Density Functional Theory Study of Low-Dimensional (2D, 1D, 0D) Boron Nitride Nanomaterials Catalyzing Acetylene Acetate Reaction

Abstract

In this paper, density functional theory (DFT) was used to study the possibility of low-dimensional (2D, 1D, 0D) boron nitride nanomaterials to catalyze acetylene acetate reaction, and further explore the possible source of this catalytic activity. It is found that the catalytic activity of boron nitride nanomaterials for acetylene acetate reaction will change with the change of the geometric structure (dimension) and reaction site of the catalyst. From the geometric structure, the reaction components and the zero-dimensional BN catalyst can form chemical bonds and form complexes, while only physical adsorption occurs on the surface of the one-dimensional and two-dimensional BN catalysts. From the reaction site, the properties of different C sites on the B12N12NC-C2H2 complexes are different. Namely, a C atom connected with a B atom is more likely to have an electrophilic reaction with H+, and a C atom connected with an N atom is more likely to have a nucleophilic reaction with CH3COO−. Through the study of three kinds of BN nanomaterials with low dimensions, we found that the zero-dimensional B12N12 nanocage broke the inherent reaction inertia of BN materials and showed good catalytic activity in an acetylene acetate reaction, which is very likely to be a non-metallic catalyst for the acetylene gas-phase preparation of vinyl acetate.