Evidence of technetium and iodine release from a sodalite-bearing ceramic waste form

James J. Neeway, Nikolla P. Qafoku, Benjamin D. Williams, Michelle M.V. Snyder, Christopher F. Brown, Eric M. Pierce

Research output: Contribution to journalArticlepeer-review

11 Scopus citations

Abstract

Sodalites have been proposed as a possible host of certain radioactive species, specifically 99Tc and 129I, which may be encapsulated into the cage structure of the mineral. To demonstrate the ability of this framework silicate mineral to encapsulate and immobilize 99Tc and 129I, single-pass flow-through (SPFT) tests were conducted on a sodalite-bearing multi-phase ceramic waste form produced through a steam reforming process. Two samples made using a steam reformer samples were produced using non-radioactive I and Re (as a surrogate for Tc), while a third sample was produced using actual radioactive tank waste containing Tc and added Re. One of the non-radioactive samples was produced with an engineering-scale steam reformer while the other non-radioactive sample and the radioactive sample were produced using a bench-scale steam reformer. For all three steam reformer products, the similar steady-state dilute-solution release rates for Re, I, and Tc at pH (25 °C) = 9 and 40 °C were measured. However, it was found that the Re, I, and Tc releases were equal or up to 4.5x higher compared to the release rates of the network-forming elements, Na, Al, and Si. The similar releases of Re and Tc in the SPFT test, and the similar time-dependent shapes of the release curves for samples containing I, suggest that Re, Tc, and I partition to the sodalite minerals during the steam reforming process.

Original languageEnglish
Pages (from-to)210-218
Number of pages9
JournalApplied Geochemistry
Volume66
DOIs
StatePublished - Mar 1 2016

Funding

These studies were supported by the U.S. Department of Energy (DOE) through the Office of Environmental Management . Pacific Northwest National Laboratory (PNNL) is operated for the DOE by Battelle Memorial Institute under Contract DE-AC06-76RLO 1830. We would like to recognize our PNNL colleagues Elsa Cordova, Sara Strandquist, DeNomy Dage, Jesse Lang, Michael Schweiger, and Cristian Iovin for the contributions to the tests used in this study, as well as the Savannah River National Laboratory (SRNL) team who prepared the samples, including Carol Jantzen, Charles Crawford, Christopher Bannochie, Paul Burket, Alex Cozzi, Gene Daniel, Connie Herman, Charles Nash, Donald Miller, and Holly Hall. We would also like to thank R. Jeffrey Serne of PNNL and Carol Jantzen of SRNL for their helpful comments to greatly improve the quality of this paper. Heather Culley (PNNL) provided technical editing of this document.

FundersFunder number
U.S. Department of Energy
BattelleDE-AC06-76RLO 1830
Office of Environmental Management

    Keywords

    • Mineral dissolution
    • Radioactive waste form
    • Sodalite
    • Technetium

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