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Heterogenizing Homogeneous Catalysts through Covalent Integration into Porous Materials:
Challenges and Opportunities

Professor SonBinh T. Nguyen
Professor of Chemistry and Director of the Integrated Science Program
Department of Chemistry
Northwestern University
Evanston IL 60208-3113

Institute for Atom-Efficient Chemical Transformations
Argonne National Laboratory
Argonne, IL, 60439

Nguyen Group Website

Abstract

As hybrid materials derived from well-defined molecular building blocks, newly emerged porous materials such as metal-organic frameworks (MOFs) and porous organic polymers (POPs) have many of the desirable features of zeolites, such as high surface area and porosity, and can be similarly effective in size- and shape-selective catalysis.¹  However, given the enormous diversity of potential structures and chemical functional groups that can be incorporated into the pores of MOFs and POPs, these porous materials have the potential to extend catalysis far beyond the realm of zeolitic chemistry to include enzyme-like behaviors such as adapted flexibility during catalysis, substrate pre-concentration effects,² active-site isolation and protection,³ and tunable hydrophobicity.⁴  This presentation will discuss recent advances achieved by the groups at Northwestern University and Argonne National Laboratory in the integration of homogeneous catalysts into MOFs and POPs.

¹    “Metal organic framework materials as catalysts”  Lee, J. Y.; Farha, O. K.; Roberts, J.; Scheidt, K. A.; Nguyen, S. T.; Hupp, J. T.  Chem. Soc. Rev. 2009, 38, 1450-1459. 

²    “A catalytically active, permanently microporous MOF with metalloporphyrin struts”  Schultz, A. M.; Farha, O. K.; Hupp, J. T.; Nguyen, S. T.  J. Am. Chem. Soc. 2009, 131(12), 4204-4205. 

³    “A Metal-Organic Framework Material that Functions as an Enantioselective Catalyst for Olefin Epoxidation”  Cho, S.-H.; Ma, B.; Albretch-Schmidt, T. A.; Nguyen, S. T.; Hupp, J. T.  Chem Commun. 2006, 2563-2565.

⁴    a) “Selective bifunctional modification of a non-catenated metal-organic framework material via “click” chemistry”  Gadzikwa, T.; Farha, O. K.; Malliakas, C. D.; Kanatzidis, M. G.; Hupp, J. T.; Nguyen, S. T.  J. Am. Chem. Soc. 2009, 131(38), 13613-13615.  b) “Covalent surface modification of a metal-organic framework:  Selective surface engineering via Cu^I-catalyzed Huisgen cycloadditions”.  Gadzikwa, T.; Lu, G.; Stern, C. L.; Wilson, S. R.; Hupp, J. T.; Nguyen, S. T.  Chem. Commun. 2008, 5493-5495.