Towards a unifying mechanistic model for silicate glass corrosion
Source abstract
Abstract
Abstract Borosilicate glasses are currently used for the immobilization of highly radioactive waste and are materials of choice for many biomedical and research industries. They are metastable materials that corrode in aqueous solutions, reflected by the formation of silica-rich surface alteration layers (SAL). Until now, there is no consensus in the scientific community about the reaction and transport mechanism(s) and the rate-limiting steps involved in the formation of SALs. Here we report the results of multi-isotope tracer (2H,18O,10B, 30Si, 44Ca) corrosion experiments that were performed with precorroded and pristine glass monoliths prepared from the six-component international simple glass and a quaternary aluminum borosilicate glass. Results of transmission electron microscopy and nanoscale analyses by secondary ion mass spectrometry reveal a nanometer-sharp interface between the SAL and the glass, where decoupling of isotope tracer occurs, while proton diffusion and ion exchange can be observed within the glass. We propose a unifying mechanistic model that accounts for all critical observations so far made on naturally and experimentally corroded glasses. It is based on an interface-coupled glass dissolution-silica precipitation reaction as the main SAL forming process. However, a diffusion-controlled ion exchange front may evolve in the glass ahead of the dissolution front if SAL formation at the reaction interface significantly slows down due to transport limitations.
Source: crossref · Quality: baseline
Research context
OpenAlex topics: Glass properties and applications · Nuclear materials and radiation effects · Radioactive element chemistry and processing
SciVX discovery tags are terminology-based. OpenAlex topics are source-provided classifications.
References (50)
Show source-provided references
1. Gin, S. et al. Nuclear glass durability: new insight into alteration layer properties. J. Phys. Chem. C. 115, 18696–18706 (2011).10.1021/jp205477q ↗
2. Gin, S., Ryan, J. V., Schreiber, D. K., Neeway, J. & Cabié, M. Contribution of atom-probe tomography to a better understanding of glass alteration mechanisms: application to a nuclear glass specimen altered 25years in a granitic environment. Chem. Geol. 349–350, 99–109 (2013).10.1016/j.chemgeo.2013.04.001 ↗
3. Verney-Carron, A., Gin, S., Frugier, P. & Libourel, G. Long-term modeling of alteration-transport coupling: application to a fractured Roman glass. Geochim. Cosmochim. Acta 74, 2291–2315 (2010).10.1016/j.gca.2010.01.001 ↗
4. Verney-Carron, A., Gin, S. & Libourel, G. A fractured roman glass block altered for 1800 years in seawater: analogy with nuclear waste glass in a deep geological repository. Geochim. Cosmochim. Acta 72, 5372–5385 (2008).10.1016/j.gca.2008.08.018 ↗
5. Buchmeier, W., Jeschke, P. & Sorg, R. Machine dishwashing of glass in private households: research results on glass damage. Glass Sci. Technol. 69, 159–166 (1996).
6. Rebiscoul, D., Frugier, P., Gin, S. & Ayral, A. Protective properties and dissolution ability of the gel formed during nuclear glass alteration. J. Nucl. Mater. 342, 26–34 (2005).10.1016/j.jnucmat.2005.03.018 ↗
7. Dohmen, L. et al. Pattern formation in silicate glass corrosion zones. Int. J. Appl. Glass Sci. 4, 357–370 (2013).10.1111/ijag.12046 ↗
8. Geisler, T. et al. Aqueous corrosion of borosilicate glass under acidic conditions: a new corrosion mechanism. J. Non-Cryst. Solids 356, 1458–1465 (2010).10.1016/j.jnoncrysol.2010.04.033 ↗
9. Sterpenich, J. & Libourel, G. Using stained glass windows to understand the durability of toxic waste matrices. Chem. Geol. 174, 181–193 (2001).10.1016/S0009-2541(00)00315-6 ↗
10. Schalm, O. & Anaf, W. Laminated altered layers in historical glass: density variations of silica nanoparticle random packings as explanation for the observed lamellae. J. Non-Cryst. Solids 442, 1–16 (2016).10.1016/j.jnoncrysol.2016.03.019 ↗
