Bifunctional Dynamic Adaptive Interphase Reconfiguration for Zinc Deposition Modulation and Side Reaction Suppression in Aqueous Zinc Ion Batteries

Abstract

Dendrite growth and electrode/electrolyte interface side reactions in aqueous zinc-ion batteries (AZIBs) not only impair the battery lifetime but also pose serious safety concerns for the battery system, hindering its application in large-scale energy storage systems. Herein, by introducing positively charged chlorinated graphene quantum dot (Cl-GQD) additives into the electrolyte, a bifunctional dynamic adaptive interphase is proposed to achieve Zn deposition regulation and side reaction suppression in AZIBs. During the charging process, the positively charged Cl-GQDs are adsorbed onto the Zn surface, acting as an electrostatic shield layer that facilitates smooth Zn deposition. In addition, the relative hydrophobic properties of chlorinated groups also build a hydrophobic protective interface for the Zn anode, mitigating the corrosion of the Zn anode by water molecules. More importantly, the Cl-GQDs are not consumed throughout the cell operation and exhibit a dynamic reconfiguration behavior, which ensures the stability and sustainability of this dynamic adaptive interphase. Consequently, the cells mediated by the dynamic adaptive interphase enable dendrite-free Zn plating/stripping for more than 2000 h. Particularly, even at 45.5% depth of discharge, the modified Zn//LiMn₂O₄ hybrid cells still retain 86% capacity retention after 100 cycles, confirming the feasibility of this simple approach for application with limited Zn sources.