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Where Are We to Day in the Overlap Between Homogeneous And Frontiers in Molecular Catalysis Science PR 2 X Ir + H2 PR 2 Zeo l i t e (H+ - S Z2 5 ; 25 % w/) > 600 turnovers re f lux, b. p. 20 5 °C up to 99% selectivity Meeting of the Catalysis Science Program Chemical Sciences, Geosciences, and Biosciences Division Office of Basic Energy Sciences U.S. Department of Energy Annapolis, Maryland May 18-21, 2008 Frontiers in Molecular Catalysis Science Meeting of the Catalysis Science Program Chemical Sciences, Geosciences and Biosciences Division Office of Basic Energy Scineces, U. S. Department of Energy Annapolis, MD ─ May 18-21, 2008 Cover figures (top left to bottom right): 1. S. Nguyen, J. Hupp: chiral epoxidation of chromene catalyzed by chiral (salen)Mn in metal organic framework 2. C. Hill, et al.: water oxidation catalyst, Rb8K2[{Ru4O4(OH)2(H2O)4}(γ- SiW10O36)2]·25H2O 3. A. Goldman: tandem dehydrogenation catalysis with a pincer-ligated iridium complex 4. R. Bergman, K. Raymond: “nanovessels” for controlling stereo-, chemo- and/or regioselectivity 5. V. Lin et al.: multifunctional mesoporous nanoparticles for selective catalysis and biofuel applications 6. A. Sygula, P. W. Rabideau: double concave hydrocarbon catcher for buckminsterfullerene C60 This document was produced under contract number DE-AC05-060R23100 between the U.S. Department of Energy and Oak Ridge Associated Universities. FOREWORD The 2008 Catalysis Science Program Meeting is sponsored by the Division of Chemical Sciences, Geosciences and Biosciences, Office of Basic Energy Sciences (OBES), U.S. Department of Energy. It is being held on May 18-21, 2008, at the Doubletree Hotel Annapolis, Annapolis, MD. The purposes of this meeting are to discuss the recent advances in organometallic, inorganic and bioinspired chemistry and catalysis, to foster exchange of ideas and cooperation among participants, and to discuss the new opportunities for catalysis and chemical transformations at the interfaces with other disciplines and technologies, including nanoscience, hydrogen fuel generation and storage, solar energy conversion and bioinspired chemistry. Catalysis activities within OBES emphasize fundamental research aimed at understanding and controlling the chemical reactivity of fluid and condensed matter. The long-term goal of this research is to discover the fundamental principles and develop the techniques to predict structure-reactivity relations. Such knowledge, integrated with advances in synthesis, instrumentation, characterization, and theory, will help us to control chemical reactions along desired pathways. Ultimately, this new knowledge will result in chemical and materials processes to efficiently convert fossil and renewable resources, or to generate, convert and store energy, with minimum impact to our environment. Special thanks go to our invited speakers, who will expose us to recent advances in their fields, to the program investigators and their students, postdocs, and collaborators, for their dedication to the continuous success and visibility of the OBES Catalysis Science Program, and to the session moderators, for their invaluable help. We also thank the Oak Ridge Institute of Science and Education staff, Ms. Margaret Lyday and other contributing staff members of ORISE for the logistical and web support and the compilation of this volume. Andreja Bakac1, Aaron Sadow1, Michael Chen2 and Raul Miranda2 1Ames Laboratory and Department of Chemistry, Iowa State University Ames, IA 2Chemical Sciences, Geosciences and Biosciences Division Office of Basic Energy Sciences U.S. Department of Energy i AGENDA Sunday Evening, 18 May 2008 Session Chair: William Evans (California-Irvine) 5:30 – 6:45 Dinner 7:00 – 7:10 Welcoming Remarks 7:10 – 7:55 Invited Talk: Catalysis by Design: A Predictive Approach of Heterogeneous Catalysis via Surface Organometallic Chemistry Jean-Marie Basset (Laboratoire de Chimie Organométallique de Surface) 7:55 – 8:30 Nanocluster Catalysts Formation and Stabilization Fundamental Studies Richard Finke (Colorado State University) 8:30 – 11:00 Social Hour / Poster Session Odd-Numbered Posters* *All posters may be set up starting on Sunday 4:00 pm, will stay posted during the entire meeting, and must be taken down by Tuesday midnight at the latest. Poster presenters must stand by their poster on Sunday (odd-numbered) and Monday (even-numbered). All poster presenters are encouraged to circulate and interact but be available for questions on the Tuesday session. Tom Autrey - Control of Hydrogen Release and P1 Uptake in Condensed Phases Perla B. Balbuena - Theory-Guided Design of Nano- P3 Nanoscale Multimetallic Nanocatalysts for Fuel Cells Perla B. Balbuena - Modeling Catalyzed Growth of P5 Single-Wall Carbon Nanotubes Robert G. Bergman - Exploratory and