Accelerated Leach Testing of Glass (ALTGLASS): II. Mineralization of hydrogels by leachate strong bases
Abstract
The durability of high level nuclear waste glasses must be predicted on geological time scales. Waste glass surfaces form hydrogels when in contact with water for varying test durations. As the glass hydrogels age, some exhibit an undesirable resumption of dissolution at long times while others exhibit near steady-state dissolution, that is, nonresumption of dissolution. Resumption of dissolution is associated with the formation of zeolitic phases while nonresumption of dissolution is associated with the formation of clay minerals. Hydrogels with a stoichiometry close to that of imogolite, (Al2O3·Si(OH)4), with ferrihydrite (Fe2O3·0.5H2O), have been shown to be associated with waste glasses that resume dissolution. Aluminosilicate hydrogels with a stoichiometry of allophane-hisingerite ((Al,Fe)2O3·1.3-2Si(OH)4) have been shown to be associated with waste glasses that exhibit near steady-state dissolution at long times. These phases are all amorphous and poorly crystalline and are also found on natural weathered basalt glasses. Interaction of these hydrogels with excess alkali and OH– (strong base) in the leachates, causes the Al2O3·nSiO2 (where n=1-2) hydrogels to mineralize to zeolites. Excess alkali in the leachate is generated by alkali in the glass. As a result, preliminary rate-determining leach layer forming exchange reactions are hypothesized based on these findings.
- Authors:
-
- Savannah River National Lab., Aiken, SC (United States)
- Publication Date:
- Research Org.:
- Savannah River Site (SRS), Aiken, SC (United States)
- Sponsoring Org.:
- USDOE
- OSTI Identifier:
- 1372632
- Report Number(s):
- SRNL-STI-2014-00381
Journal ID: ISSN 2041-1286
- Grant/Contract Number:
- AC09-08SR22470
- Resource Type:
- Accepted Manuscript
- Journal Name:
- International Journal of Applied Glass Science
- Additional Journal Information:
- Journal Volume: 8; Journal Issue: 1; Journal ID: ISSN 2041-1286
- Publisher:
- American Ceramic Society
- Country of Publication:
- United States
- Language:
- English
- Subject:
- 12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE WASTES FROM NUCLEAR FACILITIES; 36 MATERIALS SCIENCE; corrosion; glass durability; glass leaching; modeling; nuclear waste; aging
Citation Formats
Jantzen, Carol M., Trivelpiece, Cory L., Crawford, Charles L., Pareizs, John M., and Pickett, John B. Accelerated Leach Testing of Glass (ALTGLASS): II. Mineralization of hydrogels by leachate strong bases. United States: N. p., 2017.
Web. doi:10.1111/ijag.12264.
Jantzen, Carol M., Trivelpiece, Cory L., Crawford, Charles L., Pareizs, John M., & Pickett, John B. Accelerated Leach Testing of Glass (ALTGLASS): II. Mineralization of hydrogels by leachate strong bases. United States. https://doi.org/10.1111/ijag.12264
Jantzen, Carol M., Trivelpiece, Cory L., Crawford, Charles L., Pareizs, John M., and Pickett, John B. Sat .
"Accelerated Leach Testing of Glass (ALTGLASS): II. Mineralization of hydrogels by leachate strong bases". United States. https://doi.org/10.1111/ijag.12264. https://www.osti.gov/servlets/purl/1372632.
