DOE PAGES title logo U.S. Department of Energy
Office of Scientific and Technical Information

Title: A crucible salt saturation method for determining sulfur solubility in glass melt

Abstract

Abstract Experiments were conducted to determine sulfur solubility in Hanford low‐activity waste ( LAW ) glass melts by a sulfur saturation method. Sulfur‐incorporated glass melts were prepared by salt saturation and bubbling methods. The salt saturation method was performed by mixing crushed premelted baseline glasses with an excess amount of Na 2 SO 4 prior to melting the mixture at 1150°C for 1 hour. The bubbling method involved bubbling the glass melt at 1150°C in a Pt crucible with an SO 2 /O 2 /N 2 gas mix to equilibrate the melt at a known pressure of SO 3 . Preliminary results suggested that performing 1 cycle of mixing and melting was not sufficient to saturate the glass. The bubbling method successfully incorporated sulfur into the glass but caused significant losses of sodium from the melt. In order to saturate the glass melt with sulfate without causing noticeable sodium loss, a modified crucible salt saturation method was developed by repeating the mixing and melting of the glass and salt mixture. For all 3 representative LAW glasses tested in this study, it was found that after 3 mixing and melting cycles, the sulfur concentration reaches a plateau, indicating reasonable sulfur saturation.

Authors:
ORCiD logo [1];  [1];  [1];  [1];  [1];  [1];  [1];  [1];  [2]
  1. Pacific Northwest National Laboratory Richland Washington
  2. U.S. Department of Energy, Office of River Protection Richland Washington
Publication Date:
Sponsoring Org.:
USDOE
OSTI Identifier:
1457593
Resource Type:
Publisher's Accepted Manuscript
Journal Name:
International Journal of Applied Glass Science
Additional Journal Information:
Journal Name: International Journal of Applied Glass Science Journal Volume: 10 Journal Issue: 1; Journal ID: ISSN 2041-1286
Publisher:
Wiley-Blackwell
Country of Publication:
United States
Language:
English

Citation Formats

Jin, Tongan, Kim, Dongsang, Darnell, Lori P., Weese, Brigitte L., Canfield, Nathan L., Bliss, Mary, Schweiger, Michael J., Vienna, John D., and Kruger, Albert A. A crucible salt saturation method for determining sulfur solubility in glass melt. United States: N. p., 2018. Web. doi:10.1111/ijag.12366.
Jin, Tongan, Kim, Dongsang, Darnell, Lori P., Weese, Brigitte L., Canfield, Nathan L., Bliss, Mary, Schweiger, Michael J., Vienna, John D., & Kruger, Albert A. A crucible salt saturation method for determining sulfur solubility in glass melt. United States. https://doi.org/10.1111/ijag.12366
Jin, Tongan, Kim, Dongsang, Darnell, Lori P., Weese, Brigitte L., Canfield, Nathan L., Bliss, Mary, Schweiger, Michael J., Vienna, John D., and Kruger, Albert A. Thu . "A crucible salt saturation method for determining sulfur solubility in glass melt". United States. https://doi.org/10.1111/ijag.12366.
@article{osti_1457593,
title = {A crucible salt saturation method for determining sulfur solubility in glass melt},
author = {Jin, Tongan and Kim, Dongsang and Darnell, Lori P. and Weese, Brigitte L. and Canfield, Nathan L. and Bliss, Mary and Schweiger, Michael J. and Vienna, John D. and Kruger, Albert A.},
abstractNote = {Abstract Experiments were conducted to determine sulfur solubility in Hanford low‐activity waste ( LAW ) glass melts by a sulfur saturation method. Sulfur‐incorporated glass melts were prepared by salt saturation and bubbling methods. The salt saturation method was performed by mixing crushed premelted baseline glasses with an excess amount of Na 2 SO 4 prior to melting the mixture at 1150°C for 1 hour. The bubbling method involved bubbling the glass melt at 1150°C in a Pt crucible with an SO 2 /O 2 /N 2 gas mix to equilibrate the melt at a known pressure of SO 3 . Preliminary results suggested that performing 1 cycle of mixing and melting was not sufficient to saturate the glass. The bubbling method successfully incorporated sulfur into the glass but caused significant losses of sodium from the melt. In order to saturate the glass melt with sulfate without causing noticeable sodium loss, a modified crucible salt saturation method was developed by repeating the mixing and melting of the glass and salt mixture. For all 3 representative LAW glasses tested in this study, it was found that after 3 mixing and melting cycles, the sulfur concentration reaches a plateau, indicating reasonable sulfur saturation.},
doi = {10.1111/ijag.12366},
journal = {International Journal of Applied Glass Science},
number = 1,
volume = 10,
place = {United States},
year = {Thu Jun 28 00:00:00 EDT 2018},
month = {Thu Jun 28 00:00:00 EDT 2018}
}

