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

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

doi:10.1016/j.apgeochem.2015.12.017

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

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Abstract

We proposed sodalites 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. We produced two samples made using a steam reformer samples using nonradioactive 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. Moreover, the similar releases of Re and Tc in the SPFT test, and the similar time-dependent shapesmore »« less

Authors:

Neeway, James J. ^[1]; Qafoku, Nikolla P. ^[1]; Williams, Benjamin D. ^[1]; Snyder, Michelle M. V. ^[1]; Brown, Christopher F. ^[1]; Pierce, Eric M. ^[2]

Pacific Northwest National Lab. (PNNL), Richland, WA (United States)
Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States)

Publication Date:: Thu Dec 31 00:00:00 EST 2015

Research Org.:: Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States)

Sponsoring Org.:: USDOE Office of Environmental Management (EM)

OSTI Identifier:: 1265816

Alternate Identifier(s):: OSTI ID: 1249912

Grant/Contract Number:: AC05-00OR22725; AC06-76RLO 1830

Resource Type:: Accepted Manuscript

Journal Name:: Applied Geochemistry

Additional Journal Information:: Journal Volume: 66; Journal Issue: C; Journal ID: ISSN 0883-2927

Publisher:: Elsevier

Country of Publication:: United States

Language:: English

Subject:: 12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE WASTES FROM NUCLEAR FACILITIES; Technetium; Radioactive waste form; Mineral dissolution; Sodalite

Citation Formats


                    Neeway, James J., Qafoku, Nikolla P., Williams, Benjamin D., Snyder, Michelle M. V., Brown, Christopher F., and Pierce, Eric M. Evidence of technetium and iodine release from a sodalite-bearing ceramic waste form.  United States: N. p., 2015. 
Web.  doi:10.1016/j.apgeochem.2015.12.017.

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                    Neeway, James J., Qafoku, Nikolla P., Williams, Benjamin D., Snyder, Michelle M. V., Brown, Christopher F., & Pierce, Eric M. Evidence of technetium and iodine release from a sodalite-bearing ceramic waste form.  United States.  https://doi.org/10.1016/j.apgeochem.2015.12.017

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                    Neeway, James J., Qafoku, Nikolla P., Williams, Benjamin D., Snyder, Michelle M. V., Brown, Christopher F., and Pierce, Eric M. Thu .  
"Evidence of technetium and iodine release from a sodalite-bearing ceramic waste form".  United States.  https://doi.org/10.1016/j.apgeochem.2015.12.017.  https://www.osti.gov/servlets/purl/1265816.

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@article{osti_1265816,

  title        = {Evidence of technetium and iodine release from a sodalite-bearing ceramic waste form},

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

  abstractNote = {We proposed sodalites 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. We produced two samples made using a steam reformer samples using nonradioactive 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. Moreover, 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.},

  doi          = {10.1016/j.apgeochem.2015.12.017},

  journal      = {Applied Geochemistry},

  number       = C,

  volume       = 66,

  place        = {United States},

  year         = {Thu Dec 31 00:00:00 EST 2015},

  month        = {Thu Dec 31 00:00:00 EST 2015}

}

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