Publikationsrepositorium - Helmholtz-Zentrum Dresden-Rossendorf
1 PublikationXAS Towards the Bottom of the Periodic Table
Kvashnina, K.
Abstract
Understanding the mechanisms of different chemical reactions with actinides (An) at the atomic level is a key step towards safe disposal of nuclear wastes and towards the identification of physical-chemical processes of radionuclides in the environment. X-ray absorption spectroscopy in high energy resolution fluorescence detection (HERFD) mode at the An M4,5 edges is now a common technique to probe the electronic structure and the An 5f states. I will provide an overview of the recently performed studies on Uranium, Thorium and Plutonium-containing materials at the European Synchrotron (ESRF) in Grenoble (France). I will show how the detailed information about the An oxidation state, electron-electron interactions, hybridization between molecular orbitals can be obtained by a combination of experimental data and electronic structure calculations. It might be of interest for fundamental research in chemistry and physics of actinides as well as for applied science.
Reading:
[1] K. O. Kvashnina, S. M. Butorin, P. Martin, and P. Glatzel, “Chemical State of Complex Uranium Oxides,” Phys. Rev. Lett., vol. 111, no. 25, p. 253002, Dec. 2013, doi: 10.1103/PhysRevLett.111.253002.
[2] K. O. Kvashnina, Y. O. Kvashnin, and S. M. Butorin, “Role of resonant inelastic X-ray scattering in high-resolution core-level spectroscopy of actinide materials,” J. Electron Spectros. Relat. Phenomena, vol. 194, pp. 27–36, Jun. 2014, doi: 10.1016/j.elspec.2014.01.016.
[3] S. M. Butorin, K. O. Kvashnina, J. R. Vegelius, D. Meyer, and D. K. Shuh, “High-resolution X-ray absorption spectroscopy as a probe of crystal-field and covalency effects in actinide compounds,” Proc. Natl. Acad. Sci., vol. 113, no. 29, pp. 8093–8097, Jul. 2016, doi: 10.1073/pnas.1601741113.
[4] K. O. Kvashnina et al., “A Novel Metastable Pentavalent Plutonium Solid Phase on the Pathway from Aqueous Plutonium(VI) to PuO 2 Nanoparticles,” Angew. Chemie Int. Ed., vol. 58, no. 49, pp. 17558–17562, Dec. 2019, doi: 10.1002/anie.201911637.
[5] E. Gerber et al., “The missing pieces of the PuO 2 nanoparticle puzzle,” Nanoscale, vol. 12, no. 35, pp. 18039–18048, 2020, doi: 10.1039/D0NR03767B.
[6] I. Pidchenko, J. März, M. O. J. Y. Hunault, S. Bauters, S. M. Butorin, and K. O. Kvashnina, “Synthesis, Structural, and Electronic Properties of K 4 Pu VI O 2 (CO 3 ) 3(cr) : An Environmentally Relevant Plutonium Carbonate Complex,” Inorg. Chem., vol. 59, no. 17, pp. 11889–11893, Sep. 2020, doi: 10.1021/acs.inorgchem.0c01335.
[7] L. Amidani et al., “The Application of HEXS and HERFD XANES for Accurate Structural Characterisation of Actinide Nanomaterials: The Case of ThO 2,” Chem. – A Eur. J., vol. 27, no. 1, pp. 252–263, Jan. 2021, doi: 10.1002/chem.202003360.
[8] E. Gerber et al., “Insight into the structure–property relationship of UO 2 nanoparticles,” Inorg. Chem. Front., p. accepted, 2021, doi: 10.1039/D0QI01140A.
Beteiligte Forschungsanlagen
- Rossendorf Beamline an der ESRF DOI: 10.1107/S1600577520014265
Verknüpfte Publikationen
- DOI: 10.1107/S1600577520014265 is cited by this (Id 32843) publication
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Eingeladener Vortrag (Konferenzbeitrag) (Online Präsentation)
GlobalXAS, 04.02.2021, Washington, USA
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