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The Helmholtz Young Investigators Group (VH-NG-734)

“Advanced synchrotron based systematic investigations of lanthanide and actinide systems to understand and predict their reactivity”

is financially supported within the 07.2011-10.2019 time period by the Helmholtz Association of German Research Centers (HGF) and the Karlsruhe Institute of Technology (KIT), Faculty of Chemistry and Biosciences, Institute for Nuclear Waste Disposal (INE)

 

 

We systematically investigate the electronic and coordination structures of actinide (An) and chemical homologue lanthanide (Ln) systems with novel synchrotron-based high energy resolution X-ray emission/absorption/inelastic scattering techniques. The experimental results are supported by theoretical calculations and simulations with quantum chemical codes. These investigations improve our understanding of An/Ln reactivity in repository systems and waste matrices on a molecular scale and thereby support the reliability of safety case evaluation of the repository long term safety. The elucidation of electronic and coordination structures of, e.g., An/Ln extraction ligand complexes finds on the one hand application in optimization of separation technologies of lanthanide cations from minor actinides (partitioning), while at the same time provides basic insight into structure-reactivity relationships of actinide elements, which is a present scientific frontier.

 

The Team

Group Leader

Teaching activities:

  • Karlsruhe Institute of Technology
  • Faculty of Chemistry and Biosciences, Winter Semester
  • Lecture “Instrumental Analytics”

Tonya Vitova

Tonya.Vitova∂kit.edu

+49 721 608 24024

 

 

Members

Bianca Schacherl, KIT

bianca.schacherl∂student.kit.edu

+49 721 608-28079

Aaron Beck, KIT

Aaron.Beck∂student.kit.edu

+49 721 608-28079

Jurij Galanzew, KIT

 

 

Master thesis:

“Speciation of Np in illite by X-ray spectroscopy methods”

 

PhD Project:

"High energy resolution X-ray spectroscopy investigations of nuclear waste"

Master thesis:

"Electronic structure studies of Th systems by high energy resolution X-ray spectroscopy and computational methods

Former members

Aaron Beck, Karlsruhe Institute of Technology (KIT), Germany

 

12.2016 - 06.2017: Master thesis

“Immobilization of cesium- and rhenium-rich simulated high level solid waste residues in different host matrices”

Sebastian Bahl, Karlsruhe Institute of Technology (KIT), Germany

 

2013 - 2017: PhD project

“Characterisation of nuclear waste glass forms by advanced spectroscopy and microscopy techniques”

Alisa Prokopchuk, Karlsruhe Institute of Technology (KIT), Germany

 

10.2016 - 04.2017: Master thesis

„Preparation of Rb2UO2X4 compounds (X= F,Cl,Br) and characterizytion of bonding differences by spectroscopy and quantum chemical methods“

Ivan Pidchenko, Institut für Nukleare Entsorgung, Karlsruhe Institute of Technology (KIT), Germany

 

10.2016 - 04.2017: PhD project

2017 - Postdoc

„Characterisation of actinide species in systems relevant for safety assessment of a nuclear waste repository by high-resolution X-ray emission/absorption spectroscopy“

Tim Prüßmann, Institut für Nukleare Entsorgung, Karlsruhe Institute of Technology (KIT), Germany

 

07.2011 - 04.2015: PhD project

„Characterization of bonding differences by advanced synchrotron based X-ray spectroscopy“

Sebastian Bahl, Karlsruhe Institute of Technology (KIT), Germany

 

02.2013 - 07.2013: Diploma thesis

„Charakterisierung von verglasten, hochradioaktiven, Mo/P/Zr/Cs-reichen Simulatabfällen mittels verschiedener spektroskopischer Techniken“, Grade: 1.0 (highest in Germany)

Veronika Koldeisz, Budapest University of Technology and Economics (BME), Hungary

 

09.2013 – 07.2014: Master's thesis

“Characterization of uranium in multi-component borosilicate glass by high-energy resolution X-ray spectroscopy techniques”, Grade: 5.0 (highest in Hungary)

Paul Estevenon, École Nationale Supérieure de Chimie de Montpellier (ENSCM), France

 

06.2014 - 09.2014: Internship

"Characterization of simulated Tc- and Cs-rich solid waste residue"

Andrea Kutzer, Karlsruhe Institute of Technology (KIT), Germany

 

2011 - 2014: PhD project

“Untersuchungen zum Inkorporationsverhalten von simulierten HLW-Borosilikatgläsern zur Immobilisierung Mo(VI)-reicher Abfälle”

 

Alexander Ernst, Karlsruhe Institute of Technology (KIT)

 

04.2012 - 09.2012: practical part of “berufliche Ausbildung”

"Design and technical drawings of positioning part of a detector positioning assembly"

 

Valentine Traunfelder, Karlsruhe Institute of Technology (KIT)

 

04.2013 – 01.2014: practical part of “berufliche Ausbildung”

“Design and technical drawings of liquid cells for M edge high resolution X-ray absorption spectroscopy studies of actinide materials”

 

 

 

Internship students

Heloise Morin, École des Mines de Nantes (Mines Nantes), France

 

05.2011 - 08.2011

“Measurements, data reduction and comparison of N K-edge XANES spectra of n-Pr-BTP ligand and [Ln(n-Pr-BTP)3](NO3)3 complexes”

 

