Engineering Glass Passivation Layers -Model Results

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The immobilization of radioactive waste into glass waste forms is a baseline process of nuclear waste management not only in the United States, but worldwide. The rate of radionuclide release from these glasses is a critical measure of the quality of the waste form. Over long-term tests and using extrapolations of ancient analogues, it has been shown that well designed glasses exhibit a dissolution rate that quickly decreases to a slow residual rate for the lifetime of the glass. The mechanistic cause of this decreased corrosion rate is a subject of debate, with one of the major theories suggesting that ... continued below

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Skorski, Daniel C.; Ryan, Joseph V.; Strachan, Denis M. & Lepry, William C. August 8, 2011.

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The immobilization of radioactive waste into glass waste forms is a baseline process of nuclear waste management not only in the United States, but worldwide. The rate of radionuclide release from these glasses is a critical measure of the quality of the waste form. Over long-term tests and using extrapolations of ancient analogues, it has been shown that well designed glasses exhibit a dissolution rate that quickly decreases to a slow residual rate for the lifetime of the glass. The mechanistic cause of this decreased corrosion rate is a subject of debate, with one of the major theories suggesting that the decrease is caused by the formation of corrosion products in such a manner as to present a diffusion barrier on the surface of the glass. Although there is much evidence of this type of mechanism, there has been no attempt to engineer the effect to maximize the passivating qualities of the corrosion products. This study represents the first attempt to engineer the creation of passivating phases on the surface of glasses. Our approach utilizes interactions between the dissolving glass and elements from the disposal environment to create impermeable capping layers. By drawing from other corrosion studies in areas where passivation layers have been successfully engineered to protect the bulk material, we present here a report on mineral phases that are likely have a morphological tendency to encrust the surface of the glass. Our modeling has focused on using the AFCI glass system in a carbonate, sulfate, and phosphate rich environment. We evaluate the minerals predicted to form to determine the likelihood of the formation of a protective layer on the surface of the glass. We have also modeled individual ions in solutions vs. pH and the addition of aluminum and silicon. These results allow us to understand the pH and ion concentration dependence of mineral formation. We have determined that iron minerals are likely to form a complete incrustation layer and we plan to look more closely at Vivianite [Fe3(PO4)2-8(H2O)] and Siderite [FeCO3] in the next stage of the project.

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  • Report No.: PNNL-20615
  • Grant Number: AC05-76RL01830
  • DOI: 10.2172/1031991 | External Link
  • Office of Scientific & Technical Information Report Number: 1031991
  • Archival Resource Key: ark:/67531/metadc843772

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  • August 8, 2011

Added to The UNT Digital Library

  • May 19, 2016, 3:16 p.m.

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  • Nov. 23, 2016, 6:46 p.m.

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Skorski, Daniel C.; Ryan, Joseph V.; Strachan, Denis M. & Lepry, William C. Engineering Glass Passivation Layers -Model Results, report, August 8, 2011; Richland, Washington. (digital.library.unt.edu/ark:/67531/metadc843772/: accessed September 22, 2018), University of North Texas Libraries, Digital Library, digital.library.unt.edu; crediting UNT Libraries Government Documents Department.