Characterization of the NIST seaweed Standard Reference Material.

The National Institute of Standards and Technology (NIST) Standard Reference Material (SRM) for seaweed was developed through an interlaboratory comparison with 24 participants from 16 countries. After evaluating different techniques to calculate certified values for the radionuclides, the median method was found to be the most representative technique. The certified values were provided for 13 radionuclides and information values were given for 15 more radionuclides. Results for the natural decay series showed disequilibrium in both the uranium and thorium series.

Characterization of uranium and plutonium containing particles originating from the nuclear weapons accident in Thule, Greenland, 1968.

To improve long-term radioecological impact assessment for the contaminated ecosystem of Bylot Sound, Greenland, U and Pu containing particles have been characterized with respect to particle size, elemental distribution, morphology and oxidation states. Based on scanning electron microscopy with XRMA, particles ranging from about 20 to 40 microm were isolated. XRMA and mu-XRF mapping demonstrated that U and Pu were homogeneously distributed throughout the particles, indicating that U and Pu have been fused. Furthermore, mu-XANES showed that U and Pu in the particles were present as mixed oxides. U was found to be in oxidation state IV whereas Pu apparently is a mixture of Pu(III) and Pu(IV). As previous assessments are based on PuO2 only, revisions should be made, taking Pu(III) into account.

Distribution and flux of 238Pu, 239,240Pu, 241Am, 137Cs and 210Pb to high arctic lakes in the Thule district (Greenland).

Environmental samples (soil, sediment and lake water) in the Thule area (NW Greenland) have been studied to assess the contamination of radionuclides originating from a nuclear weapons accident (the Thule accident in 1968). Four lakes were chosen at different distances from the point of impact with the Thule air base community situated in between. The sedimentation rates in the lakes varied from 0.4 mm a(-1) (5 mg cm(-2) a(-1)) to 1.6 mm a(-1) (82 mg cm(-2) a(-1)). With these sedimentation rates, it is not possible to resolve the (239,240)Pu global fallout peak from a possible (239,240)Pu "accident" peak in the sediment depth profiles. However, the (239,240)Pu/(137)Cs and the (238)Pu/(239,240)Pu ratios agreed well with global fallout ratios, indicating that plutonium originating from the accident had not reached these lakes. This also indicates that the Thule air base community has probably only been exposed to radionuclides from the accident to a very limited extent. A limited study showed that (210)Pb could not be used as a normalizing nuclide to explain the transport of transuranic elements from the catchment area to the lake, i.e. (210)Pb has a different transport mechanism from that of the transuranic elements studied in this investigation.

Iodine-129 and caesium-137 in Chernobyl contaminated soil and their chemical fractionation.

Soil samples from areas in Belarus, Russia and Sweden contaminated by the Chernobyl accident were analysed for (129)I by radiochemical neutron activation analysis, as well as for 137Cs by gamma-spectrometry. The atomic ratio of (129)I/137Cs in the upper layer of the examined soil cores ranged from 0.10 to 0.30, with an average of 0.18, and no correlation between (129)I/137Cs ratio and the distance from Chernobyl reactor to sampling location was observed. It seems feasible to use the (129)I/137Cs ratio to reconstruct the deposition pattern of 131I in these areas. The association of (129)I and 137Cs in the Chernobyl soil and Irish Sea sediment was investigated by a sequential extraction method. Similar speciation of (129)I in the Chernobyl soil and Irish Sea sediment was found. Approximately 70% of (129)I is bound to oxides and organic matter, and 10-20% is in the readily available phase, while most of the 137Cs (73%) in Chernobyl soil remains in the extraction residue.

Iodine-129 in thyroid and urine in Ukraine and Denmark.

