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Title: Compositional Dependence of Solubility/Retention of Molybdenum Oxides in Aluminoborosilicate-Based Model Nuclear Waste Glasses

Abstract

We present that molybdenum oxides are an integral component of the high-level waste streams being generated from the nuclear reactors in several countries. Although borosilicate glass has been chosen as the baseline waste form by most of the countries to immobilize these waste streams, molybdate oxyanions (MoO 4 2-) exhibit very low solubility (~1 mol %) in these glass matrices. In the past three to four decades, several studies describing the compositional and structural dependence of molybdate anions in borosilicate and aluminoborosilicate glasses have been reported in the literature, providing a basis for our understanding of fundamental science that governs the solubility and retention of these species in the nuclear waste glasses. However, there are still several open questions that need to be answered to gain an in-depth understanding of the mechanisms that control the solubility and retention of these oxyanions in glassy waste forms. This article is focused on finding answers to two such questions: (1) What are the solubility and retention limits of MoO 3 in aluminoborosilicate glasses as a function of chemical composition? (2) Why is there a considerable increase in the solubility of MoO 3 with incorporation of rare-earth oxides (for example, Nd 2O 3) inmore » aluminoborosilicate glasses? Accordingly, three different series of aluminoborosilicate glasses (compositional complexity being added in a tiered approach) with varying MoO 3 concentrations have been synthesized and characterized for their ability to accommodate molybdate ions in their structure (solubility) and as a glass-ceramic (retention). The contradictory viewpoints (between different research groups) pertaining to the impact of rare-earth cations on the structure of aluminoborosilicate glasses are discussed, and their implications on the solubility of MoO 3 in these glasses are evaluated. Lastly, a novel hypothesis explaining the mechanism governing the solubility of MoO 3 in rare-earth containing aluminoborosilicate glasses has been proposed.« less

Authors:
 [1];  [2];  [1];  [3];  [3];  [4];  [5]; ORCiD logo [6]; ORCiD logo [1]
  1. Rutgers Univ., Piscataway, NJ (United States)
  2. Washington State Univ., Pullman, WA (United States)
  3. Corning Research & Development Corporation, Corning, NY (United States)
  4. Pennsylvania State Univ., University Park, PA (United States)
  5. Univ. of Sheffield (United Kingdom)
  6. Washington State Univ., Pullman, WA (United States) ; Univ. of Sheffield (United Kingdom)
Publication Date:
Research Org.:
Washington State Univ., Pullman, WA (United States)
Sponsoring Org.:
USDOE Office of Nuclear Energy (NE)
OSTI Identifier:
1485490
Grant/Contract Number:  
NE0008431; NE0008597
Resource Type:
Accepted Manuscript
Journal Name:
Journal of Physical Chemistry. B, Condensed Matter, Materials, Surfaces, Interfaces and Biophysical Chemistry
Additional Journal Information:
Journal Volume: 122; Journal Issue: 5; Journal ID: ISSN 1520-6106
Publisher:
American Chemical Society
Country of Publication:
United States
Language:
English
Subject:
36 MATERIALS SCIENCE; 11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS

Citation Formats

Brehault, Antoine, Patil, Deepak, Kamat, Hrishikesh, Youngman, Randall E., Thirion, Lynn M., Mauro, John C., Corkhill, Claire L., McCloy, John S., and Goel, Ashutosh. Compositional Dependence of Solubility/Retention of Molybdenum Oxides in Aluminoborosilicate-Based Model Nuclear Waste Glasses. United States: N. p., 2018. Web. doi:10.1021/acs.jpcb.7b09158.
Brehault, Antoine, Patil, Deepak, Kamat, Hrishikesh, Youngman, Randall E., Thirion, Lynn M., Mauro, John C., Corkhill, Claire L., McCloy, John S., & Goel, Ashutosh. Compositional Dependence of Solubility/Retention of Molybdenum Oxides in Aluminoborosilicate-Based Model Nuclear Waste Glasses. United States. doi:10.1021/acs.jpcb.7b09158.
Brehault, Antoine, Patil, Deepak, Kamat, Hrishikesh, Youngman, Randall E., Thirion, Lynn M., Mauro, John C., Corkhill, Claire L., McCloy, John S., and Goel, Ashutosh. Sun . "Compositional Dependence of Solubility/Retention of Molybdenum Oxides in Aluminoborosilicate-Based Model Nuclear Waste Glasses". United States. doi:10.1021/acs.jpcb.7b09158. https://www.osti.gov/servlets/purl/1485490.
@article{osti_1485490,
title = {Compositional Dependence of Solubility/Retention of Molybdenum Oxides in Aluminoborosilicate-Based Model Nuclear Waste Glasses},
author = {Brehault, Antoine and Patil, Deepak and Kamat, Hrishikesh and Youngman, Randall E. and Thirion, Lynn M. and Mauro, John C. and Corkhill, Claire L. and McCloy, John S. and Goel, Ashutosh},
abstractNote = {We present that molybdenum oxides are an integral component of the high-level waste streams being generated from the nuclear reactors in several countries. Although borosilicate glass has been chosen as the baseline waste form by most of the countries to immobilize these waste streams, molybdate oxyanions (MoO42-) exhibit very low solubility (~1 mol %) in these glass matrices. In the past three to four decades, several studies describing the compositional and structural dependence of molybdate anions in borosilicate and aluminoborosilicate glasses have been reported in the literature, providing a basis for our understanding of fundamental science that governs the solubility and retention of these species in the nuclear waste glasses. However, there are still several open questions that need to be answered to gain an in-depth understanding of the mechanisms that control the solubility and retention of these oxyanions in glassy waste forms. This article is focused on finding answers to two such questions: (1) What are the solubility and retention limits of MoO3 in aluminoborosilicate glasses as a function of chemical composition? (2) Why is there a considerable increase in the solubility of MoO3 with incorporation of rare-earth oxides (for example, Nd2O3) in aluminoborosilicate glasses? Accordingly, three different series of aluminoborosilicate glasses (compositional complexity being added in a tiered approach) with varying MoO3 concentrations have been synthesized and characterized for their ability to accommodate molybdate ions in their structure (solubility) and as a glass-ceramic (retention). The contradictory viewpoints (between different research groups) pertaining to the impact of rare-earth cations on the structure of aluminoborosilicate glasses are discussed, and their implications on the solubility of MoO3 in these glasses are evaluated. Lastly, a novel hypothesis explaining the mechanism governing the solubility of MoO3 in rare-earth containing aluminoborosilicate glasses has been proposed.},
doi = {10.1021/acs.jpcb.7b09158},
journal = {Journal of Physical Chemistry. B, Condensed Matter, Materials, Surfaces, Interfaces and Biophysical Chemistry},
number = 5,
volume = 122,
place = {United States},
year = {2018},
month = {1}
}

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