Interdisciplinary Round-Robin Test on Molecular Spectroscopy of the U(VI) Acetate System

Müller, Katharina; Foerstendorf, Harald; Steudtner, Robin; Tsushima, Satoru; Kumke, Michael U.; Lefèvre, Grégory; Rothe, Jörg; Mason, Harris; Szabó, Zoltán; Yang, Ping; Adam, Christian K.  R.; André, Rémi; Brennenstuhl, Katlen; Chiorescu, Ion; Cho, Herman M.; Creff, Gaëlle; Coppin, Frédéric; Dardenne, Kathy; Den Auwer, Christophe; Drobot, Björn; Eidner, Sascha; Hess, Nancy J.; Kaden, Peter; Kremleva, Alena; Kretzschmar, Jerome; Krüger, Sven; Platts, James A.; Panak, Petra J.; Polly, Robert; Powell, Brian A.; Rabung, Thomas; Redon, Roland; Reiller, Pascal E.; Rösch, Notker; Rossberg, André; Scheinost, Andreas C.; Schimmelpfennig, Bernd; Schreckenbach, Georg; Skerencak-Frech, Andrej; Sladkov, Vladimir; Solari, Pier Lorenzo; Wang, Zheming; Washton, Nancy M.; Zhang, Xiaobin

doi:10.1021/acsomega.9b00164

Title: Interdisciplinary Round-Robin Test on Molecular Spectroscopy of the U(VI) Acetate System

Journal Article · 03 May 2019 · ACS Omega

DOI: https://doi.org/10.1021/acsomega.9b00164 · OSTI ID:1510554

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Helmholtz-Zentrum Dresden-Rossendorf (HZDR), Dresden (Germany)
Helmholtz-Zentrum Dresden-Rossendorf (HZDR), Dresden (Germany); Tokyo Inst. of Technology (Japan)
Univ. Of Potsdam (Germany)
Institut de Recherche de Chimie Paris (IRCP), Paris (France)
Karlsruhe Inst. of Technology (KIT) (Germany)
Lawrence Livermore National Lab. (LLNL), Livermore, CA (United States)
KTH Royal Inst. of Technology, Stockholm (Sweden)
Los Alamos National Lab. (LANL), Los Alamos, NM (United States)
Univ. of Toulon, Toulon (France)
Technische Univ. Munchen, Garching (Germany)
Pacific Northwest National Lab. (PNNL), Richland, WA (United States)
Univ. of Côte d'Azur, Nice (France)
Institut de Radioprotection et de Sûreté Nucléaire (IRSN/PSE-ENV/SRTE/LR2T), Saint Paul lez Durance (France)
Institute for Nuclear Waste Disposal (KIT-INE), Karlsruhe Institute of Technology, P.O. Box 3640, 76021 Karlsruhe, Germany
Helmholtz-Zentrum Dresden-Rossendorf (HZDR), Dresden (Germany); Technische Universität Dresden (Germany)
Helmholtz-Zentrum Dresden-Rossendorf (HZDR), Dresden (Germany); Karlsruhe Inst. of Technology (KIT) (Germany)
Institute of Resource Ecology, Helmholtz-Zentrum Dresden—Rossendorf, Bautzner Landstr. 400, D-01328 Dresden, Germany
Department of Chemistry, Technische Universität München, Lichtenbergstr. 4, 85748 Garching, Germany
Cardiff Univ., Cardiff (United Kingdom)
Karlsruhe Inst. of Technology (KIT) (Germany); Heidelberg Univ. (Germany)
Clemson Univ., Anderson, SC (United States)
Univ. Paris-Saclay, Gif-sur-Yvette (France)
Technische Univ. Munchen, Garching (Germany); Inst. of High Performance Computing, Agency for Science, Technology and Research (Singapore)
Helmholtz-Zentrum Dresden-Rossendorf (HZDR), Dresden (Germany); European Synchrotron Radiation Facility (ESRF), Grenoble (France)
Univ. of Manitoba, Winnipeg, MN (Canada)
Univ. Paris-Sud, Orsay (France)
Synchrotron SOLEIL, Gif-sur-Yvette (France)

A comprehensive molecular analysis of a simple aqueous complexing system–U(VI) acetate–selected to be independently investigated by various spectroscopic (vibrational, luminescence, X-ray absorption, and nuclear magnetic resonance spectroscopy) and quantum chemical methods was achieved by an international round-robin test (RRT). Twenty laboratories from six different countries with a focus on actinide or geochemical research participated and contributed to this scientific endeavor. The outcomes of this RRT were considered on two levels of complexity: first, within each technical discipline, conformities as well as discrepancies of the results and their sources were evaluated. The raw data from the different experimental approaches were found to be generally consistent. Specifically, for complex setups such as accelerator-based X-ray absorption spectroscopy, the agreement between the raw data was high. By contrast, luminescence spectroscopic data turned out to be strongly related to the chosen acquisition parameters. Second, the potentials and limitations of coupling various spectroscopic and theoretical approaches for the comprehensive study of actinide molecular complexes were assessed. Previous spectroscopic data from the literature were revised and the benchmark data on the U(VI) acetate system provided an unambiguous molecular interpretation based on the correlation of spectroscopic and theoretical results. The multimethodologic approach and the conclusions drawn address not only important aspects of actinide spectroscopy but particularly general aspects of modern molecular analytical chemistry.

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Research Organization:: Lawrence Livermore National Laboratory (LLNL), Livermore, CA (United States); Los Alamos National Laboratory (LANL), Los Alamos, NM (United States); Pacific Northwest National Laboratory (PNNL), Richland, WA (United States)

Sponsoring Organization:: USDOE National Nuclear Security Administration (NNSA); USDOE Office of Science (SC), Basic Energy Sciences (BES). Chemical Sciences, Geosciences, and Biosciences Division

Grant/Contract Number:: AC52-07NA27344; AC52-06NA25396; SC0010355; 89233218CNA000001; AC05-76RL01830

OSTI ID:: 1510554

Alternate ID(s):: OSTI ID: 1523827; OSTI ID: 1524394; OSTI ID: 1560369; OSTI ID: 1835691

Report Number(s):: LA-UR-18-20138; PNNL-SA-143380; LLNL-JRNL-799343

Journal Information:: ACS Omega, Vol. 4, Issue 5; ISSN 2470-1343

Publisher:: American Chemical Society (ACS)Copyright Statement

Country of Publication:: United States

Language:: English

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Equilibria and dynamics in binary and ternary uranyl oxalate and acetate/fluoride complexes † Aas, Wenche; Szabó, Zoltán; Grenthe, Ingmar Journal of the Chemical Society, Dalton Transactions, Issue 8 https://doi.org/10.1039/a808416e	journal	January 1999
Advanced Statistical and Numerical Methods for Spectroscopic Characterization of Protein Structural Evolution Shashilov, Victor A.; Lednev, Igor K. Chemical Reviews, Vol. 110, Issue 10 https://doi.org/10.1021/cr900152h	journal	July 2010
Accurate and Precise Wavelength Calibration for Wide Bandwidth Array Spectrometers Martinsen, Paul; Jordan, Bob; McGlone, Andrew Applied Spectroscopy, Vol. 62, Issue 9 https://doi.org/10.1366/000370208785793399	journal	September 2008
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