废旧锂离子电池回收工艺研究进展及其安全风险分析

doi:10.11949/0438-1157.20221550

摘要/Abstract

摘要：

随着锂离子电池(LIBs)市场的快速增长，探索回收退役LIBs的有效策略已成为迫在眉睫的问题。未来，资源化回收将受到广泛关注。资源化回收既可以解决有价金属锂、镍、钴、锰资源短缺的问题，又可抑制废旧电池堆积而引起的危害，但运输、存储以及金属富集过程中的安全性问题仍得不到保障。针对退役电池回收工艺研究进展进行综述，重点对整个回收过程，包括运输存储、预处理、金属富集等步骤进行了全过程安全风险分析。通过对退役电池回收过程中的安全风险进行全面分析和梳理，旨在为国内外企业后续的电池回收方案提供参考。

关键词: 废旧锂离子电池, 资源化管理, 回收工艺, 安全风险分析

Abstract:

With the rapid growth of the lithium-ion batteries (LIBs) market, exploring effective strategies to recycle retired LIBs has become an urgent issue. In the future, resource-based recycling will receive wide attention. Resource-based recycling can not only solve the problem of shortage of valuable metals such as lithium, nickel, cobalt and manganese, but also solve the hazards caused by the accumulation of used batteries. However, the safety of transportation, storage and metal enrichment processes cannot be guaranteed. In this paper, we review the progress of the recycling process of retired LIBs, and focus on the safety risk analysis of the whole recycling process, including transportation, storage, pretreatment and metal enrichment. By analyzing and organizing the safety risks in the recycling process of retired LIBs, we hope to provide guidance for the subsequent battery recycling programs of domestic and foreign enterprises.

Key words: waste lithium-ion batteries, resourceful management, recycling process, safety risk analysis

中图分类号:

A 150.55

肖忠良, 尹碧露, 宋刘斌, 匡尹杰, 赵亭亭, 刘成, 袁荣耀. 废旧锂离子电池回收工艺研究进展及其安全风险分析[J]. 化工学报, 2023, 74(4): 1446-1456.

Zhongliang XIAO, Bilu YIN, Liubin SONG, Yinjie KUANG, Tingting ZHAO, Cheng LIU, Rongyao YUAN. Research progress of waste lithium-ion battery recycling process and its safety risk analysis[J]. CIESC Journal, 2023, 74(4): 1446-1456.

