First-principles study on screening diatomic catalysts for electrocatalytic NO reduction on single-layer BAs

Abstract

Electrocatalytic NO reduction reaction (NORR) technology can not only synthesize a highly significant chemical compound, NH 3 , but also provide a green and efficient method for removing the harmful NO gas. Based on density functional theory (DFT), diatomic catalysts (DACs) with TM 2 C 4 coordination environment were constructed on the surface of BAs in this work. The catalytic performance and reduction mechanism of NH 3 synthesis by NO reduction were calculated and screened in detail, and the formation mechanism of by-products under high concentration coverage and competitive reaction was compared. The results showed that Zn 2 C 4 @BAs exhibits excellent catalytic activity and high selectivity for NH 3 synthesis. Additionally, elementary reaction kinetics were investigated through microkinetic modeling.Furthermore, by studying the adsorption performance and activation degree of NO on the catalyst surface, the descriptor of NO activation degree was explored and predicted.It was found that the d-band center, the first ionization energy and the number of d electrons were strongly correlated with the parameters representing the activation degree of NO. This work provides a way to construct diatomic catalyst for NORR.