Engineering atomically dispersed single Cu-N3 catalytic sites for highly selective oxidation of benzene to phenol

Yitao Zhao, Haoran Xing, Qiang Wang, Yinjuan Chen, Jiawei Xia, Hui Xu, Guangyu He, Fengxiang Yin, Qun Chen, Haiqun Chen

Research output: Contribution to journalArticlepeer-review

2 Scopus citations

Abstract

Developing efficient approaches for selective oxidation of arene C-H bonds has been a challenging goal. Here we report a facile and practical strategy to fabricate an N-doped reduced graphene oxide (NRGO) based single-atom Cu catalyst (SACu-NRGO) by calcinating dicyandiamide (DCDA) and graphene oxide (GO) wrapped with Cu mesh for the selective oxidation of benzene to phenol at room temperature. According to extended X-ray absorption fine structure (EXAFS) and X-ray absorption near edge structure (XANES) analyses and density functional theory (DFT) calculations, single atomic Cu is anchored by three adjacent pyrrolic N atoms to form CuN3 active sites in the NRGO skeleton, which originates from the gaseous Cu(NH3)n generated via the reaction between Cu mesh and the ammonia pyrolyzed from DCDA. The SACu-NRGO exhibits excellent catalytic performance towards oxidation of benzene with the selectivity of phenol up to 98.6%, owing to the large specific surface area, fully exposed and homogeneously dispersed CuN3 active sites, as well as the coordination effect between Cu and N species. Furthermore, the structure of the single-atom active sites and the mechanism of the oxidation process are elucidated in depth by DFT calculations.

Original languageEnglish
JournalInorganic Chemistry Frontiers
DOIs
StateAccepted/In press - 1 Jan 2022
Externally publishedYes

ASJC Scopus subject areas

  • Inorganic Chemistry

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