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A review of contemporary actinide research that focuses on new advances in experiment and theory, and the interplay between these two realms
Experimental and Theoretical Approaches to Actinide Chemistry offers a comprehensive review of the key aspects of actinide research. Written by noted experts in the field, the text includes information on new advances in experiment and theory and reveals the interplay between these two realms. The authors offer a multidisciplinary and multimodal approach to the nature of actinide chemistry, and explore the interplay between multiple experiments and theory, as well as between basic and applied actinide chemistry.
The text covers the basic science used in contemporary studies of the actinide systems, from basic synthesis to state-of-the-art spectroscopic and computational techniques. The authors provide contemporary overviews of each topic area presented and describe the current and anticipated experimental approaches for the field, as well as the current and future computational chemistry and materials techniques. In addition, the authors explore the combination of experiment and theory. This important resource:
Written for academics, students, professionals and researchers, this vital text contains a thorough review of the key aspects of actinide research and explores the most recent advances in experiment and theory.
Autorentext
Edited by John K. Gibson, is Senior Scientist, Lawrence Berkeley National Laboratory, USA. He is experienced in fundamental actinide chemistry research, ranging from solid state synthesis of transuranium compounds to actinide chemistry in the gas phase. Wibe A. de Jong, is Senior Scientist, Lawrence Berkeley National Laboratory, USA. He has years of experience in advancing fundamental actinide chemistry research, and in developing and using a variety of computational chemistry approaches.
Inhalt
List of Contributors xi Preface xiii 1 Probing Actinide Bonds in the Gas Phase: Theory and Spectroscopy 1 Michael C. Heaven and Kirk A. Peterson 1.1 Introduction 1 1.2 Techniques for Obtaining Actinide?]Containing Molecules in the Gas Phase 2 1.3 Techniques for Spectroscopic Characterization of Gas?]Phase Actinide Compounds 5 1.3.1 Conventional Absorption and Emission Spectroscopy 5 1.3.2 Photoelectron Spectroscopy 6 1.3.3 Velocity Modulation and Frequency Comb Spectroscopy 6 1.3.4 LIF Spectroscopy 7 1.3.5 Two?]Photon Excitation Techniques 12 1.3.6 Anion Photodetachment Spectroscopy 15 1.3.7 Action Spectroscopy 17 1.3.8 Bond Energies and Reactivities from Mass Spectrometry 20 1.4 Considerations for Characterizing Actinide?]Containing Molecules in the Gas Phase by Ab Initio Methods 23 1.4.1 Electron Correlation Methods 24 1.4.2 Relativistic Effects 27 1.4.3 Basis Sets 29 1.5 Computational Strategies for Accurate Thermodynamics of Gas?]Phase Actinide Molecules 30 1.6 Ab Initio Molecular Spectroscopy of Gas?]Phase Actinide Compounds 34 1.6.1 Pure Rotational and Ro?]Vibrational Spectroscopy 34 1.6.2 Electronic Spectroscopy 37 1.7 Summary and Outlook 38 Acknowledgments 39 References 39 2 Speciation of Actinide Complexes, Clusters, and Nanostructures in Solution 53 Rami J. Batrice, Jennifer N. Wacker, and Karah E. Knope 2.1 Introduction 53 2.2 Potentiometry 54 2.2.1 Potentiometric Titrations to Reveal Speciation 54 2.2.2 Overview of Potentiometry in Aqueous Actinide Chemistry 59 2.3 Optical Spectroscopy 60 2.3.1 UV?]vis?]NIR Spectroscopy in Actinide Speciation 60 2.3.2 Fluorescence Spectroscopy 63 2.3.3 Overview of Optical Spectroscopy in Aqueous Actinide Speciation 68 2.4 NMR Spectroscopy 69 2.4.1 Probing Chemical Equilibria by NMR 69 2.4.2 Monitoring Product Formation/Evolution by