Valuable metals recovery from spent ternary lithium-ion battery: A review

Abstract

Ternary lithium-ion batteries (LIBs), widely used in new energy vehicles and electronic products, are known for their high energy density, wide operating temperature range, and excellent cycling performance. With the rapid development of the battery industry, the recycling of spent ternary LIBs has become a hot topic because of their economic value and environmental concerns. To date, a considerable amount of literature has reported on the recycling of spent ternary LIBs designed to provide an efficient, economical, and environmentally friendly method for battery recycling. This article examines the latest developments in various technologies for recycling spent ternary LIBs in both research and practical production, including pretreatment, pyrometallurgy, hydrometallurgy, pyro-hydrometallurgy, and direct regeneration. Suggestions for addressing challenges based on the benefits and disadvantages of each method are made. Finally, through a comparison of the feasibility and economic benefits of various technologies, the challenges faced during battery recycling are summarized, and future development directions are proposed.

Keywords

spent ternary LIBs / recycling technologies / valuable metals / economic analysis

References

[1] J. Xie and Y.C. Lu, A retrospective on lithium-ion batteries, Nat. Commun., 11(2020), No. 1, art. No. 2499.

[2] V. Gupta, X.L. Yu, H.P. Gao, C. Brooks, W.K. Li, and Z. Chen, Scalable direct recycling of cathode black mass from spent lithium-ion batteries, Adv. Energy Mater., 13(2023), No. 6, art. No. 2203093.

[3] Yu JD, He YQ, Ge ZZ, Li H, Xie WN, Wang S. A promising physical method for recovery of LiCoO₂ and graphite from spent lithium-ion batteries: Grinding flotation. Sep. Purif. Technol.. 2018, 190: 45

[4] Z.G. Cun, P. Xing, C.Y. Wang, et al., Stepwise recovery of critical metals from spent NCM lithium-ion battery via calcium hydroxide assisted pyrolysis and leaching, Resour. Conserv. Recycl., 202(2024), art. No. 107390.

[5] W.H. Yu, Y.C. Zhang, J.H. Hu, et al., Controlled carbothermic reduction for enhanced recovery of metals from spent lithium-ion batteries, Resour. Conserv. Recycl., 194(2023), art. No. 107005.

[6] Tan JH, Wang Q, Chen S, et al. . Recycling-oriented cathode materials design for lithium-ion batteries: Elegant structures versus complicated compositions. Energy Storage Mater.. 2021, 41: 380

[7] Wei JC, Zhao SC, Ji LX, et al. . Reuse of Ni–Co–Mn oxides from spent Li-ion batteries to prepare bifunctional air electrodes. Resour. Conserv. Recycl.. 2018, 129: 135

[8] Winslow KM, Laux SJ, Townsend TG. A review on the growing concern and potential management strategies of waste lithium-ion batteries. Resour. Conserv. Recycl.. 2018, 129: 263

[9] Mrozik W, Rajaeifar MA, Heidrich O, Christensen PA. Environmental impacts, pollution sources and pathways of spent lithium-ion batteries. Energy Environ. Sci.. 2021, 14(12): 6099

[10] Y.F. Shen, Recycling cathode materials of spent lithium-ion batteries for advanced catalysts production, J. Power Sources, 528(2022), art. No. 231220.

[11] Song JL, Yan WY, Cao HB, et al. . Material flow analysis on critical raw materials of lithium-ion batteries in China. J. Clean. Prod.. 2019, 215: 570

[12] Harper G, Sommerville R, Kendrick E, et al. . Recycling lithium-ion batteries from electric vehicles. Nature. 2019, 575(7781): 75

[13] B. Makuza, Q.H. Tian, X.Y. Guo, K. Chattopadhyay, and D.W. Yu, Pyrometallurgical options for recycling spent lithium-ion batteries: A comprehensive review, J. Power Sources, 491(2021), art. No. 229622.

[14] X.F. Hu, E. Mousa, and G.Z. Ye, Recovery of Co, Ni, Mn, and Li from Li-ion batteries by smelting reduction-Part II: A pilot-scale demonstration, J. Power Sources, 483(2021), art. No. 229089.

