Geochemical fractionation of plutonium in anoxic Irish Sea sediments using an optimised sequential extraction protocol

Lucey, Julie; Gouzy, Aurélien; Boust, D.; Vintró, Luis León; Bowden, Louise; Finegan, P.P.; Kershaw, P. J.; Mitchell, P.I.

doi:10.1016/j.apradiso.2003.11.045

Cited by 28 publications

(19 citation statements)

References 8 publications

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“…The average solid partitioning of these isotopes among the fractions defined above (Tab. 2) is very similar to that reported previously on a core collected in the Esk estuary [13]. In both cases, plutonium is mainly associated with the R0 exchangeable/readily oxidisable and R1 acido-soluble fractions.…”

Section: Solid Partition Of the Plutoniumsupporting

confidence: 78%

“…Special attention was paid to both the determination of acid-volatile sulphides (AVS) and chromium reducible sulphides (CRS) [12], and to the solid partitioning of plutonium. A thoroughly validated sequential extraction procedure [13] was applied to the squeezed sediment sections. The protocol employed considers five fractions, namely exchangeable/readily oxidisable (including reactive sulphide -AVS), acido-soluble (including carbonates), reducible, oxidisable (organics and CRS sulphides), and residual fractions (hereafter referred to as R0, R1, R2, R3 and R4, respectively).…”

Section: Methodsmentioning

confidence: 99%

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Diagenetic reactivity of the plutonium in marine anoxic sediments (Cumbrian mud patch - eastern Irish Sea)

et al. 2005

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Abstract. An extensive diagenetic study carried out on a sediment core collected in the Cumbrian mud patch off the Sellafield nuclear reprocessing plant, is presented. Sequential leaching data, using a thoroughly validated protocol specifically designed to prevent any resorption of the released plutonium in the course of the extraction, demonstrate that a significant proportion of the plutonium is loosely bound to sites that readily exchange with seawater, oxidise upon oxygenated water contact (reactive sulphides) or easily dissolve upon changes in pH. Such a result contradicts many previous sequential extraction studies which have reported that little of the plutonium in Irish Sea sediments is in a readily available form. The profile of dissolved plutonium in pore waters indicates an active uptake process at depth, probably linked to sulphide (Acid Volatile Sulphide) precipitation. These reactive sulphides are liable to act as source of plutonium to the overlying water if they are brought close the interface by bioturbation or in contact with oxygenated seawater by burrowing activity.

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Section: Solid Partition Of the Plutoniumsupporting

confidence: 78%

Section: Methodsmentioning

confidence: 99%

Diagenetic reactivity of the plutonium in marine anoxic sediments (Cumbrian mud patch - eastern Irish Sea)

et al. 2005

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“…7b). This reinforces the idea that AVS are an important sink phase for plutonium, as well as a very reactive carrier phase as reported by [5][6] from field studies in the eastern Irish Sea.…”

Section: Plutonium Solid Partitionsupporting

confidence: 74%

Post-depositional reactivity of the plutonium in different sediment facies from the English Channel - an experimental approach

et al. 2005

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Abstract. The post-depositional reactivity of the plutonium was investigated in bottom sediments collected in the central English Channel using an experimental approach. Medium to coarse grained surficial sediments and fine-grained undisturbed sediment cores were spiked with 238 Pu. After a one-month incubation, pore waters were extracted under strictly anoxic conditions and dissolved plutonium was analysed by liquid scintillation techniques. Kd values ranged from 10 2 to 10 5 in surficial sediments undergoing oxic diagenesis, and were shown to be grain-size dependant. In fine-grained sediments undergoing anoxic diagenesis, Kd values ranged between 10 3 and 10 5 . Kd profile suggests an active recycling of the plutonium in the topmost sediment layers, and subsequent efficient uptake process at depth, tentatively acido-volatile sulphide (AVS) precipitation. This hypothesis was further confirmed by a correlation between the AVS content and the loosely bound plutonium extracted using an oxidising/complexing solution from sediment subsamples. In surficial sediments, by contrast, loosely bound plutonium was likely to be associated with the carbonate phase as surface complexes.

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“…Recent work by Lucey et al (2004) has suggested that in inter-tidal sediments plutonium speciation may be influenced by pH changes within estuarine waters. However, there is no direct evidence from the field to suggest that this is the case for offshore sediments.…”

Section: Interactions Within Sedimentsmentioning

confidence: 99%

A process-based model for the partitioning of soluble, suspended particulate and bed sediment fractions of plutonium and caesium in the eastern Irish Sea

Batlle¹,

Bryan²,

McDonald³

2008

Journal of Environmental Radioactivity

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Geochemical fractionation of plutonium in anoxic Irish Sea sediments using an optimised sequential extraction protocol

Cited by 28 publications

References 8 publications

Diagenetic reactivity of the plutonium in marine anoxic sediments (Cumbrian mud patch - eastern Irish Sea)

Diagenetic reactivity of the plutonium in marine anoxic sediments (Cumbrian mud patch - eastern Irish Sea)

Post-depositional reactivity of the plutonium in different sediment facies from the English Channel - an experimental approach

A process-based model for the partitioning of soluble, suspended particulate and bed sediment fractions of plutonium and caesium in the eastern Irish Sea

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