硅酸盐学报

废旧锂离子电池原位还原焙烧水浸提锂及杂质影响

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李金辉 ¹ , 任权兵 ² , 龙光武 ³ , 邓方坤 ⁴ , 王爽 ⁴ , 李楠 ⁵ , 丁浩亮 ⁶ , 胡伟杰 ¹ , 肖宇 ⁷ , 翁雅青 ⁴

硅酸盐学报 | 支撑碳中和目标的新能源材料与器件循环利用专题—研究论文 2025,53(8): 2109-2114

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硅酸盐学报 |支撑碳中和目标的新能源材料与器件循环利用专题—研究论文 2025 , 53 (8) : 2109 -2114

废旧锂离子电池原位还原焙烧水浸提锂及杂质影响

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李金辉¹, 任权兵², 龙光武³, 邓方坤⁴, 王爽⁴, 李楠⁵, 丁浩亮⁶, 胡伟杰¹, 肖宇⁷, 翁雅青⁴

作者信息

^1．江西理工大学，江西赣州 341000

^2．江西江钨浩运科技有限公司，南昌 330000

^3．江西森能新材料科技有限公司，江西宜春 336100

^4．江西省科学院，南昌 330095

^5．南昌航空大学，南昌 330063

^6．华东交通大学，南昌 330013

^7．东华理工大学，南昌 330013

通讯作者:

翁雅青（1985—），女，博士，副高级研究员。

作者简介:

李金辉（1978—），男，博士，教授。

Selective Extraction of Lithium from Spent Lithium-ion Batteries Based on an In-situ Reduction Roasting Process and Influence of Impurities

Jinhui LI¹, Quanbing REN², Guangwu LONG³, Fangkun DENG⁴, Shuang WANG⁴, Nan LI⁵, Haoliang DING⁶, Weijie HU¹, Yu XIAO⁷, Yaqing WENG⁴

Affiliations

^1.Jiangxi University of Science and Technology, Ganzhou 341000, Jiangxi, China

^2.Jiangxi Jiangwu Haoyun High-Tech Co., Ltd., Nanchang 330000, China

^3.Jiangxi Senneng New Materials Technology Co., Ltd., Yichun 336100, Jiangxi, China

^4.Jiangxi Academy of Sciences, Nanchang 330095, China

^5.Nanchang Hangkong University, Nanchang 330063, China

^6.East China Jiaotong University, Nanchang 330013, China

^7.East China University of Technology, Nanchang 330013, China

Corresponding Author:

WENG Yaqing (1985-), female, Ph.D., Associate Research Fellow. E-mail: wengyaqing@126.com

LI Jinhui (1978-), male, Ph.D., Professor. E-mail: jinhuili@jxust.edu.cn

出版时间: 2025-08-20 doi: 10.14062/j.issn.0454-5648.20250196

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摘要

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废旧锂离子电池不仅蕴含极高的有价金属资源，同时具备典型工业固废特征，针对传统湿法冶金工艺中存在的提锂流程长、锂元素损失、工序复杂等问题，以废旧锂离子电池正、负极混合料为原料，无须额外添加试剂，原位还原焙烧-水浸提锂工艺选择性提取锂。采用单因素实验确定最佳工艺条件，在焙烧温度600 ℃、焙烧时间30 min、搅拌时间4 h的条件下，Li的浸出率为72.23%，Ni、Co、Mn几乎不浸出，而不含杂质的商用纯三元废料（NCM）在相同条件下Li的浸出率达96.6%，Ni、Co、Mn几乎不浸出。

关键词

废旧锂离子电池 / 原位还原焙烧 / 水浸提锂 / 杂质

Abstract

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Introduction

To enhance the lithium leaching rate, carbon thermal reduction can be employed to convert lithium into lithium carbonate, thereby enabling selective recovery through water leaching. However, due to the relatively low solubility of lithium carbonate, it is challenging to significantly improve the efficiency of water leaching. Furthermore, the extent of carbon thermal reduction is highly dependent on factors such as the amount of added carbon source, reaction temperature, and reaction time. Consequently, there is an urgent need for advanced technologies that are characterized by low energy consumption, a simplified process, and high efficiency for the recovery of active cathode materials from spent lithium-ion batteries. While traditional metallurgical recovery processes can effectively extract most valuable metals from cathode waste, the current lithium extraction process typically requires multi-stage extraction or stepwise precipitation to produce lithium carbonate. This results in a lengthy back-end lithium extraction process, with intermediate steps prone to lithium metal loss, leading to a recovery rate of only 60% to 80%. In the context of comprehensive utilization recycling technologies, efficient lithium extraction and selective leaching of target elements remain bottleneck issues. To address the challenge of efficient lithium extraction, this study proposes the use of waste ternary positive and negative electrode mixed materials as raw materials, employing a process flow of "reduction roasting for priority lithium extraction" followed by water leaching and acid leaching to comprehensively recover valuable metals from the waste.

Methods

Weigh accurately an appropriate amount of experimental raw materials and transfer them into a mortar for thorough grinding. Subsequently, transfer the ground materials into a corundum crucible. Place the crucible containing the raw materials into a tube furnace for roasting. Prior to initiating the program, introduce argon gas at a flow rate of 200 mL/min for 30 min to ensure an inert atmosphere. Heat the materials at a controlled heating rate of 5 ℃/min until reaching the set temperature. Once the temperature naturally decreases to room temperature, carefully weigh the mass of the roasted product and record the mass difference before and after roasting. Transfer the roasted product into a beaker, add pure water at a liquid-to-solid ratio of 80 mL/g, and stir using a mechanical stirrer at a constant speed of 500 r/min. Systematically investigate the effects of roasting temperature (500-700 ℃), roasting time (30-150 min), and stirring time (water leaching time of 2-10 h) on the leaching rate of lithium. Calculate the mass differences of various elements based on the recorded mass differences of the roasted products before and after treatment, combined with the leaching efficiency.

