Role of oxygen vacancy inducer for graphene in graphene-containing anodes

Abstract

Currently, graphene is only considered as a conductive additive and expansion inhibitor in oxides/graphene composite anodes. In this study, a new graphene role (oxygen vacancy inducer) in graphene/oxides composites anodes, which are treated at high-temperature, is proposed and verified using experiments and density functional theory calculations. During high-temperature processing, graphene forms carbon vacancies due to increased thermal vibration, and the carbon vacancies capture oxygen atoms, facilitating the formation of oxygen vacancies in oxides. Moreover, the induced oxygen vacancy concentrations can be regulated by sintering temperatures, and the behavior is unaffected by oxide crystal structures (crystalline and amorphous) and morphology (size and shape). According to density functional theory calculations and electrochemical measurements, the oxygen vacancies enhance the lithium-ion storage performance. The findings can result in a better understanding of graphene’s roles in graphene/oxide composite anodes, and provide a new method for designing high-performance oxide anodes.

Key words： oxide; oxygen vacancy; graphene; anode; density functional theory calculation

Acknowledgments

The authors thank the supply of CASTEP code from Analytical & Testing Center of Sichuan University. The authors would like to thank Shiyanjia Lab for the support of XPS tests.

Electronic Supplementary Material

Supplementary material is available in the online version of this article at https://dx.doi.org/10.1007/s11705-022-2213-8 and is accessible for authorized users.

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