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  Surface roughness effects in the catalytic behavior of vanadia supported on SBA-15

Smith, M. A., Zoelle, A., Yang, Y., Rioux, R. M., Hamilton, N., Amakawa, K., et al. (2014). Surface roughness effects in the catalytic behavior of vanadia supported on SBA-15. Journal of Catalysis, 312, 170-178. doi:10.1016/j.jcat.2014.01.011.

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1936530.pdf (Correspondence), 94KB
 
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 Creators:
Smith, Michael A.1, Author
Zoelle, Alexander1, Author
Yang, Yong2, Author
Rioux, Robert M.2, Author
Hamilton, Neil3, Author              
Amakawa, Kazuhiko3, Author              
Nielsen, Pia Kjaer3, Author              
Trunschke, Annette3, Author              
Affiliations:
1Department of Chemical Engineering, Villanova University, Villanova, PA 19085, United States, ou_persistent22              
2Department of Chemical Engineering, Pennsylvania State University, University Park, PA 16802, United States, ou_persistent22              
3Inorganic Chemistry, Fritz Haber Institute, Max Planck Society, ou_24023              

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Free keywords: SBA-15; Mesoporous silica; Vanadia; Partial oxidation; Methanol; Propane; Selective oxidation
 Abstract: SBA-15 is a template-synthesized mesoporous silica that has found extensive use as a model support for catalytic studies. Thorough structural analyses describe a dual micropore–mesopore structure with a broad distribution of micropore size that we alternatively describe as fractal surface roughness. SBA-15 materials with varying surface roughness were systematically prepared followed by grafting with sub-monolayer coverage of vanadium oxide (VOx). VOx-SBA-15 samples were characterized using nitrogen adsorption, UV–vis spectroscopy, and Raman spectroscopy and tested in the catalytic partial oxidation of methanol to formaldehyde as well as propane to propene. SBA-15 supports with smoother surfaces favor the formation of more polymeric vanadia species at the same surface density loading. Smooth surface catalysts result in a ∼20% lower selectivity of methanol to formaldehyde, and the apparent activation energy on smooth surfaces is ∼25 kJ/mol lower than on rough surfaces (75 versus 100 kJ/mol, respectively). In contrast to methanol, propane results show a 15% higher selectivity to propene on smooth surfaces. A model of silica hydroxyl distribution is proposed to explain the differences in vanadia speciation and resulting catalytic behavior. These results are significant for our understanding of the nature of vanadium species in partial oxidation catalysts and illustrate the importance of considering differences in support surface morphology in analyzing catalytic behavior.

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Language(s): eng - English
 Dates: 2014-01-112013-09-062014-01-142014-02-252014-04
 Publication Status: Published in print
 Pages: 9
 Publishing info: -
 Table of Contents: -
 Rev. Type: Peer
 Identifiers: DOI: 10.1016/j.jcat.2014.01.011
 Degree: -

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Title: Journal of Catalysis
Source Genre: Journal
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Publ. Info: San Diego, CA. : Academic Press
Pages: - Volume / Issue: 312 Sequence Number: - Start / End Page: 170 - 178 Identifier: ISSN: 0021-9517
CoNE: https://pure.mpg.de/cone/journals/resource/954922645027