Esk Estuary Research Articles

Kinetic reactive transport explains distinct subsurface deposition patterns of pollutants in sediments. The case of the Sellafield-derived 236U, 137Cs and 239,240Pu in the Esk Estuary, UK

The kinetics of the uptake of pollutants by solids in sediments interacts with transitional eddy diffusivity in the pore fluid, leading to different depth-distribution patterns. This work aims to gain insights into the still poorly understood behaviour in the marine environment of the anthropogenic 236U, a recently postulated tracer of water masses. It is hypothesized that the transition from mobile U(VI) to highly particle-reactive U(IV) in the anoxic zone of the sediment produces a subsurface deposition pattern. A novel numerical model for kinetic reactive transport in sediments, which merges diagenetic processes for transport and box models for the uptake, is used for concept demonstration. It is applied to synthetic environments with high eddy diffusivity to obtain the singular depth-distribution patterns of pulsed inputs of tracers that mimic the anthropogenic 239,240Pu, 137Cs, and 236U. While the first is retained in the upper cm, the second shows an exponential penetration pattern over few cm, and 236U is deposited with a Gaussian-like pattern centred below the transition to the anoxic zone. These patterns are then merged into a diagenetic model to compute the depth distribution at decadal or centennial scales of dissolved and particle-bound inputs of these radiotracers. It is successfully applied to a real case using literature data for a sediment core from the Esk Estuary, UK, affected by radioactive releases from the Sellafield nuclear reprocessing plant. This work provides insight into until now poorly understood field data and provides a novel view of broad implications in the study of the behaviour of pollutants in surficial aquatic sediments.

Time-Integrated Bioavailability Proxy for Actinides in a Contaminated Estuary.

Actinides accumulate within aquatic biota in concentrations several orders of magnitude higher than in the seawater [the concentration factor (CF)], presenting an elevated radiological and biotoxicological risk to human consumers. CFs currently vary widely for the same radionuclide and species, which limits the accuracy of the modeled radiation dose to the public through seafood consumption. We propose that CFs will show less dispersion if calculated using a time-integrated measure of the labile (bioavailable) fraction instead of a specific spot sample of bulk water. Herein, we assess recently developed configurations of the diffusive gradients in thin films (DGT) sampling technique to provide a more accurate predictor for the bioaccumulation of uranium, plutonium, and americium within the biota of the Sellafield-impacted Esk Estuary (UK). We complement DGT data with the cross-flow ultrafiltration of bulk seawater to assess the DGT-labile fraction versus the bulk concentration. Sequential elution of Fucus vesiculosis reveals preferential internalization and strong intracellular binding of less particle-reactive uranium. We find significant variations between CF values in biota calculated using a spot sample versus using DGT, which suggest an underestimation of the CF by spot sampling in some cases. We therefore recommend a revision of CF values using time-integrated bioavailability proxies.

Plutonium mobilization from contaminated estuarine sediments, Esk Estuary (UK)

Since 1952, liquid radioactive effluent containing238-242Pu, 241Am, 237Np, 137Cs, and 99Tc has been released with authorization from the Sellafield nuclear complex (UK) into the Irish Sea. This represents the largest source of plutonium (Pu) discharged in all western Europe, with 276 kg having been released. In the Eastern Irish Sea, the majority of the transuranic activity has settled into an area of sediments (Mudpatch) located off the Cumbrian coast. Radionuclides from the Mudpatch have been re-dispersed via particulate transport in fine-grained estuarine and intertidal sediments to the North-East Irish Sea, including the intertidal saltmarsh located at the mouth of the Esk Estuary. Saltmarshes are highly dynamic systems which are vulnerable to external agents (sea level change, erosion, sediment supply, and freshwater inputs), and their stability remains uncertain under current sea level rise projections and possible increases in storm activity. In this work, we examined factors affecting Pu mobility in contaminated sediments collected from the Esk Estuary by conducting leaching experiments under both anoxic and oxic conditions. Leaching experiments were conducted over a 9-month period and were periodically sampled to determine solution phase Pu via multicollector-inductively coupled plasma-mass spectrometry (MC-ICP-MS), and to measure redox indicators (Eh, pH and extractable Fe(II)). Microbial community composition was also characterized in the sediments, and at the beginning and end of the anoxic/oxic experiments. Results show that: 1) Pu leaching is about three times greater in solutions leached under anoxic conditions compared to oxic conditions, 2) the sediment slurry microbial communities shift as conditions change from anoxic to oxic, 3) Pu leaching is enhanced in the shallow sediments (0–10 cm depth), and 4) the magnitude of Pu leached from sediments is not correlated with total Pu, indicating that the biogeochemistry of sediment-associated Pu is spatially heterogeneous. These findings provide constraints on the stability of redox sensitive Pu in biogeochemically dynamic/transient environments on a timescale of months and suggests that anoxic conditions can enhance Pu mobility in estuarine systems.

