Brick‐Layer Templating of (002)‐Oriented Zn at Battery Anodes

ABSTRACT Aqueous zinc‐ion batteries (AZIBs) are promising candidates for future large‐scale energy storage because of their high safety and low cost. However, dendritic Zn growth at the anode severely compromises its long‐term cyclability and thus impedes practical deployment of AZIBs. From a crystallographic perspective, enforcing preferential Zn growth along the (002) orientation can effectively suppress dendrite formation, but most existing strategies rely on pre‐texturing of anodes or substantially altering the electrolyte composition, both of which add additional complexity and cost. In this regard, achieving robust (002)‐oriented Zn deposition on commercial Zn foil in a ZnSO 4 ‐dominated electrolyte remains crucial to the future development of AZIBs. Herein, we develop a new electrolyte additive, 2,4,6‐trimethoxy‐s‐triazine (TST), which functions at trace concentrations to enable (002)‐oriented Zn deposition at battery anodes. Via pre‐adsorption on the anode surface, TST promotes a hexagonally ordered Zn adlayer as an interfacial brick template, thereby enabling texture‐inherited (002) plating during subsequent electrodeposition. The proposed mechanism is corroborated through multi‐dimensional characterization, and the resulting Zn anodes deliver markedly improved cycling stability across multiple cell configurations. We believe this work can inspire future studies on crystallographic orientation engineering‐based Zn anode protection and can accelerate the practical implementation of AZIBs.