Towards High Value-Added Recycling of Spent Lithium-Ion Batteries for Catalysis Application

Abstract

With the proposal of the global carbon neutrality target, lithium-ion batteries (LIBs) are bound to set off the next wave of applications in portable electronic devices, electric vehicles, and energy-storage grids due to their unique merits. However, the growing LIB market poses a severe challenge for waste management during LIB recycling after end-of-life, which could cause serious environmental pollution and resource waste without proper treatment. Pyrometallurgical, hydrometallurgical, and direct recycling of spent LIBs have been developed, guided by the “waste to wealth” principle, and were applied to LIB remanufacturing. However, some spent LIB materials with low values or great direct regeneration difficulties may not be suitable for the above options, necessitating expanded application ranges of spent LIBs. Considering their unique compositions, using waste electrode materials directly or as precursors to prepare advanced catalysts has been proposed as another promising disposal technology for end-of-life LIBs. For example, transition metal elements in the cathode, like Ni, Co, Mn, and Fe, have been identified as catalytic active centers, and graphite anodes can serve as the catalyst loading matrix. This scheme has been adopted in various catalysis applications, and preliminary progress has been made. Therefore, this review summarizes and discusses the application of spent LIB recycling materials in catalysis and classified it into three aspects: environmental remediation, substance conversion, and battery-related catalysis. Moreover, the existing challenges and possible foci of future research on spent LIB recycling are also discussed. This review is anticipated to mark the start of close attention to the high-value-added applications of spent LIB products, enhancing economic efficiency and sustainable development.

Graphical Abstract

Continuing global growth in consumer electronics, electric vehicles and new energy power generation has caused tremendous demand for lithium ion batteries (LIBs), and the recycling of end-of-life LIBs has become a priority for sustainable development. In addition to the remanufacturing of LIBs, spent LIB products with high value-added components have received more attention in catalysis. Catalysts prepared from spent LIB electrode materials exhibit superior performance in the field of environmental remediation, substance conversion, and batteries-related catalysis, which are summarized and discussed in this review.

Keywords

Spent lithium-ion batteries / Recycling / Catalyst / Environmental remediation / Substance conversion / Battery-related catalysis

References

[1] Goodenough JB, Park KS. The Li-ion rechargeable battery: a perspective. J. Am. Chem. Soc., 2013, 135: 1167-1176

[2] Choi SH, Kwon TW, Coskun A, et al.. Highly elastic binders integrating polyrotaxanes for silicon microparticle anodes in lithium ion batteries. Science, 2017, 357: 279-283

[3] Ding YL, Cano ZP, Yu AP, et al.. Automotive Li-ion batteries: current status and future perspectives. Electrochem. Energ. Rev., 2019, 2: 1-28

[4] Roy JJ, Rarotra S, Krikstolaityte V, et al.. Green recycling methods to treat lithium-ion batteries e-waste: a circular approach to sustainability. Adv. Mater., 2022, 34: 2103346

[5] Wu ZS, Ren WR, Wen LW, et al.. Graphene anchored with Co₃O₄ nanoparticles as anode of lithium ion batteries with enhanced reversible capacity and cyclic performance. ACS Nano, 2010, 4: 3187-3194

[6] Ye YS, Chou LY, Liu Y, et al.. Ultralight and fire-extinguishing current collectors for high-energy and high-safety lithium-ion batteries. Nat. Energy, 2020, 5: 786-793

[7] Shen YF. Recycling cathode materials of spent lithium-ion batteries for advanced catalysts production. J. Power Sources, 2022, 528: 231220

[8] Pender JP, Jha G, Youn DH, et al.. Electrode degradation in lithium-ion batteries. ACS Nano, 2020, 14: 1243-1295

[9] Xiong R, Pan Y, Shen WX, et al.. Lithium-ion battery aging mechanisms and diagnosis method for automotive applications: recent advances and perspectives. Renew. Sust. Energ. Rev., 2020, 131: 110048

[10] Keil P, Schuster SF, Wilhelm J, et al.. Calendar aging of lithium-ion batteries. J. Electrochem. Soc., 2016, 163: A1872-A1880

[11] Yu WH, Guo Y, Xu SL, et al.. Comprehensive recycling of lithium-ion batteries: fundamentals, pretreatment, and perspectives. Energy Storage Mater., 2023, 54: 172-220

[12] Harper G, Sommerville R, Kendrick E, et al.. Recycling lithium-ion batteries from electric vehicles. Nature, 2019, 575: 75-86

[13] Ciez RE, Whitacre JF. Examining different recycling processes for lithium-ion batteries. Nat. Sustain., 2019, 2: 148-156

[14] Dunn JB, Gaines L, Kelly JC, et al.. The significance of Li-ion batteries in electric vehicle life-cycle energy and emissions and recycling's role in its reduction. Energy Environ. Sci., 2015, 8: 158-168

[15] Wang P, Guo YG, Guan J, et al.. Applications of spent lithium battery electrode materials in catalytic decontamination: a review. Catalysts, 2023, 13: 189

[16] Zheng MT, Salim H, Liu TF, et al.. Intelligence-assisted predesign for the sustainable recycling of lithium-ion batteries and beyond. Energy Environ. Sci., 2021, 14: 5801-5815

[17] Yang Y, Okonkwo EG, Huang GY, et al.. On the sustainability of lithium ion battery industry: a review and perspective. Energy Storage Mater., 2021, 36: 186-212

