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.

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.

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].

Erratum to: Pyrometallurgical recycling of end -of-life lithium-ion batteries

Erratum to:International Journal of Minerals,Metallurgy and Materials Volume 31,Number 7,July 2024,Page 1554 https://doi.org/10.1007/s12613-024-2907-7 In this article,affiliation 1 has been erroneously given as Department of Materials Science and Engineering,Seoul 03722,Korea.

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.

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.

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.

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.

Fuel recycling feedback control via real-time boron powder injection in EAST with full metal wall

A feedback control of fuel recycling via real-time boron powder injection,addressing the issue of continuously increasing recycling in long-pulse plasma discharges,has been successfully developed and implemented on EAST tokamak.The feedback control system includes four main parts:the impurity powder dropper(IPD),a diagnostic system measuring fuel recycling level represented by D_(α)emission,a plasma control system(PCS)implementing the Proportional Integral Derivative(PID)algorithm,and a signal converter connecting the IPD and PCS.Based on this control system,both active control and feedback control experiments have recently been performed on EAST with a full metal wall.The experimental results show that the fuel recycling can be gradually reduced to lower level as PCS control voltage increases.In the feedback control experiments,it is also observed that the D_(α)emission is reduced to the level below the target D_(α)value by adjusting boron injection flow rate,indicating successful implementation of the fuel recycling feedback control on EAST.This technique provides a new method for fuel recycling control of long pulse and high parameter plasma operations in future fusion devices.

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.

Recyclable Technology of Thermosetting Resins for High Thermal Conductivity Materials Based on Physical Crushing

Epoxy resin,characterized by prominent mechanical and electric-insulation properties,is the preferred material for packaging power electronic devices.Unfortunately,the efficient recycling and reuse of epoxy materials with thermally cross-linked molecular structures has become a daunting challenge.Here,we propose an economical and operable recycling strategy to regenerate waste epoxy resin into a high-performance material.Different particle size of waste epoxy micro-spheres(100–600μm)with core-shell structure is obtained through simple mechanical crushing and boron nitride surface treatment.By using smattering epoxy monomer as an adhesive,an eco-friendly composite material with a“brick-wall structure”can be formed.The continuous boron nitride pathway with efficient thermal conductivity endows eco-friendly composite materials with a preeminent thermal conductivity of 3.71 W m^(−1)K^(−1) at a low content of 8.5 vol%h-BN,superior to pure epoxy resin(0.21 W m^(−1)K^(−1)).The composite,after secondary recycling and reuse,still maintains a thermal conductivity of 2.12 W m^(−1)K^(−1) and has mechanical and insulation properties comparable to the new epoxy resin(energy storage modulus of 2326.3 MPa and breakdown strength of 40.18 kV mm^(−1)).This strategy expands the sustainable application prospects of thermosetting polymers,offering extremely high economic and environmental value.

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.

Prediction Model-based Multi-objective Optimization for Mix-ratio Design of Recycled Aggregate Concrete

The prediction model for mechanical properties of RAC was established through the Bayesian optimization-based Gaussian process regression(BO-GPR)method,where the input variables in BO-GPR model depend on the mix ratio of concrete.Then the compressive strength prediction model,the material cost,and environmental factors were simultaneously considered as objectives,while a multi-objective gray wolf optimization algorithm was developed for finding the optimal mix ratio.A total of 730 RAC datasets were used for training and testing the predication model,while the optimal design method for mix ratio was verified through RAC experiments.The experimental results show that the predicted,testing,and expected compressive strengths are nearly consistent,illustrating the effectiveness of the proposed method.

Long-term performance of recycled asphalt mixtures containing high RAP and RAS

The application of reclaimed asphalt pavement(RAP)and reclaimed asphalt shingles(RAS)on asphalt pavement can reduce the asphalt paving cost,conserve energy and protect the environment.However,the use of high contents of RAP and RAS in asphalt pavement may lead to durability issues,especially the fatigue cracking and thermal cracking.It is necessary to conduct a series of analyses on asphalt mixtures containing high RAP and RAS,and seek methods to enhance their long-term performance.This paper provides a comprehensive over-view of the long-term performance of recycled asphalt mixtures containing high contents of RAP and RAS.The findings in this research show that rutting resistance of high recycled asphalt mixtures is not a concern,whereas their resistance to fatigue and thermal cracking is not conclusive.Recycling agents can be used to improve the thermal cracking resistance of high recycled asphalt mixtures.An optimum decision on recycling agents will improve the durability properties of high recycled asphalt mixtures.It is recommended that to use a balanced mixture design approach with testing of the blended asphalt binders will provide better understanding of long-term performance of recycled asphalt mixtures containing high RAP and RAS.

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).

Residual fluoride self-activated effect enabling upgraded utilization of recycled graphite anode

Recycling graphite anode from spent lithium-ion batteries(SLIBs)is regarded as a crucial approach to promoting sustainable energy storage industry.However,the recycled graphite(RG)generally presents degraded structure and performance.Herein,the residual fluoride self-activated effect is proposed for the upgraded utilization of RG.Simple and low-energy water immersion treatment not only widens the interlayer spacing,but also retains appropriate fluoride on the surface of RG.Theoretical analysis and experiments demonstrate that the residual fluoride can optimize Li~+migration and deposition kinetics,resulting in better Li~+intercalation/deintercalation in the interlayer and more stable Li metal plating/stripping on the surface of RG,As a result,the designed LFP||RG full cells achieve ultrahigh reversibility(~100%Coulombic efficiency),high capacity retention(67%after 200 cycles,0.85 N/P ratio),and commendable adaptability(stable cycling without short-circuiting,0.15 N/P ratio).The energy density is improved from 334 Wh kg^(-1)of 1.1 N/P ratio to 367 Wh kg^(-1)of 0.85 N/P ratio(total mass based on cathode and anode).The exploration of RG by residual fluoride self-activated effect achieves upgraded utilization beyond fresh commercial graphite and highlights a new strategy for efficient reuse of SLIBs.

