Thesis for the Degree of Doctor of Philosophy - DTU Orbit

More documents

Recommendations

Info

Table of Contents 1 Introduction……………………………………………………………………………………….……..….14 1.1 Iodine in nature………………………………………………………………………………………....14 1.1.1 Stable iodine ( 127 I)…………………………………………………………………………………..14 1.1.2 Radioactive iodine ( 129 I)………………………………………………………………………….....17 1.1.2.1 Natural sources……………………………………………………………………………………18 1.1.2.2 Anthropogenic sources……………………………………………………………………………18 1.2 Measurement of 129 I and 127 I…………………………………………………………………………..…20 1.3 Chemical speciation analysis …………………………………………………………………..………22 1.4 Overview of analytical techniques for chemical speciation analysis of iodine ( 129 I and 127 I) in environmental samples………………………………………………………………………………...……23 1.4.1 Speciation analysis of 127 I and 129 I in fresh and seawater…………………………………………...23 1.4.2. Speciation analysis of 127 I and 129 I in soil and sediment………………………………….…………24 1.4.3 Speciation analysis of 127 I and 129 I in seaweed………………………………………………………25 1.5 Scope of the study………………………………………………………………………………………26 2 Analytical procedures used in this work……………………………................……………………………..27 2.1 Experimental materials………………………………………………………………….......………….27 2.2 On-line HPLC-ICP-MS method for the direct speciation analysis of 127 I in water and leachate of soil and sediment samples………………………………………………………………………………………27 2.3 Quantification of total iodine including iodine organic and inorganic species in fresh water and seawater samples by adsorption onto activated charcoal and DEAE 32 cellulose………….…………...…29 2.4 Quantification of total iodine in fresh water by oxidation of organic matter followed by reduction to iodide of all species and precipitation as silver iodine……………………………………………………..31 2.5 A rapid method for quantification of total iodine including iodine organic and inorganic species in fresh water and seawater samples by NaClO and NaOH oxidation of iodine species…………………………....32 2.6 Chemical speciation analysis of 129 I and 127 I in soil and sediment …………………………………….32 2.7 Chemical speciation analysis of 129 I and 127 I (as iodide and iodate) in fresh water and seawater ….….33 2.8 Analysis of 129 I and 127 I total concentration in seaweed samples………………………………………33 2.9 Extraction of iodine from leachate seaweed, soil, sediment and eluent and effluent of water samples……………………………………………………………………………………………………...34 2.10 Preparation of 129 I for AMS measurements………………………………………...…………………34 2.11 127 I preparation for ICP-MS measurements………………………………………...…………………34 3 Results and Discussion…………………………………………………….………………………………36 12
3.1 Analytical Development……… ……………..……………………………………….………………..36 3.1.1 Optimization of HPLC-ICP-MS chromatographic parameters for chemical speciation analysis of 127 I in water samples and leachate from soil and sediments…………………………………………….…………36 3.1.2 Quantification of total concentration of iodine in fresh and seawater samples by adsorption on activated charcoal or DEAE 32 cellulose……………………………………………………………………………..38 3.1.3 Quantification of total concentration of iodine including iodine organic and inorganic species in fresh and seawater samples by oxidation of iodine organic matter followed by reduction of iodine species and precipitation……………………………………………………………………………………..………….41 3.2 Analytical Development and Environmental Studies……………………………………………………..44 3.2.1 Speciation analysis of iodine as iodide, iodate and total iodine in fresh water samples by alkaline oxidation with NaOH - NaClO for total iodine and anion exchange chromatography for separation of iodide and iodate……………………………………………………………………………………………44 3.2.2 Partition of Iodine ( 129 I and 127 I) Isotopes in Soil and Marine Sediments...............................................45 3.3 Environmental studies…………………………………………………...………………………...………45 3.3.1 Speciation analysis of iodine as iodide, iodate and total iodine in seawater profile samples by collected from Baltic Proper, Skagerrak and Kattegat……………………………………………………..…………45 3.3.2 Spatial and temporal variation of 129 I and 127 I by analysis of archived Fucus Vesiculosus samples from Denmark …………………………....……………………………………………………………………...49 4 Conclusions and recommendations (perspectives)…………………………………..………………………53 Reference……………………………………………………………………….…………………………….56 13
