Institute of Resource Ecology Institut für Ressourcenökologie

Institute of Resource Ecology | www.hzdr.de

Institute of Resource Ecology

Institut für Ressourcenökologie

G. Geipel, G. Bernhard, J. Lippmann-Pipke, V. Brendler, N.Jordan, K. Müller, L. Lütke

French - German Research for Nuclear Safety: Chemistry of the f-ElementsStrasbourg, February, 22nd - 23rd, 2012

Member of the Helmholtz AssociationPage 2Institute of Resource Ecology | www.hzdr.de

The Research Field Health The Programme Cancer Research

The Research Field Energy The Programme Nuclear Safety Research The Programme Materials, Energy, and Resource Efficiency

The Research Field MatterThe Programme Matter and CosmosThe Programme From Matter to Materials and Life The Programme Matter and Technologies

Helmholtz‐Zentrum Dresden – RossendorfResearch and Structure 2012


Institutes at HZDR

Institute of Radiation Physicsoperating Elbe Sourcehigh power laser systems

Dresden High Magnetic Field Laboratorypulsed magnetic fields near to 100 Tesla

Institute of Ion Beam Physics and Materials Researchincluding reactor materials

Institute of Radiopharmacyoperating Cyclotron in Leipzig

Institute of Resource Technologyoperating AMS in Rossendorf


Institute of Fluid Dynamicssimulation of turbulent fluid systems


Reasons:- Policy (nuclear phase out, no budget growth for Nuclear Research),- Focusing the research on 3 Research Areas,- New research aspect “Resources” was included,

Foundation of a new Institute of Resource Technology (HZDR/University BA Freiberg)

- Foundation of 2 new Institutes

- Institute of Safety Research => Institute of Fluid Dynamics- Institute of Radiochemistry => Institute of Resource Ecology

HZDRChanging of Research and Structure in 2012


- MotivationProtection of humankind and the environment from hazards caused by pollutants resulting from technical processes connected with the generation of energy and raw materials. The scientific challenge is to treat technology and ecology in a unified way which opens the possibility to contribute to the safety and public acceptance of technical processes of great importance for the future of humankind.

- ScienceThe science is focused on the ecology of radioactive and non-radioactive hazardous substances in the context of nuclear waste disposal, the production of nuclear energy, and of processes along the value chain of metalliferous raw materials.

- ResearchThe research aims of the institute are concentrated on- safety aspects of nuclear waste disposals, future transmutation facilities, and of current and

future reactors to develop strategies for risk mitigation, in particular the avoidance and limitationof potential accidents.

- the interactions of biological systems with long-lived radionuclides and non-radioactive metalson a molecular and macroscopic level in environmental and technical processes for a better prediction of their mobilization or immobilization in nature,



Mission:Application oriented basic research in Radioecology.Protection of human and envorinment against the danger fromof radioactive and heavy metals Into the biosphere.

Goal:Investigation of interactions and mobility of Actinides (U, Np, Pu, Am, Cm) and heavy metals on a molecularlevel in Geo- and Biosystems, to increase the macroscopicknowledge of ongoing prozesses and to model them.



Facilities in Dresden and Leipzig I• Controlled areas for handling radioactive

materials (actinides)– Special laboratories for handling gen-manipulated

organisms– Laser-Induced spectroscopy

• Designed for actinides and lanthanides aswell as for organic compounds

• Tunable solid state laser systems– ns – pulses

» Time resolved luminescence spectroscopy» Photoacoustic spectroscopy

– fs – pulses» Time resolved fluorescence spectroscopy

– Time range from sub-ns to ms• Cryo techniques

– ~100 K and 2 K (in construction)


– CLS Microscopy and conventional microscopy

– IR (ATR FT-IR) and Raman Spectroscopy

– Microcalorimetry

– Geo-PET

– CD Spectroscopy

– Analytics etc.

Facilities in Dresden and Leipzig I


ROBLGrenoble Leipzig

New since01.01.2012


Research Fields and Programmes of HZDR Topics (Institute of Resource Ecology)


Organization of Research “NSR”- Subtopics


Organization of Research “MER”‐ Subtopics


Human

Meat MilkFruit Bread

GrainAnimal

Plant

Water Soil Air

Uraniumspeciation

Research:

Water- Ground Water- Surface Water- Drinking Water- Seepage Water

Soil- Rocks- Minerals- Pore Water

Nuclear Waste Disposal- Near field- Far field- Data bases

Bacteria- Cell- Membrane- Biomass- Bio-Film- Diversity

Plant- Cell- Biomass- Compartments

Human- Cell- Bio-Fluid

Chemistry of Long-lived Radionuclides

Food Chain

Speciation and TransportPhenomena


• Essential goals of Research in Nuclear Waste Disposal– Structure of Binding forms

– Stability of Binding forms

– Transport phenomena

• Need of a broad spectrum of methods– Determination of

• Oxidation states• Bond distances• Characterization of neighboring elements


Long lived radionuclides in final disposal systems

• THEREDA database– opened for access to first data

• System salts in oceans• System Nd / Am / Cm• Links to modeling with EQ 3/6 and GWB

