Synergetic effect of VOx and TeOx species in mesoporous SiO2 on selective oxidation of propane to acrolein

被引:16
|
作者
Shi, Lei [1 ]
Zhu, Xue-Quan [1 ]
Su, Yuan [1 ]
Weng, Wei-Zheng [1 ]
Feng, Huan [2 ]
Yi, Xiao-Dong [1 ]
Liu, Zhen-Xian [3 ]
Wan, Hui-Lin [1 ]
机构
[1] Xiamen Univ, Natl Engn Lab Green Chem Prod Alcohols Ethers & E, State Key Lab Phys Chem Solid Surfaces, Dept Chem,Coll Chem & Chem Engn, Xiamen 361005, Peoples R China
[2] Montclair State Univ, Dept Earth & Environm Studies, Montclair, NJ 07043 USA
[3] Carnegie Inst Sci, Geophys Lab, Washington, DC 20015 USA
基金
中国国家自然科学基金;
关键词
Vanadium; Tellurium; Mesoporous silica; Selective propane oxidation; Acrolein; Active site; Synergetic effect; MIXED-OXIDE CATALYSTS; VANADIUM-OXIDE; ACTIVE-CENTERS; MOVTENB OXIDE; ACRYLIC-ACID; M1; PHASE; NB-O; SILICA; DEHYDROGENATION; SURFACE;
D O I
10.1016/j.jcat.2013.07.019
中图分类号
O64 [物理化学(理论化学)、化学物理学];
学科分类号
070304 ; 081704 ;
摘要
A mesoporous silica with incorporated vanadium (V) and tellurium (Te) (3%VTezOx-MS; z = 0-0.33), synthesized by an evaporation-induced self-assembly route, was used as a model catalyst to investigate the synergetic effect of VOx and TeOx species on propane oxidation to acrolein. It was found that V in the catalyst was predominantly present as a highly dispersed VO4 species, while Te existed as a highly dispersed TeOx species when the Te/V atomic ratio was below 0.2. Acrolein formation rate was positively correlated with TeOx content when both VOx and TeOx in the-catalysts-were in a highly dispersed state. Study of the propane oxidation pathways further indicated that highly dispersed VO4 in close contact with highly dispersed TeOx constituted the active sites for direct oxidation of propane to acrolein. These binary sites satisfied all the required functions for the reactions, including consecutive sequence of activation of propane and propylene intermediate followed by inserting oxygen into the as-formed allylic species. (C) 2013 Elsevier Inc. All rights reserved.
引用
收藏
页码:316 / 326
页数:11
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