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

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 Zn2+ ions was accelerated via the SO4 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 SO4 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 %).