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| Identification of Pyrolytic Products and Strategies of Stepwise Recovery for Spent LiNixCoyMnzO2 Lithium-ion Batteries |
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Received:March 26, 2025
Published Online:May 30, 2025
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| View Full Text View/Add Comment Download reader |
| DOI：10.20237/j.issn.1007-7545.2025.06.001 |
| KeyWord:spent LiNixCoyMnzO2 batteries; pyrolysis; product identification; recycling |
| Author | Institution |
| CUN Zhigen |
中国科学院绿色过程与工程重点实验室，战略金属资源绿色循环利用国家工程研究中心，中国科学院 过程工程研究所，北京;中国科学院大学 化学工程学院，北京 ; |
| LI Huiquan |
中国科学院绿色过程与工程重点实验室，战略金属资源绿色循环利用国家工程研究中心，中国科学院 过程工程研究所，北京;中国科学院大学 化学工程学院，北京 ; |
| XING Peng |
中国科学院绿色过程与工程重点实验室，战略金属资源绿色循环利用国家工程研究中心，中国科学院 过程工程研究所，北京;中国科学院大学 化学工程学院，北京 ; |
| DAI Yu |
湖南顶立科技股份有限公司，长沙 ; |
| WANG Chenye |
中国科学院绿色过程与工程重点实验室，战略金属资源绿色循环利用国家工程研究中心，中国科学院 过程工程研究所，北京;中国科学院大学 化学工程学院，北京 ; |
| WANG Haibei |
矿冶科技集团有限公司，北京 ; |
| KE Yanchun |
中国资源循环集团有限公司，天津 |
| ZHOU Qiang |
湖南顶立科技股份有限公司，长沙 ; |
| WANG Xingrui |
中国科学院绿色过程与工程重点实验室，战略金属资源绿色循环利用国家工程研究中心，中国科学院 过程工程研究所，北京;中国科学院大学 化学工程学院，北京 ; |
| WANG Yanyan |
湖南顶立科技股份有限公司，长沙 ; |
| ZHOU Pengfei |
中国资源循环集团有限公司，天津 |
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| Abstract: |
| Lithium-ion batteries offer several advantages, including high operating voltage, high energy density, fast charge and discharge rates, excellent cycle stability, and lightweight design. These attributes make them widely used in electronic devices, electric vehicles, and other applications. LiNixCoyMnzO2 lithium-ion battery (NCM LIB) are particularly favored for their higher theoretical energy density, gaining significant market attention. However, the layered structure of the NCM cathode material is inherently unstable, causing battery performance to degrade after repeated charge-discharge cycles. Moreover, spent NCM LIB contain valuable strategic metals such as nickel, cobalt, and lithium, as well as organic components like separators, electrolytes, and binders. Improper disposal of these materials results in a resource wastage and an environmental pollution. This study focuses on the combination of various components of spent NCM LIB, examining the composition of pyrolytic products during the pyrolysis process. The research reveals the compositional patterns of pyrolytic products derived from the thermal decomposition of different battery components. Based on the analysis of the composition and distribution of these pyrolysis products, a pretreatment and recovery strategy for spent NCM LIB was proposed, facilitating the recovery of both organic and inorganic materials within the battery cell. The main conclusions are as follows: During the pyrolysis process, organic matter volatilizes or decomposes, with the electrolyte having a relatively low volatilization temperature, ranging from 150 °C to 200 °C. As the pyrolysis temperature is increased to 450 °C, the electrolyte, separator, and binder undergo bond cleavage, cracking, and recombination. This results in the formation of the first long-chain hydrocarbons, alcohols, and esters, such as C4H8O3, C11H22, C17H34, and C10H22O, which exist in the form of pyrolysis oil. These long-chain organic compounds undergo further pyrolysis, producing small molecular gases such as CO2, CH4, C2H6, C2H2, and C3H6. As a result, the pyrolysis gas acquires the ability to reduce the cathode material. The inorganic substances in the battery are present in the pyrolysis residue. During the pyrolysis process, the cracking of the binder facilitates the dissociation of the electrode materials, enabling the separation of the black powder from the Cu-Al current collector. Multi-component pyrolysis enhances the reduction of the cathode materials, which can be attributed to the reductive pyrolysis gases. Among these, the pyrolysis products of the separator play a key role in the reduction reaction. A recycling strategy for spent NCM LIB based on pyrolysis technology was developed to achieve the stepwise recovery of all battery components. The electrolyte is regenerated through low-temperature volatilization and condensation. At elevated temperatures, the separator and binder decompose into long-chain hydrocarbons and alcohols, which exist as pyrolysis oil and can be utilized as fuel for energy supply. These long-chain hydrocarbons and alcohols are further decomposed into small molecular reductive pyrolysis gases. Copper and aluminum powders, as well as black powder, can be obtained by separating the resulting pyrolysis residue. Additionally, nickel, cobalt, manganese, and lithium chemicals can be extracted through wet separation processes such as acid leaching and extraction, without the need for reducing agents. This study presents a novel approach for the pyrolysis and mass recovery of ternary lithium batteries. |
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