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Frontiers at the Interface of Homogeneous and Heterogeneous Catalysis

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Frontiers at the Interface of Homogeneous and Heterogeneous Catalysis FRONTIERS AT THE INTERFACE OF HOMOGENEOUS AND HETEROGENEOUS CATALYSIS Meeting of the Catalysis Science Program Chemical Sciences, Geosciences and Biosciences Division Office of Basic Energy Sciences U.S. Department of Energy Westin Annapolis Annapolis, Maryland June 30 – July 2, 2013 This document was produced under contract number DE-AC05-060R23100 between the U.S. Department of Energy and Oak Ridge Associated Universities. FOREWORD The 2013 Catalysis Science Program Meeting is sponsored by the Division of Chemical Sciences, Geosciences and Biosciences, Office of Basic Energy Sciences (BES), U.S. Department of Energy. It is being held on June 30 through July 2, 2013, at the Westin Annapolis Hotel, Annapolis, Maryland. The purposes of this meeting are to discuss the recent advances in the chemical, physical, and biological bases of catalysis science, to foster exchange of ideas and cooperation among participants, and to discuss the new challenges and opportunities recently emerging in energy technologies. Catalysis activities within BES emphasize fundamental research aimed at initially understanding and finally controlling the chemical conversion of natural and artificial feedstocks. The long-term goal of this research is to discover fundamental principles and produce ever more insightful approaches to predict structure-reactivity behavior. Such knowledge, integrated with advances in chemical and materials synthesis, in situ and operando analytical instrumentation, and chemical kinetics and quantum chemistry methods, will allow the control of chemical reactions along desired pathways. Ultimately, this new knowledge should impact the efficiency of conversion of natural resources into fuels, chemicals, materials, or other forms of energy, while minimizing the impact to the environment. This year’s meeting is focused on three topical areas: (i) the interface of homogeneous and heterogeneous catalysis, (ii) catalysis for biomass or solar energy conversion, and (iii) molecular catalysis, with an emphasis on organic synthesis. Special thanks go to our invited speakers and guest junior scientists, 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 BES Catalysis Science Program; and to the session moderators, for their invaluable help. We also thank the Oak Ridge Institute for Science and Education staff for the logistical and web support and the compilation of this volume. Christopher Jones1 and Raul Miranda2 1Georgia Institute of Technology 2Office of Basic Energy Sciences - U.S. Department of Energy i This page is intentionally blank. ii AGENDA Sunday Afternoon and Evening, June 30, 2013 10:00 - on Registration 12:00 - 1:00 pm Lunch and Welcoming Remarks Session I, Moderator: Alex Katz (UC Berkeley) 1:00 – 1:40 pm Invited Speaker: Cristophe Copéret (ETH Zürich) “Controlled Functionalization and Molecular Understanding of Surfaces: Towards Supported Single-Site Catalysts and Beyond” 1:40 – 2:10 pm T. Don Tilley (UC Berkeley, LBNL) “Molecular Routes to Single-Site Catalytic Surface Species for Selective Oxidations” 2:10 – 2:40 pm Steven Tait (Indiana Univ.) “Metal/Organic Surface Catalyst for Low-Temperature Methane Oxidation: Bi-Functional Union of Metal-Organic Complex and Chemically Complementary Surface” 2:40 – 3:10 pm Tobin Marks (Northwestern Univ.) “Supported Organometallic Complexes: Surface Chemistry, Spectroscopy, Catalysis and Homogeneous Models” Session II, Moderator: Ted Betley (Harvard University) 3:30 – 4:00 pm Susannah Scott (UC Santa Barbara) “Exploring the Relationship between Homogeneous and Heterogeneous Reaction Kinetics” 4:00 – 4:30 pm Justin Notestein (Northwestern University) “Templating Routes to Supported Oxide Catalysts by Design” 4:30 – 5:00 pm Liviu Mirica (Washington University –St. Louis) “Novel Palladium Catalysts for the Oxidative Oligomerization of Methane & Carbon Dioxide Reduction” 5:00 – 5:30 pm Aaron Appel (PNNL) “An Energy-Based Approach to Bifunctional Molecular Catalysis for CO2 Reduction and Fuel Utilization” 5:30 - 6:30 pm Dinner Session III, Moderator: Brent Gunnoe (University of Virginia) 6:30 – 7:10 pm Invited Speaker: Huw Davies (Emory University) “Center Approach to C-H Functionalization” iii 7:10 – 7:40 pm Dean Toste (UC Berkeley, LBNL) “Selective Reactions of Carbon-Carbon π-Bonds Catalyzed by Cations and Anions” 7:40 – 8:20 pm Invited Speaker: Scott Miller (Yale University) “Asymmetric Catalysis in Complex Molecular Environments” 8:20 – 10:00 pm Poster Session I (Odd Numbers) Monday Morning, July 1 7:00 - 8:15 am Breakfast Session IV, Moderator: Morris Bullock (PNNL) 8:30 - 9:10 am Invited Speaker: