Sources and vertical distribution of 137Cs, 238Pu, 239+240Pu and 241Am in peat profiles from southwest Spitsbergen

This paper presents a detailed survey of the activities of selected man-made radionuclides in peat deposits located in SW Spitsbergen. Peat cores from the High Arctic (SW Spitsbergen) were analyzed by gamma spectrometry (¹³⁷Cs), alpha spectrometry (²³⁸Pu, ^239,240Pu, ²⁴¹Am activities) and by ICPMS (²⁴⁰Pu/²³⁹Pu atom ratios). Maximum activities evident in the peats correspond to the 1963/1964 global maximum fallout from atmospheric testing of nuclear weapons; some of the activity profiles have been altered post-deposition by water infiltration. Activity ratios of ²³⁸Pu/^239+240Pu, ²⁴¹Am/^239+240Pu, ^239+240Pu/¹³⁷Cs and ²⁴⁰Pu/²³⁹Pu atom ratios indicate mixing between global (stratospheric) and regional (tropospheric) sources of these radionuclides in the Svalbard area. The ²³⁸Pu/^239+240Pu activity ratios varied from 0.02 ± 0.01 to 0.09 ± 0.03, suggesting global fallout as the dominant source of Pu. The ^239+240Pu/¹³⁷Cs activity ratios varied from 0.01 ± 0.01 to 0.42 ± 0.11, which apparently arises from the post-depositional mobility of ¹³⁷Cs. The ²⁴¹Am/^239+240Pu activity ratios ranged between 0.10 ± 0.02 and 1.5 ± 0.3 and exceed the published global fallout ratio for Svalbard of 0.37 due to the relatively higher geochemical mobility of Pu vs. Am and/or ingrowth of Am from the decay of ²⁴¹Pu. The atom ratio ²⁴⁰Pu/²³⁹Pu ranged from 0.142 ± 0.006 to 0.241 ± 0.027; however, the vast majority of peat samples exhibited ²⁴⁰Pu/²³⁹Pu atom ratios similar to the stratospheric fallout (∼0.18).     

Delivery of transuranic elements by rain to the Mediterranean Sea

The concentrations of ²³⁸Pu, ^{239 + 240}Pu, ²⁴¹Am and ¹³⁷Cs were determined in rain samples collected at Monaco in the course of 1978–1979. Based on these data, the annual deliveries of these radionuclides to the Mediterranean by rain are computed to be 0.18 ± 0.01 pCim^?2 for ²³⁸Pu, 8.1 ± 0.1 pCim^?2 for ^{239 + 240}Pu, 0.58 ± 0.02 pCim^?2 for ²⁴¹Am and 351 ± 4 pCim^?2 for ¹³⁷Cs.Comparing the delivery data with the mixed layer inventories of ^{239 + 240}Pu and ²⁴¹Am in the Mediterranean, the upper limits of the mean residence time of these radionuclides in the mixed layer were estimated to be 12.3 yr for ^{239 + 240}pu and 2.9 yr for ²⁴¹Am. These values are consistent with the conclusion deduced from the vertical distribution pattern of these transuranic elements in the Mediterranean.Based on delivery values, the annual activity ratios for ${}^{238}\text{pu}{}^{\mathrm{239\; +\; 240}}\text{Pu}$, ${}^{241}\text{Am}{}^{\mathrm{239\; +\; 240}}\text{Pu}$ and ${}^{\mathrm{239\; +\; 240}}\text{pu}{}^{137}\text{Cs}$ are found to be 0,022, 0.072 and 0.023 respectively. The ${}^{238}\text{pu}{}^{\mathrm{239\; +\; 240}}\text{pu}$ and ${}^{\mathrm{239\; +\; 240}}\text{Pu}{}^{137}\text{Cs}$ activity ratios vary within relatively narrow ranges with time, while a much wider variation was observed for the ${}^{241}\text{Am}{}^{\mathrm{239\; +\; 240}}\text{Pu}$ activity ratio. The cause of the wider variation of the ${}^{241}\text{Am}{}^{\mathrm{239\; +\; 240}}\text{Pu}$ ratio may be related to the difference in the mean age of fallout brought down in different seasons.     

