Impacts of glass composition, pH, and temperature on glass forward dissolution rate
Source abstract
Abstract
Abstract Nuclear waste glasses dissolve at the forward dissolution rate (rf) in very dilute aqueous solutions, which can isolate the impact of the glass composition from solution feedback and alteration product effects. While it has long been known that pH and temperature (T) strongly impact rf, the impacts of glass composition have remained uncertain. In this work, rf data from 19 nuclear waste glasses were used with the aim of identifying the effect of glass composition on rf. The rf values were modeled as: rf = k010–ηpHexp(−Ea/RT), with k0, η, Ea, and R, respectively, being the intrinsic rate constant, pH coefficient, apparent activation energy, and gas constant. However, no predictive correlation could be established between the individual model parameters (log[k0], η, and Ea) and glass composition for the glasses considered in this study, an outcome that was attributed to the strong positive correlation between the log[k0] and Ea parameters. Therefore, a model was fitted directly to the combined rf from all 19 glasses. This approach showed that 90% of the variation in rf data could be accounted for solely by T and pH effects. Therefore, any composition effects must be relatively small. After normalizing for differences in pH and T, the only notable differences in rf between the glasses were found to correlate with variations in the fraction of glass forming tetrahedra contributed by tetrahedral boron, f([4]B), with an abrupt threshold at a high value of f([4]B) (~0.22), where higher rf are predicted with no discernable composition effects below the threshold.
Source: crossref · Quality: baseline
Research context
OpenAlex topics: Nuclear materials and radiation effects · Glass properties and applications · Radioactive element chemistry and processing
SciVX discovery tags are terminology-based. OpenAlex topics are source-provided classifications.
References (54)
Show source-provided references
1. Vienna, J. D. Nuclear waste vitrification in the United States: recent developments and future options. Int. J. Appl. Glass Sci. 1, 309–321 (2010).10.1111/j.2041-1294.2010.00023.x ↗
2. Donald, I. W., Metcalfe, B. L. & Taylor, R. N. J. Review: the immobilization of high level radioactive wastes using ceramics and glasses. J. Mater. Sci. 32, 5851–5887 (1997).10.1023/A:1018646507438 ↗
3. Vienna, J. D., Ryan, J. V., Gin, S. & Inagaki, Y. Current understanding and remaining challenges in modeling long-term degradation of borosilicate nuclear waste glasses. Int. J. Appl. Glass Sci. 4, 283–294 (2013).10.1111/ijag.12050 ↗
4. Gin, S., Beaudoux, X., Angéli, F., Jégou, C. & Godon, N. Effect of composition on the short-term and long-term dissolution rates of ten borosilicate glasses of increasing complexity from 3 to 30 oxides. J. Noncryst. Solids 358, 2559–2570 (2012).10.1016/j.jnoncrysol.2012.05.024 ↗
5. Gin, S. et al. An international initiative on long-term behavior of high-level nuclear waste glass. Mater. Today 16, 243–248 (2013).10.1016/j.mattod.2013.06.008 ↗
6. Frankel, G. S. et al. Corrosion of glasses, ceramics, and metals; a comparative review. npj Mater. Degred. 2, 15 (2018).10.1038/s41529-018-0037-2 ↗
7. Chick, L. A. et al. The Effects of Composition on Properties in an 11-Component Nuclear Waste Glass System. Report No. PNL-3188 (Pacific Northwest Laboratory, Richland, WA, 1981).
8. Frugier, P., Martin, C., Ribet, I., Advocat, T. & Gin, S. The effect of composition on the leaching of three nuclear waste glasses: R7T7, AVM and VRZ. J. Nucl. Mater. 346, 194–207 (2005).10.1016/j.jnucmat.2005.06.023 ↗
9. Hrma, P. et al. in Ceramic Transactions (eds Jain, V. & Palmer, R.) Vol. 61, 497–504 (American Ceramic Society, Westerville, OH, 1995).
