In this work, spin-polarized density functional theory calculations are conducted to evaluate the possible applicability of a single Si atom doped boron nitride graphyne-like nansoheet (Si@BN-yne) for reduction of nitrous oxide (N2O). The calculations show that Si-doping in BN graphene is energetically favorable, and the resulting Si@BN-yne is both dynamically and thermodynamically stable. According to our findings, N2O spontaneously dissociates when it interacts with the Si@BN-yne from its O site without the need for an energy barrier, releasing 2.89 eV of energy. The adsorption energy of CO molecule on the Si@BN-yne is less negative than that of N2O, implying that N2O will predominately occupy the catalyst surface. The CO + Oad reaction is used to remove the remaining oxygen atom (Oad) from the Si@BN-yne surface. The calculations show that the reaction proceeds through a low energy barrier of 0.05 eV, which is much lower than the previously reported catalysts. This demonstrates the high catalytic activity of Si@BN-yne nanosheet. Furthermore, the adsorption of H2O and O2 species on the Si@BN-yne nanosheet is investigated. The results show that the presence of these species has no effect on the catalytic activity of the Si@BN-yne for N2O reduction. These results show that the proposed novel Si@BN-yne catalyst can be regarded as an efficient material in the development of promising active catalysts for N2O elimination from the environment.
