Meeting of the Catalysis Science Program Chemical Sciences, Geosciences and Biosciences Division Office of Basic Energy Sciences U.S. Department of Energy Annapolis, Maryland June 1‐4, 2010 This document was produced under contract number DE-AC05-060R23100 between the U.S. Department of Energy and Oak Ridge Associated Universities. FOREWORD The 2010 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 June 1 through June 4, 2010, 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 OBES emphasize fundamental research aimed at initially understanding and finally controlling the chemical reactivity of matter in all its states. The long-term goal of this research is to discover fundamental principles and produce ever more insightful approaches to predict structure-reactivity relations. Such knowledge, integrated with advances in chemical and materials synthesis, in situ analytical instrumentation, and chemical kinetics and dynamics methods, will allow the control of chemical reactions along desired pathways. Ultimately, this new knowledge should impact the efficiency of conversion of natural resources (mass and energy) into fuels, chemicals, materials, or other forms of energy, while minimizing the impact to the environment. 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 OBES 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. Richard Kemp1, Elena Rybak-Akimova2 and Raul Miranda3 1 University of New Mexico and Sandia National Laboratory 2 Tufts University 3 Office of Basic Energy Sciences - U.S. Department of Energy i MEETING OVERVIEW 2010 DOE/BES Catalysis Sciences Meeting June 1–4, 2010 Annapolis, MD Time Tuesday, June 1 Wednesday, June 2 Thursday, June 3 Friday, June 4 Breakfast Breakfast Breakfast 7:00 AM Outside Senate A&B Outside Senate A&B Outside Senate A&B 8:30 Wednesday morning session Thursday morning session Friday morning session Capitol D Capitol D Capitol D 11:15 Working lunch noon Lunch 12:20 PM Lunch Outside Senate A&B Outside Senate A&B 1:00 Poster take-down Meeting adjourns 3:00 Networking Registration/Poster setup Networking Outside Senate A&B (until 6:00) 5:00 Reception Dinner Dinner Capitol C&D Capitol B&C Capitol B&C 6:00 Dinner Capitol C&D 6:15 Wednesday evening session Thursday evening session Capitol D Capitol D 7:00 Tuesday evening session Capitol C&D 8:20 Social hour / Social hour / Poster session II: Poster session III: even-numbered posters all posters Senate A&B Senate A&B 8:40 Social hour/Poster session I: odd-numbered posters Senate A&B ii AGENDA Tuesday Evening, 1 June 2010 Registration: 3:00 – 6:00 (Outside Senate A&B) Reception: 5:00 – 6:00 (Capitol C&D) Dinner: 6:00 – 7:00 (Capitol C&D) Session Chair: Thomas Rauchfuss 7:00 – 7:10 Welcoming Remarks 7:10 – 7:55 Invited Speaker: William Tolman (U Minnesota) Mechanistic Insights Into O2 and N2O Activation By Copper Complexes 7:55 – 8:40 Invited Speaker: Licheng Sun (Royal Inst Techn (KTH) Sweden) Bioinspired Molecular Catalysts for Efficient Water Oxidation Driven by Visible Light and Mechanism for O-O Bond Formation 8:40 – 10:00 Social Hour / Poster Session I (Senate A&B) Wednesday Morning, 2 June 2010 7:00 – 8:15 Breakfast (Outside Senate A&B) Session Chair: Ayusman Sen (Capitol D) 8:30 – 9:15 Invited Speaker: Philip Power (UC-Davis) Activation of Hydrogen under Ambient Conditions by Main Group Molecules 9:15 – 9:50 Dan DuBois (PNNL) A Modular Energy-Based Approach to Molecular Catalyst Design 9:50 – 10:15 Coffee Break (Outside Senate A&B) 10:15 – 10:50 Keith Woo (Iowa State U) Organometallic Chemistry and Catalysis on Metal Surfaces 10:50 – 11:25 John Hartwig (U Illinois) Chemistry of Complexes with Transition Metal-Heteroatom Bonds: Novel Insertion Chemistry and X-H Bond Activation 11:25 – 12:05 Morris Bullock (PNNL) Center for Molecular Electrocatalysis; and Brent Gunnoe (Virginia) Center for Catalytic Hydrocarbon Functionalization Overview of New Energy Frontier Research Centers 12:20 Lunch (Outside Senate A&B) iii Wednesday Evening, 2 June 2010 5:00 – 6:00 Dinner (Capitol B&C) Session Chair: Shannon Stahl (Capitol D) 6:15 – 7:00 Invited Speaker: Andrew Bocarsly (Princeton U) The Electrocatalyzed Conversion of Carbon Dioxide and Water to Alcohols 7:00 – 7:35 Roy Periana (Scripps Res Inst) Low Oxidation State Catalysts for Oxidation Reactions: Overcoming the Seeming Dilemma and Realizing the Advantages 