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Chemical Speciation of Long-Lived Radionuclides in the Environment

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Chemical Speciation of Long-Lived Radionuclides in the Environment Chemical Speciation of Long-Lived Radionuclides in the Environment Xiaolin Hou Risø-R-1677(EN) Risø National Laboratory for Sustainable Energy Technical University of Denmark Roskilde, Denmark November 2008 Author: Xiaolin Hou Risø-R-1677(EN) November 2008 Title: Chemical Speciation of Long-Lived Radionuclides in the Environment Division: Radiation Research Division Abstract (max. 2000 char.): ISSN 0106-2840 ISBN 978-87-550-3730-4 This project started in November 2005 and ended in November 2008, the work and research approaches are summarized in this report. This project studied the speciation of radionuclides in environment. A number of speciation analytical methods are developed for 129 99 237 determination of species of I, Tc, isotopes of Pu, and Np in Contract no.: seawater, fresh water, soil, sediment, vegetations, and concrete. The developed methods are used for the investigation of the chemical speciation of these radionuclides as well as their environmental Group's own reg. no.: behaviours, especially in Danish environment. In addition the speciation of Pu isotopes in waste samples from the decommissioning of Danish nuclear facilities is also investigated. The report summarizes these works completed in this project. Sponsorship: Through this research project, a number of research papers have Supported by the Villum been published in the scientific journals, the research results has Kann Rasmussen Foundation also been presented in the Nordic and international conference/meeting and communicated to international colleagues. Cover : Some publications are also enclosed to this report. Participants of this project: Xiaolin Hou (Risø-DTU, project leader)) Per Roos (Risø-DTU) Sven P. Nielsen (Risø-DTU) Jussi Jernstroem (Risø-DTU) Svend Olsen (Risø-DTU) Violeta Hansen (Risø-DTU) Ala Aldahan (Uppsala University, Sweden) Göran Possnert (Uppsala University, Sweden) Susanne Persson (Uppsala University, Sweden) Pages: 145 Edvard Englund (Uppsala University, Sweden) Information Service Department Acknowledgement: Risø National Laboratory for We like to thank the Villum Kann Rasmussen Foundation for the Sustainable Energy Technical University of Denmark finical support to complete this project. P.O.Box 49 DK-4000 Roskilde We also like to thank all stuffs in Radioecology and Tracer Denmark Program, Radiation Research Division, Risø National laboratory for Telephone +45 46774004 Sustainable Energy, Technical University of Denmark for their [email protected] contributions to this work. Fax +45 46774013 www.risoe.dtu.dk 2 Risø-R-1677(EN) Contents: 1. Objectives of the project 2. Instrumentations 2.1 X SeriesII ICP-MS and HPLC 2.2 Air sampler for iodine species collection from atmosphere 2.3 Combustion furnace 3. Development of analytical methods 3.1 Determination of 127I in environmental samples using ICP-MS 3.1.1 Separation of iodine from solid sample using combustion 3.1.2 Measurement of iodine using ICP-MS 3.2 Determiantion of 129I using accelerator mass spectrometry (AMS) 3.3 Determination of Pu isotopes and 237Np in environment 3.3.1 Separation of Pu and Np from environmental samples 3.3.2 Measurement of 238Pu, 239,240Pu and 237Np using alpha spectrometry 3.3.3 Measurement of 239Pu, 240Pu, 241Pu and 237Np using ICP_MS 3.3.4 Measurement of 241Pu using liquid scintillation counting 3.4 Determination of 99Tc and Pu/Am in environmental samples using HPLC coupled with ICP-MS. 3.4. 1 Separation of Pu and Am using ion chromatography HPLC 3.4.1.1 Extraction chromatography for separating trivalent light lanthanides and actinides 3.4.1.2 Cation exchange column for pre-concentrating trivalent actinides 3.4.1.3 Ion chromatography column for final separation of trivalent actinides 3.4.2 Separation of Tc using ion chromatography HPLC 3.4.2.1 Separation procedure 3.4.2.2 Elution of technetium from ion chromatography column 3.5 Method for the speciation of 129I and 127I in water samples 3.5.1 Speciation separation of iodine in water samples using ion exchange chromatography. 3.5.2 Speciation of 129I in water using extraction and co-precipitation 3.5.2 Speciation/fractionation of 129I and 127I in soil/sediment samples 3.5.3. Speciation method for 129I and 127I in atmosphere 3.6 Speciation/fractionation of plutonium isotopes, 237Np and 241Am in soil, sediment and concrete samples using dynamic sequential extraction 3.7 Analytical method for the determination of rhenium Risø-R-1677(EN) 3 3.8 Investigation on Re-absorption of Pu during the fractionation of Pu in soil and sediment 4. Investigation of speciation of the radionuclides in environmental samples 4.1 Speciation of 129I in North Sea surface water 4.2 Speciation of 129I in precipitation collected in Roskilde, Denmark 2001-2006 4.3. Partition of 137Cs and 129I in the Nordic lake sediment, pore-water and lake water 4.4 129I and 127I and their speciation in lake sediment 4.5 Iodine isotopes (127I and 129I) in aerosols 4.6. Speciation of Pu in soil, sediment and concrete samples from decommissioning of Danish nuclear reactor 4.7 Speciation of 99Tc and Re in seaweed samples 4.8 Speciation of Pu isotopes and 237Np in water samples collected from Framvaren fjord 4.9 Speciation of 129I and 127I in atmosphere for investigation of geochemical cycle of iodine using reprocessing 129I as tracer. 