Interface‐Dominated Zn²⁺ Storage in Hydrogen‐Bonding Interfaces

Abstract Interface storage is an exciting mechanism for electrode materials to obtain high‐energy and high‐power densities simultaneously. However, constructing suitable and abundant interfaces in composites to achieve interface‐dominated storage is greatly challenging. Here, it is demonstrated for the first time that interface‐dominated Zn²⁺ storage can be realized in the hydrogen‐bonding (H‐bonding) interface between vanadium oxide (VO_x) and graphene oxide (GO). This interface featuring reversibility, universality, self‐healing nature, and high per‐volume concentration can store more Zn²⁺ faster than the bulk by decoupling transport and storage of Zn²⁺ and electrons through reversible break/reconstruction of the interfacial N···H─O bonds. Density functional theory calculations reveal that an appropriate number of N···H─O bonds is crucial for maintaining high reversibility of interface storage. Additionally, the presence of carbon vacancies in the GO plane near the interfacial bonds facilitates an expansion of the interface storage limitation. Finally, it is demonstrated that intercalation pseudocapacitance is the nature of interface storage, which circumvents the solid‐state diffusion limitation in the bulk and achieves a high level of pseudocapacitive storage in the interface (464 and 126 mAh g⁻¹ at 0.1 and 10.0 A g⁻¹, respectively). This work establishes an excellent paradigm for implementing interface‐dominated Zn²⁺ storage in H‐bonding interfaces and demonstrates exceptional universality and broad application prospects.