Rapid remobilisation of plutonium from estuarine sediments

Plutonium remobilisation experiments, using contaminated Esk Estuary sediments and uncontaminated River Esk and North Sea waters, have successfully reproduced the observed non-conservative behaviour of dissolved Pu in the Esk Estuary, Cumbria, UK. Remobilisation is greatest at low salinites (<4%) and, under these conditions, Pu(III, IV) and Pu(V, VI) are released into solution in similar absolute amounts. The remobilisation process appears to be associated with a rapid (equilibrium achieved in 15 min) exchange reaction involving competition between Pu species, protons and major cations for the available surface sites. The experimental results show a systematic variation in distribution coefficients (i.e. K_d) for total Pu (7·2 × 10⁴−4·1 × 10⁶), Pu(III, IV) (1·0 × 10⁵−5·8 × 10⁶) and Pu(V, VI) (6·4 × 10³−5·5 × 10⁵).     

Diffusive gradient in thin FILMS (DGT) compared with soil solution and labile uranium fraction for predicting uranium bioavailability to ryegrass

The usefulness of uranium concentration in soil solution or recovered by selective extraction as unequivocal bioavailability indices for uranium uptake by plants is still unclear. The aim of the present study was to test if the uranium concentration measured by the diffusive gradient in thin films (DGT) technique is a relevant substitute for plant uranium availability in comparison to uranium concentration in the soil solution or uranium recovered by ammonium acetate. Ryegrass (Lolium perenne L. var. Melvina) is grown in greenhouse on a range of uranium spiked soils. The DGT-recovered uranium concentration (C_DGT) was correlated with uranium concentration in the soil solution or with uranium recovered by ammonium acetate extraction. Plant uptake was better predicted by the summed soil solution concentrations of UO₂²⁺, uranyl carbonate complexes and UO₂PO₄⁻. The DGT technique did not provide significant advantages over conventional methods to predict uranium uptake by plants.     

Radon transport through a cool-season grass

²²²Rn released by mature tall fescue (Festuca arundinacea Schreb.) growing on uranium mill wastes in a controlled environment was a direct function of leaf area and essentially unrelated to the quantity of water transpired by the plants. The quantity of ²²²Rn released by the grass blades at maturity was approximately 0·01 Bq m⁻² s⁻¹ (0·3 pCi m⁻² s⁻¹). We suggest that the radioactive gas is transported from the rooting medium to leaves by mass flow in liquid water, but from leaves to the atmosphere by a path generally independent of water, i.e., primarily through the leaf cuticle and epicuticular wax.     

Experimental studies of the transfer of neptunium from sea water to sediments and organisms (annelids and molluscs)

This paper deals with the physico-chemical behaviour of neptunium in sea water and with its capacity for transfer to coastal or deep-sea sediments and for uptake by two benthic species, Arenicola marina (L.) and Cerastoderma edule (L.). We used the ²³⁹Np isotope with mass concentrations in sea water of about 2·5 × 10⁻¹⁰−5·4×10⁻¹² g litre⁻¹, which are close to the concentrations observed in the environment for ²³⁷Np. The experimental results show that Np occurs in solution mainly as the neptunyl ion NpO₂⁺, but soluble anionic and neutral complexes and particulate forms were also detected. The distribution coefficients for the sediments varied from 350 to 6500. The carbonate phase plays a decisive role in neptunium transfer but other fixation processes are also possible. Concentration factors after 13 days were found to have values of 40 and 14 for the shells and soft parts of cockles, respectively, while polychaetes had a concentration factor of 2. Thus Np has a smaller probability of transfer to sediments and organisms than have plutonium and americium.     

The transfer of 60Co from feed into vitamin B12 in cow liver,milk and beef

The transfer of the radionuclide ⁶⁰Co from feed to milk, meat and the organs of a cow and its incorporation into vitamin B12 were studied in order to determine the transfer coefficient of ⁶⁰Co into vitamin B12 in cattle. Upper limits of transfer coefficients for ⁶⁰Co organically complexed into vitamin B12 were determined to be 6·0 × 10⁻⁵ days/litre in milk and 3·9 × 10⁻⁵ days/kg in meat, based on values measured after 140 days in bovine liver.     