5. Conclusion and perspective 6. List of papers published and to be published 7. Papers presented in conferences and meetings Appendix: Some published materials Paper-1-EST-129I-NorthSea-2007.pdf Paper-2-JER-Dynamic adsorption2008.pdf Paper-3-129I-speciation-review-ACA2008.pdf Paper-4-ACA-review-article-2008.pdf Paper-5-Handbook of Iodine-CH015-iodine speciation-2009.pdf Paper-6-EST-modeling129I-2008.pdf Paper-7- Jussi-PuAm.pdf 4 Risø-R-1677(EN) 1. Objectives of the project: The aim of the project is to study the chemical speciation of the radionuclides iodine-129 (129I), plutonium-238, -239, -240, -241 (238,239,240,241Pu), technetium-99 and neptunium-237 (237Np) in order to obtain information on their behaviour in the environment. Once released to the environment these radionuclides and their radioactive decay products remain for a long time due to their very long halflives. The results of the project will provide understanding and data for the quantification of the environmental processes governing the dispersion and biological transfer of these radionuclides and thus enable reliable assessments to be made of the associated risks to man and environment. Specific aims of the project include: 1) To examine the chemical speciation of the radionuclides in environmental samples with emphasis on the radioactive contamination and nuclear waste repositories covering − Speciation analysis of Pu isotopes in contaminated environmental samples from Thule, Greenland, − Speciation analysis of Pu isotopes, 129I and 99Tc in samples related to nuclear waste from the operation and decommissioning of nuclear facilities in Denmark − Environmental behaviour study of Pu isotopes, 129I and 99Tc related to their transfer in the environment and to humans with an emphasis on the Danish environment. 2) To develop analytical methods for the chemical speciation of 129I, isotopes of Pu, 99Tc and 237Np in relation to risk assessment involving − Development of ultra-trace analysis methods for 99Tc, 129I, isotopes of Pu and 237Np with inductively-coupled plasma mass spectrometry, accelerator mass spectrometry, alpha spectrometry and liquid scintillation counting techniques. − Development of separation methods for the chemical speciation of 129I, isotopes of Pu, 99Tc, and 237Np in environmental samples using chromatographic techniques as well as extraction, and sequential extraction. The project focuses on a quantitative understanding of the chemical speciation of radionuclides in the environment that can be used for risk assessment of the plutonium contamination in Thule, Greenland, issues related to a Danish repository for nuclear waste and radionuclides in Danish waters from European reprocessing facilities. Risø-R-1677(EN) 5 2. Instrumentations 2.1 X SeriesII ICP-MS and HPLC An X SeriesII ICP-MS and HPLC equipments were purchased from Thermo Electron Corporation, the instruments have been installed and tested in July 2006 (Figure 1). The performance of the instruments have been tested and optimized for the determination of the target radionuclides and speciation separation- determination. Satisfied results (sensitivity, detection limit, stability, etc.) have beenobtained 127 99 for the determination of I, Tc, isotopes of Pu, Figure 1 Thermo X SeriesII ICP-MS coupled with HPLC 237 and Np. The HPLC has been coupled to ICP- for speciation analysis of nuclides MS for the automated separation and speciation of analytes including 127I, 99Tc, and isotopes of Pu and 237Np. 2.2 Air sampler for iodine species collection from atmosphere Two sets of air sampler was designed and manufactured by a commercial company (Staplex, USA), which has been used to collect different chemical speciation of iodine from atmosphere, such as particle, inorganic gaseous iodine, and organic gaseous iodine. The equipments have been installed and tested (Figure 2). A satisfied performance has been obtained, except the problems of vacuum pump, in which carbon brush has to be replaced every 150 hours operation. The equipment has been successfully applied to collect atmospheric samples from different location in Denmark, Sweden and Lithuania. Figure 2 Air sampler setup for collecting particulates associated, in organic gaseous and organic gaseous iodine 6 Risø-R-1677(EN) 2.3 Combustion furnace A specific combustion furnace was designed and manufactured by a commercial company (Carbolite, UK), which is used to separate iodine from various solid samples such as soil, sediment, vegetation, tissues, air particles, filters, and active charcoal. The furnace has been installed and tested (Figure 3), a good separation efficiency (>80%) was obtained. The equipment has been successfully used for the analysed the samples for 129I and 127I in solid samples. Figure 3 Schematic diagram and picture of combustion facility (Carbolite, UK) for the separation of iodine from solid sample.
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