Plutonium and americium in anoxic marine sediments: Evidence against remobitization

^{239 + 240}Pu activities of 100–450dpm/kg are found down to 15–18 cm in anoxic Saanich Inlet sediments, with a subsurface maximum in undisturbed deposits. Integrated ^{239 + 240}Pu inventories which overlap delivery estimates are present both in two cores of anoxic sediments from Saanich Inlet and in one core of oxic sediments 65 km away in Dabob Bay, Washington. ${}^{241}\text{Am}{}^{\mathrm{239\; +\; 240}}\text{Pu}$ ratios in Saanich Inlet sediments overlap ratios in unfractionated midnorthern latitude fallout, in oxic sediments from the Washington continental shelf, and in anoxic sediments from two basins off southern California and Mexico. The ${}^{\mathrm{239\; +\; 240}}\text{Pu}{}^{137}\text{Cs}$ ratios in three intervals of Saanich Inlet sediments are also in agreement with ratios previously reported for oxic coastal marine sediments. The Pu inventories, the $\text{Am}\text{Pu}$ and $\text{Pu}\text{Cs}$ ratios, and the Saanich Inlet Dabob Bay comparison all argue that Pu is not rapidly remobilized in anoxic sediments.The subsurface ^{239 + 240}Pu activity maximum is not in agreement with the historical record of peak Pu fallout in 1963–1964 unless our ²¹⁰Pb-derived sedimentation rates are incorrectly high. However, they are in good agreement with previous ²¹⁰Pb and varve chronologies in Saanich Inlet, and also give reasonable dates for times when ^{239 + 240}Pu and SNAP-9A supplied ²³⁸Pu first appear in the sediments. We conclude they properly date the maximum in sedimentary ^{239 + 240}Pu activity at 1970–1973, and seek explanations for the 7–10yr time lag after peak fallout.^{239 + 240}Pu inventories in one core from the eastern basin of the Cariaco Trench and in two cores from Golfo Dulce. an anoxic basin off the Pacific coast of Costa Rica, are also in reasonable agreement with fallout delivery to these latitudes when excess ²¹⁰Pb inventories and fluxes are used to verify recovery of at least a major fraction of the most recently deposited sediments.     

Migration of transuranic elements in groundwater from the near-surface radioactive waste site

Field experiments and laboratory studies were performed to investigate migration processes of plutonium isotopes from a near-surface radioactive waste trench to the underlying sandy aquifer at the Red Forest waste dump in the Chernobyl zone. The objectives of these experiments were to characterize the spatial distribution and possible migration mechanisms of plutonium in the aquifer. During 2002–2007 experimental investigations were carried out and spatial distributions of plutonium isotopes (^239,240Pu, ²³⁸Pu), ⁹⁰Sr and major ions in the aquifer in the direction of the groundwater flow were obtained. Specific activities of radionuclides in groundwater depended on the location of the piezometer and varied in the range of 1–360 mBq kg⁻¹ for ^239,240Pu, 0.5–180 mBq kg⁻¹ for ²³⁸Pu and n–n·10⁴ Bq kg⁻¹ for ⁹⁰Sr. It was found that the spatial features of the distributions of plutonium and strontium specific activities in the upper eolian aquifer were similar, i.e. there was a correlation between the positions of the activity maxima of the radionuclides. The Pu isotopes plume in the aquifer spreads about 15 m downstream of the radionuclides source. Characterization of the initial radionuclide composition of the waste showed that all plutonium in the aquifer originated from the trench. The ratio of plutonium isotopes (^239,240Pu/²³⁸Pu) at the sampling time was the same in waste material and in groundwater samples. In situ ultrafiltration of several groundwater samples was carried out. The size fractionation data obtained suggest that a significant part of plutonium (50–98%) in the groundwater sampled close to the source from the upper part of the aquifer is associated with a very low molecular weight fraction (<1 kDa).     