@article{osti_1372632,
title = {Accelerated Leach Testing of Glass (ALTGLASS): II. Mineralization of hydrogels by leachate strong bases},
author = {Jantzen, Carol M. and Trivelpiece, Cory L. and Crawford, Charles L. and Pareizs, John M. and Pickett, John B.},
abstractNote = {The durability of high level nuclear waste glasses must be predicted on geological time scales. Waste glass surfaces form hydrogels when in contact with water for varying test durations. As the glass hydrogels age, some exhibit an undesirable resumption of dissolution at long times while others exhibit near steady-state dissolution, that is, nonresumption of dissolution. Resumption of dissolution is associated with the formation of zeolitic phases while nonresumption of dissolution is associated with the formation of clay minerals. Hydrogels with a stoichiometry close to that of imogolite, (Al2O3·Si(OH)4), with ferrihydrite (Fe2O3·0.5H2O), have been shown to be associated with waste glasses that resume dissolution. Aluminosilicate hydrogels with a stoichiometry of allophane-hisingerite ((Al,Fe)2O3·1.3-2Si(OH)4) have been shown to be associated with waste glasses that exhibit near steady-state dissolution at long times. These phases are all amorphous and poorly crystalline and are also found on natural weathered basalt glasses. Interaction of these hydrogels with excess alkali and OH– (strong base) in the leachates, causes the Al2O3·nSiO2 (where n=1-2) hydrogels to mineralize to zeolites. Excess alkali in the leachate is generated by alkali in the glass. As a result, preliminary rate-determining leach layer forming exchange reactions are hypothesized based on these findings.},
doi = {10.1111/ijag.12264},
journal = {International Journal of Applied Glass Science},
number = 1,
volume = 8,
place = {United States},
year = {Sat Feb 18 00:00:00 EST 2017},
month = {Sat Feb 18 00:00:00 EST 2017}
}
Web of Science
Works referenced in this record:
Weathering characteristics of natural glass and influences on associated water chemistry
journal, September 1984
- White, Art F.
- Journal of Non-Crystalline Solids, Vol. 67, Issue 1-3
36. Hydrothermal chemistry of the silicates. Part VIII. Low-temperature crystal growth of aluminosilicates, and of some gallium and germanium analogues
journal, January 1959
- Barrer, R. M.; Baynham, J. W.; Bultitude, F. W.
- Journal of the Chemical Society (Resumed)
Applications of NMR Spectroscopy to the Study of Zeolite Synthesis
book, July 1989
- Bell, Alexis T.
- Zeolite Synthesis
First-Principles Study of Hydrolysis Reaction Barriers in a Sodium Borosilicate Glass
journal, November 2013
- Zapol, Peter; He, Haiying; Kwon, Kideok D.
- International Journal of Applied Glass Science, Vol. 4, Issue 4
Zeolite formation during the alkaline reaction of bentonite [Zeolite formation during the alkaline reaction of bentonite]
journal, May 2001
- De La Villa, Raquel Vigil; Cuevas, Jaime; Ramírez, Susana
- European Journal of Mineralogy, Vol. 13, Issue 3
The mechanism of the sodalite-to-cancrinite phase transformation in synthetic spent Bayer liquor
journal, November 1999
- Barnes, Mark C.; Addai-Mensah, Jonas; Gerson, Andrea R.
- Microporous and Mesoporous Materials, Vol. 31, Issue 3
Binders for radioactive waste forms made from pretreated calcined sodium bearing waste
journal, January 2004
- Bao, Yun; Kwan, S.; Siemer, D. D.
- Journal of Materials Science, Vol. 39, Issue 2
Chemical corrosion of highly radioactive borosilicate nuclear waste glass under simulated repository conditions
journal, May 1990
- Werme, Las; Björner, Inga K.; Bart, Gerhard
- Journal of Materials Research, Vol. 5, Issue 5
Possibilities and limitations of the prediction of the Si/Al ratios of zeolites from the batch composition
journal, November 2000
- Lechert, Hans
- Microporous and Mesoporous Materials, Vol. 40, Issue 1-3
Hydrothermal behaviour of simulated waste glass—And waste—Rock interactions under repository conditions
journal, June 1982
- Savage, D.; Chapman, N. A.
- Chemical Geology, Vol. 36, Issue 1-2
Nature and role of natural alteration gels formed on the surface of ancient volcanic glasses (Natural analogs of waste containment glasses)
journal, September 2003
- Crovisier, Jean-Louis; Advocat, Thierry; Dussossoy, Jean-Luc
- Journal of Nuclear Materials, Vol. 321, Issue 1
The effect of molecular structure on borosilicate glass leaching
journal, October 1986
- Bunker, B. C.; Arnold, G. W.; Day, D. E.
- Journal of Non-Crystalline Solids, Vol. 87, Issue 1-2
Zeolite synthesis and crystallization
journal, January 1980
- Sand, L. B.
