Iodine Isotopes and their Species in Surface Water from the North Sea to the Northeastern Atlantic Ocean

Abstract: Huge amounts of anthropogenic 129I have been and still are released to the environment through liquid and gaseous discharges from the nuclear fuel reprocessing facilities worldwide and in particular the ones in Europe. Most of this 129I signal has been accumulated in the marine environment which plays a major role in the iodine natural pool.  In this thesis, an overview of available 129I concentrations in waters of the oceans and marginal seas together with new data about 129I and 127I spatial distribution in surface seawater along a transect between the North Sea and the northeastern Atlantic Ocean are presented. After comprehensive chemical separation, the concentrations of iodine isotopes (127I and 129I) and their species (iodide and iodate) were analysed using accelerator mass spectrometry and inductively-coupled plasma mass spectrometry. The results show that, generally, changes in the 127I and 127I-/127IO3- are comparable to data from other marine waters which are related to natural distribution patterns. A considerable variation of 129I along the transect is observed with the highest values occurring in the eastern English Channel and relatively low values obtained in the northeastern Atlantic Ocean. Inventory estimations of 129I in the North Sea and the English Channel are 147 kg and 78 kg, respectively, where more than 90% resides in the Southern Bight and the eastern English Channel. Iodate is the dominant iodine species for both 127I and 129I in most seawater samples from the North Sea to the Atlantic Ocean. 129I species variability suggests a slow process of 129I- oxidation in the open sea. It takes at least 10 years for the 129I-/129IO3- pair to reach their natural equilibrium as the water is transported from the English Channel. The results suggest a main transport of 129I from the western English Channel via the Biscay Bay into the northeastern Atlantic Ocean. Further, high 129I/127I and distinctive 129I-/129IO3- values south of 40°N indicate possible contribution of 129I through Mediterranean Outflow Water. The environmental radioactive impact of 129I and possible applications in ecosystem studies are also discussed.