D. Copplestone

The use of sediment cores from stable and developing salt marshes to reconstruct historical contamination profiles in the Mersey Estuary, UK

Abstract Depth-profiled sediment cores from two marshes in the Mersey Estuary were analysed for concentrations of 137Cs, 238Pu, 239,240Pu, 241Am, As, Cr, Cu, Pb, Hg and Zn. Mersey sediments contain three diagnostic and persistent chemical species arising from either a unique, or a dominant, source – 137Cs, Hg and DDT. Dating of features in these cores has been completed using up to four benchmark events identifiable from these chemical species – the initial expansion of the chemical industry, commencement of DDT manufacture, initial appearance of radionuclides from a reprocessing site in NW England, and the introduction of new technology to reduce mercury discharges. The sediment pollutant profiles depend on the rate of sediment accumulation but clearly record the historical increase in discharges of metals to the environment between the mid-19th and 20th centuries. They also reflect recent regulatory and technological efforts to minimise estuarine contamination and the discontinuation of specific manufacturing and refining processes. ©

The organochlorine contamination history of the Mersey estuary, UK, revealed by analysis of sediment cores from salt marshes

Sediment profiles in the Banks, Ince and Widnes Warth salt marshes in Northwest England contain a mappable record of historic pollution. For persistent organochlorine compounds this stretches back over 90 years. The PCB and HCH profiles can be successfully rationalised by dating methods, and they can be related to the dates of initial production and subsequent withdrawal from use of these chemicals as a result of restrictive environmental legislation. HCB has a more complex pollution profile as it has been manufactured in Northwest England, both deliberately as a pesticide and accidentally as a by-product of several chlorination processes, dating back to the start of the 20th century. The concentrations of degradation products of DDT are relatively constant through the sediment profile and are dominated by op- and pp-DDD with only minor contributions from the most toxic species, pp-DDT. The quantities of these compounds resident in the reservoir of pollutants under these marshes have been calculated, and have fallen progressively in the last 30-50 years.

Radionuclide behaviour and transport in a coniferous woodland ecosystem:vegetation, invertebrates and wood mice, Apodemus sylvaticus

Activity concentrations of radionuclides (134Cs, 137Cs, 238Pu, 239 + 240Pu and 241Am) were measured in vegetation, invertebrates and wood mice, Apodemus sylvaticus, collected in Lady Wood, a coniferous woodland in the vicinity of the British Nuclear Fuels reprocessing plant at Sellafield, Cumbria, UK. Vegetation was of low diversity and biomass with activity concentrations ranging from 1 to 5 Bq kg-1 (134Cs), 0.3-0.5 Bq kg-1 (238Pu), 0.8-8 Bq kg-1 (239 + 240Pu), and 0.6-16 Bq kg-1 (241Am), dry wt. Caesium-137 activity concentrations were high compared to the reference site in Cheshire, varying between 65 and 280 Bq kg-1. Marked inter-specific and temporal differences in radionuclide activity concentrations were recorded for invertebrate populations. Caesium-137, 238Pu, 239 + 240Pu and 241Am activity concentrations in detritivorous invertebrates were consistently higher than in all other invertebrate groups reflecting contamination of the leaf litter. The activity concentrations in detritivores increased during the autumn and winter, reflecting changes in diet as food sources varied throughout the year. Activity concentrations in invertebrates caught in Lady Wood were generally an order of magnitude higher than for the reference site. Activity concentrations in wood mice varied between 7 and 150 Bq kg-1 (137Cs), 0.1-0.3 Bq kg-1 (238Pu), 0.1-0.6 Bq kg-1 (239 + 240Pu) and 0.2-0.4 Bq kg-1 (241Am). There were clear differences in the activity concentration of 137Cs (P < 0.01), 239 + 240Pu (P < 0.05) and 241Am (P < 0.05) in animals caught in Lady Wood compared to the reference site. However, the activity concentrations for 238Pu were similar at both sites, reflecting a low gastrointestinal transfer. Seasonal variation in activity concentrations was observed for 137Cs, 238Pu and 241Am. This variation is attributed to changes in the age structure of the population and diet throughout the year.

Behaviour and transport of radionuclides in soil and vegetation of a sand dune ecosystem

