Plutonium uptake in biota at former nuclear sites

Plutonium (Pu) is of ongoing interest as worldwide inventories continue to increase and plans for permanent storage of Pu wastes have stalled in many countries leaving large amounts in temporary storage. Pu also remains as environmental contamination at various locations due to: accidents (e.g., Chernobyl, UKR; Thule, GRL); research and processing releases (e.g., Los Alamos, USA, Mayak, RUS); and former weapons testing (e.g., Nevada Test Site, USA; Semipalatinsk, KAZ; and Maralinga, AUS). We assessed the availability and uptake of Pu in a range of wildlife types at legacy sites with the focus on new data from outside of the remediation zone at the former Taranaki site, Maralinga, South Australia. Of key interest are the uptake and biokinetics of Pu in mammals, particularly from environmental exposure to the undetonated Pu-oxide forms at Taranaki that are representative of much of the worldwide inventory. Our results confirm that environmentally dispersed Pu can remain accessible for uptake by biota over decadal time scales. For example, after more than 50 years since deposition at Taranaki, 62% of Pu has remained in the 0-2 cm surface layer, and nearly 100% in the 0-10 cm of soil depths. Although a small fraction of the Pu is migrating downward at —0.2 cm per year, it appears that most Pu will continue to remain accessible into the future for plants and animals that inhabit the surface, or shallow soil layers. The uptake of Pu into terrestrial animals occurs mainly by inhalation and ingestion, and can be persistent over time as indicated by constant uptake rates for mammals, and a potential increase for reptiles, in data spanning 30 years. The rates of soil-to-animal transfer at Taranaki, align well with those from similar sites where undetonated Pu was tested (e.g., Nevada Test Site, US). However, the uptake values at these sites are lower than general world-wide values, likely due to the presence of less-absorbable forms of Pu. The importance of the physico-chemical form of the Pu on uptake was also seen in data from fish exposed to more absorbable forms of Pu in liquid discharge ponds near processing facilities in the US. These fish had two orders of magnitude higher uptake values than those for similar species receiving Pu solely from atmospheric fallout. The physico-chemical form of the Pu can also influence how it is distributed among mammalian organs. The relatively insoluble forms at Taranaki, which include particulates, led to elevated concentrations of unabsorbed Pu in the lung, gastrointestinal tract, and adhered to skin/fur of mammals. This elevated Pu can provide a secondary source during human, and ecological, food-chain consumption. Of the Pu that was absorbed within the body, much higher accumulation was measured in the skeleton, and much lower in the liver, in mammals at Taranaki as compared with the standard model of 50% skeleton, and 30% liver (ICRP 1986). Our data provides specific quantification of Pu uptake rates in wildlife and the subsequent accumulation in various mammalian organs. These will aid future assessments of the Maralinga site, as well as more general evaluations related to the low-solubility forms of Pu that make up a large share of the worldwide inventory