Effect of solution chemistry on the iodine release from iodoapatite in aqueous environments

Zhang, Zelong; Gustin, Léa; Xie, Weiwei; Lian, Jie; Valsaraj, Kalliat T.; Wang, Jianwei

doi:10.1016/j.jnucmat.2019.07.034

Effect of solution chemistry on the iodine release from iodoapatite in aqueous environments

Journal Article · Sat Jul 27 00:00:00 EDT 2019 · Journal of Nuclear Materials

DOI:https://doi.org/10.1016/j.jnucmat.2019.07.034· OSTI ID:1600976

Zhang, Zelong ^[1]; Gustin, Léa ^[2]; Xie, Weiwei ^[3]; Lian, Jie ^[4]; Valsaraj, Kalliat T. ^[3]; Wang, Jianwei ^[3]

Louisiana State Univ., Baton Rouge, LA (United States); Louisiana State University
Louisiana State Univ., Baton Rouge, LA (United States); Univ. of Wisconsin, Madison, WI (United States)
Louisiana State Univ., Baton Rouge, LA (United States)
Rensselaer Polytechnic Inst., Troy, NY (United States)

To ensure the safe disposal of nuclear waste, understanding the release process of radionuclides retained in the nuclear waste forms is of vital importance. Iodoapatite Pb_9.85(VO₄)₆I_1.7, a potential waste form for iodine-129, was selected as a model system for ceramic waste forms in this study to understand the effect of aqueous species on iodine release. Semi-dynamic leaching tests were conducted on bulk samples in cap-sealed Teflon vessels with 0.1 mol/L NaCl, Na₂CO₃, Na₃PO₄, and Na₂SO₄ solutions under 90 °C, fixed sample surface area to solution volume ratio of 5/m, and periodic replacement of leaching solutions. The reacted solutions were then analyzed by Inductively Coupled Plasma-Mass Spectrometry and Inductively Coupled Plasma-Optical Emission Spectrometry; the leached surfaces were characterized by X-ray diffraction, scanning electron microscopy, and infrared spectroscopy. The finding shows that, compared to deionized water, the ion-rich solutions enhanced the iodine release as a result of the increased ionic strength, reduced activity coefficient of dissolved species, and increased solution pH. Surface reactions can lead to the formations of secondary phases by ion-exchange and precipitation. These findings indicate that an ion-rich environment in the geological repository can be detrimental to the disposal safety of the nuclear waste form.

View Accepted Manuscript (DOE)

Research Organization:: Energy Frontier Research Centers (EFRC) (United States). Center for Performance and Design of Nuclear Waste Forms and Containers (WastePD); Louisiana State Univ., Baton Rouge, LA (United States); Rensselaer Polytechnic Inst., Troy, NY (United States)

Sponsoring Organization:: USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22)

Grant/Contract Number:: SC0016584

OSTI ID:: 1600976

Alternate ID(s):: OSTI ID: 1562593
OSTI ID: 22882241

Journal Information:: Journal of Nuclear Materials, Journal Name: Journal of Nuclear Materials Journal Issue: C Vol. 525; ISSN 0022-3115

Publisher:: ElsevierCopyright Statement

Country of Publication:: United States

Language:: English

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