Active Sites and Mechanisms for Direct Oxidation of Benzene to Phenol over Carbon Catalysts

The direct oxidation of benzene to phenol with H2O2 as the oxidizer, which is regarded as an environmentally friendly process, can be efficiently catalyzed by carbon catalysts. However, the detailed roles of carbon catalysts, especially what is the active site, are still a topic of debate controvers...

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Bibliographic Details
Published in:Angewandte Chemie (International ed.) 2015-03, Vol.54 (13), p.4105-4109
Main Authors: Wen, Guodong, Wu, Shuchang, Li, Bo, Dai, Chunli, Su, Dang Sheng
Format: Article
Language:English
Subjects:
Benzene
Carbon
Catalysis
Catalysts
Defects
Hydrocarbons
model catalysts
Oxidation
Phenol
Phenols
Spectra
Spectrum analysis
static secondary ion mass spectroscopy
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Summary:The direct oxidation of benzene to phenol with H2O2 as the oxidizer, which is regarded as an environmentally friendly process, can be efficiently catalyzed by carbon catalysts. However, the detailed roles of carbon catalysts, especially what is the active site, are still a topic of debate controversy. Herein, we present a fundamental consideration of possible mechanisms for this oxidation reaction by using small molecular model catalysts, Raman spectra, static secondary ion mass spectroscopy (SIMS), DFT calculations, quasi in situ ATR‐IR and UV spectra. Our study indicates that the defects, being favorable for the formation of active oxygen species, are the active sites for this oxidation reaction. Furthermore, one type of active defect, namely the armchair configuration defect was successfully identified. Watching the defectives: Combining model catalysts with Raman spectra, secondary ion mass spectra, and quasi in situ ATR‐IR and UV spectra gives an insight into the mechanism of direct oxidation of benzene over carbon materials, such as carbon nanotubes. The defects in the armchair configuration (see picture) are capable of forming active oxygen species, and are the active sites.
ISSN:1433-7851
1521-3773
DOI:10.1002/anie.201410093