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Abstract  

The distribution of134Cs,137Cs and214Am in surface and core sediments from areas in north Wales has been investigated. Coastal sites show a predominance of Sellafield-derived material for all three radionuclides whereas estuarine sites show an increased proportion of Chemobyl-derived caesium present. By the use of the134Cs/137Cs ratio, a mean proportion of Chemobyl-derived137Cs in surface sediments collected in 1991 fell from 34% at an estuarine site to 11% at a coastal site. In deeper sections of cores representing sedimentation dates near the Chemobyl accident, up to 90% of137Cs at the estuarine site and 26% at the coastal site can be attributed to Chemobyl. By using the position of the Chemobyl134Cs and137Cs peak in the cores, sedimentation rates of 0.7 mm·a–1 were calculated.

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Abstract  

Long-lived radionuclides,99Tc,137Cs,237Np, Pu isotopes and241Am were determined in the long sediment cores collected from nine intertidal sites around the west Cumbria of the Irish Sea, UK. The inventories of all nuclides measured varied considerably among the sampling sites, but generally their inventories decreased with increasing distance from Sellafield. Furthermore, the inventory ratios with respect to relationship with distance from Sellafield enabled comparison of transport behavior of99Tc,137Cs,237Np and241Am compared with239,240Pu. As a consequence, the apparent fractional rate of solution transport to the intertidal sediment was found to increase as follows:99Tc>137Cs>237Np>239,240Pu≥241Am.

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Abstract  

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.

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Abstract  

The Esk estuary, U.K. receives inputs of dissolved and particulate plutoniun from discharges of waste into the Irish Sea from the Sellafield nuclear fuel reprocessing plant. Field and laboratory methods have been developed to examine the phenomenon of rapid plutonium remobilization from contaminated Esk sediments during estuarine mixing which was first identified in 1981.Both types of studies have shown comparable, non-conservative behavior for the two oxidation state categories of238Pu and239,240Pu (i.e. Pu (III/IV) and Pu (V/VI)) with enrichment in low salinity waters due to desorption of plutonium from resuspended sediments.

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Abstract  

An analytical method has been developed for the determination of low-level99Tc in environmental samples by High Resolution ICP-MS. The method consists of leaching of99Tc by HNO3 and separation by three different solvent extractions with 30% TOA-xylene, MEK, and cyclohexanone. Finally, purification of99Tc was made by using an anion exchange resin column to reduce dissolved solids content. The final solution was adjusted to 1M HNO3 for introducing into the HR-ICP-MS. The accuracy and precision of the method was confirmed to be satisfactory by applying this technique to the determination of99Tc in IAEA marine algae sample (AG-B-1). Measurements of99Tc using 0.5–2.5 g of sediment samples from the Irish Sea, UK, were successfully performed by the present method.

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Abstract  

Depth profiles and inventories of237Np in sediment cores from the Ribble Estuary in the Irish Sea have been studied along with those of Pu isotopes,241Am and137Cs, to allow a more detailed look of anomalously high237Np content observed in this estuary previously. The comprehensive data obtained showed that the depth profiles of both237Np contents and237Np/239,240Pu activity ratios were clearly different from those of239,240Pu,241Am, and137Cs and their activity ratios. As much as 80–90% of237Np inventories (0.32–1.06 kBq/m2), found in three cores, were estimated to be derived from a source other than Sellafield, on the basis of comparison of the237Np/239,240Pu inventory ratio (0.65–1.74%) found in the Ribble Estuary cores with those (0.10–0.16%) in the Ravenglass Estuary cores.

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Abstract  

Intertidal coastal and estuarine sediments from 24 sites in the Irish Sea have been analyzed for99Tc,237Np,238Pu,239,240Pu and241Am. The237Np activity and239Pu/240Pu ratio were measured simultaneously by ICP-MS, and99Tc was determined by HR-ICP-MS which is ten times more sensitive than Q-ICP-MS.The activities of99Tc,237Np,239,240Pu and241Am were distributed over a wide range of 1.5–70.5, 0.01–13.3, 2.3–1589, 2.6–1894 Bq/kg, respectively. Activities of these radionuclides decreased exponentially with distance from the Sellafield source. The241Am/239,240Pu and237Np/239,240Pu ratios were almost constant with distance from the Sellafield. This result suggests that the distribution and behavior of Np and Pu are controlled by complicated factors such as the influence of transport, the variation with time of Np/Pu ratio in the Sellafield discharges and sedimentary mixing processes in the Irish Sea.

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Journal of Radioanalytical and Nuclear Chemistry
Authors:
D. Assinder
,
M. Yamamoto
,
C. Kim
,
R. Seki
,
Y. Takaku
,
Y. Yamauchi
,
S. Igarashi
,
K. Komura
, and
K. Ueno

Abstract  

A survey has been carried out of40K,60Co,99Tc,106Ru,125Sb,129I,134Cs,137Cs,154Eu,226Ra,228Ra,237Np,238Pu,239,240Pu,241Pu,241Am,242Cm, and243,244Cm activities in sediments from the Irish Sea. Several of these radionuclides were measured independently at two separate laboratories to enable the intercomparison of the results produced. The comprehensive data set generated allows the present spatial distributions of these radionuclides in coastal sediments to be examined in relation to sediment textural characteristics and by comparison with earlier survey, enables the temporal trends in their activities to be determined. In general all artificial radionuclides showed lower activities in sediments in response to falling discharges from Sellafield and relationships with either grain size, distance from Sellafield or both. Isotope ratios were similar to cumulative weighted activity ratios rather than present day values due to sediment mixing. Pu levels supplied evidence for the lag in response of sediment deposits with increasing distance from Sellafield due to sediment transport.

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