The distribution of plutonium,Americium and curium isotopes in pond and stream sediments of the Savannah river plant,South Carolina,USA

The concentrations of ²³⁸Pu, ^239,240Pu, ²⁴¹Am and ²⁴⁴Cm were determined in sediment samples from five streams and two ponds on the Savannah River Plant (SRP) and in four sediment samples from the Savannah River above and below the plant site. The following concentration ranges were determined: ²³⁸Pu, 0·07–386 fCi g⁻¹; ^239,240Pu, 0·37–1410 fCi g⁻¹; ²⁴¹Am, 0·1–4360 fCi g⁻¹; ²⁴⁴Cm, <0·01–392 fCi g⁻¹. Comparisons of the elemental and isotopic ratios of the sediments show that the majority of the sediments studied have been impacted upon by plant operations and that sediments outside the plant boundary in the Savannah River have only been influenced by aerial releases. Atom ratios of ²⁴⁰Pu/²³⁹Pu indicate that up to 86% of the Pu in these sediments is derived from plant operations. However, comparisons of the concentration data with values for other impacted sediments near nuclear facilities indicate that the levels are relatively small. Finally, <13% of the Pu, Am or Cm in pond sediments is associated with humic or fulvic acids, indicating that little of the material should be remobilized in oxic environments through organic complexation.     

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.     

Environmental radioactivity around tokai-works after the reactor accident at chernobyl

Following the reactor accident at Chernobyl, environmental samples of air, rain water and agricultural and marine products were collected and analyzed by gamma- and alpha-spectrometry. The highest concentrations of ¹³¹I in the environmental samples were as follows: 1·0×⁻¹ Bqm⁻³ (aerosol-associated in air); 3·0×10⁻¹ Bqm⁻³ (gaseous in air); 2·1×10² bq kg⁻¹ (plants); 1·4×10¹ Bq litre⁻¹ (milk). Other nuclides such as ⁹⁵Zr, ⁹⁵Nb, ¹⁰³Ru, ¹⁰⁶Ru, ¹²⁵Sb, ^129mTe, ¹³²I/¹³²Te, ¹³⁴Cs, ¹³⁷Cs, ¹⁴⁰Ba/¹⁴⁰La, ¹⁴¹Ce and ¹⁴⁴Ce were also observed in various environmental samples. ^110mAg was only detected in marine products such as cephalopoda and shellfish, ^239,240Pu and ²⁴¹Am originating from the accident were not identified.Based on the monitoring results at one dairy farm, we have derived an equation to model the transport of ¹³¹I from pasture grass to milk. This equation was then applied to the data from two other farms around Tokai-Works and the calculated ¹³¹I activities in milk were compared with those measured. The equation shows good predictive capabilities for quantification of the peak concentrations of ¹³¹I in milk but underestimates longer-term activities.     

Size distributions and growth of natural and chernobylderived submicron aerosols in Tennessee

