Integrated Structural Modulation Inducing Fast Charge Transfer in Aqueous Zinc‐Ion Batteries

Abstract Aqueous Zn‐ion batteries (AZIBs) are promising energy‐storage devices owing to their exceptional safety, long cycle life, simple production, and high storage capacity. Manganese oxides are considered potential cathode materials for AZIBs, primarily because of their safety, low cost, simple synthesis, and high storage capacity. However, MnO₂‐based cathodes tend to deteriorate structurally during long‐term cycling, which reduces their reversible capacity. In this study, an advanced α‐MnO₂@SnO₂ nanocomposite via facile hydrothermal synthesis is developed. The synergistic effects of lattice disorder and increased electron conductivity in the α‐MnO₂@SnO₂ nanocomposite mitigate structural degradation and enhance the overall electrochemical performance. The nanocomposite exhibits a high reversible capacity of 347 mAh g⁻¹ at a current density of 100 mA g⁻¹ after 50 cycles. Furthermore, it exhibits excellent rate performance and stable capacity even after 1000 cycles, maintaining a capacity of 78 mAh g⁻¹ at a high current density of 5 A g⁻¹. This excellent electrochemical performance is attributed to the reversible Zn intercalation in α‐MnO₂@SnO₂ nanocomposites due to the increased structural stability and fast ion/electron exchange caused by the distortion of the tunnel structure, on the basis of various ex situ experiments, density functional theory calculations, and electrochemical characterizations.