Upcycling spent lithium-ion battery cathodes into cobalt-polyphenol networks by DES dissolution and solvent-induced crystallization†

IF 9.3 1区化学 Q1 CHEMISTRY, MULTIDISCIPLINARY

Green Chemistry Pub Date : 2024-05-20 DOI:10.1039/d4gc01036a

Zeyu Wang , Yu Chen , Fengyi Zhou , Rui Qin , Yurun Tian , Zhimin Xue , Tiancheng Mu

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Abstract

The industrialization of the recycling of spent lithium-ion batteries presents promising opportunities and challenges. Herein, we developed a strategy of combining task-specific deep eutectic solvent (3,4,5-trihydroxybenzoic acid: choline chloride) dissolution and the following solvent-induced crystallization (SIC) for upcycling LiCoO₂ (LCO) battery cathodes into cobalt-polyphenol networks. It has been confirmed that protic solvents (ethylene glycol, methanol, ethanol, and H₂O) serve as effective inducing agents to achieve this strategy, playing a role in: (1) regulating the coordination environment of metal ions, initiating the self-assembly process with polyphenol anions and (2) provoking the precipitation of metal-polyphenol network particles (MPNPs) by altering the solubility. Comprehensive research indicated that when organic building blocks (phenolic acid, polyphenol compounds and their derivatives), Cl⁻, and inducing agents concurrently exist in the system, one-step conversion from LCO to MPNPs could be achieved. A tandem scheme is proposed based on the research for upcycling LCO into MPNPs, which are applied widely in separation, purification and catalysis. Experiments on ternary electrode materials demonstrated the robust generalizability of our strategy. This work provides valuable insights for the industrialization of spent LCO battery recycling and its transformation into novel materials.

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通过 DES 溶解和溶剂诱导结晶，将废旧锂离子电池正极升级再造为钴-多酚网络

废旧锂离子电池回收利用的产业化带来了大有可为的机遇和挑战。在此，我们开发了一种将特定任务的深共晶溶剂（3,4,5-三羟基苯甲酸：氯化胆碱）溶解和随后的溶剂诱导结晶（SIC）相结合的策略，用于将钴酸锂（LCO）电池正极升级回收为钴-多酚网络。研究证实，原生质溶剂（乙二醇、甲醇、乙醇和 H2O）是实现这一策略的有效诱导剂，在以下方面发挥作用：(1) 调节金属离子的配位环境，启动与多酚阴离子的自组装过程；(2) 通过改变溶解度促进金属-多酚网络颗粒（MPNPs）的沉淀。综合研究表明，当有机构建模块（酚酸、多酚化合物及其衍生物）、Cl- 和诱导剂同时存在于体系中时，可实现从 LCO 到 MPNPs 的一步转化。在此研究的基础上，提出了一种串联方案，用于将 LCO 向上循环转化为 MPNPs，MPNPs 广泛应用于分离、纯化和催化领域。三元电极材料的实验证明了我们的策略具有强大的通用性。这项工作为废旧 LCO 电池回收的工业化及其向新型材料的转化提供了宝贵的见解。

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来源期刊

Green Chemistry 化学-化学综合

CiteScore

16.10

自引率

7.10%

发文量

677

审稿时长

1.4 months

期刊介绍： Green Chemistry is a journal that provides a unique forum for the publication of innovative research on the development of alternative green and sustainable technologies. The scope of Green Chemistry is based on the definition proposed by Anastas and Warner (Green Chemistry: Theory and Practice, P T Anastas and J C Warner, Oxford University Press, Oxford, 1998), which defines green chemistry as the utilisation of a set of principles that reduces or eliminates the use or generation of hazardous substances in the design, manufacture and application of chemical products. Green Chemistry aims to reduce the environmental impact of the chemical enterprise by developing a technology base that is inherently non-toxic to living things and the environment. The journal welcomes submissions on all aspects of research relating to this endeavor and publishes original and significant cutting-edge research that is likely to be of wide general appeal. For a work to be published, it must present a significant advance in green chemistry, including a comparison with existing methods and a demonstration of advantages over those methods.