The median aerodynamic diameters of aerosol-associated SO₄²⁻, ²¹⁰Pb, ⁷Be, and Chernobyl-derived fission products in Tennessee were examined using high-volume cascade impactors. Regardless of season, the ‘steady-state’ size distributions of SO₄²⁻ shifted to larger sizes than found for either ²¹⁰Pb or ⁷Be, and for ⁷Be sizes showed a weaker seasonal dependency than for either SO₄²⁻ or ²¹⁰Pb. It is suggested that the size differences are the result of the different spatial distributions of these species in the atmosphere during aerosol formation and growth. The mean growth rate of aerosols between ≈0·2 μm and ≈0·4 μm was estimated to be ≈0·03 μm d⁻¹ from a comparison of the median diameter of ²¹⁰Pb when it is first produced from ²¹⁴Po decay with the median diameter after a mean atmospheric residence time of 7 d.Measurements of the size distributions of radioactive aerosols released during the nuclear reactor accident at Chernobyl were made in May and June 1986, and provided rare information on growth rates of aerosols released to the atmosphere over a short time period. A linear growth rate of ≈0·013 μm d⁻¹ was observed in the lower troposphere after the median diameter had reached ≈0·4 μm. Chernobyl-derived ^134,137Cs was less soluble than ⁷Be, suggesting the presence of an aerosol core derived from reactor constituents. An analysis of time intervals and trends in both concentrations and isotopic ratios, when compared to Soviet data on the time course of radioactive releases from the damaged reactor, suggested that the large releases which occurred in early May were an important component of the globally transported ¹³⁷Cs.     

Scavenging of 234Th in the Eastern Irish Sea

Measurements of the disequilibria of ²³⁴Th/²³⁸U in seawater and in suspended particulate and seabed sediment in the eastern Irish Sea reveal that the residence time of dissolved ²³⁴Th (0·5–7·7 days) is controlled by the concentration of particles in suspension (0·4–6·9 mg litre⁻¹, which reflects the rate of sediment resuspension (0·5–5·9 kg m⁻²y⁻¹). The residence time of ²³⁴Th with respect to removal to the seabed is longer (7–50 d) and is less dependent on variations in the suspended load. Anthropogenic sources of ²³⁸U contribute up to 8–15% of the water column production of ²³⁴Th. Enhanced scavenging occurs near the coast and there appears to be a net horizontal flux of ²³⁴Th within this region.     

Transport of 131I through the grass-cow-milk pathway at a northeast US dairy following the chernobyl accident

Following the Chernobyl accident, samples of pasture grass and fresh farm milk were collected in northern New Jersey. The time-integrated activities of ¹³¹I were used to calculate a milk transfer coefficient of 0·001 d liter⁻¹. This value is at the lower range of those previously reported. No significant difference in the value of the transfer coefficient was seen when calculated based on the integrated ¹³¹I in the total grass as compared to only the upper portion of the grass. Therefore, for this event, the height of the vegetation grazed by the cows would not have influenced the concentration of ¹³¹I in fresh milk.     

Soil to plant transfer of Radium-226

A study of the uptake of ²²⁶Ra by vegetables was carried out in zones contaminated by wastes from an abandoned radium salts factory and from uranium mines and in uncontaminated regions of purely natural radioactivity. Radium-226 uptake depends on its concentration in the soil, the logarithm of its concentration in the vegetables being a linear function of the logarithm of the concentration in the soil. Concentration factors for ²²⁶Ra uptake by cabbage leaves range from 0·007 to 0·11; for herbage, they range from 0·09 to 0·5.     

Laboratory studies of the chemical behaviour of plutonium associated with contaminated estuarine sediments

Laboratory experiments, with contaminated Esk Estuary sediment and uncontaminated River Esk and North Sea waters, have provided detailed information on Pu remobilisation behaviour. Of the 977 mBq g⁻¹ Pu (III, IV) associated with the sediment, 2·6% is subject to a rapid reversible exchange reaction. Well-defined distribution coefficients (K_d) have been determined with respect to this labile fraction (e.g. 5 × 10³ litres kg⁻¹ for remobilisation into river water). A low level of Pu (III, IV) remobilisation can be maintained following complete removal of the labile fraction, probably through a rate-limited reaction involving a more strongly bound form of Pu. Plutonium (V, VI) remobilisation occurs both through rapid exchange of a comparable labile component and through a mechanism involving photo-oxidation of Pu (III, IV).A dominant proportion of the remobilised Pu (III, IV) in solution is anionic with a molecular weight1000 daltons, probably in the form of an organic complex. Remobilised Pu (V, VI) is mainly in true solution in variously charged forms. Addition of natural colloidal organic carbon (COC) to river water increased the level of labile Pu (III, IV) remobilisation. The effect can be described by two competing equilibria in which labile Pu (III, IV) (a) is complexed by COC, and (b) is adsorbed by the sediment. The same additions of COC reduced the level of Pu (V, VI) remobilisation, either through its action as a reducing agent or through the indirect effect of associated pH changes. Increasing the carbonate alkalinity (NaHCO₃) in river water decreases the remobilisation of both Pu (III, IV) and Pu (V, VI).     

