4.7 Article

Dissolution mechanisms of water in depolymerized silicate (peridotitic) glasses based on infrared spectroscopy

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GEOCHIMICA ET COSMOCHIMICA ACTA
卷 342, 期 -, 页码 45-61

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PERGAMON-ELSEVIER SCIENCE LTD
DOI: 10.1016/j.gca.2022.11.029

关键词

Peridotitic glasses; Polymerization; Free hydroxyl; Water speciation; Water dissolution mechanisms

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The dissolution of water in melts and its impact on glass structure were studied using Fourier transform infrared spectroscopy. It was found that the proportion of water molecules in the glass decreases with increasing depolymerization. Additionally, a new peak related to a specific hydroxyl group was identified, and the position of another peak was found to shift with depolymerization. These findings provide insights into the dissolution mechanisms of water in highly depolymerized glasses and their effect on glass structure.
The dissolution of water changes the chemical and physical properties of melts. The effect of water dissolution depends on the bulk H2O content and dissolution mechanisms. Previous research mainly focused on relatively polymerized glasses, whereas dissolution mechanisms of water in highly depolymerized glasses have not been well studied. We investigated three sets of hydrous (up to 5 wt% H2O), highly depolymerized glasses using Fourier transform infrared spectroscopy. The three suites of glasses can be classified as tephritic (non-bridging oxygens to tetrahedral cations, NBO/T approximate to 0.9), basanitic (NBO/T approximate to 1.5), and peridotitic (NBO/T approximate to 2.5). The comparison of infrared spectra indicated four prominent features. First, the combination band related to molecular H2O at similar to 5200 cm(-1) decreases in relative intensity with increasing depolymerization. At 2 wt% bulk H2O, the proportion of H2O molecules decreases from the tephritic through basanitic to peridotitic glasses, where the proportion of H2O molecules is below 10 %. At 5 wt% bulk H2O, the proportion of H2O molecules in the peridotitic glass is around 20 %, whereas it is around 50 % in the basaltic glass with the same H2O content. Second, a second peak appears at 4270-4180 cm(-1), next to the (Si,Al)OH combination peak (network hydroxyl), with increasing CaO and MgO contents in basanitic (similar to 25 wt% CaO) and peridotitic (similar to 40 wt% MgO) glasses, respectively. We assign this peak to the (Mg,Ca)OH group (free hydroxyl); this is the first identification of this group based on infrared spectroscopy. This assignment is also supported by IR data on Mg(OH)(2) and Ca(OH)(2) crystalline phases from the literature. Third, the ratio of (Si,Al)OH and (Mg,Ca)OH peak absorbances remains nearly constant with increasing water content in basanitic and peridotitic glasses, suggesting no effect of water on polymerization of extremely depolymerized melts. Fourth, the (Si,Al)OH peak shifts to lower wavenumbers with increasing depolymerization. As a result, the (Si,Al)OH peak position could potentially be used to evaluate the degree of melt polymerization in general, and the effect of water on melt polymerization in particular.(c) 2022 Elsevier Ltd. All rights reserved.

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