单相梯度溶剂化电解稳定锂金属电池
近日,南京大学周豪慎团队报道了单相梯度溶剂化电解稳定锂金属电池。2026年7月8日,《自然》杂志发表了这一成果。
基于醚类电解液在锂金属电极方面已取得巨大成功。然而,在高电压全电池的充电过程中,溶剂和阴离子为容纳正极释放的锂离子而发生去溶剂化,这会加剧电解液的氧化分解。此外,在长时间循环中组分的持续消耗会显著改变溶剂化结构,导致氧化还原稳定性恶化。
研究组将一种靶向配体反溶剂(TLAS)引入富阴离子醚基电解液中。由于TLAS在静态下与Li+的缔合能力相对较弱,它几乎不参与锂离子的溶剂化。但在高电压全电池的强电场作用下,TLAS的取向和分布发生显著变化,其在正极表面的配位能力被激活。这种由TLAS介导的动态溶剂化行为绕过了传统电解液体系中溶剂和阴离子在正极上固有的去配位与再配位过程,从而最大限度地减少了电解液重构和界面劣化。
借助这种梯度溶剂化电解液,研究组研制出能量密度为450 Wh·kg-1的锂金属软包电池,实现了超过750次循环的长寿命(容量保持率80%)。此外还验证了能量密度高达605 Wh·kg-1的锂金属软包电池,该电池在150次循环后容量保持率达96%。这种梯度溶剂化策略为金属离子电池的电解液工程提供了一条可行路径。
附:英文原文
Title: Single-phase gradient-solvation-electrolyte-stabilized Li metal batteries
Author: Yang, Wujie, Cai, Jianfeng, Chen, Aoyuan, Li, Xiang, He, Ping, Zhou, Haoshen
Issue&Volume: 2026-07-08
Abstract: Ether-based electrolytes have shown great success for lithium metal electrodes1,2,3,4,5. However, during the charging process of high-voltage full cells, the desolvation of solvents and anions to accommodate Li ions released from the positive electrode exacerbates oxidative decomposition of the electrolyte6. In addition, the continuous consumption of components over extended cycling substantially alters the solvation structure, resulting in deteriorating redox stability. Here we incorporate a targeted ligand anti-solvent (TLAS) into an anion-rich ether-based electrolyte. The TLAS barely participates in the solvation of Li+ owing to its relatively weaker association ability in a static state. Under the strong electric field of high-voltage full cells, the orientation and distribution of the TLAS undergo substantial transformation, with coordination ability activated on the positive electrode surface. The TLAS-mediated dynamic solvation behaviour bypasses the inherent decoordination and recoordination of solvents and anions on the positive electrode in conventional electrolyte systems, thus minimizing electrolyte reconstruction and interphase deterioration. Leveraging this gradient solvation electrolyte, we develop a 450Whkg1 lithium metal pouch cell that achieves a long cycle life exceeding 750 cycles (80% capacity retention). Furthermore, we validated a lithium metal pouch cell with a high energy density of 605Whkg1, which achieves 150 cycles with 96% capacity retention. This gradient solvation strategy provides a feasible pathway of electrolyte engineering for metal-ion batteries.
DOI: 10.1038/s41586-026-10732-z
Source: https://www.nature.com/articles/s41586-026-10732-z
期刊信息
Nature:《自然》,创刊于1869年。隶属于施普林格·自然出版集团,最新IF:69.504
官方网址:http://www.nature.com/
投稿链接:http://www.nature.com/authors/submit_manuscript.html


