Accumulation of plutonium in mammalian wildlife tissues following dispersal by accidental-release tests.

We examined the distribution of plutonium (Pu) in the tissues of mammalian wildlife inhabiting the relatively undisturbed, semi-arid former Taranaki weapons test site, Maralinga, Australia. The accumulation of absorbed Pu was highest in the skeleton (83% ± 6%), followed by muscle (10% ± 9%), liver (6% ± 6%), kidneys (0.6% ± 0.4%), and blood (0.2%). Pu activity concentrations in lung tissues were elevated relative to the body average. Foetal transfer was higher in the wildlife data than in previous laboratory studies. The amount of Pu in the gastrointestinal tract was highly elevated relative to that absorbed within the body, potentially increasing transfer of Pu to wildlife and human consumers that may ingest gastrointestinal tract organs. The Pu distribution in the Maralinga mammalian wildlife generally aligns with previous studies related to environmental exposure (e.g. Pu in humans from worldwide fallout), but contrasts with the partitioning models that have traditionally been used for human worker-protection purposes (approximately equal deposition in bone and liver) which appear to under-predict the skeletal accumulation in environmental exposure conditions.

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.

Assessing doses to terrestrial wildlife at a radioactive waste disposal site: inter-comparison of modelling approaches.

Radiological doses to terrestrial wildlife were examined in this model inter-comparison study that emphasised factors causing variability in dose estimation. The study participants used varying modelling approaches and information sources to estimate dose rates and tissue concentrations for a range of biota types exposed to soil contamination at a shallow radionuclide waste burial site in Australia. Results indicated that the dominant factor causing variation in dose rate estimates (up to three orders of magnitude on mean total dose rates) was the soil-to-organism transfer of radionuclides that included variation in transfer parameter values as well as transfer calculation methods. Additional variation was associated with other modelling factors including: how participants conceptualised and modelled the exposure configurations (two orders of magnitude); which progeny to include with the parent radionuclide (typically less than one order of magnitude); and dose calculation parameters, including radiation weighting factors and dose conversion coefficients (typically less than one order of magnitude). Probabilistic approaches to model parameterisation were used to encompass and describe variable model parameters and outcomes. The study confirms the need for continued evaluation of the underlying mechanisms governing soil-to-organism transfer of radionuclides to improve estimation of dose rates to terrestrial wildlife. The exposure pathways and configurations available in most current codes are limited when considering instances where organisms access subsurface contamination through rooting, burrowing, or using different localised waste areas as part of their habitual routines.

Biotic, temporal and spatial variability of tritium concentrations in transpirate samples collected in the vicinity of a near-surface low-level nuclear waste disposal site and nearby research reactor.

The results of a 21 month sampling program measuring tritium in tree transpirate with respect to local sources are reported. The aim was to assess the potential of tree transpirate to indicate the presence of sub-surface seepage plumes. Transpirate gathered from trees near low-level nuclear waste disposal trenches contained activity concentrations of (3)H that were significantly higher (up to ∼700 Bq L(-1)) than local background levels (0-10 Bq L(-1)). The effects of the waste source declined rapidly with distance to be at background levels within 10s of metres. A research reactor 1.6 km south of the site contributed significant (p < 0.01) local fallout (3)H but its influence did not reach as far as the disposal trenches. The elevated (3)H levels in transpirate were, however, substantially lower than groundwater concentrations measured across the site (ranging from 0 to 91% with a median of 2%). Temporal patterns of tree transpirate (3)H, together with local meteorological observations, indicate that soil water within the active root zones comprised a mixture of seepage and rainfall infiltration. The degree of mixing was variable given that the soil water activity concentrations were heterogeneous at a scale equivalent to the effective rooting volume of the trees. In addition, water taken up by roots was not well mixed within the trees. Based on correlation modelling, net rainfall less evaporation (a surrogate for infiltration) over a period of from 2 to 3 weeks prior to sampling seems to be the optimum predictor of transpirate (3)H variability for any sampled tree at this site. The results demonstrate successful use of (3)H in transpirate from trees to indicate the presence and general extent of sub-surface contamination at a low-level nuclear waste site.

