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Using Corroded Ancient Glasses as a Means to an Improved Understanding of the Long-term Chemical Reactivity of Glasses


EMSL Project ID
49141

Abstract

EMSL resources are requested to enable an international team of collaborators to solve fundamental problems in interfacial glass corrosion chemistry. With the recent dismissal of Yucca Mountain as a national nuclear waste repository and increasing international interest in developing the recycling of used nuclear fuel, there is a pressing need to reevaluate the current methods of processing nuclear waste. The preferred method for high-level waste (HLW) disposition is vitrification: incorporating radioactive cations directly into the structure of a glass. This results in a highly durable waste product. However, the current US models for the corrosion of high level waste (HLW) glasses were developed for a mixed-waste repository system and are highly conservative. An international collaboration (USA, UK, France, Japan, and Belgium) was recently developed to investigate unresolved issues in glass corrosion phenomena, mechanisms, and processes. Incomplete understanding in this area has limited the performance of the best corrosion models to date. Novel research projects are ongoing in this area involving isotopic tagging experiments, the study of ancient man-made and natural analogue materials, and the advanced characterization of internationally supplied long-term corrosion samples, several of which are radioactive. The complete realization of these experiments requires the unique capabilities of EMSL to couple state-of-the-art interfacial analysis on radioactive samples with theory and advanced computational modeling. These experiments have already led to important revisions to corrosion theory as well as significant public and media attention. The goal now is to provide data that will conclusively determine the key geochemical processes behind long-term waste glass corrosion and improve the confidence and accuracy of the source term for radionuclide fate and transport models. With a strong, consensus corrosion model, the extraordinary durability of waste glasses can be leveraged for efficient disposal, representing a real opportunity to improve long-term international nuclear waste storage, minimizing the risk to the environment and enabling the carbon-neutral energy source of nuclear power.

Project Details

Start Date
2015-10-16
End Date
2016-09-30
Status
Closed

Team

Principal Investigator

Joseph Ryan
Institution
Pacific Northwest National Laboratory

Co-Investigator(s)

Jamie Weaver
Institution
National Institute of Standards and Technology

Team Members

Daniel Schreiber
Institution
Pacific Northwest National Laboratory

Carolyn Pearce
Institution
Pacific Northwest National Laboratory

Sebastien Kerisit
Institution
Pacific Northwest National Laboratory

Tiffany Kaspar
Institution
Pacific Northwest National Laboratory

Edgar Buck
Institution
Pacific Northwest National Laboratory

Related Publications

Asmussen RM, JJ Neeway, TC Kaspar, and JV Crum. 2017. "Corrosion Behavior and Microstructure Influence of Glass Ceramic Waste Forms." Corrosion 73(11):1306-1319. doi:10.5006/2449
Kaspar TC, JT Reiser, JV Ryan, and NAO Wall. 2018. "Non-destructive characterization of corroded glass surfaces by spectroscopic ellipsometry." Journal of Non-crystalline Solids 481:260-266. doi:10.1016/j.jnoncrysol.2017.10.054
Lu X, DK Schreiber, JJ Neeway, JV Ryan, and J Du. 2017. "Effects of Optical Dopants and Laser Wavelength on Atom Probe Tomography Analyses of Borosilicate Glasses." Journal of the American Ceramic Society 100(10):4801-4815. doi:10.1111/jace.14987
Sjoblom R, JL Weaver, DK Peeler, JS Mccloy, AA Kruger, E Ogenhall, and E Hjarthner-Jolder. 2016. "Vitrified hillforts as anthropogenic analogues for nuclear waste glasses - project planning and initiation." In Environmental Impact 2016, vol. 11, pp. 897-906. No publisher listed. doi:10. 2495
Weaver J.L., C.I. Pearce, R. Sjoblom, J.S. McCloy, M.D. Miller, T. Varga, and B.W. Arey, et al. 2018. "Pre-Viking Swedish Hillfort Glass: A Prospective Long-Term Alteration Analogue for Vitrified Nuclear Waste." International Journal of Applied Glass Science 9. PNNL-26864. doi:10.1111/ijag.12351
Weaver JL, McCloy JS, Ryan JV, Kruger AA. 2016. "Ensuring longevity: Ancient glasses help predict durability of vitrified nuclear waste." American Ceramic Society Bulletin. Cover Article. 95(4):18 · 23. April 2016
Zhang J., J.J. Neeway, Y. Zhang, J.V. Ryan, W. Yuan, T. Wang, and Z. Zhu. 2017. "Nanoscale Imaging of Alteration Layers of Corroded International Simple Glass Particles using ToF-SIMS." Nuclear Instruments and Methods in Physics Research. Section B, Beam Interactions with Materials and Atoms 404. PNNL-SA-122961. doi:10.1016/j.nimb.2017.01.053