Recommended Values of 239Pu, 240Pu and 239+240Pu Concentrations in Reference Material IAEA-315 (Marine Sediment) Estimated by Thermal Ionisation Mass Spectrometry, Inductively Coupled Plasma-Mass Spectrometry and Alpha Spectrometry

The recommended concentrations of ²³⁹Pu, ²⁴⁰Pu and ^239+240Pu in reference material IAEA‐315 (marine sediment) were estimated by three analytical methods: isotope dilution thermal ionisation mass spectrometry (TIMS), isotope dilution inductively coupled plasma‐mass spectrometry (ICP‐MS) and alpha spectrometry. The determination of ²³⁹Pu and ²⁴⁰Pu (^239+240Pu by alpha spectrometry) was carried out with samples from randomly selected bottles using each method. Plutonium‐238 was also measured by alpha spectrometry. A plutonium‐242 reference material was used as a spike for the quantitative analysis. The influence of ²⁴²Pu in the samples was therefore calculated; however, this contribution was less than the range of uncertainty and did not influence the final results. The obtained data were statistically analysed using variance component analysis and paired comparison. The combined standard uncertainties from “method/measurement”, “bottle” and “sub‐sample” were in the order of 3 to 6%. The main contributions to the uncertainty were from the material heterogeneity and from systematic differences between methods. Based on this study with twenty‐seven analyses using 10–14 g sample mass, concentrations of (38 ± 3) Bq kg^?1, (28 ± 3) Bq kg^?1 and (66 ± 4) Bq kg^?1 are proposed as recommended values for ²³⁹Pu, ²⁴⁰Pu and ^239+240Pu, respectively, and (9.5 ± 0.4) Bq kg^?1 for ²³⁸Pu as an information value in reference material IAEA‐315. In mass concentration units, these amount to (16.4 ± 1.2) ng kg^?1, (3.3 ± 0.4) ng kg^?1 and (0.015 ± 0.003) ng kg^?1 for ²³⁹Pu, ²⁴⁰Pu and ²³⁸Pu, respectively. The certified reference materials NIST 4350B and NIST 4354 were also analysed by TIMS for quality assurance of the method used in this study.     

Sources of plutonium to the tropical Northwest Pacific Ocean (1943-1999) identified using a natural coral archive

The Pu isotopes, ²³⁹Pu and ²⁴⁰Pu, were determined in annually-banded skeletons of an accurately dated (1943-1999) modern coral (Porites lobata) from Guam Island to identify historical Pu sources to the tropical Northwest Pacific Ocean. Activity concentrations of ^239+240Pu and ²⁴⁰Pu/²³⁹Pu atom ratios were determined in the dated coral bands using multi-collector inductively coupled plasma mass spectrometry (MC-ICP-MS). Close-in fallout from the former US Pacific Proving Grounds (PPG) in the Marshall Islands and global fallout were identified as the two main sources. The Guam site was dominated by PPG close-in fallout in the 1950s, with an average ²⁴⁰Pu/²³⁹Pu atom ratio of 0.315 ± 0.005. In addition, a higher ²⁴⁰Pu/²³⁹Pu atom ratio (0.456 ± 0.020) was observed that could be attributed to fallout from the “Ivy Mike” thermonuclear detonation in 1952. The atom ratio decreased in the 1960s and 1970s due to increase in the global fallout with a low ²⁴⁰Pu/²³⁹Pu atom ratio (∼0.18). Recent coral bands (1981-1999) are dominated by the transport of remobilised Pu, with high ²⁴⁰Pu/²³⁹Pu atom ratios, from the Marshall Islands to Guam Island along the North Equatorial Current (NEC). This remobilised Pu was estimated to comprise 69% of the total Pu in the recent coral bands, although its contribution was variable over time.     

Annual cycle of radionuclide contamination on tide-washed pasture in the Mersey Estuary, NW England

The radionuclide burden of vegetation comprising a tide-washed pasture at Ince Marsh in the Mersey Estuary, U.K., derives mainly from adhered external particulates originating as suspended sediments in estuarine water. Radionuclide concentrations are dominated by the growth cycle of the vegetation, with the highest winter levels of contamination activity an order of magnitude greater than the lowest levels in mid-summer. A secondary effect due to sediment transfer during periods of severe flooding produces subsidiary features on this dominant seasonal profile. Radionuclide concentrations on vegetation are in the range¹³⁷Cs=8–191,¹³⁴Cs=0.3–0.9,²⁴¹Am=0.6–46,²³⁸Pu=0.1–1.5, and^239/240Pu=0.8–44 Bq kg⁻¹. These ranges reflect the relative concentrations of radionuclides in estuarine sediment (¹³⁷Cs=615,²⁴¹Am=202, and^239/240Pu=104 Bq kg⁻¹) rather than the values in filtered estuary water (¹³⁷Cs=0.4,²⁴¹Am=0.001, and^239/240Pu=0.001 Bq 1⁻¹). Median K_d values for these radionuclide species are Cs=1,400, Am=200,000, and Pu=80,000 1 kg⁻¹).     

