Fortifying Zinc Metal Anodes against Uncontrollable Side‐Reactions and Dendrite Growth for Practical Aqueous Zinc Ion Batteries: A Novel Composition of Anti‐Corrosive and Zn2+ Regulating Artificial Protective Layer

Abstract Aqueous zinc‐ion batteries (AZIBs) have recently gained significant attention for grid‐scale energy storage applications owing to their high intrinsic energy density, low cost, and environmental benignity. Nevertheless, uncontrolled Zn dendrite accumulation, H 2 gas generation, and inevitable corrosion resulting from intricate water‐induced side‐reactions remain the main hurdles to AZIB commercialization. To overcome these problems, it is imperative to develop easy‐to‐handle strategies for the construction of versatile artificial protective layers (APL) on Zn surfaces. Inspired by the suppressed HER and anti‐corrosive properties of zinc silicate (Zn 2 SiO 4 ), this study rationally designed a novel APL consisting of Zn 2 SiO 4 nanospheres and decorated surface‐modified carbon nanotube (CNT) to produce a stable and durable Zn anode (C‐ZSL@Zn). The C‐ZSL layer simultaneously improved Zn 2+ transport kinetics and the Zn 2+ de‐solvation effect, maintained electrically insulating properties, and uniformized Zn 2+ flux on the Zn surface, synergistically enabling corrosion‐free and dendrite‐free Zn plating/stripping behavior on C‐ZSL@Zn. Consequently, the C‐ZSL@Zn achieved prolonged lifespans of ≈1600 (at 1 mA cm –2 ) and ≈1100 h (at a high depth of discharge of ≈51.24%) with ultralow voltage hysteresis in symmetric cells, together with improved cycling stability for coin‐ and pouch‐type Zn||α‐MnO 2 full‐cells. This study creates a new avenue for constructing stable APL@Zn anodes for practical applications.