Certified reference material for radionuclides in fish flesh sample IAEA-414 (mixed fish from the Irish Sea and North Sea).

A certified reference material (CRM) for radionuclides in fish sample IAEA-414 (mixed fish from the Irish Sea and North Seas) is described and the results of the certification process are presented. Nine radionuclides (40K, 137Cs, 232Th, 234U, 235U, 238U, 238Pu, 239+240Pu and 241Am) were certified for this material. Information on massic activities with 95% confidence intervals is given for six other radionuclides (90Sr, 210Pb(210Po), 226Ra, 239Pu, 240Pu 241Pu). Less frequently reported radionuclides (99Tc, 129I, 228Th, 230Th and 237Np) and information on some activity and mass ratios are also included. The CRM can be used for quality assurance/quality control of the analysis of radionuclides in fish sample, for the development and validation of analytical methods and for training purposes. The material is available from IAEA, Vienna, in 100 g units.

A review of measurements of radionuclides in members of the public in the UK.

This paper summarises a comprehensive review of radio-analytical data from autopsy, whole or partial body monitoring and the assay of teeth, foetuses and urine for non-occupationally exposed members of the public in the UK between 1957 and 2003. Most attention has been given to measurements of artificial radionuclides formed in the nuclear fuel cycle, uranium and thorium. The review concentrates on measurements on people in the UK who live or have lived in the vicinity of nuclear power sites. When UK data are unavailable, or for the purposes of comparison, information has been included from studies in other countries. Highlights of key findings of the document are listed: The concentrations of strontium-90 in bone and teeth have reflected changes in the amounts present in the environment due to fallout from nuclear testing. There are higher concentration levels of 239+240Pu in samples from West Cumbria compared with the rest of the UK. However, the levels are so low that any increase in risk of induced skeletal tumours (including leukaemia) would be very small compared with those arising from the intake of natural radionuclides. As expected there have been only a few published autopsy studies. Both tissue sample mass and radionuclide concentrations were low, leading to relatively large measurement uncertainties. Whole body measurements of 137Cs in residents in Berkshire and Oxfordshire clearly show the effect of atmospheric testing of nuclear weapons and of the Chernobyl accident. A survey of whole body 137Cs and 134Cs content following the Chernobyl accident showed that residents of Central Scotland, North-West England and North Wales had twice the radiocaesium content of residents in the rest of England and Wales. Measurements of 131I in the thyroid have been reported following the accidents at Windscale and Chernobyl for most regions of the UK. Few excretion studies have been reported although this does not diminish their importance. One study on the urinary excretion rate of 90Sr in adults and children living in the Dounreay area suggested that the results did not support this radionuclide as being the cause of increased childhood leukaemia. Similar conclusions were drawn from another study involving the assay of 239Pu. It is suggested that a national database of measurements made on members of the public should be initiated. The database would provide a means for identifying future trends.

210Pb, 210Po, 226Ra, U and Th in arable crops and ovine liver: variations in concentrations in the United Kingdom and resultant doses.

Concentrations of a range of naturally occurring radionuclides have been determined in the same crops grown at two sites in the UK. Ovine liver has also been studied. One site was in an area where concentrations in soil are typical of the UK (the 'control' site) and the other in an area where levels were well above average (the 'test' site). For an average adult consumer of all of the foodstuffs studied, the doses from consumption for the test site were about 4 times higher than those for the control site. However, the differences were small compared with the variability in overall doses from natural background across the UK. 210Pb and 210Po were important contributors to doses for both sites, but at the test site the contribution from 226Ra was also significant. Of the foodstuffs studied, consumption of leafy vegetables and liver gave the highest doses. The doses from leafy vegetables were sensitive to the weather conditions prior to harvesting. Consequently, rigorous monitoring programmes should be based on several samples collected throughout the year; extrapolations based on a single annual sample are unlikely to be reliable.

Development of the NIST bone ash standard reference material for environmental radioactivity measurement.

