研究领域
Design and Study of Coordination Catalysts for Small Molecule Conversion
CH4 (and other hydrocarbons) N2, O2, H2O and CO2 are among the most abundant raw materials on Earth. The chemical conversions of these small molecules generate the majority of the World’s energy and materials. However, in spite of over 75 years of research, key fundamental chemistry challenges remain that lead to the generation of substantially more emissions, faster depletion of reserves, higher costs and greater dependence on petroleum than required. The focus of our research is to address these challenges and to design a new generation, Single-Site, coordination catalysts for the direct, selective, low temperature conversion of these molecules that would be substantially more efficient, lower cost and allow the use of abundant CH4 for the production of Energy, Fuels and Chemicals. Our Approach is based on the rational, de novo design of homogeneous, transition metal, (Single-Site) coordination catalysts through an iterative process involving conceptual design, computational study, synthesis, characterization and study of reaction chemistry and mechanisms. Our research interests include catalysts for: CH hydroxylation; N2 fixation, O22 activation, olefin hydration and CO2 reduction.
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"Iridium(III) catalyzed trifluoroacetoxylation of aromatic hydrocarbons." Bischof, Steven M.; Lokare, Kapil S.; Gunsalus, Niles; Yousufuddin, Muhammed; Periana, Roy A. ; Hashiguchi, Brian G. RSC Adv. 2014, 4, 35639-35648.
"Selective CH Functionalization of Methane, Ethane, and Propane by a Perfluoroarene Iodine(III) Complex." Konnick, Michael M.; Hashiguchi, Brian G.; . Devaraja, Deepa; Boaz, Nicholas, C.; Gunnoe, T. Brent; Groves, John T.; Gunsalus, Niles; Ess, Daniel H.; Periana, Roy A. Angew. Chem. Int. Ed. 2014, 53, 10490-10494.
"A Mechanistic Change Results in 100-times faster CH Functionalization for Ethane versus Methane by a Homogeneous Pt Catalyst." Konnick, Michael M.; Bischof, Steven M.; Yousufuddin, Muhammed; Hashiguchi, Brian G.; Ess, Daniel H.; Periana, Roy A. J. Am. Chem. Soc. 2014, 136, 10085–10094.
"Selective Monooxidation of Light Alkanes Using Chloride and Iodate." Fortman, George, C.; Boaz, Nicholas, C.; Munz, Dominik; Konnick, Michael M.; Periana, Roy A.; Groves, John T.; Gunnoe, T. Brent J. Am Chem. Soc., 2014, 136, 8393-8401.
"Making Water the Exciting Way: A Classroom Demonstration of Catalysis." Stowe, Ryan L.; Bischof, Steven M.; Konnick, Michael M.; H?velmann, Claas H.; Leach-Scampavia, Deborah; Periana, Roy A.; Hashiguchi, Brian G. J. Chem. Ed. 2014, 91, 550–553.
"Main group compounds selectively oxidize mixtures of methane, ethane, and propane to alcohol esters." Hashiguchi, Brian G.; Konnick, Michael M.; Bischof, Steven M.; Gustafson, Samantha J.; Devarajan, Deepa; Gunsalus, Niles; Ess, Daniel H.; Periana, Roy A.; Science 2014, 343, 1232-1237.
"Base accelerated generation of N2 and NH3 from an osmium nitride." Konnick, Michael M.; Bischof, Steven M.; Periana.Roy A.; Hashiguchi, Brian G. J. Mol. Cat. A. 2014, 382, 1-7.
"Computational study of carbon–hydrogen bond deprotonation by alkali metal superbases." Pardue, Daniel, B.; Gustafson, Samantha, J.; Periana.Roy A.; Ess, Daniel, H.; Cundari, Thomas, R. Comp. Theor. Chem. 2013, 1019, 85-93.
"Using Reduced Catalysts for Oxidation Reactions: Mechanistic Studies of the “Periana-Catalytica” System for CH4 Oxidation." Mironov, Oleg A.; Bischof, Steven M.; Konnick, Michael M.; Hashiguchi, Brian G.; Goddard, William A., III; Ahlquist, M?rten; Periana.Roy A. J. Am. Chem. Soc. 2013, 135, 14644-14658.