A sand dune ecosystem in the vicinity of the British Nuclear Fuels reprocessing plant at Sellafield, Cumbria, UK was used to examine the spatial, temporal and depth distributions of 134Cs, 137Cs, 238Pu, 239 + 240Pu and 241Am in soil and in two species of vegetation (Festuca rubra, Ammophila arenaria). Core samples showed evidence of the accumulation of radionuclides derived mainly from sea-to-land transfer. Accumulated deposits of radioactivity (0-0.1 m) lie within the range: 1.1-3.4 Bq kg-1 (134Cs), 260-440 Bq kg-1 (137Cs), 31-40 Bq kg-1 (238Pu), 150-215 Bq kg-1 (239 + 240Pu) and 190-240 Bq kg-1 (241Am). Soil profiles showed greater activity concentrations in their deeper regions and this is attributed to leaching of radionuclides in percolating drainage water accentuated by the coarse texture, low organic matter and clay mineral content of coastal sands. Radionuclide activity concentrations in F. rubra and A. arenaria were similar, in the ranges 20-70 Bq kg-1 (137Cs), 1-5 Bq kg-1 (238Pu), 10-30 Bq kg-1 (239 + 240Pu) and 10-65 Bq kg-1 (241Am). Clear temporal and spatial variations were observed in both species of vegetation, reflecting the weather conditions antecedent to the sampling period and the influence of sea-to-land transfer. Concentration ratios (vegetation:soil) for activity concentrations in the two species were similar, in the ranges: 0.05-0.14 (137Cs), 0.025-0.097 (238Pu), 0.022-0.057 (239 + 240Pu) and 0.025-0.212 (241Am).

Effect of forest edges on deposition of radioactive aerosols

Abstract The possible enhancement of aerosol deposition at forest edges was investigated in a wind tunnel and in the field. The wind tunnel study was carried out using 0.82xa0μm mass median aerodynamic diameter uranium particles and a composite canopy of rye grass and spruce saplings. The field study was undertaken at a coniferous woodland near to BNFL Sellafield, Cumbria, UK. Two transects were set through the woodland to determine the influence of the forest edge on atmospheric deposition of radionuclides released under authorisation from the Sellafield site. Results from the wind tunnel study showed that the deposition flux of uranium particles decreased with distance downwind from the grass–tree edge towards the interior of the canopy. The deposition flux at the edge was maximal at about 4×10−7xa0μg of Uxa0cm−2xa0s−1. This was 3 times higher than that observed over grass where a constant flux of about 1.32×10−7xa0μg of Uxa0cm−2xa0s−1 occurred. Results from the field study showed a clear influence of the forest edge on the atmospheric deposition of 241Am and 137Cs. Activity depositions of around 4750 and 230xa0Bqm−2 for 137Cs and 241Am, respectively, were measured in front of the woodland. Activity deposition inside the forest edge, however, rose to levels of between 20,200 and 50,900xa0Bqxa0m−2 and 1100 and 3200xa0Bqxa0m−2 for 137Cs and 241Am, respectively, depending upon the transect. Similar activity concentrations were measured in the pasture to the front and behind Lady Wood. Results from these studies corroborate those obtained from various studies on air pollutants including radionuclides. This underlines the importance of deposition at the edge of forests and its contribution to the overall canopy deposition. The edge effect is therefore an important factor that should be considered in the assessment of fallout impact, whether this is to be made by either direct sampling or by modelling.

Radionuclide Behaviour and Transport in a Coniferous Woodland Ecosystem: The Distribution of Radionuclides in Soil and Leaf Litter

A coniferous woodland in the vicinity of theBritish Nuclear Fuels reprocessing plant atSellafield, Cumbria, was used to examine the spatial,temporal and depth distribution of 134Cs,137Cs, 238Pu, 239+240Pu and 241Amin soil and leaf litter. All the radionuclides, withthe exception of 134Cs, showed a consistent fallin accumulated soil and litter deposits withincreasing distance from the woodland edge nearest toSellafield. 137Cs levels in soil declined from 53to 28 kBq m-2, 239+240Pu from 5.5 to 3.6 kBqm-2 and 241Am from 2.9 to 1.1 kBq m-2within 100 m of the forest edge. This decline isattributed to greater deposition occurring at theleading edge of the woodland. The uniform depositionpattern of 134Cs in soil is consistent with thehypothesis that, at the time of sampling, thesedeposits derived largely from wet deposition duringpassage of the Chernobyl plume over Cumbria in May1986. Results for the leaf litter indicate a similarspatial distribution to that observed in soil.Radionuclide concentrations were also similar but thisis not attributable to adventitious soil contaminationbecause significant differences between isotopicratios of 134Cs:137Cs and 238Pu:239+240Pu imply that the contamination on leaflitter is of more recent origin than that in soils.

Recent trends in organochlorine residues in mussels (Mytilus edulis) from the Mersey Estuary

Blue mussels (Mytilus edulis) taken from several sites in the Mersey Estuary, an urban-industrial water body in NW England, have been analyzed for residues of the persistent organochlorines, DDT, PCB congeners nos. 28, 52, 101, 118, 138, 153 and 180 (ICES7), and alpha-MHCH (alpha-methyl hexachlorocyclohexane). The concentration range for sigmaPCB (ICES7) was 13.9-34.9 microg kg(-1) in 1994 compared with 9.6-31.9 microg kg(-1) in 1998, whilst the equivalent concentrations of sigmaDDT were 8.9-32.4 microg kg(-1) and 4.5-16.8 microg kg(-1), respectively. The concentration of alpha-MHCH, an organochlorine largely restricted to the Mersey Estuary, was 1.2-11 microg kg(-1) in 1994 and 0.3-1.3 microg kg(-1) in 1998. At both sampling dates the inner estuary sites of Rock Ferry and Egremont were more contaminated than the outer estuary sites of New Brighton. Dove Point and Caldy Blacks. The lower concentrations of organochlorines in mussels in 1998 compared with 1994 are thought to be early evidence of significant improvements in water quality derived from major capital investment in the treatment of industrial effluents and sewage wastewater, linked to a combination of stricter legislative controls and the environmental benefits from the adoption of new, clean technologies in manufacturing.

