Plutonium in sheep faeces as an indicator of deposition on vegetation

In order to study the deposition on vegetation of plutonium arising from the testing of nuclear weapons and discharges from nuclear facilities, sheep faeces were collected from the South-west and North of England. The plutonium content of faeces has been shown to be a reproducible and sensitive indicator of deposition on herbage and, with this technique, plutonium discharged from the Sellafield Works of British Nuclear Fuels LImited can be detected 60 km from the site. On moorland pastures the concentration of ^239+240Pu in faeces, expressed as activity per gram of ash, is roughly equal numerically to the deposit of plutonium on 1 m² of vegetation.Some of the plutonium ingested by a grazing sheep is absorbed and the highest concentrations are found in liver. The liver of a sheep grazing on pasture where the ^239+240Pu concentration in faeces was about 2 pCi (74 mBq) g⁻¹ of ash, was found to contain <1% of the Generalised Derived Limit for mutton and offal, and the meat <0·001%.     

Describing the annual cyclic behaviour of 7Be concentrations in surface air in Oceania

Surface air concentrations of (7)Be at a number of stations in Oceania show a distinct annual cycle. We apply a sinusoidal model to describe this cycle. The results show that peak (7)Be concentrations in surface air occur during early spring at tropical latitudes and during mid-to-late summer at middle latitudes. Comparison with available (90)Sr surface air data for the southern hemisphere indicates that stratosphere-to-troposphere exchange is an active atmospheric process controlling the (7)Be annual cycle throughout the Oceania region. Vertical transport of air within the troposphere also seems to influence the observed annual cycle. Seasonality in rainfall is not thought to control the annual cyclic behaviour of (7)Be in surface air.     

Sea to land transfer of anthropogenic radionuclides to the North Wales coast, Part I: external gamma radiation and radionuclide concentrations in intertidal sediments, soil and air

Previous projects specifically aimed at performing radiological assessments in the vicinity of North Wales, investigating the presence and transfer of radionuclides from sea to land, were in 1986 and 1989. Since then, changes have occurred in the radioactive discharges from the British Nuclear Group Sellafield site. Annual discharges of (137)Cs, (238)Pu, (239,340)Pu and (241)Am have decreased markedly whereas, up until recent years, discharges of (99)Tc have increased. It is therefore desirable to quantify current transfer processes of radionuclides in the North Wales region and thus provide an update on 15-year-old studies. A field campaign was conducted collecting soil samples from 10 inland transects and air particulates on air filters from three High Volume Air Samplers, along the northern coast of Wales at Amlwch, Bangor Pier and Flint. Complementary field data relating to external gamma dose rates were collected at the soil sites. The field data generated for (137)Cs, (238)Pu, (239,340)Pu and (241)Am were consistent with what had been reported 15 years previously. Therefore, there has been no increase in the supply of these Sellafield-derived radionuclides to the terrestrial environment of the North Wales coast. The (99)Tc data in sediments were consistent with reported values within annual monitoring programmes, however, a relatively high activity concentration was measured in one sediment sample. This site was further investigated to determine the reason why such a high value was found. At present there is no clear evidence as to why this elevated concentration should be present, but the role of seaweed and its capacity in accumulating (99)Tc and transferring it to sediment is of interest. The analysis of the field samples for (99)Tc, (137)Cs, (238)Pu, (239,240)Pu and (241)Am has provided a data set that can be used for the modelling of the transfer of anthropogenic radionuclides from sea to land and its subsequent radiological implications and is reported in an accompanying paper.     

Possible use of terrestrial mosses in detection of atmospheric deposition of 7Be over large areas

The activities of naturally occurring radionuclides (7)Be, (214)Bi and (210)Pb were measured in samples of terrestrial mosses collected in Serbia (42 degrees 26'19'N-45 degrees 23'12'N). The objective of this work was to establish if detectable amounts of (7)Be and (210)Pb can be found in mosses and investigate their possible variabilities over some area. These are the first steps in introducing mosses as a medium in possible monitoring of spatial distribution of (7)Be atmospheric deposition. The mean value of 360 Bq/kg of (7)Be activity was found in collected moss samples and some nonuniformity in spatial distribution (a 2.8-fold range in measured values) was observed.     

