Journal
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY
Volume 140, Issue 14, Pages 4849-4859Publisher
AMER CHEMICAL SOC
DOI: 10.1021/jacs.7b12901
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- Bavarian Ministry of Economic Affairs and Media, Energy and Technology (Bayerisches Staatsministerium fur Wirtschaft und Medien, Energie und Technologie) [LaBay74]
- Bavarian State Ministry of Education, Science and the Arts (Bayerisches Staatsministerium fur Bildung und Kultus, Wissenschaft und Kunst)
- Alexander von Humboldt foundation
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The active sites for propane dehydrogenation in Ga/H-WZSM-5 with moderate concentrations of tetrahedral aluminum in the lattice were identified to be Lewis-Bronsted acid pairs. With increasing availability, Ga+ and Bronsted acid site concentrations changed inversely, as protons of Bronsted acid sites were exchanged with Ga+. At a Ga/Al ratio of 1/2, the rate of propane dehydrogenation was 2 orders of magnitude higher than with the parent H-ZSM-5, highlighting the extraordinary activity of the Lewis-Bronsted acid pairs. Density functional theory calculations relate the high activity to a bifunctional mechanism that proceeds via heterolytic activation of the propane C-H bond followed by a monomolecular elimination of H-2 and desorption of propene.
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