Feng Qilin, Jiang Jiangmin, Li Shuang, Zhou Gaoyu, Kong Xiangkai, Chen Yaxin, Zhuang Quanchao, Ju Zhicheng
Jiangsu Province Engineering Laboratory of High Efficient Energy Storage Technology and Equipments, School of Materials Science and Physics, China University of Mining and Technology, Xuzhou, 221116, China.
Guangdong-Hong Kong-Macau Joint Laboratory for Photonic-Thermal-Electrical Energy Materials and Devices, Institute of Applied Physics and Materials Engineering, University of Macau, Macau, 999078, China.
Small. 2025 Mar;21(9):e2406506. doi: 10.1002/smll.202406506. Epub 2024 Sep 23.
Low-cost graphite has emerged as the most promising anode material for potassium-ion batteries (PIBs). Constructing the inorganic-rich solid electrolyte interface (SEI) on the surface of graphite anode is crucial for achieving superior electrochemical performance of PIBs. However, the compositions of SEI formed by conventional strongly solvating electrolytes are mainly organic, leading to the SEI structure being thick and causing the co-intercalation behavior of ions with the solvent. Herein, a weakly solvating electrolyte is applied to weaken the cation-solvent interaction and alter the cation solvation sheath structures, conducing to the inorganic composition derived from anions also participating in the formation of SEI, together with forming a uniformly shaped SEI with superior mechanical properties, and thus improving the overall performance of PIBs. The electrolyte solvation structure rich in aggregated ion pairs (AGGs) (69%) enables remarkable potassium-ion intercalation behavior at the graphite anode (reversible capacity of 269 mAh g) and highly stable plating/stripping of potassium metal anode (96.5%). As a practical device application, the assembled potassium-ion full-battery (PTCDA//Graphite) displays superior cycle stability. The optimizing strategy of cation solvation sheath structures offers a promising approach for developing high-performance electrolytes and beyond.
低成本石墨已成为钾离子电池(PIB)最有前景的负极材料。在石墨负极表面构建富含无机成分的固体电解质界面(SEI)对于实现PIB卓越的电化学性能至关重要。然而,传统强溶剂化电解质形成的SEI组成主要为有机成分,导致SEI结构较厚,并引发离子与溶剂的共嵌入行为。在此,采用弱溶剂化电解质来减弱阳离子 - 溶剂相互作用并改变阳离子溶剂化鞘层结构,有助于源自阴离子的无机成分也参与SEI的形成,同时形成具有优异机械性能的均匀形状的SEI,从而提高PIB的整体性能。富含聚集离子对(AGG)(69%)的电解质溶剂化结构使得在石墨负极处具有显著的钾离子嵌入行为(可逆容量为269 mAh g)以及钾金属负极高度稳定的镀/脱钾行为(96.5%)。作为实际的器件应用,组装的钾离子全电池(PTCDA//石墨)表现出优异的循环稳定性。阳离子溶剂化鞘层结构的优化策略为开发高性能电解质及其他方面提供了一种有前景的方法。