退役锂离子电池正极的湿法冶金回收工艺：可持续技术的进展与应用

doi:10.3866/PKU.WHXB202309028

物理化学学报 >> 2024, Vol. 40 >> Issue (10): 2309028.doi: 10.3866/PKU.WHXB202309028

退役锂离子电池正极的湿法冶金回收工艺：可持续技术的进展与应用

张思宇¹^,², 谷昆泓¹, 鲁兵安³, 韩俊伟¹^,*(), 周江²^,*()

¹ 中南大学资源加工与生物工程学院, 长沙 410083
² 中南大学材料科学与工程学院, 长沙 410083
³ 湖南大学物理与微电子科学学院, 长沙 410082

收稿日期:2023-09-18 修回日期:2023-10-09 录用日期:2023-10-16 发布日期:2024-03-13
通讯作者: Email: hanjunwei@csu.edu.cn (韩俊伟)zhou_jiang@csu.edu.cn (周江)
基金资助:
国家自然科学基金(52174269); 国家自然科学基金(52374293); 湖南省自然科学基金(2021JJ10064); 湖南省自然科学基金(2021JJ20062)

Hydrometallurgical Processes on Recycling of Spent Lithium-lon Battery Cathode: Advances and Applications in Sustainable Technologies

Siyu Zhang¹^,², Kunhong Gu¹, Bing'an Lu³, Junwei Han¹^,*(), Jiang Zhou²^,*()

¹ School of Minerals Processing and Bioengineering, Central South University, Changsha 410083, China
² School of Materials Science and Engineering, Central South University, Changsha 410083, China
³ School of Physics and Electronics, Hunan University, Changsha 410082, China

Received:2023-09-18 Revised:2023-10-09 Accepted:2023-10-16 Published:2024-03-13
Contact: Email: hanjunwei@csu.edu.cn (Junwei Han)zhou_jiang@csu.edu.cn (Jiang Zhou)
Supported by:
the National Natural Science Foundation of China(52174269); the National Natural Science Foundation of China(52374293); the Natural Science Foundation of Hunan Province(2021JJ10064); the Natural Science Foundation of Hunan Province(2021JJ20062)

摘要/Abstract

摘要：

电子信息和新能源汽车等产业的迅速发展导致锂离子电池(LIBs)的需求量激增，随之引发了其报废潮。可持续的回收技术对于以环保的方式解决大量退役锂离子电池(EOL LIBs)至关重要。本文全面综述了基于湿法冶金的LIBs正极废料中有价金属的提取技术，从环境、技术和工业化可行性的角度出发，对无机酸、有机酸和低共熔溶剂(DESs)等方法进行了详细的讨论和分析，以期优化技术并降低对环境的影响。此外，本文也详细探讨了绿色的生物质废料等还原剂和高效环保的EOL LIBs内循环机械活化技术等在强化LIBs正极废料有价金属溶浸中的应用，并由此提出了EOL LIBs回收过程中可能存在的研究机会和挑战。

关键词: 锂离子电池, 浸出, 湿法冶金, 生物质废料, 机械化学

Abstract:

Rechargeable lithium-ion batteries (LIBs) have garnered global attention as a prominent solution for storing intermittent renewable energy, addressing energy scarcity, and mitigating environmental pollution. In the previous century, Sony introduced the "lithium-ion battery" concept, heralding a new era for LIBs and effectively bringing them into commercial use. The initial commercially available LIBs utilized lithium cobalt oxide as the cathode material and graphite as the anode material. Capitalizing on their attributes encompassing elevated energy density, substantial specific capacity, portability, and ecological compatibility, LIBs have secured substantial market share throughout the commercialization trajectory. Their commercial viability and scope have been markedly enhanced through the continuous advancement of LIBs' cathode materials and innovative implementations encompassing battery design, assembly, and thermal management. In recent years, the rapid expansion of sectors such as cellular phones and new energy vehicles, coupled with the drive towards "carbon peaking" and "carbon neutrality, " has propelled the robust growth of the LIBs sector, which has resulted in widespread adoption across diverse industrial domains and daily applications spanning road transportation, materials, chemicals, and information technology. However, the swift proliferation of the LIBs industry has incited an influx of end-of-life (EOL) batteries, which pose risks of flammability, explosiveness, and the presence of toxic and hazardous elements, including fluorides. These aspects collectively pose a formidable environmental and human health hazard, warranting urgent and harmless disposal measures. Simultaneously, EOL LIBs are rich reservoirs of resources like lithium, nickel, cobalt, and manganese, boasting metal contents in cathode waste that significantly exceed those found in their natural mineral counterparts, presenting a substantial opportunity for resource reclamation. Therefore, extracting valuable metals from LIBs cathode waste simultaneously addresses critical environmental and human health concerns linked to improper EOL LIBs disposal while playing a pivotal role in mitigating metal resource shortages. This dual-purpose endeavor aligns with the overarching goal of promoting sustainable resource circulation. The recovery of LIBs cathode materials is a central topic of global research discussion. This study comprehensively overviews valuable metal extraction from LIBs cathode waste using hydrometallurgical methodologies. It delves deeply into diverse approaches encompassing inorganic, organic, and deep eutectic solvents (DESs), scrutinizing environmental, technical, and industrial feasibilities. The objective is to optimize extraction techniques and mitigate their environmental impact. Furthermore, this paper meticulously discusses the utilization of environmentally friendly reducing agents like green biomass waste, coupled with the efficient and eco-conscious EOL LIBs internal cycle mechanical activation technology, to enhance the leaching of valuable metals from cathode waste. This inquiry culminates in identifying potential research avenues and challenges within the EOL LIBs recycling process.

