低共熔溶剂回收废旧锂离子电池正极材料的研究进展

doi:10.16085/j.issn.1000-6613.2023-0633

摘要/Abstract

摘要：

在“碳达峰、碳中和”背景下，中国新能源汽车数量激增，锂离子电池大规模应用导致其报废带来的问题不容小觑，如战略金属资源的浪费，对环境、人体健康的影响等。因此，废旧锂离子电池资源再利用是十分必要的，特别是正极材料的回收。目前正极材料的回收方法主要包含火法冶金、湿法冶金、微生物冶金和低共熔溶剂浸出等，本文着重介绍了新兴的低共熔溶剂浸出法，根据氢键供体和受体的不同以及有无外场辅助将低共熔溶剂分为5类，总结了低共熔溶剂浸出法的最新进展，概述了DES浸出正极材料的还原作用，通过缩核模型解释了DES浸出的化学反应动力学原理和作用机制，同时对低共熔溶剂回收废旧电池的发展提出了面临的问题并进行了展望。该工作为低共熔溶剂浸出正极材料的进一步深入研究与规模化应用提供了可行性的指导与参考。

关键词: 低共熔溶剂, 废旧锂离子电池, 湿法冶金, 浸取, 回收, 正极材料

Abstract:

In the context of “carbon peaking and carbon neutrality goals”, the number of new energy vehicles in China has begun to surge, but after the large-scale application of lithium-ion batteries, the problems brought by their scrapping can not be underestimated, such as the waste of strategic metal resources, the impact on the environment and human health. Therefore, the reuse of waste lithium-ion battery resources is very necessary, especially the recovery of cathode materials. At present, the recovery methods of cathode materials mainly include fire metallurgy, hydrometallurgy, microbial metallurgy and deep eutectic solvent leaching, etc. This study focuses on the emerging deep eutectic solvent leaching methods, according to the difference of hydrogen bond donor and acceptor and whether there is external field assistance, the deep eutectic solvent leaching method is divided into 5 categories, the latest progress of deep eutectic solvent leaching method is summarized, the reduction effect of DES leaching cathode materials is overviewed, and the chemical reaction kinetic principle and mechanism of DES leaching are explained by shrinking core model. At the same time, the problems facing the development of recycling waste batteries with low eutectic solvents are put forward and the prospect is made. This work provides a feasible guidance and reference for further research and large-scale application of eutectic solvent leaching of cathode materials.

Key words: deep eutectic solvents, spent lithium-ion battery, hydrometallurgy, leaching, recovery, cathode material

中图分类号:

马伊, 曹世伟, 王家骏, 林立群, 邢延, 曹腾良, 卢峰, 赵振伦, 张志军. 低共熔溶剂回收废旧锂离子电池正极材料的研究进展[J]. 化工进展, 2023, 42(S1): 219-232.

MA Yi, CAO Shiwei, WANG Jiajun, LIN Liqun, XING Yan, CAO Tengliang, LU Feng, ZHAO Zhenlun, ZHANG Zhijun. Research progress in recovery of spent cathode materials for lithium-ion batteries using deep eutectic solvents[J]. Chemical Industry and Engineering Progress, 2023, 42(S1): 219-232.

图/表 10

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DES	液固比	T/℃	t/h	浸出效果	参考文献
ChCl∶Gly比为1∶2	2.5g/L	180	2	Co：47.59%，Li：50.4%	[19]
ChCl∶LAA比为2∶1.6	1∶25	50	1	Ni、Co、Mn>96%	[19]
ChCl∶BSA∶EtOH比为1∶1∶2	20g/L	90	2	Co：98%，Li：99%	[57]
ChCl∶MAL∶PTSA	20g/L	100	24	Co：98.61%，Li：98.78%	[38]
ChCl∶Urea∶EG比为1∶1∶2	9.69g/L	100	72	Co：1.61%，Li：92.82%，Ni：0.72%，Mn：0.42%	[58]
TA(20g/L)∶CH₃COOH(1mol/L)	20g/L	80	2	Co：94%，Li：99%	[39]
EG∶CA比为2.5∶1	15g/L	95	10	Co：96.2%，Li：99.1%，Ni：97.6%，Mn：98.3%	[59]
PEG∶PSA比为1∶1	20g/L	100	24	Co：99.5%	[46]
ChCl∶LA比为2∶1		70	24	Li、Ni、Co、Mn为100%	[35]
ChCl∶CA比为2∶1, 35% H₂O	20g/L	40	1	Co>98%	[52]
BCl∶EG比为1∶5	25g/kg	140	0.17	Li、Ni、Co、Mn>99%	[28]
ChCl∶EG	12.5g/L	180	240	Li：91.63%，Co：92.52%，Ni：94.92%，Mn：95.47%	[29]
ChCl∶OA∶2H₂O	20g/L	100	0.17	Li：99.05%，Co：99.21%	[55]
EG∶SAD比为12∶1	40g/L	110	6	Li：98.3%，Co：93.5%，Ni：99.1%，Mn：100%	[44]

DES	液固比	T/℃	t/h	浸出效果	参考文献
ChCl∶Gly比为1∶2	2.5g/L	180	2	Co：47.59%，Li：50.4%	[19]
ChCl∶LAA比为2∶1.6	1∶25	50	1	Ni、Co、Mn>96%	[19]
ChCl∶BSA∶EtOH比为1∶1∶2	20g/L	90	2	Co：98%，Li：99%	[57]
ChCl∶MAL∶PTSA	20g/L	100	24	Co：98.61%，Li：98.78%	[38]
ChCl∶Urea∶EG比为1∶1∶2	9.69g/L	100	72	Co：1.61%，Li：92.82%，Ni：0.72%，Mn：0.42%	[58]
TA(20g/L)∶CH₃COOH(1mol/L)	20g/L	80	2	Co：94%，Li：99%	[39]
EG∶CA比为2.5∶1	15g/L	95	10	Co：96.2%，Li：99.1%，Ni：97.6%，Mn：98.3%	[59]
PEG∶PSA比为1∶1	20g/L	100	24	Co：99.5%	[46]
ChCl∶LA比为2∶1		70	24	Li、Ni、Co、Mn为100%	[35]
ChCl∶CA比为2∶1, 35% H₂O	20g/L	40	1	Co>98%	[52]
BCl∶EG比为1∶5	25g/kg	140	0.17	Li、Ni、Co、Mn>99%	[28]
ChCl∶EG	12.5g/L	180	240	Li：91.63%，Co：92.52%，Ni：94.92%，Mn：95.47%	[29]
ChCl∶OA∶2H₂O	20g/L	100	0.17	Li：99.05%，Co：99.21%	[55]
EG∶SAD比为12∶1	40g/L	110	6	Li：98.3%，Co：93.5%，Ni：99.1%，Mn：100%	[44]

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