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Thesis for the Degree of Doctor of Philosophy - DTU Orbit

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Among iodine isotopes, 129 I has a half-life <strong>of</strong> 15,7 My and it is naturally <strong>for</strong>med by cosmic-<br />

ray-induced spallation <strong>of</strong> xenon in <strong>the</strong> upper atmosphere, spontaneous fission <strong>of</strong> 238 U in <strong>the</strong><br />

geosphere and in minor quantities, by neutron bombardment <strong>of</strong> tellurium. Thermal neutron<br />

induced fission <strong>of</strong> 235 U is ano<strong>the</strong>r minor natural source in <strong>the</strong> lithosphere. The reported natural<br />

isotopic ratio <strong>of</strong> 129 I/ 127 I is about10 -12 in terrestrial and marine environment (Hou et al., 2009;<br />

Fehn et al., 2007). Presently, <strong>the</strong> source <strong>of</strong> additional 129 I in <strong>the</strong> environment is mainly from<br />

human nuclear activity such as nuclear reprocessing facilities, nuclear weapons testing and<br />

accidents associated with nuclear power plants. Over <strong>the</strong> past decade, liquid and gaseous<br />

releases <strong>of</strong> 129 I from reprocessing facilities such as La Hague (France) and Sellafield (UK) has<br />

increased <strong>the</strong> natural environmental concentration by several orders <strong>of</strong> magnitude (Alfimov et<br />

al., 2004; Fehn et al., 2007; Aldahan et al., 2007). In <strong>the</strong> period 1999 - 2009, respectively 14.6<br />

and 4.6 TBq <strong>of</strong> 129 I have been discharged into <strong>the</strong> English Channel from <strong>the</strong> La Hague<br />

reprocessing plant and to <strong>the</strong> Irish Sea from <strong>the</strong> Sellafield reprocessing plant (www.ospar.org).<br />

It is well known that seaweed accumulates iodine from seawater and that <strong>the</strong> process depends<br />

strongly on seaweed type/species (Leblanc et al., 2006) as well as <strong>the</strong> region in which <strong>the</strong>y are<br />

found (Shah et al., 2005). Fur<strong>the</strong>rmore marine algae play an important role (Leblanc et al.,<br />

2006) in <strong>the</strong> global cycle <strong>of</strong> iodine in <strong>the</strong> environment in <strong>the</strong> sense that <strong>the</strong>y accumulate iodine<br />

as iodide (Kupper et al., 1998) from seawater and trans<strong>for</strong>m a part <strong>of</strong> it into volatile organic<br />

iodine (VOI), such as methyl iodide (CH3I) or diiodomethane (CH2I2; Carpenter et al. 2007).<br />

Once released from <strong>the</strong> seawater surface <strong>the</strong> volatile organic iodine are broken down by<br />

photolysis and reactions with ozone (O3) (Jones & Carpenter, 2005; Martino et al. 2006)<br />

<strong>for</strong>ming a reactive pool <strong>of</strong> iodine species which afterwards contribute to <strong>the</strong> ozone depletion,<br />

particulates <strong>for</strong>mation and cloud condensation nuclei <strong>for</strong>mation (Küpper et al., 2008; O’Dowd<br />

2

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