[15] Schwich L, Friedrich B. Proven methods for recovery of lithium from spent batteries. DERA Workshop Lithium. 2017

[16] Wang C, Wang SB, Yan F, Zhang Z, Shen XH, Zhang ZT. Recycling of spent lithium-ion batteries: Selective ammonia leaching of valuable metals and simultaneous synthesis of high-purity manganese carbonate. Waste Manage.. 2020, 114: 253

[17] Wang HY, Huang K, Zhang Y, et al. . Recovery of lithium, nickel, and cobalt from spent lithium-ion battery powders by selective ammonia leaching and an adsorption separation system. ACS Sustainable Chem. Eng.. 2017, 5(12): 11489

[18] Yang Y, Lei SY, Song SL, Sun W, Wang LS. Step-wise recycling of valuable metals from Ni-rich cathode material of spent lithium-ion batteries. Waste Manage.. 2020, 102: 131

[19] Horeh NB, Mousavi SM, Shojaosadati SA. Bioleaching of valuable metals from spent lithium-ion mobile phone batteries using Aspergillus Niger. J. Power Sources. 2016, 320: 257

[20] Hu JT, Zhang JL, Li HX, Chen YQ, Wang CY. A promising approach for the recovery of high value-added metals from spent lithium-ion batteries. J. Power Sources. 2017, 351: 192

[21] Lei SY, Zhang YT, Song SL, et al. . Strengthening valuable metal recovery from spent lithium-ion batteries by environmentally friendly reductive thermal treatment and electrochemical leaching. ACS Sustainable Chem. Eng.. 2021, 9(20): 7053

[22] Jiang GH, Zhang YN, Meng Q, et al. . Direct regeneration of LiNi_0.5Co_0.2Mn_0.3O₂ cathode from spent lithium-ion batteries by the molten salts method. ACS Sustainable Chem. Eng.. 2020, 8(49): 18138

[23] Shi Y, Chen G, Liu F, Yue XJ, Chen Z. Resolving the compositional and structural defects of degraded LiNi_xCo_yMn_zO₂ particles to directly regenerate high-performance lithium-ion battery cathodes. ACS Energy Lett.. 2018, 3(7): 1683

[24] Xing CX, Da HR, Yang P, et al. . Aluminum impurity from current collectors reactivates degraded NCM cathode materials toward superior electrochemical performance. ACS Nano. 2023, 17(3): 3194

[25] Z.Y. Qin, Z.X. Wen, Y.F. Xu, et al., A ternary molten salt approach for direct regeneration of LiNi_0.5Co_0.2Mn_0.3O₂ cathode, Small, 18(2022), No. 43, art. No. 2106719.

[26] Tarascon JM, Armand M. Issues and challenges facing rechargeable lithium batteries. Nature. 2001, 414: 359

[27] Zheng XH, Zhu ZW, Lin X, et al. . A mini-review on metal recycling from spent lithium ion batteries. Engineering. 2018, 4(3): 361

[28] Arshad F, Li L, Amin K, et al. . A comprehensive review of the advancement in recycling the anode and electrolyte from spent lithium ion batteries. ACS Sustainable Chem. Eng.. 2020, 8(36): 13527

[29] Leal VM, Ribeiro JS, Coelho ELD, Freitas MBJG. Recycling of spent lithium-ion batteries as a sustainable solution to obtain raw materials for different applications. J. Energy Chem.. 2023, 79: 118

[30] Ordoñez J, Gago EJ, Girard A. Processes and technologies for the recycling and recovery of spent lithium-ion batteries. Renewable Sustainable Energy Rev.. 2016, 60: 195

[31] Lebedeva NP, Boon-Brett L. Considerations on the chemical toxicity of contemporary Li-ion battery electrolytes and their components. J. Electrochem. Soc.. 2016, 163(6): A821

[32] Lv WG, Wang ZH, Cao HB, Sun Y, Zhang Y, Sun Z. A critical review and analysis on the recycling of spent lithium-ion batteries. ACS Sustainable Chem. Eng.. 2018, 6(2): 1504

[33] Zhang XX, Li L, Fan ES, et al. . Toward sustainable and systematic recycling of spent rechargeable batteries. Chem. Soc. Rev.. 2018, 47(19): 7239