Seasonal and spatial variation of atmospheric 210Pb and 7Be deposition: features of the Japan Sea side of Japan

Monthly depositional fluxes of (210)Pb and (7)Be at Tatsunokuchi, Japan which faces the Japan Sea were studied over a 12-year period from 1991 to 2002. The data were compared with the spatial variability of these fluxes at Taejon in Korea and at 11 other sites in Japan from Ishigaki of the southern islands of Okinawa to Wakkanai of the northern end of Hokkaido over a 2-year period from 2000 to 2001. The monthly depositions of both (210)Pb and (7)Be at Tatsunokuchi revealed very similar seasonal variations with a single peak; both depositions were high in winter and low in summer. This phenomenon was found to be not transient but stationary. The deposition of these nuclides was much greater on the Japan Sea side of Japan than on the Pacific Ocean side. The cause for high deposition of (210)Pb and (7)Be in winter might be explained by a combination of a series of the following processes: blowing out of air masses with a high (210)Pb concentration near the surface layer over the continent by strong winter monsoons, additional flow of cold air masses with high (7)Be concentration at high latitude, well-mixing with generation of ascending current and convection clouds over the Japan Sea, and heavy snowfalls accompanying them.     

226Ra, 40K and 7Be activity concentrations in plants in the environment of Kaiga,India

Leaves, stem and bark samples from several plant species were collected from tropical forest of Kaiga, in the west coast of India where two nuclear power reactors of 220 MW each have just been commissioned and another two are under construction, and analysed for their (226)Ra, (40)K and (7)Be concentrations. The activities of (226)Ra and (40)K in plants were found to vary in the range BDL-13.2 and 12.0-797.3 Bq kg(-1), respectively. Plants show significant (7)Be activity in leaves, the activity varies in 72.5-1,060.8 Bq kg(-1). Stem and bark of plants show higher levels of (226)Ra and (40)K when compared to leaves. Soil-to-plant transfer factor for (226)Ra and (40)K were found to vary in the range BDL-0.37 and 0.09-5.61, respectively for different plants. The concentration of (226)Ra and (40)K in leaves depends on the age of the leaves.     

Acid deposition and watershed characteristics in relation to lake chemistry in northeastern Minnesota

The relationship between lake sensitivity to atmospheric acidic inputs and the neutralization capacity of watersheds is examined for 267 lakes in northeastern Minnesota. Three water chemistry/sensitivity measures (color, sulfate, and alkalinity) are correlated with variables representative of precipitation and sulfate inputs, hydrology, and the acid neutralization capacity of various watershed components. An ordinal scale for ranking bedrock and surficial deposit neutralization capacity is presented. The watershed variables found to account for the largest percentages of the variability in measured color, sulfate, and alkalinity levels are determined. Color is strongly related to the presence of peat or marsh and hydrologic renewal time, whereas sulfate is primarily related to atmospheric deposition, evaporative concentration, bedrock type, and the presence of coniferous forest. Variation in alkalinity is the most difficult of the water chemistry measures to explain; for headwater lakes, atmospheric sulfate input, water renewal time, the presence of deciduous forest, and the weatherability of underlying bedrock determine much of its variability. The results illustrate important averaging properties of watersheds from small headwater systems to large drainages and the difficulty in obtaining correlations for some water quality measures (e.g., alkalinity) when some variables, such as soils and land cover, are available only as large-area averages.     

Sea to land transfer of anthropogenic radionuclides to the North Wales coast, Part II: aerial modelling and radiological assessment

Modelling calculations have been performed to predict the radiological impact of the sea to land transfer pathway to members of the public in North Wales from 1952 to 2004. The radionuclides of interest were (99)Tc, (137)Cs, (239,240)Pu and (241)Am and the exposure routes considered were food consumption, external and inhalation. The consumption of locally grown terrestrial food in the early to mid 1980s was the most significant source of exposure to all of the groups considered, with (239,240)Pu being the radionuclide contributing most to the dose. A maximum dose of 1.46muSvy(-1) was calculated for adult members of the critical consumption group in 1985, with doses for 2004 reducing to 0.59muSvy(-1). Despite the conservative approach of the dose calculations, the dose rate values are very low, less than 0.15% of the annual limit of 1000muSvy(-1) for the UK public from controlled radiation sources (excluding medical).     

