Chemically Copolymerized P( AM ‐co‐ AA )/Zn 2+ Gel Electrolyte for High‐Stability Aqueous Zinc‐Ion Batteries

ABSTRACT Hydrogel electrolytes offer promising solutions to Zn anode challenges in aqueous zinc‐ion batteries (AZIBs), combining electrochemical stability, mechanical strength, and structural tunability to address dendritic growth and parasitic reactions. This study presents a novel strategy involving chemical copolymerization to fabricate a dual‐network P(AM‐co‐AA)/Zn 2+ hydrogel electrolyte through the rational molecular design of acrylamide (AM) and acrylic acid (AA) polymer matrices. The chemically crosslinked dual‐network architecture not only endows the hydrogel with remarkable mechanical resilience (demonstrating a 980% strain and 0.77 MPa stress tolerance) but also facilitates precise ion regulation through strategically immobilized carboxylate (COO − ) functional groups. These structural features synergistically establish ordered ion transport channels that promote uniform Zn 2+ flux distribution, achieving an elevated Zn 2+ transference number of 0.60 while effectively suppressing both dendritic growth and parasitic reactions. The quasi–solid‐state AZIBs incorporating this hydrogel electrolyte exhibit exceptional cycling stability and reversibility. Specifically, the Zn//Zn cell demonstrates stable cycling for over 800 h, while the Zn//Cu cell maintains a coulombic efficiency close to 100%. Additionally, the Zn//MnO 2 cell retains a high capacity of 148.5 mAh g −1 after 500 cycles at a current density of 0.1 A g −1 .