Effect of zeolite type, temperature, and pH on Stage III glass alteration behavior for two nuclear waste glasses

Parruzot, Benjamin P. G.; Crum, Jarrod; Reiser, Joelle T. G.; Neeway, James J.; Kerisit, Sebastien N.; Daniel, Richard C.; Bonnett, Jeff F.; Reyes, Richard A.; Seymour, Lorraine M.; Burns, Carolyn AM; Ryan, Joseph V.; Smith, Gary L.; Asmussen, Robert M.

doi:10.1016/j.jnucmat.2022.153717

Effect of zeolite type, temperature, and pH on Stage III glass alteration behavior for two nuclear waste glasses

Journal Article · Wed Apr 06 00:00:00 EDT 2022 · Journal of Nuclear Materials

DOI:https://doi.org/10.1016/j.jnucmat.2022.153717· OSTI ID:1876554

^[1]; Crum, Jarrod ^[1]; Reiser, Joelle T. G. ^[1]; ^[1]; Kerisit, Sebastien N. ^[1]; ^[1]; Bonnett, Jeff F. ^[1]; ^[1]; Seymour, Lorraine M. ^[1]; Burns, Carolyn AM ^[1]; Ryan, Joseph V. ^[1]; Smith, Gary L. ^[1]; ^[1]

Pacific Northwest National Laboratory (PNNL), Richland, WA (United States)

We report long-term laboratory scale static alteration tests (up to 1500 d) were conducted on two low-activity waste glasses (LAWA44 and IDF18-A161) at S/V = 2000 m^–1. Tests were seeded with either analcime, clinoptilolite, zeolite P1, or zeolite P2 to induce Stage III glass alteration behavior. The effect of several parameters on glass Stage III behavior was studied with consideration of several variables, including temperature (22 °C – 90 °C) and pH (floating or initially set using KOH at values from 9.5 to 11.5). Temporal solution data and solids characterization at the end of the experiments are reported. Solution data demonstrated the occurrence of a sustained rate acceleration at temperatures down to 40 °C and the activation energy for these Stage III rates was determined for both glasses. Three major secondary phases were identified at the end of the experiments for both glasses: zeolite P1, zeolite P2, and/or analcime (along with minor phases: zeolites, clays, carbonates). The identification of the crystalline phases at the end of the experiment often differed from the zeolite seed phase. In addition, the use of the Avrami equation showed unimpeded zeolite growth (3-dimensional) in certain conditions, suggesting that in certain conditions the glass dissolution rate is controlled by zeolite formation kinetics whereas in other conditions the glass corrosion process impeded zeolite formation kinetics. The morphological evolution of the samples revealed the growth of the zeolites which completely fill the intergranular space in the powder bed. These results are discussed with regards to previous seeded and unseeded Stage III dissolution rate experiments performed on low- and high-activity nuclear waste glasses.

View Accepted Manuscript (DOE)

Research Organization:: Pacific Northwest National Laboratory (PNNL), Richland, WA (United States)

Sponsoring Organization:: USDOE

Grant/Contract Number:: AC05-76RL01830; AC06-76RL01830

OSTI ID:: 1876554

Alternate ID(s):: OSTI ID: 1960829

Report Number(s):: PNNL-SA-166084

Journal Information:: Journal of Nuclear Materials, Journal Name: Journal of Nuclear Materials Vol. 567; ISSN 0022-3115

Publisher:: ElsevierCopyright Statement

Country of Publication:: United States

Language:: English

References (38)

