A Reversible Zinc Metal Anode with an Inorganic/Organic Solid Electrolyte Interphase Enriched for Epitaxial Deposition Along the Zn (101) Plane

Aqueous zinc-metal batteries (AZMBs) have triggered extensive attention by virtue of their intrinsic safety and high theoretical capacity. However, the unstable electrode/electrolyte interface hinders its further industrialization. Herein, chelating additive (GLDA-4Na) is incorporated into 2M ZnSO₄ electrolyte to prolong Zn anode lifespan. Theoretical calculations and experimental results show that GLDA-4Na additive can induce a robust solid electrolyte interphase (SEI) to stabilize zinc anodes. Meanwhile, its multiple COO^- polar groups can act as solvation sites to coordinate with Zn²⁺, reducing the H₂O molecules in the Zn²⁺ solvation sheaths. Finally, GLDA anions exhibit strong adsorption on the Zn(101) crystal plane, inducing preferential Zn deposition along the (101) plane. Such synergistic regulation constructs a Zn²⁺-rich and H₂O-poor Helmholtz plane to regulate Zn deposition chemistry. As a result, the Zn anode can deliver an ultralong cycle life of over 5500 h at 8 mA cm^-2. Even under extreme conditions (-10 °C), the Zn anodes are still able to cycle stably for over 2800 h at 0.5 mA cm^-2. Furthermore, the NH₄V₄O₁₀||Zn full cells with GLDA-4Na exhibit a capacity retention of 84.47% after 1260 cycles at 4.66 A g^-1. This work presents a simple, viable approach to a stable Zn anode for high-performance AZMBs.