The bone ash standard reference material (SRM), a blend of 4% contaminated human bone and 96% diluent bovine bone, has been developed for radiochemical method validation and quality control for radio-bone analysis. The massic activities of 90Sr, 226Ra, 230Th, 232Th, 234U, 235U, 238U, 238Pu, (239 + 240)Pu and (243 + 244)Cm were certified using a variety of radiochemical procedures and detection methods. Measurements confirmed undetectable radionuclide heterogeneity down to a sample size of 5 g. thereby implying adequate blending of particulate materials with dilution factors of up to 17,900. The results among most of the intercomparison laboratories and their methods were consistent. Disequilibrium was observed for decay chains: 234U(0.67 mBq/g)-230Th(0.47 mBq/g)-226Ra(15.1 mBq/g)-210Pb(23 mBq/g)-210Po(13 mBq/g) and 232Th(0.99 mBq/g)-228 Ra(6.1 mBq/g)-228Th(7.1 mBq/g). The disequilibria were the results of mixing occupationally contaminated human bone with natural bovine bone and the fractionation during internal biological processes. The massic activity of 210Pb, 228Th and 241Am were not certified because of insufficient 228Ra and 241Pu data and lack of knowledge in how 222Rn and its daughters will be fractionated in the SRM bottle over time.

The gastrointestinal absorption of neptunium, plutonium and americium in a primate (C. jacchus).

Mixtures of Np, Pu and Am were administered to primates (C. jacchus) by gastric intubation to measure their fractional gastrointestinal absorption (f1 values). The values obtained were about 2 x 10(-3) and 1 x 10(-3), respectively, for Np and Pu administered as the citrate, and 2 x 10(-3) and 6 x 10(-4), respectively, for Pu and Am in potato. The significance of these values in terms of absorption in humans is discussed.

Speciation of plutonium in potato and the gastrointestinal transfer of plutonium and americium from potato.

Complexation of Pu(IV) and Am(III) by naturally occurring agents such as citrate and phytate might enhance their uptake from the digestive tract. However, the extent to which they enhance the gastrointestinal uptake of actinides from foodstuffs is far from resolved, as this study shows. Investigations of the chemical forms of Pu(IV) and Am(III), by gel permeation chromatography, in simulated digests of potato tubers naturally radiolabelled with 239Pu(IV) and 241Am(III) have shown that neither citrate nor phytate appear to determine their chemical forms. Therefore, it is possible that these are not the complexing anions which determine the gastrointestinal transfer of these radioelements from potato meal. Isotachophoretic analyses of the juices pressed from tubers and solutions prepared by simulated digestion of potato tubers have demonstrated the presence of several low molecular weight anions. These anions might be complexing agents because they possess an isotachophoretic mobility similar to that of citrate; some of these anions remain unidentified. Whereas 239Pu and 241Am were used in the foregoing studies, 238Pu and 241Am were used to produce either in vitro or naturally radiolabelled potatoes for gastrointestinal transfer measurements using rats and hamsters. Gastrointestinal transfer values of 0.13 +/- 0.05% (mean +/- standard error of mean) and 0.16 +/- 0.06% were determined with rats for the uptake of 238Pu and 241Am, respectively, from naturally labelled potato meal. Higher gastrointestinal transfer values were obtained for hamsters: for 238Pu and 241Am the transfer values from naturally labelled meal were 0.25 +/- 0.08% and 0.33 +/- 0.07%, respectively. Similar values were observed for uptake from in vitro labelled potato meal. On the basis of the similarity of the values for the naturally labelled potato meal and for the 'spiked' potato meal it would appear that biological incorporation is not necessary for the binding of the actinides to the ligands which will determine gastrointestinal transfer.

Measurements of actinide gut-transfer factors in humans.

Measurements have been made of the gastrointestinal absorption in humans of 239Np and 242Cm administered together in citrate media. Using five volunteers, consistent results of (2.0 +/- 0.2) x 10(-4) and (1.7 +/- 0.3) x 10(-4) were obtained for Np and Cm respectively; the quoted uncertainties are the standard errors of the means. A progress report is given of work to measure the f1 value for Pu in humans. Early work suggests an f1 value of 2 x 10(-4).

Radioactivity in environmental samples taken in the Sellafield, Ravenglass and Morecambe Bay areas of west Cumbria.

Seaborne sediments deposited in the estuaries of the Esk, Duddon, Leven and Kent have been analysed for fission products and actinides discharged in waste from the Sellafield processing works in west Cumbria, and the values compared with the generally expected values due to fallout from atmospheric nuclear weapons tests. Analyses of tissues from sheep grazing the marshes of these estuaries show that the internal radiation dose of the general public through eating mutton or liver from these animals would be at most a few percent of recommended limits. Analytical data are presented on the actinide content of beef cattle, and on potato crops grown under field conditions; these data show that, as with the sheep data, the radiation dose to the consumer would be small.