[34] Wang FF, Zhang T, He YQ, et al. . Recovery of valuable materials from spent lithium-ion batteries by mechanical separation and thermal treatment. J. Clean. Prod.. 2018, 185: 646

[35] Li J, Wang GX, Xu ZM. Generation and detection of metal ions and volatile organic compounds (VOCs) emissions from the pretreatment processes for recycling spent lithium-ion batteries. Waste Manage.. 2016, 52: 221

[36] Granata G, Pagnanelli F, Moscardini E, Takacova Z, Havlik T, Toro L. Simultaneous recycling of nickel metal hydride, lithium ion and primary lithium batteries: Accomplishment of European Guidelines by optimizing mechanical pre-treatment and solvent extraction operations. J. Power Sources. 2012, 212: 205

[37] He LP, Sun SY, Mu YY, Song XF, Yu JG. Recovery of lithium, nickel, cobalt, and manganese from spent lithium-ion batteries using l-tartaric acid as a leachant. ACS Sustainable Chem. Eng.. 2017, 5(1): 714

[38] E. Mossali, N. Picone, L. Gentilini, O. Rodrìguez, J.M. Pérez, and M. Colledani, Lithium-ion batteries towards circular economy: A literature review of opportunities and issues of recycling treatments, J. Environ. Manage., 264(2020), art. No. 110500.

[39] Ojanen S, Lundstróm M, Santasalo-Aarnio A, Serna-Guerrero R. Challenging the concept of electrochemical discharge using salt solutions for lithium-ion batteries recycling. Waste Manage.. 2018, 76: 242

[40] Zhong XH, Liu W, Han JW, Jiao F, Zhu HL, Qin WQ. Pneumatic separation for crushed spent lithium-ion batteries. Waste Manage.. 2020, 118: 331

[41] Hanisch C, Loellhoeffel T, Diekmann J, Markley KJ, Haselrieder W, Kwade A. Recycling of lithium-ion batteries: A novel method to separate coating and foil of electrodes. J. Clean. Prod.. 2015, 108: 301

[42] Y. Ji, C.T. Jafvert, N.N. Zyaykina, and F. Zhao, Decomposition of PVDF to delaminate cathode materials from end-of-life lithium-ion battery cathodes, J. Clean. Prod., 367(2022), art. No. 133112.

[43] Ferreira DA, Prados LMZ, Majuste D, Mansur MB. Hydrometallurgical separation of aluminium, cobalt, copper and lithium from spent Li-ion batteries. J. Power Sources. 2009, 187(1): 238

[44] Nayaka GP, Pai KV, Manjanna J, Keny SJ. Use of mild organic acid reagents to recover the Co and Li from spent Li-ion batteries. Waste Manage.. 2016, 51: 234

[45] Nan JM, Han DM, Zuo XX. Recovery of metal values from spent lithium-ion batteries with chemical deposition and solvent extraction. J. Power Sources. 2005, 152: 278

[46] Mu DY, Ma WL, Yang W, Dai CS. Discharge of spent lithium ion battery and separation and recovery of cathode electrode. Environ. Prot. Chem. Ind.. 2020, 40(1): 63

[47] Yang Y, Huang GY, Xu SM, He YH, Liu X. Thermal treatment process for the recovery of valuable metals from spent lithium-ion batteries. Hydrometallurgy. 2016, 165: 390

[48] Yang L, Xi GX, Xi YB. Recovery of Co, Mn, Ni, and Li from spent lithium ion batteries for the preparation of LiNi_xCo_yMn_zO₂ cathode materials. Ceram. Int.. 2015, 41(9): 11498

[49] Li L, Chen RJ, Sun F, Wu F, Liu JR. Preparation of LiCoO₂ films from spent lithium-ion batteries by a combined recycling process. Hydrometallurgy. 2011, 108(3–4): 220

[50] Li L, Dunn JB, Zhang XX, Gaines L, Chen RJ, Wu F, Amine K. Recovery of metals from spent lithium-ion batteries with organic acids as leaching reagents and environmental assessment. J. Power Sources. 2013, 233: 180

[51] Xu YN, Song DW, Li L, et al. . A simple solvent method for the recovery of Li_xCoO₂ and its applications in alkaline rechargeable batteries. J. Power Sources. 2014, 252: 286

[52] Zhang GW, He YQ, Feng Y, et al. . Enhancement in liberation of electrode materials derived from spent lithium-ion battery by pyrolysis. J. Clean. Prod.. 2018, 199: 62

[53] G. Lombardo, B. Ebin, M.R.S.J. Foreman, B.M. Steenari, and M. Petranikova, Incineration of EV lithium-ion batteries as a pretreatment for recycling–determination of the potential formation of hazardous by-products and effects on metal compounds, J. Hazard. Mater., 393(2020), art. No. 122372.

