CIESC Journal ›› 2023, Vol. 74 ›› Issue (4): 1446-1456.DOI: 10.11949/0438-1157.20221550
• Reviews and monographs • Previous Articles Next Articles
Zhongliang XIAO(), Bilu YIN, Liubin SONG(), Yinjie KUANG, Tingting ZHAO, Cheng LIU, Rongyao YUAN
Received:
2022-11-30
Revised:
2022-12-23
Online:
2023-06-02
Published:
2023-04-05
Contact:
Liubin SONG
肖忠良(), 尹碧露, 宋刘斌(), 匡尹杰, 赵亭亭, 刘成, 袁荣耀
通讯作者:
宋刘斌
作者简介:
肖忠良(1964—),男,博士,教授,xiaozhongliang@163.com
基金资助:
CLC Number:
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.
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.
浸出试剂 | 辅助试剂 | 阴极材料 | 操作条件 | 浸出率 /% | 优点 | 缺点 | |||
---|---|---|---|---|---|---|---|---|---|
Li | Ni | Co | Mn | ||||||
甲磺酸[ | 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[ | 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[ | H2O2 | LiNi0.5Co0.2Mn0.3O2 | 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[ | 亚硫酸钠 | Li(Ni1/3Co1/3Mn1/3)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[ | 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[ | 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[ | 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[ | 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[ | H2O2 | LiNi1/3Mn1/3Co1/3O2 | 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[ | 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[ | 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[ | 柠檬酸 | LiNi0.5Co0.2Mn0.3O2 | 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[ | H2O2 | LiNi1/3Mn1/3Co1/3O2 | 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[ | 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[ | 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[ | 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 |
Table 1 Comparison of the characteristics of different leaching methods in the recovery of used LIBs
浸出试剂 | 辅助试剂 | 阴极材料 | 操作条件 | 浸出率 /% | 优点 | 缺点 | |||
---|---|---|---|---|---|---|---|---|---|
Li | Ni | Co | Mn | ||||||
甲磺酸[ | 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[ | 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[ | H2O2 | LiNi0.5Co0.2Mn0.3O2 | 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[ | 亚硫酸钠 | Li(Ni1/3Co1/3Mn1/3)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[ | 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[ | 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[ | 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[ | 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[ | H2O2 | LiNi1/3Mn1/3Co1/3O2 | 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[ | 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[ | 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[ | 柠檬酸 | LiNi0.5Co0.2Mn0.3O2 | 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[ | H2O2 | LiNi1/3Mn1/3Co1/3O2 | 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[ | 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[ | 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[ | 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 |
方法 | 优点 | 缺点 |
---|---|---|
火法冶金 | 不产生废水;与湿法冶金相比,加工步骤更少;合金直接被熔化为所需回收金属 | 耗能高;有害气体排放;回收过程中的损失大 |
湿法冶金 | 高可持续性;高提取效率;能源消耗低; 危险气体排放少;成本低 | 操作步骤复杂;产生大量的酸性废物;有害气体排放如Cl2、SO3、NO x; 处理有害气体、酸性浸出物和酸性废水的额外费用高 |
生物湿法冶金 (生物沥滤) | 操作成本低;化学品的使用量最小; 在低金属浓度下效率高;无毒 | 动力学缓慢,处理时间长;电解质和黏合剂的毒性对微生物活性产生影响;在高纸浆密度下,效率较低;无法改变金属价态 |
Table 2 Comparison of various metal recovery processes for waste LIBs
方法 | 优点 | 缺点 |
---|---|---|
火法冶金 | 不产生废水;与湿法冶金相比,加工步骤更少;合金直接被熔化为所需回收金属 | 耗能高;有害气体排放;回收过程中的损失大 |
湿法冶金 | 高可持续性;高提取效率;能源消耗低; 危险气体排放少;成本低 | 操作步骤复杂;产生大量的酸性废物;有害气体排放如Cl2、SO3、NO x; 处理有害气体、酸性浸出物和酸性废水的额外费用高 |
生物湿法冶金 (生物沥滤) | 操作成本低;化学品的使用量最小; 在低金属浓度下效率高;无毒 | 动力学缓慢,处理时间长;电解质和黏合剂的毒性对微生物活性产生影响;在高纸浆密度下,效率较低;无法改变金属价态 |
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