10. Jantzen, C. M., Pickett, J. B., Brown, K. G., Edwards, T. B. & Beam, D. C. Process/Product Models for the Defense Waste Processing Facility (DWPF): Part I. Predicting Glass Durability from Composition Using a THermodynamic Hydration Energy Reaction MOdel (THERMO). Report No. WSRC-TR-93-0672 (Westinghouse Savannah River Company, Aiken, SC, 1995).
11. Vienna, J. D., Hrma, P., Schweiger, M. J. & Langowski, M. H. in Ceramic Transactions Vol. 72, (eds Jain, V. & Peeler, D. K.) 307–316 (American Ceramic Society, Westerville, OH, 1996).
12. Pegg, I. L. et al. Scientific Basis for Nuclear Waste Management XII Vol. 127, 215–221 (Materials Research Society, Berlin, Germany, 1989).
13. Hrma, P. et al. Property/Composition Relationships for Hanford High-Level Waste Glasses Melting at 1150°C. Report No. PNL-10359 (Pacific Northwest Laboratory, Richland, WA, 1994).10.2172/10121752 ↗
14. Feng, X. & Pegg, I. L. A glass dissolution model for the effects of S/V on leachate pH. J. Noncryst. Solids 175, 281–293 (1994).10.1016/0022-3093(94)90022-1 ↗
15. Piepel, G. F. et al. ILAW PCT, VHT, Viscosity, and Electrical Conductivity Model Development: VSL-07R1230-1. Report No. ORP-56502 (Vitreous State Laboratory, The Catholic University of America, Washington, DC, 2007).
16. Piepel, G. F. et al. IHLW PCT, Spinel T1%, Electrical Conductivity, and Viscosity Model Development: VSL-07R1240-4. Report No. ORP-56320 (Vitreous State Laboratory, The Catholic University of America, Washington, DC, 2008).
17. Vienna, J. D. et al. Glass Property Models and Constraints for Estimating the Glass to be Produced at Hanford by Implementing Current Advanced Glass Formulation Efforts. Report No. PNNL-22631, Rev. 1, ORP-58289 (Pacific Northwest National Laboratory, Richland, WA, 2013).10.2172/1170502 ↗
18. Vienna, J. D., Kim, D. S., Skorski, D. C. & Matyas, J. Hanford Immobilized LAW Product Acceptance Testing: Tanks Focus Area Results. Report No. PNNL-13744 (Pacific Northwest National Laboratory, Richland, WA, 2001).10.2172/15001162 ↗
19. Muller, I. S., Joseph, I., Perez-Cardenas, F. C. & Pegg, I. L. LAW Glass Testing and VHT Model Assessment. Report No. VSL-08R1410-1 (Vitreous State Laboratory at the Catholic University of America, Washington, DC, 2008).10.2172/1512509 ↗
20. Ribet, S., Muller, I. S., Pegg, I. L., Gin, S. & Frugier, P. Scientific Basis for Nuclear Waste Management XXVIII Vol. 824, 309–314 (Materials Research Society, San Francisco, CA, 2004).10.1557/PROC-824-CC5.3 ↗
21. Aagaard, P. & Helgeson, H. C. Thermodynamic and kinetic constraints on reaction rates among minerals and aqueous solutions I. Theoretical considerations. Am. J. Sci. 282, 237–285 (1982).10.2475/ajs.282.3.237 ↗
22. Grambow, B. A general rate equation for nuclear waste glass corrosion. Mater. Res. Soc. Symp. Proc. 44,15–27 (1985).10.1557/PROC-44-15 ↗
23. McGrail, B. P., Ebert, W. L., Bakel, A. J. & Peeler, D. K. Measurement of kinetic rate law parameters on a Na-Ca-Al borosilicate glass for low-activity waste. J. Nucl. Mater. 249, 175–189 (1997).10.1016/S0022-3115(97)00213-4 ↗
24. Pierce, E. M., Rodriguez, E. A., Calligan, L. J., Shaw, W. J. & McGrail, B. P. An experimental study of the dissolution rates of simulated aluminoborosilicate waste glasses as a function of pH and temperature under dilute conditions. Appl. Geochem. 23, 2559–2573 (2008).10.1016/j.apgeochem.2008.05.006 ↗
25. ASTM. Standard Practice for Measurement of the Glass Dissolution Rate Using the Single-Pass Flow-Through Test Method. ASTM C1662-10 (ASTM International, West Conshohocken, PA, 2010).
