Abstract
The environmental fate of iodine is of general geochemical interest as well as of substantial concern in the context of nuclear waste repositories and reprocessing plants. Soils, and in particular soil organic matter (SOM), are known to play a major role in retaining and storing iodine. Therefore, we investigated iodide and iodate sorption by four different reference soils for contact times up to 30 days. Selective sequential extractions and X-ray absorption spectroscopy (XAS) were used to characterize binding behavior to different soil components, and the oxidation state and local structure of iodine. For iodide, sorption was fast with 73 to 96% being sorbed within the first 24 h, whereas iodate sorption increased from 11–41% to 62–85% after 30 days. The organic fraction contained most of the adsorbed iodide and iodate. XAS revealed a rapid change of iodide into organically bound iodine when exposed to soil, while iodate did not change its speciation. Migration behavior of both iodine species has to be considered as iodide appears to be the less mobile species due to fast binding to SOM, but with the potential risk of mobilization when oxidized to iodate.
This is a preview of subscription content, log in via an institution to check access.
Similar content being viewed by others
References
Amachi S, Fujii T, Muramatsu Y (2005) Microbial influences on the mobility and transformation of radioactive iodine in the environment. J Nucl Radiochem Sci 6:21–24. https://doi.org/10.14494/jnrs2000.6.21
Ankudinov AL, Rehr JJ (1997) Relativistic calculations of spin-dependent x-ray-absorption spectra. Phys Rev B 56:1712–1728. https://doi.org/10.1103/PhysRevB.56.R1712
Bowley HE, Young SD, Ander EL, Crout NMJ, Watts MJ, Bailey EH (2016) Iodine binding to humic acid. Chemosphere 157:208–214. https://doi.org/10.1016/j.chemosphere.2016.05.028
Cardis E, Kesminiene A, Ivanov V, Malakhova I, Shibata Y, Khrouch V, Drozdovitch V, Maceika E, Zvonova I, Vlassov O, Bouville A, Goulko G, Hoshi M, Abrosimov A, Anoshko J, Astakhova L, Chekin S, Demidchik E, Galanti R, Ito M, Korobova E, Lushnikov E, Maksioutov M, Masyakin V, Nerovnia A, Parshin V, Parshkov E, Piliptsevich N, Pinchera A, Polyakov S, Shabeka N, Suonio E, Tenet V, Tsyb A, Yamashita S, Williams D (2005) Risk of thyroid cancer after exposure to (131) I in childhood. J Natl Cancer Inst 97:724–732. https://doi.org/10.1093/jnci/dji129
Cortona P (1992) Direct determination of self-consistent Total energies and charge-densities of solids - a study of the cohesive properties of the alkali-halides. Phys Rev B 46:2008–2014. https://doi.org/10.1103/PhysRevB.46.2008
Dai JL, Zhang M, Zhu YG (2004) Adsorption and desorption of iodine by various Chinese soils - I. iodate. Environ Int 30:525–530. https://doi.org/10.1016/j.envint.2003.10.007
Dai JL, Zhang M, Hu QH, Huang YZ, Wang RQ, Zhu YG (2009) Adsorption and desorption of iodine by various Chinese soils: II. Iodide and iodate. Geoderma 153:130–135. https://doi.org/10.1016/j.geoderma.2009.07.020
Funke H, Scheinost AC, Chukalina M (2005) Wavelet analysis of extended x-ray absorption fine structure data. Phys Rev B 71:094110. https://doi.org/10.1103/PhysRevB.71.094110
Hamdouni N, Ouarda B, Medjroubi ML, Meinnel J, Boudjada A (2012) Iododurene. Acta Crystallogr Sect E: Crystallographic Communications 68:o3391. https://doi.org/10.1107/S1600536812046557
Hansen V, Roos P, Aldahan A, Hou X, Possnert G (2011) Partition of iodine (I-129 and I-127) isotopes in soils and marine sediments. J Environ Radioact 102:1096–1104. https://doi.org/10.1016/j.jenvrad.2011.07.005
Hormann V, Fischer HW (2013) Estimating the distribution of radionuclides in agricultural soils - dependence on soil parameters. J Environ Radioact 124:278–286. https://doi.org/10.1016/j.jenvrad.2013.06.010
Hou XL, Fogh CL, Kucera J et al (2003) Chemical fractionation of iodine-129 and cesium-137 in Chernobyl contaminated soil and Irish Sea sediment. Roy Soc Chem 291:410–417. https://doi.org/10.1039/9781847550781-00410
