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Structure and properties of fluorine-bearing aluminosilicate melts: the system Na2O-Al2O3-SiO2-F at 1 atm

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Abstract

The chemical interaction between fluorine and highly polymerized sodium aluminosilicate melts [Al/(Al+Si)= 0.125–0.250 on the join NaAlO2-SiO2] has been studied with Raman spectroscopy. Fluorine is dissolved to form F− ions that are electrically neutralized with Na+ or Al3+. There is no evidence for association of fluorine with either Si4+ or Al3+ in four-fold coordination and no evidence of fluorine in six-fold coordination with Si4+ in these melt compositions. Upon solution of fluorine nonbridging oxygens are formed and are a part of structural units with nonbridging oxygen per tetrahedral cations (NBO/T) about 2 and 1. The proportions of these two depolymerized units in the melts increase systematically with increasing F/(F+O) at constant Al/(Al+Si) and with decreasing Al/(Al+Si) at constant F/(F+O). Depolymerization (increasing NBO/T) of silicate melts results from a fraction of aluminum and alkalies (in the present study; Na+) reacting to form fluoride complexes. In this process an equivalent amount of Na+ (orginally required for Al-3+charge-balance) or Al3+ (originally required Na+ to exist in tetrahedral coordination) become network-modifiers.

The structural data have been used to develop a method for calculating the viscosity of fluorine-bearing sodium aluminosilicate melts at 1 atm. Where experimental viscosity data are available, the calculated and measured values are within 5% of each other.

A method is also suggested by which the liquidus phase equilibria of fluorine-bearing aluminosilicate melts may be predicted. In accord with published experimental data it is suggested, for example, that — on the basis of the determined solubility mechanism of fluorine in aluminosilicate melts — with increasing fluorine content of feldspar-quartz systems, the liquidus boundaries between aluminosilicate minerals (e.g., feldspars) and quartz shift away from silica.

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  1. Geophysical Laboratory, Carnegie Institution of Washington, 20008, Washington, DC, USA

    Bjørn O. Mysen & David Virgo

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  1. Bjørn O. Mysen
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  2. David Virgo
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Mysen, B.O., Virgo, D. Structure and properties of fluorine-bearing aluminosilicate melts: the system Na2O-Al2O3-SiO2-F at 1 atm. Contr. Mineral. and Petrol. 91, 205–220 (1985). https://doi.org/10.1007/BF00413348

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