Human thyroids collected from Gomel in Belarus, sheep thyroid from Jutland and human urine from Zealand in Denmark were analysed for 129I and 127I concentrations. The ratios of 129I/127I in human thyroid in Gomel are 2.65-11.0 x 10(-9) with an average of 7.21 x 10(-9), which is one order of magnitude higher than those from Asia and South America (10(-10)), but significantly lower than those observed in west Europe (10(-8)). A weak negative correlation (P < 0.05) between 129I/127I ratio in human thyroid and the age of the subjects was observed in Gomel. The average ratio of 129I/127I in sheep thyroids from Jutland of Denmark is 1.81 x 10(-7), which is two orders of magnitude higher than those in south hemisphere, and Asia. It is also significantly higher than those observed in other west European countries before 1984 and that in human thyroid in Gomel. The high thyroid 129I level in Jutland is attributed to the release of reprocessing plants in France and UK. The 129I/127I ratios in human urine in Zealand of Denmark are 0.86-2.86 x 10(-8). The possibility of using urine 129I to evaluate the thyroid exposure to 129I is investigated.

Level and origin of iodine-129 in the Baltic Sea.

Environmental samples, such as seawater, seaweed, lake water, lake sediment and grass collected from the Baltic Sea area were analyzed for 129I and 127I by radiochemical neutron activation analysis. In 2000, the concentration of 129I in the seawater from Borholm and Møen in the Baltic Sea has reached 6.0 x 10(-13) and 16 x 10(-13) g/l, respectively, these are more than two orders of magnitude higher than the global fallout level. The highest value of 270 x 10(-13) g/l being found in the seawater from the Kattegat. By comparison of the level of 129I in the lake water and precipitation in this region, it is estimated that more than 95% of 129I in the Baltic Sea originates from reprocessing emissions, especially from the French nuclear fuel reprocessing plant at La Hague. More than 30% of 129I in the south Baltic and 93% in the Kattegat directly originates from the marine discharges of the European reprocessing plants.

Process-diagnostic patterns of chlorobiphenyl congeners in two radiochronologically characterized sediment cores from the northern Baffin Bay.

Polychlorinated biphenyl (PCB) patterns were interpreted in two radioisotopically constrained sediment cores from the Arctic ocean in order to seek clues about their large-scale environmental fates. Low but clearly measurable fluxes of individual PCB congeners were observed in deeper layer sediments, corresponding to the past 170 years, in a single dated core from the Baffin Bay shelf. Fluxes of the dominant individual congeners in the surface sediments were 20-100 pg m(-2) d(-1). Combining these data with the sediment data from the Arctic Monitoring and Assessment Program, it appears that the PCB distribution in Arctic surface sediments is governed by the organic carbon (OC) content of the sediments. The historical development of the PCB congener fingerprint suggests that the modern sediments are enriched in medium-chlorinated congeners, implying that there are at least two significant, but distinctly different, sink processes acting on the PCB pool. The relative abundance of light-to-heavy congeners, in mid-shelf marine sediments of similar ages, between 40 degrees N and 76 degrees N latitude suggests a northward dilution of PCBs which is stronger attenuated for heavier congeners, consistent with a temperature-driven global fractionation process. The significant presence of PCB in historical archives pre-dating the organochlorine society, as observed in this and several previous studies, awaits a fuller explanation.

Iodine-129 in human thyroids and seaweed in China.

The concentrations of 129I and the ratios of 129I/127I in normal human thyroids collected in Tianjin, China, and some seaweed samples from the Chinese coast were determined by neutron activation analysis. The mean 129I/127I ratio in these thyroids was found to be 1.13 x 10(-9), which is two orders of magnitude higher than the level of the pre-nuclear era, but one order of magnitude lower than the level in Europe in the post-nuclear era. There is no significant difference between the ratio of 129I/127I in the thyroids for the post-nuclear era from China and other areas, which are considered not to have been directly exposed to 129I emission from a nuclear source, such as Chile, Taiwan and Tokyo. The mean 129I/127I ratio in seaweed from the Chinese coast is 2.35 x 10(-10), approximately two orders of magnitude higher than in seaweed collected in the pre-nuclear age, and similar to that from locations without direct exposure to the emission from nuclear installations, influenced only by global fallout. This indicates that the 129I level in China is within the global fallout background level.

