Ultrathin Surface Coating of Nitrogen‐Doped Graphene Enables Stable Zinc Anodes for Aqueous Zinc‐Ion Batteries

Abstract Owing to the high volumetric capacity and low redox potential, zinc (Zn) metal is considered to be a remarkably prospective anode for aqueous Zn‐ion batteries (AZIBs). However, dendrite growth severely destabilizes the electrode/electrolyte interface, and accelerates the generation of side reactions, which eventually degrade the electrochemical performance. Here, an artificial interface film of nitrogen (N)‐doped graphene oxide (NGO) is one‐step synthesized by a Langmuir–Blodgett method to achieve a parallel and ultrathin interface modification layer (≈120 nm) on Zn foil. The directional deposition of Zn crystal in the (002) planes is revealed because of the parallel graphene layer and beneficial zincophilic‐traits of the N‐doped groups. Meanwhile, through the in situ differential electrochemical mass spectrometry and in situ Raman tests, the directional plating morphology of metallic Zn at the interface effectively suppresses the hydrogen evolution reactions and passivation. Consequently, the pouch cells pairing this new anode with LiMn 2 O 4 cathode maintain exceptional energy density (164 Wh kg −1 after 178 cycles) at a reasonable depth of discharge, 36%. This work provides an accessible synthesis method and in‐depth mechanistic analysis to accelerate the application of high‐specific‐energy AZIBs.