1 School of Metallurgy and Environment, Central South University, Changsha 410083, China 2 Hunan Key Laboratory of Nonferrous Metal Resources Recycling, Changsha 410083, China 3 Hunan Engineering Research Center of Nonferrous Metal Resources Recycling, Changsha 410083, China 4 National Engineering Laboratory for High-Efficiency Recovery of Refractory Nonferrous Metals, Central South University, Changsha 410083, China 5 Engineering Research Center of the Ministry of Education for Advanced Battery Materials, Central South University, Changsha 410083, China
Abstract: Lithium-ion batteries are widely used in new energy vehicles at home and abroad due to superior performance. With the increasing demand for lithium-ion batteries, a large number of lithium-ion batteries will inevitably be retired in the near future. In order to realize the recycling of valuable metal resources and reduce potential environmental impacts of solid waste disposal, a great deal of attention has been paid to the deve-lopment of an efficient process for recycling spent ternary lithium-ion batteries. Valuable metals or battery materials can be obtained by recycling ternary lithium-ion batteries. In order to improve the recovery rate of materials, a pretreatment method is usually used to separate the current collectors and the cathode materials to achieve effective separation of materials and the further post-processing. Then, metallurgical treatment is used to extract metals and separate impurities from the cathode materials, which includes high temperature metallurgical and hydrometallurgical treatment processes. Finally, battery materials or compounds are further prepared by using the synthesis methods of materials. At the current stage of research, high-temperature metallurgical processes have the problems such as large material loss, high energy consumption, and unfriendly environment; hydrometallurgical processes have the problems such as large acid consumption, low impurity removal efficiency, and long process flows. The regeneration process of cathode materials, the cost of recycling, and the performances of resynthesized materials are the important factors that limit the application. In this paper, we review the recycling technologies of spent ternary lithium-ion batteries, including pretreatment, pyrometallurgy, hydrometallurgy, and cathode material regeneration. We compare the merit and demerit of the above methods, providing references for the development of cathode material recovery technologies in the future and putting forward the prospects and direction of the recycling of spent lithium-ion batteries.
1 Dehghani-Sanij A R, Tharumalingam E, Dusseault M B, et al. Renewable and Sustainable Energy Review,2019,104,192. 2 Ordoñez J, Gago E J, Girard A. Renewable and Sustainable Energy Reviews,2016,60,195. 3 Yang Y, Song S, Lei S, et al. Waste Management,2019,85,529. 4 Gu F, Guo J, Yao X, et al. Journal of Cleaner Production,2017,161,765. 5 https://www.variantmarketresearch.com/report-categories/semiconductor-electronics/lithium-ion-battery-market. 6 MiaoY, Hynan P, von Jouanne A, et al. Energies,2019,12(6),1074. 7 Natarajan S, Aravindan V. Advanced Energy Materials,2018,8(33),1802303. 8 Ojanen S, Lundström M, Santasalo-Aarnio A, et al. Waste Management,2018,76,242. 9 Swain B. Journal of Chemical Technology & Biotechnology,2018,93(2),311. 10 Xue Y, Wang Z, Zheng L, et al. Scientific Reports,2015,5(1),13299. 11 Zenga X, Lia J, Singh N. Environmental Science and Technology,2014,10(44),1129. 12 Zhang W, Xu C, He W, et al. Waste Management & Research,2018,36(2),99. 13 Zheng Z, Chen M, Wang Q, et al. ACS Sustainable Chemistry & Engineering,2018,6(11),13977. 14 Yun L, Sandoval J, Zhang J, et al. Journal of Electrochemical Energy Conversion and Storage,2019,16(2),21011. 15 Guo Y, Li F, Zhu H, et al. Waste Management,2016,51,227. 16 Takacova Z, Havlik T, Kukurugya F, et al. Hydrometallurgy,2016,163,9. 17 Chu S, Cui Y, Liu N. Nature Materials,2017,16,16. 18 Barik S P, Prabaharan G, Kumar B. Waste Management,2016,51,222. 19 Weng Y, Xu S, Huang G, et al. Journal of Hazardous Materials,2013,246-247,163. 20 Chen L, Tang X, Zhang, Y, et al. Hydrometallurgy,2011,108,80. 21 Li L, Bian Y, Zhang X, et al. Waste Management,2018,71,362. 22 He L, Sun S, Song X, et al. Waste Management,2015,46,523. 23 Liu K, Zhang F. Journal of Hazardous Materials,2016,316,19. 24 Li L, Zhai L, Zhang X, et al. Journal of Power Sources,2014,262,380. 25 Hanisch C, Loellhoeffel T, Diekmann J, et al. Journal of Cleaner Production,2015,108,301. 26 Yang Y, Huang G, Xu S, et al. Hydrometallurgy,2016,165,390. 