September 6, 2019
Journal Article

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

Katharina Muller
Robin Steudtner
Satoru Tsushima
Michael Kumke
Gregory Lefevre
Jorg Rothe
Harris Mason
Zoltan Szabo
Ping Yang
Christian Adam
Remi Andre
Katlen Brennenstuhl
Ion Chiorescu
Gaelle Creff
Frederic Coppin
Kathy Dardenne
Christophe Den Auwer
Bjorn Drobot
Sascha Eidner
Nancy Hess
Peter Kaden
Alena Kremleva
Jerome Kretzschmar
Sven Kruger
James Platts
Petra Panak
Brian Powell
Thomas Rabung
Roland Redon
Pascal Reiller
Notker Rosch
Andre Rossberg
Andreas Scheinost
Bernd Schimmelpfennig
Georg Schreckenbach
Andrej Skerencak-Frech
Vladimir Sladkov
Zheming Wang
Nancy Washton
Xiaobin Zhang
Harald Foerstendorf
Herman Cho
Robert Polly
Pier-Lorenzo Solari
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.

Revised: September 6, 2019 | Published: May 31, 2019

Muller K., H. Foerstendorf, R. Steudtner, S. Tsushima, M. Kumke, G. Lefevre, and J. Rothe, et al. 2019. "Interdisciplinary Round-Robin Test on Molecular Spectroscopy of the U(VI) Acetate System." ACS Omega 4, no. 5:8167-8177. PNNL-SA-143380. doi:10.1021/acsomega.9b00164