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Transition metal single atom catalysts (SACs) with M 1 -N x  coordination configuration have shown outstanding activity and selectivity for hydrogenation of nitroarenes. Modulating the atomic coordination structure has emerged as a promising strategy to further improve the catalytic performance. Herein, we report an atomic Co 1 /NPC catalyst with unsymmetrical single Co 1 -N 3 P 1  sites that displays unprecedentedly high activity and chemoselectivity for hydrogenation of functionalized nitroarenes. Compared to the most popular Co 1 -N 4  coordination, the electron density of Co atom in Co 1 -N 3 P 1  is increased, which is more favorable for H 2  dissociation as verified by kinetic isotope effect and density functional theory calculation results. In nitrobenzene hydrogenation reaction, the as-synthesized Co 1 -N 3 P 1  SAC exhibits a turnover frequency of 6560 h −1 , which is 60-fold higher than that of Co 1 -N 4  SAC and one order of magnitude higher than the state-of-the-art M 1 -N x -C SACs in literatures. Furthermore, Co 1 -N 3 P 1  SAC shows superior selectivity (&gt;99%) toward many substituted nitroarenes with co-existence of other sensitive reducible groups. This work is an excellent example of relationship between catalytic performance and the coordination environment of SACs, and offers a potential practical catalyst for aromatic amine synthesis by hydrogenation of nitroarenes.

Unprecedentedly high activity and selectivity for hydrogenation of nitroarenes with single atomic Co1-N3P1 sites