Factors controlling 7Be and 210Pb atmospheric deposition as revealed by sampling individual rain events in the region of Geneva, Switzerland

Bulk atmospheric deposition of 7Be and 210Pb has been measured at Versoix, close to Geneva, Switzerland. Collectors were continuously deployed from November 1997 through November 1998 for periods from 1 to 22 days depending on the frequency of rain. The activities of 7Be and 210Pb integrated over the sampling interval were moderately well correlated with rainfall (r2 of 0.66 and 0.55, respectively; p < 0.001) and well correlated one with the other (r2 of 0.91; p < 0.001). The 7Be/210Pb activity ratio is close to 13.5, except for samples collected in the periods of very low precipitation which have a distinctly lower ratio. A simple model accounting for rainfall, seasonal variations and reload of the local atmosphere after a rain event explains 90% of the variance of 7Be and 210Pb deposition. Concentrations of 210Pb and Ca++ in rain were correlated with transport time of air masses over the continent as indicated by reconstruction of air mass trajectories over three days.     

7Be to 210Pb concentration ratio in ground level air in Belgrade area

7Be to 210Pb concentration ratios in ground level air on two monitoring stations (MS1 and MS2) in Belgrade area were determined from 1996 to 2001. The average monthly concentrations of 7Be in ground level air were in the range of 0.6-18.3 mBq/m3 and exhibited one or two summer/early fall maxims and one minimum in winter. The maximum concentrations for 210Pb were generally observed in the fall, with the average concentrations in the range of 1.09 x 10(-4) to 30.9 x 10(-4) Bq/m3. The 7Be/210Pb ratios were in the range of 1.7-12.7 (MS1) and 1.8-11.3 (MS2), with summer maxims and late fall/winter minimums. The mean Radionuclides Loading Indices values approach zero except for 1996/1997 (MS1) and 2001 (MS2) due to higher concentrations of 7Be and 210Pb. The mean monthly concentrations of both radionuclides exhibited lognormal distributions. There is significant correlation between the 7Be/210Pb activities ratio and the air stability classes A + B + C for both monitoring stations (correlation coefficients 0.61-0.65), and no correlation with D class and E + F classes. Correlation was found between the activity of 7Be and air stability classes A + B + C (0.46-0.68), and E + F (0.38 for MS1), while for 210Pb, a moderate correlation (0.38-0.40) was found with the E + F air stability classes.     

Activity concentrations of 226Ra, 228Ra, 210Pb, 40K and 7Be and their temporal variations in surface air

Activity concentrations of the long-lived natural radionuclides ²²⁶Ra, ²²⁸Ra, ²¹⁰Pb, ⁴⁰K and of ⁷Be in surface air were measured twice monthly at a semi-rural location 10 km north of Munich (FRG) for at least three years. For the time interval 1983–1985, all values were found to be distributed log-normally, with geometric means (in μBq m⁻³) of 1·2 for ²²⁶Ra, 0·5 for ²²⁸Ra, 580 for ²¹⁰Pb, 12 for ⁴⁰K and 3500 for ⁷Be. Reflecting their common origin, the activity concentrations of ²²⁶Ra and ⁴⁰K are correlated with surface air dust concentrations (geometric mean 59 μg m⁻³). Seasonal variations of ²¹⁰Pb and ⁷Be air activity concentrations are established for the time interval 1978–1985.The contribution of local soil activity to the air activity concentrations of these radionuclides and of natural uranium is discussed. Resuspension factors are found to be of the order of 10⁻⁹m⁻¹.     