[54] Lombardo G, Ebin B, Foreman MRStJ, Steenari BM, Petranikova M. Chemical transformations in Li-ion battery electrode materials by carbothermic reduction. ACS Sustainable Chem. Eng.. 2019, 7(16): 13668

[55] Sun L, Qiu KQ. Vacuum pyrolysis and hydrometallurgical process for the recovery of valuable metals from spent lithium-ion batteries. J. Hazard. Mater.. 2011, 194: 378

[56] He LP, Sun SY, Song XF, Yu JG. Recovery of cathode materials and Al from spent lithium-ion batteries by ultrasonic cleaning. Waste Manage.. 2015, 46: 523

[57] Zhao L, Zhang XY, Lu YY, et al. . Recovery of electrode materials from a spent lithium-ion battery through a pyrolysis-coupled mechanical milling method. Energy Fuels. 2024, 38(2): 1310

[58] Huang B, Pan ZF, Su XY, An L. Recycling of lithiumion batteries: Recent advances and perspectives. J. Power Sources. 2018, 399: 274

[59] Ren GX, Xiao SW, Xie MQ, et al. . Recovery of valuable metals from spent lithium ion batteries by smelting reduction process based on FeO–SiO₂–Al₂O₃ slag system. Trans. Nonferrous Met. Soc. China. 2017, 27(2): 450

[60] van Bommel A, Dahn JR. Analysis of the growth mechanism of coprecipitated spherical and dense nickel, manganese, and cobalt-containing hydroxides in the presence of aqueous ammonia. Chem. Mater.. 2009, 21(8): 1500

[61] Zeng XL, Li JH, Shen BY. Novel approach to recover cobalt and lithium from spent lithium-ion battery using oxalic acid. J. Hazard. Mater.. 2015, 295: 112

[62] Yao YL, Zhu MY, Zhao Z, Tong BH, Fan YQ, Hua ZS. Hydrometallurgical processes for recycling spent lithiumion batteries: A critical review. ACS Sustainable Chem. Eng.. 2018, 6(11): 13611

[63] Chen XP, Fan BL, Xu LP, Zhou T, Kong JR. An atom-economic process for the recovery of high value-added metals from spent lithium-ion batteries. J. Clean. Prod.. 2016, 112: 3562

[64] Takacova Z, Havlik T, Kukurugya F, Orac D. Cobalt and lithium recovery from active mass of spent Li-ion batteries: Theoretical and experimental approach. Hydrometallurgy. 2016, 163: 9

[65] Zheng XH, Gao WF, Zhang XH, et al. . Spent lithium-ion battery recycling–Reductive ammonia leaching of metals from cathode scrap by sodium sulphite. Waste Manage.. 2017, 60: 680

[66] Wang RC, Lin YC, Wu SH. A novel recovery process of metal values from the cathode active materials of the lithium-ion secondary batteries. Hydrometallurgy. 2009, 99(3–4): 194

[67] Li L, Bian YF, Zhang XX, et al. . Process for recycling mixed-cathode materials from spent lithium-ion batteries and kinetics of leaching. Waste Manage.. 2018, 71: 362

[68] He LP, Sun SY, Song XF, Yu JG. Leaching process for recovering valuable metals from the LiNi_1/3Co_1/3Mn_1/3O₂ cathode of lithium-ion batteries. Waste Manage.. 2017, 64: 171

[69] Vieceli N, Casasola R, Lombardo G, Ebin B, Petranikova M. Hydrometallurgical recycling of EV lithium-ion batteries: Effects of incineration on the leaching efficiency of metals using sulfuric acid. Waste Manage.. 2021, 125: 192

[70] Xuan W, Otsuki A, Chagnes A. Investigation of the leaching mechanism of NMC 811 (LiNi_0.8Mn_0.1Co_0.1O₂) by hydrochloric acid for recycling lithium ion battery cathodes. RSC Adv.. 2019, 9(66): 38612