Bastien Gademann, National Graduate School of Chemistry of Montpellier (ENSCM), France

 

06.2012 - 09.2012

“Alignment procedure of a multi-analyzer crystal X-ray emission spectrometer using SPEC macros”

 

Stelyana Lechchanska, Technical University of Sofia (TU Sofia), Bulgaria

 

07.2013 - 09.2013

“Design and technical drawings of a slit system, an integral part of the multi-analyzer crystals X-ray emission spectrometer”

 

 

 

 

Guest scientists

Aurora Walesh, Trinity Collage Dublin (TCD), School of Chemistry, Ireland

 

4.03.2013 - 15.03.2013: Short term scientific mission

“Structural characterization of UO2 alteration products by X-ray techniques”

Funded by COST: European cooperation in science and technology

Yulia Podkovyrina, Southern Federal University (SFedU) Rostov-on-Don, Russia

 

02.2014 –03.2014: Scholarship

“Quantum chemical calculations of HR-XANES M edge spectra of uranium oxides”

Funded by German Russian Interdisciplinary Science Center (G-RISC)

10.2014 –03.2015: Scholarship

“Optimization of structures describing U sorption and incorporation into magnetite”

Funded by German Academic Exchange Service (DAAD)

Prof. Robert Baker, Trinity College Dublin (TCD), School of Chemistry, Ireland

 

01.2015- 03.2015: TALISMAN project

 “Neptunium Incorporation into Minerals: A Synthetic and X-ray Spectroscopic Study”

Projects

An geochemistry: The chemical state of U after interaction with magnetite

Long-term storage of high-level radioactive waste is associated with potential radioecological hazards. One chemical element of high interest is uranium (U), which mainly exists as a mobile U(VI) (oxidizing conditions) and sparingly soluble U(IV) (reducing conditions) species. It is expected that the main inorganic reducing agents for U(VI) in the environment are ferrous species in magnetite, formed on the steel canister surface as an intermediate iron (Fe) corrosion product. Continuous interaction and related phase dissolution/recrystallization processes can lead to U redox changes and structural U incorporation into Fe oxides, resulting in U immobilization. U redox state and speciation analyses are still very challenging due to simultaneous formation of several different species in such mineral systems. New advanced spectroscopic methods for speciation studies provide more precise results for the characterization of such systems. The main goal of the investigations of Ivan Pidchenko within his PhD project is to assess the U M4 edge high energy resolution X-ray absorption near edge structure (HR-XANES) spectroscopy technique for detection of U(V) possibly co-existing with U(IV) and U(VI) under reducing conditions on/in Fe containing minerals. In addition to U M4 edge HR-XANES, U L3 edge extended X-ray absorption fine structure (EXAFS), X-ray photoelectron spectroscopy (XPS) and transmission electron microscopy (TEM) techniques are applied to identify the redox states of U and if it is predominantly sorbed or incorporated in the magnetite structure. For example, a high resolution TEM image of 10000 ppm U co-precipitated with magnetite recorded by Tadahiro Yokosawa (INE) reveals formation of UO2 on the surface of the Fe3O4 nanoparticles (see the figure). Our recent U M4 edge HR-XANES results unambiguously confirm for the first time the presence of U(V) in samples with 1000 and 3000 ppm U (see I. Pidchenko et al. Environ Sci Technol, 51, (4), 2217-2225, 2017).

Vitrified nuclear waste: Differences of structural properties of model and genuine nuclear waste glasses

Understanding the long term behavior of vitrified nuclear waste requires a full and detailed characterization of the materials including their characteristics as synthesized and after exposure to groundwater. Genuine radioactive waste glass has a complex chemical composition. Therefore, Sebastian Bahl and Veronika Koldeisz within their PhD and master projects, respectively, took a simplified approach by investigating and comparing the oxidation states and local atomic environments of U, Pu and Np in high level waste (HLW) glass sampled during operation of the “vitrification plant Karlsruhe” (VEK) and in model glasses (see the figure) with the same borosilicate base glass matrix by An M edge HR-XANES, U L3 edge extended EXAFS, XPS and TEM techniques (presented as an oral contribution on the ATAS 2014 workshop and poster presentation at EUFEN4). The preparation and characterization of the model glasses are performed within the TALISMAN (Transnational Access to Large Infrastructure for a Safe Management of ActiNide) project “Advanced spectroscopic and microscopic investigations of Pu-doped borosilicate glass” in collaboration with the group of Joe Sommers, Institute for Transuranium Elements (JRC-ITU), Karlsruhe, Germany (see the PhD thesis of Sebastian Bahl).

Vitrified nuclear waste: Influence of high Mo content on the vitrification properties of borosilicate glass

Mo(VI) has low solubility in borosilicate glass, tending to separate out into molybdate rich phases during the vitrification process. These phases may crystallize in the form of soluble alkali Mo(VI) phases incorporating significant amounts of radioactive isotopes during glass melt cooling and have the potential to release radionuclides in the environment following contact with ground water. Understanding factors favoring or disfavoring their formation in borosilicate glasses allows development of glass compositions capable of incorporating high Mo loadings, yet avoiding formation of such soluble phases. Andrea Kutzer and Sebastian Bahl within their PhD and diploma projects, respectively, identified and quantified the contributions of the different crystalline (see the figure) and dispersed Mo species in the glass matrix by applying the Mo K-edge HR-XANES technique augmented by other spectroscopy and microscopy methods (Raman, XRD, SEM-EDX, TEM). Mo solubility limit determination and identification of potentially water soluble crystalline phases were also aimed (see the poster of Sebastian Bahl et al. granted a poster prize at the Actinide XAS 2014 workshop, publication is currently in preparation). The project is partially financially supported by the Wiederaufarbeitungsanlage Karlsruhe (WAK).