Oxidation-state distribution of plutonium in surface and subsurface waters at Thule, northwest Greenland.

The speciation of plutonium in Arctic waters sampled on the northwest Greenland shelf in August 1997 is discussed in this paper. Specifically, we report the results of analyses carried out on seawater sampled (a) close to the Thule air base where, in 1968, a US military aircraft carrying four nuclear weapons crashed on sea ice, releasing kilogram quantities of plutonium to the snow pack and underlying seabed sediments, and (b) at a reference station (Upernavik) located approximately 400 km to the south. The data show that most of the plutonium in the dissolved phase at Thule is in the form of Pu(V, VI) (mean: 68+/-6%; n = 6), with little if any distinction apparent between surface and bottom waters. Further, the oxidation state distribution at stations close to the accident site is similar to that measured at Upernavik, remote from this site. It is also similar to the distribution observed in shelf waters at mid-latitudes, suggesting that the underlying processes controlling plutonium speciation are insensitive to temperature over the range 0-25 degrees C. Measurements using tangential-flow ultrafiltration indicate that virtually all of the plutonium (including the fraction in a reduced chemical form) is present as fully dissolved species. Most of this plutonium would seem to be of weapons fallout origin, as the mean 238Pu/239,240Pu activity ratio in the water column (dissolved phase) at Thule (0.06+/-0.02; n = 10) is similar to the global fallout ratio at this latitude (approximately 0.04). Thus, there is little evidence of weapons-grade plutonium in the water column at Thule at the present time.

Environmental radioactive contamination in Greenland: a 35 years retrospect.

Environmental studies of anthropogenic radionuclides in Greenland over four decades are reported. The studies have comprised the marine as well as the terrestrial environments and emphasis has been laid on measurements of 90Sr and 137Cs. The temporal and the spatial trends of these radionuclides are described. The radiation exposure from consumption of locally produced diets has been calculated from consumption rates and the infinite time integrated levels of 90Sr and 137Cs concentrations in the various food products. Compared with most other Arctic people, the Greenlanders have received relatively low doses from anthropogenic radionuclides. There are several reasons for this, first of all, because of the relatively high consumption of marine products compared with terrestrial products. Secondly, because winter slaughtering of reindeer is less frequent in Greenland than in other Arctic countries and Greenland reindeer consume, in general, less lichen than most other Arctic reinder, and thirdly, because the transfer from deposition to lichen in Greenland seems lower than in other Arctic areas.

Marine radioactivity in the Arctic: a retrospect of environmental studies in Greenland waters with emphasis on transport of 90Sr and 137Cs with the East Greenland Current.

The waters around Greenland have received radioactive contamination from three major sources: Global fallout, discharges from the nuclear fuel reprocessing plant Sellafield in the UK, and the Chernobyl accident in the Former Soviet Union (FSU). The global fallout peaked in the early 1960s. The radiologically most important radionuclides from this source are 90Sr and 137Cs. The input of global fallout to arctic waters was direct deposition from the atmosphere and indirect delivery through river run off and advection from the Atlantic Ocean via the north-east Atlantic current system. The waterborne discharges from Sellafield which were at their peak between 1974 and 1981 contributed primarily 137Cs, although some 90Sr was also discharged. The Chernobyl accident in 1986 was characterised by its substantial atmospheric release of radiocaesium (134Cs and 137Cs). Other sources may, however, also have contributed to the radioactivity in the Greenland waters. Examples include La Hague, France, and radioactive discharges to the great Siberian rivers (Ob, Yenisey and Lena) from nuclear activities in the Former Soviet Union or the local fallout from the Novaya Zemlya nuclear weapons test site. Dumping of nuclear waste in the Kara and Barents Seas may be another, although minor source. From measurements in Greenland waters carried out since 1962 the transport of radionuclides with the East Greenland Current is calculated and compared with the estimated inputs of 90Sr and 137Cs to the Arctic Ocean. This study focus on 90Sr and 137Cs because the longest time series are available for these two radionuclides.

Marine radioactivity assessment of Mururoa and Fangataufa atolls.