Generic performance assessment for a deep repository for low and intermediate level waste in the UK—a case study in assessing radiological impacts on the natural environment

Concentrations of radionuclides in soil and surface water, taken from a generic performance assessment of a repository for low and intermediate level radioactive waste, assumed to be located in the UK, have been used as the basis for a case study in assessing radiological impacts on the natural environment. Simplified descriptions of the terrestrial and aquatic ecosystem types likely to be impacted have been developed. A scoping assessment has identified (226)Ra, (210)Po, (234)U, (230)Th and (238)U as having the highest potential for impact, with doses from internally incorporated alpha emitters as being potentially of particular importance. These nuclides, together with (36)Cl and (129)I (which have proved to be of importance in radiological risk assessments for humans) were included in a more detailed dose assessment. A basic methodology for dose assessment of ecosystems is described, and has been applied for the defined impacted ecosystems. Paucity of published data on concentration factors prevented a more detailed assessment for terrestrial ecosystems. For the aquatic ecosystem, a more detailed assessment was possible and highest calculated absorbed dose rates (weighted for the likely higher biological effectiveness of alpha radiation) were about 6.5 microGy h(-1). We conclude that harm to the impacted ecosystems is unlikely and make the observation that the lack of concentration factor or transfer factor data for a sufficiently wide range of species, ecosystems and nuclides appears to be the principal obstacle to establishing a comprehensive framework for the application of radiological protection to ecosystems.

Environmental effects of radionuclides - observations on natural ecosystems

To better quantify risk to non-human species from exposure to environmental radioactivity, understanding of the behaviour of radionuclides in the biosphere needs to be increased. This study outlines current thinking on ecological risk assessment (ERA) methodology and applies the indicator species or critical groups approach to biota inhabiting a semi-natural coniferous woodland contaminated with the radionuclides 137Cs, 238Pu, 239+240Pu and 241Am. The majority of these radionuclides originate from routine aerial emissions from the nuclear fuel reprocessing plant at BNFL, Sellafield, Cumbria, UK. Radionuclide activity concentrations have been determined in biota from the woodland and estimates of absorbed dose rates (mGy d(-1)) have been calculated using the dosimetric models outlined. Dose rates to the key indicator species, Oniscus asellus, Carabus violaceous and Apodemus sylvaticus (detritivorous invertebrate, predatory invertebrate and the granivorous wood mouse) have been determined at 3.0 x 10(-3) mGy d(-1), 2.2 x 10(-3) mGy d(-1) and 1.0 x 10(-3) mGy d(-1) respectively. The values are at least three orders of magnitude lower than the 1 mGy d(-1) level below which no observable effects on populations in a terrestrial ecosystem are thought to occur. Limitations of this approach are discussed.

Quantifying 137Cs aggregated transfer coefficients in a semi-natural woodland ecosystem adjacent to a nuclear reprocessing facility

Radiocaesium (137Cs) activity concentrations and aggregated transfer factors (Tag values) were calculated for vascular plants, fungal fruiting bodies and invertebrates in a semi-natural Picea sitchensis woodland (Lady Wood) adjacent to the British Nuclear Fuels plc. reprocessing facility at Sellafield, Cumbria, UK. The Tag values for vascular plants ranged from 7.1 x 10(-4) - 1.9 x 10(-2) m2 kg(-1), the maximum value being for Pteridium aquilinum. Fungal fruiting bodies had higher Tag values (1.9 x 10(-3) - 1.8 x 10(-1) m2 kg(-1)) than vascular plants, with a maximum value for Mycena galericulata. None of the activity concentrations for edible foodstuffs collected within this study (fungi and berries) exceeded the EC recommended limits of 137Cs in foodstuffs grown within the UK. The invertebrate community sampled during the study had Tag values ranging from 3.4 x 10(-4) to 1.3 x 10(-2) m2 kg(-1). There were no systematic differences in 137Cs activity concentration between invertebrate guilds, or between seasonal cohorts within guilds. The invertebrates in Lady Wood were exposed to a dose from 137Cs (internal gamma + beta and external gamma) ranging between 4.37 x 10(-4) and 6.40 x 10(-4) mGy day(-1). Including dose from radionuclides other than 137Cs and accounting for uncertainties due to the relative biological effectiveness of differing radionuclides could increase total dose by approximately an order of magnitude. These dose rates are at least three orders of magnitude lower than the 1 mGy d(-1) level at which harm may be caused to terrestrial biota, hence the risk to the invertebrate community from the effects of ionising radiation in Lady Wood is low.