Synthesizing core-shell Ni-rich LiNi_(x)Co_(y)Mn_(z)O_(2) from spent Li-ion battery leachate

As the global electric vehicle market continues to grow,the recycling of Li-ion battery (LIB) becomes more important worldwide and the resynthesis of cathode materials would be the most value-added recycling approach taking into account limited metal resources.Although resynthesized homogenous LiNi_(x)Co_(y)Mn_(z)O_(2)(NCM) from spent LIB leachate shows comparable battery performance to pristine NCM from virgin materials,there is general concern in its cycling performance.Here,we synthesize core–shell(CS) Ni-rich NCM,which consists of Ni-rich NCM as the core and NCM derived from the original or purified leachate of spent LIBs as the shell.Resynthesized CS Ni-rich NCM exhibits improved rate capability resulting from expanded interslab thickness in the NCM structure.CS Ni-rich NCM from purified LIB leachate shows improvement in cycling performance and thermal stability.It specifically delivers a capacity retention of 86.6%at a high temperature after 80 cycles compared to that (75.0%) of pristine CS Ni-rich NCM.These improvements are caused by a relatively high Mg content on the shell and the widespread distribution of Al through the CS structure.CS Ni-rich NCM derived from spent LIB leachate provides a new alternative approach to conventional LIB recycling methods,which would utilize efficiently limited metal resources for the sustainable LIB production.

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.

Recovery of Li, Ni, Co and Mn from spent lithium-ion batteries assisted by organic acids: Process optimization and leaching mechanism

The proper recycling of spent lithium-ion batteries(LIBs)can promote the recovery and utilization of valuable resources,while also negative environmental effects resulting from the presence of toxic and hazardous substances.In this study,a new environmentally friendly hydro-metallurgical process was proposed for leaching lithium(Li),nickel(Ni),cobalt(Co),and manganese(Mn)from spent LIBs using sulfuric acid with citric acid as a reductant.The effects of the concentration of sulfuric acid,the leaching temperature,the leaching time,the solid-liquid ratio,and the reducing agent dosage on the leaching behavior of the above elements were investigated.Key parameters were optimized using response surface methodology(RSM)to maximize the recovery of metals from spent LIBs.The maxim-um recovery efficiencies of Li,Ni,Co,and Mn can reach 99.08%,98.76%,98.33%,and 97.63%.under the optimized conditions(the sulfuric acid concentration was 1.16 mol/L,the citric acid dosage was 15wt%,the solid-liquid ratio was 40 g/L,and the temperature was 83℃ for 120 min),respectively.It was found that in the collaborative leaching process of sulfuric acid and citric acid,the citric acid initially provided strong reducing CO_(2)^(-),and the transition metal ions in the high state underwent a reduction reaction to produce transition metal ions in the low state.Additionally,citric acid can also act as a proton donor and chelate with lower-priced transition metal ions,thus speeding up the dissolution process.

New insights into the pre-lithiation kinetics of single-crystalline Ni-rich cathodes for long-life Li-ion batteries

Developing single-crystalline Ni-rich cathodes is an effective strategy to improve the safety and cycle life of Li-ion batteries(LIBs).However,the easy-to-loss of Li and O in high-temperature lithiation results in unsatisfactory ordered layered structure and stoichiometry.Herein,we demonstrate the synthesis of highly-ordered and fully-stoichiometric single-crystalline LiNi_(0.83)Co_(0.12)Mn_(0.05)O_(2)(SC-NCM83)cathodes by the regulation of pre-lithiation kinetics.The well-balanced pre-lithiation kinetics have been proved to greatly improve the proportion of layered phase in the intermediate by inhibiting the formation of metastable spinel phase,which promoted the rapid transformation of the intermediate into highly-ordered layered SC-NCM83 in the subsequent lithiation process.After coating a layer of Li_(2)O–B_(2)O_(3),the resultant cathodes deliver superior cycling stability with 90.9%capacity retention at 1C after 300 cycles in pouch-type full batteries.The enhancement mechanism has also been clarified.These findings exhibit fundamental insights into the pre-lithiation kinetics process for guiding the synthesis of high-quality singlecrystalline Ni-rich cathodes.

