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

Abstract

A comprehensive molecular analysis of a simple aqueous 51 complexing system?U(VI) acetate?selected to be independently inves- 52 tigated by various spectroscopic (vibrational, luminescence, X-ray absorption, 53 and nuclear magnetic resonance spectroscopy) and quantum chemical 54 methods was achieved by an international round-robin test (RRT). Twenty 55 laboratories from six different countries with a focus on actinide or 56 geochemical research participated and contributed to this scientific endeavor. 57 The outcomes of this RRT were considered on two levels of complexity: first, 58 within each technical discipline, conformities as well as discrepancies of the 59 results and their sources were evaluated. The raw data from the different experimental approaches were found to be generally 60 consistent. In particular, for complex setups such as accelerator-based X-ray absorption spectroscopy, the agreement between 61 the raw data was high. By contrast, luminescence spectroscopic data turned out to be strongly related to the chosen acquisition 62 parameters. Second, the potentials and limitations of coupling various spectroscopic and theoretical approaches for the 63 comprehensive study of actinide molecule complexes were assessed. Previous spectroscopic data from the literature were revised 64 and the benchmark data on the U(VI) acetate system provided an unambiguous molecular interpretation based onmore » the 65 correlation of spectroscopic and theoretical results. The multimethodologic approach and the conclusions drawn address not 66 only important aspects of actinide spectroscopy but particularly general aspects of modern molecular analytical chemistry.« less

