Metal-Organic Framework Supported Cobalt Catalysts for the Oxidative Dehydrogenation of Propane at Low Temperature.

Autor: Li Z; Department of Chemistry, Northwestern University , 2145 Sheridan Road, Evanston, Illinois 60208, United States., Peters AW; Department of Chemistry, Northwestern University , 2145 Sheridan Road, Evanston, Illinois 60208, United States., Bernales V; Department of Chemistry, Supercomputing Institute, and Chemical Theory Center, University of Minnesota , Minneapolis, Minnesota 55455, United States., Ortuño MA; Department of Chemistry, Supercomputing Institute, and Chemical Theory Center, University of Minnesota , Minneapolis, Minnesota 55455, United States., Schweitzer NM; Department of Chemical and Biological Engineering, Northwestern University , 2145 Sheridan Road, Evanston, Illinois 60208, United States., DeStefano MR; Department of Chemistry, Northwestern University , 2145 Sheridan Road, Evanston, Illinois 60208, United States., Gallington LC; X-ray Science Division, Advanced Photon Source, Argonne National Laboratory , Argonne, Illinois 60439-4858, United States., Platero-Prats AE; X-ray Science Division, Advanced Photon Source, Argonne National Laboratory , Argonne, Illinois 60439-4858, United States., Chapman KW; X-ray Science Division, Advanced Photon Source, Argonne National Laboratory , Argonne, Illinois 60439-4858, United States., Cramer CJ; Department of Chemistry, Supercomputing Institute, and Chemical Theory Center, University of Minnesota , Minneapolis, Minnesota 55455, United States., Gagliardi L; Department of Chemistry, Supercomputing Institute, and Chemical Theory Center, University of Minnesota , Minneapolis, Minnesota 55455, United States., Hupp JT; Department of Chemistry, Northwestern University , 2145 Sheridan Road, Evanston, Illinois 60208, United States., Farha OK; Department of Chemistry, Northwestern University, 2145 Sheridan Road, Evanston, Illinois 60208, United States; Department of Chemistry, Faculty of Science, King Abdulaziz University, Jeddah 21589, Saudi Arabia.
Jazyk: angličtina
Zdroj: ACS central science [ACS Cent Sci] 2017 Jan 25; Vol. 3 (1), pp. 31-38. Date of Electronic Publication: 2016 Nov 30.
DOI: 10.1021/acscentsci.6b00290
Abstrakt: Zr-based metal-organic frameworks (MOFs) have been shown to be excellent catalyst supports in heterogeneous catalysis due to their exceptional stability. Additionally, their crystalline nature affords the opportunity for molecular level characterization of both the support and the catalytically active site, facilitating mechanistic investigations of the catalytic process. We describe herein the installation of Co(II) ions to the Zr 6 nodes of the mesoporous MOF, NU-1000, via two distinct routes, namely, solvothermal deposition in a MOF (SIM) and atomic layer deposition in a MOF (AIM), denoted as Co-SIM+NU-1000 and Co-AIM+NU-1000, respectively. The location of the deposited Co species in the two materials is determined via difference envelope density (DED) analysis. Upon activation in a flow of O 2 at 230 °C, both materials catalyze the oxidative dehydrogenation (ODH) of propane to propene under mild conditions. Catalytic activity as well as propene selectivity of these two catalysts, however, is different under the same experimental conditions due to differences in the Co species generated in these two materials upon activation as observed by in situ X-ray absorption spectroscopy. A potential reaction mechanism for the propane ODH process catalyzed by Co-SIM+NU-1000 is proposed, yielding a low activation energy barrier which is in accord with the observed catalytic activity at low temperature.
Competing Interests: The authors declare no competing financial interest.
Databáze: MEDLINE
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