Gamma radioactivity in the Iberian Marine environment closest to the NEA dumping site

The distributions of caesium-137 and some naturally occurring gamma-emitters in a range of environmental samples, collected along the north-west Iberian coastline during April 1984, are presented. Samples, including surface waters, algae, sediments and fish, have been analyzed to establish accurate baselines for that region of the continental shelf closest to the NEA dumping site. Results indicate that caesium-137 levels were a factor of three lower than those typical of waters off the west coast of Ireland and are consistent with those expected from global fallout prior to the Chernobyl accident. The mean caesium-137 concentration in sea water at six well-separated stations near the coast was 3·85 ± 0·19 Bq m⁻³, whilst caesium-137 levels in widely consumed species of fish were in the range 1·1–6·2 Bq kg⁻¹ (dry wt). It is estimated that caesium-137, through one year's ingestion of fish and shellfish, generates a collective dose equivalent commitment to the adult Galician population of 0·78 man-Sv, which is approximately 3% of the total annula collective dose equivalent from non-medical sources of radiation.     

The distribution and inventory of fallout plutonium in sediments of the Ligurian Sea near La Spezia,Italy

Pu concentrations in surface sediments of the Ligurian Sea are about ten times higher than in adjacent river sediments and are highly correlated with sediment porosities. The integrated inventory of ^239,240Pu in a sediment core is calculated to be 3·5 mCi km^?2, nearly twice the average input from fallout at these latitudes, apparently because Pu is removed from seawater by particle scavenging.The sedimentation rate is calculated from the depth of the ^239,240Pu maximum to be 0·52 ± 0·06 cmy^?1.     

99Tc in the sub-arctic food chain Lichen-Reindeer-man

The deposition, migration and annual variations of ⁹⁹Tc fallout in carpets of lichen collected during the period 1956–1981 have been investigated. The transfer of ⁹⁹Tc to reindeer and man has also been studied. Technetium showed a shorter mean residence time than ¹³⁷Cs in the lichen carpet. The activity ratio ⁹⁹Tc/¹³⁷Cs was generally lower than the theoretical fission ratio of 1·43 × 10⁻⁴. The maximum concentration of ⁹⁹Tc in lichens occurred in 1967 (ca. 60 mBq kg⁻¹) but in 1975 higher values were found than would have been predicted from fallout. The average depth integrated concentration of ⁹⁹Tc at 62·3°N, 12·4° E in 1972 was 540 ± 100 mBq m⁻². The studies of reindeer tissues show that technetium has a short mean residence time in the muscle tissues (ca. 5 days) and is not accumulated like ¹³⁷Cs. The committed dose equivalent from ⁹⁹Tc to the local Lapp population engaged in reindeer breeding is negligible.     