[18] Bejigo KS, Natarajan S, Bhunia K, et al.. Recycling of value-added products from spent lithium-ion batteries for oxygen reduction and methanol oxidation reactions. J. Clean. Prod., 2023, 384: 135520

[19] Ji HC, Wang JX, Ma J, et al.. Fundamentals, status and challenges of direct recycling technologies for lithium ion batteries. Chem. Soc. Rev., 2023, 52: 8194-8244

[20] Wang XT, Gu ZY, Ang EHX, et al.. Prospects for managing end-of-life lithium-ion batteries: present and future. Interdiscip. Mater., 2022, 1: 417-433

[21] Niu B, Xiao JF, Xu ZM. Recycling spent LiCoO₂ battery as a high-efficient lithium-doped graphitic carbon nitride/Co₃O₄ composite photocatalyst and its synergistic photocatalytic mechanism. Energy Environ. Mater., 2023, 6: e12312

[22] Or T, Gourley SWD, Kaliyappan K, et al.. Recycling of mixed cathode lithium-ion batteries for electric vehicles: current status and future outlook. Carbon Energy, 2020, 2: 6-43

[23] Zhang XX, Li L, Fan E, et al.. Toward sustainable and systematic recycling of spent rechargeable batteries. Chem. Soc. Rev., 2018, 47: 7239-7302

[24] Fan ES, Li L, Wang ZP, et al.. Sustainable recycling technology for Li-ion batteries and beyond: challenges and future prospects. Chem. Rev., 2020, 120: 7020-7063

[25] Chen MY, Ma XT, Chen B, et al.. Recycling end-of-life electric vehicle lithium-ion batteries. Joule, 2019, 3: 2622-2646

[26] Wang JX, Liang Z, Zhao Y, et al.. Direct conversion of degraded LiCoO₂ cathode materials into high-performance LiCoO₂: a closed-loop green recycling strategy for spent lithium-ion batteries. Energy Storage Mater., 2022, 45: 768-776

[27] Wang JX, Ma J, Jia K, et al.. Efficient extraction of lithium from anode for direct regeneration of cathode materials of spent Li-ion batteries. ACS Energy Lett., 2022, 7: 2816-2824

[28] Zhao Y, Kang YQ, Fan MC, et al.. Precise separation of spent lithium-ion cells in water without discharging for recycling. Energy Storage Mater., 2022, 45: 1092-1099

[29] Lin J, Fan ES, Zhang XD, et al.. Sustainable upcycling of spent lithium-ion batteries cathode materials: stabilization by in situ Li/Mn disorder. Adv. Energy Mater., 2022, 12: 2201174

[30] Fan M, Meng QH, Chang X, et al.. In situ electrochemical regeneration of degraded LiFePO₄ electrode with functionalized prelithiation separator. Adv. Energy Mater., 2022, 12: 2103630

[31] Jin YC, Zhang T, Zhang MD. Advances in intelligent regeneration of cathode materials for sustainable lithium-ion batteries. Adv. Energy Mater., 2022, 12: 2201526

[32] Mao JF, Ye C, Zhang SL, et al.. Toward practical lithium-ion battery recycling: adding value, tackling circularity and recycling-oriented design. Energy Environ. Sci., 2022, 15: 2732-2752

[33] Wu JW, Zheng MT, Liu TF, et al.. Direct recovery: a sustainable recycling technology for spent lithium-ion battery. Energy Storage Mater., 2023, 54: 120-134

[34] Murdock BE, Toghill KE, Tapia-Ruiz N. A perspective on the sustainability of cathode materials used in lithium-ion batteries. Adv. Energy Mater., 2021, 11: 2102028

[35] 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: 20306-20314

[36] Jia K, Ma J, Wang JX, et al.. Long-life regenerated LiFePO₄ from spent cathode by elevating the d-band center of Fe. Adv. Mater., 2023, 35: 2208034

[37] Tran MK, Rodrigues MTF, Kato K, et al.. Deep eutectic solvents for cathode recycling of Li-ion batteries. Nat. Energy, 2019, 4: 339-345

[38] Xu PP, Dai Q, Gao HP, et al.. Efficient direct recycling of lithium-ion battery cathodes by targeted healing. Joule, 2020, 4: 2609-2626

[39] Cao ZQ, Zheng XH, Cao HB, et al.. Efficient reuse of anode scrap from lithium-ion batteries as cathode for pollutant degradation in electro-fenton process: role of different recovery processes. Chem. Eng. J., 2018, 337: 256-264

[40] Santana IL, Moreira TFM, Lelis MFF, et al.. Photocatalytic properties of Co₃O₄/LiCoO₂ recycled from spent lithium-ion batteries using citric acid as leaching agent. Mater. Chem. Phys., 2017, 190: 38-44

[41] Garole DJ, Hossain R, Garole VJ, et al.. Recycle, recover and repurpose strategy of spent Li-ion batteries and catalysts: current status and future opportunities. Chemsuschem, 2020, 13: 3079-3100

[42] Zheng XR, Zhao X, Lu JD, et al.. Regeneration of spent cathodes of Li-ion batteries into multifunctional electrodes for overall water splitting and rechargeable Zn-air batteries by ultrafast carbothermal shock. Sci. China Mater., 2022, 65: 2393-2400

[43] Bian HD, Wu WB, Zhu YY, et al.. Waste to treasure: regeneration of porous Co-based catalysts from spent LiCoO₂ cathode materials for an efficient oxygen evolution reaction. ACS Sustain. Chem. Eng., 2023, 11: 670-678