Radionuclide concentration ratios in Australian terrestrial wildlife and livestock: data compilation and analysis.

Radionuclide concentrations in Australian terrestrial fauna, including indigenous kangaroos and lizards, as well as introduced sheep and water buffalo, are of interest when considering doses to human receptors and doses to the biota itself. Here, concentration ratio (CR) values for a variety of endemic and introduced Australian animals with a focus on wildlife and livestock inhabiting open rangeland are derived and reported. The CR values are based on U- and Th-series concentration data obtained from previous studies at mining sites and (241)Am and (239/240)Pu data from a former weapons testing site. Soil-to-muscle CR values of key natural-series radionuclides for grazing Australian kangaroo and sheep are one to two orders of magnitude higher than those of grazing cattle in North and South America, and for (210)Po, (230)Th, and (238)U are one to two orders of magnitude higher than the ERICA tool reference values. When comparing paired kangaroo and sheep CR values, results are linearly correlated (r = 0.81) for all tissue types. However, kidney and liver CR values for kangaroo are typically higher than those of sheep, particularly for (210)Pb, and (210)Po, with values in kangaroo liver more than an order of magnitude higher than those in sheep liver. Concentration ratios for organs are typically higher than those for muscle including those for (241)Am and (239/240)Pu in cooked kangaroo and rabbit samples. This study provides CR values for Australian terrestrial wildlife and livestock and suggests higher accumulation rates for select radionuclides in semi-arid Australian conditions compared with those associated with temperate conditions.

Seasonal changes of redox potential and microbial activity in two agricultural soils of tropical Australia: some implications for soil-to-plant transfer of radionuclides.

Very little is known of the factors controlling soil-to-plant transfer of radionuclides in tropical environments. As part of an IAEA/FAO coordinated research project (CRP) designed to elucidate some of those factors, near-surface samples of two agricultural red-earth soils (Blain and Tippera) were collected from a study site in the Northern Territory. The climate is tropical monsoonal with crops being grown over the wet season from December to March/April. It is important to understand soil variables that may be related to this dramatic seasonality. In this investigation, soil redox state and microbial populations were assessed before and after the growing season with a view to generating hypotheses for future evaluation. The X-ray absorption near edge structure (XANES) technique was used to determine overall changes in the solid-state redox speciation of Fe and Mn in soils across the growing period. Fe speciation did not change but approximately 10% of the total Mn was oxidised from Mn(II) to Mn(III) and Mn(IV) in both soils between October 1999 and April 2000. An apparent disconnect between Fe and Mn was not unexpected given the >10 times higher concentration of Fe in the soils compared with Mn. These results have implications for the bioavailability of redox sensitive radionuclides such as Tc and Pu. Similarly, microbial population estimates were derived before and after the growing period. Total bacterial populations did not vary from 10(6) to 10(7) colonies per gram. Fungal populations increased over the growing season from 3-6 x 10(5) to 1-4 x 10(6) colonies per gram of soil. Fungi have the potential to decrease soil pH and hence increase the bioavailability of radionuclides such as Cs. In addition, fungi act to facilitate plant nutrition. This could lead to enhanced accumulation of nutrient analogues (e.g. Sr and Ra for Ca; Tc for Mn), but this effect may be masked by improved biomass production.

Soil-water distribution coefficients and plant transfer factors for (134)Cs, (85)Sr and (65)Zn under field conditions in tropical Australia.

