Stabilizing Anode‐Electrolyte Interface for Dendrite‐Free Zn‐Ion Batteries Through Orientational Plating with Zinc Aspartate Additive

Abstract The stability of aqueous Zn‐ion batteries (AZIBs) is detrimentally influenced by the formation of Zn dendrites and the occurrence of parasitic side reactions at the Zn metal anode (ZMA)‐electrolyte interface. The strategic manipulation of the preferential crystal orientation during Zn 2+ plating serves as an essential approach to mitigate this issue. Here, Zn aspartate (Zn‐Asp), an electrolyte additive for AZIBs, is introduced not only to optimize the solvation structure of Zn 2+ , but also to crucially promote preferential Zn 2+ plating on the (002) crystal plane of ZMA. As a result, both side reactions and Zn dendrites are effectively inhibited, ensuring an anode surface free of both dendrites and by‐products. The implementation of Zn‐Asp leads to significant enhancements in both Zn||Zn symmetric and Zn||Ti batteries, which demonstrate robust cyclability of over 3200 h and high Coulombic efficiency of 99.29%, respectively. Additionally, the Zn||NaV 3 O 8 ·1.5H 2 O full battery exhibits remarkable rate capability, realizing a high capacity of 240.77 mA h g −1 at 5 A g −1 , and retains 92.7% of its initial capacity after 1000 cycles. This research underscores the vital role of electrolyte additives in regulating the preferential crystal orientation of ZMA, thereby contributing to the development of high‐performing AZIBs.