Regulation of desolvation process and dense electrocrystalization behavior for stable Zn metal anode

Aqueous zinc metal batteries are primarily limited due to the considerable risks of uncontrollable electrodepo-sition and side reactions at the anode/electrolyte interface (AEI). The de-solvation and initial nucleation behavior at AEI are critical for promoting stable Zn anode but lacks in-depth consideration in previous research. Herein, the internal connection between the interface characteristics, de-solvation process and electrodeposition behaviors is systematically revealed in a modified aqueous electrolyte with a trace amount of organic additive. The novel organic additives can effectively regulate the Zn2+ solvation structure and optimize the de-solvation procedure. The modified electrical double layer (EDL) structure decreases the interface capacitance, leading to the elevated nucleation overpotential and decreased interfacial tension, which can further promote the rapid formation of fine-nuclei and homogeneous stacked lamellar Zn deposition. Moreover, the active water molecules are forced away from the anode surface, inhibiting the decomposition behaviors and further H2O-derived by -reactions. This work provides a novel insight for understanding the interfacial reaction of high-stability zinc anode.