26. Pierce, E. M., Reed, L. R., Shaw, W. J. & Icenhower, J. P. Effect of Al/B ratio on the dissolution of nepheline glass, Na3(Al, B)1-4Si4O16. Geochim. Cosmochim. Acta 69, A781–A781 (2005).
27. Hopf, J. et al. Glass–water interaction: effect of high-valence cations on glass structure and chemical durability. Geochim. Cosmochim. Acta 181, 54–71 (2016).10.1016/j.gca.2016.02.023 ↗
28. Hamilton, J. P., Brantley, S. L., Pantano, C. G., Criscenti, L. J. & Kubicki, J. D. Dissolution of nepheline, jadeite and albite glasses: toward better models for aluminosilicate dissolution. Geochim. Cosmochim. Acta 65, 3683–3702 (2001).10.1016/S0016-7037(01)00724-4 ↗
29. McGrail, B. P. et al. The structure of Na2O-Al2O3 -SiO2 glass: impact on sodium ion exchange in H2O and D2O. J. Noncryst. Solids 296, 10–26 (2001).10.1016/S0022-3093(01)00890-0 ↗
30. Blum, A. E. & Stillings, L. L. in Chemical Weathering Rates of Silicate Minerals Reviews In Mineralogy (eds. White, A. F. & Brantley, S. L.) 291–351 (Mineralogical Society of America, Chantilly, VA, 1995).10.1515/9781501509650-009 ↗
31. Strachan, D. M. Glass dissolution as a function of pH and its implications for understanding mechanisms and future experiments. Geochim. Cosmochim. Acta 219, 111–123 (2017).10.1016/j.gca.2017.09.008 ↗
32. Bonferroni, C. E. Teoria statistica delle classi e calcolo delle probabilità. Pubblicazioni del R Istituto Superiore di Scienze Economiche e Commerciali di Firenze (1936).
33. Neeway, J. J., Rieke, P. C., Parruzot, B. P., Ryan, J. V. & Asmussen, R. M. The dissolution behavior of borosilicate glasses in far-from equilibrium conditions. Geochim. Cosmochim. Acta 226, 132–148 (2018).10.1016/j.gca.2018.02.001 ↗
34. Du, J. & Rimsza, J. M. Atomistic computer simulations of water interactions and dissolution of inorganic glasses. Nat. Mater. Degrad. 2017, 1–16 (2017).
35. Grambow, B. Scientific Basis for Nuclear Waste Management VIII Vol. 44, 16–27 (Materials Research Society, Pittsburgh, Pennsylvania, 1985).
36. Grambow, B. Nuclear Waste Glass Dissolution: Mechanism, Model, and Application. Report No. JSS 87-02 (Hahn-Meitner-Institut: Berlin, Germany, 1987).
37. Neeway, J. J. et al. FY2016 ILAW Glass Corrosion Testing with the Single-Pass Flow-Through Method. Report No. PNNL-26169 (Pacific Northwest National Laboratory, Richland, WA, 2017).10.2172/1365447 ↗
38. Pierce, E. M. et al. Experimental determination of the effect of the ratio of B/Al on glass dissolution along the nepheline (NaAlSiO4)-malinkoite (NaBSiO4) join. Geochim. Cosmochim. Acta 74, 2634–2654 (2010).10.1016/j.gca.2009.09.006 ↗
39. Kerisit, S. N. & Pierce, E. M. Monte Carlo simulations of the dissolution of borosilicate and aluminoborosilicate glasses in dilute aqueous solutions. Geochim. Cosmochim. Acta 75(18), 5296–5309 (2011).10.1016/j.gca.2011.06.036 ↗
40. Petkus, L. L. Low Activity Container Centerline Cooling Data. Report No. CCN: 074181 (River Protection Project, Hanford Tank Waste Treatment and Immobilization Plant, Richland, WA, 2003).
