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Title: Joint EM-NE-International Study of Glass Behavior over Geologic Time Scales - 12303

Abstract

Vitrification has been chosen as the best demonstrated available technology for waste immobilization worldwide. To date, the contributions of physical and chemical processes controlling the long-term glass dissolution rate in geologic disposal remain uncertain, leading to a lack of international consensus on a rate law for glass corrosion. Existing rate laws have overcome uncertainty through conservatism, but a thorough mechanistic understanding of waste form durability in geologic environments would improve public and regulator confidence. If it is possible to take credit for the true durability of the waste form in repository system evaluations, then it is possible to design the repository with less conservatism with concomitant cost savings. To gain a fundamental understanding of the dissolution rate law, six nations have joined together to formulate a joint plan for collaborative research into the mechanisms controlling the long-term corrosion of glass. This report highlights the technical program plan behind the US portion of this effort, with an emphasis on the current understanding (and limitations) of several mechanistic theories for glass corrosion. Some recent results are presented to provide an example of the ongoing research. Atom probe tomography has been used to provide a high-resolution analysis of elemental concentration gradients present atmore » the hydrated glass / pristine glass interface in SON68 after 25.75 years of corrosion in a simulated granitic groundwater at 90 deg. C. The most valuable result of these initial studies is the success of the technique. Characterization by APT had never been previously demonstrated for glass corrosion layers. The resolution of APT is a powerful addition to the tools with which we can investigate the mechanisms dominating glass corrosion. Some other key results of this study include the observation that the elemental interfacial width between the hydrated glass and pristine glass appears to be much sharper (∼2 nm for B, Na and Al) than had been previously measured using nanoSIMS (∼240 nm). It is not clear whether the APT analysis and nanoSIMS characterizations were possibly performed on topographically unique regions, or whether nanoSIMS overestimated the elemental width. However, the APT data seems very convincing that the elemental width can be much sharper than was previously thought. This result calls into question some of the assumptions made for the diffusion-control models of glass dissolution, since such a sharp profile would not match the diffusion coefficients used to date. Other results, such as the observation of apparently layered concentration profiles, show that gel evolution is not as simple as is currently assumed in nearly every model. This task is a good example of the collaborative nature of the I-TEAM effort. Based on experimental needs and differences in expertise, scientists from DOE and CEA worked together to change the level of understanding in the field. These types of interactions are nearly ubiquitous among the tasks in the technical program plan. With the excellence of the team in place and the willingness of the participants to work together for a common understanding, the stated goal of consensus on the mechanistic basis for radionuclide release from glass is well within reach. (authors)« less

Authors:
; ; ;  [1];  [2];  [3]
  1. Pacific Northwest National Laboratory, P. O. Box 999, Richland, WA 99352 (United States)
  2. Argonne National Laboratory, Argonne, IL 60439 (United States)
  3. Lawrence Berkeley National Laboratory, One Cyclotron Road, Berkeley, CA 94720 (United States)
Publication Date:
Research Org.:
WM Symposia, 1628 E. Southern Avenue, Suite 9-332, Tempe, AZ 85282 (United States)
OSTI Identifier:
22293576
Report Number(s):
INIS-US-14-WM-12303
TRN: US14V1232115100
Resource Type:
Conference
Resource Relation:
Conference: WM2012: Waste Management 2012 conference on improving the future in waste management, Phoenix, AZ (United States), 26 Feb - 1 Mar 2012; Other Information: Country of input: France; 79 refs.
Country of Publication:
United States
Language:
English
Subject:
12 MANAGEMENT OF RADIOACTIVE WASTES, AND NON-RADIOACTIVE WASTES FROM NUCLEAR FACILITIES; 36 MATERIALS SCIENCE; CONTROL; CORROSION; DIFFUSION; DISSOLUTION; EVALUATION; GLASS; HARDNESS; INTERACTIONS; SIMULATION; WASTE FORMS

Citation Formats

Ryan, J. V., Schreiber, D. K., Strachan, D. M., Vienna, J. D., Ebert, W. L., and Icenhower, J. P. Joint EM-NE-International Study of Glass Behavior over Geologic Time Scales - 12303. United States: N. p., 2012. Web.
Ryan, J. V., Schreiber, D. K., Strachan, D. M., Vienna, J. D., Ebert, W. L., & Icenhower, J. P. Joint EM-NE-International Study of Glass Behavior over Geologic Time Scales - 12303. United States.
Ryan, J. V., Schreiber, D. K., Strachan, D. M., Vienna, J. D., Ebert, W. L., and Icenhower, J. P. Sun . "Joint EM-NE-International Study of Glass Behavior over Geologic Time Scales - 12303". United States.
@article{osti_22293576,
title = {Joint EM-NE-International Study of Glass Behavior over Geologic Time Scales - 12303},
author = {Ryan, J. V. and Schreiber, D. K. and Strachan, D. M. and Vienna, J. D. and Ebert, W. L. and Icenhower, J. P.},
abstractNote = {Vitrification has been chosen as the best demonstrated available technology for waste immobilization worldwide. To date, the contributions of physical and chemical processes controlling the long-term glass dissolution rate in geologic disposal remain uncertain, leading to a lack of international consensus on a rate law for glass corrosion. Existing rate laws have overcome uncertainty through conservatism, but a thorough mechanistic understanding of waste form durability in geologic environments would improve public and regulator confidence. If it is possible to take credit for the true durability of the waste form in repository system evaluations, then it is possible to design the repository with less conservatism with concomitant cost savings. To gain a fundamental understanding of the dissolution rate law, six nations have joined together to formulate a joint plan for collaborative research into the mechanisms controlling the long-term corrosion of glass. This report highlights the technical program plan behind the US portion of this effort, with an emphasis on the current understanding (and limitations) of several mechanistic theories for glass corrosion. Some recent results are presented to provide an example of the ongoing research. Atom probe tomography has been used to provide a high-resolution analysis of elemental concentration gradients present at the hydrated glass / pristine glass interface in SON68 after 25.75 years of corrosion in a simulated granitic groundwater at 90 deg. C. The most valuable result of these initial studies is the success of the technique. Characterization by APT had never been previously demonstrated for glass corrosion layers. The resolution of APT is a powerful addition to the tools with which we can investigate the mechanisms dominating glass corrosion. Some other key results of this study include the observation that the elemental interfacial width between the hydrated glass and pristine glass appears to be much sharper (∼2 nm for B, Na and Al) than had been previously measured using nanoSIMS (∼240 nm). It is not clear whether the APT analysis and nanoSIMS characterizations were possibly performed on topographically unique regions, or whether nanoSIMS overestimated the elemental width. However, the APT data seems very convincing that the elemental width can be much sharper than was previously thought. This result calls into question some of the assumptions made for the diffusion-control models of glass dissolution, since such a sharp profile would not match the diffusion coefficients used to date. Other results, such as the observation of apparently layered concentration profiles, show that gel evolution is not as simple as is currently assumed in nearly every model. This task is a good example of the collaborative nature of the I-TEAM effort. Based on experimental needs and differences in expertise, scientists from DOE and CEA worked together to change the level of understanding in the field. These types of interactions are nearly ubiquitous among the tasks in the technical program plan. With the excellence of the team in place and the willingness of the participants to work together for a common understanding, the stated goal of consensus on the mechanistic basis for radionuclide release from glass is well within reach. (authors)},
doi = {},
journal = {},
number = ,
volume = ,
place = {United States},
year = {2012},
month = {7}
}

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