Popularizing Holistic High‐Index Crystal Plane via Nonepitaxial Electrodeposition Toward Hydrogen‐Embrittlement‐Relieved Zn Anode

Abstract Electrodeposition is promising to fabricate Zn electrodes affording nonepitaxial single‐crystal textures. Previous research endeavors focus on achieving Zn(002) faceted deposition, nevertheless, the popularization of a high‐index Zn plane with favorable electrochemical activity remains poorly explored. There also exists a deficiency in the assessment of the electrodeposited quality of Zn. Here, a straightforward strategy to address such concerns by cultivating predominant Zn(112) texture via a potentiostatic electrodeposition mode is reported. By precisely identifying the “limiting” conditions for electrodeposition, a striking balance between improved deposition quality, tailored deposition kinetics, and suppressed hydrogen evolution is found. (002) Faceted Zn electrode is shown that be indeed produced, yet the rampant hydrodynamic convection and hydrogen embrittlement issue under such “over‐limiting” preparation conditions pose challenges in the electrode lifespan. In contrast, an optimized deposition minimizes hydrodynamic disturbances and mitigates the hydrogen embrittlement effect, where the thus‐generated high‐index (112)‐textured Zn electrode manifests impressive deposition quality and demonstrates holistic cycling stability. The pouch cell by pairing a Zn_xV₂O₅ (ZnVO) cathode manages a reversible capacity of ≈130 mAh and a capacity retention of 98.42%. This study offers guidance for the development of dendrite‐free and hydrogen‐embrittlement‐relieved Zn anodes, unleashing the potential of high‐index plane textures for advanced Zn batteries.