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Title: Liquidus temperature in the spinel primary phase field: A comparison between optical and crystal fraction methods

Liquidus temperature (TL) was measured for 38 simulated high-level waste borosilicate glasses covering a Hanford composition region, using optical microscopy and crystal-fraction extrapolation methods to analyze isothermally heat-treated specimens. Furthermore, the glasses encompassed a one-component-at-a-time variation of 16 components from a representative Hanford HLW simulant baseline composition. The TL values ranged from 1006 °C to 1603 °C. First-order models were fit to data to obtain component effects on TL (per 1 mass% additions) and then the components were grouped into three categories: TL-increasing components [i.e., Cr 2O 3 (264 °C), “Others” (minor components, 163 °C), oxides of noble metals (137 °C), NiO (91 °C), as well as Al 2O 3 and Fe 2O 3 (~ 19–21 °C)]; TL-decreasing components [i.e., K 2O (-26 °C), Na 2O (-41 °C), and Li 2O (-68 °C)]; and those of little effect [i.e., MnO, P 2O 5, ZrO 2, F, Bi 2O 3, SiO 2, B 2O 3, and CaO (9 to -12 °C)]. We also present the temperatures at which 1 vol% of spinel is at equilibrium with the melt (T1%) as these values are considered relevant to the Hanford Tank Waste Treatment and Immobilization Plant. The measured and estimated values are comparedmore » and contrasted and the effect of TL and T1% on glass formulation is discussed. The different methods for measuring TL are compared and contrasted.« less
Authors:
ORCiD logo [1] ;  [1] ;  [1] ;  [1] ;  [1] ;  [1] ;  [1]
  1. Pacific Northwest National Lab. (PNNL), Richland, WA (United States)
Publication Date:
Report Number(s):
PNNL-SA-128799
Journal ID: ISSN 0022-3093; PII: S0022309317306373; TRN: US1800978
Grant/Contract Number:
AC05-76RL01830
Type:
Accepted Manuscript
Journal Name:
Journal of Non-Crystalline Solids
Additional Journal Information:
Journal Volume: 483; Journal ID: ISSN 0022-3093
Publisher:
Elsevier
Research Org:
Pacific Northwest National Lab. (PNNL), Richland, WA (United States)
Sponsoring Org:
USDOE Office of Environmental Management (EM)
Country of Publication:
United States
Language:
English
Subject:
37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY; liquidus temperature; crystal fraction; spinel; high-level waste
OSTI Identifier:
1416963

Riley, Brian J., Hrma, Pavel, Crum, Jarrod V., Vienna, John D., Schweiger, Michael J., Rodriguez, Carmen P., and Peterson, Jacob A.. Liquidus temperature in the spinel primary phase field: A comparison between optical and crystal fraction methods. United States: N. p., Web. doi:10.1016/J.JNONCRYSOL.2017.11.033.
Riley, Brian J., Hrma, Pavel, Crum, Jarrod V., Vienna, John D., Schweiger, Michael J., Rodriguez, Carmen P., & Peterson, Jacob A.. Liquidus temperature in the spinel primary phase field: A comparison between optical and crystal fraction methods. United States. doi:10.1016/J.JNONCRYSOL.2017.11.033.
Riley, Brian J., Hrma, Pavel, Crum, Jarrod V., Vienna, John D., Schweiger, Michael J., Rodriguez, Carmen P., and Peterson, Jacob A.. 2018. "Liquidus temperature in the spinel primary phase field: A comparison between optical and crystal fraction methods". United States. doi:10.1016/J.JNONCRYSOL.2017.11.033.
@article{osti_1416963,
title = {Liquidus temperature in the spinel primary phase field: A comparison between optical and crystal fraction methods},
author = {Riley, Brian J. and Hrma, Pavel and Crum, Jarrod V. and Vienna, John D. and Schweiger, Michael J. and Rodriguez, Carmen P. and Peterson, Jacob A.},
abstractNote = {Liquidus temperature (TL) was measured for 38 simulated high-level waste borosilicate glasses covering a Hanford composition region, using optical microscopy and crystal-fraction extrapolation methods to analyze isothermally heat-treated specimens. Furthermore, the glasses encompassed a one-component-at-a-time variation of 16 components from a representative Hanford HLW simulant baseline composition. The TL values ranged from 1006 °C to 1603 °C. First-order models were fit to data to obtain component effects on TL (per 1 mass% additions) and then the components were grouped into three categories: TL-increasing components [i.e., Cr2O3 (264 °C), “Others” (minor components, 163 °C), oxides of noble metals (137 °C), NiO (91 °C), as well as Al2O3 and Fe2O3 (~ 19–21 °C)]; TL-decreasing components [i.e., K2O (-26 °C), Na2O (-41 °C), and Li2O (-68 °C)]; and those of little effect [i.e., MnO, P2O5, ZrO2, F, Bi2O3, SiO2, B2O3, and CaO (9 to -12 °C)]. We also present the temperatures at which 1 vol% of spinel is at equilibrium with the melt (T1%) as these values are considered relevant to the Hanford Tank Waste Treatment and Immobilization Plant. The measured and estimated values are compared and contrasted and the effect of TL and T1% on glass formulation is discussed. The different methods for measuring TL are compared and contrasted.},
doi = {10.1016/J.JNONCRYSOL.2017.11.033},
journal = {Journal of Non-Crystalline Solids},
number = ,
volume = 483,
place = {United States},
year = {2018},
month = {1}
}