Progress in Hydrometallurgical Separation and Recovery of Valuable Metals from Spent Lithium-ion Batteries

Abstract With the rapid development of the lithium-ion batteries (LiBs) industry, the number of spent LiBs will show an explosive growth trend, and recovery of valuable metals from spent LiBs is of great significance both in economic and environment. In order to obtain various valuable products with high purity from lixivium (Li⁺, Co²⁺, Ni²⁺, Mn²⁺, etc.) during the recycling of waste LiBs through wet chemistry, a systematic summary of the separation technology of various metal ions from lixivium were introduced. The application process and development status of metal ion separation in the lixivium mainly include chemical precipitation, solvent extraction, adsorption method, membrane separation, electrodeposition, etc. In this review, the advantages and disadvantages of various technologies were compared, and the key issues and development trends of the separation of valuable metals from waste LiBs were discussed. The analysis pointed out that the key of the current separation technology is the difficulties in purification owing to similar properties of valuable metals, and the increasing costs by large amount of reagent consumption. The future separation technologies for different valuable metals should focus on the development of low-cost, environmentally friendly separation technologies.

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	Jiang Youzhou
	Wang Yi
	Li Shuzhen
	Yan Shuxuan
	Zhou Tao
	Chen Xiangping

Keywords： spent lithium-ion batteries hydrometallurgy recovery valuable metals selectivity separation

Received 2021-09-15;

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Jiang Youzhou, Wang Yi, Li Shuzhen, Yan Shuxuan, Zhou Tao, Chen Xiangping.Progress in Hydrometallurgical Separation and Recovery of Valuable Metals from Spent Lithium-ion Batteries[J] Chemcial Industry and Engineering, 2021,V38(6): 23-33