High-efficiency Carbonation Modification Methods of Recycled Coarse Aggregates

To solve the problem of only surface carbonation and realize high-efficiency carbonation of recycled coarse aggregate,the method of carbonated recycled coarse aggregate with nano materials pre-soaking was first put forward.The carbonation effect of modified recycled coarse aggregate with three different carbonation methods was evaluated,and water absorption,apparent density and crush index of modified recycled coarse aggregate were measured.Combined with XRD,SEM,and MIP microscopic analysis,the high-efficiency carbonation strengthening mechanism of modified recycled coarse aggregate was revealed.The experimental results show that,compared with the non-carbonated recycled coarse aggregate,the physical and microscopic properties of carbonated recycled coarse aggregate are improved.The method of carbonation with nano-SiO_(2) pre-soaking can realize the high-efficiency carbonation of recycled coarse aggregate,for modified recycled coarse aggregate with the method,water absorption is reduced by 23.03%,porosity is reduced by 44.06%,and the average pore diameter is 21.82 nm.The high-efficiency carbonation strengthening mechanism show that the pre-socked nano-SiO_(2) is bound to the hydration product Ca(OH)_(2) of the old mortar with nano-scale C-S-H,which can improve the CO_(2) absorption rate,accelerate the carbonation reaction,generate more stable CaCO_(3) and nano-scale silica gel,and bond to the dense three-dimensional network structure to realize the bidirectional enhancement of nano-materials and pressurized carbonation.It is concluded that the method of carbonation with nano-SiO_(2) pre-soaking is a novel high-efficiency carbonation modification of recycled coarse aggregate.

Application of the Shrinking Particle Model for the Evaluation of Molecular Recyclability of PET versus Semi-Aromatic Polyesters

The molecular recyclability of poly (ethylene terephthalate) (PET) and three semi-aromatic polyesters poly (phloretic acid) (poly-H), poly (dihydroferulic acid) (poly-G), and poly (dihydrosinapinic acid) (poly-S) is evaluated in this study. PET is an extensively used aromatic polyester, and poly-H, poly-G, and poly-S can be considered semi-aromatic poly (lactic acid) modifications. All these polyesters have been depolymerized at neutral pH and by acid- and base-catalyzed hydrolysis at two temperatures, i.e., 50˚C and 80˚C. Base-catalyzed depolymerization of virgin PET leads to an isolated yield of 38% after 48 hours of reaction at 80˚C. Contrary to these results for PET, almost all the monomers of the semi-aromatic polyesters poly-H, poly-G, and poly-S are recovered with isolated yields larger than 90% at the same temperature after 15 minutes in a facile manner. A shrinking particle model used to determine the global kinetics of the base-catalyzed depolymerization showed that the rate rises with increasing temperature. Using the shrinking particle model, the intrinsic reaction rate constants were determined. It has been demonstrated that the rate coefficients of the depolymerization of the semi-aromatic polyesters poly-H, poly-G, and poly-S are between 2 and 3 orders of magnitude higher than those for PET.

Effect of Modification Treatment on Chloride Ions Permeability and Microstructure of Recycled Brick-mixed Aggregate Concrete

The modification methods of pozzolan slurry combined with sodium silicate and silicon-based additive were respectively adopted to treat recycled coarse brick-mixed aggregate(RCBA)in this study.The compressive strength and chloride permeability resistance of recycled aggregate concrete(RAC)before and after modification treatment were tested,and the microstructure of RAC was analyzed by mercury intrusion porosimetry(MIP)and scanning electron microscopy(SEM).The results show that the physical properties of RCBA strengthened by modification treatment are improved,and the compressive strength and chloride permeability resistance of treated RAC are also significantly improved.The modification treatment optimizes the pore size distribution of RAC,which increases the number of gel pores and transition pores,and decreases the number of capillary pores and macro pores.The surface fractal dimension shows a significant correlation with chloride diffusion coefficient,indicating that the variation of chloride permeability of treated RAC is consistent with the microstructure evolution.

Development of sustainable and efficient recycling technology for spent Li-ion batteries: Traditional and transformation go hand in hand

Clean and efficient recycling of spent lithium-ion batteries(LIBs)has become an urgent need to promote sustainable and rapid development of human society.Therefore,we provide a critical and comprehensive overview of the various technologies for recycling spent LIBs,starting with lithium-ion power batteries.Recent research on raw material collection,metallurgical recovery,separation and purification is highlighted,particularly in terms of all aspects of economic efficiency,energy consumption,technology transformation and policy management.Mechanisms and pathways for transformative full-component recovery of spent LIBs are explored,revealing a clean and efficient closed-loop recovery mechanism.Optimization methods are proposed for future recycling technologies,with a focus on how future research directions can be industrialized.Ultimately,based on life-cycle assessment,the challenges of future recycling are revealed from the LIBs supply chain and stability of the supply chain of the new energy battery industry to provide an outlook on clean and efficient short process recycling technologies.This work is designed to support the sustainable development of the new energy power industry,to help meet the needs of global decarbonization strategies and to respond to the major needs of industrialized recycling.