Theoretical Modelling of the Surface Oxidation of a Silicon Carbide Nanopowder, Based on the v(SiH) Frequency Evolution

Abstract

AbstractDue to hydrolysis by atmospheric water, the first atomic layer of silicon carbide contains oxygen atoms. The oxygen content on the surface dramatically increases for nanosized SiC powder and strongly affects the overall properties. The presence of SiH groups on the SiC surface, already proven by Fourier transform infrared spectrometry, can be used to investigate the oxidation mechanism. Indeed, the v(SiH) stretching frequency known to strongly depend on the surrounding electronegativity of the silicon atom is directly related to the oxidation degree. Based on our infrared spectroscopic experimental data, ab initio calculations were performed on models representing the SiH surface species in different environments. Using the Hartree-Fock method with 3–21G and 6–31G basis sets, the v(SiH) frequencies were calculated for each model versus the number of substituted oxygen atoms. The comparison with the experimental values led to a discussion of our proposed models and of the SiC surface oxidation mechanism.