[1] Wang Y, An N, Wen L, et al. Recent progress on the recycling technology of Li-ion batteries[J]. Journal of Energy Chemistry, 2021, 55:391-419
[2] 张笑笑, 王鸯鸯, 刘媛, 等. 废旧锂离子电池回收处理技术与资源化再生技术进展[J]. 化工进展, 2016, 35(12):4026-4032 Zhang Xiaoxiao, Wang Yangyang, Liu Yuan, et al. Recent progress in disposal and recycling of spent lithium-ion batteries[J]. Chemical Industry and Engineering Progress, 2016, 35(12):4026-4032(in Chinese)
[3] 李丽, 葛静, 陈人杰, 等. 废旧锂离子电池回收制备钴酸锂的研究进展[J]. 化工进展, 2010, 29(4):757-761 Li Li, Ge Jing, Chen Renjie, et al. Progress in LiCoO₂ preparation from spent Li-ion batteries[J]. Chemical Industry and Engineering Progress, 2010, 29(4):757-761(in Chinese)
[4] 张英杰, 宁培超, 杨轩, 等. 废旧三元锂离子电池回收技术研究新进展[J]. 化工进展, 2020, 39(7):2828-2840 Zhang Yingjie, Ning Peichao, Yang Xuan, et al. Research progress on the recycling technology of spent ternary lithium ion battery[J]. Chemical Industry and Engineering Progress, 2020, 39(7):2828-2840(in Chinese)
[5] Chen X, Cao L, Kang D, et al. Hydrometallurgical processes for valuable metals recycling from spent lithium-ion batteries[M]//Recycling of Spent Lithium-Ion Batteries. Cham:Springer International Publishing, 2019:93-139
[6] 张梦龙, 何几文, 田欢, 等. 废旧锂离子电池中有价金属的回收研究进展[J]. 化学工业与工程, 2019, 36(4):23-30 Zhang Menglong, He Jiwen, Tian Huan, et al. Research progress on recovery of valuable metals from spent lithium ion batteries[J]. Chemical Industry and Engineering, 2019, 36(4):23-30(in Chinese)
[7] Yao Y, Zhu M, Zhao Z, et al. Hydrometallurgical processes for recycling spent lithium-ion batteries:A critical review[J]. ACS Sustainable Chemistry & Engineering, 2018, 6(11):13611-13627
[8] Li L, Bian Y, Zhang X, et al. A green and effective room-temperature recycling process of LiFePO₄ cathode materials for lithium-ion batteries[J]. Waste Management, 2019, 85:437-444
[9] Chen X, Zhou T, Kong J, et al. Separation and recovery of metal values from leach liquor of waste lithium nickel cobalt manganese oxide based cathodes[J]. Separation and Purification Technology, 2015, 141:76-83
[10] Song Y, Zhao Z. Recovery of lithium from spent lithium-ion batteries using precipitation and electrodialysis techniques[J]. Separation and Purification Technology, 2018, 206:335-342
[11] Zheng Y, Song W, Mo W, et al. Lithium fluoride recovery from cathode material of spent lithium-ion battery[J]. RSC Advances, 2018, 8(16):8990-8998
[12] Wang R, Lin Y, Wu S. A novel recovery process of metal values from the cathode active materials of the lithium-ion secondary batteries[J]. Hydrometallurgy, 2009, 99(3/4):194-201
[13] Chen X, Chen Y, Zhou T, et al. Hydrometallurgical recovery of metal values from sulfuric acid leaching liquor of spent lithium-ion batteries[J]. Waste Management, 2015, 38:349-356
[14] Granata G, Moscardini E, Pagnanelli F, et al. Product recovery from Li-ion battery wastes coming from an industrial pre-treatment plant:Lab scale tests and process simulations[J]. Journal of Power Sources, 2012, 206:393-401
[15] Natarajan S, Boricha A B, Bajaj H C. Recovery of value-added products from cathode and anode material of spent lithium-ion batteries[J]. Waste Management, 2018, 77:455-465
[16] Pakarinen J, Paatero E. Recovery of manganese from iron containing sulfate solutions by precipitation[J]. Minerals Engineering, 2011, 24(13):1421-1429
[17] 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[J]. Separation and Purification Technology, 2018, 200:327-334
[18] Meshram P, Pandey B D, Mankhand T R. Hydrometallurgical processing of spent lithium ion batteries (LIBs) in the presence of a reducing agent with emphasis on kinetics of leaching[J]. Chemical Engineering Journal, 2015, 281:418-427
[19] Zhang J, Hu J, Liu Y, et al. Sustainable and facile method for the selective recovery of lithium from cathode scrap of spent LiFePO₄ batteries[J]. ACS Sustainable Chemistry & Engineering, 2019, 7(6):5626-5631
[20] Hu J, Zhang J, Li H, et al. A promising approach for the recovery of high value-added metals from spent lithium-ion batteries[J]. Journal of Power Sources, 2017, 351:192-199
[21] Xiao C, Zeng L. Thermodynamic study on recovery of lithium using phosphate precipitation method[J]. Hydrometallurgy, 2018, 178:283-286
[22] Zhao J, Qu X, Qu J, et al. Extraction of Co and Li₂CO₃ from cathode materials of spent lithium-ion batteries through a combined acid-leaching and electro-deoxidation approach[J]. Journal of Hazardous Materials, 2019, doi:10.1016/j.jhazmat.2019.120817
[23] 孟奇, 张英杰, 董鹏, 等. 废旧锂离子电池中钴、锂的回收研究进展[J]. 化工进展, 2017, 36(9):3485-3491 Meng Qi, Zhang Yingjie, Dong Peng, et al. Recovery of Co and Li from spent lithium ion batteries[J]. Chemical Industry and Engineering Progress, 2017, 36(9):3485-3491(in Chinese)
[24] Chen X, Kang D, Cao L, et al. Separation and recovery of valuable metals from spent lithium ion batteries:Simultaneous recovery of Li and Co in a single step[J]. Separation and Purification Technology, 2019, 210:690-697
[25] Sun L, Qiu K. Organic oxalate as leachant and precipitant for the recovery of valuable metals from spent lithium-ion batteries[J]. Waste Management, 2012, 32(8):1575-1582
[26] Chen X, Ma H, Luo C, et al. Recovery of valuable metals from waste cathode materials of spent lithium-ion batteries using mild phosphoric acid[J]. Journal of Hazardous Materials, 2017, 326:77-86