11. Pearson, C. Conservation of Marine Archaeological Objects. (Elsevier, New York 1988).
12. Geisler, T. et al. The mechanism of borosilicate glass corrosion revisited. Geochim. Cosmochim. Acta 158, 112–129 (2015).10.1016/j.gca.2015.02.039 ↗
13. Gin, S. et al. Atom-probe tomography, TEM and ToF-SIMS study of borosilicate glass alteration rim: a multiscale approach to investigating rate-limiting mechanisms. Geochim. Cosmochim. Acta 202, 57–76 (2017).10.1016/j.gca.2016.12.029 ↗
14. Hellmann, R. et al. Nanometre-scale evidence for interfacial dissolution–reprecipitation control of silicate glass corrosion. Nat. Mater. 14, 307–311 (2015).10.1038/nmat4172 ↗
15. Valle, N. et al. Elemental and isotopic (29Si and 18O) tracing of glass alteration mechanisms. Geochim. Cosmochim. Acta 74, 3412–3431 (2010).10.1016/j.gca.2010.03.028 ↗
16. Anaf, W. Study on the formation of heterogeneous structures in leached layers during the corrosion process of glass. CeROArt. No. EGG 1., https://journals.openedition.org/ceroart/1561 (2010).10.4000/ceroart.1561 ↗
17. Gin, S. et al. The controversial role of inter-diffusion in glass alteration. Chem. Geol. 440, 115–123 (2016).10.1016/j.chemgeo.2016.07.014 ↗
18. Putnis, A. Sharpened interface. Nat. Mater. 14, 261 (2015).10.1038/nmat4198 ↗
19. Hellmann, R. et al. Unifying natural and laboratory chemical weathering with interfacial dissolution–reprecipitation: a study based on the nanometer-scale chemistry of fluid–silicate interfaces. Chem. Geol. 294–295, 203–216 (2012).10.1016/j.chemgeo.2011.12.002 ↗
20. Grambow, B. Nuclear waste glass dissolution: mechanism, model and application. IAEA, JSS-TR--87-02 (1987).
21. Bunker, B. Molecular mechanisms for corrosion of silica and silicate glasses. J. Non-Cryst. Solids 179, 300–308 (1994).10.1016/0022-3093(94)90708-0 ↗
22. Jégou, C., Gin, S. & Larché, F. Alteration kinetics of a simplified nuclear glass in an aqueous medium: effects of solution chemistry and of protective gel properties on diminishing the alteration rate. J. Nucl. Mater. 280, 216–229 (2000).10.1016/S0022-3115(00)00039-8 ↗
23. Frugier, P. et al. SON68 nuclear glass dissolution kinetics: current state of knowledge and basis of the new GRAAL model. J. Nucl. Mater. 380, 8–21 (2008).10.1016/j.jnucmat.2008.06.044 ↗
24. Grambow, B. & Müller, R. First-order dissolution rate law and the role of surface layers in glass performance assessment. J. Nucl. Mater. 298, 112–124 (2001).10.1016/S0022-3115(01)00619-5 ↗
25. Ma, T. et al. A mechanistic model for long-term nuclear waste glass dissolution integrating chemical affinity and interfacial diffusion barrier. J. Nucl. Mater. 486, 70–85 (2017).10.1016/j.jnucmat.2017.01.001 ↗
26. Ohkubo, T., Gin, S., Collin, M. & Iwadate, Y. Molecular dynamics simulation of water confinement in disordered aluminosilicate subnanopores. Sci. Rep. 8, 3761 (2018).10.1038/s41598-018-22015-3 ↗
27. Van Iseghem, P. et al. GLAMOR: A critical evaluation of the dissolution mechanisms of high-level waste glasses in conditions of relevance for geological disposal. SCK.CEN, CEA, Subatech, PNNL, and SRNL, EUR 23097 (2004).
28. Rebiscoul, D. et al. Morphological evolution of alteration layers formed during nuclear glass alteration: new evidence of a gel as a diffusive barrier. J. Nucl. Mater. 326, 9–18 (2004).10.1016/j.jnucmat.2003.10.015 ↗
29. Cailleteau, C. et al. Insight into silicate-glass corrosion mechanisms. Nat. Mater. 7, 978–983 (2008).10.1038/nmat2301 ↗
30. Gin, S. et al. Origin and consequences of silicate glass passivation by surface layers. Nat. Commun. 6, 6360 (2015).10.1038/ncomms7360 ↗
31. Suzuki, T., Endo, H. & Shibayama, M. Analysis of surface structure and hydrogen/deuterium exchange of colloidal silica suspension by contrast-variation small-angle neutron scattering. Langmuir 24, 4537–4543 (2008).10.1021/la7039515 ↗
32. Scheetz, B. E. et al. The role of boron in monitoring the leaching of borosilicate glass waste forms. MRS Proc. 44, 129 (1984).10.1557/PROC-44-129 ↗
33. 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).10.1016/j.gca.2014.12.009 ↗
34. Bouakkaz, R., Abdelouas, A., El Mendili, Y., Grambow, B. & Gin, S. SON68 glass alteration under Si-rich solutions at low temperature (35—90 °C): kinetics, secondary phases and isotopic exchange studies. RSC Adv. 6, 72616–72633 (2016).10.1039/C6RA12404F ↗
35. Iler, R. K. The Chemistry of Silica: Solubility, Polymerization, Colloid and Surface Properties and Biochemistry of Silica. (John Wiley & Sons, New York 1979).
