Regulating electron configuration of single Cu sites via unsaturated N,O-coordination for selective oxidation of benzene.
basic_science · Level V
Where this comes from
- Record sourced from PubMed, PMID 36384968.
- Also identified by DOI 10.1038/s41467-022-34852-y and PMC identifier 9668809.
- Licence recorded as CC BY.
- The licence permits redistribution, so the abstract is shown in full and the full text is available from the publisher.
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.