7:35 – 7:45 Break (Outside Senate A&B) 7:45 – 8:20 Invited Speaker: Nancy Jackson (SNL, ACS President-Elect) Changing Paradigms in the Chemical Sciences 8:20 – 10:00 Social Hour / Poster Session II (Senate A&B) Thursday Morning, 3 June 2010 7:00 – 8:15 Breakfast (Outside Senate A&B) Session Chair: Lawrence Sita (Capitol D) 8:30 – 9:15 Invited Speaker: Gerard van Koten (Utrecht U) Cascade Catalysis and Homogeneous Metal Catalysts 9:15 – 9:40 Christine Thomas (Brandeis U) Early/Late Heterobimetallic Complexes Linked by Phosphinoamide Ligands: Rational Tuning of Redox Potentials and Capacity for Small Molecule Activation 9:40 – 10:05 Wendy Shaw (PNNL) Enhancing Hydrogen Production and Oxidation Catalysts with Proton Channels 10:05 – 10:40 Coffee Break (Outside Senate A&B) 10:40 – 11:15 Daniel Mindiola (Indiana U) Low-Coordinate and Terminal Nitrido Complexes of Vanadium and Titanium for N-atom Transfer Chemistry 11:15 – 11:40 John Berry (U Wisconsin) Catalytic C–H Functionalization: Synthesis of Intermediate Analogs and Tuning the Redox Properties of New Catalysts 12:00 Lunch (Outside Senate A&B) iv Thursday Evening, 3 June 2010 5:00 – 6:00 Dinner (Capitol B&C) Session Chair: Richard Finke (Capitol D) 6:15 – 7:00 Invited Speaker: Vincent Artero (Commissariat à l'Energie Atomique et aux Energies Renouvelables (CEA), France) From Hydrogenase Mimics to Noble-Metal Free Hydrogen-Evolving Electrocatalytic Nanomaterials 7:00 – 7:35 Guy Bertrand (UC-Riverside) Transition-Metal-Catalyzed Hydroamination of Non-activated Carbon- Carbon Multiple Bonds with Ammonia 7:35 – 7:45 Break (Outside Senate A&B) 7:45 – 8:20 Gerard Parkin (Columbia U) Fundamental Studies of Metal Centered Transformations Relevant to Catalysis 8:20 – 10:00 Social Hour / Poster Session III (Senate A&B) Friday Morning, 4 June 2010 7:00 – 8:15 Breakfast (Outside Senate A&B) Session Chairs: Elena Rybak-Akimova and Richard Kemp (Capitol D) 8:30 – 9:15 Invited Speaker: Philip Jessop (Queens U) Persuading CO2 to be Useful 9:15 – 9:50 John Bercaw (Caltech) Synthetic and Mechanistic Investigations of Olefin Polymerization Catalyzed by Early Transition Metal Compounds 9:50 – 10:00 Coffee Break (Outside Senate A&B) 10:00 – 10:35 Richard Kemp (U New Mexico/SNL) Direct Partial Oxidations Using Molecular Oxygen 10:35 – 11:00 Theodore Betley (Harvard U) New Methods for Small Molecule Activation 11:15 – 1:00 Working lunch: Future directions for the program. Discussion and conclusions. v vi Table of Contents Foreword ...................................................................................................i Meeting Overview .....................................................................................ii Agenda .................................................................................................... iii Table of Contents .................................................................................... vii Tuesday Evening Session Invited Speaker: William Tolman – Mechanistic Insights into O2 and N2O Activation by Copper Complexes .................................................................... 1 Invited Speaker: Licheng Sun – Bioinspired Molecular Catalysts for Efficient Water Oxidation Driven by Visible Light and Mechanism for O-O Bond Formation... 2 Wednesday Morning Session Invited Speaker: Philip Power – Activation of Hydrogen under Ambient Conditions by Main Group Molecules ............................................................... 3 Dan DuBois – A Modular Energy-Based Approach to Molecular Catalyst Design...... 6 Keith Woo – Organometallic Chemistry and Catalysis on Metal Surfaces............. 12 John Hartwig – Chemistry of Complexes with Transition Metal-Heteroatom Bonds: Novel Insertion Chemistry and X-H Bond Activation ............................. 14 Morris Bullock – Overview of the Center for Molecular Electrocatalysis ............... 17 Brent Gunnoe – Development of Transition Metal Catalysts for the Functionalization of Carbon-Hydrogen Bonds: Fundamental Studies of Catalytic Hydroarylation of Olefins ................................................................ 18 Wednesday Evening Session Invited Speaker: Andrew Bocarsly – The Electrocatalyzed Conversion of Carbon Dioxide and Water to Alcohols........................................................... 22 Roy Periana – Low Oxidation State Catalysts