Plutonium in wildlife and soils at the Maralinga legacy site: persistence over decadal time scales.

The mobility of plutonium (Pu) in soils, and its uptake into a range of wildlife, were examined using recent and ∼25 year old data from the Taranaki area of the former Maralinga weapons test site, Australia. Since its initial deposition in the early 1960s, the dispersed Pu has been incorporated into the soil profile and food chain through natural processes, allowing for the study of Pu sequestration and dynamics in relatively undisturbed semi-arid conditions. The data indicate downward mobility of Pu in soil at rates of ∼0.2-0.3 cm per year for the most mobile fraction. As a result, while all of the Pu was initially deposited on the ground surface, approximately 93% and 62% remained in the top 0-2 cm depth after 25- and 50-years respectively. No large-scale lateral spreading of the Taranaki plume was observed. Pu activity concentrations in 0-1 cm soils with biotic crusts were not elevated when compared with nearby bare soils, although a small number of individual data suggest retention of Pu-containing particles may be occurring in some biotic crusts. Soil-to-animal transfer, as measured by concentration ratios (CRwo-soil), was 4.1E-04 (Geometric Mean (GM)) in mammals, which aligns well with those from similar species and conditions (such as the Nevada Test Site, US), but are lower than the GM of the international mammal data reported in the Wildlife Transfer Database (WTD). These lower values are likely due to the presence of a low-soluble, particulate form of the Pu in Maralinga soils. Arthropod concentration ratios (3.1E-03 GM), were similar to those from Rocky Flats, US, while values for reptiles (2.0E-02 GM) were higher than the WTD GM value which was dominated by data from Chernobyl. Comparison of uptake data spanning approximately 30 years indicates no decrease over time for mammals, and a potential increase for reptiles. The results confirm the persistence of bioavailable Pu after more than 50 years since deposition, and also the presence of larger-sized particles which currently affect CRwo-soil calculations, and which may serve as an ongoing source of bioavailable Pu as they are subjected to weathering into the future.

Plutonium isotopes in the lower reaches of the River Rhône over the period 1945-2000: fluxes towards the Mediterranean Sea and sedimentary inventories.

Plutonium isotopes in the Rhône River originate from both the weathering of the catchment basin contaminated by global atmospheric fallout, and the liquid effluents released from the Marcoule reprocessing plant since 1961. Due to a new treatment process applied to the liquid effluents, a decrease of two orders of magnitude in the industrial plutonium discharged into the River Rhône has been registered from 1991. Today, 238Pu industrial inputs to the River Rhône are still about 10 times higher than those derived from global fallout, while 239+240Pu inputs from industrial and global fallout sources are of similar importance, i.e. 1 GBq y(-1). Our results indicate that the river sedimentary compartment act either as a sink or a delayed-source term of plutonium for the freshwaters depending on the hydraulic regime and flood events. This compartment may then represent an important industrial delayed-source term for the River Rhône freshwaters in the coming years as the Marcoule reprocessing plant is being dismantled. These results were obtained from samples collected from the lower course of the River Rhône over the 1987-1998 period and analysed for 238Pu and 239+240Pu activities. Both river sedimentary inventories of plutonium isotopes and effective outputs from the River Rhône towards the Gulf of Lions have been estimated for each year over the 1945-2000 period. Regarding 239+240Pu, the sedimentary inventory accumulated since 1945 is estimated to be 172+/-35 GBq. If mobile, this amount represents a significant delayed-source term of plutonium on the scale of the Rhône watershed.