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  The Impact of the Bulk Structure on Surface Dynamics of Complex Mo–V-based Oxide Catalysts

Trunschke, A., Noack, J., Trojanov, S., Girgsdies, F., Lunkenbein, T., Pfeifer, V., et al. (2017). The Impact of the Bulk Structure on Surface Dynamics of Complex Mo–V-based Oxide Catalysts. ACS Catalysis, 7(4), 3061-3071. doi:10.1021/acscatal.7b00130.

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Trunschke, Annette1, Author              
Noack, Johannes1, 2, Author              
Trojanov, Sergej3, Author
Girgsdies, Frank1, Author              
Lunkenbein, Thomas1, Author              
Pfeifer, Verena1, 4, Author              
Hävecker, Michael1, 5, Author              
Kube, Pierre1, Author              
Sprung, Christoph1, Author              
Rosowski, Frank6, Author
Schlögl, Robert1, Author              
Affiliations:
1Inorganic Chemistry, Fritz Haber Institute, Max Planck Society, ou_24023              
2UniCat-BASF Joint Lab, Technische Universität Berlin, Sekr. EW K 01, Hardenbergstraße 36, 10623 Berlin, Germany, ou_persistent22              
3Humboldt-Universität zu Berlin, Institut für Chemie, Brook-Taylor-Straße 2, 12489 Berlin, Germany, ou_persistent22              
4Catalysis for Energy, Group EM-GKAT, Helmholtz-Zentrum Berlin für Materialien und Energie GmbH, Elektronenspeicherring BESSY II, Albert-Einstein-Straße 15, 12489 Berlin, Germany, ou_persistent22              
5Department of Heterogeneous Reactions, Max-Planck-Institut für Chemische Energiekonversion, Stiftstraße 34-36, 45470 Mülheim a. d. Ruhr, Germany, ou_persistent22              
6BASF SE, Process Research and Chemical Engineering, Heterogeneous Catalysis, Carl-Bosch-Straße 38, 67056 Ludwigshafen, Germany, ou_persistent22              

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Free keywords: acrylic acid, M1 structure, MoV, near-ambient-pressure X-ray photoelectron spectroscopy, propane, selective oxidation, single crystal analysis, Te
 Abstract: Mixed oxides composed of the four metals Mo, V, Te, and Nb are known to be efficient catalysts in selective oxidation of lower alkanes. The outstanding catalytic performance of such mixed oxides is attributed to the presence of the so-called M1 crystal phase that contains all four elements in the metal positions of the structure. In the present work, an M1 phase composed only of Mo and V has been prepared by hydrothermal synthesis. High crystallinity was achieved by applying a synthesis temperature of 200 °C. The phase-pure mixed MoV oxide was studied as catalyst in the oxidation of propane. In contrast to previous reports, the desirable oxidation product acrylic acid is formed over the Te-free M1 structure in significant amounts, implying that Te is not necessarily required as a component of the active ensemble responsible for selective oxygen insertion. The MoV M1 oxide is, however, less selective compared to that of the M1 structure composed of the four metals Mo, V, Te, and Nb. The reason has been determined by applying a combination of synchrotron-based single crystal structure analysis and near-ambient-pressure X-ray photoelectron spectroscopy. Determination of the crystal structure of MoV M1 oxide reveals partial occupation of sites in the hexagonal channels of the M1 structure by V, which are occupied by Te in MoVTeNb M1 oxide. Hydrolysis of the M-O bonds (M = V, Te) under reaction conditions leads to migration of the metal in the hexagonal channels to the surface. Accumulation of more than 50 at % V on the surface of the MoV M1 oxide most likely causes postcombustion of formed acrylic acid, whereas enrichment of Te at the surface of MoVTeNb M1 oxide results in dilution of surface V5+ species and, consequently, high selectivity.

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Language(s): eng - English
 Dates: 2017-03-132017-01-132017-04-07
 Publication Status: Published online
 Pages: -
 Publishing info: -
 Table of Contents: -
 Rev. Type: Peer
 Identifiers: DOI: 10.1021/acscatal.7b00130
 Degree: -

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Title: ACS Catalysis
  Abbreviation : ACS Catal.
Source Genre: Journal
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Publ. Info: Washington, DC : ACS
Pages: 11 Volume / Issue: 7 (4) Sequence Number: - Start / End Page: 3061 - 3071 Identifier: Other: 2155-5435
CoNE: https://pure.mpg.de/cone/journals/resource/2155-5435