Temporal changes of 7Be, 137Cs and 210Pb activity concentrations in surface air at Monaco and their correlation with meteorological parameters

Results of analysis of ⁷Be, ¹³⁷Cs and ²¹⁰Pb on aerosol filters carried out from 1998 to 2010 in Monaco show that a weak correlation between activity concentrations of these radionuclides in the atmosphere and meteorological parameters has been found for ⁷Be and temperature (r = 0.50), ²¹⁰Pb and temperature and humidity (r = 0.43 and 0.41, respectively), and ¹³⁷Cs and precipitation (r = 0.51). The minimum and maximum ⁷Be activity concentrations were observed during 2000 and 2009, corresponding with the maximum and minimum solar activity, respectively. The maximum ¹³⁷Cs activity concentration found in May-June 1998 was due to the accident at Algeciras in Spain. The deposition velocities of ⁷Be, ¹³⁷Cs and ²¹⁰Pb depended on the precipitation rate, and attained maximum values during dry seasons. The investigated radionuclides may be used as atmospheric tracers, especially in long-term periods.     

Precipitation scavenging of 7Be and 137Cs radionuclides in air

Atmospheric depositional fluxes of the naturally occurring 7Be of cosmogenic origin and 137Cs from fallout of the Chernobyl accident were measured over a 6-year period (January 1987-December 1992) at Thessaloniki, Greece (40 degrees 38'N, 22 degrees 58'E). Total precipitation accumulation during 1987-1992 varied between 33.7 cm and 65.2 cm, reflecting a relatively dry (precipitation-free) climate. The activity concentrations of 7Be and 137Cs in rainwater depended on the precipitation rate, being higher for low precipitation rates and lesser for high precipitation rates. 137Cs was removed by rain and snow more efficiently than 7Be. Snowfall was more efficient than rainfall in removing the radionuclides from the atmosphere. The annual bulk depositional fluxes of 7Be varied between 477 and 1133 Bq m(-2) y(-1) and this variability was attributed to the amount of precipitation and the variations of the atmospheric concentrations of 7Be. The annual bulk depositional fluxes of 137Cs showed a significant decrease over time from 1987 to 1992, resulting in a removal half-life of 1.33 years. The presence of 137Cs in air, and therefore in rainwater and snow, long after the Chernobyl accident (26 April 1986) was mainly due to the resuspension process. The normalized depositional fluxes of both radionuclides showed maximal values during the spring season where the maximum amount of precipitation occurred. The relatively high positive correlation between 7Be and 137Cs normalized depositional fluxes indicates that the scavenging process of local precipitation controlled the fluxes of both radionuclides. The dry depositional flux of 7Be was less than 9.37% of total (wet and dry) depositional flux. The fraction of dry-to-total depositional flux of 137Cs was much higher than that of 7Be, due to the resuspended soil.     

Metal concentrations in mussel Crenomytilus grayanus and oyster Crassostrea gigas in relation to contamination of ambient sediments

The relationship between Zn, Cu, Cd, Pb, and Ni concentrations in soft tissues of mussels and oysters and those in ambient sediments was examined. The study area was the coastal habitats of the northwestern Sea of Japan, which has a broad range of contamination due to urban sewage. Significant increases of all metals, except Ni, were observed in mussel Crenomytilus grayanus at concentrations of easily leachable metals in ambient sediments higher than 2, 100, and 800 microg/g for Cd, Cu, and Zn, respectively. Pb was accumulated by the mussels with no distinct threshold in Pb contamination of sediments. After 2 months, C. grayanus transplanted from a pristine to a contaminated locality increased in Pb up to 12%, and Cu up to 68% of concentrations of these metals in the contaminated local mussels, but Zn and Cd concentrations increased only in the excretory tissue, not in the somatic tissue, or in the soft tissue as a whole. Such regulation of metal accumulation puts limitations on the use of C. grayanus for monitoring of slightly and moderately contaminated localities. On the other hand, the oyster Crassostrea gigas showed definite accumulation of all metals, except Ni, at moderate contamination of ambient sediments. As contamination of sediments increased, increases of Pb, Zn and Cu concentrations in C. gigas slowed, possibly due to physiological control at very high metal concentrations in oyster soft tissue. Thus, the mussel C. grayanus should be used mainly for the monitoring of heavy contaminated localities, and the oyster C. gigas is more suitable as an indicator of low and moderate contamination.     