Membrane luminescence determination of technogenic actinides and their speciation in environmental objects

Researchers of the Vernadsky Institute of Geochemistry and Analytical Chemistry of the Russian Academy of Sciences created a luminescence photometer of a new generation for the determination of trace amounts of uranium and transuranium elements (TUE). The limits of detection for actinides vary from 0.3 pg for uranium and neptunium to 2.0 pg for plutonium. For ²³⁷Np, the relative limit of detection is 0.008 Bq/L. The photometer was tested in the radioecological monitoring of a number of polluted zones in Russia. The dynamics of actinide migration in all of the studied zones enhanced in the series ²³⁹Pu < ²⁴¹Am < ²³⁷Np. In this series, concentrations of radionuclides in water-soluble and exchange forms that are most mobile and determine the migration mobility of chemical elements increased in all of the studied soil types. In the group of fulvic acids, concentrations of radionuclides decreased in the series ²³⁷Np > ²⁴¹Am > ²³⁹Pu irrespectively of the soil. In the group of humic acids, concentrations of radionuclides increased in the series ²³⁷Np < ²³⁹Pu < ²⁴¹Am. The sorption coefficients of radionuclides by bottom sediments of the Markha River (Kraton-3 underground nuclear explosion site) and Lake Kyzyltash (East Urals Radioactive Trace) were calculated. Bioaccumulation factors of radionuclides by different plants in the impact area of the Kraton underground nuclear explosion were determined depending on the plant type.     

Correlations of natural radionuclides in sediment from Danube

The correlation between specific activities of some natural radionuclides (²³⁸U, ²²⁶Ra, ²³²Th, ⁴⁰K) measured in sediment taken from river bottom was studied. The sediment was taken from the Serbian part of the Danube River. Good correlation between some of the isotopes is observed, so that their specific activity ratios are spread over a lower range than specific activities themselves. This suggests that evaluation of specific activity ratios of some natural radionuclides could be a more sensitive method for the determination of increased levels of some of them than the straightforward analysis of specific activities.     

Vertical profile of artificial radionuclide concentrations in the Central Arctic Ocean

The artificial radionuclides ⁹⁰Sr, ¹³⁷Cs, ²³⁸Pu, ^239,240Pu and ²⁴¹Am have been measured in eight water samples collected in 1979, at intervals from surface to bottom, through the ice at the LOREX satellite camp SS near the North Pole. Differences in the concentrations and ratios of these nuclides, compared with values measured, over time, in the various water masses that flow into the Arctic Ocean, can be used as semi-independent checks on rates of flow to the LOREX stations and on residence times in the Arctic Ocean. An unexpected finding was that water labelled with low-level liquid waste from the Windscale plant on the Irish Sea is a major component of the 1500 m LOREX sample, and has reached there in no more than eight to ten years. Even from this one station in the Polar Ocean, estimation of the inventories of the various radionuclides is good enough to emphasize the importance of horizontal advection of the various supply terms to the Arctic.     

Contents of radionuclides in soil and biota at the site of the Kraton-3 accidental underground nuclear test,Yakutia

The paper presents results of radiocological monitoring at the site of the Kraton-3 accidental underground nuclear test in Yakutia. The distribution and migration of ¹³⁷Cs, ⁹⁰Sr, ²³⁷Np, and ^238–240Pu in the soil and its living cover of the northern taiga are analyzed, and it is demonstrated that the radioecological conditions at the territory are still adverse in spite of the rehabilitation measures.     

