Preparation of Highly Dispersed Chromium Oxide Catalysts Supported on Mesoporous Silica for the Oxidative Dehydrogenation of Propane Using CO2: Insight into the Nature of Catalytically Active Chromium Sites

被引:173
作者
Baek, Jayeon [1 ]
Yun, Hyeong Jin [1 ]
Yun, Danim [1 ]
Choi, Youngbo [1 ]
Yi, Jongheop [1 ]
机构
[1] Seoul Natl Univ, Sch Chem & Biol Engn, World Class Univ Program Chem Convergence Energy, Inst Chem Proc, Seoul 151741, South Korea
来源
ACS CATALYSIS | 2012年 / 2卷 / 09期
基金
新加坡国家研究基金会;
关键词
Cr-MSU-x; oxidative dehydrogenation of propane; CO2; utilization; active sites in chromium oxide; CARBON-DIOXIDE; CHROMIA/ALUMINA CATALYST; I-BUTANE; ETHANE; ETHYLBENZENE; SPECTROSCOPY; CR-MCM-41; BEHAVIOR; RAMAN; REACTIVITY;
D O I
10.1021/cs300198u
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
Highly dispersed chromium oxide catalysts supported on mesoporous silica (Cr-MSU-x) were prepared via a ((NMn+)-M-0)I-0 pathway with the goal of achieving the high performance oxidative dehydrogenation of propane (ODHP) reaction. The resulting materials exhibited a mesopore structure resembling 3D wormhole-like holes, as characterized by N-2 adsorption-desorption isotherms and RR-TEM. Catalytic experimental results revealed that the catalyst with a 0.028 Cr/Si molar ratio showed the highest catalytic activity among the catalysts studied. Two types of chromium species, isolated Cr(VI) and polymeric Cr(VI) species, were observed, as evidenced by H-2-temperature-programmed reduction. They were designated as "hard Cr(VI)" and "soft Cr(VI)" sites, respectively. The initial composition of the soft Cr(VI) in the total Cr(VI) is a major determinant factor in the ODHP performance.
引用
收藏
页码:1893 / 1903
页数:11
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