[44] Dąbrowska A, Urbańska W, Warczak M, et al.. Battery powder as a source of novel graphene nanocarbons. Phys. Status Solidi B, 2022, 259: 2100588

[45] Jena KK, Mayyas AT, Mohanty B, et al.. Recycling of electrode materials from spent lithium-ion batteries to develop graphene nanosheets and graphene-molybdenum disulfide nanohybrid: environmental benefits, analysis of supercapacitor performance, and influence of density functional theory calculations. Energy Fuels, 2022, 36: 2159-2170

[46] Wu XX, Ji GJ, Wang JX, et al.. Toward sustainable all solid-state Li-metal batteries: perspectives on battery technology and recycling processes. Adv. Mater., 2023, 35: 2301540

[47] Fan M, Chang X, Meng QH, et al.. Progress in the sustainable recycling of spent lithium-ion batteries. SusMat, 2021, 1: 241-254

[48] Wu XX, Ma J, Wang JX, et al.. Progress, key issues, and future prospects for Li-ion battery recycling. Glob Chall, 2022, 6: 2200067

[49] Fang Z, Duan QL, Peng QK, et al.. Comparative study of chemical discharge strategy to pretreat spent lithium-ion batteries for safe, efficient, and environmentally friendly recycling. J. Cleaner Prod., 2022, 359: 132116

[50] Wu LX, Zhang FS, He K, et al.. Avoiding thermal runaway during spent lithium-ion battery recycling: a comprehensive assessment and a new approach for battery discharge. J. Cleaner Prod., 2022, 380: 135045

[51] Waldmann T, Iturrondobeitia A, Kasper M, et al.. Review—post-mortem analysis of aged lithium-ion batteries: disassembly methodology and physico-chemical analysis techniques. J. Electrochem. Soc., 2016, 163: A2149-A2164

[52] Dorella G, Mansur MB. A study of the separation of cobalt from spent Li-ion battery residues. J. Power Sources, 2007, 170: 210-215

[53] Chen L, Tang XC, Zhang Y, et al.. Process for the recovery of cobalt oxalate from spent lithium-ion batteries. Hydrometallurgy, 2011, 108: 80-86

[54] Grützke M, Kraft V, Hoffmann B, et al.. Aging investigations of a lithium-ion battery electrolyte from a field-tested hybrid electric vehicle. J. Power Sources, 2015, 273: 83-88

[55] Lv WG, Wang ZH, Cao HB, et al.. A critical review and analysis on the recycling of spent lithium-ion batteries. ACS Sustain. Chem. Eng., 2018, 6: 1504-1521

[56] Makuza B, Tian QH, Guo XY, et al.. Pyrometallurgical options for recycling spent lithium-ion batteries: a comprehensive review. J. Power Sources, 2021, 491: 229622

[57] Piątek J, Afyon S, Budnyak TM, et al.. Sustainable Li-ion batteries: chemistry and recycling. Adv. Energy Mater., 2020, 11: 2003456

[58] Du KD, Ang EHX, Wu XL, et al.. Progresses in sustainable recycling technology of spent lithium-ion batteries. Energy Environ. Mater., 2022, 5: 1012-1036

[59] Qu GR, Wei YG, Liu CP, et al.. Efficient separation and recovery of lithium through volatilization in the recycling process of spent lithium-ion batteries. Waste Manag., 2022, 150: 66-74

[60] Zhang A, Liang YX, Zhang H, et al.. Doping regulation in transition metal compounds for electrocatalysis. Chem. Soc. Rev., 2021, 50: 9817-9844

[61] Xin Y, Li SH, Qian YY, et al.. High-entropy alloys as a platform for catalysis: progress, challenges, and opportunities. ACS Catal., 2020, 10: 11280-11306

[62] Boutin E, Merakeb L, Ma B, et al.. Molecular catalysis of CO₂ reduction: recent advances and perspectives in electrochemical and light-driven processes with selected Fe, Ni and Co aza macrocyclic and polypyridine complexes. Chem. Soc. Rev., 2020, 49: 5772-5809

[63] Yang Y, Yang Y, Pei Z, et al.. Recent progress of carbon-supported single-atom catalysts for energy conversion and storage. Matter, 2020, 3: 1442-1476

[64] Zeng H, Deng L, Zhang H, et al.. Development of oxygen vacancies enriched CoAl hydroxide@hydroxysulfide hollow flowers for peroxymonosulfate activation: a highly efficient singlet oxygen-dominated oxidation process for sulfamethoxazole degradation. J. Hazard. Mater., 2020, 400: 123297

[65] Windsor FM, Durance I, Horton AA, et al.. A catchment-scale perspective of plastic pollution. Glob. Change Biol., 2019, 25: 1207-1221

[66] Miao YP, Liu LL, Zhang YP, et al.. An overview of global power lithium-ion batteries and associated critical metal recycling. J. Hazard. Mater., 2022, 425: 127900

[67] Hodges BC, Cates EL, Kim JH. Challenges and prospects of advanced oxidation water treatment processes using catalytic nanomaterials. Nat. Nanotechnol., 2018, 13: 642-650

[68] Moreira FC, Boaventura RAR, Brillas E, et al.. Electrochemical advanced oxidation processes: a review on their application to synthetic and real wastewaters. Appl. Catal. B-Environ., 2017, 202: 217-261

[69] Martinez-Huitle CA, Rodrigo MA, Sires I, et al.. Single and coupled electrochemical processes and reactors for the abatement of organic water pollutants: a critical review. Chem. Rev., 2015, 115: 13362-13407

