of accordion-like porous carbon from waste PET bottles-based MIL-53(Al)and its application for high-performance Zn-ion capacitor

It is of great scientific and economic value to recycle waste poly(ethylene terephthalate)(PET)into high-value PET-based metal organic frameworks(MOFs)and further convert it into porous carbon for green energy storage applications.In the present study,a facile and costeffective hydrothermal process was developed to direct recycle waste PET bottles into MIL-53(Al)with a 100% conversation,then the MOFderived porous carbon was assembled into electrodes for high-performance supercapacitors.The results indicated that the as-synthesized carbon exhibited high SSA of 1712 m^(2)g^(-1)and unique accordion-like structure with hierarchical porosity.Benefit to these advantageous characters,the assembled three-electrode supercapacitor displayed high specific capacitances of 391 F g^(-1)at the current density of 0.5 A g^(-1)and good rate capability of 73.6% capacitance retention at 20 A g^(-1)in 6 mol L^(-1)KOH electrolyte.Furthermore,the assembled zinc ion capacitor still revealed outstanding capacitance of 335 F g^(-1)at 0.1 A g^(-1),excellent cycling stability of 92.2% capacitance retention after 10000 cycles and ultra-high energy density of 150.3 Wh kg^(-1)at power density of 90 W kg^(-1)in 3 mol L^(-1)ZnSO_(4)electrolyte.It is believed that the current work provides a facile and effective strategy to recycle PET waste into high-valuable MOF,and further expands the applications of MOF-derived carbons for high-performance energy storage devices,so it is conducive to both pollution alleviation and sustainable economic development.

Targeted regeneration and upcycling of spent graphite by defect‐driven tin nucleation

The recycling of spent batteries has become increasingly important owing to their wide applications,abundant raw material supply,and sustainable development.Compared with the degraded cathode,spent anode graphite often has a relatively intact structure with few defects after long cycling.Yet,most spent graphite is simply burned or discarded due to its limited value and inferior performance on using conventional recycling methods that are complex,have low efficiency,and fail in performance restoration.Herein,we propose a fast,efficient,and“intelligent”strategy to regenerate and upcycle spent graphite based on defect‐driven targeted remediation.Using Sn as a nanoscale healant,we used rapid heating(~50 ms)to enable dynamic Sn droplets to automatically nucleate around the surface defects on the graphite upon cooling owing to strong binding to the defects(~5.84 eV/atom),thus simultaneously achieving Sn dispersion and graphite remediation.As a result,the regenerated graphite showed enhanced capacity and cycle stability(458.9 mAh g^(−1) at 0.2 A g^(−1) after 100 cycles),superior to those of commercial graphite.Benefiting from the self‐adaption of Sn dispersion,spent graphite with different degrees of defects can be regenerated to similar structures and performance.EverBatt analysis indicates that targeted regeneration and upcycling have significantly lower energy consumption(~99%reduction)and near‐zero CO_(2) emission,and yield much higher profit than hydrometallurgy,which opens a new avenue for direct upcycling of spend graphite in an efficient,green,and profitable manner for sustainable battery manufacture.

Dysfunction of synaptic endocytic trafficking in Parkinson's disease

Parkinson's disease is characterized by the selective degeneration of dopamine neurons in the nigrostriatal pathway and dopamine deficiency in the striatum.The precise reasons behind the specific degeneration of these dopamine neurons remain largely elusive.Genetic investigations have identified over 20 causative PARK genes and 90 genomic risk loci associated with both familial and sporadic Parkinson's disease.Notably,several of these genes are linked to the synaptic vesicle recycling process,particularly the clathrinmediated endocytosis pathway.This suggests that impaired synaptic vesicle recycling might represent an early feature of Parkinson's disease,followed by axonal degeneration and the eventual loss of dopamine cell bodies in the midbrain via a"dying back"mechanism.Recently,several new animal and cellular models with Parkinson's disease-linked mutations affecting the endocytic pathway have been created and extensively characterized.These models faithfully recapitulate certain Parkinson's disease-like features at the animal,circuit,and cellular levels,and exhibit defects in synaptic membrane trafficking,further supporting the findings from human genetics and clinical studies.In this review,we will first summarize the cellular and molecular findings from the models of two Parkinson's disease-linked clathrin uncoating proteins:auxilin(DNAJC6/PARK19)and synaptojanin 1(SYNJ1/PARK20).The mouse models carrying these two PARK gene mutations phenocopy each other with specific dopamine terminal pathology and display a potent synergistic effect.Subsequently,we will delve into the involvement of several clathrin-mediated endocytosis-related proteins(GAK,endophilin A1,SAC2/INPP5 F,synaptotagmin-11),identified as Parkinson's disease risk factors through genome-wide association studies,in Parkinson's disease pathogenesis.We will also explore the direct or indirect roles of some common Parkinson's disease-linked proteins(alpha-synuclein(PARK1/4),Parkin(PARK2),and LRRK2(PARK8))in synaptic endocytic trafficking.Additionally,we will discuss the emerging novel functions of these endocytic proteins in downstream membrane traffic pathways,particularly autophagy.Given that synaptic dysfunction is considered as an early event in Parkinson's disease,a deeper understanding of the cellular mechanisms underlying synaptic vesicle endocytic trafficking may unveil novel to rgets for early diagnosis and the development of interventional therapies for Parkinson's disease.Future research should aim to elucidate why generalized synaptic endocytic dysfunction leads to the selective degeneration of nigrostriatal dopamine neurons in Parkinson's disease.