Bioavailable actinide fluxes to the Irish Sea from Sellafield-labelled sediments

Nuclear discharges to the oceans have given rise to significant accumulations of radionuclides in sediments which can later remobilise back into the water column. A continuing supply of radionuclides to aquatic organisms and the human food chain can therefore exist, despite the absence of ongoing nuclear discharges. Radionuclide remobilisation from sediment is consequently a critical component of the modelled radiation dose to the public. However, radionuclide remobilisation fluxes from contaminated marine sediments have never been quantitatively determined in-situ to provide a valid assessment of the issue. Here, we combine recent advances in the Diffusive Gradients in Thin Films (DGT) sampling technique with ultrasensitive measurement by accelerator mass spectrometry (AMS) to calculate the remobilisation fluxes of plutonium, americium and uranium isotopes from the Esk Estuary sediments (UK), which have accumulated historic discharges from the Sellafield nuclear reprocessing facility. Isotopic evidence indicates the local biota are accumulating remobilised plutonium and demonstrates the DGT technique as a valid bioavailability proxy, which more accurately reflects the elemental fractionation of the actinides in the biota than traditional bulk water sampling. These results provide a fundamental evaluation of the re-incorporation of bioavailable actinides into the biosphere from sediment reservoirs. We therefore anticipate this work will provide a tool and point of reference to improve radiation dose modelling and contribute insight for other environmental projects, such as the near-surface and deep disposal of nuclear waste.

Plutonium Mobilization from Contaminated Estuary Sediments, Esk Estuary (UK)

Plutonium Mobilization from Contaminated Estuary Sediments, Esk Estuary (UK)

Controls on anthropogenic radionuclide distribution in the Sellafield-impacted Eastern Irish Sea

Understanding anthropogenic radionuclide biogeochemistry and mobility in natural systems is key to improving the management of radioactively contaminated environments and radioactive wastes. Here, we describe the contemporary depth distribution and phase partitioning of 137Cs, Pu, and 241Am in two sediment cores taken from the Irish Sea (Site 1: the Irish Sea Mudpatch; Site 2: the Esk Estuary). Both sites are located ~10 km from the Sellafield nuclear site. Low-level aqueous radioactive waste has been discharged from the Sellafield site into the Irish Sea for >50 y. We compare the depth distribution of the radionuclides at each site to trends in sediment and porewater redox chemistry, using trace element abundance, microbial ecology, and sequential extractions, to better understand the relative importance of sediment biogeochemistry vs. physical controls on radionuclide distribution/post-depositional mobility in the sediments. We highlight that the distribution of 137Cs, Pu, and 241Am at both sites is largely controlled by physical mixing of the sediments, physical transport processes, and sediment accumulation. Interestingly, at the Esk Estuary, microbially-mediated redox processes (considered for Pu) do not appear to offer significant controls on Pu distribution, even over decadal timescales. We also highlight that the Irish Sea Mudpatch likely still acts as a source of historical pollution to other areas in the Irish Sea, despite ever decreasing levels of waste output from the Sellafield site.

