Unravelling solvation structure and interfacial mechanism of pyrrolidinium-based ionic liquid electrolytes in potassium-ion batteries

Ionic liquid-based electrolytes (ILEs) show great potential in mitigating the dissolution of organic electrode materials as well as manipulating the interfacial electrochemistry for long lifespan of potassium-ion batteries (PIBs). Herein, KFSI/Pyr13FSI ILEs with varying K+ and Pyr13+ ratios were designed to match a novel organic K-storage anode of p-toluic acid/CMK3 (PTA/CMK3). These ILEs exhibited facilely manipulated solvation structures, resulting into excellent compatibility with K-metal as well as promotion of the generation of robust solid-electrolyte interphase (SEI) for stable K-storage. As a result, the optimized PTA/CMK3||KFSI/Pyr13FSI K-storage system delivered a reversible capacity of 190 mAh/g(composites) alongside high coulomb efficiency of 99.7 % at a current density of 200 mA/g for 600 cycles. This work provides a fresh insight on rational design of ILEs-based advanced PIBs with high energy density and safety.