Selectivity: Origin of the bonding affinity of the BTP molecule to An compared to Ln elements

One of the major steps in the partitioning and transmutation (P&T) strategy for the reduction of the long term radiotoxicity and heat-load of spent nuclear fuel is the separation of 5f elements from their chemically similar 4f counterparts. Selective liquid-liquid extraction of An(III) from Ln(III) has been demonstrated using heterocyclic N-donor ligands, e.g., bistriazinylpyridines (BTP) and bistriazinyl-bipyridines (BTBP). However, these ligands do not yet fulfill all necessary criteria for application in an industrial process. Further ligand optimization requires a sound understanding of the chemical and physical properties responsible for their selectivity towards An(III). Systematic comparative N K-edge XANES and Ln and An L edge HR-XANES/XES investigations complemented by quantum chemical calculations can help to differentiate between subtle bonding and geometric structural differences in An(BTP)3 and Ln(BTP)3  complexes looking from the point of view of the organic ligand or the metal center. Bonding characteristics like molecular orbital energy differences and relative electronic populations can be extracted. The figure depicts an optical and a scanning transmission X-ray microscopy (STXM, inset) image of Am(BTP)3(OTf)3 crystals. The STXM image is measured in collaboration with the group of David Shuh at the Advanced Light Source (ALS), Lawrence Berkeley National Laboratory, USA (see the poster Tim Prüßmann presented at Actinide XAS 2014 ( see the dissertation of Tim Prüssmann).

Electronic structure: Probing An electronic structure by HR-XANES and XES techniques

Dicesium uranyl tetrachloride (Cs2UO2Cl4) has been a model compound for experimental and theoretical studies of electronic structure of U(VI) in the form of UO22+ (uranyl ion) for decades. We have obtained angle-resolved electronic structure information for an oriented Cs2UO2Cl4 crystal, specifically relative energies of 5f and 6d valence orbitals probed with extraordinary energy resolution by polarization dependent HR-XANES (PD-HR-XANES) (see the figure) and compare these with predictions from quantum chemical Amsterdam density functional theory (ADF) and ab initio real space multiple scattering Green’s function based FEFF codes. The obtained results have fundamental value but also demonstrate an experimental approach, which offers great potential to benchmark and drive improvement in theoretical calculations of electronic structures of actinide elements (see Vitova et al. in Inorg. Chem.)

Recent Highlights

Electrochemical cell

3D model (left) and a photograph (right) of a compact electrochemical cell for in-situ synchronized UV-VIS and X-ray absorption/emission spectroscopy investigations. The cell equipped with two Kapton windows with 8 and 13 µm thickness was developed within the PhD project of Ivan Pidchenko and was applied in March 2015 in an initial high energy resolution X-ray absorption near edge structure (HR-XANES) experiment at the U M4 absorption edge. Partial reduction of U(VI) to U(V) was successfully recorded by simultaneous UV-VIS and U M4 HR-XANES edge measurements at the INE-Beamline.

Liquid cells for air-sensitive samples

 

3D model (left) and a photograph (right) of sample holders integrated in an inert gas cell for studies of liquid samples at An M4,5 absorption edges. The inner and outer compartments are sealed by Kapton windows with 8 and 13 µm thickness, respectively. First successful application of these cells as part of the PhD project of Ivan Pidchenko was the recent Pu M5 edge HR-XANES investigation of Pu(III), Pu(IV) and Pu(VI) in aqueous solutions (prepared by David Fellhauer, INE) at the INE-Beamline in March 2015.

 

Genuine nuclear waste glass from the Vitrification Facility Karlsruhe (VEK)

First successful U M4, Pu M5 and Np M5 edge HR-XANES studies of high level waste from nuclear fuel reprocessing vitrified in borosilicate glass matrix were performed within the PhD project of Sebastian Bahl at the INE-Beamline. The sample with less than 1 mm2 size and about 200 µSv/h dose rate (left hand side in the photograph) was prepared by Ernesto Gonzalez-Robles in a shielded box line in the controlled area laboratories of INE.

 

Spent nuclear fuel

 

First successful U M4 and Pu M5 edge HR-XANES investigations of a footprint of spent nuclear fuel pellet exhibiting a high burnup structure (photograph on the left) were performed in March 2015 at the INE-Beamline as part of the PhD project of Sebastian Bahl. The photograph on the right hand side depicts the position dependent U Mβ fluorescence emitted by the sample. The sample was prepared by Ernesto Gonzalez-Robles in the controlled laboratories of INE.