Beryllium-7 in near-surface air and deposition at Brisbane, Australia

Measurements of 7Be concentrations in near-surface air and 7Be deposition were carried out at Brisbane, Australia. Concentrations of 7Be in near-surface air measured over 4 years show seasonal variations with values above the annual mean occurring mainly in the spring and summer months of each year. These higher concentrations coincide with the expected influx of stratospheric air to the planetary boundary layer in early spring and higher rates of convective circulation within the troposphere during summer. 7Be deposition measurements over 3 years show seasonal variations similar to the seasonal rainfall pattern. There is a statistically significant (p<0.001) linear relationship between monthly (7)Be deposition and rainfall amount. This relationship is used to calculate the net cumulative (7)Be areal activity density.     

Behavioral difficulties in 7-year old children in relation to developmental exposure to perfluorinated alkyl substances

BackgroundPerfluorinated alkyl substances (PFAS) are suspected endocrine disruptors that are highly persistent and neurotoxic in animals. Human epidemiological studies of exposure-related deviations of children's behaviors are sparse. We assessed the associations between prenatal, 5- and 7-year PFAS exposures and behavioral problem scores in 7-year Faroese children.MethodsConcentrations of perfluorooctanoic acid (PFOA), perfluorononanoic acid (PFNA), and perfluorodecanoic acid (PFDA), perfluorooctane sulfonate (PFOS), and perfluorohexane sulfonic acid (PFHxS) were measured in maternal serum and in serum from children at ages 5 and 7 years (n = 539, 508, and 491, respectively). We used multivariable regressions and structural equations models to estimate the covariate-adjusted associations between serum-PFAS concentrations and behavioral difficulties, as assessed by the strengths and difficulties questionnaire (SDQ) at age 7.ResultsSerum-PFOS and PFHxS concentrations declined over time, whereas PFOA, PFNA, and PFDA tended to increase. No associations were observed between prenatal PFAS concentrations and SDQ scores. However, a two-fold increase in 5-year serum-PFOA, PFNA, and PFDA concentrations was associated with increases in total SDQ scores by 1.03 (95% CI: 0.11, 1.95), 0.72 (95% CI: 0.07, 1.38) and 0.78 points (95% CI: 0.01, 1.55), respectively. For SDQ subscales, significant associations were found in regard to hyperactivity, peer relationship, and conduct problems, as well as internalizing and externalizing problems and autism screening composite scores. Cross-sectional analyses at age 7 years showed possible sex-dimorphic associations between PFAS concentrations and SDQ scores, where girls had consistently positive associations with SDQ scores whereas boys exhibited a pattern of negative or null associations.ConclusionsHigher serum PFAS concentrations at ages 5- and 7-years, but not prenatally, were associated with parent-reported behavioral problems at age 7.     

Mercury and docosahexaenoic acid levels in maternal and cord blood in relation to segmental maternal hair mercury concentrations at parturition

Fish is a major source of harmful methylmercury (MeHg) and beneficial docosahexaenoic acid (DHA) in the developing brain. In this study, we investigated the correlations among maternal and umbilical cord (cord) MeHg and DHA levels at parturition, and mercury (Hg) concentration in 1-cm incremental segments hair samples which grew during gestation representing monthly MeHg exposure levels throughout the period. Whole blood Hg and plasma DHA levels were measured in blood sample pairs collected from 54 mothers at early gestation and parturition, and in cord blood. Maternal hair samples were collected at parturition, and Hg concentrations were measured in 1-cm incremental segments. Hg level in mothers at parturition was slightly lower than that at early gestation and the level in cord blood were approximately 1.9 times higher than that in mothers at parturition. On the other hand, DHA level in mothers at parturition was approximately 2.3 and 1.6 times higher than those in mothers at early gestation and in cord plasma, respectively. These results indicate that kinetics of these chemicals in mothers during gestation and placental transfer are completely different. However, Hg and DHA levels had significant positive correlation in fetal circulation. The cord blood Hg showed the strongest correlation with maternal hair Hg in the first 1-cm segment from the scalp at parturition (r = 0.87), indicating that fetal MeHg level reflects maternal MeHg burden at late gestation. In contrast, maternal and cord plasma DHA concentrations at parturition showed the highest correlation coefficients with Hg in the fifth (r = 0.43) and fourth (r = 0.38) 1-cm hair segments, suggesting that maternal and fetal DHA levels reflects maternal fish intake during mid-gestation.     