Downward migration of Chernobyl-derived radionuclides in soils in Poland and Sweden

Vertical profiles of ¹³⁷Cs and ^239,240Pu were measured in soils collected from two sites in southern Sweden and three sites in southern Poland and were modeled using both a solute transport model and a bioturbation model to better understand their downward migration. A time series of measured ¹³⁷Cs profiles indicates that ¹³⁷Cs from Chernobyl was found at the soil surface in 1986 but it has migrated progressively downward into the soil 4.5-25.5 cm since. However, because of dispersion during the migration and mixing following Chernobyl deposition and the much higher activities of ¹³⁷Cs from Chernobyl, stratospheric fallout of ¹³⁷Cs from the 1960s cannot be identified as a second ¹³⁷Cs activity maximum lower in the soil column at any of the sites. Conversely, the ²⁴⁰Pu/²³⁹Pu ratio indicates that no Chernobyl-derived Pu is present in any of the cores with the exception of one sample in Sweden. This difference may be attributed to the nature of the release from Chernobyl. Cesium volatilized at the reactor temperature during the accident, and was released as a vapor whereas Pu was not volatile and was only released in the form of minute fuel particles that traveled regionally. Both the solute diffusion and the bioturbation models accurately simulate the downward migration of the radionuclides at some sites but poorly describe the distributions at other sites. The distribution coefficients required by the solute transport model are about 100 times lower than reported values from the literature indicating that even though the solute transport model can simulate the profile shapes, transport as a solute is not the primary mechanism governing the downward migration of either Cs or Pu. The bioturbation model uses reported values from the literature of the distribution coefficients and can simulate the downward migration because that model buries the fallout by placing soil from depth on top and mixing it slightly throughout the mixing zone (0.6-2% per year of mixing). However, mixing in that model predicts concentrations in the top parts of the soil profiles which are too high in many cases. Future progress at understanding the downward migration of radionuclides and other tracers will require a more comprehensive approach, combining solute transport with bioturbation and including other important soil processes.     

I/I ratios in Scottish coastal surface sea water: Geographical and temporal responses to changing emissions

This work constitutes the first survey of I isotope ratios for Scottish sea water including the first data for the west of Scotland. These data are of importance because of the proximity to the world’s second largest emission source of ¹²⁹I to the sea, the Sellafield nuclear reprocessing plant, because of the increasing importance of the sea to land transfer of ¹²⁹I and also as input data for dose estimates based on this pathway of ¹²⁹I. ¹²⁹I/¹²⁷I ratios in SW Scotland reached 3 × 10⁻⁶ in 2004. No strong variation of I isotope ratios was found from 2003 to 2005 in Scottish sea waters. Iodine isotope ratios increased by about a factor of 6 from 1992 to 2003 in NE Scotland, in agreement with the increase of liquid ¹²⁹I emissions from Sellafield over that time period. It is demonstrated that ¹²⁹I/¹²⁷I ratios agree better than ¹²⁹I concentrations for samples from similar locations taken in very close temporal proximity, indicating that this ratio is more appropriate to interpret than the radionuclide concentration.     

An analysis of naturally occurring radionuclides and <Superscript>137</Superscript>Cs in the soils of urban areas using gamma-ray spectrometry

This study of environmental radioactivity was carried out in the soils of an urban area. Naturally occurring gamma-emitting radionuclides and man-made ¹³⁷Cs were found in the soil profiles collected from four parks in the central Belgrade city area and the soil layer was examined every 10 cm and to a depth of 50 cm. Radioisotope activity concentrations (Bq kg^?1) in the samples of urban soil using the gamma-ray spectrometry method were in the range of 14–46 for ²³⁸U, 33–50 for ²²⁶Ra, 29–63 for ²¹⁰Pb, 1.2–3.4 for ²³⁵U, 28–50 for ²³²Th, 424–576 for ⁴⁰K and 0.7–35.8 for ¹³⁷Cs. Some of the basic physicochemical soil properties (pH, organic matter content, calcium-carbonate content, particle size distribution) were determined to investigate the impact on the vertical distribution of radionuclides. The results of this investigation showed that variations of activity concentration ratios of radionuclides that belong to the same (²³⁸U/²²⁶Ra) or different radioactive series (²³²Th/²²⁶Ra; ²³⁵U/²³⁸U), including ²¹⁰Pb/¹³⁷Cs ratios could well be explained by the properties of the soil. Alkaline pH reaction, the accumulation of organic matter in the uppermost and of carbonates in the deepest layers of urban soil had an effect on ²³⁸U/²²⁶Ra, and ²¹⁰Pb/¹³⁷Cs activity concentration ratio values, while ²³²Th/²²⁶Ra and partially ²³⁵U/²³⁸U ratios were associated with the particle sizes vertical distribution. A study of radionuclides in the samples of leaves of two deciduous tree species common for these parks was also conducted and ²¹⁰Pb and ⁴⁰K were found concentrated in leaves rather than other investigated radionuclides.     