图/表 6

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浸出试剂	辅助试剂	阴极材料	操作条件	浸出率 /%				优点	缺点
浸出试剂	辅助试剂	阴极材料	操作条件	Li	Ni	Co	Mn	优点	缺点
甲磺酸^[70]	H₂O₂	LiCoO₂	0.9%（体积分数） H₂O₂, 1 mol/L, 70℃, 1 h	约100	—	约100	—	操作简单，成本低	腐蚀性,无选择性
甲磺酸+对甲苯磺酸^[71]	H₂O₂	LiFePO₄	4 mol/L甲磺酸， S/L 40 g/L，室温，90 min	95	—	—	—	绿色,成本低	选择性低
硫酸钠^[72]	H₂O₂	LiNi_0.5Co_0.2Mn_0.3O₂	电解, pH=6, 60℃, 2%（体积分数） H₂O₂	>99	—	>99	—	绿色,操作简单	高能耗
氨水-硫酸铵^[73]	亚硫酸钠	Li(Ni_1/3Co_1/3Mn_1/3)O₂	50℃，10~50 g/L 纸浆密度	97	95	89	—	操作简单,成本低,	锰的选择性低
硫酸^[74]	Na₂S₂O₅	Li(Mn, Ni, Co)O₂	>1.25 mol/L H₂SO₄, 0.1 mol/L Na₂S₂O₅, S/L 100 g/L, 60℃, 2.5 h	约90	约90	约90	约90	操作简单	腐蚀性强, 浸出液量大
硫酸^[75]	H₂O₂	LiMn₂O₄	0.5 mol/L H₂SO₄, 2%（体积分数）H₂O₂, S/L 50 g/L, 80℃, 60 min	99.62	—	98.13	—	操作简单	一定的腐蚀性, 高温
磷酸^[76]	葡萄糖	LiCoO₂	1.5mol/L H₃PO₄，0.02 mol/L 葡萄糖，S/L 2 g/L, 80℃，2 h	100	—	98	—	浸出液少,效率高	一定的腐蚀性, 高温
单宁酸^[77]	醋酸	废弃的LIBs 阴极	1 mol/L 醋酸, 20 g/L 单宁酸, 80℃， 4 h	99	—	94	—	浸出液少,效率高	一定的腐蚀性,高温
丙醇酸^[78]	H₂O₂	LiNi_1/3Mn_1/3Co_1/3O₂	0.5% H₂O₂（体积分数）, 1.5 mol/L 丙醇酸, S/L 20 g/L, 70℃, 20 min	95	>98	>98	>98	绿色,操作简单	一定的腐蚀性,高温
柠檬酸^[79]	H₂O₂	废弃的LIBs 阴极	2 mol/L 柠檬酸,2% H₂O₂（体积分数）, 80℃, S/L 20 g/L, 90 min	约100	—	约99	—	绿色,操作简单	无选择性, 高温
柠檬酸^[80]	橘子皮	LiCoO₂	200 mg 橘子皮,1.5 mol/L 柠檬酸, 100℃, 4 h	80.5	90.1	91.3	92.2	绿色, 成本低	高温
草酸盐^[81]	柠檬酸	LiNi_0.5Co_0.2Mn_0.3O₂	0.2 mol/L H₃PO₄, 0.4 mol/L 柠檬酸, pH=1.98	约100	约100	约100	约100	操作简单	一定的腐蚀性
乳酸^[82]	H₂O₂	LiNi_1/3Mn_1/3Co_1/3O₂	1.5 mol/ L 乳酸，2%（体积分数） H₂O₂, S/L 20 g/L, 70℃, 20 min	97.7	98.2	98.9	98.4	高效, 无毒气	高温, 成本高
硫酸+ 丙醇酸^[83]	H₂O₂	LiNi _x Co _y Mn _z O₂	0.93 mol/L H₂SO₄, 0.85 mol/L 丙酮酸, S/L 61 g/L, 70℃, 81 min	99.8	99.5	97.2	96.9	操作简单,高效	一定的腐蚀性, 高温
柠檬酸+ DL-苹果酸^[84]	H₂O₂	废弃的LIBs 阴极	1 mol/L 柠檬酸, 2%（体积分数） H₂O₂, 95℃, 30 min	>96	—	>98	—	操作简单,绿色	高温, 无选择性
酒石酸^[85]	抗坏血酸	LiCoO₂	0.4 mol/L 酒石酸，80℃, 5 h， 0.02 mol/L 抗坏血酸，S/L 2 g/L	99	—	96	—	高效, 无毒气	渗滤液量大,温度高

