TY - JOUR
T1 - Vanadium Catalyst on Isostructural Transition Metal, Lanthanide, and Actinide Based Metal-Organic Frameworks for Alcohol Oxidation
AU - Wang, Xingjie
AU - Zhang, Xuan
AU - Li, Peng
AU - Otake, Ken Ichi
AU - Cui, Yuexing
AU - Lyu, Jiafei
AU - Krzyaniak, Matthew D.
AU - Zhang, Yuanyuan
AU - Li, Zhanyong
AU - Liu, Jian
AU - Buru, Cassandra T.
AU - Islamoglu, Timur
AU - Wasielewski, Michael R.
AU - Li, Zhong
AU - Farha, Omar K.
N1 - Funding Information:
This work was supported as part of the Inorganometallic Catalyst Design Center, an EFRC funded by the DOE, Office of Science, Basic Energy Sciences (DE-SC0012702). EPR spectroscopy (M.D.K. and M.R.W.) was supported as part of the Center for Light Energy Activated Redox Processes, an EFRC funded by the DOE, Office of Science, Basic Energy Sciences (DE-SC0001059). X.W. gratefully acknowledges support from China Scholarship Council (CSC) during his visit to North-western University (201706150062). This work made use of the J. B. Cohen X-ray Diffraction Facility supported by the MRSEC program of the National Science Foundation (DMR-1720139) at the Materials Research Center of Northwestern University. This work made use of Keck-II facilities of the NUANCE Center at Northwestern University, which has received support from the Soft and Hybrid Nanotechnology Experimental (SHyNE) Resource (NSF NNCI-1542205); the MRSEC program (NSF DMR-1720139) at the Materials Research Center; the International Institute for Nanotechnology (IIN); the Keck Foundation; and the State of Illinois, through the IIN. This work made use of the IMSERC at Northwestern University, which has received support from the NSF (CHE-1048773 and DMR-0521267); SHyNE Resource (NSF NNCI-1542205); and the State of Illinois and IIN.
Publisher Copyright:
© 2019 American Chemical Society. All rights reserved.
PY - 2020
Y1 - 2020
N2 - 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.
AB - 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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U2 - 10.1021/jacs.9b02603
DO - 10.1021/jacs.9b02603
M3 - Article
C2 - 31083934
AN - SCOPUS:85066112992
VL - 141
SP - 8306
EP - 8314
JO - Journal of the American Chemical Society
JF - Journal of the American Chemical Society
SN - 0002-7863
IS - 20
ER -