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Methanol Oxidation on a Copper Catalyst Investigated Using in Situ X-ray Photoelectron Spectroscopy Full article

Общее Language: Английский, Genre: Full article,
Status: Published, Source type: Original
Journal The Journal of Physical Chemistry B
ISSN: 1520-6106 , E-ISSN: 1520-5207
Output data Year: 2004, Volume: 108, Number: 38, Pages: 14340-14347 Pages count : 8 DOI: 10.1021/jp040080j
Authors Bluhm Hendrik 1 , Hävecker Michael 1 , Knop-Gericke Axel 1 , Kleimenov Evgueni 1 , Schlögl Robert 1 , Teschner Detre 2 , Bukhtiyarov Valerii I. 3 , Ogletree D.Frank 4 , Salmeron Miquel 4
Affiliations
1 Abteilung Anorganische Chemie, Fritz-Haber-Institut der Max-Planck-Gesellschaft, Faradayweg 4-6, D-14195 Berlin, Germany
2 Institute of Isotope & Surface Chemistry, CRC, Hungarian Academy of Sciences, P.O. Box 77, Budapest, H-1525 Hungary
3 Boreskov Institute of Catalysis, 6300090 Novosibirsk, Russia
4 Materials Sciences DiVision, Lawrence Berkeley National Laboratory, One Cyclotron Road, Berkeley, California 94720

Funding (2)

1 United States Department of Energy DE-AC03-76SF00098
2 German Research Foundation Schl. 332/4-1

Abstract: The surface and near-surface regions of an active catalyst and the adjacent gas-phase reactants were investigated simultaneously under reaction conditions using in situ X-ray photoelectron spectroscopy (XPS). This investigation of methanol oxidation on a copper catalyst showed that there was a linear correlation between the catalytic activity of the sample and the presence of a subsurface oxygen species that can only be observed in situ. The concentration profile of the subsurface oxygen species within the first few nanometers below the surface was determined using photon-energy-dependent depth-profiling. The chemical composition of the surface and the near-surface regions varied strongly with the oxygen-to-methanol ratio in the reactant stream. The experiments show that the pure metal is not an active catalyst for the methanol oxidation reaction, but that a certain amount of oxygen has to be present in the subsurface region to activate the catalytic reaction. Oxide formation was found to be detrimental to formaldehyde production. Our results demonstrate also that for an understanding of heterogeneous catalysts a characterization of the surface alone may not be sufficient, and that subsurface characterization is essential.
Cite: Bluhm H. , Hävecker M. , Knop-Gericke A. , Kleimenov E. , Schlögl R. , Teschner D. , Bukhtiyarov V.I. , Ogletree D.F. , Salmeron M.
Methanol Oxidation on a Copper Catalyst Investigated Using in Situ X-ray Photoelectron Spectroscopy
The Journal of Physical Chemistry B. 2004. V.108. N38. P.14340-14347. DOI: 10.1021/jp040080j publication_identifier_short.wos_identifier_type publication_identifier_short.scopus_identifier_type publication_identifier_short.rinz_identifier_type
Files: Full text from publisher
Dates:
Submitted: Jan 28, 2004
Accepted: Mar 25, 2004
Published online: May 14, 2004
Published print: Sep 1, 2004
Identifiers:
publication_identifier.wos_identifier_type WOS:000223922500018
publication_identifier.scopus_identifier_type 2-s2.0-4944266771
publication_identifier.rinz_identifier_type 13460171
publication_identifier.accession_number_identifier_type 2004:390665
publication_identifier.chemical_accession_number_identifier_type 141:190414
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