• Diffusion of uranium in Opalinus clay • Resulting kd values agree with batch experiments• Overall no significant dependence on temperature• High potential of retention (0.1cm / a for uranium(VI) )

• Colloid formation of tetravalent Actinides• Containing silicate due to formation in near neutral geogenic

solutions• Stable over many years• Size < 20 nm• Coffinit analogue structure


• MOs are ubiquitous in nature, having a significant impact on the sorption and hence the migration behavior of actinides (metals in general) necessity of characterization of actinide-bacteria species formed and elucidation of interaction mechanisms

• Actinide bacteria interactions can be subdivided into:a) direct interaction processes

e.g. metal uptake, bio sorption,-reduction, -mineralization

b) indirect interaction processes

e.g. complexation by released cellular bioligands

Bacteria Metal Interactions

[2] Merroun et al. (2008) J. Contam. Hydrol. 102, 285–295.

[1 Moll, H. et al. (2005) final report of BMWi project 02E9491, FZR-422, FZD, Germany.

[2]

[2]

[1][2]

Uptake

Bioreduction


Reactions of uranium with ligands in the cytoplasm of plant cellsI. Complexation with glutathione [1]

UO22+ + 2H+ + GS- => UO2H2GS+

log β°121 = 38,7

II. Reduction Uran(VI) to U(IV) [2]

III. Formation of phytochelatins and metallothioneinsa)

Reducing agents?a) Glutathione by 33 %b) Cellular Reductase

Reducing activity of cytoplasmatic proteins, Protein blot after gelelektrophoreticSeparation

Sulfur

Uranium

Ring formation between two carboxylic groups, no interaction with the SH-group

DFT-Calculation (Prof. S. Tsushima)

Uran(IV) in the Cytoplasm, laser-induced Photoacoustik

Synthesis of phytochelatins needs metal bindung at the thiolgoup of the glutathion > there bindung of uranium(IV)

Acidic hydrolysis of DNP-labelled phytochelatin-fractions (HPLC)

14 KDaDNP-GSH Hydrolysis

[1] Frost et al. Radiochim. Acta, 2011[2] Viehweger et al. BioMetals, 2011.

Gelelektrophoretic separation of cytoplasmatic proteins

Protein bond to uranium (Detection by Laser-Induced Spectroscopy)

IV. SummaryPhytochelatins Metallothioneins

• Different oxidation states of uranium in the cytoplasm.• Bond to different ligands and different functional groups.

a) Cooperation with Prof. W. Maret, King‘s College London


Cooperation with Dr. G. LefèvreÉcole Nationale Supérieure de Chimie de Paris (ENSCP)

Short‐term post doc position for K. Müller at ENSCPMüller, K.; Lefèvre, G. Vibrational Characteristics of Outer‐Sphere Surface Complexes: Example of Sulfate Ions Adsorbed onto Metal (Hydr)oxides. Langmuir 2011, 27, (11), 6830‐6835.

Visiting fellowships for G. Lefèvre at HZDRMüller, K.; Foerstendorf, H.; Meusel, T.; Brendler, V.; Lefèvre, G.; Comarmond, M. J.; Payne, T. E. Sorption of U(VI) at the TiO2 ‐ water interface: An in situ vibrational spectroscopic study. Geochimica et Cosmochimica Acta 2012, 76, (0), 191‐205.

In progress: Bilateral joint project on “Formation of ternary metal complexes on mineral oxide surfaces”(ANR‐DFG 2012 ?)


Ion transfer from surface to crystal: mechanisms of pollutant trapping

Ph.D. Student: Andrea Sabău

Aims: Investigate the processes that promote Eu(III), Ni(II) and U(VI) trapping into calcite

Incorporation of results into

transport model

Batch experiments at different pCO2 and pH:

generate sorption isotherms

Surface species and sorption/incorporation processes: ATR FT-IR,

TRLFS, RBS, Tof-SIMS, PIXE


International Workshop on

Advanced Techniques in Actinide Spectroscopy (ATAS)05.‐07.11.2012, Helmholtz‐Zentrum Dresden‐Rossendorf, Germany

Focus on recent advances in actinide chemistry from both a spectroscopic and theoretical point of view:

Vibrational spectroscopy (IR and Raman) Laser‐induced spectroscopy (luminescence and photoacoustic) X‐ray absorption spectroscopy and Quantum chemical calculations

Topics Improvements of in situ experimental setups Applications of quantum chemical methods in predictive and interpretative ways New data processing algorithms

Scientific commitee S. Tsushima (HZDR / IRE) K. Müller (HZDR / IRE) R. Steudtner (HZDR / IRE) A. Scheinost (HZDR / IRE) Chr. Den Auwer (Nice S. A. Univ.) T. Stumpf (KIT /INE) J. Tits (PSI) T. Kimura (JAEA) V. Vallet (Lille Univ.) F. Livens (Manchester Univ.)

Invited and confirmed talks P. Yang (Pacific Northwest National

Laboratory, USA) P. Persson (Umeå University, Sweden) T. Saito (Tokyo University, Japan) J. Li (Tsinghua University Peking,

China)

1st announcement soon!!!


Thank you

Institute of Resource Ecology Institut für Ressourcenökologie

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