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Sediment cores were collected at the outlet of the highly anthropogenized catchment of the Seine River at two contrasting sites: a flood plain of the lower Seine River and a quasi-permanently submerged harbour basin (or wet dock) in the upper tidal estuary. Analyses of artificial radionuclides ((137)Cs and plutonium isotopes), coupled with hydrological and bathymetric data, lead to a precise dating of the sediment cores collected at the two sites. (137)Cs signals originating from global fallout (early 1960s) and from the Chernobyl accident (1986) are identified, but at different levels due to the incomplete nature or variable continuity of the records. Anomalous (238)Pu concentrations found at both sites (1-2 Bq kg(-1)) are attributed to unknown industrial releases originating from upstream. Interpolating (137)Cs sediment activities under the assumption of a constant sediment rate, those releases were dated back to 1975 ± 1, thus providing a local but reliable time-marker. Age models have highlighted a very contrasting sediment filling dynamics in these two sites. This study presents the first sediment record of alpha- and gamma-emitting artificial radionuclides obtained at the outlet of the huge catchment area of the River Seine, over a period covering the last 50 years., (Copyright © 2013 Elsevier Ltd. All rights reserved.)

Contamination of the marine environment following the accident in the Fukushima Dai-ichi nuclear power plant represented the most important artificial radioactive release flux into the sea ever known. The radioactive marine pollution came from atmospheric fallout onto the ocean, direct release of contaminated water from the plant and transport of radioactive pollution from leaching through contaminated soil. In the immediate vicinity of the plant (less than 500 m), the seawater concentrations reached 68,000 Bq.L(-1) for (134)Cs and (137)Cs, and exceeded 100,000 Bq.L(-1) for (131)I in early April. Due to the accidental context of the releases, it is difficult to estimate the total amount of radionuclides introduced into seawater from data obtained in the plant. An evaluation is proposed here, based on measurements performed in seawater for monitoring purposes. Quantities of (137)Cs in seawater in a 50-km area around the plant were calculated from interpolation of seawater measurements. The environmental halftime of seawater in this area is deduced from the time-evolution of these quantities. This halftime appeared constant at about 7 days for (137)Cs. These data allowed estimation of the amount of principal marine inputs and their evolution in time: a total of 27 PBq (12 PBq-41 PBq) of (137)Cs was estimated up to July 18. Even though this main release may be followed by residual inputs from the plant, river runoff and leakage from deposited sediments, it represents the principal source-term that must be accounted for future studies of the consequences of the accident on marine systems. The (137)Cs from Fukushima will remain detectable for several years throughout the North Pacific, and (137)Cs/(134)Cs ratio will be a tracer for future studies., (Copyright © 2011 Elsevier Ltd. All rights reserved.)

A sequential extraction protocol has been used to determine the solid-phase partition of (210)Po and (210)Pb in anoxic marine sediment from the roads of Cherbourg (France) in the central English Channel. Measurements were also obtained in pore waters, in which (210)Po activities range between 1 and 20 mBq L(-1) and (210)Pb activities between 2.4 and 3.8 mBq L(-1), with highest activities in the topmost layer. These activities are higher than in seawater, suggesting that sediment act as a source of both (210)Po and (210)Pb for overlying water. The (210)Po profile in the pore waters is apparently correlated with those obtained for Fe, Mn and SO(4)(2)(-), suggesting an influence of early diagenetic processes on the (210)Po solid-liquid distribution. In the sediment, (210)Po is predominantly bound to organic matter or chromium reducible sulphides, and residuals (clay minerals and refractory oxides). Our results indicate that (210)Po is not significantly bound to AVS, i.e. acid volatile sulphides: bioturbation could play a role by the early redistribution of (210)Po bound to acid volatile sulphides in the sediment. (210)Po, (210)Pb and Pb exhibit differences in terms of distribution, probably due to a different mode of penetration in the sediment. This work provides information on solid and liquid distribution of (210)Po and (210)Pb in marine sediment. These data are very scarce in the literature.

Sequential extraction has been used extensively to study the solid partitioning of radionuclides in soils and sediments. A difficulty with sequential extraction is that radionuclides released by a particular extractant can be resorbed and artificially redistributed amongst the remaining solid phases. Here, we describe experiments (on selected model phase and natural materials), which were designed to determine whether the inclusion of a chelating agent (sodium citrate) in an established sequential extraction protocol (a) inhibits post-extraction resorption of plutonium, (b) increases non-targeted dissolution of sediment phases, and (c) gives rise to unwanted ligand competition for plutonium. The results clearly demonstrate the capacity of citrate to inhibit the resorption of plutonium from the various extractants, and confirm that there is no discernible increase in non-targeted phase dissolution, but indicate significant ligand competition with the carbonate phase. The merits of using citrate are discussed and an optimised sequential extraction protocol that includes citrate is proposed. Finally, the protocol is applied to oxic and anoxic sediments sampled in the NE Irish Sea and the Roads of Cherbourg, and it is shown that the bulk of the plutonium on these sediments is associated with the more labile geochemical fractions.

In this paper we report and compare the concentrations of 234Th and 238U measured in surface and subsurface waters collected in the course of a sampling campaign in the north east Atlantic in June-July 1998. Dissolved 234Th concentrations in surface waters ranged from 5 to 20 Bq m(-3), showing a large deficiency relative to 238U concentrations (typically 42 Bq m-3). This disequilibrium is indicative of active 234Th scavenging from surface waters. Observed 234Th/238U activity ratios, together with corresponding 234Th particulate concentrations, were used to calculate mean residence times for 234Th with respect to scavenging onto particles (tau(diss)) and subsequent removal from surface waters (tau(part)). Residence times in the range 5-30 days were determined for tau(diss) and 4-18 days for tau(part) (n=14). In addition, ultrafiltration experiments at six stations in the course of the same expedition revealed that in north-east Atlantic surface waters a significant fraction (46+/-17%; n=6) of the thorium in the (operationally-defined) dissolved phase (<0.45 microm) is in colloidal form. These observations are consistent with the 'colloidal pumping' model in which it is assumed that 234Th is rapidly absorbed by colloidal particles, which then aggregate, albeit at a slower rate, into larger filterable particles. In essence, colloids act as intermediaries in the transition from the fully dissolved to the filter-retained (>0.45 microm) phase. Thus, the time (tau(c)) for fully dissolved 234Th to appear in the filter-retained fraction is dependent on the rate of colloidal aggregation. Here, we determined tau(c) values in the range 3-17 days.