- Pure and Applied Chemistry, Vol. 52, Issue 9
Solubility of Zeolite A and Its Amorphous Precursor under Synthesis Conditions
journal, May 1999
- Ejaz, Tabassum; Jones, Alan G.; Graham, Peter
- Journal of Chemical & Engineering Data, Vol. 44, Issue 3
Crystal Chemistry of Hydrous Iron Silicate Scale Deposits at the Salton Sea Geothermal Field
journal, January 1995
- Manceau, A.
- Clays and Clay Minerals, Vol. 43, Issue 3
Hydroceramics, a “new” cementitious waste form material for U.S. defense-type reprocessing waste
journal, September 2002
- Siemer, Darryl D.
- Materials Research Innovations, Vol. 6, Issue 3
Solubility of aluminosilicates in alkaline solutions and a thermodynamic equilibrium model
journal, April 1992
- Gasteiger, Hubert A.; Frederick, William J.; Streisel, Robert C.
- Industrial & Engineering Chemistry Research, Vol. 31, Issue 4
Accelerated Leach Testing of GLASS (ALTGLASS): I. Informatics approach to high level waste glass gel formation and aging
journal, February 2017
- Jantzen, Carol M.; Trivelpiece, Cory L.; Crawford, Charles L.
- International Journal of Applied Glass Science, Vol. 8, Issue 1
Ostwald ripening and its application to precipitates and colloids in ionic crystals and glasses
journal, August 1978
- Jain, S. C.; Hughes, A. E.
- Journal of Materials Science, Vol. 13, Issue 8
Zeolite Formation from Synthetic and Natural Glasses
book, August 1974
- Aiello, R.; Colella, C.; Sersale, R.
- Molecular Sieve Zeolites-I
Bayer process plant scale: transformation of sodalite to cancrinite
journal, January 1997
- Gerson, Andrea R.; Zheng, Kali
- Journal of Crystal Growth, Vol. 171, Issue 1-2
Preparation and Properties of Hydroceramic Waste Forms Made with Simulated Hanford Low-Activity Waste
journal, December 2005
- Bao, Yun; Grutzeck, Michael W.; Jantzen, Carol M.
- Journal of the American Ceramic Society, Vol. 88, Issue 12
Polymerization of silicate and aluminate tetrahedra in glasses, melts, and aqueous solutions—IV. Aluminum coordination in glasses and aqueous solutions and comments on the aluminum avoidance principle
journal, July 1983
- de Jong, B. H. W. S.; Schramm, Charles M.; Parziale, Victor E.
- Geochimica et Cosmochimica Acta, Vol. 47, Issue 7
Alteration effects and leach rates of basaltic glasses: Implications for the long-term stability of nuclear waste form borosilicate glasses
journal, September 1984
- Malow, G.; Lutze, W.; Ewing, R. C.
- Journal of Non-Crystalline Solids, Vol. 67, Issue 1-3
Structure of boroaluminosilicate glasses: Impact of [Al O ]/[SiO ] ratio on the structural role of sodium
journal, August 2012
- Zheng, Q. J.; Youngman, R. E.; Hogue, C. L.
- Physical Review B, Vol. 86, Issue 5
Geothermal mineral equilibria
journal, March 1981
- Giggenbach, Werner F.
- Geochimica et Cosmochimica Acta, Vol. 45, Issue 3
Synthesis and characterisation of materials based on inorganic polymers of alumina and silica: sodium polysialate polymers
journal, September 2000
- Barbosa, Valeria F. F.; MacKenzie, Kenneth J. D.; Thaumaturgo, Clelio
- International Journal of Inorganic Materials, Vol. 2, Issue 4
Energetics of the Charge-Coupled Substitution Si4+ Na+ + T3+ in the-Glasses NaTO2-SiO2 (T = Al, Fe, Ga, B)
journal, July 1990
- Yoreo, James J.; Navrotsky, Alexandra; Dingwell, Don B.
- Journal of the American Ceramic Society, Vol. 73, Issue 7
Thermodynamic model of natural, medieval and nuclear waste glass durability
journal, September 1984
- Jantzen, C. M.; Plodinec, M. J.
