Amorphization-induced surface electronic states modulation of cobaltous oxide nanosheets for lithium-sulfur batteries

Lithium-sulfur batteries show great potential to achieve high-energy-density storage, but their long-term stability is still limited due to the shuttle effect caused by the dissolution of polysulfides into electrolyte. Herein, we report a strategy of significantly improving the polysulfides adsorption capability of cobaltous oxide by amorphization-induced surface electronic states modulation. The amorphous cobaltous oxide nanosheets as the cathode additives for lithium-sulfur batteries demonstrates the rate capability and cycling stability with an initial capacity of 1248.2 mAh g(-1) at 1C and a substantial capacity retention of 1037.3 mAh g(-1) after 500 cycles. X-ray absorption spectroscopy analysis reveal that the coordination structures and symmetry of ligand field around Co atoms of cobaltous oxide nanosheets are notably changed after amorphization. Moreover, DFT studies further indicate that amorphization-induced re-distribution of d orbital makes more electrons occupy high energy level, thereby resulting in a high binding energy with polysulfides for favorable adsorption. Regulating the adsorption behaviour of the polysulfide species is the key to achieving highly stable Li-S batteries. Here, the authors show that amorphization-induced redistribution of d orbitals enable CoO to be a favourable candidate for polysulfide adsorption and conversion.

Automated summary

Amorphization-induced surface electronic states modulation significantly improves the polysulfides adsorption capability of cobaltous oxide, leading to enhanced performance and cycling stability of lithium-sulfur batteries. Compared to crystalline materials, amorphous cobaltous oxide nanosheets demonstrate superior adsorption of polysulfides, making them a promising candidate for cathode additives in Li-S batteries.