V‐O‐Ru Heterogeneous Interphase Reversible Reconstruction Endowing Zn0.85V10O24·7.4H2O/0.65RuO2 Cathode Robust H+/Zn2+ Storage

Abstract Intercalation‐type layered vanadium oxides have been widely explored as cathode materials for aqueous zinc–ion batteries (AZIBs). However, attaining both high power density and superior stability remains a formidable challenge. Herein, layered vanadium oxides are pre‐intercalated with Zn 2+ to form Zn 0.85 V 10 O 24 ·7.4H 2 O (ZVO), which is then combined with RuO 2 nanoparticles to construct a ZVO/RuO 2 heterostructure featuring interphase V─O─Ru bonds. ZVO/RuO 2 heterostructure exhibits a dynamic stable coupling at the interphase via V─O─Ru chemical bonds reconstruction during discharging/charging processes. The dynamically reversible reconstruction of interphase V─O─Ru bonds provides a fast electron transfer channel between RuO 2 and ZVO cathode, as demonstrated by ex situ X‐ray photoelectron spectroscopy (XPS) and density functional theory (DFT) calculations, making RuO 2 an additional electron acceptor and donor, and accelerating the migration of H + /Zn 2+ in layered ZVO cathode. Therefore, an ultra‐high capacity (411 mAh g −1 at 0.5 A g −1 , 225 mAh g −1 at 20 A g −1 ) and long cycling stability (a retention of 92.2% at 20 A g −1 over 20000 cycles) performances are achieved. This interphase reversible reconstruction route provides a promising approach to achieving excellent cycling stability in cathode materials.