期刊
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY
卷 141, 期 20, 页码 8306-8314出版社
AMER CHEMICAL SOC
DOI: 10.1021/jacs.9b02603
关键词
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资金
- Inorganometallic Catalyst Design Center, an EFRC - DOE, Office of Science, Basic Energy Sciences [DE-SC0012702]
- China Scholarship Council (CSC) [201706150062]
- MRSEC program of the National Science Foundation at the Materials Research Center of Northwestern University [DMR-1720139]
- Soft and Hybrid Nanotechnology Experimental (SHyNE) Resource [NSF NNCI-1542205]
- MRSEC program at the Materials Research Center [NSF DMR-1720139]
- International Institute for Nanotechnology (IIN)
- Keck Foundation
- State of Illinois, through the IIN
- NSF [CHE-1048773, DMR-0521267]
- SHyNE Resource [NSF NNCI-1542205]
- State of Illinois
- IIN
- Center for Light Energy Activated Redox Processes, an EFRC - DOE, Office of Science, Basic Energy Sciences [DE-SC0001059]
The understanding of the catalyst-support interactions has been an important challenge in heterogeneous catalysis since the supports can play a vital role in controlling the properties of the active species and hence their catalytic performance. Herein, a series of isostructural mesoporous metal organic frameworks (MOFs) based on transition metals, lanthanides, and actinides (Zr, Hf, Ce, Th) were investigated as supports for a vanadium catalyst. The vanadium species was coordinated to the oxo groups of the MOF node in a single-ion fashion, as determined by single-crystal X-ray diffraction, diffuse reflectance infrared Fourier transform spectroscopy, and diffuse reflectance UV-vis spectroscopy. The support effects of these isostructural MOFs were then probed using the aerobic oxidation of 4-methoxybenzyl alcohol as a model reaction. The turnover frequency was found to be correlated with the electronegativity and oxidation state of the metal cations on the supporting MOF nodes, highlighting an important consideration when designing catalyst supports.
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