The Instrumentation

High energy resolution X-ray emission spectrometer

The utility of high energy resolution X-ray absorption near edge structure (HR-XANES), X-ray emission (XES) and resonant inelastic X-ray scattering (RIXS) spectroscopy techniques in studies of An elements was the motivator for installing and commissioning a multi-analyzer Johann type X-ray emission spectrometer (MAC-spectrometer, see the figure above) at the INE-Beamline for actinide research at the ANKA synchrotron radiation facility, Karlsruhe, Germany. The MAC-spectrometer is ultimately destined to be the central instrument at the radioactive end station of the newly constructed beamline for catalysis and actinide research (CAT-ACT-Beamline, beginning operation in 2016). The MAC-spectrometer is an adapted design of the XES spectrometer at the ID26 Beamline, ESRF, Grenoble, France, containing five spherically bent analyzer crystals with 1 m bending radius. Our set-up is optimized for An M4,5 edge HR-XANES and XES/RIXS experiments; absorption of 3-4 keV photons by air is minimized by a He environment enclosing sample, https://wsm10.scc.kit.edu/cms/RedDotTemp/E8D1E516BFA249CBA172FDDB96EB2148/7A9300D552E142D8A44DBD1A157F6C93/bla2.pngcrystals, and detector, thereby enhancing efficiency. This instrument, combined with access to the controlled area laboratory at INE in close proximity, is worldwide unique, enabling An M4,5 edge HR-XANES and XES/RIXS investigations of solid and liquid phase radioactive materials, including those under extreme conditions. The Figures depict Pu M5 edge HR-XANES, conventional XANES spectra (below) and a 3d4f RIXS map (2 hours measurement, left) of 50 mM Pu(VI) in aqueous solution prepared by David Fellhauer (INE) and measured with our MAC-Spectrometer at the INE-Beamline, ANKA. We would like to specifically thank Alexander Gensch (INE), Volker Krepper, Tim Prüßmann (HYIG, INE), and Jörg Rothe (INE) for the very successful design and manufacture of the He environment.

https://wsm10.scc.kit.edu/cms/RedDotTemp/E8D1E516BFA249CBA172FDDB96EB2148/7A9300D552E142D8A44DBD1A157F6C93/bla2.png

