Hydrogen Atom Abstraction by Heterogeneous-Homogeneous Hybrid Catalyst of CeO2and 2-Cyanopyridine via Redox of CeO2for C-H Bond Oxidation with Air

Masazumi Tamura, Eiji Sagawa, Akira Nakayama, Yoshinao Nakagawa, Keiichi Tomishige

Research output: Contribution to journalArticlepeer-review

Abstract

Hybrid catalysts composed of heterogeneous and homogeneous components are promising for obtaining unique catalysis and tuning and controlling the catalytic performance; however, the examples on the development and application of the hybrid catalysts are limited. Here, we present that the hybrid catalyst of CeO2 and 2-cyanopyridine can work as an H atom abstractor of C-H bonds in alkanes. The hybrid catalyst showed high activity for the oxidation of alkanes with air as an oxidant, providing high selectivity to the alcohols and ketones. The experimental studies and DFT calculations indicate that the N atom in the CN group of 2-cyanopyridine adsorbed on CeO2 can function like an N-radical center driven by the redox of CeO2. The H atom was abstracted by the N atom in the CN group, which is induced by the reduction of Ce4+ to Ce3+ in CeO2 via the electron transfer.

Original languageEnglish
Pages (from-to)11867-11872
Number of pages6
JournalACS Catalysis
DOIs
Publication statusAccepted/In press - 2021

Keywords

  • cerium oxide
  • hybrid catalyst
  • oxidation
  • radical
  • redox

ASJC Scopus subject areas

  • Catalysis
  • Chemistry(all)

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