期刊
ACS CENTRAL SCIENCE
卷 3, 期 1, 页码 31-38出版社
AMER CHEMICAL SOC
DOI: 10.1021/acscentsci.6b00290
关键词
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资金
- Inorganometallic Catalyst Design Center, an EFRC - DOE, Office of Basic Energy Sciences [DE-SC0012702]
- Department of Defense (DoD) through the National Defense Science and Engineering Fellowship (NDSEG) program
- Ministry of Economy and Knowledge from the Catalan Government [BP-DGR 2014]
- MRSEC program of the National Science Foundation at the Materials Research Center of Northwestern University [DMR-1121262]
- Soft and Hybrid Nanotechnology Experimental (SHyNE) Resource [NSF NNCI-1542205]
- MRSEC program at the Materials Research Center [NSF DMR-1121262]
- International Institute for Nanotechnology (IIN)
- Keck Foundation
- State of Illinois, through the IIN
- U.S. Department of Energy, Office of Science, and Office of Basic Energy Sciences [DE-AC02-06CH11357]
- Department of Energy
- MRCAT member institutions
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 degrees 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.
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