NMR Spectroscopy 74 2.4.3 Monitoring Actinide Self?]Assembly by NMR Spectroscopy 75 2.4.4 Following Cluster Stability in Solution by NMR Spectroscopy 76 2.4.5 Overview of NMR Spectroscopy in Aqueous Actinide Chemistry 82 2.5 Raman Spectroscopy 82 2.5.1 Cluster Formation and Assembly 83 2.5.2 Spectral Deconvolution of Raman Data to Yield Speciation 85 2.5.3 Identifying the Nature of Cation-Cation Interactions in Solution 86 2.5.4 In the Absence of an "yl": Pa(V) Speciation in HF Solutions 89 2.5.5 Computational Assignment of Vibrational Spectra 92 2.5.6 Overview of Raman Spectroscopy 92 2.6 X?] ray Absorption Spectroscopy 93 2.6.1 EXAFS 94 2.6.2 Actinide Solution Speciation by EXAFS 95 2.6.3 EXAFS Structural Comparison of Complexes with Varying Oxidation States and Geometries 99 2.6.4 Overview of EXAFS 101 2.7 Small?] Angle X?]ray Scattering (SAXS) 102 2.7.1 Structure Elucidation by SAXS 102 2.7.2 SAXS Analysis of Cluster Evolution 104 2.7.3 Understanding Self?]Assembly Processes by SAXS 107 2.7.4 Overview of SAXS 110 2.8 High?] Energy X?]ray Scattering (HEXS) 110 2.8.1 Determining Coordination Number and Environment about a Metal Center 111 2.8.2 Deducing Metal-Ligand Coordination Modes 113 2.8.3 Following Oligomer Formation and Stability 116 2.8.4 Overview of HEXS 117 References 118 3 Complex Inorganic Actinide Materials 128 Matthew L. Marsh and Thomas E. Albrecht?]Schmitt 3.1 Introduction 128 3.2 Fluorides 129 3.2.1 Trivalent and Tetravalent Fluorides 129 3.2.2 Pentavalent and Hexavalent Fluorides 131 3.2.3 Fluoride Architectures 132 3.3 Borates 137 3.3.1 Functionalized Borates 138 3.3.2 Transuranic Borates 141 3.4 Sulfates 154 3.4.1 Thorium and Uranium 154 3.4.2 Transuranic Frameworks 162 3.5 Phosphates 167 3.6 Conclusion 176 References 176 4 Organometallic Actinide Complexes with Novel Oxidation States and Ligand Types 181 Trevor W. Hayton and Nikolas Kaltsoyannis 4.1 Introduction 181 4.2 Overview of Actinide Organometallic Chemistry 181 4.2.1 Overview of Thorium Organometallics 183 4.2.2 Overview of Uranium Organometallics 184 4.2.3 Overview of Transuranium Organometallics 184 4.3 Overview of Theoretical Methods 184 4.4 New Theoretical and Experimental Tools for Evaluating Covalency in the 5f Series 186 4.4.1 The Quantum Theory of Atoms?]in?]Molecules 186 4.4.2 Ligand K?]edge X?]ray Absorption Spectroscopy 187 4.4.3 Optical Spectroscopy 189 4.4.4 Nuclear Magnetic Resonance (NMR) Spectroscopy 191 4.4.5 Electrochemistry 192 4.5 Notable Discoveries in Actinide?]Carbon Chemistry 194 4.5.1 An(II) Complexes 195 4.5.2 pi?]Acceptor Ligand Complexes 195 4.5.3 (Inverted) Arene Sandwich Complexes 198 4.5.4 Phosphorano?]Stabilized Carbene Complexes 199 4.5.5 Homoleptic Alkyl and Aryl Complexes 201 4.6 Single and Multiple Bonding between Uranium and Group 15 Elements 202 4.7 Complexes with Group 16 Donor Ligands 206 4.7.1 Terminal Mono?]oxo Complexes 206 4.7.2 Complexes with Heavy Chalcogen (S, Se, Te) Donors 207 4.8 Actinyl and Its Derivatives 210 4.8.1 Inverse Trans Influence (ITI) 211 4.8.2 Imido?]Substituted Analogues of Uranyl 212 4.8.3 Progress Toward the Isolation of a cis?]Uranyl Complex 216 4.9 Organoactinide Single?]Molecule Magnets 217 4.10 Future Work 219 Acknowledgments 220 References 220 5 Coordination of Actinides and the Chemistry Behind Solvent Extraction 237 Aurora E. Clark, Ping Yang, and Jenifer C. Shafer 5.1 Introduction 237 5.2 Overview of Separations Processes 238 5.2.1 Classic Processes - U/Pu Recovery 238 5.2.2 Advanced Separation Processes - Am/Cm Recovery 240 5.2.3 Aqueous?]Based Complexants for Trivalent An/Ln Separation 240 5.2.4 Recent Trends in Aqueous?]Based Trivalent An/Ln Separations 241 5.2.5 Separation of Hexavalent Actinides (SANHEX) Processes 241 5.3 C…