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

Lingli Ni(Technical University of Munich), Rachit Khare(Technical University of Munich), Ricardo Bermejo‐Deval(Technical University of Munich), Ruixue Zhao(Technical University of Munich), Lei Tao(Technical University of Munich), Yue Liu(Technical University of Munich), Johannes A. Lercher(Pacific Northwest National Laboratory)
Journal of the American Chemical Society
June 30, 2022
Cited by 74Open Access
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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 Brønsted acid strength of the hydrated Ga sites.


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