A HER‐Inhibiting Layer Based on M‐H Bond Regulation for Achieving Stable Zinc Anodes in Aqueous Zinc‐Ion Batteries

Abstract A hydrogen evolution reaction (HER) Strategy is developed through material design to address the persistent challenge of the HER at the zinc anode. Unlike previous strategies, first‐principles calculations are used to screen the low‐coordinated Nb₂C MXene as the inhibitory medium. By taking advantage of the dual merits of its high |Δ G *H | (1.03 eV) and excellent structural stability, the HER‐Inhibiting layer Nb₂C@Znp is designed, which demonstrates the following key advancements: I) The onset potential for hydrogen evolution of 1.97 V (vs Zn 2 ⁺/Zn) is achieved, representing a positive shift of 0.51 V compared with the bare zinc anode; II) It shows excellent cycling stability, being able to maintain for 2000 h at a current density of 2 mA cm⁻ 2 and for 700 h at a current density of 10 mA cm⁻ 2 . III) The simultaneous inhibition of the hydrogen evolution reaction and the mitigation of dendrite growth are achieved through the regulation of the interfacial electron structure. Mechanistic studies indicate that the Nb₂C matrix weakens the bond energy of the M‐H bond, and at the same time creates preferential migration channels for Zn 2 ⁺, achieving a synergistic effect of inhibiting hydrogen adsorption and homogenizing zinc deposition, which greatly improves the CE and cycling stability.