Ion-Electron Diffusion Interphase Enables Fast Kinetics toward Dendrite-Free Zinc Metal Anodes

Abstract Aqueous zinc metal batteries are promising for safe and low-cost energy storages, but their practical operation is limited by unstable Zn/electrolyte interfacial reactions, sluggish Zn2+ transport, parasitic hydrogen evolution reaction (HER), and dendritic growth. Here, we report a strategy of constructing a dual-functional rapidly ion-accelerated versatile electron-regulating interphase on Zn metal anode (DRIVE@Zn) through a room-temperature immersion co-deposition process. Specifically, the Ag/Bi-derived DRIVE interphase regulates Zn2+ pathway, facilitates desolvation, homogenizes Zn2+ flux, and guides Zn deposition at the interface rather than on random exposed surface defects, which are verified by simulations and in situ electrochemical analyses. Consequently, DRIVE@Zn delivers an average Coulombic efficiency of 99.65%, stable Zn∥Zn cycling for over 3100 h at 5 mA cm–2, and durable Zn∥I2 full-cell lifespan for 25,000 cycles at 5 A g–1. This work highlights interphase-regulated Zn2+ pathway as an effective route toward long-cycling aqueous Zn metal anodes.