In Situ Nitrogen‐Rich Interphase Engineering Boosting Zn (002) Plane Texture with High Depth of Discharge for Long‐Term Zinc Metal Batteries

Abstract Due to uncontrollable interfacial reactions in aqueous electrolytes, zinc metal anodes typically suffer from severe dendrite growth and side reactions, significantly hindering the practical application of aqueous zinc metal batteries. Herein, a nitrogen‐rich interphase is in situ constructed on the surface of the zinc anode by incorporating tetraethylenepentamine (TEPA) into the electrolyte. The nitrogen‐rich interphase regulates interfacial charge via electrostatic shielding effect, enabling Zn 2 ⁺ to be guided by uniform electric fields during deposition. Meanwhile, the nitrogen‐rich groups coordinate with or electrostatically adsorb Zn 2+ , driving preferential deposition on the low‐surface‐energy (002) plane rather than high‐energy crystal planes (e.g., (100), (101)) and thereby suppressing the occurrence of disordered dendrites and side reactions. As a result, the Zn symmetric batteries with the nitrogen‐rich interphase exhibit excellent stability for over 340 h under a depth of discharge of 65.3%, and still achieve stable cycling for over 450 h at an ultrahigh current density of 63.0 mA cm −2 . Furthermore, the assembled Zn||NH 4 V 4 O 10 full batteries can retain 91.2% of initial capacity after 1000 cycles at 5 A g −1 . Such a finding provides valuable guidance for rationally designing interphases to address interfacial issues in long‐life zinc metal batteries.