Superlong cycle-life sodium-ion batteries supported by electrode/active material interaction and heteroatom doping:...

To achieve both the capacity and stability of metal sulfides simultaneously remains a significant challenge. In this study, we have synthesized the manganese-doped copper sulfide three-dimensional (3D) hollow flower-like sphere (M/CuS-NSC), encapsulated in a nitrogen and sulfur co-doped carbon. The hollow lamellae structure allows the rational self-aggregation process of numerous active surface area enlarged nanosheets, thereby enhancing electrochemical activity. The subsurface framework characterized by CSC bonds enhances the pseudo-capacitive properties. Furthermore, the transformation of sulfur and the isomerization of carbon contribute to the enhancement of sodium ion storage. The incorporation of Mn into CuS lattice increases the interplanar distance, providing additional space for the accommodation of sodium ions. Mn doping facilitates the localization of electrons near the Fermi level, thereby improving conductivity. Additionally, Cu foils coated with M/CuS-NSC-2 engage with the electrolyte and sulfur, initiating the reaction sequence through the formation of Cu₉S₈. Consequently, M/CuS-NSC-2 exhibits highly reversible capacities of 676.24 mAh g^-1 after 100 cycles at 0.1 A g^-1 and 511.52 mAh g^-1 after 10000 cycles at 10 A g^-1, with an average attenuation ratio of only 0.009 %. In this study, we propose an effective strategy that combines structural design with heteroatom doping, providing a novel approach to enhance the electrochemical performance of monometallic sulfide.