Understanding Trade‐Off Between Zincophilicity and Hydrogen‐Evolution: Toward Ultra‐Stable Aqueous Zinc Metal Batteries

ABSTRACT The development of robust Zn anodes is often constrained by the thermodynamic trade‐off between zincophilicity and hydrogen evolution reaction (HER) suppression. Herein, this work proposes a facile one‐step pyrolysis strategy utilizing metal‐ion‐adsorbed metal organic framework (MOF) precursors to construct a series of Zn metal alloys encapsulated in nitrogen‐doped carbon foams (ZnM@NCF). Theoretical simulations and experimental verifications demonstrate that the ZnBi@NCF layer uniquely optimizes the trade‐off derived from the linear scaling relationship of charge transfer, achieving an optimal balance between strong Zn interactions for uniform deposition and minimized H interactions for HER suppression. Furthermore, the conductive N‐doped framework and rigid hydrophobic structure provide synergistic electrochemical regulation and physical protection. Consequently, the optimized ZnBi@NCF anode exhibits superior stability, sustaining over 3600 cycles at an ultrahigh current density of 80 mA cm −2 with a Coulombic efficiency of 99.9%. Symmetric cells exhibit filling‐type Zn deposition behavior and can withstand a deep discharge of 85.7%. This work elucidates the intrinsic competition in surface adsorption and provides a new avenue for the design of highly stable metal anodes in aqueous batteries.