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Title: Conversion of Nuclear Waste to Molten Glass: Cold-Cap Reactions in Crucible Tests

Abstract

The feed-to-glass conversion, which comprises complex chemical reactions and phase transitions, occurs in the cold cap during nuclear waste vitrification. Here, to investigate the conversion process, we analyzed heat-treated samples of a simulated high-level waste feed using X-ray diffraction, electron probe microanalysis, leaching tests, and residual anion analysis. Feed dehydration, gas evolution, and borate phase formation occurred at temperatures below 700°C before the emerging glass-forming melt was completely connected. Above 700°C, intermediate aluminosilicate phases and quartz particles gradually dissolved in the continuous borosilicate melt, which expanded with transient foam. Finally, knowledge of the chemistry and physics of feed-to-glass conversion will help us control the conversion path by changing the melter feed makeup to maximize the glass production rate.

Authors:
ORCiD logo [1];  [1];  [1];  [1];  [1];  [1];  [2]
  1. Pacific Northwest National Lab. (PNNL), Richland, WA (United States)
  2. U.S. Department of Energy, Office of River Protection, Richland, WA (United States)
Publication Date:
Research Org.:
Pacific Northwest National Lab. (PNNL), Richland, WA (United States)
Sponsoring Org.:
USDOE
OSTI Identifier:
1341439
Report Number(s):
PNNL-SA-115889
Journal ID: ISSN 0002-7820
Grant/Contract Number:  
AC05-76RL01830
Resource Type:
Accepted Manuscript
Journal Name:
Journal of the American Ceramic Society
Additional Journal Information:
Journal Volume: 99; Journal Issue: 9; Journal ID: ISSN 0002-7820
Publisher:
American Ceramic Society
Country of Publication:
United States
Language:
English
Subject:
12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE WASTES FROM NUCLEAR FACILITIES; nuclear waste; glass; reaction path

Citation Formats

Xu, Kai, Hrma, Pavel, Rice, Jarrett A., Schweiger, Michael J., Riley, Brian J., Overman, Nicole R., and Kruger, Albert A. Conversion of Nuclear Waste to Molten Glass: Cold-Cap Reactions in Crucible Tests. United States: N. p., 2016. Web. doi:10.1111/jace.14310.
Xu, Kai, Hrma, Pavel, Rice, Jarrett A., Schweiger, Michael J., Riley, Brian J., Overman, Nicole R., & Kruger, Albert A. Conversion of Nuclear Waste to Molten Glass: Cold-Cap Reactions in Crucible Tests. United States. doi:10.1111/jace.14310.
Xu, Kai, Hrma, Pavel, Rice, Jarrett A., Schweiger, Michael J., Riley, Brian J., Overman, Nicole R., and Kruger, Albert A. Mon . "Conversion of Nuclear Waste to Molten Glass: Cold-Cap Reactions in Crucible Tests". United States. doi:10.1111/jace.14310. https://www.osti.gov/servlets/purl/1341439.
@article{osti_1341439,
title = {Conversion of Nuclear Waste to Molten Glass: Cold-Cap Reactions in Crucible Tests},
author = {Xu, Kai and Hrma, Pavel and Rice, Jarrett A. and Schweiger, Michael J. and Riley, Brian J. and Overman, Nicole R. and Kruger, Albert A.},
abstractNote = {The feed-to-glass conversion, which comprises complex chemical reactions and phase transitions, occurs in the cold cap during nuclear waste vitrification. Here, to investigate the conversion process, we analyzed heat-treated samples of a simulated high-level waste feed using X-ray diffraction, electron probe microanalysis, leaching tests, and residual anion analysis. Feed dehydration, gas evolution, and borate phase formation occurred at temperatures below 700°C before the emerging glass-forming melt was completely connected. Above 700°C, intermediate aluminosilicate phases and quartz particles gradually dissolved in the continuous borosilicate melt, which expanded with transient foam. Finally, knowledge of the chemistry and physics of feed-to-glass conversion will help us control the conversion path by changing the melter feed makeup to maximize the glass production rate.},
doi = {10.1111/jace.14310},
journal = {Journal of the American Ceramic Society},
number = 9,
volume = 99,
place = {United States},
year = {2016},
month = {5}
}

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Works referenced in this record:

Environmental cleanup: The challenge at the Hanford Site, Washington, USA
journal, July 1993

  • Gray, Robert H.; Becker, C. Dale
  • Environmental Management, Vol. 17, Issue 4
  • DOI: 10.1007/BF02394662

Managing the Environmental Legacy of U.S. Nuclear-Weapons Production
journal, January 2002

  • Crowley, Kevin; Ahearne, John
  • American Scientist, Vol. 90, Issue 6
  • DOI: 10.1511/2002.6.514

Turning nuclear waste into glass
journal, February 2015


Nuclear waste vitrification efficiency: Cold cap reactions
journal, December 2012


Mathematical modeling of cold cap
journal, October 2012


Temperature Distribution within a Cold Cap during Nuclear Waste Vitrification
journal, June 2015

  • Dixon, Derek R.; Schweiger, Michael J.; Riley, Brian J.
  • Environmental Science & Technology, Vol. 49, Issue 14
  • DOI: 10.1021/acs.est.5b00931

Cold-cap reactions in vitrification of nuclear waste glass: Experiments and modeling
journal, May 2013


Application of evolved gas analysis to cold-cap reactions of melter feeds for nuclear waste vitrification
journal, September 2014


Melter Feed Reactions at   700°C for Nuclear Waste Vitrification
journal, July 2015

  • Xu, Kai; Hrma, Pavel; Rice, Jarrett
  • Journal of the American Ceramic Society, Vol. 98, Issue 10
  • DOI: 10.1111/jace.13766

Effect of Alumina Source on the Rate of Melting Demonstrated with Nuclear Waste Glass Batch
journal, February 2012


Cluster formation of silica particles in glass batches during melting
journal, June 2010


Conversion of batch to molten glass, II: Dissolution of quartz particles
journal, February 2011


Kinetic model for quartz and spinel dissolution during melting of high-level-waste glass batch
journal, November 2013


Determination of Temperature-Dependent Heat Conductivity and Thermal Diffusivity of Waste Glass Melter Feed
journal, May 2013

  • Pokorny, Richard; Rice, Jarrett A.; Schweiger, Michael J.
  • Journal of the American Ceramic Society, Vol. 96, Issue 6
  • DOI: 10.1111/jace.12313

Determination of Heat Conductivity and Thermal Diffusivity of Waste Glass Melter Feed: Extension to High Temperatures
journal, May 2014

  • Rice, Jarrett A.; Pokorny, Richard; Schweiger, Michael J.
  • Journal of the American Ceramic Society, Vol. 97, Issue 6
  • DOI: 10.1111/jace.12971

Rhenium volatilization in waste glasses
journal, September 2015


Effect of Bubbles and Silica Dissolution on Melter Feed Rheology during Conversion to Glass
journal, October 2014

  • Marcial, José; Chun, Jaehun; Hrma, Pavel
  • Environmental Science & Technology, Vol. 48, Issue 20
  • DOI: 10.1021/es5018625

Melting of glass batch: Model for multiple overlapping gas-evolving reactions
journal, August 2012


A Method for Determining Bulk Density, Material Density, and Porosity of Melter Feed During Nuclear Waste Vitrification
journal, September 2015

  • Hilliard, Zachary; Hrma, Pavel
  • Journal of the American Ceramic Society, Vol. 99, Issue 1
  • DOI: 10.1111/jace.13919

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