Revealing the key role of non-solvating diluents for fast-charging and low temperature Li-ion batteries

Fast-charging and low temperature operation are of vital importance for the further development of lithium-ion batteries(LIBs),which is hindered by the utilization of conventional carbonate-based electrolytes due to their slow kinetics,narrow operating temperature and voltage range.Herein,an acetonitrile(AN)-based localized high-concentration electrolyte(LHCE)is proposed to retain liquid state and high ionic conductivity at ultra-low temperatures while possessing high oxidation stability.We originally reveal the excellent thermal shielding effect of non-solvating diluent to prevent the aggregation of Li^(+) solvates as temperature drops,maintaining the merits of fast Li transport and facile desolvation as at room temperature,which bestows the graphite electrode with remarkable low temperature performance(264 mA h g^(-1) at-20 C).Remarkably,an extremely high capacity retention of 97%is achieved for high-voltage high-energy graphite||NCM batteries after 250 cycles at-20 C,and a high capacity of 110 mA h g^(-1)(71%of its room-temperature capacity)is retained at-30°C.The study unveils the key role of the non-solvating diluents and provides instructive guidance in designing electrolytes towards fast-charging and low temperature LIBs.

Selective leaching of lithium from spent lithium-ion batteries using sulfuric acid and oxalic acid

Traditional hydrometallurgical methods for recovering spent lithium-ion batteries(LIBs)involve acid leaching to simultaneously extract all valuable metals into the leachate.These methods usually are followed by a series of separation steps such as precipitation,extraction,and stripping to separate the individual valuable metals.In this study,we present a process for selectively leaching lithium through the synergistic effect of sulfuric and oxalic acids.Under optimal leaching conditions(leaching time of 1.5 h,leaching temperature of 70°C,liquid-solid ratio of 4 mL/g,oxalic acid ratio of 1.3,and sulfuric acid ratio of 1.3),the lithium leaching efficiency reached89.6%,and the leaching efficiencies of Ni,Co,and Mn were 12.8%,6.5%,and 21.7%.X-ray diffraction(XRD)and inductively coupled plasma optical emission spectrometer(ICP-OES)analyses showed that most of the Ni,Co,and Mn in the raw material remained as solid residue oxides and oxalates.This study offers a new approach to enriching the relevant theory for selectively recovering lithium from spent LIBs.

Invited Review Reduction,reuse and recycle of spent Li-ion batteries for automobiles:A review

The demand for Li-ion batteries (LIBs) for vehicles is increasing. However, LIBs use valuable rare metals, such as Co and Li, aswell as environmentally toxic reagents. LIBs are also necessary to utilize for a long period and to recycle useful materials. The reduction, reuse,and recycle (3R) of spent LIBs is an important consideration in constructing a circular economy. In this paper, a flowsheet of the 3R of LIBs isproposed and methods to reduce the utilization of valuable rare metals and the amount of spent LIBs by remanufacturing used parts and designingnew batteries considering the concept of 3R are described. Next, several technological processes for the reuse and recycling of LIBs are introduced.These technologies include discharge, sorting, crushing, binder removal, physical separation, and pyrometallurgical and hydrometallurgicalprocessing. Each process, as well as the related physical, chemical, and biological treatments, are discussed. Finally, the problem of developedtechnologies and future subjects for 3R of LIBs are described.

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.

Upcycling the spent graphite/LiCoO_(2) batteries for high-voltage graphite/LiCoPO_(4)-co-workable dual-ion batteries

The worldwide proliferation of portable electronics has resulted in a dramatic increase in the number of spent lithium-ion batteries(LIBs).However,traditional recycling methods still have limitations because of such huge amounts of spent LIBs.Therefore,we proposed an ecofriendly and sustainable double recycling strategy to concurrently reuse the cathode(LiCoO_(2))and anode(graphite)materials of spent LIBs and recycled LiCoPO_(4)/graphite(RLCPG)in Li^(+)/PF^(-)_(6) co-de/intercalation dual-ion batteries.The recycle-derived dualion batteries of Li/RLCPG show impressive electrochemical performance,with an appropriate discharge capacity of 86.2 mAh·g^(-1) at25 mA·g^(-1) and 69%capacity retention after 400 cycles.Dual recycling of the cathode and anode from spent LIBs avoids wastage of resources and yields cathode materials with excellent performance,thereby offering an ecofriendly and sustainable way to design novel secondary batteries.