Geochemical association of Pu and Am in selected host-phases of contaminated soils from the UK and their susceptibility to chemical and microbiological leaching

Understanding the biogeochemical behaviour and potential mobility of actinides in soils and groundwater is vital for developing remediation and management strategies for radionuclide-contaminated land. Pu is known to have a high Kd in soils and sediments, however remobilization of low concentrations of Pu remains a concern. Here, some of the physicochemical properties of Pu and the co-contaminant, Am, are investigated in contaminated soils from Aldermaston, Berkshire, UK, and the Esk Estuary, Cumbria, UK, to determine their potential mobility. Sequential extraction techniques were used to examine the host-phases of the actinides in these soils and their susceptibility to microbiological leaching was investigated using acidophilic sulphur-oxidising bacteria. Sequential extractions found the majority of 239,240Pu associated with the highly refractory residual phase in both the Aldermaston (63.8–85.5 %) and Esk Estuary (91.9–94.5%) soils. The 241Am was distributed across multiple phases including the reducible oxide (26.1–40.0%), organic (45.6–63.6%) and residual fractions (1.9–11.1%). Plutonium proved largely resistant to leaching from microbially-produced sulphuric acid, with a maximum 0.18% leached into solution, although up to 12.5% of the 241Am was leached under the same conditions. If Pu was present as distinct oxide particles in the soil, then 241Am, a decay product of Pu, would be expected to be physically retained in the particle. The differences in geochemical association and bioleachability of the two actinides suggest that this is not the case and hence, that significant Pu is not present as distinct particles. These data suggest the majority of Pu in the contaminated soils studied is highly recalcitrant to geochemical changes and is likely to remain immobile over significant time periods, even when challenged with aggressive “bioleaching” bacteria.

Natural Variability and Anthropogenic Effects on the Morphodynamics of a Beach–Dune System at Montrose Bay, Scotland

MILNE, F.D.; DONG, P., and DAVIDSON, M., 2012. Natural variability and anthropogenic effects on the morphodynamics of a beach–dune system at Montrose Bay, Scotland.Beach–dune systems are valuable geomorphic assets providing a buffer between the coastal hinterland and the sea. Sustained coastal erosion can diminish the protective capability of the beach–dune system with potentially negative implications for coastal amenities, infrastructure, ecology, and archaeology. To develop suitable management solutions in response to erosion, it is necessary to ascertain spatiotemporal variations in the processes that affect site-specific coastal morphology. This study examines a beach–dune system at Montrose Bay in eastern Scotland that is undergoing severe erosion, threatening the current layout of the Montrose Medal Golf Course. Sediment eroded from the golf course frontage is deposited at the northern end of the bay where contemporaneous accretion has occurred. Analysis of sediment transport rates, time-series aerial photography, and historical maps indicate that the current spatial distribution of erosion and accretion at Montrose Bay is likely due to a strengthening of northerly drift, driven by wave–climate change during the 1980s. This natural variability was examined further through assessment of earlier changes in coastal morphology apparent in historical mapping and from archaeological evidence of shoreline change reflecting the temporal dynamism of soft sedimentary coasts. The removal of sediment dredged from the South Esk estuary in the closed coastal system is shown to be a major anthropogenic influence on the beach–dune system in recent decades based on a simple quantitative analysis of dune erosion due to removal of beach sediments during dredging operations.

Temporal record of Pu isotopes in inter-tidal sediments from the northeastern Irish Sea

A depth profile of 239Pu and 240Pu specific activities and isotope ratios was determined in an inter-tidal sediment core from the Esk Estuary in the northeastern Irish Sea. The study site has been impacted with plutonium through routine radionuclide discharges from the Sellafield nuclear reprocessing plant in Cumbria, NW England. A pronounced sub-surface maximum of ~ 10 kBq kg -1 was observed for 239 + 240 Pu, corresponding to the peak in Pu discharge from Sellafield in 1973, with a decreasing trend with depth down to ~ 0.04 kBq kg -1 in the deeper layers. The depth profile of 239 + 240 Pu specific activities together with results from gamma-ray spectrometry for 137Cs and 241Am was compared with reported releases from the Sellafield plant in order to estimate a reliable sediment chronology. The upper layers (1992 onwards) showed higher 239 + 240 Pu specific activities than would be expected from the direct input of annual Sellafield discharges, indicating that the main input of Pu is from the time-integrated contaminated mud patch of the northeastern Irish Sea. The 240Pu/ 239Pu atom ratios ranged from ~ 0.03 in the deepest layers to > 0.20 in the sub-surface layers with an activity-weighted average of 0.181. The decreasing 240Pu/ 239Pu atom ratio with depth reflects the changing nature of operations at the Sellafield plant from weapons-grade Pu production to reprocessing spent nuclear fuel with higher burn-up times in the late 1950s. In addition, recent annual 240Pu/ 239Pu atom ratios in winkles collected during 2003–2008 from three stations along the Cumbrian coastline showed no significant spatial or temporal differences with an overall average of 0.204, which supports the hypothesis of diluted Pu input from the contaminated mud patch.