Measurements of soil-to-plant transfer of (134)Cs, (85)Sr and (65)Zn from two tropical red earth soils ('Blain' and 'Tippera') to sorghum and mung crops have been undertaken in the north of Australia. The aim of the study was to identify factors that control bioaccumulation of these radionuclides in tropical regions, for which few previous data are available. Batch sorption experiments were conducted to determine the distribution coefficient (K(d)) of the selected radionuclides at pH values similar to natural pH values, which ranged from about 5.5 to 6.7. In addition, K(d) values were obtained at one pH unit above and below the soil-water equilibrium pH values to determine the effect of pH. The adsorption of Cs showed no pH dependence, but the K(d) values for the Tippera soils (2300-4100 ml/g) exceeded those for the Blain soils (800-1200 ml/g) at equilibrium pH. This was related to the greater clay content of the Tippera soil. Both Sr and Zn were more strongly adsorbed at higher pH values, but the K(d) values showed less dependence on the soil type. Strontium K(d)s were 30-60 ml/g whilst Zn ranged from 160 to 1630 ml/g for the two soils at equilibrium pH. With the possible exception of Sr, there was no evidence for downward movement of radionuclides through the soils during the course of the growing season. There was some evidence of surface movement of labelled soil particles. Soil-to-plant transfer factors varied slightly between the soils. The average results for sorghum were 0.1-0.3 g/g for Cs, 0.4-0.8 g/g for Sr and 18-26 g/g for Zn (dry weight) with the initial values relating to Blain and the following values to Tippera. Similar values were observed for the mung bean samples. The transfer factors for Cs and Sr were not substantially different from the typical values observed in temperate studies. However, Zn transfer factors for plants grown on both these tropical soils were greater than for soils in temperate climates (by more than an order of magnitude). This may be related to trace nutrient deficiency and/or the growth of fungal populations in these soils. The results indicate that transfer factors depend on climatic region together with soil type and chemistry and underline the value of specific bioaccumulation data for radionuclides in tropical soils.

Generic values for soil-to-plant transfer factors of radiocesium.

There is a need for soil-to-plant transfer factors of radionuclides that take into account all possible crops on all soil varieties to support dose assessment studies. Because only limited experimental data exist for worldwide soil systems, such values should necessarily have a generic character. This paper describes a generic system for 137Cs, mainly based on a reference soil-to-plant transfer factor which depends solely on soil properties such as nutrient status, exchangeable K-content, pH and moisture content. Crops are divided into crop groups, cereals serving as reference group. The transfer of other crop groups can be calculated by multiplying data for cereals by a conversion factor. Existing data present in the IUR (International Union of Radioecologists) databank and in large part the work of a FAO (Food and Agriculture Organisation)/IAEA(International Atomic Energy Agency)/IUR project on tropical systems provided the basis for the derivation of the conversion factors and reference values.

Recovery of fish communities in the Finniss River, northern Australia, following remediation of the Rum Jungle uranium/copper mine site.

The Finniss River in the wet-dry tropics of northern Australia has received acid rock drainage (ARD) contaminants from the Rum Jungle uranium/copper mine site over more than four decades. Annual-cycle loads of Cu, Zn, Mn, and sulfate, calculated from daily water and flow measurements, have been determined both prior to and following mine-site remediation, that began in the early 1980s. The effects of varying contaminant loads on the relative abundances of seven fish species, sampled by enmeshing nets during dry seasons, were determined by nonmetric multidimensional scaling (nMDS), in combination with cluster-analysis and other nonparametric statistical techniques. These analyses showed that (i) prior to remediation, the impacted region of the Finniss River in 1974 had significantly dissimilar (P < 0.001) and more heterogeneous fish communities, generally characterized by reduced diversity and abundance, compared to sites unexposed to elevated contaminant water concentrations and (ii) postremediation, recovery in fish communities from the impacted region was indicated because they were not significantly dissimilar from those sampled at contemporary (P = 0.16) unimpacted sites, that were also similar to preremedial unimpacted sites. Even though considerable contaminant loads are still being delivered to the impacted region of the Finniss River over the annual cycle, the recovery in fish diversity and abundances is consistent with (a) reductions of in situ contaminant water concentrations at the time of fish sampling, (b) reductions in annual-cycle contaminant loads of sulfate, Cu, Zn, and Mn by factors of 3-7, (c) greatly reduced frequencies of occurrence and magnitude of elevated contaminant water concentrations over the annual cycle, that was most pronounced for Cu, and (d) the absence of extensive fish-kills during the first-flushes of contaminants into the Finniss river proper at the beginning of the wet season, that were observed prior to remediation. As such, the results indicate that there has been ecological benefit to the Finniss River attributable to remedial works undertaken at the Rum Jungle mine site. Recovery in abundances of these fishes may also be due to their time-dependent evolution of tolerance to mine-waste contaminants over their long period of exposure.