[70] Dong GH, Chen B, Liu B, et al.. Advanced oxidation processes in microreactors for water and wastewater treatment: development, challenges, and opportunities. Water Res., 2022, 211: 118047

[71] Wang SZ, Wang JL. Electron beam technology coupled to fenton oxidation for advanced treatment of dyeing wastewater: from laboratory to full application. ACS EST Water, 2022, 2: 852-862

[72] Fenton HJH. Oxidation of tartaric acid in presence of iron. J. Chem. Soc., 1894, 65: 899-910

[73] He J, Yang XF, Men B, et al.. Interfacial mechanisms of heterogeneous Fenton reactions catalyzed by iron-based materials: a review. J. Environ. Sci., 2016, 39: 97-109

[74] Yang ZC, Qian JS, Yu AQ, et al.. Singlet oxygen mediated iron-based Fenton-like catalysis under nanoconfinement. Proc. Natl. Acad. Sci., 2019, 116: 6659-6664

[75] Goncalves MC, Garcia EM, Taroco HA, et al.. Chemical recycling of cell phone Li-ion batteries: application in environmental remediation. Waste Manage., 2015, 40: 144-150

[76] Guo J, Zhang J, Chen C, et al.. Rapid photodegradation of methyl orange by oxalic acid assisted with cathode material of lithium ion batteries LiFePO₄. J. Taiwan Inst. Chem. Eng., 2016, 62: 187-191

[77] Xu L, Chen C, Huo JB, et al.. Iron hydroxyphosphate composites derived from waste lithium-ion batteries for lead adsorption and fenton-like catalytic degradation of methylene blue. Environ. Technol. Innov., 2019, 16: 100504

[78] Yang L, Xi G, Lou TJ, et al.. Preparation and magnetic performance of Co_0.8Fe_2.2O₄ by a sol–gel method using cathode materials of spent Li-ion batteries. Ceram. Int., 2016, 42: 1897-1902

[79] Yao L, Xi YB, Xi G, et al.. Synthesis of cobalt ferrite with enhanced magnetostriction properties by the sol−gel−hydrothermal route using spent Li-ion battery. J. Alloys Compd., 2016, 680: 73-79

[80] Al-Kahtani AA, Abou Taleb MF. Photocatalytic degradation of Maxilon C.I. basic dye using CS/CoFe₂O₄/GONCs as a heterogeneous photo-Fenton catalyst prepared by gamma irradiation. J. Hazard. Mater., 2016, 309: 10-19

[81] Moura MN, Barrada RV, Almeida JR, et al.. Synthesis, characterization and photocatalytic properties of nanostructured CoFe₂O₄ recycled from spent Li-ion batteries. Chemosphere, 2017, 182: 339-347

[82] Rocha AKS, Magnago LB, Santos JJ, et al.. Copper ferrite synthesis from spent Li-ion batteries for multifunctional application as catalyst in photo Fenton process and as electrochemical pseudocapacitor. Mater. Res. Bull., 2019, 113: 231-240

[83] Chen X, Deng F, Liu X, et al.. Hydrothermal synthesis of MnO₂/Fe(0) composites from Li-ion battery cathodes for destructing sulfadiazine by photo-Fenton process. Sci. Total. Environ., 2021, 774: 145776

[84] Yi CX, Zhou LJ, Wu XQ, et al.. Technology for recycling and regenerating graphite from spent lithium-ion batteries. Chin. J. Chem. Eng., 2021, 39: 37-50

[85] Niu B, Xiao JF, Xu ZM. Advances and challenges in anode graphite recycling from spent lithium-ion batteries. J. Hazard. Mater., 2022, 439: 129678

[86] Guan J, Li ZX, Chen S, et al.. Zero-valent iron supported on expanded graphite from spent lithium-ion battery anodes and ferric chloride for the degradation of 4-chlorophenol in water. Chemosphere, 2022, 290: 133381

[87] Jin Q, Chen Q, Shen JM, et al.. Development of Fe(II) system based on N, Nʹ-dipicolinamide for the oxidative removal of 4-chlorophenol. J. Hazard. Mater., 2018, 354: 206-214

[88] Yang J, He XQ, Dai J, et al.. Electron-transfer-dominated non-radical activation of peroxydisulfate for efficient removal of chlorophenol contaminants by one-pot synthesized nitrogen and sulfur codoped mesoporous carbon. Environ. Res., 2021, 194: 110496

[89] Cai C, Zhang H, Zhong X, et al.. Ultrasound enhanced heterogeneous activation of peroxymonosulfate by a bimetallic Fe-Co/SBA-15 catalyst for the degradation of orange II in water. J. Hazard. Mater., 2015, 283: 70-79

[90] Pi YQ, Gao HQ, Cao YD, et al.. Cobalt ferrite supported on carbon nitride matrix prepared using waste battery materials as a peroxymonosulfate activator for the degradation of levofloxacin hydrochloride. Chem. Eng. J., 2020, 379: 122377

[91] Zhao YL, Yuan XZ, Jiang LB, et al.. Reutilization of cathode material from spent batteries as a heterogeneous catalyst to remove antibiotics in wastewater via peroxymonosulfate activation. Chem. Eng. J., 2020, 400: 125903

[92] Zhao YL, Wang H, Li XD, et al.. Recovery of CuO/C catalyst from spent anode material in battery to activate peroxymonosulfate for refractory organic contaminants degradation. J. Hazard. Mater., 2021, 420: 126552