[71] Liu PC, Xiao L, Tang YW, Chen YF, Ye LG, Zhu YR. Study on the reduction roasting of spent LiNi_xCo_yMn_zO₂ lithium-ion battery cathode materials. J. Therm. Anal. Calorim.. 2019, 136(3): 1323

[72] Z.M. Yan, A. Sattar, and Z.S. Li, Priority Lithium recovery from spent Li-ion batteries via carbothermal reduction with water leaching, Resour. Conserv. Recycl., 192(2023), art. No. 106937.

[73] Y. Ahn, W. Koo, K. Yoo, and R.D. Alorro, Carbothermic reduction roasting of cathode active materials using activated carbon and graphite to enhance the sulfuric-acid-leaching efficiency of nickel and cobalt, Minerals, 12(2022), No. 8, art. No. 1021.

[74] L.W. Ma, X.L. Xi, Z.Z. Zhang, and Z. Lyu, Separation and comprehensive recovery of cobalt, nickel, and lithium from spent power lithium-ion batteries, Minerals, 12(2022), No. 4, art. No. 425.

[75] Meng XQ, Hao J, Cao HB, et al. . Recycling of LiNi_1/3Co_1/3Mn_1/3O₂ cathode materials from spent lithium-ion batteries using mechanochemical activation and solid-state sintering. Waste Manage.. 2019, 84: 54

[76] Y. Shi, M.H. Zhang, Y.S. Meng, and Z. Chen, Ambient-pressure relithiation of degraded Li_xNi_0.5Co_0.2Mn_0.3O₂ (0 < x < 1) via eutectic solutions for direct regeneration of lithium-ion battery cathodes, Adv. Energy Mater., 9(2019), No. 20, art. No. 1900454.

[77] Zhang XH, Xie YB, Cao HB, Nawaz F, Zhang Y. A novel process for recycling and resynthesizing LiNi_1/3Co_1/3Mn_1/3O₂ from the cathode scraps intended for lithium-ion batteries. Waste Manaeg.. 2014, 34(9): 1715

[78] S.E. Sloop, L. Crandon, M. Allen, et al., Cathode healing methods for recycling of lithium-ion batteries, Sustain. Mater. Technol., 22(2019), art. No. e00113.

[79] Xiao SW, Ren GX, Xie MQ, et al. . Recovery of valuable metals from spent lithium-ion batteries by smelting reduction process based on MnO–SiO₂–Al₂O₃ slag system. J. Sustain. Metall.. 2017, 3(4): 703

[80] Vezzini A. Pistoia G. Manufacturers, materials and recycling technologies. Lithium-Ion Batteries: Advances and Applications. 2014, Amsterdam, Elsevier: 529

[81] Dutta D, Kumari A, Panda R, et al. . Close loop separation process for the recovery of Co, Cu, Mn, Fe and Li from spent lithium-ion batteries. Sep. Purif. Technol.. 2018, 200: 327

[82] Ren LY, Liu B, Bao SX, et al. . Recovery of Li, Ni, Co and Mn from spent lithium-ion batteries assisted by organic acids: Process optimization and leaching mechanism. Int. J. Miner. Metall. Mater.. 2024, 31(3): 518

[83] Yu HJ, Wang DX, Rao S, et al. . Selective leaching of lithium from spent lithium-ion batteries using sulfuric acid and oxalic acid. Int. J. Miner. Metall. Mater.. 2024, 31(4): 688

[84] Li L, Bian YF, Zhang XX, et al. . Economical recycling process for spent lithium-ion batteries and macro- and micro-scale mechanistic study. J. Power Sources. 2018, 377: 70

[85] Zhuang LQ, Sun CH, Zhou T, Li H, Dai AQ. Recovery of valuable metals from LiNi_0.5Co_0.2Mn_0.3O₂ cathode materials of spent Li-ion batteries using mild mixed acid as leachant. Waste Manage.. 2019, 85: 175

[86] Jegan Roy J, Srinivasan M, Cao B. Bioleaching as an eco-friendly approach for metal recovery from spent NMC-based lithium-ion batteries at a high pulp density. ACS Sustainable Chem. Eng.. 2021, 9(8): 3060

