废旧锂离子电池负极石墨循环再生的研究进展

doi:10.16085/j.issn.1000-6613.2023-0419

化工进展 ›› 2024, Vol. 43 ›› Issue (3): 1524-1534.DOI: 10.16085/j.issn.1000-6613.2023-0419

• 资源与环境化工 • 上一篇

废旧锂离子电池负极石墨循环再生的研究进展

楚振普¹(), 陈禹蒙²^,³(), 李俊国³, 孙庆轩², 刘科¹^,³^,⁴()

^1.南方科技大学化学系，广东深圳 518055
^2.深圳职业技术学院机电工程学院，广东深圳 518055
^3.南方科技大学创新创业学院，广东深圳 518055
^4.广东省催化重点实验室，广东深圳 518055

收稿日期:2023-03-20 修回日期:2023-05-30 出版日期:2024-03-10 发布日期:2024-04-11
通讯作者: 陈禹蒙,刘科
作者简介:楚振普（1999—），男，硕士研究生，研究方向为废旧锂离子电池资源化回收。E-mail：12232778@mail.sustech.edu.cn。
基金资助:
深圳市科技计划(KQTD20180411143418361);广东省催化重点实验室(2020B121201002)

Review on recycling of graphite anode from spent lithium-ion batteries

CHU Zhenpu¹(), CHEN Yumeng²^,³(), LI Junguo³, SUN Qingxuan², LIU Ke¹^,³^,⁴()

^1.Department of Chemistry, Southern University of Science and Technology, Shenzhen 518055, Guangdong, China
^2.School of Mechanical and Electrical Engineering, Shenzhen Polytechnic, Shenzhen 518055, Guangdong, China
^3.School of Innovation and Entrepreneurship, Southern University of Science and Technology, Shenzhen 518055, Guangdong, China
^4.Guangdong Provincial Key Laboratory of Catalysis, Southern University of Science and Technology, Shenzhen 518055, Guangdong, China

Received:2023-03-20 Revised:2023-05-30 Online:2024-03-10 Published:2024-04-11
Contact: CHEN Yumeng, LIU Ke

摘要/Abstract

摘要：

锂离子电池使用6~8年后，其容量会出现一定程度的衰减，从而产生大量废弃物。负极石墨在电池中质量分数占比为12%~21%，对其回收利用有利于保护环境和发展经济。针对废旧锂离子电池负极石墨再生为电池级石墨的方法展开综述，主要介绍了浸出煅烧组合、石墨表面涂覆、制备复合材料和杂原子掺杂的方法，并在能耗、电化学性能等方面做了简要比较。目前，在众多再循环方向中，将废旧石墨再生为电池级石墨是最合适的路径，而且能从根源上解决负极材料的再生问题。在此基础上，未来应开发更加高效环保的浸出剂，寻求多路径的低温煅烧方法，尝试其他高容量负极材料与废旧石墨复合或者石墨表面的低成本涂层，加强杂原子在石墨中掺杂机理的研究。

关键词: 废旧锂离子电池, 石墨, 再生, 回收, 废物处理

Abstract:

Lithium-ion battery capacity will reduce to a certain extent after used for 6—8 years and a large amount of waste are generated. The graphite anode accounts for 12%—21% of battery and its recycling is beneficial to the environment protection and economic development. In this paper, the regenerating methods of spent graphite anode into battery-grade graphite are summarized, which include the combination of leaching and calcination, graphite surface coating, preparation of composite materials and heteroatom doping. A brief comparison of these methods is also presented in terms of energy consumption and electrochemical performance. At present, direct regeneration for lithium-ion batteries is considered as the most suitable method for the regeneration of anode materials. In the future, more efficient and eco-friendly leaching agents and the multi-path low-temperature calcination methods should be investigated. In addition, high-capacity anode materials should be studied to composite with spent graphite, as well as the development of low-cost coating on the surface of graphite. Furthermore, the doping mechanism of heteroatoms in graphite is a direction worthy of research.