[93] Dang S, Zhou PS, Shi PH, et al.. In situ aluminothermic reduction induced by mechanochemical activation enhances the ability of the spent LiCoO₂ cathode to activate peroxymonosulfate. ACS Sustain. Chem. Eng., 2021, 9: 15375-15385

[94] Wang X, Zhang XF, Dai L, et al.. Recycling the cathode scrap of spent lithium-ion batteries as an easily recoverable peroxymonosulfate catalyst with enhanced catalytic performance. ACS Sustain. Chem. Eng., 2020, 8: 11337-11347

[95] Zhang XY, Wang X, Chai J, et al.. Construction of novel symmetric double Z-scheme BiFeO₃/CuBi₂O₄/BaTiO₃ photocatalyst with enhanced solar-light-driven photocatalytic performance for degradation of norfloxacin. Appl. Catal. B-Environ., 2020, 272: 119017

[96] Lee CG, Javed H, Zhang D, et al.. Porous electrospun fibers embedding TiO₂ for adsorption and photocatalytic degradation of water pollutants. Environ. Sci. Technol., 2018, 52: 4285-4293

[97] An JH, Song XT, Wan WB, et al.. Kinetics of the photoelectron-transfer process characterized by real-time single-molecule fluorescence imaging on individual photocatalyst particles. ACS Catal., 2021, 11: 6872-6882

[98] Nascimento MA, Cruz JC, Rodrigues GD, et al.. Synthesis of polymetallic nanoparticles from spent lithium-ion batteries and application in the removal of reactive blue 4 dye. J. Clean. Prod., 2018, 202: 264-272

[99] Niu B, Xiao JF, Xu ZM. Utilizing spent Li-ion batteries to regulate the π-conjugated structure of g-C₃N₄: a win–win approach for waste recycling and highly active photocatalyst construction. J. Mater. Chem. A, 2021, 9: 472-481

[100] Zhang WX, Liu ZP, Xu CJ, et al.. Preparing graphene oxide-copper composite material from spent lithium ion batteries and catalytic performance analysis. Res. Chem. Intermed., 2018, 44: 5075-5089

[101] Xu ZM, Wang J, Sun SH, et al.. Simple route for graphite recycling from waste lithium-ion batteries to environmental functional materials. ACS Sustain. Chem. Eng., 2022, 10: 13435-13443

[102] Xie LH, Liu XM, He T, et al.. Metal-organic frameworks for the capture of trace aromatic volatile organic compounds. Chem, 2018, 4: 1911-1927

[103] Hakim M, Broza YY, Barash O, et al.. Volatile organic compounds of lung cancer and possible biochemical pathways. Chem. Rev., 2012, 112: 5949-5966

[104] Mellouki A, Wallington TJ, Chen J. Atmospheric chemistry of oxygenated volatile organic compounds: impacts on air quality and climate. Chem. Rev., 2015, 115: 3984-4014

[105] Kamal MS, Razzak SA, Hossain MM. Catalytic oxidation of volatile organic compounds (VOCs): a review. Atmos. Environ., 2016, 140: 117-134

[106] Huang HB, Xu Y, Feng QY, et al.. Low temperature catalytic oxidation of volatile organic compounds: a review. Catal. Sci. Technol., 2015, 5: 2649-2669

[107] Liotta LF. Catalytic oxidation of volatile organic compounds on supported noble metals. Appl. Catal. B-Environ., 2010, 100: 403-412

[108] Liao YT, Jia L, Chen RJ, et al.. Charcoal-supported catalyst with enhanced thermal-stability for the catalytic combustion of volatile organic compounds. Appl. Catal. A-Gen, 2016, 522: 32-39

[109] Min X, Guo MM, Liu LZ, et al.. Synthesis of MnO₂ derived from spent lithium-ion batteries via advanced oxidation and its application in VOCs oxidation. J. Hazard. Mater., 2021, 406: 124743

[110] Guo MM, Li K, Liu LZ, et al.. Manganese-based multi-oxide derived from spent ternary lithium-ions batteries as high-efficient catalyst for VOCs oxidation. J. Hazard. Mater., 2019, 380: 120905

[111] Guo MM, Li K, Zhang HB, et al.. Promotional removal of oxygenated VOC over manganese-based multi oxides from spent lithium-ions manganate batteries: Modification with Fe, Bi and Ce dopants. Sci. Total. Environ., 2020, 740: 139951

[112] Guo MM, Li K, Liu LZ, et al.. Resource utilization of spent ternary lithium-ions batteries: synthesis of highly active manganese-based perovskite catalyst for toluene oxidation. J. Taiwan Inst. Chem. Eng., 2019, 102: 268-275

[113] Guo MM, Li K, Liu LZ, et al.. Insight into a sustainable application of spent lithium-ion cobaltate batteries: preparation of a cobalt-based oxide catalyst and its catalytic performance in toluene oxidation. Ind. Eng. Chem. Res., 2019, 59: 194-204

[114] Dai TC, Zhou H, Liu Y, et al.. Synergy of lithium, cobalt, and oxygen vacancies in lithium cobalt oxide for airborne benzene oxidation: a concept of reusing electronic wastes for air pollutant removal. ACS Sustain. Chem. Eng., 2019, 7: 5072-5081

[115] Liu Y, Gao W, Zhan JJ, et al.. One-pot synthesis of Ag–H₃PW₁₂O₄₀-LiCoO₂ composites for thermal oxidation of airborne benzene. Chem. Eng. J., 2019, 375: 121956

[116] Liu Y, Gao W, Zhou H, et al.. Highly reactive bulk lattice oxygen exposed by simple water treatment of LiCoO₂ for catalytic oxidation of airborne benzene. Mol. Catal., 2020, 492: 111003

