Modelling the sulfate capacity of simulated radioactive waste borosilicate glasses

P. A. Bingham; S. Vaishnav; S. D. Forder; A. Scrimshire; B. Jaganathan; J. Rohini; J. C. Marra; K. M. Fox; E. M. Pierce; P. Workman; J. D. Vienna

doi:10.1016/j.jallcom.2016.11.110

Modelling the sulfate capacity of simulated radioactive waste borosilicate glasses

P. A. Bingham, S. Vaishnav, S. D. Forder, A. Scrimshire, B. Jaganathan, J. Rohini, J. C. Marra, K. M. Fox, E. M. Pierce, P. Workman, J. D. Vienna

Environmental Sciences Division

Research output: Contribution to journal › Article › peer-review

31 Scopus citations

Abstract

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% SO₄ ²⁻) 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, Λ_th(R²≈ 0.930) or non-bridging oxygen per tetrahedron ratio, NBO/T (R²≈ 0.919), are used. 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.

Original language	English
Pages (from-to)	656-667
Number of pages	12
Journal	Journal of Alloys and Compounds
Volume	695
DOIs	https://doi.org/10.1016/j.jallcom.2016.11.110
State	Published - 2017

Funding

The authors gratefully acknowledge funding from the U.S. Department of Energy – Office of Environmental Management via the International Cooperation Program. The authors also wish to thank Papken Hovsepian for help with some of the Raman measurements, and an anonymous reviewer for their insightful comments and suggestions.

Funders	Funder number
U.S. Department of Energy
Office of Environmental Management

Keywords

Borosilicate
Capacity
Glass
Radioactive
Sulfate
Waste

UN SDGs

This output contributes to the following UN Sustainable Development Goals (SDGs)

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10.1016/j.jallcom.2016.11.110

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title = "Modelling the sulfate capacity of simulated radioactive waste borosilicate glasses",

abstract = "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 M{\"o}ssbauer 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% SO4 2−) 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. 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.",

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author = "Bingham, {P. A.} and S. Vaishnav and Forder, {S. D.} and A. Scrimshire and B. Jaganathan and J. Rohini and Marra, {J. C.} and Fox, {K. M.} and Pierce, {E. M.} and P. Workman and Vienna, {J. D.}",

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AU - Bingham, P. A.

AU - Vaishnav, S.

AU - Forder, S. D.

AU - Scrimshire, A.

AU - Jaganathan, B.

AU - Rohini, J.

AU - Marra, J. C.

AU - Fox, K. M.

AU - Pierce, E. M.

AU - Workman, P.

AU - Vienna, J. D.

PY - 2017

Y1 - 2017

N2 - 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% SO4 2−) 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. 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.

AB - 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% SO4 2−) 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. 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.

KW - Borosilicate

KW - Capacity

KW - Glass

KW - Radioactive

KW - Sulfate

KW - Waste

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Modelling the sulfate capacity of simulated radioactive waste borosilicate glasses

Abstract

Funding

Keywords

UN SDGs

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