Morphology-dependent properties of Co3O4/CeO2 catalysts for low temperature dibromomethane (CH2Br2) oxidation

被引:79
作者
Mei, Jian [1 ]
Ke, Yu [1 ]
Yu, Zhongjue [1 ]
Hu, Xiaofang [1 ]
Qu, Zan [1 ]
Yan, Naiqiang [1 ]
机构
[1] Shanghai Jiao Tong Univ, Sch Environm Sci & Engn, 800 Dong Chuan Rd, Shanghai 200240, Peoples R China
基金
中国国家自然科学基金;
关键词
Dibromomethane; Co3O4; CeO2; nanocrystals; Metal-support interaction; METHANOL SYNTHESIS; TRANSITION-METAL; CEO2; PERFORMANCE; ADSORPTION; CO3O4/TIO2; CO3O4-CEO2; MECHANISM; FTIR;
D O I
10.1016/j.cej.2017.03.038
中图分类号
X [环境科学、安全科学];
学科分类号
08 ; 0830 ;
摘要
Brominated hydrocarbons are a typical pollutant in purified terephthalic acid (PTA) exhaust gas, which is harmful for human health and the environment once released to the atmosphere. In this study, three Co3O4/CeO2 catalysts with different CeO2 morphologies (rod, plate, and cube) were prepared and were used for low temperature dibromomethane (CH2Br2) oxidation, which was used as the model compound for brominated hydrocarbons. The experimental results showed that Co3O4/CeO2-rod achieved significantly higher catalytic activity, with a T-90 of approximately 312 degrees C for CH2Br2 oxidation and higher selectivity to CO2 than Co3O4/CeO2-plate and Co3O4/CeO2-cube. All of the Co3O4/CeO2 catalysts investigated were stable for at least 30 h at 500 ppm CH2Br2 and 10% O-2 at a GHSV of 75,000 mL/(g.h)(-1),and the final products were COx Br-2, and HBr, without the formation of other Br -containing organic byproducts. The higher catalytic activity of Co3O4/CeO2-rod was attributed to the high content of Co3+, more surface -adsorbed oxygen, and more oxygen vacancies in their exposed {1 0 0} and {1 1 0} planes. In addition, Co3O4 had a stronger interaction with CeO2-rod, making it superior for CH2Br2 oxidation. Moreover, on the basis of the analysis of products and in situ DRIFTS studies, a credible reaction mechanism for CH2Br2 oxidation over Co3O4/CeO2 catalysts was proposed. (C) 2017 Published by Elsevier B.V.
引用
收藏
页码:124 / 134
页数:11
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