Glassy Wasteforms for Nuclear Waste Immobilization Ojovan, Michael I.; Lee, William E. Metallurgical and Materials Transactions A, Vol. 42, Issue 4 https://doi.org/10.1007/s11661-010-0525-7	journal	November 2010
The kinetics of silica-water reactions Rimstidt, J. D.; Barnes, H. L. Geochimica et Cosmochimica Acta, Vol. 44, Issue 11, p. 1683-1699 https://doi.org/10.1016/0016-7037(80)90220-3	journal	November 1980
The dissolution kinetics of amorphous silica into sodium chloride solutions: effects of temperature and ionic strength Icenhower, Jonathan P.; Dove, Patricia M. Geochimica et Cosmochimica Acta, Vol. 64, Issue 24 https://doi.org/10.1016/S0016-7037(00)00487-7	journal	December 2000
Compositional effects on long-term dissolution of borosilicate glass Strachan, Denis M.; Croak, Theresa L. Journal of Non-Crystalline Solids, Vol. 272, Issue 1 https://doi.org/10.1016/S0022-3093(00)00154-X	journal	July 2000
SON 68 nuclear glass alteration kinetics between pH 7 and pH 11.5 Gin, S.; Mestre, J. P. Journal of Nuclear Materials, Vol. 295, Issue 1 https://doi.org/10.1016/S0022-3115(01)00434-2	journal	May 2001
Nature and role of natural alteration gels formed on the surface of ancient volcanic glasses (Natural analogs of waste containment glasses) Crovisier, Jean-Louis; Advocat, Thierry; Dussossoy, Jean-Luc Journal of Nuclear Materials, Vol. 321, Issue 1 https://doi.org/10.1016/S0022-3115(03)00206-X	journal	September 2003
Dissolution of subglacial volcanic glasses from Iceland: laboratory study and modelling Crovisier, J. -L.; Honnorez, J.; Fritz, B. Applied Geochemistry, Vol. 7 https://doi.org/10.1016/S0883-2927(09)80064-4	journal	January 1992
Acceleration of glass alteration rates induced by zeolite seeds at controlled pH Neeway, James J.; Parruzot, Benjamin P.; Bonnett, Jeffrey F. Applied Geochemistry, Vol. 113 https://doi.org/10.1016/j.apgeochem.2019.104515	journal	February 2020
Glass–water interphase reactivity with calcium rich solutions Chave, T.; Frugier, P.; Gin, S. Geochimica et Cosmochimica Acta, Vol. 75, Issue 15 https://doi.org/10.1016/j.gca.2011.05.005	journal	August 2011
The fate of silicon during glass corrosion under alkaline conditions: A mechanistic and kinetic study with the International Simple Glass Gin, Stéphane; Jollivet, Patrick; Fournier, Maxime Geochimica et Cosmochimica Acta, Vol. 151 https://doi.org/10.1016/j.gca.2014.12.009	journal	February 2015
Role of neoformed phases on the mechanisms controlling the resumption of SON68 glass alteration in alkaline media Ribet, Solange; Gin, Stéphane Journal of Nuclear Materials, Vol. 324, Issue 2-3 https://doi.org/10.1016/j.jnucmat.2003.09.010	journal	January 2004
Multi-glass investigation of Stage III glass dissolution behavior from 22 to 90 °C triggered by the addition of zeolite phases Parruzot, Benjamin; Ryan, Joseph V.; George, Jaime L. Journal of Nuclear Materials, Vol. 523 https://doi.org/10.1016/j.jnucmat.2019.05.050	journal	September 2019
An international initiative on long-term behavior of high-level nuclear waste glass Gin, S.; Abdelouas, A.; Criscenti, L. J. Materials Today, Vol. 16, Issue 6 https://doi.org/10.1016/j.mattod.2013.06.008	journal	June 2013
Effect of Zeolite Formation on Borosilicate Glass Dissolution Kinetics Fournier, Maxime; Frugier, Pierre; Gin, Stéphane Procedia Earth and Planetary Science, Vol. 7 https://doi.org/10.1016/j.proeps.2013.03.085	journal	January 2013
Recent Advances in Corrosion Science Applicable To Disposal of High-Level Nuclear Waste Frankel, Gerald S.; Vienna, John D.; Lian, Jie Chemical Reviews, Vol. 121, Issue 20 https://doi.org/10.1021/acs.chemrev.0c00990	journal	July 2021
Silicate Glass and Mineral Dissolution: Calculated Reaction Paths and Activation Energies for Hydrolysis of a Q ³ Si by H ₃ O ⁺ Using Ab Initio Methods Criscenti, Louise J.; Kubicki, James D.; Brantley, Susan L. The Journal of Physical Chemistry A, Vol. 110, Issue 1 https://doi.org/10.1021/jp044360a	journal	January 2006
Contribution of zeolite-seeded experiments to the understanding of resumption of glass alteration Fournier, Maxime; Gin, Stéphane; Frugier, Pierre npj Materials Degradation, Vol. 1, Issue 1 https://doi.org/10.1038/s41529-017-0018-x	journal	November 2017
Impacts of glass composition, pH, and temperature on glass forward dissolution rate Vienna, John D.; Neeway, James J.; Ryan, Joseph V. npj Materials Degradation, Vol. 2, Issue 1 https://doi.org/10.1038/s41529-018-0042-5	journal	August 2018
Influence of young cement water on the corrosion of the International Simple Glass Mann, Colleen; Ferrand, Karine; Liu, Sanheng npj Materials Degradation, Vol. 3, Issue 1 https://doi.org/10.1038/s41529-018-0059-9	journal	January 2019
