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
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.
ACS Omega. 2019 May 3;4(5):8167-8177. doi: 10.1021/acsomega.9b00164. eCollection 2019 May 31.
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. In particular, 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.
通过国际循环试验（RRT），对一个简单的水相络合体系——醋酸铀酰（VI）进行了全面的分子分析，该体系被选定由各种光谱方法（振动光谱、发光光谱、X射线吸收光谱和核磁共振光谱）以及量子化学方法独立研究。来自六个不同国家的20个专注于锕系元素或地球化学研究的实验室参与并为这项科学工作做出了贡献。此次RRT的结果在两个复杂程度层面上进行了考量：首先，在每个技术学科内部，评估了结果的一致性以及差异及其来源。发现来自不同实验方法的原始数据总体上是一致的。特别是对于基于加速器的X射线吸收光谱等复杂装置，原始数据之间的一致性很高。相比之下，发光光谱数据结果与所选的采集参数密切相关。其次，评估了耦合各种光谱和理论方法用于锕系元素分子络合物综合研究的潜力和局限性。对文献中以前的光谱数据进行了修订，并且基于光谱和理论结果的相关性，醋酸铀酰（VI）体系的基准数据提供了明确的分子解释。这种多方法学方法以及得出的结论不仅涉及锕系元素光谱学的重要方面，而且特别涉及现代分子分析化学的一般方面。
