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Principles of Chemical Recognition and Transport in Extractive 2011 Separations and Heavy Element Chemistry Research Meeting Hyatt Regency, Baltimore, MD April 26 - 29, 2011 Office of Basic Energy Sciences Chemical Sciences, Geosciences & Biosciences Division Program and Abstracts for the 2011 Separations and Heavy Element Chemistry Research Meeting Hyatt Regency Baltimore, MD April 26–29, 2011 Chemical Sciences, Geosciences, and Biosciences Division Office of Basic Energy Sciences Office of Science U.S. Department of Energy i Cover Graphics: The cover artwork is used by permission from the authors and journals for the associated covers. These covers are related to recently published papers by PIs speaking in this meeting’s program. From left to right and top to bottom they are: Christopher Cahill on p. 19 of this book. Also see C. E. Rowland and C. L. Cahill (2010) "Capturing Hydrolysis Products in the Solid State: Effects of pH on Uranyl Squarates under Ambient Conditions." Inorganic Chemistry, 49(19), 8668–8673. Wibe A. de Jong on p. 77 of this book. Also see V.A. Glezakou and W.A. de Jong, "Cluster-models for Uranyl(VI) adsorption on α-alumina." J. Phys. Chem. A 2011, 115, 1257 (2011). Jaqueline Kiplinger on p. 9 of this book. Also see Thomson, R. K.; Graves, C. R.; Scott, B. L.; Kiplinger, J. L. “Noble Reactions for the Actinides: Safe Gold-Based Access to Organouranium and Azide Complexes,” Eur. J. Inorg. Chem. 2009, 1451–1455. Jaqueline Kiplinger on p. 9 of this book. Also see Cantat, T.; Graves, C. R.; Scott, B. L.; Kiplinger, J. L. “Challenging the Metallocene Dominance in Actinide Chemistry with a Soft PNP Pincer Ligand: New Uranium Structures and Reactivity Patterns,” Angew. Chem., Int. Ed. 2009, 48, 3681–3684. Copyright Wiley-VCH Verlag GmbH & Co.KGaA. Reproduced with permission. Jonathan Sessler on p. 17 of this book. Also see Rambo, B. M.; Sessler, J. L. “Oligopyrrole Macrocycles: Receptors and Chemosensors for Potentially Hazardous Materials,” Chem. Eur. J., in press. James Wishart on p. 3 of this book. Also see Wishart, J. F., “Ionic Liquids and Ionizing Radiation: Reactivity of Highly Energetic Species,” J. Phys. Chem. Lett. 2010, 1, 3225–3231. http://dx.doi.org/10.1021/jz101096b. This document was produced under contract number DE-AC05-06OR23100 between the U.S. Department of Energy and Oak Ridge Associated Universities. The research grants and contracts described in this document are supported by the U.S. DOE Office of Science, Office of Basic Energy Sciences, Chemical Sciences, Geosciences and Biosciences Division. ii Foreword This abstract booklet provides a record of the eleventh U.S. Department of Energy contractors’ meeting in separations sciences and the sixth in heavy element chemistry. This year the meeting is co-chaired by Dr. Lynda Soderholm (Argonne National Laboratory) and Professor Sue Clark (Washington State University). The Chemical Sciences, Geosciences and Biosciences Division of the Office of Basic Energy Sciences and its predecessors have sponsored research in heavy element chemistry and separations sciences for some sixty years. Although these are distinct disciplines, they have much in common for many reasons, in particular because novel separations research is needed to produce pure heavy-element samples and because heavy element chemistry provides the basis for many separations processes. In addition, separation processes are major industrial sources of energy consumption and waste generation. This is the fifth joint meeting of these programs. The objective of this meeting is to provide a fruitful environment in which researchers with common interests will present and exchange information about their activities, will build collaborations among research groups with mutually reinforcing strengths, will identify needs of the research community, and will focus on opportunities for future research directions. The agenda includes invited talks, oral presentations, as well as invited and regular posters, organized so that papers in related disciplines are loosely clustered together. Invited presentations this year include oral and poster presentations representing an Energy Frontier Research Center and related programs in DOE Office of Nuclear Energy. With ample time for discussion and interactions, we emphasize that this is an informal meeting for exchange of information and building of collaborations; it is not a review of researchers’ achievements or a forum to choose future directions. We are pleased to collaborate with Lynda Soderholm and Sue Clark in organizing this joint meeting and appreciate their service to this community. We also appreciate the privilege of serving as the managers of our respective research programs. In carrying out these tasks, we learn from the achievements and share the excitement