Regulating electron configuration of single Cu sites via unsaturated N,O-coordination for selective oxidation of benzene

Ting Zhang, Zhe Sun, Shiyan Li, Baojun Wang, Yuefeng Liu (), Riguang Zhang () and Zhongkui Zhao ()
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Ting Zhang: Dalian University of Technology
Zhe Sun: Dalian University of Technology
Shiyan Li: Chinese Academy of Science
Baojun Wang: Taiyuan University of Technology
Yuefeng Liu: Chinese Academy of Science
Riguang Zhang: Taiyuan University of Technology
Zhongkui Zhao: Dalian University of Technology

Nature Communications, 2022, vol. 13, issue 1, 1-8

Abstract: Abstract Developing highly efficient catalyst for selective oxidation of benzene to phenol (SOBP) with low H2O2 consumption is highly desirable for practical application, but challenge remains. Herein, we report unique single-atom Cu1-N1O2 coordination-structure on N/C material (Cu-N1O2 SA/CN), prepared by water molecule-mediated pre-assembly-pyrolysis method, can efficiently boost SOBP reaction at a 2:1 of low H2O2/benzene molar ratio, showing 83.7% of high benzene conversion with 98.1% of phenol selectivity. The Cu1-N1O2 sites can provide a preponderant reaction pathway for SOBP reaction with less steps and lower energy barrier. As a result, it shows an unexpectedly higher turnover frequency (435 h−1) than that of Cu1-N2 (190 h−1), Cu1-N3 (90 h−1) and Cu nanoparticle (58 h−1) catalysts, respectively. This work provides a facile and efficient method for regulating the electron configuration of single-atom catalyst and generates a highly active and selective non-precious metal catalyst for industrial production of phenol through selective oxidation of benzene.

Date: 2022
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DOI: 10.1038/s41467-022-34852-y

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