Element concentrations in the flesh and osteoderms of estuarine crocodiles (Crocodylus porosus) from the Alligator Rivers Region, Northern Australia: biotic and geographic effects.

The concentrations of Na, K, Ca, Mg, Ba, Sr, Fe, Al, Mn, Zn, Pb, Cu, Ni, Cr, Co, Se, U, and Ti were determined in the flesh and osteoderms of estuarine crocodiles (Crocodylus porosus) captured in three adjacent catchments of Kakadu National Park, within the Alligator Rivers Region of northern Australia. This study provides, for the first-time, baseline concentrations of elements in both flesh and osteoderms of wild crocodiles. Multiple linear regression analyses were used to determine the effects of total crocodile length, estimated age, gender, inferred reproductive status, physical condition, and catchment of capture on element concentrations in both tissues. The Mg concentration (log10) in the flesh and osteoderms of C. porosus significantly (p < or = 0.001) decreased with increasing length (1.7-5.0 m) and estimated age (5-40 years). Similarly, the Ti concentration (log10) in flesh significantly (p < or = 0.01) decreased with increasing length. In contrast, Zn and Se concentration (log10) in flesh significantly (p < or = 0.001) increased with increasing length and/or age, suggesting that these relationships are mediated by biological rather than environmental chemical factors. In flesh, Fe and Na concentrations (log10) significantly (p < or = 0.05) increased as the physical condition of C. porosus deteriorated. No significant (p > 0.05) effects of gender or inferred reproductive status on element concentrations in the flesh and osteoderms were found. The mean concentrations (log10) of Al, Ba, Cr, Ni, and Pb in flesh and Co, Fe, Mg, Mn, and U in the osteoderms were significantly (p < or = 0.01) different between catchments. The significant (p < or = 0.05) effects of catchment on the concentrations of various elements indicate that C. porosus reflects the chemistry of its environmental milieu and therefore has a certain degree of catchment fidelity, even though the catchments are adjacent to one another. Such catchment-specific signals may be useful in the determination of the provenance of itinerant crocodiles. They also point to the utility of crocodiles as long-term biomonitors of their environment.

An intercomparison of gamma-spectrometry on two samples of biological origin by eight laboratories in four countries.

This report gives details of the first inter-laboratory comparison of gamma-spectrometry to be run within SPERA, the South Pacific Environmental Radioactivity Association since its inauguration in 1991. Laboratories in Australia, Chile, French Polynesia and New Zealand participated in the exercise. Two 'unknown' samples of biological origin were analysed. The first was a sample of milk powder derived from IAEA reference material. This sample provided an assessment of overall accuracy of 134Cs, 137Cs and 40K determinations. The second sample consisted of dried fish flesh including natural 40K and spiked with a mixed nuclide solution containing 210Pb, 109Cd, 54Mn, 60Co and trace 133Ba. Together the samples gave information on analytical precision over a range of energies and activities. When the results were compared with the recommended values and confidence intervals of the IAEA reference material, the overall accuracy of the gamma-spectrometry analytical procedures was found to be good. The average mean values for combined laboratory data fell within the recommended value ranges for each isotope. Ninety percent of the individual laboratory isotope mean values were within two standard errors of the 95% confidence interval of the standard, 75% were within 1 s.e., and 33% of the analyses fell within the confidence interval. Technical precision was also adequate with the overall errors being of the same magnitude as that of the reference material values for each isotope with relative standard deviations of 5-10%. There was a tendency for standard deviations of the combined results to be larger than those reported or derived from individual laboratory results by a factor between 1.2-5.6. This result suggested an under-estimate of systematic errors within individual laboratories. The largest sources of error were derived from reporting and calculation of results which gave a 16% gross error rate.