Publications


2017
Zeitschriftenaufsätze
CAT-ACT—A new highly versatile x-ray spectroscopy beamline for catalysis and radionuclide science at the KIT synchrotron light facility ANKA.
Zimina, A.; Dardenne, K.; Denecke, M. A.; Doronkin, D. E.; Huttel, E.; Lichtenberg, H.; Mangold, S.; Pruessmann, T.; Rothe, J.; Spangenberg, T.; Steininger, R.; Vitova, T.; Geckeis, H.; Grunwaldt, J.-D.
2017. Review of scientific instruments, 88 (11), Art. Nr.: 113113. doi:10.1063/1.4999928
Pu Coexists in Three Oxidation States in a Borosilicate Glass: Implications for Pu Solubility.
Bahl, S.; Peuget, S.; Pidchenko, I.; Pruessmann, T.; Rothe, J.; Dardenne, K.; Delrieu, J.; Fellhauer, D.; Jégou, C.; Geckeis, H.; Vitova, T.
2017. Inorganic chemistry, 56 (22), 13982-13990. doi:10.1021/acs.inorgchem.7b02118
Evaluating the electronic structure of formal LnII ions in LnII(C5H4SiMe3)31- using XANES spectroscopy and DFT calculations.
Fieser, M. E.; Ferrier, M. G.; Su, J.; Batista, E.; Cary, S. K.; Engle, J. W.; Evans, W. J.; Lezama Pacheco, J. S.; Kozimor, S. A.; Olson, A. C.; Ryan, A. J.; Stein, B. W.; Wagner, G. L.; Woen, D. H.; Vitova, T.; Yang, P.
2017. Chemical science, 8 (9), 6076-6091. doi:10.1039/c7sc00825b
The role of the 5f valence orbitals of early actinides in chemical bonding.
Vitova, T.; Pidchenko, I.; Fellhauer, D.; Bagus, P. S.; Joly, Y.; Pruessmann, T.; Bahl, S.; Gonzalez-Robles, E.; Rothe, J.; Altmaier, M.; Denecke, M. A.; Geckeis, H.
2017. Nature Communications, 8, 16053. doi:10.1038/ncomms16053
Tc interaction with crystalline rock from Äspö (Sweden): Effect of in-situ rock redox capacity.
Huber, F. M.; Totskiy, Y.; Marsac, R.; Schild, D.; Pidchenko, I.; Vitova, T.; Kalmykov, S.; Geckeis, H.; Schäfer, T.
2017. Applied geochemistry, 80, 90–101. doi:10.1016/j.apgeochem.2017.01.026
Uranium Redox Transformations after U(VI) Coprecipitation with Magnetite Nanoparticles.
Pidchenko, I.; Kvashnina, K. O.; Yokosawa, T.; Finck, N.; Bahl, S.; Schild, D.; Polly, R.; Bohnert, E.; Rossberg, A.; Göttlicher, J.; Dardenne, K.; Rothe, J.; Schäfer, T.; Geckeis, H.; Vitova, T.
2017. Environmental science & technology, 51 (4), 2217–2225. doi:10.1021/acs.est.6b04035
Buchaufsätze
Computational chemistry.
Polly, R.; Trumm, M.; Schimmelpfennig, B.; Tasi, A.; Gaona, X.; Pidchenko, I.; Vitova, T.; Adam, C.; Maiwald, M.; Panak, P. J.; Skerencak-Frech, A.; Geist, A.
2017. Annual Report 2016 - Institute for Nuclear Waste Disposal. Ed.: H. Geckeis, 71-74, KIT Scientific Publishing, Karlsruhe
R&D projects conducted at the INE-Beamline for actinide research and the new CAT-ACT beamline at ANKA.
Bahl, S.; Bauer, A.; Bohnert, E.; Dardenne, K.; González-Robles, E.; Herm, M.; Krepper, V.; Metz, V.; Pidchenko, I.; Rothe, J.; Vespa, M.; Vitova, T.
2017. Annual Report 2016 - Institute for Nuclear Waste Disposal. Ed.: H. Geckeis, 53-58, KIT Scientific Publishing, Karlsruhe
2016
Zeitschriftenaufsätze
Towards Printed Organic Light-Emitting Devices: A Solution-Stable, Highly Soluble Cu-NHetPHOS.
Wallesch, M.; Verma, A.; Fléchon, C.; Flügge, H.; Zink, D. M.; Seifermann, S. M.; Navarro, J. M.; Vitova, T.; Göttlicher, J.; Steininger, R.; Weinhardt, L.; Zimmer, M.; Gerhards, M.; Heske, C.; Bräse, S.; Baumann, T.; Volz, D.
2016. Chemistry - a European journal, 22 (46), 16400–16405. doi:10.1002/chem.201603847
The CAT-ACT Beamline at ANKA : A new high energy X-ray spectroscopy facility for CATalysis and ACTinide research.
Zimina, A.; Dardenne, K.; Denecke, M. A.; Grunwaldt, J. D.; Huttel, E.; Lichtenberg, H.; Mangold, S.; Pruessmann, T.; Rothe, J.; Steininger, R.; Vitova, T.
2016. Journal of physics / Conference Series, 712 (1), Art. Nr. 012019. doi:10.1088/1742-6596/712/1/012019
Probing Covalency in the UO3 Polymorphs by U M4 edge HR- XANES.
Podkovyrina, Y.; Pidchenko, I.; Prüßmann, T.; Bahl, S.; Göttlicher, J.; Soldatov, A.; Vitova, T.
2016. Journal of physics / Conference Series, 712 (1), 012092. doi:10.1088/1742-6596/712/1/012092
Aqueous U(VI) interaction with magnetic nanoparticles in a mixed flow reactor system: HR-XANES study.
Pidchenko, I.; Heberling, F.; Kvashnina, K. O.; Finck, N.; Schild, D.; Bohnert, E.; Schäfer, T.; Rothe, J.; Geckeis, H.; Vitova, T.
2016. Journal of physics / Conference Series, 712, 012086/1-4. doi:10.1088/1742-6596/712/1/012086
Further insights into the chemistry of the Bi–U–O system.
Popa, K.; Prieur, D.; Manara, D.; Naji, M.; Vigier, J.-F.; Martin, P. M.; Blanco, O. D.; Scheinost, A. C.; Prüβmann, T.; Vitova, T.; Raison, P. E.; Somers, J.; Konings, R. J. M.
2016. Dalton transactions, 45 (18), 7847-7855. doi:10.1039/C6DT00735J
2015
Zeitschriftenaufsätze
Polarization dependent high energy resolution X-ray absorption study of dicesium uranyl tetrachloride.
Vitova, T.; Green, J. C.; Denning, R. G.; Löble, M.; Kvashnina, K.; Kas, J. J.; Jorissen, K.; Rehr, J. J.; Malcherek, T.; Denecke, M. A.
2015. Inorganic Chemistry, 54, 174-182. doi:10.1021/ic5020016
A portable ultrahigh-vacuum system for advanced synchrotron radiation studies of thin films and nanostructures: EuSi₂ nano-islands.
Ibrahimkutty, S.; Seiler, A.; Prüßmann, T.; Vitova, T.; Pradip, R.; Bauder, O.; Wochner, P.; Plech, A.; Baumbach, T.; Stankov, S.
2015. Journal of Synchrotron Radiation, 22, 91-98. doi:10.1107/S1600577514019705
Buchaufsätze
R&D projects conducted at the INE-Beamline for radionuclide research at ANKA and at external SR sources.