(137)Cs concentration in zooplankton and its relation to taxonomic composition in the western North Pacific Ocean

To study the role of zooplankton in the transport of (137)Cs in the ocean, zooplankton samples were collected in October 2005 and June 2006 in the western North Pacific Ocean. The peak zooplankton biomass was observed in the surface layer, and gelatinous plankton was more abundant in October 2005 than in June 2006 reflecting exchange of water masses. The concentrations of (137)Cs in zooplankton varied from 11 to 24 mBq kg wet(-1) and were higher in October 2005 than in June 2006. The elevated abundance of gelatinous zooplankton probably led to higher concentration of (137)Cs in zooplankton in October 2005. Annual export fluxes of (137)Cs by ontogenetic vertical migrant copepods were estimated to be 0.8 and 0.6 mBq m(-2) year(-1) at 200 and 1000 m depths, respectively; this suggested that transport of (137)Cs by zooplankton may be no trivial pathway.     

Temporal variation of Be concentrations in atmosphere for 8 y from 2000 at Yamagata,Japan: solar influence on the Be time series

We have been continuously observing the daily ⁷Be concentrations in surface air at Yamagata, Japan (38.25° N, 140.35° E) since 2000. The yearly profile of the ⁷Be concentration indicates the variation in galactic cosmic rays owing to solar modulation. Over 8 y, the ⁷Be concentration, cosmic neutrons, and number of sunspots varied by 37.4%, 12.2%, and 92.8%, respectively. The influence of precipitation on the ⁷Be variability was approximately 5%. Hence, the yearly ⁷Be concentration was mainly varied by the solar modulation of the ⁷Be production rates. Based on the production rates found in an EXPACS simulation, the observed variability indicates ⁷Be transport from high latitudes. The daily ⁷Be concentrations have two significant periodic components of 19 d and 36 d. The 36-d component implies a relationship between the sun's rotation and the vertical transport of air masses under quiet solar activity.     

Relationship between variations of Be, Pb and Pb concentrations and sub-regional atmospheric transport: Simultaneous observation at distant locations

In order to investigate the applicability of ²¹²Pb as a tracer for atmospheric transport in the sub-regional scale (few hundred kilometers in horizontal direction and up to ∼1 km by height), we measured the air concentrations of the short-lived radionuclide ²¹²Pb along with the long-lived ⁷Be and ²¹⁰Pb near the ground surface. For this purpose, simultaneous observations were continued for several days at three locations: a reference point representative for standard land surface atmosphere conditions, a second location at an altitude 650 m near the reference point, and on a solitary island ∼180 km from the reference point. Measurements of radioactivity in aerosol particle samples collected at intervals of 2-3 h with a high-volume air sampler were performed by extremely low background gamma-ray spectrometry with the use of Ge detectors located at the Ogoya Underground Laboratory. Concentration of ⁷Be or ²¹⁰Pb and their variation patterns was found to be similar among the three points during the whole observation period except for moment of the passage of a cold front. The results indicate that distributions of concentrations of the long-lived nuclides were uniform in this range. On the other hand, concentration levels and the variation patterns of the short-lived ²¹²Pb differed greatly from one location to another, reflecting differences in geographical location and altitude of the observation points. Additionally, there were certain indications that observed concentration of ²¹²Pb contained two components: an autogenous component from sources nearby and a heterogenous one from faraway sources carried by atmospheric horizontal transport. Results of this study provide experimental proof that ²¹²Pb can be used as a tracer of sub-regional atmospheric transport.