Journal Article:
Free Publicly Available Full Text
Publisher's Version of Record
https://doi.org/10.1111/ijag.12366

Citation Metrics:
Cited by: 11 works
Citation information provided by
Web of Science

Save / Share:

Works referenced in this record:

Diffusion of the 35S isotope in soda–lime–silica and sodium trisilicate glass melts
journal, July 2011


Modelling the sulfate capacity of simulated radioactive waste borosilicate glasses
journal, February 2017


Redox-dependent solubility of technetium in low activity waste glass
journal, June 2014

  • Soderquist, Chuck Z.; Schweiger, Michael J.; Kim, Dong-Sang
  • Journal of Nuclear Materials, Vol. 449, Issue 1-3
  • DOI: 10.1016/j.jnucmat.2014.03.008

Chromium phase behavior in a multi-component borosilicate glass melt
journal, July 2006


Volatile species of technetium and rhenium during waste vitrification
journal, February 2018


The effects of melting reactions on laboratory-scale waste vitrification
journal, August 1995

  • Smith, Peter A.; Vienna, John D.; Hrma, Pavel
  • Journal of Materials Research, Vol. 10, Issue 8
  • DOI: 10.1557/JMR.1995.2137

Salt Mineralogy of Hanford High-Level Nuclear Waste Staged for Treatment
journal, July 2013

  • Reynolds, Jacob G.; Cooke, Gary A.; Herting, Daniel L.
  • Industrial & Engineering Chemistry Research, Vol. 52, Issue 29
  • DOI: 10.1021/ie400822r

Vanadium and chromium redox behavior in borosilicate nuclear waste glasses
journal, July 2011


Toward Understanding the Effect of Low-Activity Waste Glass Composition on Sulfur Solubility
journal, July 2014

  • Vienna, John D.; Kim, Dong-Sang; Muller, Isabelle S.
  • Journal of the American Ceramic Society, Vol. 97, Issue 10
  • DOI: 10.1111/jace.13125

Retention of Sulfate in Savannah River Site High-Level Radioactive Waste Glass: Retention of Sulfate in SRS HLW Glass
journal, November 2010


Role of Sulfate in Structural Modifications of Sodium Barium Borosilicate Glasses Developed for Nuclear Waste Immobilization
journal, December 2008


Sulfate Decomposition and Sodium Oxide Activity in Soda-Lime-Silica Glass Melts
journal, November 2003


Determination of sulfur environments in borosilicate waste glasses using X-ray absorption near-edge spectroscopy
journal, January 2004


Dissolution Mechanisms of Tetravalent Sulphur in Silicate Melts: Evidences from Sulphur K Edge XANES Studies on Glasses
journal, March 2008


Quantitation of sulfate solubility in borosilicate glasses using Raman spectroscopy
journal, August 2009


Reactions during melting of low-activity waste glasses and their effects on the retention of rhenium as a surrogate for technetium-99
journal, October 2015


Miscibility Gap in the System Sodium Oxid Silica-Sodium Sulfate at 1200oC
journal, January 1965


Barium borosilicate glass – a potential matrix for immobilization of sulfate bearing high-level radioactive liquid waste
journal, November 2006


Raman studies of sulfur in borosilicate waste glasses: sulfate environments
journal, August 2001


Sulfur behavior in silicate glasses and melts: Implications for sulfate incorporation in nuclear waste glasses as a function of alkali cation and V2O5 content
journal, January 2007


Solubility of Cr 2 O 3 and Speciation of Chromium in Soda-Lime-Silicate Melts
journal, February 2010


Oxygen Ion Activity and the Solubility of Sulfur Trioxide in Sodium Silicate Melts
journal, September 1966