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

页码：1893 / 1903

页数：11

共 57 条

[21] Characterization of Cr-MCM-41 and Al,Cr-MCM-41 mesoporous catalysts for gas-phase oxidative dehydrogenation of cyclohexane [J].