Interface-reinforced solid-state electrochromic Li-ion batteries enabled by in-situ liquid-solid transitional plastic glues

The electrochromic Li-ion batteries(ELIBs) combine the functions of electrochromism and energy storage,realizing the display of energy-storage levels by visual signals. However, the accompanying interfacial issues including physical contact and(electro)chemical stability should be taken into account when the conventional liquid/gel electrolytes are replaced with solid-state counterparts. Herein, the in-situ liquid-solid transitional succinonitrile(SCN) plastic glues are constructed between electrodes and poly(ethylene oxide)(PEO) polymer electrolytes, enabling an interface-reinforced solid-state ELIB.Specifically, the liquid SCN precursor can adequately wet electrode/PEO interfaces at high temperature,while it returns back to solid state at room temperature, leading to seamless interfacial contact and smooth ionic transfer without changing the solid state of the device. Moreover, the SCN interlayer suppresses the direct contact of PEO with electrodes containing high-valence metal ions, evoking the improved interfacial stability by inhibiting the oxidation of PEO. Therefore, the resultant solid-state ELIB with configuration of LiMn_(2)O_(4)/SCN-PEO-SCN/WO_(3) delivers an initial discharge capacity of 111 m A h g^(-1) along with a capacity retention of 88.3% after 200 cycles at 30 ℃. Meanwhile, the electrochromic function is integrated into the device by distinguishing its energy-storage levels through distinct color changes. This work proposes a promising solid-state ELIB with greatly reinforced interfacial compatibility by introducing in-situ solidified plastic glues.

Selective lithium recovery and regeneration of ternary cathode from spent lithium-ion batteries:Mixed HCl-H_(2)SO_(4) leaching-spray pyrolysis approach

The recycling of spent lithium-ion batteries(LIBs) is crucial for environmental protection and resource sustainability.However,the economic recovery of spent LIBs remains challenging due to low Li recovery efficiency and the need for multiple separation operations.Here,we propose a process involving mixed HCl-H_(2)SO_(4) leaching-spray pyrolysis for recycling spent ternary LIBs,achieving both selective Li recovery and the preparation of a ternary oxide precursor.Specifically,the process transforms spent ternary cathode(LiNi_(x)Co_yMn_(2)O_(2),NCM) powder into Li_(2)SO_(4) solution and ternary oxide,which can be directly used for synthesizing battery-grade Li_(2)CO_(3) and NCM cathode,respectively.Notably,SO_(4)^(2-) selectively precipitates with Li^(+) to form thermostable Li_(2)SO_(4) during the spray pyrolysis,which substantially improves the Li recovery efficiency by inhibiting Li evaporation and intercalation.Besides,SO_(2) emissions are avoided by controlling the molar ratio of Li^(+)/SO_(4)^(2-)(≥2:1),The mechanism of the preferential formation of Li_(2)SO_(4) is interpreted from its reverse solubility variation with temperature.During the recycling of spent NCM811,92% of Li is selectively recovered,and the regenerated NCM811 exhibits excellent cycling stability with a capacity retention of 81.7% after 300 cycles at 1 C.This work offers a simple and robust process for the recycling of spent NCM cathodes.

Li-Ion Transport Mechanisms in Selenide-Based Solid-State Electrolytes in Lithium-Metal Batteries:A Study of Li_(8)SeN_(2),Li_(7)PSe_(6),and Li_(6)PSe_(5)X(X=Cl,Br,I)

To achieve high-energy-density and safe lithium-metal batteries(LMBs),solid-state electrolytes(SSEs)that exhibit fast Li-ion conductivity and good stability against lithium metal are of great importance.This study presents a systematic exploration of selenide-based materials as potential SSE candidates.Initially,Li_(8)SeN_(2)and Li_(7)PSe_(6)were selected from 25 ternary selenides based on their ability to form stable interfaces with lithium metal.Subsequently,their favorable electronic insulation and mechanical properties were verified.Furthermore,extensive theoretical investigations were conducted to elucidate the fundamental mechanisms underlying Li-ion migration in Li_(8)SeN_(2),Li_(7)PSe_(6),and derived Li_(6)PSe_(5)X(X=Cl,Br,I).Notably,the highly favorable Li-ion conduction mechanism of vacancy diffusion was identified in Li6PSe5Cl and Li_(7)PSe_(6),which exhibited remarkably low activation energies of 0.21 and 0.23 eV,and conductivity values of 3.85×10^(-2)and 2.47×10^(-2)S cm^(-1)at 300 K,respectively.In contrast,Li-ion migration in Li_(8)SeN_(2)was found to occur via a substitution mechanism with a significant diffusion energy barrier,resulting in a high activation energy and low Li-ion conductivity of 0.54 eV and 3.6×10^(-6)S cm^(-1),respectively.Throughout this study,it was found that the ab initio molecular dynamics and nudged elastic band methods are complementary in revealing the Li-ion conduction mechanisms.Utilizing both methods proved to be efficient,as relying on only one of them would be insufficient.The discoveries made and methodology presented in this work lay a solid foundation and provide valuable insights for future research on SSEs for LMBs.

