Anti‐Fatigue Hydrogel Electrolyte for All‐Flexible Zn‐Ion Batteries

Abstract Hydrogel electrolytes are widely explored in Zn metal batteries for application in wearable electronics. While extensive studies have been conducted on optimizing the chemical structure and boosting the tensile elasticity, the mechanical stability of the hydrogel under repeated deformation is largely overlooked, leading to unsatisfactory performance at large cycling capacity. This work systematically analyzes the compressive fatigue‐resistance properties of the hydrogel electrolyte, revealing the critical roles of the salt and copolymer matrix on crack initiation and propagation. It shows that, on the premise of homogeneous Zn deposition, an improved anti‐fatigue property is essential to achieve high‐capacity Zn metal anodes. The optimal Zn(ClO₄)₂‐polyacrylamide/chitosan hydrogel electrolyte (C‐PAMCS) exhibits an unprecedented lifespan of 1500 h for Zn//Zn cells at a current density of 10 mA cm⁻² and a high areal capacity of 10 mAh cm⁻². The potential application of C‐PAMCS is exemplified in all‐flexible Zn‐ion batteries enabled by a flexible current collector consisting of a Ag nanowires embedded elastomer. This study provides the rationale under hydrogel electrolyte engineering toward advanced Zn‐ion battereis and the application in flexible devices.