Temporal changes in gamma dose rates in the Esk Estuary, UK

Over the last 30 years there has been a reduction in the radioactive discharges from the UK's Sellafield site. Radionuclide activity concentrations in the environment around Sellafield have declined as a result. However, routine monitoring results from the nearby Esk Estuary show a less clear trend, with fluctuations in gamma dose rate measurements being reported from year to year. A comprehensive survey (n = 576) of gamma dose rates in the Esk Estuary was undertaken in 2007 and the data compared to a similar survey carried out in 1989. There was a highly statistically significant decrease in the external gamma dose rates within the Esk Estuary between 1989 and 2007. The measured total gamma dose rate range in 2007 was 0.064 - 0.235Gy h −1 with a mean of 0.123Gy h −1 . This equates to a maximum exposure of 0.200Sv h −1 . There was no evidence of large-scale sediment redistribution under current conditions. However, there was limited evidence to suggest that part of the reason for the reduction in measured dose rates was the burial of contaminated sediment deposits by uncontaminated sediments transported by tidal processes.

The launching of the River Esk bridge, UK

The River Esk bridge carries the southbound carriageway of the M6 motorway over the River Esk estuary and forms part of the recently constructed M6 Carlisle to Guards Mill motorway extension, which provides the missing link in the motorway network between England and Scotland. The bridge is a 180 m long four-span steel composite viaduct. Due to site constraints the most economical and practical method of construction was to launch the steelwork into position rather than to lift the steelwork in by crane. The bridge steelwork, weighing over 800 t, was assembled on the northern approach to the bridge and launched southwards over the River Esk estuary. This paper demonstrates that the design and construction of a launched bridge can be significantly more complicated than the design of a comparable bridge that is constructed using conventional methods and that there are many more load cases and construction details to consider. This paper covers the approach for carrying out the analysis, design, detailing and construction of the structure and focuses specifically on the key issues relating to launching steelwork.

Identification and characterisation of radioactive particles in salt marsh sediments

Radionuclides from authorized low level radioactive effluent discharges from the nuclear fuel reprocessing plant at Sellafield, UK, are present in the Irish Sea sediments. The distribution of radionuclides in salt marsh sediment profiles can be related to the discharge history from Sellafield. Radioactive particles, from the intertidal salt marsh sediments in the Esk estuary (10 km from Sellafield), have been isolated and investigated. Autoradiography and heavy liquid density separation were used to find and isolate these particles. Scanning electron microscopy, combined with energy dispersive X-ray analysis (SEM-EDX), was used to obtain information on the morphology and elemental composition of the particles, and alpha spectrometry for radionuclide composition. Particles are typically 1 — 20 μm size. Elemental analysis suggests that they are composed mainly of uranium. Alpha spectrometry shows that they have been irradiated, and transuranium nuclides (Pu, Am, Cm) can be identified in them.

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

AbstractNuclear 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.

