Molecular Adsorption-Induced Interfacial Solvation Regulation to Stabilize Graphite Anode in Ethylene Carbonate-Free Electrolytes

Abstract

Many organic solvents have excellent solution properties, but fail to serve as lithium-ion batteries (LIBs) electrolyte solvents, due to their electrochemical incompatibility with graphite anodes. Herein, a new strategy is proposed to address this issue by introducing a surface-adsorbed molecular layer to regulate the interfacial solvation structure without the alteration of electrolyte composition and properties. As a proof-of-concept study, it is demonstrated for the first time that the intrinsically incompatible propylene carbonate (PC)-based electrolyte becomes completely compatible with graphite anodes by introducing a layer of adsorbed hexafluorobenzene (HFB) molecules to weaken the Li+-PC coordination strength and facilitate the interfacial desolvation process. As a consequence, the graphite/ NCM811 pouch cells using the PC-based electrolyte containing only 1 vol.% HFB demonstrate excellent long-term cycling stabilities over 1150 cycles. This strategy is also proved to be applicable to other ethylene carbonate (EC)–free electrolytes, thus providing a new avenue for developing advanced LIB electrolytes.