A Hafnium-Based Metal-Organic Framework as a Nature-Inspired Tandem Reaction Catalyst

M. Hassan Beyzavi; Nicolaas A. Vermeulen; Ashlee J. Howarth; Samat Tussupbayev; Aaron B. League; Neil M. Schweitzer; James R. Gallagher; Ana E. Platero-Prats; Nema Hafezi; Amy A. Sarjeant; Jeffrey T. Miller; Karena W. Chapman; J. Fraser Stoddart; Christopher J. Cramer; Joseph T. Hupp; Omar K. Farha

doi:10.1021/jacs.5b08440

A Hafnium-Based Metal-Organic Framework as a Nature-Inspired Tandem Reaction Catalyst

M. Hassan Beyzavi, Nicolaas A. Vermeulen, Ashlee J. Howarth, Samat Tussupbayev, Aaron B. League, Neil M. Schweitzer, James R. Gallagher, Ana E. Platero-Prats, Nema Hafezi, Amy A. Sarjeant, Jeffrey T. Miller, Karena W. Chapman, J. Fraser Stoddart, Christopher J. Cramer, Joseph T. Hupp, Omar K. Farha

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120 Scopus citations

Abstract

Tandem catalytic systems, often inspired by biological systems, offer many advantages in the formation of highly functionalized small molecules. Herein, a new metal-organic framework (MOF) with porphyrinic struts and Hf ₆ nodes is reported. This MOF demonstrates catalytic efficacy in the tandem oxidation and functionalization of styrene utilizing molecular oxygen as a terminal oxidant. The product, a protected 1,2-aminoalcohol, is formed selectively and with high efficiency using this recyclable heterogeneous catalyst. Significantly, the unusual regioselective transformation occurs only when an Fe-decorated Hf ₆ node and the Fe-porphyrin strut work in concert. This report is an example of concurrent orthogonal tandem catalysis.

Original language	English (US)
Pages (from-to)	13624-13631
Number of pages	8
Journal	Journal of the American Chemical Society
Volume	137
Issue number	42
DOIs	https://doi.org/10.1021/jacs.5b08440
State	Published - Oct 28 2015

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Beyzavi, M. H., Vermeulen, N. A., Howarth, A. J., Tussupbayev, S., League, A. B., Schweitzer, N. M., Gallagher, J. R., Platero-Prats, A. E., Hafezi, N., Sarjeant, A. A., Miller, J. T., Chapman, K. W., Stoddart, J. F., Cramer, C. J., Hupp, J. T., & Farha, O. K. (2015). A Hafnium-Based Metal-Organic Framework as a Nature-Inspired Tandem Reaction Catalyst. Journal of the American Chemical Society, 137(42), 13624-13631. https://doi.org/10.1021/jacs.5b08440

Beyzavi, MH, Vermeulen, NA, Howarth, AJ, Tussupbayev, S, League, AB, Schweitzer, NM, Gallagher, JR, Platero-Prats, AE, Hafezi, N, Sarjeant, AA, Miller, JT, Chapman, KW, Stoddart, JF, Cramer, CJ, Hupp, JT & Farha, OK 2015, 'A Hafnium-Based Metal-Organic Framework as a Nature-Inspired Tandem Reaction Catalyst', Journal of the American Chemical Society, vol. 137, no. 42, pp. 13624-13631. https://doi.org/10.1021/jacs.5b08440

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title = "A Hafnium-Based Metal-Organic Framework as a Nature-Inspired Tandem Reaction Catalyst",

abstract = " Tandem catalytic systems, often inspired by biological systems, offer many advantages in the formation of highly functionalized small molecules. Herein, a new metal-organic framework (MOF) with porphyrinic struts and Hf 6 nodes is reported. This MOF demonstrates catalytic efficacy in the tandem oxidation and functionalization of styrene utilizing molecular oxygen as a terminal oxidant. The product, a protected 1,2-aminoalcohol, is formed selectively and with high efficiency using this recyclable heterogeneous catalyst. Significantly, the unusual regioselective transformation occurs only when an Fe-decorated Hf 6 node and the Fe-porphyrin strut work in concert. This report is an example of concurrent orthogonal tandem catalysis. ",

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AU - League, Aaron B.

AU - Schweitzer, Neil M.

AU - Gallagher, James R.

AU - Platero-Prats, Ana E.

AU - Hafezi, Nema

AU - Sarjeant, Amy A.

AU - Miller, Jeffrey T.

AU - Chapman, Karena W.

AU - Stoddart, J. Fraser

AU - Cramer, Christopher J.

AU - Hupp, Joseph T.

AU - Farha, Omar K.

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N2 - Tandem catalytic systems, often inspired by biological systems, offer many advantages in the formation of highly functionalized small molecules. Herein, a new metal-organic framework (MOF) with porphyrinic struts and Hf 6 nodes is reported. This MOF demonstrates catalytic efficacy in the tandem oxidation and functionalization of styrene utilizing molecular oxygen as a terminal oxidant. The product, a protected 1,2-aminoalcohol, is formed selectively and with high efficiency using this recyclable heterogeneous catalyst. Significantly, the unusual regioselective transformation occurs only when an Fe-decorated Hf 6 node and the Fe-porphyrin strut work in concert. This report is an example of concurrent orthogonal tandem catalysis.

AB - Tandem catalytic systems, often inspired by biological systems, offer many advantages in the formation of highly functionalized small molecules. Herein, a new metal-organic framework (MOF) with porphyrinic struts and Hf 6 nodes is reported. This MOF demonstrates catalytic efficacy in the tandem oxidation and functionalization of styrene utilizing molecular oxygen as a terminal oxidant. The product, a protected 1,2-aminoalcohol, is formed selectively and with high efficiency using this recyclable heterogeneous catalyst. Significantly, the unusual regioselective transformation occurs only when an Fe-decorated Hf 6 node and the Fe-porphyrin strut work in concert. This report is an example of concurrent orthogonal tandem catalysis.

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A Hafnium-Based Metal-Organic Framework as a Nature-Inspired Tandem Reaction Catalyst

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