4.8 Article

Highly Active and Selective Sites for Propane Dehydrogenation in Zeolite Ga-BEA

Journal

JOURNAL OF THE AMERICAN CHEMICAL SOCIETY
Volume 144, Issue 27, Pages 12347-12356

Publisher

AMER CHEMICAL SOC
DOI: 10.1021/jacs.2c03810

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Funding

  1. Chinese Scholarship Council
  2. U.S. Department of Energy (DOE) , Office of Science, Office of Basic Energy Sciences (BES) , Division of Chemical Sciences, Geosciences and Biosciences [FWP 47319]

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A highly selective Ga-modified zeolite BEA has been successfully synthesized for propane dehydrogenation. The propane dehydrogenation rate is determined by different factors under different conditions. The active sites are identified as dehydrated and tetrahedrally coordinated Ga3+, and the selectivity towards aromatics is low.
ABSTRACT: A highly selective Ga-modified zeolite BEA for propane dehydrogenation has been synthesized by grafting Ga on Zn-BEA followed by removal of Zn in the presence of H2. A propene selectivity of 82% at 19% propane conversion illustrates the high selectivity at 813 K. The kinetic model of the catalyzed dehydrogenation including the elementary steps of propane adsorption, first and second C-H bond cleavage, and propene and H2 desorption demonstrates that the propane dehydrogenation rate is determined by the first C-H bond cleavage at low pC3H8, while at high pC3H8, the rate is limited by the desorption of H2. The active sites have been identified as dehydrated and tetrahedrally coordinated Ga3+ in the *BEA lattice. The low selectivity toward aromatics is concluded to be associated with the high Lewis acid strength of lattice Ga3+ and the low Bronsted acid strength of the hydrated Ga sites.

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