Interfacial Domino Effect Triggered by β‐Alanine Cations Realized Highly Reversible Zinc‐Metal Anodes

Abstract

Abstract Realizing durative dense, dendrite‐free, and no by‐product deposition configuration on Zn anodes is crucial to solving the short circuit and premature failure of batteries, which is simultaneously determined by the Zn interface chemistry, electro‐reduction kinetics, mass transfer process, and their interaction. Herein, this work unmasks a domino effect of the β‐alanine cations (Ala + ) within the hydrogel matrix, which effectively triggers the subsequent electrostatic shielding and beneficial knock‐on effects via the specifical adsorption earliest event on the Zn anode surface. The electrostatic shielding effect regulates the crystallographic energetic preference of Zn deposits and retards fast electro‐reduction kinetics, thereby steering stacked stockier block morphology and realizing crystallographic optimization. Meanwhile, the mass transfer rate of Zn 2+ ions was accelerated via the SO 4 2− anion immobilized caused by Ala + in bulk electrolyte, finally bringing the balance between electroreduction kinetics and mass transfer process, which enables dendrite‐free Zn deposition behavior. Concomitantly, the interfacial adsorbed Ala + cations facilitate the electrochemical reduction of interfacial SO 4 2− anions to form the inorganic‐organic hybrid solid electrolyte interphase layer. The above domino effects immensely improve the utilization efficiency of Zn anodes and long‐term stability, as demonstrated by the 12 times longer life of Zn||Zn cells (3650 h) and ultrahigh Coulombic efficiency (99.4 %).