In-situ monitoring of seeded and unseeded stage III corrosion using Raman spectroscopy Ryan, Joseph V.; Parruzot, Benjamin; Lines, Amanda M. npj Materials Degradation, Vol. 3, Issue 1 https://doi.org/10.1038/s41529-019-0095-0	journal	October 2019
Aqueous alteration of silicate glass: state of knowledge and perspectives Gin, Stéphane; Delaye, Jean-Marc; Angeli, Frédéric npj Materials Degradation, Vol. 5, Issue 1 https://doi.org/10.1038/s41529-021-00190-5	journal	August 2021
Kinetics of Phase Change. I General Theory Avrami, Melvin The Journal of Chemical Physics, Vol. 7, Issue 12, p. 1103-1112 https://doi.org/10.1063/1.1750380	journal	December 1939
Kinetics of Phase Change. II Transformation‐Time Relations for Random Distribution of Nuclei Avrami, Melvin The Journal of Chemical Physics, Vol. 8, Issue 2 https://doi.org/10.1063/1.1750631	journal	February 1940
Granulation, Phase Change, and Microstructure Kinetics of Phase Change. III Avrami, Melvin The Journal of Chemical Physics, Vol. 9, Issue 2, p. 177-184 https://doi.org/10.1063/1.1750872	journal	February 1941
Current Understanding and Remaining Challenges in Modeling Long-Term Degradation of Borosilicate Nuclear Waste Glasses Vienna, John D.; Ryan, Joseph V.; Gin, Stéphane International Journal of Applied Glass Science, Vol. 4, Issue 4 https://doi.org/10.1111/ijag.12050	journal	November 2013
Accelerated Leach Testing of GLASS (ALTGLASS): I. Informatics approach to high level waste glass gel formation and aging Jantzen, Carol M.; Trivelpiece, Cory L.; Crawford, Charles L. International Journal of Applied Glass Science, Vol. 8, Issue 1 https://doi.org/10.1111/ijag.12262	journal	February 2017
Durable Glass for Thousands of Years Jantzen, Carol M.; Brown, Kevin G.; Pickett, John B. International Journal of Applied Glass Science, Vol. 1, Issue 1 https://doi.org/10.1111/j.2041-1294.2010.00007.x	journal	March 2010
Seeded Stage III glass dissolution behavior of a statistically designed glass matrix Crum, Jarrod V.; Reiser, Joelle T.; Parruzot, Benjamin P. Journal of the American Ceramic Society, Vol. 104, Issue 8 https://doi.org/10.1111/jace.17823	journal	April 2021
Hydration Aging of Nuclear Waste Glass Bates, J. K.; Jardine, L. J.; Steindler, M. J. Science, Vol. 218, Issue 4567 https://doi.org/10.1126/science.218.4567.51	journal	October 1982
A Comparison of Glass Reaction at High and Low Glass Surface/Solution Volume Ebert, William L.; Bates, John K. Nuclear Technology, Vol. 104, Issue 3 https://doi.org/10.13182/NT93-A34898	journal	December 1993
Kinetics of Glass Dissolution and Zeolite Formation Under Hydrothermal Conditions Hawkins, Daniel B. Clays and Clay Minerals, Vol. 29, Issue 5 https://doi.org/10.1346/CCMN.1981.0290503	journal	January 1981
The Long-Term Corrosion and Modelling of Two Simulated Belgian Reference High-Level Waste Glasses Van Iseghem, P.; Grambow, B. MRS Proceedings, Vol. 112 https://doi.org/10.1557/PROC-112-631	journal	January 1987
Alteration of Nuclear Waste Glass by Hydration Bates, John K.; Steindler, Martin J. MRS Proceedings, Vol. 15 https://doi.org/10.1557/PROC-15-83	journal	January 1982
The Effect of Phase Formation on Glass Leaching Haaker, Richard; Malow, Gonter; Offermann, Peter MRS Proceedings, Vol. 44 https://doi.org/10.1557/PROC-44-121	journal	January 1984
The Role of Alteration Phases in Influencing the Kinetics of Glass Dissolution Wronkiewicz, D. J.; Arbesman, K. A. MRS Proceedings, Vol. 608 https://doi.org/10.1557/PROC-608-745	journal	January 1999
The dissolution of simulant UK Ca/Zn-modified nuclear waste glass: Insight into Stage III behavior Fisher, Adam J.; Harrison, Mike T.; Hyatt, Neil C. MRS Advances, Vol. 5, Issue 3-4 https://doi.org/10.1557/adv.2020.50	journal	January 2020
Nuclear Waste Glasses - How Durable? Grambow, B. Elements, Vol. 2, Issue 6 https://doi.org/10.2113/gselements.2.6.357	journal	December 2006
Formation of Zeolites in Open Hydrologic Systems Sheppard, R. A.; Hay, R. L. Reviews in Mineralogy and Geochemistry, Vol. 45, Issue 1 https://doi.org/10.2138/rmg.2001.45.8	journal	January 2001

Similar Records

Multi-glass investigation of Stage III glass dissolution behavior from 22 to 90 °C triggered by the addition of zeolite phases

Journal Article · Thu May 30 20:00:00 EDT 2019 · Journal of Nuclear Materials · OSTI ID:1561285

In-situ monitoring of seeded and unseeded stage III corrosion using Raman spectroscopy

Journal Article · Tue Oct 15 20:00:00 EDT 2019 · npj Materials Degradation · OSTI ID:1619760

Related Subjects

12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE WASTES FROM NUCLEAR FACILITIES
glass durability
long-term behavior
low-activity waste glass
zeolite

Effect of zeolite type, temperature, and pH on Stage III glass alteration behavior for two nuclear waste glasses

Citation Formats

References (38)

Similar Records

Related Subjects