Inhibiting Interfacial Electron Leakage via An Artificial Rectified Layer for Longevous Zinc Metal Anodes

Dendrites and water‐induced side reactions impose greatly challenge on the implementation of aqueous zinc ion batteries. To tackle these problems, an artificial rectified layer (ARL) with hydrophobic, zincophilic and insulating features was in‐situ synthesized on Zn surface rapidly to prevent the electron leakage from Zn anode to aqueous electrolyte, which is the underlying logic for uneven Zn deposition and parasitic side reactions. The ARL also displays a high Zn2+ transference number of 0.71 and can build fast Zn2+ transport channels to homogenize the interfacial ion flux and electric field according to the calculated work function and multi‐physics phase simulation results. Therefore, the Zn anode with ARL shows preferred plating along with (002) crystal facet and an admirable Coulombic efficiency of 99.86% over 3200 cycles. Zn symmetric cells can withstand large current density up to 40 mA cm‐2 and operate stably at 44.2% depth of discharge for 250 hours, surpassing most of published reports. The ARL also enables the Zn||MnO2 full batteries to circulate over 2600 cycles with a high‐capacity retention of 80.1% and low self‐discharge at 1 A g‐1. This work provides a different perspective to comprehend and design satisfactory solid electrolyte interphase for Zn metal anodes.