Sulfur behavior in silicate glasses and melts: Implications for sulfate incorporation in nuclear waste glasses as a function of alkali cation and V2O5 content

Manara, D.; Grandjean, Agnès; Pinet, O.; Dussossoy, Jean-Luc; Neuville, Daniel R.

doi:10.1016/j.jnoncrysol.2006.09.041

Cited by 103 publications

(139 citation statements)

References 45 publications

(105 reference statements)

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“…However, they do not greatly detract from it either, indicating some involvement of B 2 O 3 and Al 2 O 3 in the determination of sulfate solubilities, consistent with the cation field strength approach. A French study [15] showed that variation in the ratio R = [Na [Balance] ratio of 0.6667, which is consistent with the data modelled here, as shown in Figure 12.…”

Section: Modelling Using Simple Compositional Modelssupporting

confidence: 89%

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Summary of Fy11 Sulfate Retention Studies for Defense Waste Processing Facility Glass

Fox¹,

Edwards²

2012

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Section: Modelling Using Simple Compositional Modelssupporting

confidence: 89%

“…13,14 A well characterized standard glass was used to determine the appropriate spindle constants. 14,15 Measurements were taken over a range of temperatures from 1050 to 1250 °C in 50 °C intervals. Measurements at a See data in SRNL-L3100-2011-00038, transmitted by email to the University of Sheffield March 1, 2011.…”

Section: Influence Of Viscositymentioning

confidence: 99%

Summary of Fy11 Sulfate Retention Studies for Defense Waste Processing Facility Glass

Fox¹,

Edwards²

2012

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“…As summarised elsewhere [67][68][69][70][71] There is no suggestion of lower oxidation of sulfur states than S(VI) in these glasses. The absence of Raman bands related to S-S bonds, S(IV) or S(V) complexes, which provide broad bands in the region 300 -460 cm -1 [72,73] supports this.…”

Section: Accepted Manuscriptmentioning

confidence: 67%

Modelling the sulfate capacity of simulated radioactive waste borosilicate glasses

Bingham

Vaishnav

Forder

et al. 2017

Journal of Alloys and Compounds

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(2017). Modelling the sulfate capacity of simulated radioactive waste borosilicate glasses. Journal of Alloys and Compounds, 695,[656][657][658][659][660][661][662][663][664][665][666][667]. This is a PDF file of an unedited manuscript that has been accepted for publication. As a service to our customers we are providing this early version of the manuscript. The manuscript will undergo copyediting, typesetting, and review of the resulting proof before it is published in its final form. Please note that during the production process errors may be discovered which could affect the content, and all legal disclaimers that apply to the journal pertain. Copyright and re-use policy M A N U S C R I P T A C C E P T E D ACCEPTED MANUSCRIPT

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“…Sulfate is present in nuclear waste most usually due to the use of [Fe(NH 2 SO 3 ) 2 ] as a reducing agent of Pu 4+ to Pu 3+ [3][4][5] . The sulfate can also be a result of effluents of radioactive solutions, ion -exchanging resins, or of incineration before vitrification [6] .…”

Section: General Sulfur Behaviormentioning

confidence: 99%

“…Some factors that influence the valence state of the sulfur are temperature, reactivity, the partial pressure of sulfur-containing species over the glass melt, and the reduction-oxidation (redox) conditions of the melt [6] . In reducing conditions, the dissolution of sulfur is strongly dependent on Fe and less dependent on f(O 2 ), whereas in oxidizing conditions, it is strongly dependent on f(O 2 ).…”

Section: General Sulfur Behaviormentioning

confidence: 99%

Additive Testing for Improved Sulfur Retention: Preliminary Report

Amoroso¹,

Fox²

2011

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The Savannah River National Laboratory is collaborating with Alfred University to evaluate the potential for additives in borosilicate glass to improve sulfur retention. This preliminary report provides further background on the incorporation of sulfur in glass and outlines the experiments that are being performed by the collaborators. A simulated waste glass composition has been selected for the experimental studies. The first phase of experimental work will evaluate the impacts of BaO, PbO, and V 2 O 5 at concentrations of 1.0, 2.0, and 5.0 wt % on sulfate retention in simulated high level waste borosilicate glass. The second phase of experimental work will evaluate the effects of time at the melt temperature on sulfur retention. The resulting samples will be characterized to determine the amount of sulfur remaining as well as to identify the formation of any crystalline phases. The results will be used to guide the future selection of frits and glass forming chemicals in vitrifying Department of Energy wastes containing high sulfur concentrations. SRNL-STI-2011-00524Revision 0 vi LIST OF TABLES IntroductionSulfur has a low solubility in borosilicate glasses. This presents a significant challenge to the U.S. Department of Energy (DOE) immobilization campaigns for wastes with high sulfur concentrations since borosilicate glass is being used to vitrify high level radioactive waste (HLW) at the Savannah River Site (SRS) and is planned for use in vitrifying wastes at Hanford. A more thorough understanding of the incorporation of sulfur in the borosilicate glass network (and the issues that hinder its incorporation) could lead to improvements in sulfur retention, allowing for a higher level of waste loading in the glass.The Savannah River National Laboratory (SRNL) is collaborating with Alfred University (AU) to evaluate the potential for additives in the borosilicate glass frit or glass forming chemicals to improve sulfur retention. This preliminary report provides further background on the incorporation of sulfur in glass and outlines the experiments that will be performed by the collaborators. AU has completed a survey of relevant literature and provided recommendations for the experimental work. That document is included as Appendix A. The experimental work will be performed using simulated, non-radioactive glasses, with the intent of identifying modifications that can be made to the frit compositions recommended for future operation of the Defense Waste Processing Facility (DWPF) at SRS for improved sulfur retention. SRNL-STI-2011-00524Revision 0 2 Evaluation of Frit AdditivesCollaborators at AU have recommended that three frit additives, BaO, PbO, and V 2 O 5 , be evaluated for potential improvements in sulfate retention. Batching, melting, and some characterization of test glasses for this phase of the experimental work will be completed by AU. The recommended additives will be added in concentrations of 1.0, 2.0, and 5.0 wt %. The concentrations of the frit components in the glass will be reduced propo...

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Sulfur behavior in silicate glasses and melts: Implications for sulfate incorporation in nuclear waste glasses as a function of alkali cation and V2O5 content

Cited by 103 publications

References 45 publications

Summary of Fy11 Sulfate Retention Studies for Defense Waste Processing Facility Glass

Summary of Fy11 Sulfate Retention Studies for Defense Waste Processing Facility Glass

Modelling the sulfate capacity of simulated radioactive waste borosilicate glasses

Additive Testing for Improved Sulfur Retention: Preliminary Report

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