Key words: spent lithium-ion batteries, graphite, regeneration, recovery, waste treatment

中图分类号:

X705

楚振普, 陈禹蒙, 李俊国, 孙庆轩, 刘科. 废旧锂离子电池负极石墨循环再生的研究进展[J]. 化工进展, 2024, 43(3): 1524-1534.

CHU Zhenpu, CHEN Yumeng, LI Junguo, SUN Qingxuan, LIU Ke. Review on recycling of graphite anode from spent lithium-ion batteries[J]. Chemical Industry and Engineering Progress, 2024, 43(3): 1524-1534.

图/表 5

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工艺	容量 /mAh·g^-1	首次充电比容量 /mAh·g^-1	首次库仑效率 /%	容量保持率 /%	参考文献
①硫酸固化-酸浸法 ②Ar气氛，1500℃煅烧2h		349（0.1C）	88.3	98.8	[43]
①N₂气氛，1400℃煅烧4h ②超声振动和筛分	360.8			几乎100（100次循环，1C）	[49]
①500℃高温热处理 ②0.1mol/L酸性溶液浸出一夜 ③N₂气氛，3000℃煅烧6h		352.5		97.3（1000次循环）； 87.88（1600次循环）	[50]
①35℃下浸泡在2mol/L硫酸中过夜 ②60℃下干燥12h ③酸浸石墨与硝酸钴加入适量的醇中并搅拌直至醇干燥 ④N₂气氛，900℃煅烧4h	358（1次循环，0.1C）； 245.4（500次循环，1C）				[42]
①硫酸固化酸浸处理 ②微波煅烧600~900℃，1~3h	354.1（0.1C）		83.4	98.3（60次循环，0.1C）	[48]
①95℃下，200g/L硫酸溶液中液固比（L/S）为1mL∶5g，浸出4h ②Ar气氛，900℃煅烧2h		358.1（0.1C）		98.8（100次循环）	[44]
①加入硫酸盐、氟化钠250℃低温焙烧 ②水浸			85.71	91.2（400次循环）	[51]
①110℃真空干燥箱干燥10h ②与不同质量比的NH₄F粉末手动搅拌混合2h ③空气气氛，200℃煅烧60min	340.9		92.13	96（100次循环，1C） 96（400次循环，1C/1C，全电池）	[52]

工艺	容量 /mAh·g^-1	首次充电比容量 /mAh·g^-1	首次库仑效率 /%	容量保持率 /%	参考文献
①硫酸固化-酸浸法 ②Ar气氛，1500℃煅烧2h		349（0.1C）	88.3	98.8	[43]
①N₂气氛，1400℃煅烧4h ②超声振动和筛分	360.8			几乎100（100次循环，1C）	[49]
①500℃高温热处理 ②0.1mol/L酸性溶液浸出一夜 ③N₂气氛，3000℃煅烧6h		352.5		97.3（1000次循环）； 87.88（1600次循环）	[50]
①35℃下浸泡在2mol/L硫酸中过夜 ②60℃下干燥12h ③酸浸石墨与硝酸钴加入适量的醇中并搅拌直至醇干燥 ④N₂气氛，900℃煅烧4h	358（1次循环，0.1C）； 245.4（500次循环，1C）				[42]
①硫酸固化酸浸处理 ②微波煅烧600~900℃，1~3h	354.1（0.1C）		83.4	98.3（60次循环，0.1C）	[48]
①95℃下，200g/L硫酸溶液中液固比（L/S）为1mL∶5g，浸出4h ②Ar气氛，900℃煅烧2h		358.1（0.1C）		98.8（100次循环）	[44]
①加入硫酸盐、氟化钠250℃低温焙烧 ②水浸			85.71	91.2（400次循环）	[51]
①110℃真空干燥箱干燥10h ②与不同质量比的NH₄F粉末手动搅拌混合2h ③空气气氛，200℃煅烧60min	340.9		92.13	96（100次循环，1C） 96（400次循环，1C/1C，全电池）	[52]

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废旧锂离子电池负极石墨循环再生的研究进展

Review on recycling of graphite anode from spent lithium-ion batteries

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