[87] Xin YY, Guo XM, Chen S, Wang J, Wu F, Xin BP. Bioleaching of valuable metals Li, Co, Ni and Mn from spent electric vehicle Li-ion batteries for the purpose of recovery. J. Clean. Prod. 2016, 116: 249

[88] Baniasadi M, Vakilchap F, Bahaloo-Horeh N, Mousavi SM, Farnaud S. Advances in bioleaching as a sustainable method for metal recovery from e-waste: A review. J. Ind. Eng. Chem.. 2019, 76: 75

[89] Zhang YC, Wang WQ, Fang Q, Xu SM. Improved recovery of valuable metals from spent lithium-ion batteries by efficient reduction roasting and facile acid leaching. Waste Manage.. 2020, 102: 847

[90] Zhang YC, Wang WQ, Hu JH, Zhang T, Xu SM. Stepwise recovery of valuable metals from spent lithium ion batteries by controllable reduction and selective leaching and precipitation. ACS Sustainable Chem. Eng.. 2020, 8(41): 15496

[91] C. Yang, J.L. Zhang, B.Y. Yu, H. Huang, Y.Q. Chen, and C.Y. Wang, Recovery of valuable metals from spent LiNi_xCo_yMn_zO₂ cathode material via phase transformation and stepwise leaching, Sep. Purif. Technol., 267(2021), art. No. 118609.

[92] Zhang JL, Liang GQ, Yang C, Hu JT, Chen YQ, Wang CY. A breakthrough method for the recycling of spent lithium-ion batteries without pre-sorting. Green Chem.. 2021, 23(21): 8434

[93] C. Yang, J.L. Zhang, G.Q. Liang, H. Jin, Y.Q. Chen, and C.Y. Wang, An advanced strategy of “metallurgy before sorting” for recycling spent entire ternary lithium-ion batteries, J. Clean. Prod., 361(2022), art. No. 132268.

[94] Zhang YC, Yu WH, Xu SM. Enhanced leaching of metals from spent lithium-ion batteries by catalytic carbothermic reduction. Rare Met.. 2023, 42(8): 2688

[95] S.B. Ma, F.P. Liu, K.B. Li, et al., Separation of Li and Al from spent ternary Li-ion batteries by in situ aluminum-carbon reduction roasting followed by selective leaching, Hydrometallurgy, 213(2022), art. No. 105941.

[96] W.Q. Wang, Y.C. Zhang, L. Zhang, and S.M. Xu, Cleaner recycling of cathode material by in situ thermite reduction, J. Clean. Prod., 249(2020), art. No. 119340.

[97] F.P. Liu, C. Peng, Q.X. Ma, et al., Selective lithium recovery and integrated preparation of high-purity lithium hydroxide products from spent lithium-ion batteries, Sep. Purif. Technol., 259(2021), art. No. 118181.

[98] Liu H, Zhang JL, Liang GQ, Wang M, Chen YQ, Wang CY. Selective lithium recovery from black powder of spent lithium-ion batteries via sulfation reaction: Phase conversion and impurities influence. Rare Met.. 2023, 42(7): 2350

[99] Yang C, Zhang JL, Cao ZH, Jing QK, Chen YQ, Wang CY. Sustainable and facile process for lithium recovery from spent LiNi_xCo_yMn_zO₂ cathode materials via selective sulfation with ammonium sulfate. ACS Sustainable Chem. Eng.. 2020, 8(41): 15732

[100] Lin J, Li L, Fan ES, et al. . Conversion mechanisms of selective extraction of lithium from spent lithium-ion batteries by sulfation roasting. ACS Appl. Mater. Interfaces. 2020, 12(16): 18482

[101] Peng C, Liu FP, Wang ZL, Wilson BP, Lundstróm M. Selective extraction of lithium (Li) and preparation of battery grade lithium carbonate (Li₂CO₃) from spent Li-ion batteries in nitrate system. J. Power Sources. 2019, 415: 179

[102] Y. Huang, P.H. Shao, L.M. Yang, et al., Thermochemically driven crystal phase transfer via chlorination roasting toward the selective extraction of lithium from spent LiNi_1/3Co_1/3Mn_1/3O₂, Resour. Conserv. Recycl., 174(2021), art. No. 105757.