Authors:
ORCiD logo [1]; ORCiD logo [1];  [1]; ORCiD logo [2]; ORCiD logo [3]; ORCiD logo [4];  [5]; ORCiD logo [6];  [7]; ORCiD logo [8]; ORCiD logo [5];  [9];  [3];  [10]; ORCiD logo [11];  [12];  [13];  [5]; ORCiD logo [12]; ORCiD logo [14] more »;  [3];  [15]; ORCiD logo [16]; ORCiD logo [10];  [1];  [10]; ORCiD logo [17];  [18]; ORCiD logo [5]; ORCiD logo [19];  [5];  [20];  [21]; ORCiD logo [22];  [23]; ORCiD logo [23];  [5]; ORCiD logo [24]; ORCiD logo [18]; ORCiD logo [25];  [26];  [15];  [27];  [24] « less
  1. Institute of Resource Ecology, Helmholtz-Zentrum Dresden—Rossendorf, Bautzner Landstr. 400, D-01328 Dresden, Germany
  2. Institute of Resource Ecology, Helmholtz-Zentrum Dresden—Rossendorf, Bautzner Landstr. 400, D-01328 Dresden, Germany, Institute of Innovative Research, Tokyo Tech World Research Hub Initiative (WRHI), Tokyo Institute of Technology, 152-8550 Tokyo, Japan
  3. Institute of Chemistry, University of Potsdam, 14476 Potsdam, Germany
  4. Chimie ParisTech, PSL Research University, CNRS, Institut de Recherche de Chimie Paris (IRCP), F-75005 Paris, France
  5. Institute for Nuclear Waste Disposal (KIT-INE), Karlsruhe Institute of Technology, P.O. Box 3640, 76021 Karlsruhe, Germany
  6. Physical and Life Science Directorate, Lawrence Livermore National Laboratory, 7000 East Avenue, Livermore, 94550 California, United States
  7. School of Chemistry, Organic Chemistry, Royal Institute of Technology, S-100 44 Stockholm, Sweden
  8. Theoretical Division, Physics and Chemistry of Materials, Los Alamos National Laboratory, Los Alamos, 87545 New Mexico, United States
  9. Laboratoire LIS-UMR CNRS 7020, Aix-Marseille Université, Université de Toulon, 83041 Toulon Cedex 9, France
  10. Department of Chemistry, Technische Universität München, Lichtenbergstr. 4, 85748 Garching, Germany
  11. Physical and Computational Sciences Directorate, Pacific Northwest National Laboratory, MS K2-57, Richland, 99352 Washington, United States
  12. Université Côte d’Azur, CNRS, Institut de Chimie de Nice, UMR7272, 06108 Nice, France
  13. Institut de Radioprotection et de Sûreté Nucléaire (IRSN/PSE-ENV/SRTE/LR2T), CE Cadarache, BP3, 13115 Saint Paul lez Durance, France
  14. Institute of Resource Ecology, Helmholtz-Zentrum Dresden—Rossendorf, Bautzner Landstr. 400, D-01328 Dresden, Germany, Central Radionuclide Laboratory, Technische Universität Dresden, Zellescher Weg 19, 01069 Dresden, Germany
  15. Environmental Molecular Sciences Laboratory, Pacific Northwest National Laboratory, 3335 Innovation Blvd, Richland, 99354 Washington, United States
  16. Institute of Resource Ecology, Helmholtz-Zentrum Dresden—Rossendorf, Bautzner Landstr. 400, D-01328 Dresden, Germany, Institute for Nuclear Waste Disposal (KIT-INE), Karlsruhe Institute of Technology, P.O. Box 3640, 76021 Karlsruhe, Germany
  17. School of Chemistry, Cardiff University, Park Place, CF10 3AT Cardiff, U.K.
  18. Institute for Nuclear Waste Disposal (KIT-INE), Karlsruhe Institute of Technology, P.O. Box 3640, 76021 Karlsruhe, Germany, Institute of Physical Chemistry, Heidelberg University, Im Neuenheimer Feld 253, D-69120 Heidelberg, Germany
  19. Department of Environmental Engineering and Earth Sciences, Department of Chemistry, Clemson University, 342 Computer Court, Anderson, 29625 South Carolina, United States
  20. Laboratoire MIO—CS 60584, Université de Toulon, 83041 Toulon cedex 9, France
  21. Den—Service d’Études Analytiques et de Réactivité des Surfaces (SEARS), CEA, Université Paris-Saclay, F 91191 Gif-sur-Yvette, France
  22. Department of Chemistry, Technische Universität München, Lichtenbergstr. 4, 85748 Garching, Germany, Institute of High Performance Computing, Agency for Science, Technology and Research, 1 Fusionopolis Way, #16-16 Connexis, Singapore, Singapore 138632
  23. Institute of Resource Ecology, Helmholtz-Zentrum Dresden—Rossendorf, Bautzner Landstr. 400, D-01328 Dresden, Germany, The Rossendorf Beamline (BM20), European Synchrotron Radiation Facility, B.P. 220, F-38043 Grenoble Cedex, France
  24. Department of Chemistry, University of Manitoba, 144 Dysart Road, Winnipeg, Manitoba, R3T 2N2, Canada
  25. Institut de Physique Nucléaire (IPN), CNRS/IN2P3, Université Paris-Sud, 91406 Orsay, France
  26. Synchrotron SOLEIL, Ligne de lumière MARS, L’Orme des Merisiers, Saint-Aubin, BP 48, F-91192 Gif-sur-Yvette Cedex, France
  27. Pacific Northwest National Laboratory, 902 Battelle Blvd, Richland, 99352 Washington, United States
Publication Date:
Research Org.:
Lawrence Livermore National Lab. (LLNL), Livermore, CA (United States); Los Alamos National Lab. (LANL), Los Alamos, NM (United States); Pacific Northwest National Lab. (PNNL), Richland, WA (United States)
Sponsoring Org.:
USDOE National Nuclear Security Administration (NNSA); USDOE Office of Science (SC), Basic Energy Sciences (BES). Chemical Sciences, Geosciences, and Biosciences Division
OSTI Identifier:
1510554
Alternate Identifier(s):
OSTI ID: 1523827; OSTI ID: 1524394; OSTI ID: 1560369
Report Number(s):
LA-UR-18-20138; PNNL-SA-143380
Journal ID: ISSN 2470-1343
Grant/Contract Number:  
AC52-06NA25396; AC52-07NA27344; SC0010355; 89233218CNA000001; AC05-76RL01830
Resource Type:
Published Article
Journal Name:
ACS Omega
Additional Journal Information:
Journal Name: ACS Omega Journal Volume: 4 Journal Issue: 5; Journal ID: ISSN 2470-1343
Publisher:
American Chemical Society
Country of Publication:
United States
Language:
English
Subject:
37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY; Uranium (VI), Round Robin Exercise

