研究领域
Catalysis science, energy, materials and nanoscience
Catalytic materials are central to most industrial processes. We develop novel designs and syntheses of catalysts, adsorbents, and other functional materials especially for the purpose of more sustainable routes to important chemicals and fuels. We frequently collaborate with industry and national laboratories on such projects. We typically synthesize materials by modifying existing particle or MOF surfaces with organic functionalities (e.g. amines or carboxylates), inorganic complexes (e.g. Mn triazacyclononane, Ta calixarenes) or we build up additional, ultra-thin oxide layers. These groups are intended to control isolated or cooperative active sites consisting of acids, bases, redox groups, metals, and designed cavities in ways that can be difficult to engineer with traditional homogeneous or heterogeneous catalysts. The active sites on these new materials are also functional models for spectroscopy and simulation for the development of improved structure-function relationships. It is our guiding hypothesis that increasing control over - and diversity of - the active sites available for heterogeneous catalysts promises to yield new, more selective, and better understood chemical transformations. We have developed supported metal nanoparticle catalysts, oxide catalysts, immobilized molecular catalysts, and nanocavity catalysts. Chemical transformations currently being explored include selective oxidation, NO reduction, hydrotreating (hydrodenitrogenation and hydrodeoxygenation), photocatalysis, CO2 photoreduction, carbon capture and conversion, aldol condensation and related reactions, sugar and other biomass conversions, dehydration, decarboxylation, and selective adsorption of butanol and other molecules. An overarching long-term goal is to be able to design systems of active sites on a single surface capable of complex, efficient transformations of challenging molecules, in ways that mimic the connectivity of biological reaction pathways.
近期论文
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AS Rosen, JM Notestein, RQ Snurr, "Comparing GGA, GGA+U, and meta-GGA functionals for redox-dependent binding at open metal sites in metal–organic frameworks", The Journal of Chemical Physics 2020 [Link]
AS Rosen, JM Notestein, RQ Snurr, "High‐Valent Metal–Oxo Species at the Nodes of Metal–Triazolate Frameworks: The Effects of Ligand Exchange and Two‐State Reactivity for C−H Bond Activation", Angewandte Chemie 2020 [Link]
PA Ignacio-de Leon, M Ferrandon, LM Savereide, SL Nauert, J Moncada, R Klet, K Chapman, M Delferro, J Camacho-Bunquin, CA Carrero, JM Notestein, ST Nguyen, "Promoter Effects on Catalyst Selectivity and Stability for Propylene Partial Oxidation to Acrolein", Catalysis Letters 2020 [Link]
AS Rosen, MR Mian, T Islamoglu, H Chen, OK Farha, JM Notestein, RQ Snurr, "Tuning the Redox Activity of Metal–Organic Frameworks for Enhanced, Selective O2 Binding: Design Rules and Ambient Temperature O2 Chemisorption in a Cobalt–Triazolate Framework", Journal of the American Chemical Society 2020 [Link]
S Ahn, SL Nauert, KE Hicks, MA Ardagh, NM Schweitzer, OK Farha, JM Notestein, "Demonstrating the critical role of solvation in supported Ti and Nb epoxidation catalysts via vapor-phase kinetics", ACS Catalysis 2020 [Link]