[117] Suen NT, Hung SF, Quan Q, et al.. Electrocatalysis for the oxygen evolution reaction: recent development and future perspectives. Chem. Soc. Rev., 2017, 46: 337-365

[118] Zhu J, Hu LS, Zhao PX, et al.. Recent advances in electrocatalytic hydrogen evolution using nanoparticles. Chem. Rev., 2020, 120: 851-918

[119] Mahmood N, Yao YD, Zhang JW, et al.. Electrocatalysts for hydrogen evolution in alkaline electrolytes: mechanisms, challenges, and prospective solutions. Adv. Sci., 2018, 5: 1700464

[120] Natarajan S, Anantharaj S, Tayade RJ, et al.. Recovered spinel MnCo₂O₄ from spent lithium-ion batteries for enhanced electrocatalytic oxygen evolution in alkaline medium. Dalton Trans., 2017, 46: 14382-14392

[121] Natarajan S, Krishnamoorthy K, Sathyaseelan A, et al.. A new route for the recycling of spent lithium-ion batteries towards advanced energy storage, conversion, and harvesting systems. Nano Energy, 2022, 101: 107595

[122] Wang JH, Cui W, Liu Q, et al.. Recent progress in cobalt-based heterogeneous catalysts for electrochemical water splitting. Adv. Mater., 2016, 28: 215-230

[123] Lee SW, Carlton C, Risch M, et al.. The nature of lithium battery materials under oxygen evolution reaction conditions. J. Am. Chem. Soc., 2012, 134: 16959-16962

[124] Lu Z, Wang HT, Kong DS, et al.. Electrochemical tuning of layered lithium transition metal oxides for improvement of oxygen evolution reaction. Nat. Commun., 2014, 5: 4345

[125] Gardner G, Al-Sharab J, Danilovic N, et al.. Structural basis for differing electrocatalytic water oxidation by the cubic, layered and spinel forms of lithium cobalt oxides. Energy Environ. Sci., 2016, 9: 184-192

[126] Chen N, Qi J, Du X, et al.. Recycled LiCoO₂ in spent lithium-ion battery as an oxygen evolution electrocatalyst. RSC Adv., 2016, 6: 103541-103545

[127] Antolini E. LiCoO₂: formation, structure, lithium and oxygen nonstoichiometry, electrochemical behaviour and transport properties. Solid State Ionics, 2004, 170: 159-171

[128] Pegoretti VCB, Dixini PVM, Magnago L, et al.. High-temperature (HT) LiCoO₂ recycled from spent lithium ion batteries as catalyst for oxygen evolution reaction. Mater. Res. Bull., 2019, 110: 97-101

[129] Huang C, Lv H, Yang ZH, et al.. Exfoliating spent cathode materials with robust interlayer interactions into atomic-thin nanosheets for boosting the oxygen evolution reaction. J. Mater. Chem. A, 2022, 10: 3359-3372

[130] de Bruin-Dickason C, Budnyk S, Piątek J, et al.. Valorisation of used lithium-ion batteries into nanostructured catalysts for green hydrogen from boranes. Mater Adv, 2020, 1: 2279-2285

[131] Arif A, Xu M, Rashid J, et al.. Efficient recovery of lithium cobaltate from spent lithium-ion batteries for oxygen evolution reaction. Nanomaterials, 2021, 11: 3343

[132] Liu TT, Cai S, Zhao GF, et al.. Recycling valuable cobalt from spent lithium ion batteries for controllably designing a novel sea-urchin-like cobalt nitride-graphene hybrid catalyst: towards efficient overall water splitting. J. Energy Chem., 2021, 62: 440-450

[133] Cui BH, Liu C, Zhang JF, et al.. Waste to wealth: defect-rich Ni-incorporated spent LiFePO₄ for efficient oxygen evolution reaction. Sci. China Mater., 2021, 64: 2710-2718

[134] Fan XM, Hu GR, Zhang B, et al.. Crack-free single-crystalline Ni-rich layered NCM cathode enable superior cycling performance of lithium-ion batteries. Nano Energy, 2020, 70: 104450

[135] Chen ZJ, Wei WF, Zou WS, et al.. Integrating electrodeposition with electrolysis for closed-loop resource utilization of battery industrial wastewater. Green Chem., 2022, 24: 3208-3217

[136] Chen ZJ, Zou WS, Zheng RJ, et al.. Synergistic recycling and conversion of spent Li-ion battery leachate into highly efficient oxygen evolution catalysts. Green Chem., 2021, 23: 6538-6547

[137] Yang YX, Yang HL, Cao HB, et al.. Direct preparation of efficient catalyst for oxygen evolution reaction and high-purity Li₂CO₃ from spent LiNi_0.5Mn_0.3Co_0.2O₂ batteries. J. Clean. Prod., 2019, 236: 117576

[138] Lv H, Huang HJ, Huang C, et al.. Electric field driven de-lithiation: a strategy towards comprehensive and efficient recycling of electrode materials from spent lithium ion batteries. Appl. Catal. B-Environ., 2021, 283: 119634

[139] Li L, Li XD, Sun YF, et al.. Rational design of electrocatalytic carbon dioxide reduction for a zero-carbon network. Chem. Soc. Rev., 2022, 51: 1234-1252

[140] Huang XF, Zhang YB. Reticular materials for electrochemical reduction of CO₂. Coord. Chem. Rev., 2021, 427: 213564

