Selective Activation of Methane on Single-Atom Catalyst of Rhodium Dispersed on Zirconia for Direct Conversion

Cited 22 time in webofscience Cited 0 time in scopus
  • Hit : 119
  • Download : 0
Direct methane conversion into value-added products has become increasingly important. Because of inertness of methane, cleaving the first C–H bond has been very difficult, requiring high reaction temperature on the heterogeneous catalysts. Once the first C–H bond becomes activated, the remaining C–H bonds are successively dissociated on the metal surface, hindering the direct methane conversion into chemicals. Here, a single-atom Rh catalyst dispersed on ZrO2 surface has been synthesized and used for selective activation of methane. The Rh single atomic nature was confirmed by extended X-ray fine structure analysis, electron microscopy images, and diffuse reflectance infrared Fourier transform spectroscopy. A model of the single-atom Rh/ZrO2 catalyst was constructed by density functional theory calculations, and it was shown that CH3 intermediates can be energetically stabilized on the single-atom catalyst. The direct conversion of methane was performed using H2O2 in the aqueous solution or using O2 in gas phase as oxidants. Whereas Rh nanoparticles produced CO2 only, the single-atom Rh catalyst produced methanol in aqueous phase or ethane in gas phase.
Publisher
AMER CHEMICAL SOC
Issue Date
2017-12
Language
English
Article Type
Article
Keywords

H BOND ACTIVATION; SUPPORTED RHODIUM; HYDROGEN-PEROXIDE; OXIDATION-STATE; MORDENITE; PLATINUM; OXYGEN; MODEL; DEHYDROGENATION; NANOPARTICLES

Citation

JOURNAL OF THE AMERICAN CHEMICAL SOCIETY, v.139, no.48, pp.17694 - 17699

ISSN
0002-7863
DOI
10.1021/jacs.7b11010
URI
http://hdl.handle.net/10203/238801
Appears in Collection
CBE-Journal Papers(저널논문)
Files in This Item
There are no files associated with this item.
This item is cited by other documents in WoS
⊙ Detail Information in WoSⓡ Click to see webofscience_button
⊙ Cited 22 items in WoS Click to see citing articles in records_button

qr_code

  • mendeley

    citeulike


rss_1.0 rss_2.0 atom_1.0