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  How Strain Affects the Reactivity of Surface Metal Oxide Catalysts

Amakawa, K., Sun, L., Guo, C., Hävecker, M., Kube, P., Wachs, I. E., et al. (2013). How Strain Affects the Reactivity of Surface Metal Oxide Catalysts. Angewandte Chemie International Edition, 52(51), 13553-13557. doi:10.1002/anie.201306620.

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 Creators:
Amakawa, Kazuhiko1, Author           
Sun, Lili1, Author           
Guo, Chunsheng1, Author           
Hävecker, Michael1, 2, Author           
Kube, Pierre1, Author           
Wachs, Israel E.3, Author
Lwin, Soe3, Author
Frenkel, Anatoly I.4, Author
Patlolla, Anitha4, Author
Hermann, Klaus1, Author           
Schlögl, Robert1, Author           
Trunschke, Annette1, Author           
Affiliations:
1Inorganic Chemistry, Fritz Haber Institute, Max Planck Society, ou_24023              
2Helmholtz-Zentrum Berlin fuer Materialien und Energy GmbH, Division Solar Energy Research, Elektronenspeicherring BESSY II, ou_persistent22              
3Operando Molecular Spectroscopy & Catalysis Laboratory Department of Chemical Engineering Lehigh University, Bethlehem, Pennsylvania 18015 (USA), ou_persistent22              
4Department of Physics Yeshiva University, 245 Lexington Avenue, New York, NY 10016 (USA), ou_persistent22              

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Free keywords: heterogeneous catalysis; molybdenum; olefin metathesis; oxidation; supported catalysts
 Abstract: Highly dispersed molybdenum oxide supported on mesoporous silica SBA-15 has been prepared by anion exchange resulting in a series of catalysts with changing Mo densities (0.2–2.5 Mo atoms nm-2). X-ray absorption, UV/Vis, Raman, and IR spectroscopy indicate that doubly anchored tetrahedral dioxo MoO4 units are the major surface species at all loadings. Higher reducibility at loadings close to the monolayer measured by temperature-programmed reduction and a steep increase in the catalytic activity observed in metathesis of propene and oxidative dehydrogenation of propane at 8 % of Mo loading are attributed to frustration of Mo oxide surface species and lateral interactions. Based on DFT calculations, NEXAFS spectra at the O-K-edge at high Mo loadings are explained by distorted MoO4complexes. Limited availability of anchor silanol groups at high loadings forces the MoO4 groups to form more strained configurations. The occurrence of strain is linked to the increase in reactivity.

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Language(s): eng - English
 Dates: 2013-07-2920132013-11-202013-12-16
 Publication Status: Published in print
 Pages: 5
 Publishing info: -
 Table of Contents: -
 Rev. Type: Peer
 Identifiers: DOI: 10.1002/anie.201306620
 Degree: -

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Title: Angewandte Chemie International Edition
  Abbreviation : Angew. Chem. Int. Ed.
Source Genre: Journal
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Publ. Info: Weinheim : Wiley-VCH
Pages: - Volume / Issue: 52 (51) Sequence Number: - Start / End Page: 13553 - 13557 Identifier: Other: 1433-7851
ISSN: 1521-3773
CoNE: https://pure.mpg.de/cone/journals/resource/0570-0833