Abstract
Extended X-ray absorption fine structure (EXAFS) spectroscopy at the iodine K-edge was performed to investigate the immobilization of iodide by AFm-Cl2/CO3/SO4 phases. AFm-I2 and various compositions of AFm-(I2, Cl2), AFm-(I2, CO3), and AFm-(I2, SO4) were synthesized by coprecipitation and exchange reaction. X-ray diffraction (XRD) showed that AFm-(I2, Cl2) sample crystallize in two separate crystalline phases AFm-I2 and AFm-Cl2. This finding was supported by EXAFS measurements, which showed that the coordination environment of iodine is similar for AFm-(I2, Cl2) and pure AFm-I2. AFm-(I2, CO3) interlayers alternately filled with I− and with (OH−–CO3 2−) were observed by XRD, whereas a more limited short-range ordering of iodide was found by EXAFS spectroscopy. XRD indicated that AFm-(I2, SO4) forms a solid solution between AFm-I2 and AFm-SO4. In addition, the EXAFS spectra revealed that I− and SO4 2− occupy neighbouring positions. The formation of an AFm-I2–AFm-SO4 solid solution together with the complete mixing of I− and SO4 2− confirms the capability of AFm-SO4 to trap 129I.
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References
Nagra (2002): Technical Report. NTB 02-05.
Bonhoure, I, Scheidegger, AM, Wieland, E, and Dähn, R (2002): Iodine species uptake by cement and CSH studied by I K-edge X-ray absorption spectroscopy. Radiochimica Acta (90): 647–651.
Atkins, M, Beckley, AN, and Glasser, FP (1988): Influence of cement on the near-field environment and its specific interactions with uranium and iodine. Radiochimica Acta (44–45): 255–261.
Rapin, JP, Walcarius, A, Lefèvre, G, and Francois, M (1999): A double-layered hydroxide, 3CaO×Al2O3×CaI2×10H2O. Acta Crystallographica Section C-Crystal Structure Communications (55): 1957–1959.
Walcarius, A, Lefèvre, G, Rapin, JP, Renaudin, G, and Francois, M (2001): Voltammetric detection of iodide after accumulation by Friedel's salt. Electroanalysis (13): 313–320.
Evans, DG, and Slade, RCT (2006): Structural aspects of layered double hydroxides. In: Layered Double Hydroxides (119): 1–87.
Kuzel, HJ, and Pöllmann, H (1991): Hydration of C3A in the presence of Ca(OH)2, CaSO4×2H2O and CaCO3. Cement and Concrete Research (21): 885–895.
Brown, DR, and Grutzeck, MW (1985): The synthesis and characterization of calcium aluminate monoiodide. Cement and Concrete Research (15): 1068–1078.
Kuzel, HJ (1971): Zur Frage der Mischkristallbildung von Calciumaluminiumhydroxysalzen. Neues Jahrbuch für Mineralogie, Monatshefte: 477–491.
Reed, WA, May, I, Livens, FR, Charnock, JM, Jeapes, AP, Gresley, M, Mitchell, RM, and Knight, P (2002): XANES fingerprinting of iodine species in solution and speciation of iodine in spent solvent from nuclear fuel reprocessing. Journal of Analytical Atomic Spectrometry (17): 541–543.
Yamaguchi, N, Nakano, M, Tanida, H, Fujiwara, H, and Kihou, N (2006): Redox reaction of iodine in paddy soil investigated by field observation and the I K-edge XANES fingerprinting method. Journal of Environmental Radioactivity (86): 212–226.
Kodama, S, Takahashi, Y, Okumura, K, and Uruga, T (2006): Speciation of iodine in solid environmental samples by iodine K-edge XANES: application to soils and ferromanganese oxides. Science of the Total Environment (363): 275–284.
Shimamoto, YS, and Takahashi, Y (2008): Superiority of K-edge XANES over L-III-edge XANES in the speciation of iodine in natural soils. Analytical Sciences (24): 405–409.
D’Angelo, P, Zitolo, A, Migliorati, V, and Pavel, NV (2008): Measurement of X-ray multielectron photoexcitations at the I- K edge. Physical Review B (78): 144105.
Gomilsek, JP, Arcon, I, De Panfilis, S, and Kodre, A (2009): X-ray absorption in atomic iodine in the K-edge region. Physical Review A (79): 032514.
Yagi, K, Umezawa, S, Terauchi, H, and Kasatani, H (2001): EXAFS study of phase transitions in KIO3. Journal of Synchrotron Radiation (8): 803–805.
Lezama-Pacheco, J, De Leon, JM, Espinosa, FJ, Rabago, F, and Conradson, S (2004): Local atomic structure around iodine in ZnSe:I. Solar Energy Materials and Solar Cells (82): 151–157.
Michel, T, Alvarez, L, Sauvajol, JL, Almairac, R, Aznar, R, Bantignies, JL, and Mathon, O (2006): EXAFS investigations of iodine-doped carbon nanotubes. Physical Review B (73): 195419.
Feiters, MC, Kupper, FC, and Meyer-Klaucke, W (2005): X-ray absorption spectroscopic studies on model compounds for biological iodine and bromine. Journal of Synchrotron Radiation (12): 85–93.
Hou, XQ, Bish, DL, Wang, SL, Johnston, CT, and Kirkpatrick, RJ (2003): Hydration, expansion, structure, and 15 dynamics of layered double hydroxides. American Mineralogist (88): 167–179.
Matschei, T, Lothenbach, B, and Glasser, FP (2007): The AFm phase in Portland cement. Cement and Concrete Research (37): 118–130.
Ravel, B, and Newville, M (2005): ATHENA, ARTEMIS, HEPHAESTUS: data analysis for X-ray absorption spectroscopy using IFEFFIT. Journal of Synchrotron Radiation (12): 537–541.
Taviot-Guého, C, Feng, YJ, Faour, A, and Leroux, F (2010): Intercalation chemistry in a LDH system: anion exchange process and staging phenomenon investigated by means of time-resolved, in situ X-ray diffraction. Dalton Transactions (39): 5994–6005.
Acknowledgments
The authors thank Dr. Barbara Lothenbach (Empa) for providing the C3A and for valuable advice during sample preparation. Thanks are extended to the beamline scientists of the DUBBLE beamline (ESRF, Grenoble, France) for their technical support. Dr. Urs Eggenberger and Christoph Wanner (UniBern) are acknowledged for assistance during the XRD measurements. Financial support was provided by the Helmholtz virtual institute of advanced solid-aqueous radio-geochemistry and by the National Cooperative for the Disposal of Radioactive Waste (Nagra), Switzerland.
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Aimoz, L., Wieland, E., Taviot-Guého, C., Vespa, M., Dähn, R. (2012). Iodine K-Edge Exafs Spectroscopy of Iodine-Bearing AFm-(Cl2, CO3, SO4). In: Broekmans, M. (eds) Proceedings of the 10th International Congress for Applied Mineralogy (ICAM). Springer, Berlin, Heidelberg. https://doi.org/10.1007/978-3-642-27682-8_1
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