17.08.2013 Views

Thesis for the Degree of Doctor of Philosophy - DTU Orbit

Thesis for the Degree of Doctor of Philosophy - DTU Orbit

Thesis for the Degree of Doctor of Philosophy - DTU Orbit

SHOW MORE
SHOW LESS

Create successful ePaper yourself

Turn your PDF publications into a flip-book with our unique Google optimized e-Paper software.

302 V. Hansen et al. / Science <strong>of</strong> <strong>the</strong> Total Environment 412-413 (2011) 296–303<br />

August<br />

April<br />

Salinity<br />

a b<br />

c d<br />

isotopes species and oxygen is observed (Table 3). These results suggest<br />

that <strong>the</strong> oxidation conditions <strong>of</strong> surface water do not influence<br />

<strong>the</strong> iodine speciation in <strong>the</strong> studied basins. This situation is also illustrated<br />

by Figs. 4 and 5, which show that despite ra<strong>the</strong>r uni<strong>for</strong>m oxygen<br />

concentration in <strong>the</strong> surface water, <strong>the</strong>re is a large variability in<br />

<strong>the</strong> iodine isotopes distribution. The different distribution pattern <strong>of</strong><br />

iodide and iodate ( 129 I and 127 I) along <strong>the</strong> surface water <strong>of</strong> Skagerrak,<br />

Kattegat and Belt Sea (Fig. 1, station 12) is most likely due to <strong>the</strong> mixing<br />

process between saline North Sea-Atlantic and Baltic Sea fresher<br />

water (Figs. 2 and 3). North Sea surface water with high 129 I and<br />

127 I iodide concentrations and high salinity (Hou et al., 2007) enters<br />

Skagerrak and mixes with <strong>the</strong> relatively low iodide concentrations<br />

(Figs. 2 and 3) and low salinity (Fig. 5) outflow waters from <strong>the</strong> Baltic<br />

Sea in <strong>the</strong> Kattegat through <strong>the</strong> Belt Sea (station 12, Fig. 1).<br />

4.2. Iodide and iodate in surface water <strong>of</strong> Arkona Sea and Baltic Proper<br />

In <strong>the</strong> Arkona Sea, higher 129 I − / 129 IO 3 − happened in August<br />

(Fig. 3c) and could be explained as a reduction <strong>of</strong> 129 IO3 - along <strong>the</strong><br />

water pr<strong>of</strong>ile from Kattegat through <strong>the</strong> Belt Sea to 129 I - as found<br />

along <strong>the</strong> surface water <strong>of</strong> sou<strong>the</strong>rn Baltic Sea. However, ratio <strong>of</strong><br />

127 I − / 127 IO3 − , shows instead higher values in April (Fig. 2f), indicating<br />

a selective reduction <strong>of</strong> iodate that may be a significant process governing<br />

<strong>the</strong> out <strong>of</strong> equilibrium (freshly added to <strong>the</strong> environment)<br />

129 I isotope compared to <strong>the</strong> naturally equilibrated 127 I isotope. As<br />

<strong>the</strong> Arkona Basin is end-member <strong>of</strong> relatively saline water, iodide<br />

and iodate concentration are severely affected by <strong>the</strong> mixing process.<br />

Variability in <strong>the</strong> relative 129 I − / 127 I − and 129 IO 3 − / 127 IO3 − values<br />

(Fig. 4) between <strong>the</strong> sampling campaigns (August-2006 and April-<br />

2007) can reflect seasonal and input effects. Addition <strong>of</strong> huge fresh<br />

water to <strong>the</strong> system during spring snow and ice melting may preferentially<br />

alter <strong>the</strong> concentrations and iodine speciation, specifically in<br />

near coastal regions. During August, extensive algal blooming may<br />

on <strong>the</strong> o<strong>the</strong>r hand contribute to increase <strong>the</strong> iodide species, particularly<br />

near to coastal and shallow water regions. The present distribution<br />

<strong>of</strong> <strong>the</strong> studied sampling sites is ra<strong>the</strong>r limited and does not<br />

provide enough coverage to deduce specific distribution patterns <strong>of</strong><br />

<strong>the</strong> isotopes in <strong>the</strong> surface water. Fur<strong>the</strong>rmore, addition <strong>of</strong> data on iodine<br />

speciation in depth pr<strong>of</strong>iles <strong>of</strong> <strong>the</strong> sampling site will expose better<br />

<strong>the</strong> interplay between regional water transport and environmental conditions.<br />

Never<strong>the</strong>less, <strong>the</strong> data presented here has shown <strong>for</strong> <strong>the</strong> first<br />

time <strong>the</strong> extent and general distribution patterns <strong>of</strong> iodine isotopes species<br />

that add new valuable in<strong>for</strong>mation <strong>for</strong> future environmental<br />

analysis.<br />

5. Conclusions<br />

We here present data on iodine isotopes ( 129 I and 127 I) and <strong>the</strong>ir<br />

species (iodide and iodate) in surface water collected from 16 locations<br />

in August 2006 and 19 locations in April 2007 in <strong>the</strong> Baltic Proper,<br />

Kattegat and Skagerrak. From those results we draw <strong>the</strong> following<br />

conclusions: a) reduction <strong>of</strong> iodate and oxidation <strong>of</strong> iodide in Skagerrak<br />

and Kattegat may be a slow process since insignificant change in<br />

129 I and 127 I speciation was found; b) reduction <strong>of</strong> iodate to iodide<br />

seems to be a relatively fast process in surface water <strong>of</strong> <strong>the</strong> sou<strong>the</strong>rn<br />

Baltic Sea; c) oxidation conditions <strong>of</strong> <strong>the</strong> surface water are not exerting<br />

a marked effect on <strong>the</strong> iodine speciation in <strong>the</strong> studied basins; d)<br />

seasonal and input effects may alter <strong>the</strong> concentrations and speciation<br />

modes specifically in near coastal regions.<br />

Acknowledgements<br />

Oxygen (ml/L)<br />

Fig. 5. Distribution <strong>of</strong> salinity and oxygen in <strong>the</strong> surface water <strong>of</strong> Skagerrak, Kattegat and Baltic Sea, during August 2006 and April 2007.<br />

Table 3<br />

Correlation relationship (R 2 ) between iodine species and oxygen and salinity.<br />

127 I −<br />

127 IO3 −<br />

129 I −<br />

129 IO3 −<br />

127 I-<br />

127 IO3 − 129 I − 129 IO3 −<br />

Oxgyen Salinity<br />

0.14 0.44 0.52 −0.03 0.49<br />

0.37 0.36 −0.2 0.55<br />

0.79 −0.08 0.8<br />

−0.04 0.75<br />

Funding <strong>for</strong> <strong>the</strong> sampling was provided by <strong>the</strong> Swedish Meteorological<br />

and Hydrological Institute (SMHI). We thank Lars Andersson<br />

and Bodil Thorstensson and all <strong>the</strong> crew and scientific team on<br />

board <strong>of</strong> <strong>the</strong> research vessel Argos <strong>for</strong> <strong>the</strong> help during <strong>the</strong> sampling<br />

expeditions. X.L. Hou appreciates <strong>the</strong> support by “BaiRen” Project <strong>of</strong><br />

CAS (Grant No. KZCX2-YW-BR-13).

Hooray! Your file is uploaded and ready to be published.

Saved successfully!

Ooh no, something went wrong!