Jammoul A, Dumas S, D'Anna B, George C (2009) Photoinduced oxidation of sea salt halides by aromatic ketones: a source of halogenated radicals. Atmos Chem Phys 9:4229–4237. https://doi.org/10.5194/acp-9-4229-2009
Kaplan DI, Denham ME, Zhang S, Yeager C, Xu C, Schwehr KA, Li HP, Ho YF, Wellman D, Santschi PH (2014) Radioiodine biogeochemistry and prevalence in groundwater. Crit Rev Environ Sci Technol 44:2287–2335. https://doi.org/10.1080/10643389.2013.828273
Kocher DC(1981) A dynamic model of the global iodine cycle and estimation of dose to the world population from releases of iodine-129 to the environment. Environ Int 5(1):15–31
Lee YM, Kang CH, Hwang YS (2007) Nuclide release from an HLW repository: development of a compartment model. Ann Nucl Energy 34:782–791. https://doi.org/10.1016/j.anucene.2007.04.005
Lieser KH, Steinkopff T (1989) Chemistry of radioactive iodine in the hydrosphere and in the geosphere. Radiochim Acta 46:49–55. https://doi.org/10.1524/ract.1989.46.1.49
Louer M, Grandjean D, Weigel D (1973) Crystalline-structure and thermal-expansion of nickel iodide hexahydrate. J Solid State Chem 7:222–228. https://doi.org/10.1016/0022-4596(73
Lucas BW (1985) Structure (neutron) of potassium iodate at 100 and 10 k. Acta Crystallogr Sect C-Crystal Struct Commun 41:1388–1391. https://doi.org/10.1107/s0108270185007880
Luo MY, Hou XL, Zhou WJ, He C, Chen N, Liu Q, Zhang L (2013) Speciation and migration of I-129 in soil profiles. J Environ Radioact 118:30–39. https://doi.org/10.1016/j.jenvrad.2012.11.011
Muramatsu Y, Yoshida S (1999) Effects of microorganisms on the fate of iodine in the soil environment. Geomicrobiol J 16:85–93. https://doi.org/10.1080/014904599270776
Muramatsu Y, Uchida S, Sriyotha P, Sriyotha K (1990) Some considerations on the sorption and desorption phenomena of iodide and iodate on soil. Water Air Soil Pollut 49:125–138. https://doi.org/10.1007/Bf00279516
Nishimaki K, Satta N, Maeda M (1994) Sorption and migration of radioiodine in saturated sandy soil. J Nucl Sci Technol 31:828–838. https://doi.org/10.1080/18811248.1994.9735229
Reiller P, Moulin V (2003) Influence of organic matter in the prediction of iodine migration in natural environment. Mater Res Soc Symp P 757:565–570. https://doi.org/10.1524/ract.2006.94.9-11.739
Ressler T (1998) WinXAS: a program for X-ray absorption spectroscopy data analysis under MS-Windows. J Synchrotron Radiat 5:118–122. https://doi.org/10.1107/S0909049597019298
Scheinost AC, Abend S, Pandya KI, Sparks DL (2001) Kinetic controls on Cu and Pb sorption by ferrihydrite. Environ Sci Technol 35:1090–1096. https://doi.org/10.1021/Es000107m
Schlegel ML, Reiller P, Mercier-Bion F, Barré N, Moulin V (2006) Molecular environment of iodine in naturally iodinated humic substances: insight from X-ray absorption spectroscopy. Geochim Cosmochim Ac 70:5536–5551. https://doi.org/10.1016/j.gca.2006.08.026
Schwehr KA, Santschi PH, Kaplan DI (2009) Organo-iodine formation in aquifer sediments at ambient concentrations. Geochim Cosmochim Acta 73:A1187–A1187
Shetaya WH, Young SD, Watts MJ, Ander EL, Bailey EH (2012) Iodine dynamics in soils. Geochim Cosmochim Acta 77:457–473. https://doi.org/10.1016/j.gca.2011.10.034
Shimamoto YS, Takahashi Y, Terada Y (2011) Formation of organic iodine supplied as iodide in a soil-water system in Chiba, Japan. Environ Sci Technol 45:2086–2092. https://doi.org/10.1021/es1032162
Soderlund M, Virkanen J, Aromaa H et al (2017) Sorption and speciation of iodine in boreal forest soil. J Radioanal Nucl Chem 311:549–564. https://doi.org/10.1007/s10967-016-5022-z
Takeda A, Tsukada H, Takahashi M, Takaku Y, Hisamatsu S (2015) Changes in the chemical form of exogenous iodine in forest soils and their extracts. Radiat Prot Dosim 167:181–186. https://doi.org/10.1093/rpd/ncv240
Tanida H, Watanabe I (2000) Dependence of EXAFS (extended X-ray absorption fine structure) parameters of iodide anions in various solvents upon a solvent parameter. B Chem Soc Jpn 73:2747–2752. https://doi.org/10.1246/Bcsj.73.2747