Carbon-14 discharges from the nuclear fuel cycle: 2. Local effects

Environemtnal ¹⁴C levels around various types of nuclear installations within the UK have been monitored during recent years. Enhanced ¹⁴C levels have been detected around both the nuclear fuel reprocessing plant as Sellafield and the thermal nuclear power station complex at Hunterston. From these measurements, the radiological impact of the ¹⁴C discharges on the local population is assessed. It is conservatively estimated that the ¹⁴CO₂ emissions from Sellafield between 1952 and 1985 could have delivered an 8·4 man Sv collective effective dose equivalent commitment to the population living within 40 km of the site. The maximum possible collective dose to the population within 15 km of Hunterston in 1984 was 15 × 10⁻³ man Sv. Conservative estimates of maximum annual effective dose equivalents to individuals around Sellafield and Hunterston are 0·2 mSv (in 1982) and 12 μSv (in 1984), respectively. These dose levels do not exceed the limits recommended by ICRP but the former value clearly indicates that, for the larger discharges at least, consideration and optimisation of ¹⁴C releases are fully justified. The same ¹⁴C measurements are also used to test the validity of two atmospheric dispersion models, the Gaussian plume and the so-called ‘hyperbolic’ models. The former is excellent in predicting downwind ¹⁴C levels around Hunterston but is unsatisfactory when applied to Sellafield, whereas the latter proves reliable at both sites. Further investigations suggest that the Gaussian plume model's poor performance at Sellafield can be explained by inaccurate input data.     

Fallout in the New York metropolitan area following the chernobyl accident

In the metropolitan New York area, maximum concentrations in air of radioactive aerosol and gaseous debris from the Chernobyl accident of April 1986 were much lower than those measured in Europe. The observed maxima were: for gaseous ¹³¹I, 23mBq m⁻³; for aerosol samples, 20mBq m⁻³ of ¹³¹I and 9·mBq m⁻³ of ¹³⁷Cs. The data suggest that little gas-to-particle transformation of iodine occurred during transport of the radioactive cloud from the Ukraine to New York. The ratios of ¹⁰³Ru and other refractories to ¹³⁷Cs were low in the first debris sampled, debris which probably was emitted from Chernobyl in late April during the early stages of the accident. In subsequent samples these ratios were higher, presumably because debris from the later, hotter stages of the fire had reached our sampling sites. A significant fraction (25–40%) of the deposition of ¹³¹I and ¹³⁷Cs into our samplers and on grass was by dry deposition. The total deposition of Chernobyl ¹³⁷Cs in the area was <1% of that already present in the soil from fallout from past nuclear weapon tests. The highest concentration of ¹³¹I measured in fresh milk was about 1.5 B1 liter⁻¹, <0.1% of the US action level. The dose to the thyroid of a six-month-old infant who had fresh milk as a sole food source would be about 70 μGy (7 mrad).     

Transfer of 241Am and 237Pu from euphausiid moults to a carbonate-rich marine sediment

Concentrations of ²⁴¹Am and ²³⁷Pu adsorbed onto moulted exoskeletons from the euphausiid Megancytiphanes norvegica decreased exponentially with 50% retention times of 3–7 d when moults were incubated in filtered seawater with small amounts of a carbonate-rich sediment. Over 95% of sediment weight was present as < 43 μm silt particles and 91 ± 4% of radioactivity lost from moults was recovered in this size fraction. Adsorption of both actinides (atoms μm⁻²) was greatest in the medium-fine sand fraction which had the highest carbonate content. These particles constituted <0·4% of total sediment dry weight but their reactivity (atoms μm⁻² surface: atoms μm⁻³ in solution) was 10³–10⁴ times higher than similar quotients for <43 μm particles. The enrichment shows that non-homogeneous distributions may arise between particle types when actinides such as ²⁴¹Am and ²³⁷Pu sorbed to surfaces of organic particles are transferred to sediments.     

Plant uptake of neptunium-237 and technetium-99 under field conditions

Plant uptake of ⁹⁹Tc freshly added to soils was compared with uptake of ⁹⁹Tc ‘aged’ in soil for more than a decade. A combination of alkaline soil and freshly added ⁹⁹Tc resulted in elevated uptake into radish foliage (plant/soil concentration ratios ranged from 37 to 46). Neptunium-237 was freshly added to all soils. Neptunium uptake via plant roots into foliage was strongly affected by soil pH. Neptunium uptake was greatest from acidic soils. The observed plant/soil concentration ratios for ²³⁷Np under field conditions were approximately 10⁻² from acidic soils (pH 5·6–5·7) and were comparable to field concentration ratios for ²³⁹Pu, that is 10⁻³, from a basic soil (pH 7·5).