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Title: Durability of Silicate Glasses: An Historical Approach

Abstract

We present a short review of current theories of glass weathering, including glass dissolution, and hydrolysis of nuclear waste glasses, and leaching of historical glasses from an XAFS perspective. The results of various laboratory leaching experiments at different timescales (30 days to 12 years) are compared with results for historical glasses that were weathered by atmospheric gases and soil waters over 500 to 3000 years. Good agreement is found between laboratory experiments and slowly leached historical glasses, with a strong enrichment of metals at the water/gel interface. Depending on the nature of the transition elements originally dissolved in the melt, increasing elemental distributions are expected to increase with time for a given glass durability context.

Authors:
; ; ; ; ; ; ; ; ; ; ;
Publication Date:
Research Org.:
Stanford Linear Accelerator Center (SLAC)
Sponsoring Org.:
USDOE
OSTI Identifier:
896945
Report Number(s):
SLAC-PUB-12221
TRN: US200705%%85
DOE Contract Number:
AC02-76SF00515
Resource Type:
Conference
Resource Relation:
Conference: Contributed to 13th International Conference on X-ray Absorption Fine Structure (XAFS13), Stanford, California, 9-14 Jul 2006
Country of Publication:
United States
Language:
English
Subject:
12 MANAGEMENT OF RADIOACTIVE WASTES, AND NON-RADIOACTIVE WASTES FROM NUCLEAR FACILITIES; ABSORPTION; DISSOLUTION; FINE STRUCTURE; GASES; GLASS; HYDROLYSIS; LEACHING; RADIOACTIVE WASTES; SILICATES; SOILS; TRANSITION ELEMENTS; WEATHERING; Other,BIO

Citation Formats

Farges, Francois, /Museum Natl. Hist. Natur. /Stanford U., Geo. Environ. Sci., Etcheverry, Marie-Pierre, /Marne la Vallee U., Haddi, Amine, /Marne la Valle U., Trocellier, Patrick, /Saclay, Curti, Enzo, /PSI, Villigen, Brown, Gordon E., Jr., and /SLAC, SSRL. Durability of Silicate Glasses: An Historical Approach. United States: N. p., 2007. Web.
Farges, Francois, /Museum Natl. Hist. Natur. /Stanford U., Geo. Environ. Sci., Etcheverry, Marie-Pierre, /Marne la Vallee U., Haddi, Amine, /Marne la Valle U., Trocellier, Patrick, /Saclay, Curti, Enzo, /PSI, Villigen, Brown, Gordon E., Jr., & /SLAC, SSRL. Durability of Silicate Glasses: An Historical Approach. United States.
Farges, Francois, /Museum Natl. Hist. Natur. /Stanford U., Geo. Environ. Sci., Etcheverry, Marie-Pierre, /Marne la Vallee U., Haddi, Amine, /Marne la Valle U., Trocellier, Patrick, /Saclay, Curti, Enzo, /PSI, Villigen, Brown, Gordon E., Jr., and /SLAC, SSRL. Tue . "Durability of Silicate Glasses: An Historical Approach". United States. doi:. https://www.osti.gov/servlets/purl/896945.
@article{osti_896945,
title = {Durability of Silicate Glasses: An Historical Approach},
author = {Farges, Francois and /Museum Natl. Hist. Natur. /Stanford U., Geo. Environ. Sci. and Etcheverry, Marie-Pierre and /Marne la Vallee U. and Haddi, Amine and /Marne la Valle U. and Trocellier, Patrick and /Saclay and Curti, Enzo and /PSI, Villigen and Brown, Gordon E., Jr. and /SLAC, SSRL},
abstractNote = {We present a short review of current theories of glass weathering, including glass dissolution, and hydrolysis of nuclear waste glasses, and leaching of historical glasses from an XAFS perspective. The results of various laboratory leaching experiments at different timescales (30 days to 12 years) are compared with results for historical glasses that were weathered by atmospheric gases and soil waters over 500 to 3000 years. Good agreement is found between laboratory experiments and slowly leached historical glasses, with a strong enrichment of metals at the water/gel interface. Depending on the nature of the transition elements originally dissolved in the melt, increasing elemental distributions are expected to increase with time for a given glass durability context.},
doi = {},
journal = {},
number = ,
volume = ,
place = {United States},
year = {Tue Jan 02 00:00:00 EST 2007},
month = {Tue Jan 02 00:00:00 EST 2007}
}

Conference:
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  • We present a short review of current theories of glass weathering, including glass dissolution, and hydrolysis of nuclear waste glasses, and leaching of historical glasses from an XAFS perspective. The results of various laboratory leaching experiments at different timescales (30 days to 12 years) are compared with results for historical glasses that were weathered by atmospheric gases and soil waters over 500 to 3000 years. Good agreement is found between laboratory experiments and slowly leached historical glasses, with a strong enrichment of metals at the water/gel interface. Depending on the nature of the transition elements originally dissolved in the melt,more » increasing elemental distributions are expected to increase with time for a given glass durability context.« less
  • The corrosion by water of glass made by fusing nepheline syenite with various fluxing agents has been investigated. The objective is to obtain a workable glass that would incorporate waste fission products and have a high resistance to attack by water. Glass of composition 15 wt.% CaO, 85 wt.% nepheline syenite, has been found to have a corrosion rate of 2 x 10/sup -8/ g glass/cm/sup 2/day at room temperature after the first few days of water contact. The effect of pH on the corrosion rate has been investigated and also the selective leaching of cations of different valency. (auth)
  • The research efforts to evaluate the process of radiation damage in nuclear waste materials has centered about the description of radiation damage in borosilicate and binary silicate glasses. The mechanism by which radiation damage occurs in these glasses from electrons is due to the formation of molecular oxygen by ionization processes. The aggregation of the oxygen depends upon the migration of the associated cation interstitials from the damage siltes and the local oxygen concentration is not significantly altered by the formation of the bubbles in the early stages of growth. Investigations into the radiation damage of nuclear waste materials frommore » heavy particles has shown that for uniform ion dose at low energy and moderate flux microstructures similar to those formed from electron irradiation can result. It is apparent, however, that the two radiation damage processes are completely different. The model for the durability of amorphous nuclear waste material is continuing and comparisons with diffusion experiments show that a reasonable fit to the models can be made in glass. The diffusion is described in terms of anion and cation diffusion through a polygonal hole network with various binding energies favoring the ions to particular sites because of charge compensation. 12 references, 1 figure.« less
  • Simulated high-level waste glass samples of the DWPF projected compositions were annealed at various times and temperatures in order to develop time-temperature-transformation diagrams. These heat treated glasses were subjected to the Product Consistency Test (PCT) to evaluate glass durability. The B, Li, and Na concentrations in the leachate (the PCT results) were compared to the PCT results of the Environmental Assessment benchmark glass. Durability as a function of glass composition and crystallinity was also examined.