Results and discussion

Using the positive and negative electrode mixtures from waste lithium-ion batteries as raw materials, lithium was selectively extracted via an in-situ reduction roasting-water leaching process without requiring additional reagents. Single-factor experiments were conducted to determine the optimal process conditions, which were identified as a roasting temperature of 600 ℃, a roasting time of 30 min, and a stirring time of 4 h. Under these conditions, the leaching rate of Li reached 72.23%, while Ni, Co, and Mn exhibited negligible leaching. The elemental contents before and after carbon-thermal reduction were quantitatively analyzed using SEM-EDS. In conjunction with ICP-OES detection results, it was determined that the raw materials contained impurities such as Al, F, and P. Carbon-thermal reduction reactions of commercial ternary cathode materials free of impurities were performed under identical conditions. The leaching rate of Li from the pure ternary material reached 96.6%, significantly higher than that achieved with impure materials (72.23%). Roasting products under various conditions were characterized by X-ray diffraction. It was observed that as the roasting temperature increased from 500 ℃ to 600 ℃, the characteristic peaks of NCM disappeared, indicating the complete destruction of the NCM (LiNi_xCo_yMn_1-_x_-_yO₂) crystal structure. The resulting roasting products primarily consisted of Li₂CO₃, Co, Ni, CoO, NiO, and unreacted graphite.

Conclusions

The optimal process were identified to be roasting temperature of 600 ℃, roasting duration of 30 min, and stirring time of 4 h, through single-factor experiments. The lithium leaching efficiency of 72.23% was achieved, while nickel, cobalt, and manganese exhibited negligible dissolution. Notably, under identical conditions, commercially sourced pure ternary cathode materials demonstrated significantly enhanced lithium recovery at 96.6%, maintaining minimal co-leaching of transition metals (<0.5%). To optimize the comprehensive lithium recovery efficiency in spent lithium-ion battery recycling, strategic introduction of additives capable of exerting synergistic reduction effects during the carbon thermal reduction stage is proposed. Subsequent research should focus on systematic evaluation of additive economics coupled with rigorous quantification of their lithium extraction enhancement potential.

Key words

spent lithium-ion batteries / in-situ reduction roasting / lithium extraction by water leaching / impurities

引用本文

李金辉, 任权兵, 龙光武, 邓方坤, 王爽, 李楠, 丁浩亮, 胡伟杰, 肖宇, 翁雅青. 废旧锂离子电池原位还原焙烧水浸提锂及杂质影响. 硅酸盐学报, 2025 , 53 (8) : 2109 -2114 . DOI: 10.14062/j.issn.0454-5648.20250196

Jinhui LI, Quanbing REN, Guangwu LONG, Fangkun DENG, Shuang WANG, Nan LI, Haoliang DING, Weijie HU, Yu XIAO, Yaqing WENG. Selective Extraction of Lithium from Spent Lithium-ion Batteries Based on an In-situ Reduction Roasting Process and Influence of Impurities[J]. Journal of the Chinese Ceramic Society, 2025 , 53 (8) : 2109 -2114 . DOI: 10.14062/j.issn.0454-5648.20250196

基金

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国家重点研发计划子课题(2023YFC3905904-03)
江西省科学院省级财政科研项目(2023YSBG22022)
国家自然科学基金项目(52064018)
江西省高等学校井冈学者特聘教授岗位资助

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2025年第53卷第8期

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文章信息

doi: 10.14062/j.issn.0454-5648.20250196

接收时间：2025-03-09
首发时间：2026-10-21
出版时间：2025-08-20

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出版历史

收稿日期：2025-03-09
修回日期：2025-03-23

基金

国家重点研发计划子课题(2023YFC3905904-03)

江西省科学院省级财政科研项目(2023YSBG22022)

国家自然科学基金项目(52064018)

江西省高等学校井冈学者特聘教授岗位资助

作者信息

^1．江西理工大学，江西赣州 341000

^2．江西江钨浩运科技有限公司，南昌 330000

^3．江西森能新材料科技有限公司，江西宜春 336100

^4．江西省科学院，南昌 330095

^5．南昌航空大学，南昌 330063

^6．华东交通大学，南昌 330013

^7．东华理工大学，南昌 330013

通讯作者:

翁雅青（1985—），女，博士，副高级研究员。

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https://castjournals.cast.org.cn/joweb/gsyxb/CN/10.14062/j.issn.0454-5648.20250196

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2种不同金属材料的力学参数

科 Family	属数 Number of genus	种数 Number of species	占总种数比例 Percentage of total species (%)	属 Genus	种数 Number of species	占总种数比例 Percentage of total species (%)
鹅膏菌科Amanitaceae	2	11	5.26	鹅膏菌属 Amanita	10	4.78
小菇科 Mycenaceae	2	12	5.74	丝盖伞属 Inocybe	5	2.39
多孔菌科 Polyporaceae	8	14	6.70	蜡蘑属 Laccaria	5	2.39
红菇科 Russulaceae	3	23	11.00	小皮伞属 Marasmius	6	2.87
				小菇属 Mycena	11	5.26
				光柄菇属 Pluteus	5	2.39
				红菇属 Russula	17	8.13
				栓菌属 Trametes	5	2.39

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