[27] Cai G, Fung K Y, Ng K M, et al. Process development for the recycle of spent lithium ion batteries by chemical precipitation[J]. Industrial & Engineering Chemistry Research, 2014, 53(47):18245-18259
[28] 黎华玲, 陈永珍, 宋文吉, 等. 湿法回收退役三元锂离子电池有价金属的研究进展[J]. 化工进展, 2019, 38(2):921-932 Li Hualing, Chen Yongzhen, Song Wenji, et al. Research progress on the recovery of valuable metals in retired LiNi_xCo_yMn_zO₂ batteries by wet process[J]. Chemical Industry and Engineering Progress, 2019, 38(2):921-932(in Chinese)
[29] Hong H, Kim D, Choi H, et al. Solvent extraction of co, Ni and Mn from NCM sulfate leaching solution of Li(NCM)O₂ secondary battery scraps[J]. Archives of Metallurgy and Materials, 2017, 62(2):1011-1014
[30] Lv W, Wang Z, Cao H, et al. A critical review and analysis on the recycling of spent lithium-ion batteries[J]. ACS Sustainable Chemistry & Engineering, 2018, 6(2):1504-1521
[31] Liu T, Chen J, Li H, et al. An integrated process for the separation and recovery of valuable metals from the spent LiNi_0.5Co_0.2Mn_0.3O₂ cathode materials[J]. Separation and Purification Technology, 2020, doi:10.1016/j.seppur.2020.116869
[32] Yang Y, Lei S, Song S, et al. Stepwise recycling of valuable metals from Ni-rich cathode material of spent lithium-ion batteries[J]. Waste Management, 2020, 102:131-138
[33] Liu Y, Lee M, Senanayake G. Potential connections between the interaction and extraction performance of mixed extractant systems:A short review[J]. Journal of Molecular Liquids, 2018, 268:667-676
[34] Zhao J, Shen X, Deng F, et al. Synergistic extraction and separation of valuable metals from waste cathodic material of lithium ion batteries using Cyanex272 and PC-88A[J]. Separation and Purification Technology, 2011, 78(3):345-351
[35] Zhang L, Li L, Rui H, et al. Lithium recovery from effluent of spent lithium battery recycling process using solvent extraction[J]. Journal of Hazardous Materials, 2020, doi:10.1016/j.jhazmat.2020.122840
[36] Zante G, Masmoudi A, Barillon R, et al. Separation of lithium, cobalt and nickel from spent lithium-ion batteries using TBP and imidazolium-based ionic liquids[J]. Journal of Industrial and Engineering Chemistry, 2020, 82:269-277
[37] Othman E A, van Der Ham A G J, MiedemA H, et al. Recovery of metals from spent lithium-ion batteries using ionic liquid[P8888] [Oleate[J]. Separation and Purification Technology, 2020, doi:10.1016/j.seppur.2020.117435
[38] Purnomo C W, Kesuma E P, Perdana I, et al. Lithium recovery from spent Li-ion batteries using coconut shell activated carbon[J]. Waste Management, 2018, 79:454-461
[39] Wang H, 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[J]. ACS Sustainable Chemistry & Engineering, 2017, 5(12):11489-11495
[40] Peres E C, Cunha J M, Dortzbacher G F, et al. Treatment of leachates containing cobalt by adsorption on Spirulina sp. and activated charcoal[J]. Journal of Environmental Chemical Engineering, 2018, 6(1):677-685
[41] Da Cunha J M, Klein L, Bassaco M M, et al. Cobalt recovery from leached solutions of lithium-ion batteries using waste materials as adsorbents[J]. The Canadian Journal of Chemical Engineering, 2015, 93(12):2198-2204
[42] Long X, Chen R, Tan J, et al. Electrochemical recovery of cobalt using nanoparticles film of copper hexacyanoferrates from aqueous solution[J]. Journal of Hazardous Materials, 2020, doi:10.1016/j.jhazmat. 2019.121252
[43] Gomaa H, Shenashen M A, Yamaguchi H, et al. Extraction and recovery of Co²⁺ions from spent lithium-ion batteries using hierarchical mesosponge γ-Al₂O₃ monolith extractors[J]. Green Chemistry, 2018, 20(8):1841-1857
[44] Guo F, Nishihama S, Yoshizuka K. Selective recovery of valuable metals from spent Li-ion batteries using solvent-impregnated resins[J]. Environmental Technology, 2013, 34(10):1307-1317
[45] Sonoc A C, Jeswiet J, Murayama N, et al. A study of the application of Donnan dialysis to the recycling of lithium ion batteries[J]. Hydrometallurgy, 2018, 175:133-143
[46] Gao J, Qiu Y, Li M, et al. Separation of valuable metals in spent LiNi_0.46Co_0.2Mn_0.34O₂ battery by shear induced dissociation coupling with ultrafiltration[J]. Hydrometallurgy, 2019, doi:10.1016/j.hydromet.2019. 105127
[47] Iizuka A, Yamashita Y, Nagasawa H, et al. Separation of lithium and cobalt from waste lithium-ion batteries via bipolar membrane electrodialysis coupled with chelation[J]. Separation and Purification Technology, 2013, 113:33-41
[48] Diaz L A, Strauss M L, Adhikari B, et al. Electrochemical-assisted leaching of active materials from lithium ion batteries[J]. Resources, Conservation and Recycling, 2020, doi:10.1016/j.resconrec.2020.104900
[49] Prabaharan G, Barik S P, Kumar N, et al. Electrochemical process for electrode material of spent lithium ion batteries[J]. Waste Management, 2017, 68:527-533
[50] 金玉健, 梅光军, 李树元. 盐析法从锂离子电池正极浸出液中回收钴盐的研究[J]. 环境科学学报, 2006, 26(7):1122-1125 Jin Yujian, Mei Guangjun, Li Shuyuan. Study on cobaltous recovery from cathode leachate of lithium-ion battery by salting out[J]. Acta Scientiae Circumstantiae, 2006, 26(7):1122-1125(in Chinese)
[51] Aktas S, Fray D J, Burheim O, et al. Recovery of metallic values from spent Li ion secondary batteries[J]. Mineral Processing and Extractive Metallurgy, 2006, 115(2):95-100