Mechanistic P7 Investigations of C-H Activation Reactions and their Applications to Catalysis and Organic Synthesis Theodore A. Betley - New Approaches to Driving P9 Multielectron Redox Chemistry Paul J. Chirik - Understanding Nitrogen Fixation P11 iii Robert H Crabtree - Bifunctional Ligands for En- P13 hanced Selectivity in Organometallic Catalysis Sheng Dai - Colloidal Deposition Synthesis of P15 Supported Gold Nanocatalysts Based on Au-Fe3O4 Dumbbell Nanoparticles for CO Oxidation Jeffrey W. Elam - Atomic Layer Deposition Synthesis P17 of Nanostructured Membrane Catalysts James A. Franz - An Energy-Based Approach to P19 Developing Interfacial Catalysts: Thermochemistry, Kinetics and Theory of Catalytic Transformations Michel R. Gagné - Selective Approaches to the P21 Activation of Carbohydrates T. Brent Gunnoe - Transition Metal Catalyzed P23 Hydro-arylation of Multiple Bonds: Exploration of Second Generation Ruthenium Catalysts and Extension to Copper Systems William D. Jones – Transition Metal Activation and P25 Functionalization of Carbon-Hydrogen Bonds Richard A. Kemp - Direct Epoxidations Using P27 Molecular Oxygen Cora E. MacBeth - Novel Ligand Platforms for P29 Transition Metal Catalyzed C-H Oxidation Reactions Daniel J. Mindiola - Catalytic Prospects Involving P31 the Carboamination and Hydrophosphination of Alkynes Oleg V. Ozerov - Catalysis of C-F activation by P33 Highly Electrophilic Si Compounds Dmitry E. Polyansky - Transition Metal Complexes as P35 Artificial NADH Analogs: Towards Photochemical Reduction of Carbon Dioxide Thomas B. Rauchfuss - Supramolecular Ensembles P37 in Catalysis Lawrence T. Scott - High Temperature Chemistry of P41 Aromatic Hydrocarbons iv Peter C. Stair - Nanostructured Membrane Catalysis P43 T. Don Tilley - Molecular Precursor Methods for the P45 Controlled Generation of Active and Selective Catalytic Sites on an Oxide Surface L. Keith Woo – Gold Metal-Catalyzed Reactions of P47 Isocyanides and CO with Amines and Oxygen Monday Morning, 19 May 2008 Session Chair: Paul Sharp (Missouri-Columbia) 7:00 – 8:15 Breakfast 8:30 – 9:15 Invited Talk: Multifunctional Mesoporous Nanoparticles for Selective Catalysis and Biofuel Applications Victor Lin (Iowa State/Ames Laboratory) 9:15 – 9:50 Transition Metal Mediated Transformations of Small Molecules Ayusman Sen (Pennsylvania State University) 9:50 – 10:20 Coffee Break 10:20 – 10:55 Coordinative Supramolecular Catalysis Joseph Hupp (Northwestern University) 10:55 – 11:30 ‘Flexible’ Heterogenization of (Salen) Mn Complexes for Catalyzing Selective Olefin Epoxidation—Lessons from Homogeneous and Biological Catalysis SonBinh Nguyen (Northwestern University) 11:30 – 11:50 Poster talk: Homolytic and Heterolytic S-H Bond Energies in Homogeneous Mo2S4 Complexes Aaron Appel, Pacific Northwest National Laboratory 12:00 Lunch Monday Evening, 19 May 2008 Session Chair: Paul Chirik (Cornell) 5:00 – 6:00 Dinner v 6:15 – 7:00 Invited Talk: Biocatalysis for Fuels and Industrial Chemicals: Enzymes, Whole Cells and Beyond Doug Cameron (Khosla Ventures, BioOils, LLC) 7:00 – 7:35 Silane Activation on a Single-Site Oxorhenium(V) Oxazoline Catalyst: A New Mechanistic Paradigm for Hydrogen Production and Hydrosilation Mahdi Abu-Omar (Purdue University) 7:35 – 7:45 Break 7:45 – 8:20 Mechanisms of Organometallic Copper Oxidase Reactions Shannon Stahl (University of Wisconsin-Madison) 8:20 – 8:40 Poster talk: Ancillary Oxazolinylboron Ligands for Transition Metal Centers Aaron Sadow (Iowa State/Ames Laboratory) 8:40 – 11:00 Social Hour / Poster Session Even-Numbered Posters Andreja Bakac - Thermodynamics of Oxygen P2 Activation by Transition Metal Complexes Guillermo C. Bazan - Catalysts for Selective Olefin P4 Oligomerization and Polymerization John E. Bercaw - Synthetic and Mechanistic P6 Investigations of Olefin Polymerization Catalyzed by Early Transition Metal Compounds K. N. Raymond, R. G. Bergman - Selective Organic P8 and Organometallic Reactions in Water-Soluble Host-Guest Supramolecular Systems R. Morris Bullock - New Bio-Inspired Molecular P10 Catalysts for Hydrogen Oxidation and Hydrogen Production Malcolm H. Chisholm - Mechanistic and Synthetic P12 Studies Aimed at the Development of Single-Site Metal Alkoxide Catalysts for the Generation of Polyesters and Polycarbonates vi Richard M. Crooks - Understanding Multimetallic P14 Catalysts using Dendrimer-Encapsulated Nano- Particles W. Nicholas Delgass - Catalyst Design by Discovery P16 Informatics – Olefin Polymerization over Single-Site Catalysts William J. Evans - Advancing Chemistry with f P18 Elements Etsuko Fujita - Water Oxidation by a Ruthenium P20 Complex with Non-Innocent Quinone Ligands: Possible Formation of an O−O Bond at a Low Oxidation State of the Metal Alan S. Goldman - Alkane Dehydrogenation and P22 Tandem
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