A kinetic barrier modulated hollow nanobox MoSe2@CuS core–shell heterostructure for high-rate and durable Li–O2 batteries

Abstract

Li–O₂ batteries have emerged as promising contenders for advanced energy storage systems, leveraging their exceptionally high theoretical energy density. Nevertheless, their practical deployment is substantially hindered by rapid capacity degradation and restricted operational durability, primarily attributed to sluggish oxygen reaction kinetics. Here, to modulate kinetic barriers, we propose an approach synergizing structural and electronic advantages by integrating heterointerface engineering and hierarchical nano-structuring. A hollow nanobox MoSe₂@CuS core–shell heterostructure is developed as a bifunctional oxygen electrode. Such a heterostructure could induce a built-in electric field to modulate charge transfer dynamics and the hollow architecture could optimize triple-phase interfacial reactions. Leveraging the synergistic attributes of its components, the MoSe₂@CuS-based Li–O₂ battery achieves an excellent specific capacity of 16 000 mAh g⁻¹ at 100 mA g⁻¹. Moreover, it demonstrates remarkable cycling durability, sustaining high performance for over 190 cycles at 200 mA g⁻¹ with a restricted capacity of 600 mAh g⁻¹. Density functional theory (DFT) calculations further illustrate the lowered energy kinetic barrier for Li₂O₂ formation/decomposition induced by the MoSe₂@CuS core–shell heterostructure. This work pioneers a universal heterointerface engineering strategy through rational design of hierarchical hollow architectures, providing new insights for developing high-performance Li–O₂ battery cathodes.