[103] G.C. Shi, N. Zhang, J. Cheng, et al., Full closed-loop green regeneration and recycling technology for spent ternary lithium batteries: Hydrogen reduction with sulfuric acid cycle-leaching process, J. Environ. Chem. Eng., 11(2023), No. 6, art. No. 111207.

[104] J.H. Zhou, X. Zhou, W.H. Yu, Z. Shang, Y. Yang, and S.M. Xu, Solvothermal strategy for direct regeneration of high-performance cathode materials from spent lithium-ion battery, Nano Energy, 120(2024), art. No. 109145.

[105] Lu YQ, Peng KY, Zhang LG. Sustainable recycling of electrode materials in spent Li-ion batteries through direct regeneration processes. ACS ES&T Eng.. 2022, 2(4): 586

[106] Yang X, Zhang YJ, Xiao J, et al. . Restoring surface defect crystal of Li-lacking LiNi_0.6Co_0.2Mn_0.2O₂ material particles toward more efficient recycling of lithium-ion batteries. ACS Sustainable Chem. Eng.. 2021, 9(50): 16997

[107] Yu XL, Yu SC, Yang ZZ, et al. . Achieving low-temperature hydrothermal relithiation by redox mediation for direct recycling of spent lithium-ion battery cathodes. Energy Storage Mater.. 2022, 51: 54

[108] Ma J, Wang JX, Jia K, et al. . Adaptable eutectic salt for the direct recycling of highly degraded layer cathodes. J. Am. Chem. Soc.. 2022, 144(44): 20306

[109] P.P. Xu, D.H.S. Tan, B.L. Jiao, H.P. Gao, X.L. Yu, and Z. Chen, A materials perspective on direct recycling of lithiumion batteries: Principles, challenges and opportunities, Adv. Funct. Mater., 33(2023), No. 14, art. No. 2213168.

[110] W.S. Chen and H.J. Ho, Recovery of valuable metals from lithium-ion batteries NMC cathode waste materials by hydrometallurgical methods, Metals, 8(2018), No. 5, art. No. 321.

[111] Meshram P, Pandey BD, Mankhand TR. Hydrometallurgical processing of spent lithium ion batteries (LIBs) in the presence of a reducing agent with emphasis on kinetics of leaching. Chem. Eng. J.. 2015, 281: 418

[112] Lupi C, Pasquali M, Dell’Era A. Nickel and cobalt recycling from lithium-ion batteries by electrochemical processes. Waste Manaeg.. 2005, 25(2): 215

[113] Chen XP, Chen YB, Zhou T, Liu DP, Hu H, Fan SY. Hydrometallurgical recovery of metal values from sulfuric acid leaching liquor of spent lithium-ion batteries. Waste Manage.. 2015, 38: 349

[114] Vasilyev F, Virolainen S, Sainio T. Numerical simulation of counter-current liquid-liquid extraction for recovering Co, Ni and Li from lithium-ion battery leachates of varying composition. Sep. Purif Technol.. 2019, 210: 530

[115] A. Keller, M.W. Hlawitschka, and H.J. Bart, Manganese recycling of spent lithium-ion batteries via solvent extraction, Sep. Purif. Technol., 275(2021), art. No. 119166.

[116] K.F. Zhang, H.L. Liang, X.C. Zhong, H.Y. Cao, R.X. Wang, and Z.Q. Liu, Recovery of metals from sulfate leach solutions of spent ternary lithium-ion batteries by precipitation with phosphate and solvent extraction with P507, Hydrometallurgy, 210(2022), art. No. 105861.

[117] C.Y. Li, G.F. Dai, R.Y. Liu, et al., Separation and recovery of nickel cobalt manganese lithium from waste ternary lithiumion batteries, Sep. Purif Technol., 306(2023), art. No. 122559.