Altmaier, M.; Bahl, S.; Bohnert, E.; Dardenne, K.; Fellhauer, D.; Gensch, A.; González-Robles, E.; Kienzler, B.; Krepper, V.; Metz, V.; Pidchenko, I.; Prüßmann, T.; Rothe, J.; Vespa, M.; Vitova, T.
2015. Annual Report 2014 / Institute for Nuclear Waste Disposal. Hrsg.: H. Geckeis, 61-65, KIT Scientific Publishing, Karlsruhe
2014
Zeitschriftenaufsätze
Growth and structure characterization of EuSi₂ films and nanoislands on vicinal Si(001) surface.
Seiler, A.; Bauder, O.; Ibrahimkutty, S.; Pradip, R.; Prüßmann, T.; Vitova, T.; Fiederle, M.; Baumbach, T.; Stankov, S.
2014. Journal of Crystal Growth, 407, 74-77. doi:10.1016/j.jcrysgro.2014.09.005
X-ray absorption spectroscopy of Ru-doped relaxor ferroelectrics with a perovskite-type structure.
Vitova, T.; Mangold, S.; Paulmann, C.; Gospodinov, M.; Marinova, V.; Mihailova, B.
2014. Physical Review B, 89, 144112/1-14. doi:10.1103/PhysRevB.89.144112
Recent advances in the study of the UO₂-PuO₂ phase diagram at high temperatures.
Böhler, R.; Welland, M. J.; Prieur, D.; Cakir, P.; Vitova, T.; Pruessmann, T.; Pidchenko, I.; Hennig, C.; Gueneau, C.; Konings, R. J. M.; Manara, D.
2014. Journal of Nuclear Materials, 448, 330-339. doi:10.1016/j.jnucmat.2014.02.029
Structure of UC₂ and U₂C₃:XRD, ¹³C NMR and EXAFS study.
Carvajal Nunez, U.; Eloirdi, R.; Prieur, D.; Martel, L.; Lopez Honorato, E.; Farnan, I.; Vitova, T.; Somers, J.
2014. Journal of Alloys and Compounds, 589, 234-239. doi:10.1016/j.jallcom.2013.11.202
Labile or stable: Can homoleptic and heteroleptic pyrphos-copper complexes be processed from solution?.
Volz, D.; Wallesch, M.; Grage, S. L.; Göttlicher, J.; Steininger, R.; Batchelor, D.; Vitova, T.; Ulrich, A. S.; Heske, C.; Weinhardt, L.; Baumann, T.; Bräse, S.
2014. Inorganic Chemistry, 53, 7837-7847. doi:10.1021/ic500135m
Ultra-small plutonium oxide nanocrystals: An innovative material in plutonium science.
Hudry, D.; Apostolidis, C.; Walter, O.; Janen, A.; Manara, D.; Griveau, J. C.; Colineau, E.; Vitova, T.; Prüßmann, T.; Wang, D.; Kübel, C.; Meyer, D.
2014. Chemistry - A European Journal, 20, 10431-10438. doi:10.1002/chem.201402008
Buchaufsätze
Pu L3 edge high energy-resolution X-ray absorption near edge structure investigations of actinide partitioning complexes.
Prüßmann, T.; Pidchenko, I.; Banik, N. L.; Dardenne, K.; Rothe, J.; Vitova, T.
2014. ANKA User Reports 2012/2013, 143-144, KIT, Karlsruhe
Investigation of Ca, Ba and Cs molybdates in a Mo bearing borosilicate glass.
Bahl, S.; Kutzer, A.; Roth, G.; Geckeis; Vitova, T.
2014. ANKA User Reports 2012/2013, 137-138, KIT, Karlsruhe
Plutonium oxidation states speciation in perchloric acid by high-energy resolution XANES technique.
Pidchenko, I.; Fellhauer, D.; Prüßmann, T.; Dardenne, K.; Rothe, J.; Vitova, T.
2014. ANKA User Reports 2012/2013, 132-133, KIT, Karlsruhe
Mü-XAFS/XRF/XRD investigation of U(VI) phases in cement alteration products.
Bube, C.; Dardenne, K.; Denecke, M. A.; Kienzler, B.; Metz, V.; Prüßmann, T.; Rothe, J.; Schild, D.; Soballa, E.; Vitova, T.
2014. ANKA User Reports 2012/2013, 30-31, KIT, Karlsruhe
Identifying the Role of Covalency in Transuranic Extractants.
Olson, A. C.; Kozimor, S. A.; Vitova, T.; Loeble, M. W.
2014. ANKA User Reports 2012/2013, 18-19, KIT, Karlsruhe
2013
Zeitschriftenaufsätze
XANES characterization of UO₂/mo(Pd) thin films as models for ε-particles in spent nuclear fuel.
Denecke, M. A.; Petersmann, T.; Marsac, R.; Dardenne, K.; Vitova, T.; Prüßmann, T.; Borchert, M.; Bösenberg, U.; Falkenberg, G.; Wellenreuther, G.
2013. Journal of Physics: Conference Series, 430, 012113/1-4. doi:10.1088/1742-6596/430/1/012113
Comparative investigation of N donor ligand-lanthanide complexes from the metal and ligand point of view.
Prüßmann, T.; Denecke, M. A.; Geist, A.; Rothe, J.; Lindqvist-Reis, P.; Löble, M.; Breher, F.; Batchelor, D. R.; Apostolidis, C.; Walter, O.; Caliebe, W.; Kvashnina, K.; Jorissen, K.; Kas, J. J.; Rehr, J. J.; Vitova, T.
2013. Journal of Physics: Conference Series, 430, 012115/1-5. doi:10.1088/1742-6596/430/1/012115
Local and electronic structure of americium-bearing PuO₂.
Prieur, D.; Carvajal-Nunez, U.; Vitova, T.; Somers, J.
2013. European Journal of Inorganic Chemistry, (9), 1518-1524. doi:10.1002/ejic.201201294
Actinide and lanthanide speciation with high-energy resolution X-ray techniques.
Vitova, T.; Denecke, M. A.; Göttlicher, J.; Jorissen, K.; Kas, J. J.; Kvashnina, K.; Prüßmann, T.; Rehr, J. J.; Rothe, J.
2013. Journal of Physics: Conference Series, 430, 012117/1-4. doi:10.1088/1742-6596/430/1/012117
Coupling XRD, EXAFS, and ¹³C NMR to study the effect of the carbon stoichiometry on the local structure of UC¹⁺⁻̽.
Carvajal Nunez, U.; Martel, L.; Prieur, D.; Lopez Honorato, E.; Eloirdi, R.; farnan, I.; Vitova, T.; Somers, J.
2013. Inorganic Chemistry, 52, 11669-11676. doi:10.1021/ic402144g
Exploring the solution behavior of f-element coordination compounds : a case study on some trivalent rare earth and plutonium complexes.
Löble, M. W.; Ona-Burgos, P.; Fernández, I.; Apostolidis, C.; Morgenstern, A.; Walter, O.; Bruchertseifer, F.; Kaden, P.; Vitova, T.; Rothe, J.; Dardenne, K.; Banik, N. L.; Geist, A.; Denecke, M. A.; Breher, F.
2013. Chemical science, 4 (9), 3717-3724. doi:10.1039/C3SC50708D
Sulfur K X-ray absorption near edge structure spectroscopy on the photochrome sodalite variety hackmanite.
Göttlicher, J.; Kotelnikov, A.; Suk, N.; Kovalski, A.; Vitova, T.; Steininger, R.
2013. Zeitschrift für Kristallographie, 228, 157-171. doi:10.1524/zkri.2013.1587
