Nature of active phase of VOx catalysts supported on SiBeta for direct dehydrogenation of propane propylene

被引:53
|
作者
Chen, Chong [1 ,2 ]
Sun, Minglei [1 ]
Hu, Zhongpan [1 ]
Liu, Yuping [2 ]
Zhang, Shoumin [2 ]
Yuan, Zhong-Yong [1 ,2 ]
机构
[1] Nankai Univ, Sch Mat Sci & Engn, Natl Inst Adv Mat, Tianjin 300350, Peoples R China
[2] Nankai Univ, Coll Chem, Collaborat Innovat Ctr Chem Sci & Engn Tianjin, Key Lab Adv Energy Mat Chem,Minist Educ, Tianjin 300071, Peoples R China
基金
中国国家自然科学基金;
关键词
Propane dehydrogenation; Propylene; VOx species; SiBeta support; Active sites; VSI-BETA ZEOLITE; OXIDATIVE DEHYDROGENATION; BEA ZEOLITE; NONOXIDATIVE DEHYDROGENATION; VOX/AL2O3; CATALYSTS; V CONTENT; VANADIUM; STABILITY; SELECTIVITY; CONVERSION;
D O I
10.1016/S1872-2067(19)63444-3
中图分类号
O69 [应用化学];
学科分类号
081704 ;
摘要
The VOx catalysts supported on dealuminated Beta zeolite (SiBeta) with varying V loadings (from 0.5 to 10 wt%) are prepared and tested for their catalytic activities in the reaction of direct dehydrogenation of propane to propylene (PDH). It is characterized that the VSiBeta catalysts possess different kinds of vanadium species on the SiBeta support, including monomeric or isolated VOx species at a low V loading, and polynuclear VOx species in different polymerization degrees at higher V loadings. The 3VSiBeta catalyst (V loading is 3 wt%), containing isolated VOx species in monolayer, shows around 40% of propane conversion with 90% of propylene selectivity (reaction conditions: 600 degrees C, 4000 mL g(-1) h(-1)) which are comparable to VSiBeta catalysts with higher V loadings. The catalytic activity exhibits a good linear relationship with the amount of generated acidic sites, which are derived from the interaction sites between VOx species and SiBeta support, and keeps stable after several regeneration cycles. Thus, as the VOx species directly contact with SiBeta support via V-O-Si bonds, a reactivity enhancement can be achieved. While, the initial valence state of V does not seem to influence the catalytic performance. Moreover, the aggregation degree of VOx species determines the propylene selectivity and deactivation rate, both of which increase as raising the V loading amount. (C) 2020, Dalian Institute of Chemical Physics, Chinese Academy of Sciences. Published by Elsevier B.V. All rights reserved.
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页码:276 / 285
页数:10
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