Citation Formats

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., and Zhang, Xiaobin. Interdisciplinary Round-Robin Test on Molecular Spectroscopy of the U(VI) Acetate System. United States: N. p., 2019. Web. https://doi.org/10.1021/acsomega.9b00164.
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. Interdisciplinary Round-Robin Test on Molecular Spectroscopy of the U(VI) Acetate System. United States. https://doi.org/10.1021/acsomega.9b00164
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., and Zhang, Xiaobin. Fri . "Interdisciplinary Round-Robin Test on Molecular Spectroscopy of the U(VI) Acetate System". United States. https://doi.org/10.1021/acsomega.9b00164.
@article{osti_1510554,
title = {Interdisciplinary Round-Robin Test on Molecular Spectroscopy of the U(VI) Acetate System},
author = {Müller, Katharina and Foerstendorf, Harald and Steudtner, Robin and Tsushima, Satoru and Kumke, Michael U. and Lefèvre, Grégory and Rothe, Jörg and Mason, Harris and Szabó, Zoltán and Yang, Ping and Adam, Christian K. R. and André, Rémi and Brennenstuhl, Katlen and Chiorescu, Ion and Cho, Herman M. and Creff, Gaëlle and Coppin, Frédéric and Dardenne, Kathy and Den Auwer, Christophe and Drobot, Björn and Eidner, Sascha and Hess, Nancy J. and Kaden, Peter and Kremleva, Alena and Kretzschmar, Jerome and Krüger, Sven and Platts, James A. and Panak, Petra J. and Polly, Robert and Powell, Brian A. and Rabung, Thomas and Redon, Roland and Reiller, Pascal E. and Rösch, Notker and Rossberg, André and Scheinost, Andreas C. and Schimmelpfennig, Bernd and Schreckenbach, Georg and Skerencak-Frech, Andrej and Sladkov, Vladimir and Solari, Pier Lorenzo and Wang, Zheming and Washton, Nancy M. and Zhang, Xiaobin},
abstractNote = {A comprehensive molecular analysis of a simple aqueous 51 complexing system?U(VI) acetate?selected to be independently inves- 52 tigated by various spectroscopic (vibrational, luminescence, X-ray absorption, 53 and nuclear magnetic resonance spectroscopy) and quantum chemical 54 methods was achieved by an international round-robin test (RRT). Twenty 55 laboratories from six different countries with a focus on actinide or 56 geochemical research participated and contributed to this scientific endeavor. 57 The outcomes of this RRT were considered on two levels of complexity: first, 58 within each technical discipline, conformities as well as discrepancies of the 59 results and their sources were evaluated. The raw data from the different experimental approaches were found to be generally 60 consistent. In particular, for complex setups such as accelerator-based X-ray absorption spectroscopy, the agreement between 61 the raw data was high. By contrast, luminescence spectroscopic data turned out to be strongly related to the chosen acquisition 62 parameters. Second, the potentials and limitations of coupling various spectroscopic and theoretical approaches for the 63 comprehensive study of actinide molecule complexes were assessed. Previous spectroscopic data from the literature were revised 64 and the benchmark data on the U(VI) acetate system provided an unambiguous molecular interpretation based on the 65 correlation of spectroscopic and theoretical results. The multimethodologic approach and the conclusions drawn address not 66 only important aspects of actinide spectroscopy but particularly general aspects of modern molecular analytical chemistry.},
doi = {10.1021/acsomega.9b00164},
journal = {ACS Omega},
number = 5,
volume = 4,
place = {United States},
year = {2019},
month = {5}
}

Journal Article:
Free Publicly Available Full Text
Publisher's Version of Record
https://doi.org/10.1021/acsomega.9b00164

Figures / Tables:

Figure 1 Figure 1: Vibrational spectra of samples U1−U4. Different colors correspond to different participants. Only the spectral regions of the $ν$3(UO2) mode from IR (A) and of the $ν$1(UO2) mode from Raman spectroscopy (B) are shown. Values are given in cm−1.

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