Comparative Estimation of the Plutonium (238Pu, 239+240Pu) and Radiocesium (137Cs) Content in Bottom Sediments and Hydrobionts of the Yenisei River

Doklady Earth Sciences - The contents of isotopes of plutonium (238Pu and 239, 240Pu) and 137Cs in samples of bottom sediments and hydrobionts (water moss, amphipods, and caddisfly larvae with...     

Transport and accumulation of actinide elements in the near-shore environment: field and modelling studies

Nuclear facilities in coastal locations often discharge low‐level liquid wastes into the sea and the radioisotopes in these discharges are of interest both in assessing possible environmental impacts and as tracers for coastal processes. The distributions of a range of artificial radionuclides, derived from the authorized discharges from British Nuclear Fuels (BNFL) Sellafield, have been determined in the sediments of an intertidal salt marsh in the Esk Estuary, Cumbria, UK. Where published discharge histories exist (for ¹³⁷Cs, ²³⁸Pu, ^239,240Pu and ²⁴¹Am), the sediment core‐profile distributions of these radionuclides have been compared with the releases from Sellafield, and consistent values of the accumulation rate (0·226 ± 0·007 g cm^?2 yr^?1) are obtained. A quantitative model has been developed, describing association of radionuclides with suspended particulate material, which is then accumulated and mixed in an offshore mud patch before resuspension and deposition in the salt marsh. The model has been used to describe radionuclide distributions observed in both the mud patch and the salt marsh, and to identify isotopes for which post‐depositional remobilization or solution transport from the discharge point are important. The behaviour of the commonly studied isotopes (¹³⁷Cs, ²³⁸Pu, ^239,240Pu and ²⁴¹Am) is similar to that observed at this and other nearby locations. The activation product isotope ²³⁶U is enhanced in these sediments over the natural baseline by four to eight orders of magnitude, and the results suggest that Sellafield‐derived uranium is comparably mobile to ¹³⁷Cs in these sediments although the processes governing the behaviour of these two elements may be different. In situ production of ²⁴¹Am by decay of its ²⁴¹Pu parent has generated only 17% of the current sediment inventory of this isotope, insufficient to account for the increase over the last 20–25 years, and suggesting that the input material for these sediments is preferentially enriched in Am relative to Pu during transport from the offshore mud patch. The discharge history of ²⁴⁴Cm, which is unknown, has also been reconstructed from the sediment profile and the model.     

铀矿床的天然类似物研究

本文叙述连山关铀矿床内的地下水和铀矿体中的12 9I和2 39Pu的测量结果。研究表明 ,铀矿床内的地下水把12 9I从铀矿石中淋滤出来 ,12 9I在地质环境中具有活泼的地球化学特征 ;铀矿体中积累的2 39Pu自该矿床形成 190 0Ma以来未发生迁移。     

Gross-beta activity in ground water: natural sources and artifacts of sampling and laboratory analysis