Wenbin Lin (Univ. of Chicago) “Metal- Organic Frameworks as Single Site Solid Catalysts” 9:10 - 9:40 am Larry Que (Univ. of Minnesota) “Bio-inspired Nonheme Iron Catalysts for Hydrocarbon Oxidations” 9:40 - 10:10 am John Hartwig (UC Berkeley–LBNL) “Studies on Homogeneous Catalysis for Efficient Synthesis from Chemical Feedstocks” Session V, Moderator: Mahdi Abu-Omar (Purdue University) 10:30 - 11:10 am Invited Speaker: Noritaka Mizuno (Univ. of Tokyo) “Design of Polyoxometalate-Based Molecular Catalysts for Bridging the Gap between Homogeneous and Heterogeneous Catalysis” 11:10 - 11:40 am Harold Kung (Northwestern University) “Nanoconfinement Effects in Heterogeneous Catalysis” 11:40 - 12:10 pm Geoffrey Coates (Cornell University) “Development and Application of New Carbonylation Catalysts: Improvements in Regioselectivity, Stereoselectivity, Activity and Exploration of New Reactions” 12:10 - 12:40 pm Robert Crabtree (Yale University) “Moving to Nonprecious Metal Catalysis” 12:40 – 2:30 pm Lunch - Networking Monday Afternoon, July 1 Session VI, Moderator: Richard Finke (Colorado State University) 2:30 - 3:10 pm Invited Speaker: Alan Goldman (Rutgers Univ.) “Addition of O-H Bonds to Olefins Catalyzed by Pincer-Iridium Complexes” iv 3:10 – 3:40 pm Malcolm Chisholm (Ohio State Univ.) “Developing s-Block Element Catalysis and New Chemical Transformations” 3:40 - 4:10 pm Christopher Marshall (ANL) “Fundamental Understanding and Control of Selectivity and Deactivation in Biomass Conversion Catalysts” 4:10 – 4:40 pm Eugene Chen (Colorado State Univ.) “Catalytic Conversion of Glucose and Cellulose into HMF and Subsequent Upgrading to Value-Added Chemicals and Liquid Fuels” 4:40 – 5:10 pm Raul Lobo (Univ. of Delaware) “Selective Catalytic Dehydration and Hydrodeoxygenation Reactions for the Production of Fuels and Chemicals from Biomass” 5:10 - 6:20 pm Dinner Monday Evening, July 1 Session VII, Moderator: Bruce Gates (UC Davis) 6:20 - 7:00 pm Johannes Lercher (PNNL, T.U. Munich) “Understanding Elementary Steps of Catalytic Conversions in Water to Achieve Complex Transformations” 7:00 - 7:30 pm Suljo Linic (Univ. of Michigan) “Photo-catalysis on Plasmonic Metal Nanoparticles” 7:30 - 8:00 pm Andreas Heyden (Univ. of South Carolina) “Theoretical Investigation of Heterogeneous Catalysis at the Solid-Liquid Interface for the Conversion of Lignocellulosic Biomass Model Molecules” 8:20 - 10:00 pm Poster Session II (Even Numbers) Tuesday Morning, July 2 7:00 - 8:15 am Breakfast Session VIII, Moderator: Robert Waymouth (Stanford University) 8:30 - 9:00 am Jens Nørskov (SLAC, Stanford Univ.) “Theoretical Description of CO2 Reduction” 9:00 - 9:30 am Aditya Bhan (Univ. of Minnesota) “One-Pot Catalytic Conversion of Biomass and Alkanes: Kinetically Coupling Deoxygenation and Dehydrogenation Pathways” 9:30 - 10:00 am Jose Rodriguez (BNL) “Catalysis: Reactivity and Structure” 10:00 - 10:20 am Coffee Break v Session IX, Moderator: Christopher Jones (Georgia Institute of Technology) 10:50 – 11:20 am Zili Wu (ORNL) “Revealing the Surface Structure of Ceria Nanocrystals with Well-Defined Facets” 11:20 – 11:50 am Will Medlin (Univ. of Colorado) “Selectivity Control through Modification of Metal Catalysts with Organic Monolayers” 11:50 - 2:00 pm Lunch and Discussion – Future Directions vi Table of Contents Foreword ..................................................................................................... i Agenda ....................................................................................................... iii Sunday Afternoon, Session I Invited Speaker: Cristophe Copéret – Controlled Functionalization and Molecular Understanding of Surfaces: Towards Supported Single-Site Catalysts and Beyond .................................................................................... 3 T. Don Tilley – Molecular Routes to Single-Site Catalytic Surface Species for Selective Oxidations ...................................................................................... 4 Steven Tait – Metal/Organic Surface Catalyst for Low-Temperature Methane Oxidation: Bi-Functional Union of Metal-Organic Complex and Chemically Complementary Surface ................................................................................. 5 Tobin Marks – Supported Organometallic Complexes: Surface Chemistry, Spectroscopy, Catalysis and Homogeneous Models ............................................ 8 Sunday Afternoon, Session II Susannah Scott – Exploring the Relationship between Homogeneous and Heterogeneous Reaction Kinetics .................................................................... 13 Justin Notestein – Templating Routes to Supported Oxide Catalysts by Design ..... 19 Liviu Mirica – Novel Palladium Catalysts for the Oxidative Oligomerization of Methane & Carbon
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