Gastrointestinal absorption of neptunium and curium in humans.

The gastrointestinal absorption of Np and Cm has been determined in five male adult volunteers. The Np and Cm, which were in citrate solution, were taken with food. An initial experiment with each individual determined the fraction of each element excreted in the urine following intravenous administration. Subsequently, the results for urinary excretion for the two routes of administration were used to calculate the fractional absorption (f1) of ingested Np and Cm. The mean f1 values were: Np (2.0 +/- 0.2) X 10(-4), range (1.2-2.9) X 10(-4), and Cm (1.7 +/- 0.3) X 10(-4), range (0.95-3.0) X 10(-4), the quoted uncertainties being the standard error of the means. Currently, the International Commission on Radiological Protection recommends a value of 10(-3) for both elements. Cumulative urinary excretion over 1 wk after intravenous injection accounted for about 20%-40% of administered Np and 7%-10% of Cm. At the conclusion of the experiment, the total committed effective dose equivalent for each volunteer was calculated to be in the range 130-250 microSv, based on the individual f1 values, and, in some cases, a knowledge of the rate of clearance of 239Np through the gut as measured by whole-body counting.

The distribution of 137Cs, plutonium and Americium in sheep.

Radiochemical measurements on tissues taken from sheep from the Cumbrian and Lancashire coast have given data which allow the tissue distribution and body content of plutonium isotopes, americium-241 and caesium-137 to be calculated. The data are particularly useful as the concentrations in lung confirm that for these animals the main route of intake is from the diet and not from inhalation. Plutonium and americium concentrate in the liver and skeleton. Caesium-137 was, as expected, found mainly in the meat of the animals. Additionally a controlled feeding experiment has been conducted to determine the gastrointestinal absorption of plutonium and americium from contaminated vegetation. A value of 0.01% for plutonium and 0.005% for americium was determined.

Plutonium and Cs-137 in autopsy tissues in Great Britain.

Tissues removed at autopsy from members of the general public contain significantly higher concentrations of plutonium and 137Cs in west Cumbrians than in people from three other regions of Great Britain. Several autopsy cases from Cumbria showed unusually high values of plutonium. Subsequently it was found that the subjects had been former employees of British Nuclear Fuels.

The gastrointestinal absorption of 'biologically incorporated' plutonium-239 in the rat.

Growing potatoes have been labelled by foliar applications of plutonium citrate. Approximately 0.4% of the radioactivity was taken up by the tubers. The potatoes were fed to rats and the gastrointestinal uptake of plutonium was estimated to be 0.34%. The significance of these results in relation to the uptake by humans is discussed.

The uptake of plutonium-238, 239, 240, americium-241, strontium-90 and caesium-137 into potatoes.

Transfer factors have been measured for 239 Pu + 240 Pu, 241 Am, 90 Sr and 137 Cs into potatoes grown in a blend of soil which included silt polluted with radioactive waste discharged into the Irish Sea. The experiment has been carried out over four seasons and attempts to assess the radiological consequences to the consumer which would arise if potatoes were to be grown in land heavily contaminated with the silt. During the course of the experiment plutonium and americium became less available for uptake, 90 Sr became slightly more available and 137 Cs remained nearly constant in its availability. The values of the transfer factors are among the lowest reported for these radionuclides into potatoes.

Factors affecting the mobility of plutonium-238 dioxide in the rat.

A major factor influencing the movement of plutonium-238 from the lungs to blood after the intubation of oxide suspensions is the presense of 0.001 micrometer diameter particles. In a polydisperse suspension of particles this fraction increases with time, due it is thought, to fragmentation of larger particles induced by alpha decay. The rate of this process could account for the greater transportability in vivo of plutonium-238 relative to plutonium-239 when the oxides are inhaled. In blood, 0.001 micrometer diameter plutonium-238 oxide particles undergo a rapid reaction to form a low molecular weight species before plutonium is complexed with transferrin and citrate ions. The filtration of this species through the kidneys may explain the observed enhanced urinary excretion of plutonium relative to administered plutonium citrate. The mechanism of urinary excretion and relationship between cumulative urinary excretion and body content for plutonium-238 is similar to that previously observed for plutonium-239, even though different methods of preparation of the oxides were used.