[141] Daryanavard M, Hadadzadeh H, Farrokhpour H, et al.. Utilization of CO₂ as a carbon source for production of CO and syngas using a ruthenium(II) electrocatalyst. J. CO2 Util., 2018, 26: 612-622

[142] Hua Y, Zhang BW, Hao WB, et al.. Boosting CO desorption on dual active site electrocatalysts for CO₂ reduction to produce tunable syngas. Cell Rep. Phys. Sci., 2022, 3: 100703

[143] Deng LP, Xu ZJ, Wang MM, et al.. CO₂ treatment enables non-hazardous, reliable, and efficacious recovery of spent Li(Ni_0.5Co_0.2Mn_0.3)O₂ cathodes. Green Chem., 2022, 24: 779-789

[144] Wang LY, Gu YY, Wei JC, et al.. Li-Ni-Co-Mn oxides powders recycled from spent lithium-ion batteries for OER electrodes in CO₂ reduction. Environ. Technol. Innovation, 2020, 18: 100732

[145] Yu JD, Zou SJ, Xu GY, et al.. In-situ enhanced catalytic reforming behavior of cobalt-based materials with inherent zero-valent aluminum in spent lithium ion batteries. Appl. Catal. B-Environ., 2022, 303: 120920

[146] Jung SY, Kwon D, Park S, et al.. Valorization of a spent lithium-ion battery electrolyte through syngas formation using CO₂-assisted catalytic thermolysis over a battery cathode material. J. CO2 Util., 2021, 50: 101591

[147] Zhou YJJ, Kerkhoven EJ, Nielsen J. Barriers and opportunities in bio-based production of hydrocarbons. Nat. Energy, 2018, 3: 925-935

[148] Chen L, Wang P, Shen YF, et al.. Spent lithium-ion battery materials recycling for catalytic pyrolysis or gasification of biomass. Bioresour. Technol., 2021, 323: 124584

[149] Wang P, Chen L, Shen YF. Recycling spent ternary lithium-ion batteries for modification of dolomite used in catalytic biomass pyrolysis: a preliminary study by thermogravimetric and pyrolysis-gas chromatography/mass spectrometry analysis. Bioresour. Technol., 2021, 337: 125476

[150] Fuentes CA, Gallegos MV, García JR, et al.. Catalytic glycolysis of poly(ethylene terephthalate) using zinc and cobalt oxides recycled from spent batteries. Waste Biomass Valori., 2019, 11: 4991-5001

[151] Paone E, Miceli M, Malara A, et al.. Direct reuse of spent lithium-ion batteries as an efficient heterogeneous catalyst for the reductive upgrading of biomass-derived furfural. ACS Sustain. Chem. Eng., 2022, 10: 2275-2281

[152] Han ZY, Gao RH, Jia YY, et al.. Catalytic effect in Li-S batteries: from band theory to practical application. Mater. Today, 2022, 57: 84-120

[153] Xu Y, Deng P, Chen G, et al.. 2D nitrogen-doped carbon nanotubes/graphene hybrid as bifunctional oxygen electrocatalyst for long-life rechargeable Zn-air batteries. Adv. Funct. Mater., 2019, 30: 1906081

[154] Primbs M, Sun YY, Roy A, et al.. Establishing reactivity descriptors for platinum group metal (PGM)-free Fe-N-C catalysts for PEM fuel cells. Energy Environ. Sci., 2020, 13: 2480-2500

[155] Zhu JW, Cao JQ, Cai GL, et al.. Non-trivial contribution of carbon hybridization in carbon-based substrates to electrocatalytic activities in Li-S batteries. Angew. Chem. Int. Ed., 2023, 62: e202214351

[156] Liao KX, Chen ST, Wei HH, et al.. Micropores of pure nanographite spheres for long cycle life and high-rate lithium-sulfur batteries. J. Mater. Chem. A, 2018, 6: 23062-23070

[157] Ng SF, Lau MYL, Ong WJ. Lithium-sulfur battery cathode design: tailoring metal-based nanostructures for robust polysulfide adsorption and catalytic conversion. Adv. Mater., 2021, 33: 2008654

[158] Zhang H, Ono L, Tong GQ, et al.. Long-life lithium-sulfur batteries with high areal capacity based on coaxial CNTs@TiN-TiO₂ sponge. Nat. Commun., 2021, 12: 4738

[159] Liu QF, Pan ZF, Wang E, et al.. Aqueous metal-air batteries: fundamentals and applications. Energy Storage Mater., 2020, 27: 478-505

[160] Jose V, Elouarzaki K, Fisher AC, et al.. Design and integration of molecular-type catalysts in fuel-cell technology. Small Methods, 2018, 2: 1800059

[161] Natarajan S, Aravindan V. Recycling strategies for spent Li-ion battery mixed cathodes. ACS Energy Lett., 2018, 3: 2101-2103

[162] Liu JJ, Shi H, Hu XY, et al.. Critical strategies for recycling process of graphite from spent lithium-ion batteries: a review. Sci. Total. Environ., 2022, 816: 151621

[163] Chen Y, Wang TY, Tian HJ, et al.. Advances in lithium-sulfur batteries: from academic research to commercial viability. Adv. Mater., 2021, 33: 2003666

[164] Feng S, Fu ZH, Chen X, et al.. A review on theoretical models for lithium–sulfur battery cathodes. InfoMat, 2022, 4: 12304

[165] Su YS, Manthiram A. A new approach to improve cycle performance of rechargeable lithium-sulfur batteries by inserting a free-standing MWCNT interlayer. Chem. Commun., 2012, 48: 8817-8819

