2. Academic Validation
  3. Atomically Dispersed Cu Catalyst for Efficient Chemoselective Hydrogenation Reaction

Atomically Dispersed Cu Catalyst for Efficient Chemoselective Hydrogenation Reaction

  • Nano Lett. 2021 Dec 22;21(24):10284-10291. doi: 10.1021/acs.nanolett.1c03381.
Hu Liu 1 2,  Xuexiang Li 3,  Zhenhui Ma 4,  Mingzi Sun 5,  Menggang Li 2,  Zhenyu Zhang 6,  Liang Zhang 1,  Zuobin Tang 1,  Yao Yao 1 6,  Bolong Huang 5,  Shaojun Guo 2
Affiliations

Affiliations

  • 1 School of Chemistry and Chemical Engineering, Xi'an University of Architecture and Technology, Xi'an 710055, China.
  • 2 School of Materials Science and Engineering, Peking University, Beijing 100871, China.
  • 3 School of Chemistry and Chemical Engineering, Northwestern Polytechnical University, Xi'an, 710072, P.R. China.
  • 4 Department of Physics, Beijing Technology and Business University, 100048, Beijing, China.
  • 5 Department of Applied Biology and Chemical Technology, The Hong Kong Polytechnic University, Hung Hom, Kowloon, Hong Kong SAR.
  • 6 School of Civil Engineering, Xi'an University of Architecture and Technology, Xi'an 710055, China.
PMID: 34882416 DOI: 10.1021/acs.nanolett.1c03381
Abstract

The Cu-based nanocatalysts have shown a high selectivity toward selective hydrogenation reaction, but the underlying catalytic mechanism is still murky. Herein, we report a new gram-scale strategy for realizing the single atom Cu site incorporated into the melem ring of graphitic carbon nitride (Cu1/CN) for understanding the catalytic mechanism of a hydrogenation reaction. The as-synthesized Cu1/CN exhibits unprecedented selectivity (100%), high activity (TOF = 2.9 × 103 h-1), and outstanding stability for selective hydrogenation of 4-nitrostyrene. We reveal that the presence of hydroxymethyl from trimethylolmelamine is beneficial to atomically disperse Cu atoms in the CN. X-ray absorption fine structure tests reveal that the Cu atom of Cu1/CN is dominated by the quaternary coordination way (Cu-N4) in the melem ring of CN. Density functional theory calculations confirm that the high reactivity and selectivity originate from the anchored Cu sites creating the optimal chemical environment for the highly efficient hydrogenation reaction.

Keywords

chemoselective hydrogenation reaction; hydrogenation mechanism; nitrostyrene; single-atom Cu.

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