The detrimental parasitic reactions and uncontrolled deposition behavior derived from inherently unstable interface have largely impeded the practical application of aqueous zinc batteries. So far, tremendous efforts have been devoted to tailoring interfaces, while stabilization of grain boundaries has received less attention. Here, we demonstrate that preferential distribution of intermetallic compounds at grain boundaries via an alloying strategy can substantially suppress intergranular corrosion. In-depth morphology analysis reveals their thermodynamic stability, ensuring sustainable potency. Furthermore, the hybrid nucleation and growth mode resulting from reduced Gibbs free energy contributes to the spatially uniform distribution of Zn nuclei, promoting the dense Zn deposition. These integrated merits enable a high Zn reversibility of 99.85% for over 4000 cycles, steady charge-discharge at 10 mA cm⁻², and impressive cyclability for roughly 3500 cycles in Zn-Ti//NH₄V₄O₁₀ full cell. Notably, the multi-layer pouch cell of 34 mAh maintains stable cycling for 500 cycles. This work highlights a fundamental understanding of microstructure and motivates the precise tuning of grain boundary characteristics to achieve highly reversible Zn anodes.

固有不稳定界面产生的有害寄生反应和不受控制的沉积行为在很大程度上阻碍了水系锌电池的实际应用。到目前为止，人们在界面的定制方面付出了巨大的努力，而晶界的稳定却受到较少的关注。在这里，我们证明通过合金化策略金属间化合物在晶界的优先分布可以显着抑制晶间腐蚀。深入的形态分析揭示了它们的热力学稳定性，确保了可持续的效力。此外，吉布斯自由能降低导致的混合成核和生长模式有助于锌核的空间均匀分布，促进致密的锌沉积。这些综合优点使得Zn-Ti//NH ₄ V ₄ O ₁₀全电池在超过4000次循环中具有99.85%的高Zn可逆性、在10 mA cm ^-2下稳定的充放电以及在大约3500次循环中令人印象深刻的循环能力。值得注意的是，34 mAh 的多层软包电池在 500 次循环后仍能保持稳定的循环。这项工作强调了对微观结构的基本理解，并促进了晶界特性的精确调节，以实现高度可逆的锌阳极。