Single non-noble metal atom doped C2N catalysts for chemoselective hydrogenation of 3-nitrostyrene

Improving the reaction selectivity and activity for challenging substrates such as nitroaromatics bearing two reducible functional groups is important in industry, yet remains a great challenge using traditional metal nanoparticle based catalysts. In this study, single metal atom doped M-C2N catalysts were theoretically screened for selective hydrogenation of 3-nitrostyrene to 3-vinylaniline with H-2 as the H-source. Among 20 M-C2N catalysts, the non-noble Mn-C2N catalyst was found to have excellent reaction selectivity. Importantly, due to the solid frustrated Lewis pair sites in the pores of Mn-C2N, a low H-2 activation energy is achieved on high-spin Mn-C2N and the rate-determining step for the hydrogenation reactions is the H diffusion from the metal site to the N site. The unraveled mechanism of the hydrogenation of 3-nitrostyrene using Mn-C2N enriches the applications of Mn based catalysts and demonstrates its excellent properties for catalyzing the challenging hydrogenation reaction of substrates with two reducible functional groups.

Automated summary

The study found that using single metal atom doped M-C2N catalysts, especially the non-noble Mn-C2N catalyst, can effectively improve the selective hydrogenation reaction of nitroaromatics, and by utilizing solid frustrated Lewis pair sites, a low H-2 activation energy is achieved on high-spin Mn-C2N, making the diffusion of hydrogen from the metal site to the N site the rate-determining step for the reaction.