The International Atomic Energy Agency (IAEA) carried out an international project. 'The Study of the Radiological Situation at the Atolls of Mururoa and Fangataufa' with the aim of assessing the present and future radiological situation at the atolls and making recommendations for either monitoring or remedial actions if they are deemed necessary. The paper concentrates on marine radioactivity aspects and gives an estimation of present radionuclide concentrations in water, sediment and biota of the Mururoa and Fangataufa lagoons and the surrounding ocean. The dominant radionuclide in both lagoons is Pu in sediments (the total inventory is approximately 30 TBq). A decline in radionuclide concentrations has been observed in recent years in lagoon water, with the exception of 3H and 90Sr, for which a contribution from underground sources is to be expected. Radionuclide concentrations in biota from the lagoons and the surrounding ocean are low and consistent with previous measurements. The observed radionuclide concentrations in both lagoons imply that no radiological risk exists for hypothetical inhabitants of Mururoa and Fangataufa Atolls.

Perturbation in the 240Pu/239Pu global fallout ratio in local sediments following the nuclear accidents at Thule (Greenland) and Palomares (Spain).

It is well established that the main source of the plutonium found in marine sediments throughout the Northern Hemisphere is global stratospheric fallout, characterized by a typical 240Pu/239Pu atom ratio of approximately 0.18. Measurement of perturbations in this ratio at various sites which had been subjected to close-in fallout, mainly from surface-based testing (e.g. Bikini Atoll, Nevada test site, Mururoa Atoll), has confirmed the feasibility of using this ratio to distinguish plutonium from different fallout sources. In the present study, the 240Pu/239Pu ratio has been examined in samples of sediment (and soil) collected at Thule (Greenland) and Palomares (Spain), where accidents involving the release and dispersion of plutonium from fractured nuclear weapons occurred in 1968 and 1966, respectively. The 240Pu/239Pu ratio was measured by high-resolution alpha spectrometry and spectral deconvolution, and confirmed in the case of the most active samples by high-resolution X-ray spectrometry. Only samples which displayed plutonium heterogeneities, i.e. hot particles or concentrations well in excess (at least two orders of magnitude) of those expected from global fallout, were selected for analysis. The analytical results showed that at Thule the mean 240Pu/239Pu atom ratio was 0.033 +/- 0.004 (n = 4), while at Palomares the equivalent ratio appeared to be significantly higher at 0.056 +/- 0.003 (n = 4). Both ratios are indicative of low burn-up plutonium and are consistent with those reported for weapons-grade plutonium. It is noteworthy that the mean 238Pu/239Pu activity ratio in the Thule samples, at 0.0150 +/- 0.0017 (n = 4), was also lower than that measured in the Palomares samples, namely, 0.0275 +/- 0.0012 (n = 4). The 241Pu/239Pu ratios were similarly different. Finally, the data show, in contrast to Palomares, that not all of the samples from the Thule accident site were contaminated with plutonium of identical isotopic composition.

Further studies of plutonium and americium at Thule, Greenland.

Eleven years after the accidental loss of nuclear weapons in 1968, the fourth scientific expedition to Thule occurred. The estimated inventory of 1 TBq 239,240Pu in the marine sediments was unchanged when compared with the estimate based on the 1974 data. Plutonium from the accident had moved further away from the impact point and at some locations the vertical distribution indicated a downward displacement of Pu in the sediment column since 1974. Seawater and seaplants showed no evidence of the presence of Pu from sources other than fallout; but Pu in benthos varied nearly proportionally with the levels in sediments. From the measurements of 239,240Pu in the Macoma community since 1970, the transfer factor to this community was estimated at 0.01 Bq a per Bq released to the sediments. The inventory of 241Am was 0.1 TBq. The vertical distribution of Am in sediments did not differ from that of Pu, but in benthos 241Am/239,240Pu were two times higher than in sediments. Seaplants showed the same value of Am/Pu as seawater. There was no indication of any biomagnification of Pu or Am through the marine food chains at Thule.