Activating the Intrinsic Zincophilicity of PAM Hydrogel to Stabilize the Metal‐Electrolyte Dynamic Interface for Stable and Long‐Life Zinc Metal Batteries

As a potential material to solve rampant dendrites and hydrogen evolution reaction (HER) problem of aqueous zinc metal batteries (AZMB), hydrogel electrolytes usually require additional additives or multi‐molecular network strategies to solve existing problems of ionic conductivity, mechanical properties and interface stability. However, the intrinsic zincophilic properties of the gel itself are widely neglected leading to the addition of additional molecules and the complexity of the preparation process. In this work, we innovatively utilize the characteristics of acrylamide‘s high zincophilic group density, activating the intrinsic zincophilic properties of PAM gel through a simple concentration control strategy which reconstructs a novel zinc‐electrolyte interface different from conventional PAM electrolyte. The activated novel gel electrolyte with intrinsic zincophilic properties has high ionic conductivity and effectively suppresses water activity, thereby inhibiting HER corrosion. Meanwhile, it induces uniform deposition of (002) crystal planes, leading to excellent deposition kinetics and long cycle life, thereby ensuring high interfacial stability. Compared with conventional PAM gel electrolytes, the activated zincophilic group‐rich hydrogel maintained excellent cycling stability (1 mA/cm2, 1 mAh/cm2) over 2250 hours; The Zn//MnO₂ coin cell using novel zincophilic group ‐rich hydrogel still retains a high specific capacity of more than 170 mAh/g at 0.5 A/g after 1000 cycles. We employ a high‐concentration activation strategy and a dual‐ion shielding effect to activate traditional PAM materials, leveraging their “intrinsic” zincophilic properties. This gel exhibits dynamic reconstruction of the metal‐electrolyte interface during electrochemical cycling, promoting uniform deposition of (002) crystal planes, which leads to excellent deposition kinetics and a highly durable deposition‐stripping process.