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Highly Active and Selective Sites for Propane Dehydrogenation in Zeolite Ga-BEA
被引:48
|作者:
Ni, Lingli
[1
,2
]
Khare, Rachit
[1
,2
]
Bermejo-Deval, Ricardo
[1
,2
]
Zhao, Ruixue
[1
,2
]
Tao, Lei
[1
,2
]
Liu, Yue
[1
,2
,3
]
Lercher, Johannes A.
[1
,2
,4
]
机构:
[1] Tech Univ Munich, Dept Chem, D-85747 Garching, Germany
[2] Tech Univ Munich, Catalysis Res Ctr, D-85747 Garching, Germany
[3] East China Normal Univ, Sch Chem & Mol Engn, Shanghai Key Lab Green Chem & Chem Proc, Shanghai 200062, Peoples R China
[4] Pacific Northwest Natl Lab, Inst Integrated Catalysis, Richland, WA 99352 USA
关键词:
LIGHT ALKANE DEHYDROGENATION;
H-GALLOSILICATE MFI;
COORDINATION ENVIRONMENT;
GALLIUM SITES;
ACID SITES;
AROMATIZATION;
CATALYSTS;
HZSM-5;
DEACTIVATION;
ACTIVATION;
D O I:
10.1021/jacs.2c03810
中图分类号:
O6 [化学];
学科分类号:
0703 ;
摘要:
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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页码:12347 / 12356
页数:10
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