Key words: Lithium-ion battery, Leaching, Hydrometallurgy, Biomass waste, Mechanochemistry

张思宇, 谷昆泓, 鲁兵安, 韩俊伟, 周江. 退役锂离子电池正极的湿法冶金回收工艺：可持续技术的进展与应用[J]. 物理化学学报, 2024, 40(10), 2309028. doi: 10.3866/PKU.WHXB202309028

Siyu Zhang, Kunhong Gu, Bing'an Lu, Junwei Han, Jiang Zhou. Hydrometallurgical Processes on Recycling of Spent Lithium-lon Battery Cathode: Advances and Applications in Sustainable Technologies[J]. Acta Phys. -Chim. Sin. 2024, 40(10), 2309028. doi: 10.3866/PKU.WHXB202309028

链接本文: https://www.whxb.pku.edu.cn/CN/10.3866/PKU.WHXB202309028

https://www.whxb.pku.edu.cn/CN/Y2024/V40/I10/2309028

图/表 8

图1

图2

图3

图4

表1

典型湿法冶金回收锂离子电池正极废料的工艺对比"

Process	Cathode category	Reducing agent	Optimal process conditions	Leaching efficiency (%)	Ref.
Acid leaching	LiNi_0.8Co_0.15Al_0.05O₂	–	4 mol∙L⁻¹ HCl; 18 h; 363 K; 50 g∙L⁻¹	~100% Ni, Co, Al, Li	26
	LiNi_1/3Co_1/3Mn_1/3O₂	NaHSO₃	1 mol∙L⁻¹ H₂SO₄; 240 min; 368 K; 20 g∙L⁻¹	96.4% Ni, 91.6% Co, 87.9% Mn, 96.7% Li	74
	LiCoO₂	H₂O₂	0.7 mol∙L⁻¹ H₃PO₄; 60 min; 313 K; 50 g∙L⁻¹	99% Co, 99% Li	28
	LiFePO₄ LiNi_xCo_yMn_zO₂	–	0.88 mol∙L⁻¹ H₃PO₄; LFP/NCM 2 : 1; 120 min; 353 K; ~30 g∙L⁻¹	99.1% Ni, 98.9% Co, 97.3% Mn, 99.6% Li, 100% Fe	27
	LiCoO₂	H₂O₂	2 mol∙L⁻¹ H₃Cit; 120 min; 333 K; 30 g∙L⁻¹	81% Co, 92% Li	29
	Mixed cathode waste	–	0.5 mol∙L⁻¹ C₆H₈O₆; 10 min; 398 K; 10 g∙L⁻¹	~100% Co, ~100% Li	30
	LiCoO₂	–	1 mol∙L⁻¹ C₂H₂O₄; 150 min; 368 K; 15 g∙L⁻¹	~97% Co, ~98% Li	32
	LiNi_x Co_yMn_zO₂	H₂O₂	0.93 mol∙L⁻¹ H₂SO₄; 0.85 mol∙L⁻¹ C₃H₄O₄; 81 min; 333 K; 61 g∙L⁻¹	99.46% Ni, 97.24% Co, 96.88% Mn, 99.79% Li	37
Bio leaching	LiCoO₂	–	Thiobacillus ferric oxide; Cu²⁺ 0.75 g∙L⁻¹; 6 d; 1%; 308 K	99.9% Co	47
Bio leaching	LiCoO₂	C₆H₈O₆	mixed sulfur-oxidizing bacteria; 48 h; 20 g∙L⁻¹; 303 K	94% Co, 95% Li	48
Alkali leaching	LiNi_xCo_yMn_1−x−yO₂	Na₂SO₃	4 mol∙L⁻¹ NH₃; 0.3 mol∙L⁻¹ Na₂SO₃; 5 g∙L⁻¹; 1 mol∙L⁻¹ (NH₄)₂CO₃; 120 min; 353 K	85.3% Ni, 86.4% Co, 1.45% Mn, 79.1% Li	58
Alkali leaching	LiNi_xCo_yMn_zO₂	(NH₄)₂SO₃	3 mol∙L⁻¹ NH₃·H₂O; 1.5 mol∙L⁻¹ (NH₄)₂SO₃; 120 min; 353 K; 20 g∙L⁻¹	97.7 % Ni, 99.1% Co	59
DESs leaching	LiCoO₂	–	ChCl + (NH₂)₂CO (7.5g + 77.5 g∙L⁻¹); 12 h; 453 K; 1 g/25 g	95% Co, 95% Li	65
	LiNi_xCo_yMn_zO₂	–	ChCl + C₆H₇O₂P (1 : 2); 80 min; 373 K; ~11 g∙L⁻¹	96.4% Ni, 97.0% Co, 93.0% Mn, 97.7% Li	69
	LiCoO₂ Li_14.8Ni_1.7Co_8.5MnO_30.5	–	EG + SAD (12 : 1); 6 h; 383 K; 40 g∙L⁻¹	99.1% Ni, 94.8% Co, 100% Mn, 100% Li	72
	Li_3.2Ni_2.4Co_1.0Mn_1.4O_8.3	–	EG + C₄H₆O₆ (5 : 1); 12 h; 393 K; 20 g∙L⁻¹	98.34% Li	71

表1

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图6

图7

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