Direct recycling of Li-ion batteries from cell to pack level:Challenges and prospects on technology,scalability,sustainability,and economics

Direct recycling is a novel approach to overcoming the drawbacks of conventional lithium-ion battery(LIB)recycling processes and has gained considerable attention from the academic and industrial sectors in recent years.The primary objective of directly recycling LIBs is to efficiently recover and restore the active electrode materials and other components in the solid phase while retaining electrochemical performance.This technology's advantages over traditional pyrometallurgy and hydrometallurgy are costeffectiveness,energy efficiency,and sustainability,and it preserves the material structure and morphology and can shorten the overall recycling path.This review extensively discusses the advancements in the direct recycling of LIBs,including battery sorting,pretreatment processes,separation of cathode and anode materials,and regeneration and quality enhancement of electrode materials.It encompasses various approaches to successfully regenerate high-value electrode materials and streamlining the recovery process without compromising their electrochemical properties.Furthermore,we highlight key challenges in direct recycling when scaled from lab to industries in four perspectives:(1)battery design,(2)disassembling,(3)electrode delamination,and(4)commercialization and sustainability.Based on these challenges and changing market trends,a few strategies are discussed to aid direct recycling efforts,such as binders,electrolyte selection,and alternative battery designs;and recent transitions and technological advancements in the battery industry are presented.

A comprehensive review on the resynthesis of ternary cathode active materials from the leachate of Li-ion batteries

This review highlights the importance of recovering valuable metals from spent Li-ion battery(LIB)cathodes through the resynthesis of cathode active materials(CAMs).The resynthesis process of CAMs,a promising recycling method that directly produces CAM precursors from LIB leachate,is explored.This process encompasses six key steps,including pretreatment,leaching,purification,adjustment of metal concentrations,precursor synthesis,and sintering.The review also investigates the potential introduction of impurity elements during CAM resynthesis and provides tolerance levels for these impurities based on thorough reference analysis.Additionally,it addresses challenges related to the commercialization of the resynthesis process.Notably,this review represents the first comprehensive assessment of CAM resynthesis,including the systematic evaluation of 12 impurity elements(Fe,Li,Al,Cu,C,P,F,Na,Cl,S,Mg,and Zn).Overall,this comprehensive review is poised to support the commercial development of resynthesized CAMs by offering valuable guidelines for managing impurities and streamlining the purification process.

Litterfall production modeling based on climatic variables and nutrient return from stands of Eucalyptus grandis Hill ex Maiden and Pinus taeda L.

Native grasslands in the Pampas of South America are increasingly being replaced by Eucalyptus and Pinus stands.The short rotation regimes used for the stands require high nutrient levels,with litterfall being a major source of nutrient return.To model the litterfall production using climatic variables and assess the nutrient return in 14-year-old Eucalyptus grandis and Pinus taeda stands,we measured litter production over 2 years,using conical litter traps,and monitored climatic variables.Mean temperature,accumulated precipitation,and mean maximum vapor pres-sure deficit at the seasonal level influenced litterfall produc-tion by E.grandis;seasonal accumulated precipitation and mean maximum temperature affected litterfall by P.taeda.The regression tree modeling based on these climatic vari-ables had great accuracy and predictive power for E.grandis(N=33;MAE(mean absolute error)=0.65;RMSE(root mean square error)=0.91;R^(2)=0.71)and P.taeda(N=108;MAE=1.50;RMSE=1.59;R^(2)=0.72).The nutrient return followed a similar pattern to litterfall deposition,as well as the order of importance of macronutrients(E.grandis:Ca>N>K>Mg>P;P.taeda:N>Ca>K>Mg>P)and micronutrients(E.grandis and P.taeda:Mn>Fe>Zn>Cu)in both species.This study constitutes a first approximation of factors that affect litterfall and nutrient return in these systems.

