Ion-Exchange Interdiffusion Model with Potential Application to Long-Term Nuclear Waste Glass Performance

Neeway, James Joseph; Kerisit, Sebastien N.; Liu, Jia; Zhang, Jiandong; Zhu, Zihua; Riley, Brian Joseph; Ryan, Joseph Vincent

doi:10.1021/acs.jpcc.6b03681

Ion-Exchange Interdiffusion Model with Potential Application to Long-Term Nuclear Waste Glass Performance

Journal Article · Tue Apr 12 00:00:00 EDT 2016 · Journal of Physical Chemistry. C

DOI:https://doi.org/10.1021/acs.jpcc.6b03681· OSTI ID:1327120

Neeway, James Joseph ^[1]; Kerisit, Sebastien N. ^[1]; Liu, Jia ^[1]; Zhang, Jiandong ^[1]; Zhu, Zihua ^[1]; Riley, Brian Joseph ^[1]; Ryan, Joseph Vincent ^[1]

Pacific Northwest National Laboratory (PNNL), Richland, WA (United States)

Ion exchange is an integral mechanism influencing the corrosion of glasses. Due to the formation of alteration layers in aqueous conditions, it is difficult to conclusively deconvolute the process of ion exchange from other processes, principally dissolution of the glass matrix. Therefore, we have developed a method to isolate alkali diffusion that involves contacting glass coupons with a solution of ⁶LiCl dissolved in functionally inert dimethyl sulfoxide. Here, we employ the method at temperatures ranging from 25 to 150 °C with various glass formulations. Glass compositions include simulant nuclear waste glasses, such as SON68 and the international simple glass (ISG), glasses in which the nature of the alkali element was varied, and glasses that contained more than one alkali element. An interdiffusion model based on Fick’s second law was developed and applied to all experiments to extract diffusion coefficients. The model expands established models of interdiffusion to the case where multiple types of alkali sites are present in the glass. Activation energies for alkali ion exchange were calculated and the results are in agreement with those obtained in glass strengthening experiments but are nearly five times higher than values reported for diffusion-controlled processes in nuclear waste glass corrosion experiments. A discussion of the root causes for this apparent discrepancy is provided. The interdiffusion model derived from laboratory experiments is expected to be useful for modeling glass corrosion in a geological repository when the silicon concentration is high.

View Accepted Manuscript (DOE)

Research Organization:: Pacific Northwest National Laboratory (PNNL), Richland, WA (United States)

Sponsoring Organization:: USDOE Office of Nuclear Energy (NE); USDOE Office of Science (SC), Biological and Environmental Research (BER)

Grant/Contract Number:: AC05-76RL01830

OSTI ID:: 1327120

Report Number(s):: PNNL-SA--116172; 47580; 49141; AF5805010

Journal Information:: Journal of Physical Chemistry. C, Journal Name: Journal of Physical Chemistry. C Journal Issue: 17 Vol. 120; ISSN 1932-7447

Publisher:: American Chemical SocietyCopyright Statement

Country of Publication:: United States

Language:: English

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