41. Crum, J. V. et al. Baseline Glass Development for Combined Fission Products Waste Streams: Advanced Fuel Cycle Initiative. Report No. AFCI-WAST-WAST-MI-DV-2009-000075 (Pacific Northwest National Laboratory: Richland, WA, 2009).10.2172/1048019 ↗
42. Papathanassiu, A. et al. ILAW Glass Testing for Disposal at IDF: Phase 1 Testing. Report No. VSL-11R2270-1 (Vitreous State Laboratory, The Catholic University of America, Washington, DC, 2011).10.2172/1266842 ↗
43. Muller, I. S., Matlack, K. S. & Pegg, I. L. Enhanced LAW Glass Correlation - Phase 1. Report No. VSL-16R4000-1 (Vitreous State Laboratory, The Catholic University of America, Washington, DC, 2016).
44. Muller, I. S. & Pegg, I. L. FY 2015 ILAW Glass Testing for Disposal at IDF. Report No. VSL-15R3790-1 (Vitreous State Laboratory, The Catholic University of America, Washington, DC, 2015).
45. Pierce, E. M. et al. Waste Form Release Data Package for the 2005 Integrated Disposal Facility Performance Assessment. Report No. PNNL-14805 (Pacific Northwest National Laboratory, Richland, WA, 2004).
46. McGrail, B. P. et al. Waste Form Release Data Package for the 2001 Immobilized Low-Activity Waste Performance Assessment. Report No. PNNL-13043, Rev. 2 (Pacific Northwest National Laboratory, Richland, WA, 2001).10.2172/971121 ↗
47. Feng, X. D. et al. Glass Optimization for Vitrification of Hanford Site Low-Level Tank Waste. Report No. PNNL-10918 (Pacific Northwest Laboratory, Richland, WA, 1996).10.2172/219300 ↗
48. Cassingham, N. et al. The initial dissolution rates of simulated UK Magnox-ThORP blend nuclear waste glass as a function of pH, temperature and waste loading. Mineral. Mag. 79, 1529–1542 (2015).10.1180/minmag.2015.079.6.28 ↗
49. Muller, I. S., Matlack, K. S. & Pegg, I. L. Enhanced LAW Glass Correlation - Phase 2. Report No. VSL-17R4140-1 (Vitreous State Laboratory, The Catholic University of America, Washington, DC, 2017).10.2172/1512925 ↗
50. 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 ↗
51. Jantzen, C. M. Glass Compositions and Frit Formulations Developed for DWPF. Report No. DPST-88-952 (Savannah River Laboratory, Aiken, SC, 1988).
52. Viragh, C., Abramowitz, H., Muller, I. S., Papathanassiu, A. E. & Pegg, I. L. FY2017 ILAW Glass SPFT Testing for Disposal at IDF: Glass IDF21-EC14. Report No. VSL-17R4320-1 (Vitreous State Laboratory, The Catholic University of America, Washington, DC, 2017).
53. Papathanassiu, A., Viragh, C., Muller, I. S., & Pegg, I. L. FY2016 ILAW Glass SPFT Testing for Disposal at IDF. Report No. VSL-17R3860-1 (Vitreous State Laboratory, The Catholic University of America, Washington, DC, 2017).
54. Neeway, J. J. et al. FY2017 ILAW Glass Corrosion Testing with the Single-Pass Flow-Through Method. Report No. PNNL-27098 (Pacific Northwest National Laboratory, Richland, WA, 2018).10.2172/1440631 ↗