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Reiser, Joelle T.
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article
Comparative structural investigations of nuclear waste glass alteration layers and sol-gel synthesized aerogels
Abstract
hile various glass alteration layer formation mechanisms have been debated in recent years, the glass alteration community generally agrees that more information on physical properties of the alteration layers is needed to further the understanding of their impacts on overall glass alteration. In this work, pore volumes and solid structures of glass (International Simple Glass, ISG) alteration layers formed in solutions of various pH conditions in initially dilute conditions at 90 °C are evaluated with positron annihilation spectroscopy, small-angle X-ray scattering, and scanning transmission electron microscopy. Pore volumes of alteration layers formed at pH 9 were found to be at their lowest near the surfaces of the alteration layers. Solid structures of alteration layers are compared with those of synthetic aerogels of comparable compositions produced under various pH conditions. Alteration layers formed at pH 11 on ISG were shown to contain large structures (>10 nm) similar to synthetic aerogels created under neutral and basic conditions whereas alteration layers formed at pH 9 did not. Available dissolved silica species defined by silica solubility were proposed to have the greatest impact on alteration layer structure.