Characterization of U(VI)-phases in corroded cement products by micro(μ)-spectroscopic methods.
Rothe, J.; Brendebach, B.; Bube, C.; Dardenne, K.; Denecke, M. A.; Kienzler, B.; Metz, V.; Prüßmann, T.; Rickers-Appel, K.; Schild, D.; Soballe, E.; Vitova, T.
2013. Journal of Physics: Conference Series, 430, 012114/1-5. doi:10.1088/1742-6596/430/1/012114
Buchaufsätze
R&D projects conducted at the INE-Beamline for Actinide Research at ANKA and at external SR sources.
Bube, C.; Dardenne, K.; Denecke, M. A.; Fröhlich, D. R.; Kienzler, B.; Metz, V.; Panak, P. J.; Prüßmann, T.; Rothe, J.; Schild, D.; Skerencak, A.; Soballa, E.; Vitova, T.
2013. Annual Report 2012 : Institute for Nuclear Waste Disposal. Ed.: H. Geckeis, 77-83, KIT Scientific Publishing, Karlsruhe
Structural investigations on the impact of increasing MoO3 loadings in borosilicate glasses for the immobilization of Mo-rich nuclear wastes.
Kutzer, A.; Vitova, T.; Kvashnina, K.; Prüßmann, T.; Rothe, J.; Adam, C.; Kaden, P.; Denecke, M. A.; Weisenburger, S.; Roth, G.; Geckeis, H.
2013. Annual Report 2012 : Institute for Nuclear Waste Disposal. Ed.: H. Geckeis, 73-75, KIT Scientific Publishing, Karlsruhe
2012
Zeitschriftenaufsätze
U(VI) removal kinetics in presence of synthetic magnetite nanoparticles.
Huber, F.; Schild, D.; Vitova, T.; Rothe, J.; Kirsch, R.; Schäfer, T.
2012. Geochimica et Cosmochimica Acta, 96, 154-173. doi:10.1016/j.gca.2012.07.019
Fabrication and characterization of (U, Am)O₂₋ₓ transmutation targets.
Vespa, M.; Rini, M.; Spino, J.; Vitova, T.; Somers, J.
2012. Journal of Nuclear Materials, 421, 80-88. doi:10.1016/j.jnucmat.2011.11.055
The INE-beamline for actinide science at ANKA.
Rothe, J.; Butorin, S.; Dardenne, K.; Denecke, M. A.; Kienzler, B.; Löble, M.; Metz, V.; Seibert, A.; Steppert, M.; Vitova, T.; Walther, C.; Geckeis, H.
2012. Review of Scientific Instruments, 83, 043105/1-13. doi:10.1063/1.3700813
Proceedingsbeiträge
High-resolution X-ray absorption spectroscopy of U in cemented waste form.
Vitova, T.; Denecke, M. A.; Finck, N.; Göttlicher, J.; Kienzler, B.; Rothe, J.
2012. 2nd Internat.Workshop on Actinide Brine Chemistry in a Salt-Based Repository (ABC-SALT (II)), Karlsruhe, November 7-8, 2011, 107-108, KIT Scientific Publishing, Karlsruhe
U removal kinetics in the presence of magnetite and maghemite nanoparticles.
Huber, F. M.; Schild, D.; Vitova, T.; Rothe, J.; Kirsch, R.; Schäfer, T.
2012. 4th Annual Workshop Proceedings of the Collaborative Project "Redox Phenomena Controlling Systems" (7th EC FP CP RECOSY). Ed.: M. Altmaier, 383-397, KIT Scientific Publishing, Karlsruhe
Study of U oxidation states in natural geological material.
Pidchenko, I.; Salminen-Paatero, S.; Vitova, T.; Suksi, J.
2012. 4th Annual Workshop Proceedings of the Collaborative Project "Redox Phenomena Controlling Systems" (7th EC FP CP RECOSY). Ed.: M. Altmaier, 223-230, KIT Scientific Publishing, Karlsruhe
Buchaufsätze
High-resolution X-ray absorption spectroscopy study of plutonium dioxide in contact with water.
Vitova, T.; Butorin, S. M.; Seibert, A.; Rothe, J.; Dardenne, K.; Vegelius, J.; Caciuffo, R.; Denecke, M. A.
2012. ANKA - Annual Report 2010/2011 Karlsruhe : Karlsruhe Institute of Technology, 2012 Also publ.online, 394-395
New insights in electronic properties of f-element coordination compounds.
Löble, M.; Vitova, T.; Brendebach, B.; Rothe, J.; Dardenne, K.; Denecke, M. A.; Breher, F.
2012. ANKA - Annual Report 2010/2011 Karlsruhe : Karlsruhe Institute of Technology, 2012 Also publ.online, 337-338
P- and S- k-edge XANES investigation of U(VI) complexes with several organic model compounds.
Li, B.; Dardenne, K.; Vitova, T.; Rothe, J.; Foerstendorf, H.; Raff, J.
2012. ANKA - Annual Report 2010/2011 Karlsruhe : Karlsruhe Institute of Technology, 2012 Also publ.online, 379
Mo K-edge XAS study of Mo-rich model nuclear waste glass.
Kutzer, A.; Vitova, T.; Denecke, M. A.; Roth, G.; Geckeis, H.
2012. ANKA - Annual Report 2010/2011 Karlsruhe : Karlsruhe Institute of Technology, 2012 Also publ.online, 336
Interaction of uranium(VI) with synthetic magnetite nanoparticles.
Vitova, T.; Huber, F.; Rothe, J.; Dardenne, K.; Schäfer, T.
2012. ANKA - Annual Report 2010/2011 Karlsruhe : Karlsruhe Institute of Technology, 2012 Also publ.online, 329-330
Probing Eu(III) adsorbed to Fe-containing clay mineral: an application for high-resolution X-ray emission spectroscopy.
Schepperle, J.; Finck, N.; Vitova, T.
2012. ANKA - Annual Report 2010/2011 Karlsruhe : Karlsruhe Institute of Technology, 2012 Also publ.online, 327-328
The latest development and optimization of the high-resolution X-ray emission spectrometer at the INE-beamline.
Vitova, T.; Dardenne, K.; Denecke, M. A.; Ernst, H.; Rothe, J.
2012. ANKA - Annual Report 2010/2011 Karlsruhe : Karlsruhe Institute of Technology, 2012 Also publ.online, 326
In-situ RIXS studies of the possibilities of the existence of Pu(V) in plutonium dioxide.
Butorin, S. M.; Vitova, T.; Vegelius, J.; Seibert, A.; Caciuffo, R.; Denecke, M. A.
2012. ANKA - Annual Report 2010/2011 Karlsruhe : Karlsruhe Institute of Technology, 2012 Also publ.online, 295-296
P and S K edge XANES investigations of lanthanide complexes consisting of a κ⁶N-donor ligand with podand topology.
Löble, M.; Vitova, T.; Brendebach, B.; Rothe, J.; Dardenne, K.; Denecke, M. A.; Breher, F.
2012. ANKA - Annual Report 2010/2011 Karlsruhe : Karlsruhe Institute of Technology, 2012 Also publ.online, 307-309

