Modelling the sulfate capacity of simulated radioactive waste borosilicate glasses
Abstract
In this paper, the capacity of simulated high-level radioactive waste borosilicate glasses to incorporate sulfate has been studied as a function of glass composition. Combined Raman, 57Fe Mössbauer and literature evidence supports the attribution of coordination numbers and oxidation states of constituent cations for the purposes of modelling, and results confirm the validity of correlating sulfate incorporation in multicomponent borosilicate radioactive waste glasses with different models. A strong compositional dependency is observed and this can be described by an inverse linear relationship between incorporated sulfate (mol% SO42-) and total cation field strength index of the glass, Σ(z/a2), with a high goodness-of-fit (R2 ≈ 0.950). Similar relationships are also obtained if theoretical optical basicity, Λth (R2 ≈ 0.930) or non-bridging oxygen per tetrahedron ratio, NBO/T (R2 ≈ 0.919), are used. Finally, results support the application of these models, and in particular Σ(z/a2), as predictive tools to aid the development of new glass compositions with enhanced sulfate capacities.
- Authors:
-
[1];
- Sheffield Hallam Univ., Sheffield (United Kingdom). Materials and Engineering Research Inst.
- Savannah River Site (SRS), Aiken, SC (United States). Savannah River National Lab. (SRNL)
- Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States). Biological and Environmental Science Directorate
- Pacific Northwest National Lab. (PNNL), Richland, WA (United States). Nuclear Sciences Division
- Publication Date:
- Research Org.:
- Oak Ridge National Laboratory (ORNL), Oak Ridge, TN (United States); Sheffield Hallam Univ., Sheffield (United Kingdom); Pacific Northwest National Laboratory (PNNL), Richland, WA (United States); Savannah River Site (SRS), Aiken, SC (United States)
- Sponsoring Org.:
- USDOE Office of Environmental Management (EM). International Cooperation Program; USDOE
- OSTI Identifier:
- 1335365
- Alternate Identifier(s):
- OSTI ID: 1397616
- Grant/Contract Number:
- AC05-00OR22725
- Resource Type:
- Accepted Manuscript
- Journal Name:
- Journal of Alloys and Compounds
- Additional Journal Information:
- Journal Volume: 695; Journal ID: ISSN 0925-8388
- Publisher:
- Elsevier
- Country of Publication:
- United States
- Language:
- English
- Subject:
- 12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE WASTES FROM NUCLEAR FACILITIES; Borosilicate; glass; sulfate; capacity; waste; radioactive
Citation Formats
Bingham, Paul A., Vaishnav, Shuchi, Forder, Sue D., Scrimshire, Alex, Jaganathan, Balaasaran, Rohini, Jijy, Marra, James C., Fox, Kevin M., Pierce, Eric M., Workman, Phyllis, and Vienna, John D. Modelling the sulfate capacity of simulated radioactive waste borosilicate glasses. United States: N. p., 2016.
Web. doi:10.1016/j.jallcom.2016.11.110.
Bingham, Paul A., Vaishnav, Shuchi, Forder, Sue D., Scrimshire, Alex, Jaganathan, Balaasaran, Rohini, Jijy, Marra, James C., Fox, Kevin M., Pierce, Eric M., Workman, Phyllis, & Vienna, John D. Modelling the sulfate capacity of simulated radioactive waste borosilicate glasses. United States. https://doi.org/10.1016/j.jallcom.2016.11.110
Bingham, Paul A., Vaishnav, Shuchi, Forder, Sue D., Scrimshire, Alex, Jaganathan, Balaasaran, Rohini, Jijy, Marra, James C., Fox, Kevin M., Pierce, Eric M., Workman, Phyllis, and Vienna, John D. Thu .
"Modelling the sulfate capacity of simulated radioactive waste borosilicate glasses". United States. https://doi.org/10.1016/j.jallcom.2016.11.110. https://www.osti.gov/servlets/purl/1335365.
@article{osti_1335365,
title = {Modelling the sulfate capacity of simulated radioactive waste borosilicate glasses},
author = {Bingham, Paul A. and Vaishnav, Shuchi and Forder, Sue D. and Scrimshire, Alex and Jaganathan, Balaasaran and Rohini, Jijy and Marra, James C. and Fox, Kevin M. and Pierce, Eric M. and Workman, Phyllis and Vienna, John D.},
abstractNote = {In this paper, the capacity of simulated high-level radioactive waste borosilicate glasses to incorporate sulfate has been studied as a function of glass composition. Combined Raman, 57Fe Mössbauer and literature evidence supports the attribution of coordination numbers and oxidation states of constituent cations for the purposes of modelling, and results confirm the validity of correlating sulfate incorporation in multicomponent borosilicate radioactive waste glasses with different models. A strong compositional dependency is observed and this can be described by an inverse linear relationship between incorporated sulfate (mol% SO42-) and total cation field strength index of the glass, Σ(z/a2), with a high goodness-of-fit (R2 ≈ 0.950). Similar relationships are also obtained if theoretical optical basicity, Λth (R2 ≈ 0.930) or non-bridging oxygen per tetrahedron ratio, NBO/T (R2 ≈ 0.919), are used. Finally, results support the application of these models, and in particular Σ(z/a2), as predictive tools to aid the development of new glass compositions with enhanced sulfate capacities.},
doi = {10.1016/j.jallcom.2016.11.110},
journal = {Journal of Alloys and Compounds},
number = ,
volume = 695,
place = {United States},
year = {Thu Nov 10 00:00:00 EST 2016},
month = {Thu Nov 10 00:00:00 EST 2016}
}
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