Skip to main content

Thank you for visiting nature.com. You are using a browser version with limited support for CSS. To obtain the best experience, we recommend you use a more up to date browser (or turn off compatibility mode in Internet Explorer). In the meantime, to ensure continued support, we are displaying the site without styles and JavaScript.

  • Article
  • Published:

Self-accelerated corrosion of nuclear waste forms at material interfaces

Nature Materials volume 19, pages 310–316 (2020)Cite this article

Subjects

Matters Arising to this article was published on 13 July 2020

Abstract

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, access via your institution

Access options

Buy this article

  • Purchase on Springer Link
  • Instant access to full article PDF
Buy now

Prices may be subject to local taxes which are calculated during checkout

Fig. 1: Illustration of crevice corrosion for a SS canister and the potential impact on contained nuclear waste forms.
Fig. 2: Characterizations of different materials after corrosion in close proximity.
Fig. 3: Surface analysis of SS after corrosion in close proximity to ISG or PTFE.
Fig. 4: Precipitation of secondary phases on SS corroded near ISG.
Fig. 5: Surface characterizations of SS and Cr-Hol after corrosion.

Similar content being viewed by others

Data availability

The data that support the findings of this study are available from the corresponding authors upon reasonable request.

References

  1. Gin, S. et al. An international initiative on long-term behavior of high-level nuclear waste glass. Mater. Today 16, 243–248 (2013).

    Article  CAS  Google Scholar 

  2. 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).

    Article  CAS  Google Scholar 

  3. Frankel, G. Pitting corrosion of metals: a review of the critical factors. J. Electrochem. Soc. 145, 2186–2198 (1998).

    Article  CAS  Google Scholar 

  4. Oldfield, J. & Sutton, W. Crevice corrosion of stainless steels: I. A mathematical model. Br. Corros. J. 13, 13–22 (1978).

    Article  CAS  Google Scholar 

  5. Rydberg, J. Groundwater Chemistry of a Nuclear Waste Repository in Granite Bedrock (Lawrence Livermore National Lab, 1981).

  6. 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).

    Article  CAS  Google Scholar 

  7. Geisler, T. et al. Aqueous corrosion of borosilicate glass under acidic conditions: a new corrosion mechanism. J. Non-Cryst. Solids 356, 1458–1465 (2010).

    Article  CAS  Google Scholar 

  8. McVay, G. L. & Buckwalter, C. Q. Effect of iron on waste‐glass leaching. J. Am. Ceram. Soc. 66, 170–174 (1983).

    Article  CAS  Google Scholar 

  9. Burger, E. et al. Impact of iron on nuclear glass alteration in geological repository conditions: a multiscale approach. Appl. Geochem. 31, 159–170 (2013).

    Article  CAS  Google Scholar 

  10. Pourbaix, M. Atlas of Electrochemical Equilibria in Aqueous Solution (National Association of Corrosion Engineers, 1974).

  11. 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).

    Article  CAS  Google Scholar 

  12. 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).

    Article  CAS  Google Scholar 

  13. 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).

    Article  Google Scholar 

  14. Fournier, M., Frugier, P. & Gin, S. Effect of zeolite formation on borosilicate glass dissolution kinetics. Proc. Earth Planet. Sci. 7, 264–267 (2013).

    Article  CAS  Google Scholar 

  15. Ringwood, A., Kesson, S., Ware, N., Hibberson, W. & Major, A. Immobilisation of high level nuclear reactor wastes in SYNROC. Nature 278, 219 (1979).

    Article  CAS  Google Scholar 

  16. 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).

  17. 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).

    Article  CAS  Google Scholar 

  18. Frugier, P., Minet, Y., Rajmohan, N., Godon, N. & Gin, S. Modeling glass corrosion with GRAAL. npj Mater. Degrad. 2, 35 (2018).

    Article  Google Scholar 

  19. Verney-Carron, A., Gin, S. & Libourel, G. Archaeological analogs and the future of nuclear waste glass. J. Nucl. Mater. 406, 365–370 (2010).

