Vanadium Catalyst on Isostructural Transition Metal, Lanthanide, and Actinide Based Metal-Organic Frameworks for Alcohol Oxidation

Xingjie Wang; Xuan Zhang; Peng Li; Ken Ichi Otake; Yuexing Cui; Jiafei Lyu; Matthew D. Krzyaniak; Yuanyuan Zhang; Zhanyong Li; Jian Liu; Cassandra T. Buru; Timur Islamoglu; Michael R. Wasielewski; Zhong Li; Omar K. Farha

doi:10.1021/jacs.9b02603

Vanadium Catalyst on Isostructural Transition Metal, Lanthanide, and Actinide Based Metal-Organic Frameworks for Alcohol Oxidation

Xingjie Wang, Xuan Zhang, Peng Li, Ken Ichi Otake, Yuexing Cui, Jiafei Lyu, Matthew D. Krzyaniak, Yuanyuan Zhang, Zhanyong Li, Jian Liu, Cassandra T. Buru, Timur Islamoglu, Michael R. Wasielewski, Zhong Li, Omar K. Farha^*

^*Corresponding author for this work

Chemistry

Research output: Contribution to journal › Article › peer-review

131 Scopus citations

Abstract

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.

Original language	English (US)
Pages (from-to)	8306-8314
Number of pages	9
Journal	Journal of the American Chemical Society
Volume	141
Issue number	20
DOIs	https://doi.org/10.1021/jacs.9b02603
State	Published - 2020

Funding

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.

ASJC Scopus subject areas

Catalysis
General Chemistry
Biochemistry
Colloid and Surface Chemistry

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10.1021/jacs.9b02603

Cite this

Wang, X., Zhang, X., Li, P., Otake, K. I., Cui, Y., Lyu, J., Krzyaniak, M. D., Zhang, Y., Li, Z., Liu, J., Buru, C. T., Islamoglu, T., Wasielewski, M. R., Li, Z., & Farha, O. K. (2020). Vanadium Catalyst on Isostructural Transition Metal, Lanthanide, and Actinide Based Metal-Organic Frameworks for Alcohol Oxidation. Journal of the American Chemical Society, 141(20), 8306-8314. https://doi.org/10.1021/jacs.9b02603

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abstract = "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.",

author = "Xingjie Wang and Xuan Zhang and Peng Li and Otake, {Ken Ichi} and Yuexing Cui and Jiafei Lyu and Krzyaniak, {Matthew D.} and Yuanyuan Zhang and Zhanyong Li and Jian Liu and Buru, {Cassandra T.} and Timur Islamoglu and Wasielewski, {Michael R.} and Zhong Li and Farha, {Omar K.}",

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Wang, X, Zhang, X, Li, P, Otake, KI, Cui, Y, Lyu, J, Krzyaniak, MD, Zhang, Y, Li, Z, Liu, J, Buru, CT, Islamoglu, T, Wasielewski, MR, Li, Z & Farha, OK 2020, 'Vanadium Catalyst on Isostructural Transition Metal, Lanthanide, and Actinide Based Metal-Organic Frameworks for Alcohol Oxidation', Journal of the American Chemical Society, vol. 141, no. 20, pp. 8306-8314. https://doi.org/10.1021/jacs.9b02603

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AU - Li, Zhanyong

AU - Liu, Jian

AU - Buru, Cassandra T.

AU - Islamoglu, Timur

AU - Wasielewski, Michael R.

AU - Li, Zhong

AU - Farha, Omar K.

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Vanadium Catalyst on Isostructural Transition Metal, Lanthanide, and Actinide Based Metal-Organic Frameworks for Alcohol Oxidation

Abstract

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ASJC Scopus subject areas

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CCDC 1899941: Experimental Crystal Structure Determination

CCDC 1899942: Experimental Crystal Structure Determination

CCDC 1876021: Experimental Crystal Structure Determination

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Vanadium Catalyst on Isostructural Transition Metal, Lanthanide, and Actinide Based Metal-Organic Frameworks for Alcohol Oxidation

Abstract

Funding

ASJC Scopus subject areas

Access to Document

Other files and links

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Datasets

CCDC 1899941: Experimental Crystal Structure Determination

CCDC 1899942: Experimental Crystal Structure Determination

CCDC 1876021: Experimental Crystal Structure Determination

Cite this