Thesis for the Degree of Doctor of Philosophy - DTU Orbit

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Paper I Hou, X.L., Hansen, V., Aldahan, A., Possnert, G., Lind, O.C., Lujaniene, G. A review on speciation of iodine-129 in the environmental and biological samples. Analytica Chimic Acta. 2009, 632, 181-196
Review Analytica Chimica Acta 632 (2009) 181–196 Contents lists available at ScienceDirect Analytica Chimica Acta journal homepage: www.elsevier.com/locate/aca A review on speciation of iodine-129 in the environmental and biological samples Xiaolin Hou a,∗ , Violeta Hansen a , Ala Aldahan b , Göran Possnert c , Ole Christian Lind d , Galina Lujaniene e a Risø National Laboratory for Sustainable Energy, NUK-202, Technical University of Denmark, DK-4000 Roskilde, Denmark b Department of Earth Science, Uppsala University, SE-758 36 Uppsala, Sweden c Tandem Laboratory, Uppsala University, SE-751 21 Uppsala, Sweden d Norwegian University of Life Science, N-1432, Ås, Norway e Institute of Physics, Savanoriu 231, LT-0230 Vilnius, Lithuania article info Article history: Received 25 August 2008 Received in revised form 2 November 2008 Accepted 6 November 2008 Available online 17 November 2008 Keywords: Iodine-129 Speciation analysis Tracer Bioavailability Environmental sample Contents abstract As a long-lived beta-emitting radioisotope of iodine, 129 I is produced both naturally and as a result of human nuclear activities. At present time, the main part of 129 I in the environment originates from the human nuclear activity, especially the releases from the spent nuclear fuel reprocessing plants, the 129 I/ 127 I ratios have being reached to values of 10 −10 to 10 −4 in the environment from 10 −12 in the pre-nuclear era. In this article, we review the occurrence, sources, inventory, and concentration level of 129 I in environment and the method for speciation analysis of 129 I in the environment. Measurement techniques for the determination of 129 I are presented and compared. An overview of applications of 129 I speciation in various scientific disciplines such as radiation protection, waste depository, and environmental sciences is given. In addition, the bioavailability and radiation toxicity (dose to thyroid) of 129 I are discussed. © 2008 Elsevier B.V. All rights reserved. 1. Introduction ......................................................................................................................................... 182 2. Iodine in the nature and its speciation.............................................................................................................. 182 2.1. Speciation of iodine in water ................................................................................................................ 182 2.2. Speciation of iodine in biological and environmental samples ............................................................................. 183 2.3. Speciation of iodine in atmosphere ......................................................................................................... 184 2.4. Speciation of iodine in soil and sediment ................................................................................................... 184 3. Sources, inventory, and concentration level of 129 I in the environment............................................................................ 184 4. Measurement of 129 I................................................................................................................................. 185 4.1. Gamma and X-ray spectrometry............................................................................................................. 185 4.2. Liquid scintillation counting (LSC) .......................................................................................................... 185 4.3. Neutron activation analysis ................................................................................................................. 185 4.4. Accelerator mass spectrometry (AMS) ...................................................................................................... 187 4.5. Inductively coupled plasma mass spectrometry (ICP-MS) .................................................................................. 188 5. Speciation analysis of 129 I in environmental and biological samples and its application .......................................................... 188 5.1. Speciation of 129 Iinwater................................................................................................................... 188 5.2. Speciation of 129 I in atmosphere ............................................................................................................ 190 Abbreviations: AMS, accelerator mass spectrometry; AmAD, activity median aerodynamic diameter; DIT, diiodotyrosine; DRC, dynamic collision/reaction cell; EXAFS, extended X-ray absorption fine structure spectra; HpGe, high purity germanium; HPLC, high performance liquid chromatography; ICP-MS, inductively coupled plasma mass spectrometry; LSC, liquid scintillation counter; MIT, monoiodothyrosine; NAA, neutron activation analysis; SIMS, secondary ion mass spectrometry; T3, triiodothyronine; rT3, reverse-triiodothyronine; T4, thyroxine; TBAH, tetrabutylammoniumhydroxide; TEDA, triethylenediamine; TBP/OK, tri-n-butyl phosphate in odourless kerosene; XANES, X-ray absorption near-edge structure. ∗ Corresponding author. Tel.: +45 4677 5357; fax: +45 4677 5347. E-mail address: xiaolin.hou@risoe.dk (X. Hou). 0003-2670/$ – see front matter © 2008 Elsevier B.V. All rights reserved. doi:10.1016/j.aca.2008.11.013
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Chemical Speciation Analysis and En
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Thesis for the Degree of Doctor of
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Abstract This thesis deals with che
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environment since they reflect the
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organiske jodformer. Adsorption af
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None of this would have been possib
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Abbreviations and acronyms b+ - pos
Page 15 and 16: 3.1 Analytical Development………
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: http://www.irsn.fr/EN/news/Document
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
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References Aldahan A, Kekli A, Poss
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Partition of iodine ( 129 I and 127
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Norway (Table 1). CTD-casts with ox
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5. Discussion 5.1. Separation of hu
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In the present study 40e60% of 129
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Hutta, M., Gora, R., 2003. Novel st
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Analysis of 129 I and 127 I in arch
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et al., 2002). Due to the fact that
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espectively. The iodine was leached
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salinities in the same area. Apart
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North Sea. 129 I/ 127 I ratios in w
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Table 2 Analytical results of 129-I
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129 I/ 127 I 1,40E-07 1,20E-07 1,00
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References Aldahan A, Englund E, Po
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O’Dowd, C.; Jimenez, J. L.; Bahre
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Iodine ( 129 I and 127 I) speciatio
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water in winter by molecular oxygen
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0.2 M KNO3. The effluent and the wa
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maximum values is at 0.03-0.06×10
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into the English Channel from the L
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References Aldahan A, Kekli A, Poss
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Risø-PhD-81(EN)
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Thesis for the Degree of Doctor of Philosophy - DTU Orbit

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