Interfacial Lattice Strain‐Induced Vacancy Evolution Facilitating Highly Reversible Dendrite‐Free Zinc Metal Anodes

Interfacial stress caused by semi‐coherent and incoherent interfaces during zinc (Zn) plating and its effect on subsequent Zn deposition are important considerations for designing electrode/electrolyte interfaces to improve the electrochemical performance of Zn anodes. Although some studies have paid attention to this issue, the influence of lattice strain induced by Zn ion diffusion in the interface coating on Zn deposition is infrequently discussed. Herein, a tin‐doped indium oxide (ITO) interfacial is constructed, and the evolution of interfacial lattice oxygen to vacancy oxygen (OV) induced by lattice stress generated by Zn ion migration in the interface during Zn deposition is confirmed. The formed OV‐rich ITO interface exhibits strong affinity and a low Zn ion diffusion barrier, accelerating the Zn ion transport kinetics. Meanwhile, the interface layer can appropriately capture anions in the electrolyte and improve the corrosion resistance of the electrode through the electrostatic repulsion effect. As a result, the OV‐rich ITO‐decorated Zn anode achieves stable Zn plating/stripping for more than 4500 h and delivers a high average Coulombic efficiency of 99.6% after 1400 cycles at 1.0 mA cm−2. This work provides a new horizon for the rational construction of the interface layer to achieve a highly reversible dendrite‐free Zn metal anode. Herein, the authors reveal the evolution of interfacial lattice oxygen to vacancy oxygen induced by lattice stress generated by Zn ion migration in a tin‐doped indium oxide interface. The formed vacancy‐rich interface‐modified Zn anode can achieve stable Zn plating/stripping for more than 4500 h and deliver a high average Coulombic efficiency of 99.6% after 1400 cycles.