[118] Virolainen S, Fallah Fini M, Laitinen A, Sainio T. Solvent extraction fractionation of Li-ion battery leachate containing Li, Ni, and Co. Sep. Purif. Technol.. 2017, 179: 274

[119] Granata G, Moscardini E, Pagnanelli F, Trabucco F, Toro L. Product recovery from Li-ion battery wastes coming from an industrial pre-treatment plant: Lab scale tests and process simulations. J. Power Sources. 2012, 206: 393

[120] T. Tawonezvi, D. Zide, M. Nomnqa, M. Madondo, L. Petrik, and B.J. Bladergroen, Recovery of Ni_xMn_yCo_z(OH)₂ and Li₂CO₃ from spent Li-ionB cathode leachates using non-Na precipitant-based chemical precipitation for sustainable recycling, Chem. Eng. J. Adv., 17(2024), art. No. 100582.

[121] Shen YF. Recovery Cobalt from discard lithium ion cells. Nonferrous Metals. 2002, 54(4): 69

[122] Prabaharan G, Barik SP, Kumar N, Kumar L. Electrochemical process for electrode material of spent lithium ion batteries. Waste Manage.. 2017, 68: 527

[123] Wang MM, Tan QY, Liu LL, Li JH. A facile, environmentally friendly, and low-temperature approach for decomposition of polyvinylidene fluoride from the cathode electrode of spent lithium-ion batteries. ACS Sustainable Chem. Eng.. 2019, 7(15): 12799

[124] D.M. Song, J.D. Yu, M.M. Wang, Q.Y. Tan, K. Liu, and J.H. Li, Advancing recycling of spent lithium-ion batteries: From green chemistry to circular economy, Energy Storage Mater., 61(2023), art. No. 102870.

[125] Liu YL, Mu DY, Li RH, Ma QX, Zheng RJ, Dai CS. Purification and characterization of reclaimed electrolytes from spent lithium-ion batteries. J. Phys. Chem. C. 2017, 121(8): 4181

[126] D.Y. Mu, J.Q. Liang, J. Zhang, Y. Wang, S. Jin, and C.S. Dai, Exfoliation of active materials synchronized with electrolyte extraction from spent lithium-ion batteries by supercritical CO₂, ChemistrySelect, 7(2022), No. 20, art. No. e202200841.

[127] He K, Zhang ZY, Alai LG, Zhang FS. A green process for exfoliating electrode materials and simultaneously extracting electrolyte from spent lithium-ion batteries. J. Hazard. Mater.. 2019, 375: 43

[128] G.C. Shi, J. Wang, S.H. Zhang, et al., Green regeneration and high-value utilization technology of the electrolyte from spent lithium-ion batteries, Sep. Purif. Technol., 335(2024), art. No. 126144.

[129] Natarajan S, Subramanyan K, Dhanalakshmi RB, Stephan AM, Aravindan V. Regeneration of polyolefin separators from spent Li-ion battery for second life. Batteries Supercaps. 2020, 3(7): 581

[130] Zhao M, Wang J, Chong CB, Yu XW, Wang LL, Shi ZQ. An electrospun lignin/polyacrylonitrile nonwoven composite separator with high porosity and thermal stability for lithium-ion batteries. RSC Adv.. 2015, 5(122): 101115

[131] Wang X, Gaustad G, Babbitt CW, Richa K. Economies of scale for future lithium-ion battery recycling infrastructure. Resour. Conserv. Recycl.. 2014, 83: 53

[132] Lin J, Wu JW, Fan ES, et al. . Environmental and economic assessment of structural repair technologies for spent lithiumion battery cathode materials. Int. J. Miner. Metall. Mater.. 2022, 29(5): 942

[133] Q. Yuan, J. Zeng, Q.X. Sui, et al., Thermodynamic and experimental analysis of lithium selectively recovery from spent lithium-ion batteries by in situ carbothermal reduction, J. Environ. Chem. Eng., 11(2023), No. 5, art. No. 111029.

[134] Yang Y, Okonkwo EG, Huang GY, Xu SM, Sun W, He YH. On the sustainability of lithium ion battery industry–A review and perspective. Energy Storage Mater.. 2021, 36: 186

[135] L. Lander, T. Cleaver, M. Ali Rajaeifar, et al., Financial viability of electric vehicle lithium-ion battery recycling, iScience, 24(2021), No. 7, art. No. 102787.

[136] M.H. Yu, B. Bai, S.Q. Xiong, and X.W. Liao, Evaluating environmental impacts and economic performance of remanufacturing electric vehicle lithium-ion batteries, J. Clean. Prod., 321(2021), art. No. 128935.