Radionuclide speciation in effluent from La Hague reprocessing plant in France.

ABSTRACT

Effluent from the La Hague nuclear fuel reprocessing plant was mixed with seawater in order to investigate the fate of the various radionuclides. Thus, a major objective of the present work is to characterize the effluent from La Hague reprocessing plant and to study how the radionuclide speciation changes with time when discharged into the marine environment. Discharges from the La Hague nuclear reprocessing plant represent an important source of artificially produced radionuclides to the North Sea. The transport, distribution, and biological uptake of radionuclides in the marine environment depends, however, on the physicochemical forms of radionuclides in the discharged effluents and on transformation processes that occur after entering the coastal waters. Information of these processes is needed to understand the transport and long-term distribution of the radionuclides. In the present work, a weekly discharged effluent from the nuclear fuel reprocessing plant at Cap La Hague in France was mixed with coastal water and fractionated with respect to particle size and charged species using ultra centrifugation and hollow fiber ultrafiltration with on line ion exchange. The size distribution pattern of gamma-emitting radionuclides was followed during a 62-h period after mixing the effluent with seawater. 54Mn was present as particulate material in the effluent, while other investigated radionuclides were discharged in a more mobile form or were mobilized after mixing with sea water (e.g., 60Co) and can be transported long distances in the sea. Sediments can act as a sink for less mobile discharged radionuclides (Skipperud et al. 2000). A kinetic model experiment was performed to provide information of the time-dependent distribution coefficients, Kd (t). The retention of the effluent radionuclides in sediments was surprisingly low (Kd 20-50), and the sediments acted as a poor sink for the released radionuclides. Due to the presence of non-reacting radionuclide species in the effluent, a major fraction of the radionuclides, such as Cs-isotopes, 106Ru and 125Sb, in the effluent will be subjected to marine transport to the Northern Seas (i.e., the North Sea, Norwegian Sea and the Barents Sea). The La Hague effluent may, therefore, contribute to enriched levels of radionuclides found in the English Channel, including 90Sr, 60Co and Pu-isotopes, and also 106Ru and 125Sb.