Dynamically Reversible Gelation of Electrolyte for Efficient Wide‐Temperature Adaptable Energy Storage

Abstract Quasi‐solid‐state electrolytes (QSEs) via gelation of liquid electrolytes (LEs) are perspective protocols for constructing ingenious potassium‐ion batteries (PIBs) due to the combined advantages of both liquid and solid state. However, most of QSEs yet researched face a trade‐off among low temperature adaptability and safely high temperature operation. Herein, in situ reversible gelation of Ni‐crosslinked pentaerythritol tetrakis (3‐mercaptopropionate) (PETMP‐Ni) co‐polymerized with tyramine‐modified hyaluronic acid (HA‐Tyr) (PHA) modified B, N modified carbon spheres (BNC) enclosing by red P (RP) is backed with compatible electrode‐electrolyte interface with laponite filler (L). Such high reversible in situ gelation displays high low temperature adaptability by LEs, and extraordinary safety in high temperature steered by QSEs, benefiting from topologic space crowding effect (TSCE) and reverse trap of Ni single atoms (Ni SAs). This work enlightens the missing prospects in constructing reversible in situ sol–gel strategy coupled by topologic space crowding effect and reverse SAs trapping stimulate toward revival hybrid electrode for wide‐temperature adaptive batteries.