Recycled graphite for more sustainable lithium-ion batteries

The demand for lithium-ion batteries(LIBs)is driven largely by their use in electric vehicles,which is projected to increase dramatically in the future.This great success,however,urgently calls for the efficient recycling of LIBs at the end of their life.Herein,we describe a froth flotation-based process to recycle graphite—the predominant active material for the negative electrode—from spent LIBs and investigate its reuse in newly assembled LIBs.It has been found that the structure and morphology of the recycled graphite are essentially unchanged compared to pristine commercial anode-grade graphite,and despite some minor impurities from the recycling process,the recycled graphite provides a remarkable reversible specific capacity of more than 350 mAh g^(−1).Even more importantly,newly assembled graphite‖NMC532 cells show excellent cycling stability with a capacity retention of 80%after 1000 cycles,that is,comparable to the performance of reference full cells comprising pristine commercial graphite.

Pyrometallurgical recycling of end-of-life lithium-ion batteries

The global importance of lithium-ion batteries(LIBs)has been increasingly underscored with the advancement of high-performance energy storage technologies.However,the end-of-life of these batteries poses significant challenges from environmental,economic,and resource management perspectives.This review paper focuses on the pyrometallurgy-based recycling process of lithium-ion batteries,exploring the fundamental understanding of this process and the importance of its optimization.Centering on the high energy consumption and emission gas issues of the pyrometallurgical recycling process,we systematically analyzed the capital-intensive nature of this process and the resulting technological characteristics.Furthermore,we conducted an in-depth discussion on the future research directions to overcome the existing technological barriers and limitations.This review will provide valuable insights for researchers and industry stakeholders in the battery recycling field.

Multifunctional phase change film with high recyclability, adjustable thermal responsiveness, and intrinsic self-healing ability for thermal energy storage

Phase change materials(PCMs) present promising potential for guaranteeing safety in thermal management systems.However,most reported PCMs have a single application in energy storage for thermal management systems,which does not meet the growing demand for multi-functional materials.In this paper,the flexible material and hydrogen-bonding function are innovatively combined to design and prepare a novel multi-functional flexible phase change film(PPL).The 0.2PPL-2 film exhibits solid-solid phase change behavior with energy storage density of 131.8 J/g at the transition temperature of42.1℃,thermal cycling stability(500 cycles),wide-temperature range flexibility(0-60℃) and selfhealing property.Notably,the PPL film can be recycled up to 98.5% by intrinsic remodeling.Moreover,the PPL film can be tailored to the desired colors and configurations and can be cleverly assembled on several thermal management systems at ambient temperature through its flexibility combined with shape-memory properties.More interestingly,the transmittance of PPL will be altered when the ambient temperature changes(60℃),conveying a clear thermal signal.Finally,the thermal energy storage performance of the PPL film is successfully tested by human thermotherapy and electronic device temperature control experiments.The proposed functional integration strategy provides innovative ideas to design PCMs for multifunctionality,and makes significant contributions in green chemistry,highefficiency thermal management,and energy sustainability.

Fully Recyclable Liquid Metal-Based Ultra-St retch able Electronics Enabled by Water-Modulation-Degradation-Reconstruction Polymer-Gel

The rapid development of stretchable electronics made by circuits,microchips,and encapsulation elastomers has caused the production of a large amount of electronic waste(e-waste).The degradation of elastomers can highly minimize the negative effects of e-wastes.However,chemicals that included acid,alkali,and organics were repeatedly used during the recycling process,which were environmentally unfriendly.Here,a water-modulation-degradation-reconstruction(WDR)polyvinylpyrrolidone(PVP)-honey composite(PHC)polymer-gel was developed and could be regarded as encapsulation elastomers to realize a fully recyclable water-degradable stretchable(WS)electronics with multi-functions.The stretchability of the PHC polymer-gel could be modulated by the change of its water retention.The Chip-integrated liquid metal(LM)circuits encapsulated with the modulated PHC encapsulation elastomer could withstand a strain value of~3000%.Moreover,we developed a WS biomedical sensor composed of PHC encapsulation elastomer,LM circuits,and microchips,which could be fully recycled by biodegrading it in water to reconstruct a new one.As before,the reconstructed WS biomedical sensor could still simultaneously realize the combination of ultra-stretchability,recycling,self-healing,self-adhesive,and self-conformal abilities.The results revealed that this study exercises a profound influence on the rational design of multi-functional WS electronics.

