Engineering Hierarchical CoO Nanospheres Wrapped by Graphene via Controllable Sulfur Doping for Superior Li Ion Storage

The inferior conductivity and large volume expansion impair the widespread applications of metal oxide-based anode materials for lithium-ion batteries. To address these issues, herein an efficient strategy of structural engineering is proposed to improve lithium storage performance of hierarchical CoO nanospheres wrapped by graphene via controllable S-doping (CoOS_0.1 @ G). S-doping promotes the Li⁺ diffusion kinetics of CoO by expanding the interplanar spacing of CoO, lowering the activation energy, and improving the pseudocapacitance contribution. Meanwhile, the electronic structure of CoO is adjusted by S-doping as confirmed by density functional theory calculations, thus enhancing the conductivity. Finite element analysis reveals that the produced Li₂ S during lithiation improves the structural stability of the S-doped electrode, which is further confirmed by experimental observation. As expected, CoOS_0.1 @ G exhibits excellent lithium storage performance with an initial discharge capacity of 1974 mAh g^-1 at 100 mA g^-1 , and high discharge capacity of 1573 mAh g^-1 after 400 cycles at 500 mA g^-1 . It is believed that the insights into the structural doping enlighten research to explore other metal oxides for fast and stable Li ion storage.