Studies of Long-lived Radionuclides in the Environment - with Emphasis on 99Tc, 237Np and Pu Isotopes

Studies of the long-lived anthropogenic radionuclides 99Tc, 237Np, 239Pu and 240Pu were performed in marine and terrestrial areas contaminated by different accidental and controlled releases of radioactive materials. The three main sources discussed in this thesis are nuclear weapons tests, nuclear reprocessing plants and the Chernobyl accident. Results are mainly based on measurements of environmental samples collected in different parts of Sweden. An analytical method for trace analysis of plutonium and neptunium in environmental samples using ICP-MS (Inductively Coupled Plasma Mass Spectrometry) is described, and the results compared with those from conventional alpha spectrometry. The use of activated carbon filters for the separation of 99Tc from marine waters, with an adsorption efficiency in the range of 70%, is described. During 1991, 1995 and 2001 brown seaweed samples were collected at several stations along the Swedish west coast. In addition to these locations, a well-defined site (Särdal; 56.76 °N, 12.63 °E) was included from which 99Tc data were collected from 1967 to 2000. The effect of discharges from the Sellafield EARP (Enhanced Actinide Removal Plant) from 1995-1996 was observed in brown seaweed from the Swedish west coast 4-5 years later, with a ten-fold increase in 99Tc activity concentration. An inverse correlation between 99Tc and 137Cs concentrations in seaweed was observed due to continuous mixing of high-Tc-low-Cs (Atlantic Sea) and low-Tc-high-Cs (Baltic Sea) waters. Radioactive materials from the Chernobyl accident contaminated various part of Sweden and by analysing lichen samples from different areas an estimate of the deposited 237Np density could be made. Through the determination of 240Pu/239Pu and 237Np/239Pu atomic ratios, source identification could be made in Swedish lichen samples. In the areas most contaminated by the Chernobyl accident in Sweden, the Chernobyl-derived 237Np contribution was up to 30% of the total concentration. However, the plutonium contributions from Chernobyl in the same samples were as high as 85%. Sellafield-derived 237Np was found in brown seaweed samples from the Swedish west coast, indicating greater mobility in the marine environment than that of Pu.