Selective propane dehydrogenation with single-site CoII on SiO2 by a non-redox mechanism

Bo Hu, Andrew Bean Getsoian, Neil M. Schweitzer, Ujjal Das, Hacksung Kim, Jens Niklas, Oleg Poluektov, Larry A. Curtiss, Peter C. Stair, Jeffrey T. Miller, Adam S. Hock

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89 Citations (Scopus)

Abstract

We report the synthesis, characterization, and catalytic performance for gas phase propane dehydrogenation of single-site Co2+ ions supported on silica. Spectroscopic characterization by resonance Raman, electron paramagnetic resonance, and X-ray near-edge and extended absorption fine structure revealed that tetrahedrally coordinated Co2+ ions are chemisorbed into the trisiloxane rings on the surface of amorphous silica. In situ XAS shows that Co is not oxidized by air nor reduced by hydrogen even at 650 °C. For catalytic propane dehydrogenation, single-site Co2+/SiO2 exhibits selectivities >95% at 550 °C and >90% at 650 °C with stable activity over 24 h. Calculations with hybrid density functional theory support a non-redox mechanism for activation of C-H and H-H bonds by Co2+ similar to that previously reported for single-site Zn2+/SiO2.

Original languageEnglish
Pages (from-to)24-37
Number of pages14
JournalJournal of Catalysis
Volume322
DOIs
Publication statusPublished - Feb 1 2015

Keywords

  • Dehydrogenation
  • EXAFS
  • Lewis acid
  • Raman spectroscopy
  • Single-site catalysis

ASJC Scopus subject areas

  • Catalysis
  • Physical and Theoretical Chemistry

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    Hu, B., Bean Getsoian, A., Schweitzer, N. M., Das, U., Kim, H., Niklas, J., Poluektov, O., Curtiss, L. A., Stair, P. C., Miller, J. T., & Hock, A. S. (2015). Selective propane dehydrogenation with single-site CoII on SiO2 by a non-redox mechanism. Journal of Catalysis, 322, 24-37. https://doi.org/10.1016/j.jcat.2014.10.018