Disordered Structure and Reversible Phase Transformation from K-Birnessite to Zn-Buserite Enable High-Performance Aqueous Zinc-Ion Batteries

Abstract

The layered δ-MnO₂ (dMO) is an excellent cathode material for rechargeable aqueous zinc-ion batteries owing to its large interlayer distance (~0.7 nm), high capacity, and low cost; however, such cathodes suffer from structural degradation during the long-term cycling process, leading to capacity fading. In this study, a Co-doped dMO composite with reduced graphene oxide (GC-dMO) is developed using a simple cost-effective hydrothermal method. The degree of disorderness increases owing to the hetero-atom doping and graphene oxide composites. It is demonstrated that layered dMO and GC-dMO undergo a structural transition from K-birnessite to the Zn-buserite phase upon the first discharge, which enhances the intercalation of Zn²⁺ ions, H₂O molecules in the layered structure. The GC-dMO cathode exhibits an excellent capacity of 302 mAh g⁻¹ at a current density of 100 mA g⁻¹ after 100 cycles as compared with the dMO cathode (159 mAh g⁻¹). The excellent electrochemical performance of the GC-dMO cathode owing to Co-doping and graphene oxide sheets enhances the interlayer gap and disorderness, and maintains structural stability, which facilitates the easy reverse intercalation and de-intercalation of Zn²⁺ ions and H₂O molecules. Therefore, GC-dMO is a promising cathode material for large-scale aqueous ZIBs.

Keywords

aqueous zinc-ion batteries / birnessite / buserite / disordered structure / phase transformation

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