Li+ Quasi-Grotthuss Topochemistry Transport Enables Direct Regeneration of Spent Lithium-Ion Battery Cathodes

IF 16.1 1区 化学 Q1 CHEMISTRY, MULTIDISCIPLINARY
Yujia He, Kai Jia, Zhihong Piao, Zhenjiang Cao, Mengtian Zhang, Pengfei Li, Zhichao Li, Zhiyuan Jiang, Guorui Yang, Huan Xi, Guangmin Zhou, Wei Tang, Zhiguo Qu, R. Vasant Kumar, Shujiang Ding, Kai Xi
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引用次数: 0

Abstract

Direct regeneration of spent lithium-ion batteries offers economic benefits and a reduced CO2 footprint. Surface prelithiation, particularly through the molten salt method, is critical in enhancing spent cathode repair during high-temperature annealing. However, the sluggish Li+ transport kinetics, which predominantly relies on thermally driven processes in the traditional molten salt methods, limit the prelithiation efficiency and regeneration of spent cathodes. Here, we introduce a special molecular configuration (benzoate) into molten salts that facilitates rapid Li+ transport to the surface of LiNi0.5Co0.2Mn0.3O2 (NCM) via a quasi-Grotthuss topochemistry mechanism. This approach effectively avoids the phase transitions that could adversely degrade the electrochemical performance due to insufficient lithiation during the repair process. Computational and experimental analyses reveal that the system enables fast Li+ migration through the topological hopping of benzoate in organic lithium salt, rather than relying solely on thermally driven diffusion, thereby significantly improving the prelithiation and repair efficiency of spent NCM cathodes. Benefiting from the quasi-Grotthuss Li+ topochemistry transport, the degraded structure and Li vacancies in the spent cathode are effectively eliminated, yieding the regenerated cathode with good cycling stability comparable to commercial counterparts. The proposed Li+ transport mechanism presents a promising route for the efficient and sustainable regeneration of spent cathodes.

Abstract Image

Li+准Grotthuss拓扑化学输运实现了废锂离子电池阴极的直接再生
废锂离子电池的直接再生提供了经济效益和减少二氧化碳足迹。表面预锂化,特别是通过熔盐法,是在高温退火过程中增强废阴极修复的关键。然而,在传统的熔盐方法中,缓慢的Li+传输动力学依赖于热驱动过程,限制了废阴极的预锂化效率和再生。在这里,我们将一种特殊的分子结构(苯甲酸盐)引入熔盐中,通过准Grotthuss拓扑化学机制,促进Li+快速传输到LiNi0.5Co0.2Mn0.3O2 (NCM)表面,有效避免了在修复过程中由于锂化程度不足而导致电化学性能下降的相变。计算和实验分析表明,该系统能够通过苯甲酸酯在有机锂盐中的拓扑跳变实现Li+的快速迁移,而不仅仅依赖于热驱动扩散,从而显著提高了废NCM阴极的预锂化和修复效率。得益于准Grotthuss Li+拓扑化学迁移,废阴极中的退化结构和Li空位被有效消除,再生阴极具有与商业阴极相当的良好循环稳定性。所提出的Li+输运机制为废阴极的高效再生提供了一条有希望的途径。
本文章由计算机程序翻译,如有差异,请以英文原文为准。
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来源期刊
CiteScore
26.60
自引率
6.60%
发文量
3549
审稿时长
1.5 months
期刊介绍: Angewandte Chemie, a journal of the German Chemical Society (GDCh), maintains a leading position among scholarly journals in general chemistry with an impressive Impact Factor of 16.6 (2022 Journal Citation Reports, Clarivate, 2023). Published weekly in a reader-friendly format, it features new articles almost every day. Established in 1887, Angewandte Chemie is a prominent chemistry journal, offering a dynamic blend of Review-type articles, Highlights, Communications, and Research Articles on a weekly basis, making it unique in the field.
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