Room-Temperature Chemoselective Hydrogenation of Nitroarene Over Atomic Metal-Nonmetal Catalytic Pair

作者：Ding, Jie; Li, Fuhua; Zhang, Jincheng; Qi, Haifeng; Wei, Zhiming; Su, Chenliang; Yang, Hong Bin^*; Zhai, Yueming^*; Liu, Bin^*

来源：Advanced Materials, 2023.

DOI：10.1002/adma.202306480

• atomically dispersed
• catalytic pairs
• heterogeneous catalysis
• hydrogenation
• nitrostyrene

Constructing atomic catalytic pair emerges as an attractive strategy to achieve better catalytic performance. Herein, an atomic Ir1P1/NPG catalyst with asymmetric IrN2P1 sites that delivers superb activity and selectivity for hydrogenation of various functionalized nitrostyrene is reported. In the hydrogenation reaction of 3-nitrostyrene, Ir1P1/NPG (NPG refers to N, P-codoped graphene) shows a turnover frequency of 1197 h-1, while the reaction cannot occur over Ir1/NG (NG refers to N-doped graphene). Compared to Ir1/NG, the charge density of the Ir site in Ir1P1/NPG is greatly elevated, which is conducive to H2 dissociation. Moreover, as revealed by density functional theory calculations and poisoning experiments, the P site in Ir1P1/NPG is found able to bind nitrostyrene, while the neighboring Ir site provides H to reduce the nitro group in chemoselective hydrogenation of nitrostyrene. This work offers a successful example of establishing atomic catalytic pair for driving important chemical reactions, paving the way for the development of more advanced catalysts to further improve the catalytic performance. @@@ An atomic Ir1P1/NPG catalyst with asymmetric Ir1N2P1 sites is designed, delivering superb activity and selectivity for the hydrogenation of nitroarene. Revealed by density functional theory calculations and poisoning experiments, the P site in Ir1P1/NPG is found able to bind nitroarene, while the neighboring Ir site activates H2 to provide H to reduce the nitro group in chemoselective hydrogenation of nitroarene.image

• 单位
  武汉大学