of the research of the many sponsored scientists and students whose names appear on the papers in the following pages. We also hope that this meeting will enhance your research efforts and will nurture future collaborations and initiatives. We thank all of the researchers whose dedication and innovation have advanced our research and made this meeting possible and, we hope, productive. We also hope that all of you will build on your successes and that we will assemble in two years for our next joint meeting. We thank Diane Marceau of the Chemical Sciences, Geosciences and Biosciences Division, and Tim Ledford and Connie Lansdon of the Oak Ridge Institute for Science and Education for their important contributions to the technical and logistical features of this meeting. Larry A. Rahn Mark Pederson Norman Edelstein iii Agenda 2011 Separations and Heavy Element Chemistry Research Meeting Hyatt Regency, Baltimore, MD, April 26–29, 2011 Tuesday, April 26, 2011 3:00 – 6:00 p.m. *** Registration *** 6:00 – 7:00 *** Reception (hors d'œuvres) *** Session 1 – Separations – Chuan He, Chair 7:10 – 7:20 p.m. Welcome – John Miller, Larry Rahn, Lynda Soderholm and Sue Clark 7:20 – 8:10 Invited speaker – Bruce Moyer – Sigma Team for Minor Actinide Separations 8:10 – 8:35 James Wishart – An Integrated Basic Research Program for Advanced Nuclear Energy Systems based on Ionic Liquids 8:35 – 9:00 Mark Jensen – Multi-stage Separation of Actinides with Biomolecules Wednesday, April 27 7:30 – 8:00 a.m. *** Breakfast *** 8:10 – 8:35 Eric Rohlfing – DOE Update Session 2 – Complexation and Coordination – William Evans, Chair 8:35 – 9:00 a.m. Jaqueline Kiplinger – Organometallic Actinide Chemistry – Metal-Ligand Multiple Bonding and Electron Correlation 9:00 – 9:25 Wayne Lukens – Fundamental Chemistry of Technetium in Iron Oxide Matrices 9:25 – 9:50 Lynn Francesconi – Fundamental Chemistry of Technetium-99 Incorporated into Metal Oxide, Phosphate and Sulfide Materials: Towards Stabilization of Low Valent Technetium 9:50 – 10:15 Jonathan Sessler – Ion Pair Receptors: Fundamental Studies and Tests 10:15 – 10:45 *** Break *** Session 3 – Complexation and Coordination – Thomas Albrecht-Schmitt, Chair n+ 10:45 – 11:10 a.m. Christopher Cahill – Control of Hydrothermal UO2 Systems: A Solution Phase Approach to New Solid State Materials 11:10 – 11:35 Trevor Hayton – Exploring the Redox and Oxo Substitution Chemistry of the Uranyl Ion: Implications for Separations and Environmental Remediation 11:35 – 12:00 Andrew Gaunt – Molecular Transuranic Discovery Science: Underpinning National Energy Security and Waste Remediation Needs 12:00 – 1:00 p.m. *** Working lunch *** Session 4 – Actinides – Lynda Soderholm, Chair 1:00 – 1:50 p.m. Invited speaker – Peter Burns – Energy Frontier Research Center: Materials Science of Actinides 1:50 – 2:15 Richard Wilson – Structural, and Chemical Properties of Lower Valent Actinide Complexes 2:15 – 2:40 Udo Becker – Actinide Incorporation and Radiation Effects in Layered-Structures 2:40 – 3:05 Kenneth Raymond – Actinide/Lanthanide Luminescence and Actinide Sequestration iv Invited Poster Introductory Presentations 3:05 – 3:10 p.m. Tori Forbes – Synthesis and Structural Characterization of Heterometallic Actinide Nanoclusters 3:10 – 5:00 *** Interaction time and put up posters for both poster sessions *** Session P1 – Poster Session 1 5:00 – 6:00 p.m. P1 Invited – Tori Forbes – Synthesis and Structural Characterization of Heterometallic Actinide Nanoclusters P3 Paula Diaconescu – C-H Activation Reactions by Uranium Alkyl Complexes P5 Guokui Liu – Electronic Interactions in Actinyl Compounds: Analysis and Simulation of Optical Spectra P7 Lætitia Delmau – Principles of Chemical Recognition and Transport in Extractive Separations, Calix[4]pyrrole Derivatives: Simple Dual Host or Ion-Pair Receptor? Thermodynamic Study of Anion Selectivity in Cesium Salt Extraction P9 Thomas Albrecht-Schmitt – Actinide Borates P11 Ken Czerwinski – Low Valent Technetium Acetate and Technetium Halide Metal-Metal Bonded Dimers Synthesized by Hydro-Solvothermal and Chemical Transport P13 Chuan He – Selective Recognition of Heavy Elements by Protein-Based Reagents P15 Robert Paine – Preorganized and Immobilized Ligands for Metal Ion Separations P17 Heino Nitsche – Heavy Element Nuclear and Radiochemistry P19 Invited – James Willit – Reproducible and Reliable Electrochemical Determination of U and TRU Concentrations P21 S. Skanthakumar – Correlations between Structure, Magnetism, and Electronic Properties in Neptunium Compounds P23 Sheng Dai – Tailoring Ionic Liquids for "Smart" Separation of Metal Ions P25 Ilya Shkrob – Ionic Liquid Based Extraction Systems: From Mechanistic Aspects of Radiation Stability to Separations Chemistry P27 Michael Morse – Spectroscopy of Organometallic
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