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Surface seawater samples collected from the North Sea and English Channel were analyzed for total 129I and 127I, as well as for iodide and iodate. Relatively high 129I concentrations (2-3 x 10(11) atoms/L) were observed in the northern part of the English Channel and in the southeastern North Sea. The atomic ratio of 129I/127I decreases from the eastern (1.0-1.9 x 10(-6)) to the western (4-6 x 10(-8)) parts of the North Sea and from the northeastern (1.5 x 10(-6)) to southwestern (1-5 x 10(-8)) parts of the English Channel. The ratios of iodide to iodate are 0.1-0.5 and 0.5-1.6 for 127I and 129I, respectively, in open seawaters, whereas these ratios range from 0.6 to 1.3 and 0.8 to 2.2, respectively, in coastal waters. The results suggest that (1) imprints of the La Hague facility dominates the 129I distribution in the surface water of the North Sea, (2) reduction of iodate to iodide is relatively fast during the transport to the European continental coast, (3) oxidation of newly produced 129I- to (129)IO3- is insignificant during water exchange between the coastal area and open sea, (4) reduction of iodate and oxidation of iodide in the open sea seems to be a slow process.

The Fukushima nuclear accident in March 2011 has released a large amount of radioactive pollutants to the environment. Of the pollutants, iodine-129 is a long-lived radionuclide and will remain in the environment for millions of years. This work first report levels and inorganic speciation of (129)I in seawater depth profiles collected offshore Fukushima in June 2011. Significantly elevated (129)I concentrations in surface water were observed with the highest (129)I/(127)I atomic ratio of 2.2 × 10(-9) in the surface seawater 40 km offshore Fukushima. Iodide was found as the dominant species of (129)I, while stable (127)I was mainly in iodate form, reflecting the fact that the major source of (129)I is the direct liquid discharges from the Fukushima NPP. The amount of (129)I directly discharged from the Fukushima Dai-ichi nuclear power plant to the sea was estimated to be 2.35 GBq, and about 1.09 GBq of (129)I released to the atmosphere from the accident was deposited in the sea offshore Fukushima. A total release of 8.06 GBq (or 1.2 kg) of (129)I from the Fukushima accident was estimated. These Fukushima-derived (129)I data provide necessary information for the investigation of water circulation and geochemical cycle of iodine in the northwestern Pacific Ocean in the future.