    Article  CAS  Google Scholar 

  20. 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).

  21. 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).

    Article  CAS  Google Scholar 

  22. 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).

  23. 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).

    Article  CAS  Google Scholar 

Download references

Acknowledgements

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.

Author information

Authors and Affiliations

  1. Department of Materials Science and Engineering, Ohio State University, Columbus, OH, USA

    Xiaolei Guo, Gopal Viswanathan, Tianshu Li & Gerald S. Frankel

  2. CEA, DEN, DE2D, SEVT, Bagnols sur Cèze, France

    Stephane Gin

  3. Department of Mechanical Aerospace and Nuclear Engineering, Rensselaer Polytechnic Institute, Troy, NY, USA

    Penghui Lei, Tiankai Yao & Jie Lian

  4. Department of Chemical Engineering and Materials Research Institute, Pennsylvania State University, University Park, PA, USA

    Hongshen Liu, Dien Ngo & Seong H. Kim

  5. Energy and Environment Directorate, Pacific Northwest National Laboratory, Richland, WA, USA

    Daniel K. Schreiber, John D. Vienna & Joseph V. Ryan

  6. Department of Materials Science and Engineering, University of North Texas, Denton, TX, USA

    Jincheng Du

Authors
  1. Xiaolei Guo
    View author publications

    You can also search for this author in PubMed Google Scholar

  2. Stephane Gin
    View author publications

    You can also search for this author in PubMed Google Scholar

  3. Penghui Lei
    View author publications

    You can also search for this author in PubMed Google Scholar

  4. Tiankai Yao
    View author publications

    You can also search for this author in PubMed Google Scholar

  5. Hongshen Liu
    View author publications

    You can also search for this author in PubMed Google Scholar

  6. Daniel K. Schreiber
    View author publications

    You can also search for this author in PubMed Google Scholar

  7. Dien Ngo
    View author publications

    You can also search for this author in PubMed Google Scholar

  8. Gopal Viswanathan
    View author publications

    You can also search for this author in PubMed Google Scholar

  9. Tianshu Li
    View author publications

    You can also search for this author in PubMed Google Scholar

  10. Seong H. Kim
    View author publications

    You can also search for this author in PubMed Google Scholar

  11. John D. Vienna
    View author publications

    You can also search for this author in PubMed Google Scholar

  12. Joseph V. Ryan
    View author publications

    You can also search for this author in PubMed Google Scholar

  13. Jincheng Du
    View author publications

    You can also search for this author in PubMed Google Scholar

  14. Jie Lian
    View author publications

    You can also search for this author in PubMed Google Scholar

  15. Gerald S. Frankel
    View author publications

    You can also search for this author in PubMed Google Scholar

Contributions

X.G., S.G., J.L., S.H.K., J.D.V., J.V.R., J.D. and G.S.F designed the research. X.G., P.L., T.Y., H.L., D.K.S. D.N. and G.V. performed the research. X.G., S.G., P.L., T.Y., H.L., D.K.S., D.N. and S.H.K. analysed the data. All the authors contributed to the editing of the paper and the approval of the content in its current form.

Corresponding author

Correspondence to Gerald S. Frankel.

Ethics declarations

Competing interests

The authors declare no competing interests.

Additional information

Publisher’s note Springer Nature remains neutral with regard to jurisdictional claims in published maps and institutional affiliations.

Supplementary information

Supplementary Information

Supplementary text, Tables 1–5, Figs. 1–5 and references.

Rights and permissions

Reprints and permissions

About this article

Check for updates. Verify currency and authenticity via CrossMark

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

Download citation

  • Received:

  • Accepted:

  • Published:

  • Issue Date:

  • DOI: https://doi.org/10.1038/s41563-019-0579-x

This article is cited by

Search

Advanced search

Quick links

Nature Briefing

Sign up for the Nature Briefing newsletter — what matters in science, free to your inbox daily.

Get the most important science stories of the day, free in your inbox. Sign up for Nature Briefing