The impact of plutonium speciation on the distribution coefficients in a sediment-sea water system, and radiological assessment of doses to humans.
When radionuclides are released from a source into the marine environment, the assessment of long term consequences to humans depends on information on the source term, transport in water, interactions with sediments (KD) and biological uptake (CF). Sensitivity analysis of assessment models demonstrates that KD is one of the most sensitive parameters contributing to large uncertainties in the assessment. Furthermore, the interaction of Pu-species with sediments is a time and temperature dependent process. The distribution coefficient, Bq kg(-1) sediment per Bq L(-1) sea water, increases with time until pseudo-equilibrium/equilibrium is reached (KD). Thus, the contact time between contaminated sea water and sediments should be taken into account in dispersion and dose assessment models. In the present work, dynamic tracer experiments have been performed where different Pu-species are added to a sediment-sea water system to obtain information on KD's. After a defined contact time, the samples have been sequentially extracted to determine mobile and bound fractions. The results indicate that the distribution coefficient, KD, for plutonium depends on Pu-species in question. Thus, sediments act as a sink for Pu(III, IV) (high KD), while Pu(III, IV)-organic and Pu(V, VI) should be considered more mobile (low KD). Furthermore, the interaction with inert fractions obtained from sequential extraction depends less on Pu-species but increase with time. For short time interactions, species-specific time functions rather than KD constants should be applied in assessment models. When the accepted KD (10(5) L kg(-1)) is implemented in the model, the estimated collective dose is about 8 x 10(-4) person-Sv, i.e., a factor of about 2 lower than for Pu(III, IV)-organic and Pu(V, VI). So changes in KD have an impact on the assessment of collective dose received from a potential release of plutonium from fallout, reactor accidents, etc., which underlines the need for more detailed studies on speciation, kinetics, and KD's in different sediment-sea water systems.
Department of Chemistry and Biotechnology, Agricultural University of Norway, Aas. lindis.skipperud@ikb.nlh.no
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D000085:Acetates / Q000737:chemistry; D000327:Adsorption; D019015:Geologic Sediments / Q000737:chemistry*; D006801:Humans; D006863:Hydrogen-Ion Concentration; D019811:Hydroxylamine / Q000737:chemistry; D008956:Models, Chemical; D017942:Nitric Acid / Q000737:chemistry; D011005:Plutonium / Q000032:analysis / Q000737:chemistry*; D011829:Radiation Dosage; D011834:Radiation Monitoring; D011851:Radioactivity; D012623:Seawater / Q000737:chemistry*; D014875:Water Pollutants, Radioactive / Q000032:analysis*
D000085:Acetates; D014875:Water Pollutants, Radioactive; D019811:Hydroxylamine; D017942:Nitric Acid; D011005:Plutonium; C018824:ammonium acetate