"Cp* Iridium Precatalysts for Selective C-H Oxidation with Sodium Periodate as the Terminal Oxidant." Zhou, Meng; Hintermair, Ulrich; Hashiguchi, Brian G.; Parent, Alexander R.; Hashmi, Sara M.; Elimelech, Menachem;. Periana, Roy A.; Brudvig, Gary W.; Crabtree, Robert H. Organometallics 2013, 32, 957-965.
"Designing Molecular Catalysts for Selective CH Functionalization." Bischof, Steven M.; Hashiguchi, Brian G.; Konnick,Michael M.; Periana, Roy A. Topics in Organometallic Chemistry -Inventing Reactions. Ed. Lukas Goo?en. Springer, New York: 2013, 44, 195-231.
"Highly Active Ru Catalyzed Hydrodefluorination of Aryl and Alkyl Fluorides in Basic Media." Konnick,Michael M.; Bischof, Steven M.; Periana, Roy A.; Hashiguchi, Brian G. Adv. Syn. Catal. 2013, 355, 362-636.
"The para-substituent effect and pH-dependence of the organometallic Baeyer-Villager oxidation of rhenium-carbon bonds." Cheng, Mu-Jeng; Bischof, Steven M.; Nielsen, Robert J.; Goddard, William A., III; Gunnoe, T. Brent; Periana, Roy A. Dalton Trans. 2012, 41, 3758-3763.
"Designing Catalysts for Functionalization of Unactivated C–H Bonds Based on the CH Activation Reaction." Hashiguchi, Brian G.; Bischof, Steven M.; Konnick, Michael, M.; Periana, Roy A.; Acc. Chem. Res. 2012, 45, 885-898.
"Reversible hydrogen storage using CO2 and a proton-switchable iridium catalyst in aqueous media under mild temperatures and pressures" Hull, Jonathan F.; Himeda, Y.; Wang, W.-H.; Hashiguchi, Brian G.; Periana, Roy A.; Szalda. David J.; Muckerman, James T.; Fujita, E. Nature Chem. 2012, 4, 383-388.
"Synthesis and Characterization of the κ2-acac-O,O Complex Os(IV)(acac)2PhCl and Study of CH Activation with Benzene." Young, Kenneth J. H.; Mironov, Oleg A.; Nielsen, Robert J.; Cheng, Mu-Jeng; Stewart, Timothy; Goddard, William A., III; Periana, Roy A. Organometallics 2011, 30, 5088-5094.
"Iridium Complexes Bearing a PNP Ligand, Favoring Facile C(sp3)-H Bond Cleavage." Lokare, Kapil S.; Nielsen, Robert J.; Yousufuddin, Muhammed, Goddard, William A., III; Periana, Roy A. Dalton Trans. 2011, 40, 9094-9097.
"Synthesis of osmium and ruthenium complexes bearing dimethyl (S,S)-2,2'-(pyridine-2,6-diyl)-bis-(4,5-dihydrooxazol-4-carboxylate) ligand and application to catalytic H/D exchange." Young, Kenneth J. H.; Lokare, Kapil S.; Leung, Chin-Hin; Cheng, Mu-Jeng; Nielsen, Robert J.; Petasis, Nicos A.; Goddard, William A., III; Periana, Roy A. J. Mol. Catal. A Chem. 2011, 339, 17-23.
"Functionalization of Rhenium Aryl Bonds by O-Atom Transfer." Bischof, Steven M., Cheng, Mu-Jeng; Nielsen, Robert J.; Gunnoe, T. Brent; Goddard, William A., III; Periana, Roy A. Organometallics 2011, 30, 2079-2082.
"Ligand Lone-pair Influence on Hydrocarbon C-H Activation: A Computational Prespective." Ess, Daniel H.; Gunnoe, T. Brent; Cundari, Thomas R.; Goddard, Willaim A., III; Periana, Roy A. Organometallics 2010, 29, 6801-6815.