L Savereide, A Gosavi, KE Hicks, JM Notestein, "Identifying properties of low-loaded CoOX/CeO2 via X-ray absorption spectroscopy for NO reduction by CO", Journal of Catalysis 2020 [Link]
E Cheng, L McCullough, H Noh, OK Farha, JT Hupp, JM Notestein, "Isobutane Dehydrogenation over Bulk and Supported Molybdenum Sulfide Catalysts", Industrial & Engineering Chemistry Research 2020 [Link]
M Barona, S Ahn, W Morris, WJ Hoover, JM Notestein, OK Farha, RQ Snurr, "Computational Predictions and Experimental Validation of Alkane Oxidative Dehydrogenation by Fe2M MOF Nodes", ACS Catalysis 2019 [Link]
IS Kim, S Ahn, NA Vermeulen, TE Webber, LC Gallington, KW Chapman, RL Penn, JT Hupp, OK Farha, JM Notestein, AB Martinson, "The Synthesis Science of Targeted Vapor-Phase Metal–Organic Framework Postmodification" Journal of the American Chemical Society 2019 [Link]
Z Bo, LR McCullough, S Dull, MA Ardagh, J Wang, J Notestein, "Strong electrostatic adsorption of Pt onto SiO2 partially overcoated Al2O3—Towards single atom catalysts", The Journal of Chemical Physics 2019 [Link]
A.R. Kim, S. Ahn, T.U. Yoon, J.M. Notestein, O.K. Farha, Y.S. Bae, "Fast Cyclohexane Oxidation Under Mild Reaction Conditions Through a Controlled Creation of Redox‐Active Fe (II/III) Sites in a Metal− Organic Framework", ChemCatChem 2019 [Link]
Bennett, C.K., Bhagat, M.N., Zhu, Y., Yu, Y., Raghuraman, A., Belowich, M.E., Nguyen, S.T., Notestein, J.M., Broadbelt, L.J., "Strong Influence of the Nucleophile on the Rate and Selectivity of 1, 2-Epoxyoctane Ring-Opening Catalyzed by Tris (pentafluorophenyl) borane, B(C6F5)3". ACS Catalysis 2019 DOI: 10.1021/acscatal.9b02607.
Ignacio-de Leon, P.A., Ferrandon, M., Savereide, L.M., Nauert, S.L., Moncada, J., Klet, R., Chapman, K., Delferro, M., Camacho-Bunquin, J., Carrero, C.A. and Notestein, J.M., "Promoter Effects on Catalyst Selectivity and Stability for Propylene Partial Oxidation to Acrolein". Catalysis Letters. 2019 DOI: 10.1007/s10562-019-02969-3.
Bhagat, M.N., Bennett, C.K., Chang, G.F., Zhu, Y., Raghuraman, A., Belowich, M.E., Nguyen, S.T., Broadbelt, L.J., Notestein, J.M. "Enhancing the regioselectivity of B (C6F5) 3-catalyzed epoxide alcoholysis reactions using hydrogen bond acceptors". ACS Catalysis 2019 DOI:10.1021/acscatal.9b03089
Kim, A.R., Ahn, S., Yoon, T.U., Notestein, J.M., Farha, O.K. and Bae, Y.S.. "Fast Cyclohexane Oxidation under Mild Reaction Conditions through a Controlled Creation of Redox‐active Fe (II/III) Sites in a Metal‐organic Framework". ChemCatChem 2019 DOI:10.1002/cctc.201901050
Liu, C., Nauert, S.L., Alsina, M.A., Wang, D., Grant, A., He, K., Weitz, E., Nolan, M., Gray, K.A. and Notestein, J.M., "Role of surface reconstruction on Cu/TiO2 nanotubes for CO2 conversion". Applied Catalysis B: Environmental. 2019 DOI: 10.1016/j.apcatb.2019.117754 .
Gosavi, A.A., Hedrick, J.L., Chen, PC., Notestein, J.M. and Mirkin, C.A."A tri-layer approach to controlling nanopore formation in oxide supports". Nano Research. 2019 DOI: 10.1007/s12274-019-2332-9
Rosen, A.S., Notestein, J.M. and Snurr, R.Q. "Structure− Activity Relationships that Identify Metal− Organic Framework Catalysts for Methane Activation." ACS Catalysis 2019, DOI: 10.1021/acscatal.8b05178.
Rosen, A. S., Notestein, J. M., & Snurr, R. Q. "Identifying promising metal–organic frameworks for heterogeneous catalysis via high‐throughput periodic density functional theory" Journal of Computational Chemistry 40, 2019 1305‐1318. DOI: 10.1002/jcc.25787