Atomistic understanding of capacity loss in LiNiO_(2)for high-nickel Li-ion batteries:First-principles study

Combining the first-principles calculations and structural enumeration with recognition,the delithiation process of LiNiO_(2)is investigated,where various supercell shapes are considered in order to obtain the formation energy of Li_(x)NiO_(2).Meanwhile,the voltage profile is simulated and the ordered phases of lithium vacancies corresponding to concentrations of 1/4,2/5,3/7,1/2,2/3,3/4,5/6,and 6/7 are predicted.To understand the capacity decay in the experiment during the charge/discharge cycles,deoxygenation and Li/Ni antisite defects are calculated,revealing that the chains of oxygen vacancies will be energetically preferrable.It can be inferred that in the absence of oxygen atom in high delithiate state,the diffusion of Ni atoms is facilitated and the formation of Li/Ni antisite is induced.

Two-dimensional MOF-based materials:Preparations and applications as electrodes in Li-ion batteries

Two-dimensional(2D)metal-organic frameworks(MOFs)are rapidly emerging as a unique class of mushrooming family of 2D materials offering distinctive features,such as hierarchical porosity,extensive surface area,easily available active sites,and versatile,adaptable structures.These promising characteristics have positioned them as highly appealing alternatives for a wide range of applications in energy storage technologies,including lithium batteries.Nevertheless,the poor conductivity and limited stability of 2D MOFs have limited their real applications in electrochemical energy storage.These limitations have therefore warranted ongoing research to enhance the performance of 2D MOFs.Given the significance of 2D MOF-based materials as an emerging class of advanced materials,a multitude of strategy has been devised to address these challenges such as synthesizing 2D conductive MOFs and derivatives along with 2D MOF hybridization.One promising approach involves the use of 2D MOF derivatives,including transition metal oxides,which due to their abundant unsatu rated active metal sites and shorter diffusion paths,offer superior electrochemical performance.Additionally,by combining pristine 2D MOFs with other materials,hybrid 2D MOF materials can be created.These hybrids,with their enhanced stability and conductivity,can be directly utilized as active materials in lithium batteries.In the present review,we categorize 2D MOF-based materials into three distinct groups:pristine 2D MOFs,2D MOFderived materials,and 2D MOF hybrid materials.The synthesis methods for each group,along with their specific applications as electrode materials in lithium-ion batteries,are discussed in detail.This comprehensive review provides insights into the potential of 2D MOFs while highlighting the opportunities and challenges that are present in this evolving field.

Preparation of lithium-ion battery anode materials from graphitized spent carbon cathode derived from aluminum electrolysis

Graphitized spent carbon cathode(SCC)is a hazardous solid waste generated in the aluminum electrolysis process.In this study,a flotation-acid leaching process is proposed for the purification of graphitized SCC,and the use of the purified SCC as an anode material for lithium-ion batteries is explored.The flotation and acid leaching processes were separately optimized through one-way experiments.The maximum SCC carbon content(93wt%)was achieved at a 90%proportion of−200-mesh flotation particle size,a slurry concentration of 10wt%,a rotation speed of 1600 r/min,and an inflatable capacity of 0.2 m^(3)/h(referred to as FSCC).In the subsequent acid leaching process,the SCC carbon content reached 99.58wt%at a leaching concentration of 5 mol/L,a leaching time of 100 min,a leaching temperature of 85°C,and an HCl/FSCC volume ratio of 5:1.The purified graphitized SCC(referred to as FSCC-CL)was utilized as an anode material,and it exhibited an initial capacity of 348.2 mAh/g at 0.1 C and a reversible capacity of 347.8 mAh/g after 100 cycles.Moreover,compared with commercial graphite,FSCC-CL exhibited better reversibility and cycle stability.Thus,purified SCC is an important candidate for anode material,and the flotation-acid leaching purification method is suitable for the resourceful recycling of SCC.