Collaborations

Polly Arnold

University of Edinburgh, UK

http://www.homepages.ed.ac.uk/parnold/

 

Robert Baker

Trinity College Dublin, Ireland

https://sites.google.com/site/bakeresearchgroup/home

 

       

Melissa Denecke

 

The University of Manchester, UK

http://www.chemistry.manchester.ac.uk/people/staff/profile/?ea=melissa.denecke

 

Stosh Kozimor

 

Los Alamos National Laboratory, USA

https://www.lanl.gov/

 

Kristina Kvashnina

 

European Synchrotron Radiation Facility, France

http://www.esrf.eu/home/Members/content/staff-web-pages/kvashnin.html

 

Philippe Martin

 

CEA, DEN, DEC, CEN Cadarache, France

http://www.pubfacts.com/author/Philippe+M+Martin

 

       

 

Joe Somers

Thiery Wiss

Olaf Walter

Karin Popa

Antonio Bulgheroni

Dario Manara

Nicola Magnani

Roberto Caciuffo

 

Joint Research Center-Karlsruhe, Germany

https://ec.europa.eu/jrc/en/about/jrc-site/karlsruhe

 

John Rehr

University of Washington, USA

http://faculty.washington.edu/jjr/

David Shuh

 

Lawrence Berkeley National Laboratory, USA

 

http://actinide.lbl.gov/gtsc/Staff/dkshuh/

 

Laura Simonelli ALBA Synchrotron Radiation Facility, Spain http://www.cells.es/en/beamlines/bl22-claess/staff

Svetoslav Stankov

Jörg Göttlicher

Stefan Schuppler

Peter Nagel

 

ANKA Synchrotron Radiation Facility, Germany

http://nanodynamics-group.com/stankov.html

 

 

Alexander Soldatov

Southern Federal University http://www.nano.sfedu.ru/contacts.html

Contact us!

If you are looking for a bachelor, master or PhD project with exciting topic including application of novel synchrotron based X-ray spectroscopy methods contact us. You will have the opportunity to reveal structural properties of actinide and lanthanide systems important for example for molecular scale understanding of processes in a nuclear waste repository. You will work in a young, motivated and enthusiastic team and will perform experiments at the ANKA, KIT and other national and international synchrotron radiation facilities.

Email: Tonya.Vitova∂kit.edu
Telephone: +49 721 608 24024
Address: Karlsruhe Institute of Technology
Institute for Nuclear Waste Disposal
Hermann von Helmholtz Platz 1
76344 Eggenstein-Leopoldshafen, Germany

The Group life