Tailoring the Solvation Sheath of Cations by Constructing Electrode Front‐Faces for Rechargeable Batteries

Abstract Solvent molecules within the solvation sheath of cations (e.g., Li⁺, Na⁺, Zn²⁺) are easily to be dehydrogenated especially when coupled with high‐voltage cathodes, and lead to detrimental electrolytes decompositions which finally accelerate capacity decays of rechargeable batteries. Tremendous efforts are devoted to tackle with this long‐lasting issue. Among them, salt‐concentrated strategies are frequently employed to tailor the solvation sheath of cations and improve the stabilities of electrolytes. However, the cost challenges caused by adding extra dose of expensive salts, additives/cosolvents in preparing highly concentrated electrolytes, hinder their further utilizations to some extent. Introducing porous materials‐based electrode front‐faces on the surface of electrodes even within dilute electrolytes can transfer the high‐energy‐state desolvated solvents from the reactive electrodes to the nonconductive porous material surfaces, thus eliminate the contact chances between desolvated solvents and electrode materials, and greatly reduce solvents‐related decomposition issues. Herein, recent advances in using electrode front‐faces to tailor the solvation sheath of metal ions for rechargeable batteries are discussed. Finally, perspectives to the future challenges and opportunities of constructing electrode front‐faces to tailor the solvation sheath of cations by constructing electrode front‐face for rechargeable batteries are provided.