TY - JOUR
T1 - Highly Active and Selective Sites for Propane Dehydrogenation in Zeolite Ga-BEA
AU - Ni, Lingli
AU - Khare, Rachit
AU - Bermejo-Deval, Ricardo
AU - Zhao, Ruixue
AU - Tao, Lei
AU - Liu, Yue
AU - Lercher, Johannes A.
N1 - Publisher Copyright:
© 2022 American Chemical Society.
PY - 2022/7/13
Y1 - 2022/7/13
N2 - 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.
AB - 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.
UR - http://www.scopus.com/inward/record.url?scp=85134187419&partnerID=8YFLogxK
U2 - 10.1021/jacs.2c03810
DO - 10.1021/jacs.2c03810
M3 - Article
C2 - 35771043
AN - SCOPUS:85134187419
SN - 0002-7863
VL - 144
SP - 12347
EP - 12356
JO - Journal of the American Chemical Society
JF - Journal of the American Chemical Society
IS - 27
ER -