Few-layer Mg-deficient borophene nanosheets: I2 oxidation and ultrasonic delamination from MgB2

Abstract

By using I₂ as an oxidant and CH₃CN as a reaction medium, few-layer Mg-deficient borophene nanosheets (FBN) with a stoichiometric ratio of Mg_0.22B₂ are prepared by oxidizing MgB₂ in a mixture of CH₃CN and HCl for 14 days under nitrogen protection and followed by ultrasonic delaminating in CH₃CN for 2 h. The prepared FBN possess a two-dimensional flake morphology, and they show a clear interference fringe with a d-spacing of 0.251 nm corresponding to the (208) plane of rhombohedral boron. While maintaining the hexagonal boron networks of MgB₂, the FBN have an average thickness of about 4.14 nm (four monolayer borophene) and a lateral dimension of 500 nm, and the maximum Mg deintercalation rate can reach 78%. The acidity of the reaction system plays an important role; the HCl reaction system not only facilitates the oxidation of MgB₂ by I₂, but also increases the deintercalation ratio of Mg atoms. Etching of the Mg atom layer with HCl, the negative charge decrease of the boron layer by I₂ oxidation, and the Mg chelating effect from CH₃COOH due to the hydrolysis of CH₃CN in an HCl environment led to a high deintercalation rate of the Mg atom. Density functional theory (DFT) calculations further support the result that the maximum deintercalation rate of Mg atoms is about 78% while maintaining the hexagonal layer structure of boron. This research solves the problems of low Mg atom deintercalation rate and hexagonal boron structure destruction when using the precursor MgB₂ to produce borophene nanosheets, which is of great significance for large-scale novel preparation and application of borophene nanosheets.