- Journal of Non-Crystalline Solids, Vol. 67, Issue 1-3
The hydrothermal synthesis of zeolites: Precursors, intermediates and reaction mechanism
journal, July 2005
- Cundy, Colin S.; Cox, Paul A.
- Microporous and Mesoporous Materials, Vol. 82, Issue 1-2
Durable Glass for Thousands of Years
journal, March 2010
- Jantzen, Carol M.; Brown, Kevin G.; Pickett, John B.
- International Journal of Applied Glass Science, Vol. 1, Issue 1
Role of neoformed phases on the mechanisms controlling the resumption of SON68 glass alteration in alkaline media
journal, January 2004
- Ribet, Solange; Gin, Stéphane
- Journal of Nuclear Materials, Vol. 324, Issue 2-3
Experimental determination of the effect of the ratio of B/Al on glass dissolution along the nepheline (NaAlSiO4)–malinkoite (NaBSiO4) join
journal, May 2010
- Pierce, E. M.; Reed, L. R.; Shaw, W. J.
- Geochimica et Cosmochimica Acta, Vol. 74, Issue 9
Distribution and genesis of authigenic silicate minerals in tuffs of Pleistocene Lake Tecopa, Inyo County, California
report, January 1968
- Sheppard, Richard A.; Gude, Arthur J.
- USGS
Radiation effects in moist-air systems and the influence of radiolytic product formation on nuclear waste glass corrosion
report, July 1997
- Wronkiewicz, D. J.; Bates, J. K.; Buck, E. C.
Hierarchical Modeling of HLW Glass-Gel-Solution Systems for Stage 3 Glass Degradation
journal, January 2015
- Jantzen, Carol M.; Crawford, Charles L.
- MRS Proceedings, Vol. 1744
Thermodynamic Modeling of the SRS Evaporators: Part I. The 2H and 2F System
report, May 2002
- Jantzen, C. M.; Laurinat, J. E.; Brown, K. G.
Thermodynamic Modeling of the SRS Evaporators: Part II. The 3H System
report, May 2002
- Jantzen, C. M.; Laurinat, J. E.; Brown, K. G.
Thermodynamic Modeling of the SRS Evaporators: Part III. Temperature, Evaporation, and Composition Effects on Process Control Strategy
report, September 2002
- Jantzen, C. M.; Brown, K. G.; Edwards, T. B.
Thermodynamic Modeling of the SRS Evaporators: Part IV. Incorporation of High Caustic Aluminosilicate Solubility Data
report, April 2003
- Jantzen, C. M.; Pareizs, J. M.; Edwards, T. B.
Thermodynamic Modeling of the SRS Evaporators: Part V. Validation
report, July 2003
- Pareizs, J. M.; Jantzen, C. M.
Phase Transformation of Zeolite P to Y and Analcime Zeolites due to Changing the Time and Temperature
journal, January 2013
- Azizi, Seyed Naser; Alavi Daghigh, Akram; Abrishamkar, Maryam
- Journal of Spectroscopy, Vol. 2013
Works referencing / citing this record:
Authigenic Mineral Texture in Submarine 1979 Basalt Drill Core, Surtsey Volcano, Iceland
journal, July 2019
- Jackson, M. D.; Couper, S.; Stan, C. V.
- Geochemistry, Geophysics, Geosystems, Vol. 20, Issue 7
A comparative review of the aqueous corrosion of glasses, crystalline ceramics, and metals
journal, May 2018
- Frankel, Gerald S.; Vienna, John D.; Lian, Jie
- npj Materials Degradation, Vol. 2, Issue 1
In-situ monitoring of seeded and unseeded stage III corrosion using Raman spectroscopy
journal, October 2019
- Ryan, Joseph V.; Parruzot, Benjamin; Lines, Amanda M.
- npj Materials Degradation, Vol. 3, Issue 1
Pre-Viking Swedish hillfort glass: A prospective long-term alteration analogue for vitrified nuclear waste
journal, April 2018
- Weaver, Jamie L.; Pearce, Carolyn I.; Sjöblom, Rolf
- International Journal of Applied Glass Science, Vol. 9, Issue 4