Gas/Liquid-Phase Catalysis Using MOF-Supported Catalysts

Structural ambiguity of active sites represents a major hurdle for rational catalyst design in heterogeneous catalysis. Using metal–organic frameworks, or MOFs, as the catalyst supports offers a potential solution to this challenge due to their well-defined structures and high crystallinity. Central to our efforts is the use of a zirconium-based MOF featuring a 1,3,6,8-(p-benzoate)pyrene ligand, named NU-1000. Using atomic layer deposition or solvothermal deposition, a wide variety of metal-oxide or -sulfide clusters have been anchored uniformly to the MOF support in large quantity. These clusters can facilitate many shale-gas upgrade processes, including alkane oxidative dehydrogenation, alkene dimerization/oligomerization and selective alkane oxidation to alcohol. Collaborating with other scientists within the Inorganometallic Catalyst Design Center (ICDC) (a Department of Energy-sponsored Energy Frontier Research Center), we aim to elucidate the structure of the active sites of these MOF-supported catalysts using techniques such as synchrotron X-ray absorption and diffraction, microscopic imaging, and computational modeling.

Selected Publications 

Peters, A. W.; Otake, K.; Platero-Prats, A. E.; Li, Z.; DeStefano, M. R.; Chapman, K. W.; Farha, O. K.; Hupp, J. T., Site-Directed Synthesis of Cobalt Oxide Clusters in a Metal-Organic Framework. ACS Appl Mater Interfaces 2018, 10 (17), 15073-15078.
DOI: 
10.1021/acsami.8b02825 

Cui, Y.; Rimoldi, M.; Platero-Prats, A. E.; Chapman, K. W.; Hupp, J. T.; Farha, O. K., Stabilizing a Vanadium Oxide Catalyst by Supporting on a Metal-Organic Framework. ChemCatChem 2018, 10 (8), 1772-1777.
DOI: 10.1002/cctc.201701658

Kim, I. S.; Li, Z.; Zheng, J.; Platero-Prats, A. E.; Mavrandonakis, A.; Pellizzeri, S.; Ferrandon, M.; Vjunov, A.; Gallington, L. C.; Webber, T. E.; Vermeulen, N. A.; Penn, R. L.; Getman, R. B.; Cramer, C. J.; Chapman, K. W.; Camaioni, D. M.; Fulton, J. L.; Lercher, J. A.; Farha, O. K.; Hupp, J. T.; Martinson, A. B. F., Sinter-Resistant Platinum Catalyst Supported by Metal-Organic Framework. Angew Chem Int Ed Engl 2018, 57 (4), 909-913.
DOI: 10.1002/anie.201708092

Li, Z.; Peters, A. W.; Platero-Prats, A. E.; Liu, J.; Kung, C. W.; Noh, H.; DeStefano, M. R.; Schweitzer, N. M.; Chapman, K. W.; Hupp, J. T.; Farha, O. K., Fine-Tuning the Activity of Metal-Organic Framework-Supported Cobalt Catalysts for the Oxidative Dehydrogenation of Propane. J Am Chem Soc 2017, 139 (42), 15251-15258.
DOI: 10.1021/jacs.7b09365

Noh, H.; Cui, Y.; Peters, A. W.; Pahls, D. R.; Ortuno, M. A.; Vermeulen, N. A.; Cramer, C. J.; Gagliardi, L.; Hupp, J. T.; Farha, O. K., An Exceptionally Stable Metal-Organic Framework Supported Molybdenum(VI) Oxide Catalyst for Cyclohexene Epoxidation. J Am Chem Soc 2016, 138 (44), 14720-14726.
DOI: 10.1021/jacs.6b08898