Thermal decomposition kinetics of basic carbonate cobalt nanosheets obtained from spent Li-ion batteries:Deconvolution of overlapping complex reactions

A new non-isothermal method of kinetic analysis was employed to investigate the thermal decomposition kinetic modeling of the basic carbonate cobalt nanosheets（n-BCoC） synthesized from spent lithium-ion batteries（LIBs）. Fraser–Suzuki function was applied to deconvoluting overlapping complex processes from the overall differential thermal curves obtained under the linear heating rate conditions, followed by the kinetic analysis of the discrete processes using a new kinetic analysis method. Results showed that the decomposition of n-BCo C in air occurred through two consecutive reactions in the 136-270 ℃ temperature intervals. Decomposition started by hydroxide component（Co（OH）2） decomposition until to 65% and simultaneously carbonate phase decarbonation began. The process was continued by CO2 evolution and finally carbonate cobalt nanosheets have been produced. The reaction mechanism of the whole process can be kinetically characterized by two successive reactions： a phase boundary contracting reaction followed by an Avrami-Erofeev equation. Mechanistic information obtained by the kinetic study was in good agreement with FT-IR（Fourier transform infrared spectroscopy） and SEM（scanning electron microscopy） results.

Enhanced Li storage of pure crystalline-C_(60) and TiNb_(2)O_(7)-nanostructure composite for Li-ion battery anodes

We propose a method for producing composite materials(hTNO@C_(60))comprising crystalline C_(60)particles and hollow-structu red TiNb_(2)O_(7)(hTNO)nanofibers via facile liquid-liquid interface precipitation followed by low-temperature annealing.This allows the systematic design of crystalline C_(60)as an active material for Li-ion battery anodes.The hTNO@C_(60)composite demonstrates outstanding cyclic stability,retaining a capacity of 465 mA h g^(-1)after 1,000 cycles at 1 A g^(-1)It maintains a capacity of 98 mA h g^(-1)even after16,000 ultralong cycles at 8 A g^(-1)The enhancement in electrochemical properties is attributed to the successful growth and uniform doping of crystalline C_(60),resulting in improved electrical conductivity.The excellent electrochemical stability and properties of these composites make them promising anode materials.

Effect of Heatpipe Array Condenser Section Length on Thermal Cooling of Li-Ion Batteries

One of the new methods for ensuring that the battery in a thermal energy storage system is kept at the proper temperature is the heat pipe-based ThermalManagement System(TMS).In this study,the improvement of cooling performance of a heat pipe based TMS is examined through the variation of condenser section length of heat pipes in an array.The TMSs with an array of heat pipes with different condenser section lengths are considered.The system performances are evaluated using a validated numerical method.The results show that a heat pipebased TMS provides the best cooling performance when a wavy-like variation is employed and when the condenser section length of the last set of the heat pipe in the array is greater than that of the penultimate set.The maximum cell temperature and the maximum temperature difference within the cell of this TMS are decreased by 4.2 K and 1.1 K,respectively,when compared to the typical heat pipe based TMS with zero variation in its condenser section length.Conclusively,the strategy offers an improvement in the thermal uniformity for all the TMS cases.

Preparation of LiNi_(1/3)Co_(1/3)Mn_(1/3)O_2 cathode materials from spent Li-ion batteries

A recycling process including separation of electrode materials by ultrasonic treatment,acid leaching,Fe-removing,precipitation of cobalt,nickel,manganese and lithium has been applied successfully to recycle spent lithium-ion batteries and to synthesize LiNi1/3Co1/3Mn1/3O2. When ultrasonic treatment with 2-nitroso-4-methylphenol(NMP) at 40 ℃ for 15 min,the electrode materials are separated completely. Above 99% of Co,Ni,Mn and Li,95% of Fe in the separated electrodes are acid-leached in the optimized conditions of 2 mol/L H2SO4,1∶2 H2O2-H2SO4(molar ratio),70 ℃,1∶10 initial S∶L ratio,and 1 h. 99.5% of Fe and less than 1% of Co,Ni,Mn in the leaching solution can be removed in the conditions of initial pH value 2.0-2.5 adjusted by adding 18% Na2CO3,90 ℃ and stirring time 3 h. After adjusted to be equal by adding NiSO4,CoSO4 and MnSO4 solution,97.1% of Ni,Co,Mn in the Fe-removing surplus leaching solution can be recovered as Ni1/3Co1/3Mn1/3(OH)2. 94.5% of Li in the surplus filtrate after the deposition of Co,Ni and Mn can be recovered as Li2CO3. The LiNi1/3Co1/3Mn1/3O2,prepared from the recovered compounds,is found to have good characteristics of the layered structure and elecrtochemical performance.

Low-temperature chlorination roasting technology for the simultaneous recovery of valuable metals from spent LiCoO_(2)cathode material

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.