期刊
JOURNAL OF CATALYSIS
卷 267, 期 2, 页码 158-166出版社
ACADEMIC PRESS INC ELSEVIER SCIENCE
DOI: 10.1016/j.jcat.2009.08.005
关键词
Carbon catalysts; Oxidative dehydrogenation; Isobutane; Isobutene; Graphitized mesoporous carbon; Edge sites; Quinone sites
资金
- Center for Nanophase Materials Sciences
- Oak Ridge National Laboratory
- Office of Basic Energy Sciences
- U.S. Department of Energy
- Oak Ridge Institute for Science and Education (ORISE) and ORNL
Reaction network analysis of the oxidative dehydrogenation (ODH) reaction of isobutane over model carbon catalysts with tailored open-edge graphitic structure and quinone-type oxygenated functionalities was used to identify the selective pathways for the formation of isobutene. Carbon-based materials have been widely used in catalysis, but the active sites are not well-understood due to the complexity of the carbon structure. Correct identification of these sites is essential for learning how to manipulate material structure to achieve high catalytic yields of the desired products. In this study, we created model catalysts with controllable surface concentration of oxygen based on graphitized mesoporous carbon (GMC). Our studies reveal that the ODH reaction of isobutane on carbon catalysts is a parallel-consecutive pathway with partial oxidative dehydrogenation for the formation of isobutene and deep oxidation pathway for the direct formation of CO and CO2 from isobutane. These two pathways show different dependence on the quinone-type oxygen sites: the rate constant leading to the desired partial oxidation product does not show a strong correlation to the density of the oxygen sites, whereas the rate constant leading to the unselective COx products increases continuously with the density of oxygen sites. (C) 2009 Elsevier Inc. All rights reserved.
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