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.
引用
收藏
页码:12347 / 12356
页数:10
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