期刊
JOURNAL OF CATALYSIS
卷 329, 期 -, 页码 177-186出版社
ACADEMIC PRESS INC ELSEVIER SCIENCE
DOI: 10.1016/j.jcat.2015.05.014
关键词
Ru/CeO2 catalysts; CO2 methanation reaction; Oxygen vacancy; Morphology dependence; Metal-support interaction
资金
- 973 Program [2011CBA00504]
- National Natural Science Foundation of China (NSFC)
- Scientific Fund from Beijing Municipal Commission of Education
- Beijing Natural Science Foundation [2132043]
- China National Funds for Distinguished Young Scientists of the NSFC
The existence of oxygen vacancies in heterogeneous catalysis plays an essential role in determining the catalytic reactivity of metal catalysts. In this work, Ru nanoparticles were immobilized onto the CeO2 nanocubes (NCs), nanorods (NRs), and nanopolyhedrons (NPs) with the dominantly exposed (100), (1 1 0), and {111 facet of CeO2 support, respectively. Their catalytic behavior toward CO2 methanation was studied in detail, and the highest catalytic rate per gram of catalyst was obtained over the Ru(3%)/CeO2-NCs catalyst (reaction rate: 4.85 x 10(-8) mol g(cat)(-1)s(-1); selectivity: 99%; 150 degrees C). The temperature-programmed reduction (TPR), Raman spectra, and oxygen storage capacity (OSC) test confirm that the Ru(3%)/CeO2-NCs catalyst possesses the highest concentration of oxygen vacancies owing to the Ru-promoted formation of oxygen vacancy on the CeO2-NCs. In addition, in situ infrared spectroscopy measurements demonstrate that the abundant oxygen vacancy in Ru(3%)/CeO2-NCs serves as the active site for CO2 activation, accounting for the significantly enhanced low-temperature reaction rate per gram of Ru/CeO2 catalyst. (C) 2015 Elsevier Inc. All rights reserved.
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