Recyclable Turing‐Structured Polymer Electrolytes for Sustainable Solid‐State Batteries

Abstract

Abstract Solid polymer electrolytes (SPEs) face critical limitations in ionic conductivity, ion transference numbers, and recyclability. We report a recyclable Turing‐structured polymer electrolyte (TPE) prepared at gas/liquid/solid interface through evaporation/diffusion‐driven instability. The Turing structure provides fast ion‐conduction surfaces/channels with periodic lithium (Li)‐ion (Li + ) self‐concentration domains to enable a 3D percolating Li + conduction, reducing migration barriers to achieve a high Li + conductivity (1.6 × 10 −3 S cm −1 at 25 °C) and transference number (0.61). TPEs enable stable cycling performance in various solid‐state batteries at low‐temperature conditions (−20 °C), alongside excellent self‐healing, flame‐retardant, and recyclable properties. Closed‐loop recycling recovers 86.5% of polymer precursors and 82.6% of costly Li bis(trifluoromethanesulfonyl)imide (LiTFSI) salt, with regenerated electrolytes retaining their initial performance. These results highlight the potential of Turing structure as a scalable design paradigm for sustainable and high‐performance energy storage and conversion systems.