Gross-beta activity has been used as an indicator of beta-emitting isotopes in water since at least the early 1950s. Originally designed for detection of radioactive releases from nuclear facilities and weapons tests, analysis of gross-beta activity is widely used in studies of naturally occurring radioactivity in ground water. Analyses of about 800 samples from 5 ground-water regions of the United States provide a basis for evaluating the utility of this measurement. The data suggest that measured gross-beta activities are due to (1) long-lived radionuclides in ground water, and (2) ingrowth of beta-emitting radionuclides during holding times between collection of samples and laboratory measurements.Although⁴⁰K and²²⁸Ra appear to be the primary sources of beta activity in ground water, the sum of⁴⁰K plus²²⁸Ra appears to be less than the measured gross-beta activity in most ground-water samples. The difference between the contribution from these radionuclides and gross-beta activity is most pronounced in ground water with gross-beta activities > 10 pCi/L, where these 2 radionuclides account for less than one-half the measured ross-beta activity. One exception is groundwater from the Coastal Plain of New Jersey, where⁴⁰K plus²²⁸Ra generally contribute most of the gross-beta activity. In contrast,⁴⁰K and²²⁸Ra generally contribute most of beta activity in ground water with gross-beta activities < 1 pCi/L.The gross-beta technique does not measure all beta activity in ground water. Although³H contributes beta activity to some ground water, it is driven from the sample before counting and therefore is not detected by gross-beta measurements. Beta-emitting radionuclides with half-lives shorter than a few days can decay to low values between sampling and counting. Although little is known about concentrations of most short-lived beta-emitting radionuclides in environmental ground water (water unaffected by direct releases from nuclear facilities and weapons tests), their activities are expected to be low.Ingrowth of beta-emitting radionuclides during sample holding times can contribute to gross-beta activity, particularly in ground water with gross-beta activities > 10 pCi/L. Ingrowth of beta-emitting progeny of²³⁸U, specifically²³⁴Pa and²³⁴Th, contributes much of the measured gross-beta activity in ground water from 4 of the 5 areas studied. Consequently, gross-beta activity measurements commonly overestimate the abundance of beta-emitting radionuclides actually present in ground water. Differing sample holding times before analysis lead to differing amounts of ingrowth of the two progeny. Therefore, holding times can affect observed gross-beta measurements, particularly in ground water with²³⁸U activities that are moderate to high compared with the activity of⁴⁰K plus²²⁸Ra. Uncertainties associated with counting efficiencies for beta particles with different energies further complicate the interpretation of gross-beta measurements.     

I/I ratios in surface waters of the English Lake District

Accelerator Mass Spectrometry (AMS) was used to measure ¹²⁹I/¹²⁷I ratios in surface sea, lake, and river water samples collected in 2004 and 2005 from the English Lake District and from SW Scotland, areas which are in relatively close proximity to the Sellafield nuclear fuel reprocessing plant in NW England. The ¹²⁹I/¹²⁷I ratios in surface water collected from the shore of the Irish Sea were in the range 2.8 × 10⁻⁶ to 8.2 × 10⁻⁶. These ratios are one order of magnitude higher than that of seawater collected from the Irish Sea in 1992, correlating with the increase in ¹²⁹I content of the Sellafield liquid effluent discharge over the last decade. The ¹²⁹I/¹²⁷I ratios in lakes in the Lake District were in the range 0.7 × 10⁻⁶ to 6.4 × 10⁻⁶ and decreased exponentially as a function of distance from Sellafield. Consideration of the relative variation of stable I concentrations and ¹²⁹I/¹²⁷I ratios suggests that Sellafield gaseous discharges may be the dominant source of ¹²⁹I to the lakes.     

Safe management of actinides in the nuclear fuel cycle: Role of mineralogy

During the past 60 years, more than 1800 metric tonnes of Pu, and substantial quantities of the “minor” actinides, such as Np, Am and Cm, have been generated in nuclear reactors. Some of these transuranium elements can be a source of energy in fission reactions (e.g., ²³⁹Pu), a source of fissile material for nuclear weapons (e.g., ²³⁹Pu and ²³⁷Np), and of environmental concern because of their long-half lives and radiotoxicity (e.g., ²³⁹Pu and ²³⁷Np). There are two basic strategies for the disposition of these heavy elements: (1) to “burn” or transmute the actinides using nuclear reactors or accelerators; (2) to “sequester” the actinides in chemically durable, radiation-resistant materials that are suitable for geologic disposal. There has been substantial interest in the use of actinide-bearing minerals, especially isometric pyrochlore, A₂B₂O₇ (A = rare earths; B = Ti, Zr, Sn, Hf), for the immobilization of actinides, particularly plutonium, both as inert matrix fuels and nuclear waste forms. Systematic studies of rare-earth pyrochlores have led to the discovery that certain compositions (B = Zr, Hf) are stable to very high doses of alpha-decay event damage. Recent developments in our understanding of the properties of heavy element solids have opened up new possibilities for the design of advanced nuclear fuels and waste forms.