Estimation of marine source-term following Fukushima Dai-ichi accident.

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.

Solid partitioning and solid-liquid distribution of 210Po and 210Pb in marine anoxic sediments: roads of Cherbourg at the northwestern France.

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.

Multi-isotopic determination of plutonium (239Pu, 240Pu, 241Pu and 242Pu) in marine sediments using sector-field inductively coupled plasma mass spectrometry.

Among the transuranic elements present in the environment, plutonium isotopes are mainly attached to particles, and therefore they present a great interest for the study and modelling of particle transport in the marine environment. Except in the close vicinity of industrial sources, plutonium concentration in marine sediments is very low (from 10(-4) ng kg(-1) for (241)Pu to 10 ng kg(-1) for (239)Pu), and therefore the measurement of (238)Pu, (239)Pu, (240)Pu, (241)Pu and (242)Pu in sediments at such concentration level requires the use of very sensitive techniques. Moreover, sediment matrix contains huge amounts of mineral species, uranium and organic substances that must be removed before the determination of plutonium isotopes. Hence, an efficient sample preparation step is necessary prior to analysis. Within this work, a chemical procedure for the extraction, purification and pre-concentration of plutonium from marine sediments prior to sector-field inductively coupled plasma mass spectrometry (SF-ICP-MS) analysis has been optimized. The analytical method developed yields a pre-concentrated solution of plutonium from which (238)U and (241)Am have been removed, and which is suitable for the direct and simultaneous measurement of (239)Pu, (240)Pu, (241)Pu and (242)Pu by SF-ICP-MS.

Dynamics of sulfate-reducing microorganisms (dsrAB genes) in two contrasting mudflats of the Seine estuary (France).

By combining molecular biology and biochemical approaches, the dynamics of sulfate-reducing microorganisms (SRM) was investigated in the sediments of the Seine estuary (France). Both intertidal mixing-zone and freshwater mudflats were sampled during a 1-year period; the quantification of SRM was realized by using competitive polymerase chain reaction (PCR) based on dsrAB gene amplification, previously described by Leloup et al. (2004), and sulfate reduction rate (SRR) was determined via the SO4(2-) radiotracer method. Throughout the year, abundance of dsrAB genes and SRR were predominantly high in the top 15 cm of the sediment. A seasonal dynamic was observed; a predominance of activity was noted during the early summer, and seems to be mainly controlled by physical-chemical parameters (temperature and dissolved organic carbon concentration) and topographic evolution of the mudflat (erosion/deposit erosion).

Uranium-thorium disequilibrium in north-east Atlantic waters.

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.

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

An optimised five-step sequential extraction protocol, incorporating the use of sodium citrate to inhibit resorption, has been used to assess the solid partition of plutonium under anoxic conditions in intertidal sediments from the Ravenglass Estuary in the north-eastern Irish Sea. The data reveal that the plutonium is predominantly bound to geochemical phases targeted by the acido-soluble and the exchangeable extractants, indicating that a significant proportion of the plutonium in these and similar sediments is associated with relatively mobile geochemical phases. The results are consistent with the relatively high level of plutonium remobilisation now known to be taking place throughout the north-eastern Irish Sea.