Page 1 and 2: Chemical Speciation Analysis and En
Page 3 and 4: Thesis for the Degree of Doctor of
Page 5 and 6: Abstract This thesis deals with che
Page 7 and 8: environment since they reflect the
Page 9 and 10: organiske jodformer. Adsorption af
Page 11 and 12: None of this would have been possib
Page 13: Abbreviations and acronyms b+ - pos
Page 17 and 18: Table 1 Some properties of iodine P
Page 19 and 20: In soils/sediments iodine occurs as
Page 21 and 22: Table 2 Nuclear properties of iodin
Page 23 and 24: Liquid scintillation counting (LSC)
Page 25 and 26: The bioavailability of radioactive
Page 27 and 28: data (Englund et al., 2010; Hou et
Page 29 and 30: 2. Analytical procedures used in th
Page 31 and 32: 2.3 Quantification of total iodine
Page 33 and 34: Fig. 5 Quantification of total iodi
Page 35 and 36: iodate were measured by counting 12
Page 37 and 38: Fig. 6 Sequential extraction proced
Page 39 and 40: a Fig. 8 Calibration curve for (a)
Page 41 and 42: experiment was subjected to combust
Page 43 and 44: Table 7 Adsorption of iodine specie
Page 45 and 46: numbers 11-14), which is about the
Page 47 and 48: marine environment from nuclear fue
Page 49 and 50: 127 I - (ppb) 127 IO3 - (ppb) a b 1
Page 51 and 52: Although the oxygen concentration d
Page 53 and 54: 129 I TBq 2,00E+00 1,80E+00 1,60E+0
Page 55 and 56: • Adsorption of iodine species on
Page 57 and 58: Reference Aldahan A, Kekli A, Possn
Page 59 and 60: Fuge R& Johnson C. 1986. The geoche
Page 61 and 62: Lo´pez-Gutie´rrez JM, Garcı ´a-
Page 63 and 64: Shinohara K. 2004. Measurement and
Page 65 and 66:
http://www.irsn.fr/EN/news/Document
Page 67 and 68:
Review Analytica Chimica Acta 632 (
Page 69 and 70:
Table 1 Nuclear properties and prod
Page 71 and 72:
Fig. 2. Liquid discharges of 129 I
Page 73 and 74:
Fig. 5. Schematic diagram and pictu
Page 75 and 76:
129 I in iodide and iodate is then
Page 77 and 78:
Fig. 8. Diagram of air sampler for
Page 79 and 80:
Fig. 10. Iodine L3-edge (a) and K-e
Page 81 and 82:
analysis of 129 I in water sample a
Page 83 and 84:
Yi P, Aldahan A, Hansen V, Possnert
Page 85 and 86:
FIGURE 1. Sampling sites (the red s
Page 87 and 88:
FIGURE 3. Horizontal distribution o
Page 89 and 90:
FIGURE 5. Time series data of 129 I
Page 91 and 92:
Environmental Science & Technology
Page 93 and 94:
prepared using KI and KIO3. No diff
Page 95 and 96:
of their contribution to the Baltic
Page 97 and 98:
Fig. S-1 Sampling sites (the red so
Page 99 and 100:
Fig. S-3 Vertical distribution of I
Page 101 and 102:
Fig. S-5 Marine discharges function
Page 103 and 104:
Fig.S-7 Relationship between I-129
Page 105 and 106:
Table S-1 Results of I-129 and I-12
Page 107 and 108:
S17
Page 109 and 110:
Paper III Hansen,V., Yi, P., Hou, X
Page 111 and 112:
conversion process between iodide a
Page 113 and 114:
Table 1 Analytical results of 129 I
Page 115 and 116:
August April I-129 iodide ( 10 8 at
Page 117 and 118:
References Aldahan A, Kekli A, Poss
Page 119 and 120:
Partition of iodine ( 129 I and 127
Page 121 and 122:
Norway (Table 1). CTD-casts with ox
Page 123 and 124:
5. Discussion 5.1. Separation of hu
Page 125 and 126:
In the present study 40e60% of 129
Page 127 and 128:
Hutta, M., Gora, R., 2003. Novel st
Page 129 and 130:
Analysis of 129 I and 127 I in arch
Page 131 and 132:
et al., 2002). Due to the fact that
Page 133 and 134:
espectively. The iodine was leached
Page 135 and 136:
salinities in the same area. Apart
Page 137 and 138:
North Sea. 129 I/ 127 I ratios in w
Page 139 and 140:
Table 2 Analytical results of 129-I
Page 141 and 142:
129 I/ 127 I 1,40E-07 1,20E-07 1,00
Page 143 and 144:
References Aldahan A, Englund E, Po
Page 145 and 146:
O’Dowd, C.; Jimenez, J. L.; Bahre
Page 147 and 148:
Iodine ( 129 I and 127 I) speciatio
Page 149 and 150:
water in winter by molecular oxygen
Page 151 and 152:
0.2 M KNO3. The effluent and the wa
Page 153 and 154:
maximum values is at 0.03-0.06×10
Page 155 and 156:
into the English Channel from the L
Page 157 and 158:
References Aldahan A, Kekli A, Poss
Page 160 and 161:
Risø-PhD-81(EN)
show all

Thesis for the Degree of Doctor of Philosophy - DTU Orbit

Create successful ePaper yourself

Delete template?

Save as template?