@article{203cfc8ee5e64110b34c5b1567669d07,
title = "Selective propane dehydrogenation with single-site CoII on SiO2 by a non-redox mechanism",
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.",
keywords = "Dehydrogenation, EXAFS, Lewis acid, Raman spectroscopy, Single-site catalysis",
author = "Bo Hu and {Bean Getsoian}, Andrew and Schweitzer, {Neil M.} and Ujjal Das and Hacksung Kim and Jens Niklas and Oleg Poluektov and Curtiss, {Larry A.} and Stair, {Peter C.} and Miller, {Jeffrey T.} and Hock, {Adam S.}",
note = "Funding Information: The work was supported by the U.S. Department of Energy, Office of Basic Energy Sciences, Chemical Sciences under Contract DE-AC-02-06CH11357 . BH and ASH would like to thank the Illinois Institute of Technology for a Starr-Fieldhouse Fellowship (BH) and startup funding support. Use of the Advanced Photon Source is supported by the U.S. Department of Energy, Office of Science, and Office of Basic Energy Sciences , under Contract DE-AC02-06CH11357 . Materials Research Collaborative Access Team (MRCAT, Sectors 10 BM and 10ID) operations are supported by the Department of Energy and the MRCAT member institutions . Density functional theory calculations were performed using the computational resources available at the Argonne National Laboratory Center for Nanoscale Materials (CNM) and the computing resources provided on “Fusion” and “Blues,” high-performance computing clusters operated by the Laboratory Computing Resource Center at Argonne National Laboratory. Publisher Copyright: {\textcopyright} 2014 Published by Elsevier Inc.",
year = "2015",
month = feb,
day = "1",
doi = "10.1016/j.jcat.2014.10.018",
language = "English (US)",
volume = "322",
pages = "24--37",
journal = "Journal of Catalysis",
issn = "0021-9517",
publisher = "Academic Press Inc.",
}