浸出试剂	辅助试剂	阴极材料	操作条件	浸出率 /%				优点	缺点
浸出试剂	辅助试剂	阴极材料	操作条件	Li	Ni	Co	Mn	优点	缺点
甲磺酸^[70]	H₂O₂	LiCoO₂	0.9%（体积分数） H₂O₂, 1 mol/L, 70℃, 1 h	约100	—	约100	—	操作简单，成本低	腐蚀性,无选择性
甲磺酸+对甲苯磺酸^[71]	H₂O₂	LiFePO₄	4 mol/L甲磺酸， S/L 40 g/L，室温，90 min	95	—	—	—	绿色,成本低	选择性低
硫酸钠^[72]	H₂O₂	LiNi_0.5Co_0.2Mn_0.3O₂	电解, pH=6, 60℃, 2%（体积分数） H₂O₂	>99	—	>99	—	绿色,操作简单	高能耗
氨水-硫酸铵^[73]	亚硫酸钠	Li(Ni_1/3Co_1/3Mn_1/3)O₂	50℃，10~50 g/L 纸浆密度	97	95	89	—	操作简单,成本低,	锰的选择性低
硫酸^[74]	Na₂S₂O₅	Li(Mn, Ni, Co)O₂	>1.25 mol/L H₂SO₄, 0.1 mol/L Na₂S₂O₅, S/L 100 g/L, 60℃, 2.5 h	约90	约90	约90	约90	操作简单	腐蚀性强, 浸出液量大
硫酸^[75]	H₂O₂	LiMn₂O₄	0.5 mol/L H₂SO₄, 2%（体积分数）H₂O₂, S/L 50 g/L, 80℃, 60 min	99.62	—	98.13	—	操作简单	一定的腐蚀性, 高温
磷酸^[76]	葡萄糖	LiCoO₂	1.5mol/L H₃PO₄，0.02 mol/L 葡萄糖，S/L 2 g/L, 80℃，2 h	100	—	98	—	浸出液少,效率高	一定的腐蚀性, 高温
单宁酸^[77]	醋酸	废弃的LIBs 阴极	1 mol/L 醋酸, 20 g/L 单宁酸, 80℃， 4 h	99	—	94	—	浸出液少,效率高	一定的腐蚀性,高温
丙醇酸^[78]	H₂O₂	LiNi_1/3Mn_1/3Co_1/3O₂	0.5% H₂O₂（体积分数）, 1.5 mol/L 丙醇酸, S/L 20 g/L, 70℃, 20 min	95	>98	>98	>98	绿色,操作简单	一定的腐蚀性,高温
柠檬酸^[79]	H₂O₂	废弃的LIBs 阴极	2 mol/L 柠檬酸,2% H₂O₂（体积分数）, 80℃, S/L 20 g/L, 90 min	约100	—	约99	—	绿色,操作简单	无选择性, 高温
柠檬酸^[80]	橘子皮	LiCoO₂	200 mg 橘子皮,1.5 mol/L 柠檬酸, 100℃, 4 h	80.5	90.1	91.3	92.2	绿色, 成本低	高温
草酸盐^[81]	柠檬酸	LiNi_0.5Co_0.2Mn_0.3O₂	0.2 mol/L H₃PO₄, 0.4 mol/L 柠檬酸, pH=1.98	约100	约100	约100	约100	操作简单	一定的腐蚀性
乳酸^[82]	H₂O₂	LiNi_1/3Mn_1/3Co_1/3O₂	1.5 mol/ L 乳酸，2%（体积分数） H₂O₂, S/L 20 g/L, 70℃, 20 min	97.7	98.2	98.9	98.4	高效, 无毒气	高温, 成本高
硫酸+ 丙醇酸^[83]	H₂O₂	LiNi _x Co _y Mn _z O₂	0.93 mol/L H₂SO₄, 0.85 mol/L 丙酮酸, S/L 61 g/L, 70℃, 81 min	99.8	99.5	97.2	96.9	操作简单,高效	一定的腐蚀性, 高温
柠檬酸+ DL-苹果酸^[84]	H₂O₂	废弃的LIBs 阴极	1 mol/L 柠檬酸, 2%（体积分数） H₂O₂, 95℃, 30 min	>96	—	>98	—	操作简单,绿色	高温, 无选择性
酒石酸^[85]	抗坏血酸	LiCoO₂	0.4 mol/L 酒石酸，80℃, 5 h， 0.02 mol/L 抗坏血酸，S/L 2 g/L	99	—	96	—	高效, 无毒气	渗滤液量大,温度高

[1]	李丽1,2，葛静1，陈人杰1,2，吴锋1,2. 废旧锂离子电池回收制备钴酸锂的研究进展 [J]. CIESC Journal, 2010, 29(4): 757-.
[2]	张卫新, 马世闯, 杨则恒, 周晨旭, 王强. 基于废旧锂离子电池正极材料LiMn₂O₄制备λ-MnO₂催化剂 [J]. 化工学报, 2009, 60(5): 1181-1185.