Investigation of the selective sites on graphitic carbons for oxidative dehydrogenation of isobutane

Hong Xie, Zili Wu, Steven H. Overbury, Chengdu Liang, Viviane Schwartz

Research output: Contribution to journalArticlepeer-review

40 Scopus citations

Abstract

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.

Original languageEnglish
Pages (from-to)158-166
Number of pages9
JournalJournal of Catalysis
Volume267
Issue number2
DOIs
StatePublished - Oct 25 2009

Keywords

  • Carbon catalysts
  • Edge sites
  • Graphitized mesoporous carbon
  • Isobutane
  • Isobutene
  • Oxidative dehydrogenation
  • Quinone sites

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