36. Kaspar, T. C., Reiser, J. T., Ryan, J. V. & Wall, N. A. Non-destructive characterization of corroded glass surfaces by spectroscopic ellipsometry. J. Non-Cryst. Solids 481, 260–266 (2018).10.1016/j.jnoncrysol.2017.10.054 ↗
37. Rebiscoul, D. et al. Water dynamics in nanoporous alteration layer coming from glass alteration: an experimental approach. J. Phys. Chem. C. 119, 15982–15993 (2015).10.1021/acs.jpcc.5b03073 ↗
38. Stone, W. E. E., El Shafei, G. M. S., Sanz, J. & Selim, S. A. Association of soluble aluminum ionic species with a silica-gel surface: a solid-state NMR study. J. Phys. Chem. 97, 10127–10132 (1993).10.1021/j100141a038 ↗
39. Doremus, R. H. in Glass Surfaces 137–144 (Elsevier, New York 1975).10.1016/B978-0-7204-0419-7.50017-2 ↗
40. Doremus, R. H., Mehrotra, Y., Lanford, W. & Burman, C. Reaction of water with glass: influence of a transformed surface layer. J. Mater. Sci. 18, 612–622 (1983).10.1007/BF00560651 ↗
41. McGrail, B. P. et al. The structure of Na 2 O–Al 2 O 3–SiO 2 glass: impact on sodium ion exchange in H 2 O and D 2 O. J. Non-Cryst. Solids 296, 10–26 (2001).10.1016/S0022-3093(01)00890-0 ↗
42. Chave, T., Frugier, P., Ayral, A. & Gin, S. Solid state diffusion during nuclear glass residual alteration in solution. J. Nucl. Mater. 362, 466–473 (2007).10.1016/j.jnucmat.2007.01.095 ↗
43. Verney-Carron, A. et al. Understanding the mechanisms of Si–K–Ca glass alteration using silicon isotopes. Geochim. Cosmochim. Acta 203, 404–421 (2017).10.1016/j.gca.2017.01.030 ↗
44. Chave, T., Frugier, P., Gin, S. & Ayral, A. Glass–water interphase reactivity with calcium rich solutions. Geochim. Cosmochim. Acta 75, 4125–4139 (2011).10.1016/j.gca.2011.05.005 ↗
45. Icenhower, J. P. & Steefel, C. I. Dissolution rate of borosilicate glass SON68: a method of quantification based upon interferometry and implications for experimental and natural weathering rates of glass. Geochim. Cosmochim. Acta 157, 147–163 (2015).10.1016/j.gca.2015.02.037 ↗
46. Ribet, S. & Gin, S. Role of neoformed phases on the mechanisms controlling the resumption of SON68 glass alteration in alkaline media. J. Nucl. Mater. 324, 152–164 (2004).10.1016/j.jnucmat.2003.09.010 ↗
47. Ruiz-Agudo, E. et al. Control of silicate weathering by interface-coupled dissolution-precipitation processes at the mineral-solution interface. Geology 44, 567–570 (2016).10.1130/G37856.1 ↗
48. Schindelin, J. et al. Fiji: an open-source platform for biological-image analysis. Nat. Meth. 9, 676–682 (2012).10.1038/nmeth.2019 ↗
49. Gormanns, P., Reckow, S., Poczatek, J. C., Turck, C. W. & Lechene, C. Segmentation of multi-isotope imaging mass spectrometry data for semi-automatic detection of regions of interest. PloS One 7, e30576 (2012).10.1371/journal.pone.0030576 ↗
50. Van der Walt, S. & Smith, N. A better default colormap for Matplotlib, SciPy 2015, http://bids.github.io/colormap/ (2015).