Association of dissolved radionuclides released by the Chernobyl accident with colloidal materials in surface water

The association of dissolved Sr-90, Pu-239,Pu-240 and Am-241 with natural colloids was investigated in surface waters in the Chernobyl nuclear accident area. A 4-step ultrafiltration (UF) study (<1 kilodaltons (Da), 1-10 kDa, 10-100 kDa, 100 kDa<) showed that 49-83% of Pu-239,Pu-241 and 76% of Am-241 are distributed in colloids of the two size fractions larger than 10 kDa (nominal molecular weight limit of the filter, NMWL), while Sr-90 was found exclusively (85-88%) in the lowest molecular size fraction below 1 kDa (NMWL) for the Sahan River water at the highly contaminated area close to the Chernobyl Nuclear Power Plant (ChNPP). Consistent results were obtained by 2-step fractionation (larger than and smaller than 10 kDa (NMWL)) for river and lake waters including other locations within about 30 km away from ChNPP. It is likely that Pu and Am isotopes were preferentially associated with dissolved organic matter of high molecular size, as suggested by the fact that (i) only a few inorganic elements (Mg, Ca, Sr, Si, Mn, Al) were found in the colloidal size ranges, and (ii) the positive correlation between dissolved organic C (DOC) concentrations and UV absorbance at 280 mn, a broad absorption peak characteristic of humic substances (HS) was found. A model calculation on the complexation of Pu and Am with HS as an organic ligand suggests that the complexed form could be dominant at a low DOC concentration of 1 mgC L-1, that is commonly encountered as a lower limit in fresh surface water. The present results suggest the general importance of natural organic colloids in dictating the chemical form of actinides in the surface aquatic environment. (C) 2004 Elsevier Ltd. All rights reserved.