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

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.

SUBMITTER: Zhang T 

PROVIDER: S-EPMC9668809 | biostudies-literature | 2022 Nov

REPOSITORIES: biostudies-literature