Tang Jie, Huang Bosi, Xiao Xiao, Qu Haotian, Song Ya, Li Junfeng, Song Yanze, Ji Haocheng, Wang Junxiong, Zhu Yanfei, Zhou Guangmin
Tsinghua Shenzhen International Graduate School, Tsinghua University, Shenzhen 518055, P. R. China.
J Am Chem Soc. 2025 Jul 16;147(28):24594-24603. doi: 10.1021/jacs.5c05384. Epub 2025 Jul 3.
Direct regeneration has emerged as a pioneering paradigm in green recycling of lithium-ion battery (LIBs) cathode materials, leveraging the inherent atomic and structural advantages of degraded materials. The solution-based regeneration strategy offers significant advantages, particularly in promoting homogeneous lithiation and mitigating the thermal instability of lithium iron phosphate (LFP) materials. However, lithium supplementation for degraded LFP (DLFP) in aqueous solutions is significantly constrained by the narrow electrochemical stability window (ESW) and the limited selection of redox agents. Herein, we propose a promising water-in-salt solution system that enables the spontaneous lithiation of DLFP. This approach not only expands the ESW of the solution but also modifies the lithium solvation structure, facilitating more efficient lithium supplementation. Using the lithium chloride-gallic acid solution as a demonstration, the regenerated cathode materials exhibit excellent electrochemical performance, achieving a specific capacity of 146 mAh g at 1 C with 83% capacity retention after 500 cycles. This research offers critical insights into solution-based lithium supplementation and paves the way for the more efficient recycling of degraded LIBs.
直接再生已成为锂离子电池（LIBs）正极材料绿色回收的一种开创性范例，它利用了降解材料固有的原子和结构优势。基于溶液的再生策略具有显著优势，特别是在促进均匀锂化和缓解磷酸铁锂（LFP）材料的热不稳定性方面。然而，在水溶液中对降解的LFP（DLFP）进行锂补充受到狭窄的电化学稳定性窗口（ESW）和氧化还原剂选择有限的显著限制。在此，我们提出了一种有前景的盐包水体系，该体系能够使DLFP自发锂化。这种方法不仅扩大了溶液的ESW，还改变了锂溶剂化结构，有助于更高效地进行锂补充。以氯化锂 - 没食子酸溶液为例，再生后的正极材料表现出优异的电化学性能，在1 C下比容量达到146 mAh g，500次循环后容量保持率为83%。本研究为基于溶液的锂补充提供了关键见解，并为更高效地回收降解的LIBs铺平了道路。