Tigeras A, Bachet M, Catalette H, Simoni E (2011) PWR iodine speciation and behaviour under normal primary coolant conditions: an analysis of thermodynamic calculations, sensibility evaluations and NPP feedback. Prog Nucl Energy 53:504–515. https://doi.org/10.1016/j.pnucene.2011.02.002
Unno Y, Tsukada H, Takeda A, Takaku Y, Hisamatsu S' (2017) Soil-soil solution distribution coefficient of soil organic matter is a key factor for that of radioiodide in surface and subsurface soils. J Environ Radioact 169:131–136. https://doi.org/10.1016/j.jenvrad.2017.01.016
Watkins BM, Smith GM, Little RH, Kessler J (1999) A biosphere modeling methodology for dose assessments of the potential Yucca Mountain deep geological high level radioactive waste repository. Health Phys 76:355–367. https://doi.org/10.1097/00004032-199904000-00003
Webb SM (2006) Sixpack: a graphical user interface for XAS analysis using IFEFFIT. Phys Scr T115:1011–1014. https://doi.org/10.1238/Physica.Topical.115a01011
Whitehead DC (1973) Sorption of iodide by soils as influenced by equilibrium conditions and soil properties. J Sci Food Agric 24:547–556. https://doi.org/10.1002/jsfa.2740240508
Whitehead DC (1978) Iodine in soil profiles in relation to Iron and aluminum-oxides and organic-matter. J Soil Sci 29:88–94. https://doi.org/10.1111/j.1365-2389.1978.tb02035.x
World Reference Base (WRB) and IWG (2015): World reference base for soil resource 2014, update 2015. In: Erika SPVHCM (Hrsg.), International soil classification system for naming soils and creating legends for soil maps. World Soil Resources Reports No. 106. Food and Agriculture Organization of the United Nations (FAO) http://www.fao.org/3/i3794en/I3794en.pdf. Accessed 25 April 2019
Xu C, Zhang SJ, Ho YF, Miller EJ, Roberts KA, Li HP, Schwehr KA, Otosaka S, Kaplan DI, Brinkmeyer R, Yeager CM, Santschi PH (2011) Is soil natural organic matter a sink or source for mobile radioiodine (I-129) at the Savannah River Site? Geochim Cosmochim Acta 75:5716–5735. https://doi.org/10.1016/j.gca.2011.07.011
Xu C, Sugiyama Y, Hatcher PG et al. (2012a) Investigation of the radioiodine binding environment in terrestrial aquatic natural organic matter by FT-ICR-MS. Abstr Pap Am Chem S 243
Xu C, Zhong JY, Hatcher PG, Zhang S, Li HP, Ho YF, Schwehr KA, Kaplan DI, Roberts KA, Brinkmeyer R, Yeager CM, Santschi PH (2012b) Molecular environment of stable iodine and radioiodine (I-129) in natural organic matter: evidence inferred from NMR and binding experiments at environmentally relevant concentrations. Geochim Cosmochim Acta 97:166–182. https://doi.org/10.1016/j.gca.2012.08.030
Yamaguchi N, Nakano M, Takamatsu R, Tanida H (2010) Inorganic iodine incorporation into soil organic matter: evidence from iodine K-edge X-ray absorption near-edge structure. J Environ Radioact 101:451–457. https://doi.org/10.1016/j.jenvrad.2008.06.003
Zhang SJ, Ho YF, Creeley D, Roberts KA, Xu C, Li HP, Schwehr KA, Kaplan DI, Yeager CM, Santschi PH (2014) Temporal variation of iodine concentration and speciation (I-127 and I-129) in wetland groundwater from the Savannah River Site, USA. Environ Sci Technol 48:11218–11226. https://doi.org/10.1021/es502003q
Funding
We thank the Siebold-Sasse Foundation for funding our research.
Author information
Authors and Affiliations
Corresponding author
Additional information
Responsible editor: Roberto Terzano
Publisher’s note
Springer Nature remains neutral with regard to jurisdictional claims in published maps and institutional affiliations.
Rights and permissions
About this article
Cite this article
Köhler, F., Riebe, B., Scheinost, A.C. et al. Sorption of iodine in soils: insight from selective sequential extractions and X-ray absorption spectroscopy. Environ Sci Pollut Res 26, 23850–23860 (2019). https://doi.org/10.1007/s11356-019-05623-y
Received:
Accepted:
Published:
Issue Date:
DOI: https://doi.org/10.1007/s11356-019-05623-y