An investigation into technetium binding in sediments

Coastal environments with reducing waters and/or sediments represent potential sinks for 99Tc discharged to sea. Here, we have examined estuarine sediments from four geochemically distinct locations that have been exposed to 99Tc discharged from Sellafield. Both the relative uptake and the operationally defined sediment “component” that holds the Tc were investigated in order to establish whether particular biogeochemical processes are predominately responsible for reducing and binding Tc in sediments. Despite the artefacts that can pose problems for sequential extractions, this scheme [Int. J. Environ. Anal. Chem. 51 (1993) 187] appears to be robust with regard to Tc. The results show that relative uptake of Tc varied greatly between the sites, with the highest occurring at an almost permanently anoxic fjord (Mariager Fjord, Denmark), followed by a brackish, seasonally eutrophic fjord (Roskilde Fjord, Denmark), then a sub-oxic salt marsh (which receives particle bound radionuclides from a more reducing mud patch; Esk Estuary, UK) and finally sulfidic and iron-reducing muddy sandy sediments (Needle's Eye, Solway Firth, Scotland). High relative uptake at the fjords was explained by the greater mixing of Tc-labelled oxic seawater into the part of the system where reduction of TcO 4 − was possible. Uptake at Mariager Fjord was higher than at Roskilde Fjord, reflecting the highly reducing geochemical conditions in the water body. Low uptake at Needle's Eye may be related to the speciation of technetium at this site as the sequential extraction data suggest that Tc is associated with the carbonate phase here. Tc carbonates are largely soluble, and this is the first observation of Tc association with carbonate fractions in the natural environment. The other three sites showed that organic matter, in conjunction with reducing conditions, was very important for binding and retaining Tc in sediments. The specific role of sulfides in controlling Tc retention in sediments was unclear because sulfides and organic matter are leached simultaneously in the sequential extraction scheme we applied, but there was evidence that Tc was not associated with acid-volatile iron monosulfides.

Anthropogenic radionuclides in tide-washed pastures bordering the Irish Sea coast of England and Wales

The activity concentrations of 137Cs,238 Pu, 239,240Pu and 241Am were measured in root mat and vegetation samples collected from tide washed pastures in 17 estuaries spanning the eastern seaboard of the Irish Sea, extending from the Solway in north-west England to St. David's Head in south Wales. Some of these estuaries had been investigated in previous surveys, but this study is unique in that it covered a wide geographic range using the same sampling and analytical methodology and within a comparatively short time scale. This allows for a valid comparison within the data set of the contamination levels at the different areas. Spatial distributions of the radionuclides were consistent with transport of radionuclides discharged to the Irish Sea from the Sellafield Nuclear Reprocessing Plant, with the highest activities occurring in the Esk estuary (closest to Sellafield) and lowest at the Welsh sites. Measurable activity concentrations of238 Pu and 239,240Pu were found in root mat samples from the Solway estuary to as far south as the Gwyrfai in Wales and showed an average238 Pu/239,240Pu ratio of 0.2, consistent with Sellafield-derived Pu. The ratios of137 Cs/241Am increased with distance from the source, with values of 1:1 in estuaries near Sellafield to ratios between 2 and 5 in estuaries further south and in excess of 10:1 in Wales. This is probably due to the more rapid movement of dissolved137 Cs in Irish Sea waters compared with the actinides. In contrast, 241Am and 239,240Pu behave similarly with consistent ratios of between 2:1 and 3:1, as both are associated with particulates. Dose assessment calculations suggest that external exposure would be a maximum of 530 µSv at the most contaminated spot at the Esk estuary. Relatively lower doses arise from the ingestion of animal products (along the soil-vegetation-grazing animal pathway) due to the low availability of sediment-associated radionuclides for gut transfer. The dose assessment calculations highlight the importance of using the appropriate transfer parameters that take into account this low bioavailability.

Contemporary Flux of Radionuclides to Contaminated Saltmarshes in the Esk Estuary, Cumbria

The Esk estuary is approximately 10 km from the marine outfall fromBritish Nuclear Fuels plc (BNFL) Sellafield Site and saltmarshes here havereceived significant quantities of radionuclides as reported in many studiessince 1975. These studies have concentrated on the inventory ofradionuclides in the estuary, but they have not addressed the continualreworking of radionuclides from these deposits. A detailed investigation ofboth the concentration of 137Cs in the surface 10 cm and gammaair-kerma dose rates has been made where 120 determinations were made in agrid over 14600 m2 of saltmarsh. The surface microtopographyis shown to be important for the continuing deposition of contaminatedsediments to the saltmarsh surface.