Waste Cotton-Derived Fiber-Based Thermoelectric Aerogel for Wearable and Self-Powered Temperature-Compression Strain Dual-Parameter Sensing

The rapid development of the global economy and population growth are accompanied by the production of numerous waste textiles.This leads to a waste of limited resources and serious environmental pollution problems caused by improper disposal.The rational recycling of wasted textiles and their transformation into high-value-added emerging products,such as smart wearable devices,is fascinating.Here,we propose a novel roadmap for turning waste cotton fabrics into three-dimensional elastic fiber-based thermoelectric aerogels by a one-step lyophilization process with decoupled self-powered temperature-compression strain dual-parameter sensing properties.The thermoelectric aerogel exhibits a fast compression response time of 0.2 s,a relatively high Seebeck coefficient of 43μV·K^(-1),and an ultralow thermal conductivity of less than 0.04 W·m^(-1)·K^(-1).The cross-linking of trimethoxy(methyl)silane(MTMS)and cellulose endowed the aerogel with excellent elasticity,allowing it to be used as a compressive strain sensor for guessing games and facial expression recognition.In addition,based on the thermoelectric effect,the aerogel can perform temperature detection and differentiation in self-powered mode with the output thermal voltage as the stimulus signal.Furthermore,the wearable system,prepared by connecting the aerogel-prepared array device with a wireless transmission module,allows for temperature alerts in a mobile phone application without signal interference due to the compressive strains generated during gripping.Hence,our strategy is significant for reducing global environmental pollution and provides a revelatory path for transforming waste textiles into high-value-added smart wearable devices.

Enhancing sustainability in phosphate ore processing:Performance of frying oil as alternative flotation collector for carbonate removal

Recycling waste frying oils for the synthesis of flotation reagents presents a promising avenue for sustainable waste management.Moreover,it offers a cost-effective solution for crafting a specialized collector designed to efficiently remove carbonates and enhance phosphate enrichment in froth flotation processes.This study focuses on the synthesis of an anionic collector using the saponification reaction of a frying oil sample,subsequently applied to the flotation of calcite and dolomite.To elucidate the adsorption mechanisms of the frying oil collector(FrOC)and sodium oleate,a reference collector,on fluorapatite,calcite,dolomite,and quartz surfaces,comprehensive experiments were conducted,including zeta potential measurements and Fourier transform infrared spectroscopy.Results revealed diverse adsorption affinities of the molecules towards these minerals.To assess the practical performance of the collector,flotation tests were conducted using a natural phosphate ore mixture,employing a BoxBehnken experimental design.Notably,under optimized conditions(pH 9,1000 g/t of FrOC,3.5 min of conditioning,and 6 min of flotation),FrOC exhibited excellent performance,with calcite and dolomite recoveries exceeding 80%,while apatite recovery in the concentrate fraction remained below 10%.This work exemplifies both circular economy practices and the distinctive approach to sustainable mineral processing.

Direct Regeneration of Spent Lithium-Ion Battery Cathodes:From Theoretical Study to Production Practice

Direct regeneration method has been widely concerned by researchers in the field of battery recycling because of its advantages of in situ regeneration,short process and less pollutant emission.In this review,we firstly analyze the primary causes for the failure of three representative battery cathodes(lithium iron phosphate,layered lithium transition metal oxide and lithium cobalt oxide),targeting at illustrating their underlying regeneration mecha-nism and applicability.Efficient stripping of material from the collector to obtain pure cathode material has become a first challenge in recycling,for which we report several pretreatment methods currently available for subsequent regeneration processes.We review and discuss emphatically the research progress of five direct regeneration methods,including solid-state sintering,hydrothermal,eutectic molten salt,electrochemical and chemical lithiation methods.Finally,the application of direct regeneration technology in production practice is introduced,the problems exposed at the early stage of the industrialization of direct regeneration technol-ogy are revealed,and the prospect of future large-scale commercial production is proposed.It is hoped that this review will give readers a comprehensive and basic understanding of direct regeneration methods for used lithium-ion batteries and promote the industrial application of direct regeneration technology.

