High-throughput screening of a transition metal single-atom electrocatalyst for the CH3NO2 reduction reaction

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The hydrogenation reduction of nitro compounds involves the wide application of functional amines as important chemical intermediates in the fine chemical industry. However, the development of low-cost, mild reaction conditions and high-performance catalysts for the reduction of nitro compounds is challenging. In this study, the potential of electrocatalysts in which 26 transition metal atoms are anchored to the surface of N-doped graphene (TMN4@G) was explored to determine the mechanism of the electrocatalytic CH3NO2 reduction reaction (CNORR) via density functional theory. First, the stability of TMN4@G was evaluated to screen out the catalyst which is stable at 300 K via ab initio molecular dynamics. Second, the Gibbs free energy with all possible reaction pathways of the CNORR was calculated to search for high-performance catalysts. These results demonstrate that monodentate adsorbed CdN4@G, FeN4@G, CoN4@G and bidentate adsorbed MoN4@G exhibit excellent catalytic activity. The overpotential of MoN4@G is only 0.357 V. Finally, Finally, the role of central metal atom on the catalytic activity of single-atom catalysts in CNORR and the impact of hydrogen evolution reaction on the adsorption of CH3NO2 were further discussed. We hope that this theoretical simulation provides an effective scheme for the reduction of nitro compounds under mild conditions.