[166] Xu Q, Wang Y, Shi XY, et al.. The direct application of spent graphite as a functional interlayer with enhanced polysulfide trapping and catalytic performance for Li-S batteries. Green Chem., 2021, 23: 942-950

[167] Liu RD, Yin WZ, Chen YX, et al.. Facile utilization of spent LiCoO₂ in separator decoration of lithium-sulfur batteries. Ind. Eng. Chem. Res., 2020, 59: 17911-17917

[168] Yang XY, Li R, Yang JX, et al.. A novel route to constructing high-efficiency lithium sulfur batteries with spent graphite as the sulfur host. Carbon, 2022, 199: 215-223

[169] Liu YY, Ge Z, Sun ZH, et al.. A high-performance energy storage system from sphagnum uptake waste LIBs with negative greenhouse-gas emission. Nano Energy, 2020, 67: 104216

[170] Liu ML, Zhao ZP, Duan XF, et al.. Nanoscale structure design for high-performance Pt-based ORR catalysts. Adv. Mater., 2019, 31: 1802234

[171] Hu YM, Zhu MZ, Luo X, et al.. Coplanar Pt/C nanomeshes with ultrastable oxygen reduction performance in fuel cells. Angew. Chem. Int. Ed., 2021, 60: 6533-6538

[172] Wang HT, Xu SC, Tsai C, et al.. Direct and continuous strain control of catalysts with tunable battery electrode materials. Science, 2016, 354: 1031-1036

[173] Liivand K, Kazemi M, Walke P, et al.. Spent Li-ion battery graphite turned into valuable and active catalyst for electrochemical oxygen reduction. Chemsuschem, 2021, 14: 1103-1111

[174] Warczak M, Osial M, Urbanska W, et al.. Hydrogen peroxide generation catalyzed by battery waste material. Electrochem. Commun., 2022, 136: 107239

[175] Yamada Y, Yoshida S, Honda T, et al.. Protonated iron-phthalocyanine complex used for cathode material of a hydrogen peroxide fuel cell operated under acidic conditions. Energy Environ. Sci., 2011, 4: 2822-2825

[176] Miglbauer E, Wójcik PJ, Głowacki ED. Single-compartment hydrogen peroxide fuel cells with poly(3,4-ethylenedioxythiophene) cathodes. Chem. Commun., 2018, 54: 11873-11876

[177] Ruan DS, Zhang ZH, Wu XF, et al.. Synthesizing high-quality graphene from spent anode graphite and further functionalization applying in ORR electrocatalyst. ChemistrySelect, 2021, 6: 90-95

[178] Ruan DS, Zou K, Du K, et al.. Recycling of graphite anode from spent lithium-ion batteries for preparing Fe-N-doped carbon orr catalyst. ChemCatChem, 2021, 13: 2025-2033

[179] Nie Y, Li L, Wei ZD. Recent advancements in Pt and Pt-free catalysts for oxygen reduction reaction. Chem. Soc. Rev., 2015, 44: 2168-2201

[180] Huang YY, Wang YQ, Tang C, et al.. Atomic modulation and structure design of carbons for bifunctional electrocatalysis in metal-air batteries. Adv. Mater., 2019, 31: 1803800

[181] Chen Z, Yu A, Higgins D, et al.. Highly active and durable core-corona structured bifunctional catalyst for rechargeable metal-air battery application. Nano Lett., 2012, 12: 1946-1952

[182] Maiyalagan T, Jarvis KA, Therese S, et al.. Spinel-type lithium cobalt oxide as a bifunctional electrocatalyst for the oxygen evolution and oxygen reduction reactions. Nat. Commun., 2014, 5: 3949

[183] Jin HH, Zhou H, Ji PX, et al.. ZIF-8/LiFePO₄ derived Fe-N-P Co-doped carbon nanotube encapsulated Fe₂P nanoparticles for efficient oxygen reduction and Zn-Air batteries. Nano Res., 2020, 13: 818-823

[184] Jiao ML, Zhang Q, Ye CL, et al.. Isolating contiguous Fe atoms by forming a Co-Fe intermetallic catalyst from spent lithium-ion batteries to regulate activity for zinc-air batteries. ACS Nano, 2022, 16: 13223-13231

[185] Jiao ML, Zhang Q, Ye CL, et al.. Recycling spent LiNi_1−x−yMn_xCo_yO₂ cathodes to bifunctional NiMnCo catalysts for zinc-air batteries. Proc. Natl. Acad. Sci., 2022, 119: 2202202119

[186] Wei J, Zhao S, Ji L, et al.. Reuse of Ni-Co-Mn oxides from spent Li-ion batteries to prepare bifunctional air electrodes. Resour. Conserv. Recy., 2018, 129: 135-142

[187] Yang CG, Jin ZW, Zhang X, et al.. Ultrafast regenerating spent LiCoO₂ lithium-ion batteries into bifunctional electrodes for rechargeable Zn-air batteries. ChemElectroChem, 2022, 9: 202101494

[188] Zheng Y, Liu Y, Hou J, et al.. Unraveling the nature of sulfide ions in hydrometallurgical recycling of NCM622 cathode material. Energy Storage Mater., 2024, 65: 103128

Funding

National Natural Science Foundation of China(52072205)

Shenzhen Science and Technology Innovation Program(KQTD20210811090112002)

Guangdong Province Introduction of Innovative R&D Team(2021ZT09L197)

RIGHTS & PERMISSIONS

Shanghai University and Periodicals Agency of Shanghai University