Particle-solution behaviour of plutonium in an estuarine environment, Esk Estuary, UK

The particle-solution ( K d ) relationships of Pu(III,IV) in the Esk Estuary are investigated, using new experimental data together with a synthesis of our earlier work. Adsorption of 236Pu(IV) by a suspension of intertidal mud (40 mg L −1) from the Esk Estuary was determined after 1 h, as a function of salinity and pH, in a series of controlled laboratory experiments. Desorption of 239, 240Pu(III,IV) from this environmentally contaminated sediment was determined concurrently. The short term (i.e., within a tidal cycle) non-conservative behaviour of Pu(III,IV) in both the laboratory experiments and the estuary appears to be dominated by a rapid, reversible surface complexation reaction, although only a small fraction (<5%) of the 239,240Pu(III,IV) activity of the environmentally contaminated sediment is able to participate in the reaction. The existence of this exchangeable or labile fraction can explain the apparent dependence of Pu(III,IV) K d on sediment concentration. Thus, a single K d value is able to describe both the observed adsorption and desorption behaviour and the effect of sediment concentration, when desorption is expressed with respect to the labile 239,240Pu(III,IV) fraction. For example, in R. Esk water, the adsorption of 236Pu(III,IV) and the desorption of 236,240Pu(III,IV), over a two order of magnitude concentration range of unwashed Esk Estuary sediment, can be accounted for by a single K d of ∼3 × 10 3 L kg −1. The K d for the labile Pu(III,IV) fraction varies mainly as a function of salinity. pH is not an important factor over the pH range 4–9, although H + ion exchange does occur, probably through a similar surface complexation reaction. The kinetic and equilibrium characteristics of the Pu (III,IV) sorption behaviour conform to the pattern observed by Jannasch et al. (1988) and other workers for a range of trace elements.

Fixation of 137Cs by soils and sediments in the Esk Estuary, Cumbria, UK

Abstract Enhanced levels of 137Cs are observed on the Cumbrian coast (UK) due to the discharge of low level waste by BNFL (British Nuclear Fuels Ltd) at Sellafield. Sorption of this radionuclide onto estuarine sediments is of considerable strategic importance as these areas represent a secondary source of transfer to inland areas. The study reported here was undertaken to determine, both quantitatively and qualitatively, the characteristics of the sorption and fixation of 137Cs in sediments and soils sampled from within the Esk estuary. This was carried out by means of a detailed set of laboratory analyses on samples collected from the area. These involved a sequential solvent extraction to determine the relative proportions of 137Cs associated with exchangeable, reducible, oxidiseable and residual fractions of various substrates; a series of batch sorption experiments was also carried out to determine the sorption characteristics of a selection of the substrates sampled. To complement these investigations grain size determinations coupled with X-ray diffraction analyses were employed to determine the mechanical and mineralogical properties of each sample collected. 137Cs was most strongly associated with the residual phase as defined by the sequential leaching scheme. The more consolidated, clay rich substrates appeared to sorb the greatest quantities of 137Cs within the residual phase although there was no obvious correlation between the quantity of radiocaesium associated with this phase and the relative proportion of illite and

Chemical leaching behavior of237Np from intertidal coastal sediment in the Irish Sea

Chemical leaching experiments of237Np in the sediments from the Esk Estuary and the Ribble Estuary in the Irish Sea, U. K., have been carried out, in comparison with those of239, 240Pu and241Am, to understand the geochemical associations of these long-lived radionuclides with sediment. Experimental results show that partitioning behavior of237Np is obviously different from those of239, 240Pu and241Am.

The relationship between sediment and plutonium budgets in a small macrotidal estuary: Esk estuary, Cumbria, UK

During a spring tide, measurements were made of sediment and 239,240Pu discharges through a cross-section of the Esk estuary. These indicated that over the full tidal cycle the inner estuary had a net gain of ca. 18t of sediment and ca. 85 MBq of particulate phase 239,240Pu, and a probable net loss of ca. 1 to 2 MBq of solution phase 239,240Pu. Each of these was the net result of large gross discharges of sediment and plutonium into and out of the estuary for which the sea was the main source, with eroded estuarine sediment providing an additional minor source of sediment, of particulate phase plutonium and, via desorption, of solution phase plutonium. A net input with each tide, of sediment and its associated radionuclides, is considered to be typical for the Esk estuary under the normal conditions of low river flows.