The US plan for high-level nuclear waste includes the immobilization of long-lived radionuclides in glass or ceramic waste forms in stainless-steel canisters for disposal in deep geological repositories. Here we report that, under simulated repository conditions, corrosion could be significantly accelerated at the interfaces of different barrier materials, which has not been considered in the current safety and performance assessment models. Severe localized corrosion was found at the interfaces between stainless steel and a model nuclear waste glass and between stainless steel and a ceramic waste form. The accelerated corrosion can be attributed to changes of solution chemistry and local acidity/alkalinity within a confined space, which significantly alter the corrosion of both the waste-form materials and the metallic canisters. The corrosion that is accelerated by the interface interaction between dissimilar materials could profoundly impact the service life of the nuclear waste packages, which, therefore, should be carefully considered when evaluating the performance of waste forms and their packages. Moreover, compatible barriers should be selected to further optimize the performance of the geological repository system.
This is a preview of subscription content
Subscription info for Chinese customers
We have a dedicated website for our Chinese customers. Please go to naturechina.com to subscribe to this journal.
Get time limited or full article access on ReadCube.
All prices are NET prices.
The data that support the findings of this study are available from the corresponding authors upon reasonable request.
Gin, S. et al. An international initiative on long-term behavior of high-level nuclear waste glass. Mater. Today 16, 243–248 (2013).
Bates, J., Bradley, J., Teetsov, A., Bradley, C. & Ten Brink, M. B. Colloid formation during waste form reaction: implications for nuclear waste disposal. Science 256, 649–651 (1992).
Frankel, G. Pitting corrosion of metals: a review of the critical factors. J. Electrochem. Soc. 145, 2186–2198 (1998).
Oldfield, J. & Sutton, W. Crevice corrosion of stainless steels: I. A mathematical model. Br. Corros. J. 13, 13–22 (1978).
Rydberg, J. Groundwater Chemistry of a Nuclear Waste Repository in Granite Bedrock (Lawrence Livermore National Lab, 1981).
Long, J. C. & Ewing, R. C. Yucca Mountain: Earth-science issues at a geologic repository for high-level nuclear waste. Annu. Rev. Earth Planet. Sci. 32, 363–401 (2004).
Geisler, T. et al. Aqueous corrosion of borosilicate glass under acidic conditions: a new corrosion mechanism. J. Non-Cryst. Solids 356, 1458–1465 (2010).
McVay, G. L. & Buckwalter, C. Q. Effect of iron on waste‐glass leaching. J. Am. Ceram. Soc. 66, 170–174 (1983).
Burger, E. et al. Impact of iron on nuclear glass alteration in geological repository conditions: a multiscale approach. Appl. Geochem. 31, 159–170 (2013).
Pourbaix, M. Atlas of Electrochemical Equilibria in Aqueous Solution (National Association of Corrosion Engineers, 1974).
Brendebach, B., Altmaier, M., Rothe, J., Neck, V. & Denecke, M. EXAFS study of aqueous Zriv and Thiv complexes in alkaline CaCl2 solutions: Ca3[Zr(OH)6]4+ and Ca4[Th(OH)8]4+. Inorg. Chem. 46, 6804–6810 (2007).
Arab, M. et al. Aqueous alteration of five-oxide silicate glasses: experimental approach and Monte Carlo modeling. J. Non-Crystal. Solids 354, 155–161 (2008).
Fournier, M., Gin, S., Frugier, P. & Mercado-Depierre, S. Contribution of zeolite-seeded experiments to the understanding of resumption of glass alteration. npj Mater. Degrad. 1, 17 (2017).
Fournier, M., Frugier, P. & Gin, S. Effect of zeolite formation on borosilicate glass dissolution kinetics. Proc. Earth Planet. Sci. 7, 264–267 (2013).
Ringwood, A., Kesson, S., Ware, N., Hibberson, W. & Major, A. Immobilisation of high level nuclear reactor wastes in SYNROC. Nature 278, 219 (1979).
Shan, X. & Payer, J. H. Comparison of ceramic and polymer crevice formers on the crevice corrosion behavior of Ni–Cr–Mo Alloy C-22 in CORROSION 2007 (NACE International, 2007).
Li, T., Scully, J. & Frankel, G. Localized corrosion: passive film breakdown vs. pit growth stability: Part III. A unifying set of principal parameters and criteria for pit stabilization and salt film formation. J. Electrochem. Soc. 165, C762–C770 (2018).
Frugier, P., Minet, Y., Rajmohan, N., Godon, N. & Gin, S. Modeling glass corrosion with GRAAL. npj Mater. Degrad. 2, 35 (2018).
Verney-Carron, A., Gin, S. & Libourel, G. Archaeological analogs and the future of nuclear waste glass. J. Nucl. Mater. 406, 365–370 (2010).
Payer, J. H., Carroll, S. A., Gdowski, G. E. & Rebak, R. B. A Framework for the Analysis of Localized Corrosion at the Proposed Yucca Mountain Repository (Yucca Mountain Project Office, 2006).
Gin, S. et al. The fate of silicon during glass corrosion under alkaline conditions: a mechanistic and kinetic study with the international simple glass. Geochim. Cosmochim. Acta 151, 68–85 (2015).
Jantzen, C. M. & Bibler, N. E. in Environmental Issues and Waste Management Technologies in the Ceramic and Nuclear Industries XI: Proceedings of the 107th Annual Meeting of The American Ceramic Society, Baltimore, Maryland, USA 2005, Ceramic Transactions (eds Herman, C. C., Marra, S, Spearing, D. R., Vance, L. & Vienna, J. D.) 139–151 (Wiley–American Ceramic Society).
Smith, G. C. Evaluation of a simple correction for the hydrocarbon contamination layer in quantitative surface analysis by XPS. J. Electron Spectrosc. 148, 21–28 (2005).
This work was supported as part of the Center for Performance and Design of Nuclear Waste Forms and Containers, an Energy Frontier Research Center funded by the US Department of Energy, Office of Science, Basic Energy Sciences under Award no. DESC0016584. The authors thank C. Crawford for supplying the ISG. The authors are grateful to S. Boona and E. L. Alexander from Ohio State University and L. Dupuy from TESCAN Analytics, as well as M. J. Olszta and N. Overman from PNNL for the technical support.
The authors declare no competing interests.
Publisher’s note Springer Nature remains neutral with regard to jurisdictional claims in published maps and institutional affiliations.
About this article
Cite this article
Guo, X., Gin, S., Lei, P. et al. Self-accelerated corrosion of nuclear waste forms at material interfaces. Nat. Mater. 19, 310–316 (2020). https://doi.org/10.1038/s41563-019-0579-x
npj Materials Degradation (2022)
npj Materials Degradation (2021)
Corrosion interactions between stainless steel and lead vanado-iodoapatite nuclear waste form part I
npj Materials Degradation (2020)
Nature Materials (2020)
Corrosion interactions between stainless steel and lead vanado-iodoapatite nuclear waste form part II
npj Materials Degradation (2020)