Multi-Component Resource Recycling from Waste Light-Emitting Diode Under Hydrothermal Condition:Plastic Package Degradation,Speciation of Nano-TiO_(2),and Environmental Impact Assessment

Light emitting diodes(LEDs)have accounted for most of the lighting market as the technology matures and costs continue to reduce.As a new type of e-waste,LED is a double-edged sword,as it contains not only precious and rare metals but also organic packaging materials.In previous studies,LED recycling focused on recovering precious and strategic metals while ignoring harmful substances such as organic packaging materials.Unlike crushing and other traditional methods,hydrothermal treatment can provide an environment-friendly process for decomposing packaging materials.This work developed a closed reaction vessel,where the degradation rate of plastic polyphthalamide(PPA)was close to 100%,with nano-TiO_(2)encapsulated in plastic PPA being efficiently recovered,while metals contained in LED were also recycled efficiently.Besides,the role of water in plastic PPA degradation that has been overlooked in current studies was explored and speculated in detail in this work.Environmental impact assessment revealed that the proposed recycling route for waste LED could significantly reduce the overall environmental impact compared to the currently published processes.Especially the developed method could reduce more than half the impact of global warming.Furthermore,this research provides a theoretical basis and a promising method for recycling other plastic-packaged e-waste devices,such as integrated circuits.

Increasing Threat of Scarcity Prompts Rise in Water Recycling

In January 2018,construction wrapped on Salesforce Tower(Fig.1),a 61-story office building that now dominates the skyline of San Francisco,CA,USA.In addition to being the tallest building in the city,Salesforce Tower is the largest structure in the world with an onsite water recycling system.Built by the Australian com-pany Aquacell(Milton,NSW,Australia),the system cleans 113 m^(3)of sewage,sink,shower,and other wastewater each day for use in irrigation and flushing toilets,saving an estimated 35000 m?of water anmually[1].The building is just one of dozens in San Fran-cisco outitted with their own water recycling systems,thanks to a city mandate enacted in 2015[1].

Coated boron layers by boronization and a real-time boron coating using an impurity powder dropper in the LHD

In the Large Helical Device(LHD),diborane(B2H6)is used as a standard boron source for boronization,which is assisted by helium glow discharges.In 2019,a new Impurity Powder Dropper(IPD)system was installed and is under evaluation as a real-time wall conditioning technique.In the LHD,which is a large-sized heliotron device,an additional helium(He)glow discharge cleaning(GDC)after boronization was operated for a reduction in hydrogen recycling from the coated boron layers.This operational time of 3 h was determined by spectroscopic data during glow discharges.A flat hydrogen profile is obtained on the top surface of the coated boron on the specimen exposed to boronization.The results suggest a reduction in hydrogen at the top surface by He-GDC.Trapped oxygen in coated boron was obtained by boronization,and the coated boron,which has boron-oxide,on the first wall by B-IPD was also shown.Considering the difference in coating areas between B2H6 boronization and B-IPD operation,it would be most effective to use the IPD and B2H6 boronization coating together for optimized wall conditioning.

An efficient and mild recycling of waste melamine formaldehyde foams by alkaline hydrolysis

Melamine formaldehyde foam(MFF)generates many poisonous chemicals through the traditional recycling methods for organic resin wastes.Herein,a high MFF degradation ratio of ca.97 wt.%was achieved under the mild conditions(160℃)in a NaOH–H2O system with ammelide and ammeline as the main degradation products.The alkaline solvent had an obvious corrosion effect for MFF,as indicated by scanning electron microscopy(SEM).The reaction process and products distribution were studied by Fourier-transform infrared spectroscopy(FTIR),X-ray photoelectron spectroscopy(XPS),and ^(13)C nuclear magnetic resonance(NMR).Besides,the MFF degradation products that have the similar chemical structures and bonding performances to those of melamine can be directly used as the raw material for synthesis of melamine urea-formaldehyde resins(MUFs).Moreover,the degradation system demonstrated here showed the high degradation efficiency after reusing for 7 times.The degradation process generated few harmful pollutants and no pre-or post-treatments were required,which proves its feasibility in the safe removal or recovery of waste MFF.

Simultaneous purification of minor components in natural products using twin-column recycling chromatography with a step solvent gradient

The isolation of minor components from complex natural product matrices presents a significant challenge in the field of purification science due to their low concentrations and the presence of structurally similar compounds.This study introduces an optimized twin-column recycling chromatography method for the efficient and simultaneous purification of these elusive constituents.By introducing water at a small flowing rate between the twin columns,a step solvent gradient is created,by which the leading edge of concentration band would migrate at a slower rate than the trailing edge as it flowing from the upstream to downstream column.Hence,the band broadening is counterbalanced,resulting in an enrichment effect for those minor components in separation process.Herein,two target substances,which showed similar peak position in high performance liquid chromatography(HPLC)and did not exceed 1.8%in crude paclitaxel were selected as target compounds for separation.By using the twin-column recycling chromatography with a step solvent gradient,a successful purification was achieved in getting the two with the purity almost 100%.We suggest this method is suitable for the separation of most components in natural produces,which shows higher precision and recovery rate compared with the common lab-operated separation ways for natural products(thin-layer chromatography and prep-HPLC).