27 Chen Y, Liu N, Hu F, et al. Waste Management,2018,75,469. 28 Ferreira D A, Prados L M Z, Majuste D, et al. Journal of Power Sources,2009,187(1),238. 29 Senć anski J, Bajuk-Bogdanović D, Majstorović D, et al. Journal of Power Sources,2017,342,690. 30 Ahmed S, Nelson P A, Gallagher K G, et al. Journal of Power Sources,2016,322,169. 31 Yang L, Xi G, Xi Y. Ceramics International,2015,41(9),11498. 32 Sun L. A novel reclamation process for spent lithium-ion batteries. Master's Thesis, Central South University, China,2012(in Chinese). 孙亮.废旧锂离子电池回收利用新工艺的研究.硕士学位论文,中南大学,2012. 33 Ren G, Xiao S, Xie M, et al. Transactions of Nonferrous Metals Society of China,2017,27(2),450. 34 Georgi-Maschler T, Friedrich B, Weyhe R, et al. Journal of Power Sources,2012,207,173-182. 35 Liu P, Xiao L, Tang Y, et al. Journal of Thermal Analysis and Calorimetry,2019,136(3),1323. 36 Xiao J, Li J, Xu Z. Environmental Science & Technology,2017,51(20),11960. 37 Wang R C, Lin Y C, Wu S H. Hydrometallurgy,2009,99(3),194. 38 Kang J, Sohn J, Chang H, et al. Advanced Powder Technology,2010,21,175. 39 Lee C K, Rhee K. Hydrometallurgy,2003,68,5. 40 Chen X, Ma H, Luo C, et al. Journal of Hazardous Materials,2017,326,77. 41 Chen X, Fan B, Xu L, et al. Journal of Cleaner Production,2016,112,3562. 42 Zeng X, Li J. Journal of Hazardous Materials,2015,295,112. 43 Gao W, Song J, Cao H, et al. Journal of Cleaner Production,2018,178,833. 44 Yao Y, Zhu M, Zhao Z, et al. ACS Sustainable Chemistry & Engineering,2018,6,13611. 45 Meshram P, Pandey B D, Mankhand T R. Chemical Engineering Journal,2015,281,418. 46 Huang X Z, Chu Z, Ji Z G, et al. Chinese Journal Rare Metals,China,2018(in Chinese). 黄孝振,徐政,纪仲光,等.稀有金属,2018. 47 Zheng X, Zhu Z, Lin X, et al. Engineering,2018,3(4),361. 48 He L, Sun S, Mu Y, et al. ACS Sustainable Chemistry & Engineering,2016,5,714. 49 Chen X, Zhou T. Waste Management & Research,2014,32(11),1083. 50 Yao L, Yao H, Xi G, et al. Royal Society of Chemistry Advance,2016,6,17947. 51 He L, Sun S, Song X, et al. Waste Management,2017,64,171. 52 Zhang X, Cao H, Xie Y, et al. Separation and Purification Technology,2015,150,186. 53 Zou H, Gratz E, Apelian D, et al. Green Chemistry,2013,15(5),1183. 54 Meshram P, Abhilash, Pandey B D. The Minerals, Metals and Materials Society,2016,68(10),2613. 55 Sun C, Xu L, Chen X, et al. Waste Management & Research,2018,36(2),113. 56 Li L, Bian Y, Zhang X, et al. Journal of Power Sources,2018,377,70. 57 Gao W, Song J, Cao H, et al. Journal of Cleaner Production,2018(178),833. 58 Wu C, Li B, Yuan C, et al. Waste Management,2019,93,153. 59 Ku H, Jung Y, Jo M, et al. Journal of Hazardous Materials,2016,313,138. 60 Wang H, Huang K, Zhang Y, et al. ACS Sustainable Chemistry & Engineering,2017,5(12)11489. 61 Zheng X, Gao W, Zhang X, et al. Waste Management,2017,60,680. 62 Meng X, Han K N. Mineral Processing and Extractive Metullargy Review,1996,1(16),23. 63 Mishra D, Srivastava R R, Sahu K K, et al. Hydrometallurgy,2011,109(3-4),215. 64 Meng K, Cao Y, Zhang B, et al. ACS Sustainable Chemistry & Enginee-ring,2019,7,7750. 65 Zhang P, Yokoyama T, Itabashi O, et al. Hydrometallurgy,1998,47(2),259. 66 Kang J, Senanayake G, Sohn J, et al. Hydrometallurgy,2010,100(3-4),168. 67 Mantuano D P, Dorella G, Elias R C A, et al. Journal of Power Sources,2006,159(2),1510. 68 Suzuki T, Nakamura T, Inoue Y, et al. Separation and Purification Technology,2012,98,396. 69 Wang F, He F, Zhao J, et al. Separation and Purification Technology,2012,93,8. 70 Chen W, Ho H. Metals,2018,8(5),321. 71 Vasilyev F, Virolainen S, Sainio T. Separation and Purification Technology,2019,210,530. 72 Nguyen V T, Lee J, Jeong J, et al. Metals and Materials International,2014,20(2),357. 73 Wang F, Sun R, Xu J, et al. RSC Advances,2016,6,85303. 74 Hong H S, Kim D W, Choi H L, et al. Archives of Metallurgy and Mate-rials,2017,62(2),1011. 75 Chen X, Zhou T, Kong J, et al. Separation and Purification Technology,2015,141,76. 76 Sattar R, Ilyas S, Bhatti H N, et al. Separation and Purification Techno-logy,2019,209,725. 77 Prabaharan G, Barik S P, Kumar N, et al. Waste Management,2017,68,527. 78 Lupi C, Pasquali M. Minerals Engineering,2003,16(6),537. 79 Yang Y, Xu S, He Y. Waste Management,2017,64,219. 80 Sa Q G E H M. Journal of Power Sources,2015,82,140. 81 He L, Sun S, Yu J. Ceramics International,2018,44(1),351. 82 Zhang S, Deng C, Fu B L, et al. Powder Technology,2010,198(3),373. 83 Yao L, Fenga Y, Xi G. RSC Advances,2015,5,44107. 84 Yao L, Yao H, Xi G, et al. Royal Society of Chemistry Advance,2016,17947. 85 Meng X, Hao J, Cao H, et al. Waste Management,2019,84,54. 86 Zhou H, Zhao X, Yin C, et al. Electrochim Acta,2018,291,142.