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

Journal Article · Thu Oct 15 00:00:00 EDT 2015 · Journal of the American Chemical Society

DOI:https://doi.org/10.1021/jacs.5b08440· OSTI ID:1392408

Beyzavi, M. Hassan ^[1]; Vermeulen, Nicolaas A. ^[1]; Howarth, Ashlee J. ^[1]; Tussupbayev, Samat ^[2]; League, Aaron B. ^[2]; Schweitzer, Neil M. ^[1]; Gallagher, James R. ^[3]; Platero-Prats, Ana E. ^[4]; Hafezi, Nema ^[1]; Sarjeant, Amy A. ^[1]; Miller, Jeffrey T. ^[5]; Chapman, Karena W. ^[4]; Stoddart, J. Fraser ^[1]; Cramer, Christopher J. ^[2]; Hupp, Joseph T. ^[1]; Farha, Omar K. ^[6]

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1. International Institute for Nanotechnology (IIN) and Center for the Chemistry of Integrated Systems (CCIS), Department of Chemistry, Northwestern University, 2145 Sheridan Road, Evanston, Illinois 60208, United States
2. Department of Chemistry, Chemical Theory Center, and Supercomputing Institute, University of Minnesota, 207 Pleasant Street SE, Minneapolis, Minnesota 55455, United States
3. Chemical Science and Engineering Division, Argonne National Laboratory, 9700 South Cass Avenue, Argonne, Illinois 60439, United States
4. X-ray Science Division, Advanced Photon Source, Argonne National Laboratory, Argonne, Illinois 60439, United States
5. Chemical Science and Engineering Division, Argonne National Laboratory, 9700 South Cass Avenue, Argonne, Illinois 60439, United States; School of Chemical Engineering, Purdue University, 480 Stadium Mall Drive, West Lafayette, Indiana 47906, United States
6. International Institute for Nanotechnology (IIN) and Center for the Chemistry of Integrated Systems (CCIS), Department of Chemistry, Northwestern University, 2145 Sheridan Road, Evanston, Illinois 60208, United States; Department of Chemistry, Faculty of Science, King Abdulaziz University, Jeddah 22254, Saudi Arabia

Tandem catalytic systems, often inspired by biological systems, offer many advantages in the formation of highly functionalized small molecules. Herein, a new MOF with porphyrinic struts and Hf6 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 a Fe-decorated Hf6-node and the Fe-porphyrin strut work in concert. This report is an example of concurrent orthogonal tandem catalysis.

• Research Organization: Argonne National Lab. (ANL), Argonne, IL (United States)
• Sponsoring Organization: USDOE Office of Science (SC), Basic Energy Sciences (BES)
• DOE Contract Number: AC02-06CH11357
• OSTI ID: 1392408
• Journal Information: Journal of the American Chemical Society, Vol. 137, Issue 42; ISSN 0002-7863
• Publisher: American Chemical Society (ACS)
• Country of Publication: United States
• Language: English

Related Subjects

Hf-MOFs
MOF Catalysis
Zr-MOFs
metal organic frameworks
porphyrinic
post-synthesis modification