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Constructing atomic catalytic pair emerges as an attractive strategy to achieve better catalytic performance. Herein, an atomic Ir1─P1/NPG catalyst with asymmetric Ir─N2P1 sites that delivers superb activity and selectivity for hydrogenation of various functionalized nitrostyrene is reported. In the hydrogenation reaction of 3‐nitrostyrene, Ir1─P1/NPG (NPG refers to N, P‐codoped graphene) shows a...