In situ formation of a ZnS/In interphase for reversible Zn metal anodes at ultrahigh currents and capacities

Abstract

Aqueous zinc-ion batteries (AZIBs) have been considered next-generation promising high-energy storage systems due to their cost-effectiveness and high safety. Nevertheless, the instability of the Zn metal anode posed by dendrite growth and volume changes presents a significant hurdle for AZIB commercialization. Here, we introduce a novel approach using a ZnIn₂S₄ nanoflower-coated carbon cloth (ZISG-CC) with hierarchical spatial channels to guide the nucleation and deposition of Zn, thereby constructing a stable Zn metal anode. The designed ZISG-CC electrode exhibits distinctive features, including an enlarged surface area, enhanced zincophilicity, and in situ formation of a ZnS/In interphase during the initial discharge process. These characteristics facilitate uniform Zn nucleation and the formation of a stable electrolyte–anode interface, enabling excellent reversibility of the Zn anode. As a result, the Zn/ZISG-CC anode demonstrates outstanding charge–discharge cycling performance in a symmetric cell, achieving 550 cycles at 10 mA cm⁻²/5 mA h cm⁻² and 500 cycles at 20 mA cm⁻²/10 mA h cm⁻². Furthermore, the Zn/ZISG-CC|MnO₂-graphene full cell exhibits a high capacity retention of 87.5% after 1000 cycles at 1 A g⁻¹, along with favorable flexibility. This study introduces a novel strategy that utilizes the interaction between the electrode and electrolyte to stabilize the electrolyte–anode interface, enabling advanced Zn anodes in high-performance AZIBs.