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

Abstract

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:
Research Org.:
Pacific Northwest National Lab. (PNNL), Richland, WA (United States)
Sponsoring Org.:
USDOE Office of Environmental Management (EM)
OSTI Identifier:
1416963
Report Number(s):
PNNL-SA-128799
Journal ID: ISSN 0022-3093; PII: S0022309317306373; TRN: US1800978
Grant/Contract Number:  
AC05-76RL01830
Resource Type:
Journal Article: Accepted Manuscript
Journal Name:
Journal of Non-Crystalline Solids
Additional Journal Information:
Journal Volume: 483; Journal ID: ISSN 0022-3093
Publisher:
Elsevier
Country of Publication:
United States
Language:
English
Subject:
37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY; liquidus temperature; crystal fraction; spinel; high-level waste

Citation Formats

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., 2018. 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. Thu . "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. https://www.osti.gov/servlets/purl/1416963.
@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},
issn = {0022-3093},
number = ,
volume = 483,
place = {United States},
year = {2018},
month = {1}
}

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Figures / Tables:

Table 1 Table 1: Target compositions of all glasses in mass% [24]. The “Others” column includes BaO, CdO, MgO, PbO, PdO, Rh2O3, RuO2, SO3, SrO, TiO2, ZnO, Ce2O3, La2O3, and Nd2O3 (see Table 2 for a breakdown of "Others" components with compositional ranges). *EM07-BL-2, not listed in the table, had the samemore » targeted composition as EM07-BL-1.« less

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