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Titel Oxidation-state dependence of rheology in peralkaline glasses of phonolitic composition
VerfasserIn M. C. Scherrer, K.-U. Hess, K. T. Fehr, D. B. Dingwell
Konferenz EGU General Assembly 2012
Medientyp Artikel
Sprache Englisch
Digitales Dokument PDF
Erschienen In: GRA - Volume 14 (2012)
Datensatznummer 250063700
 
Zusammenfassung
The precise description of magmatic melts rheology at the glass transition is crucial in understanding dynamic processes in volcanology. The glass transition has been described to scale with the viscosity of the material according to Maxwell’s relaxation theory for viscoelastic liquids (Dingwell and Webb, 1989). The temperature dependence of the viscosity of multi-component systems can adequately be calculated using empirical models such as Hess et al. (1996), Giordano et al. (2008) and Hui and Zhang (2008); yet, within these calculations, the influence of oxidation state has been so far considered minor and was consequently neglected. The rheological behavior of some iron-rich silicate melts has shown noteworthy oxidation state-dependent variations (Cukierman and Uhlmann 1974, Dingwell and Virgo 1987). The focus of our study is to improve the viscosity models by investigating the necessity of an additional redox-parameter. Thirteen re-melted glass samples of natural phonolitic composition (peralkaline lavas with 8.5 wt. % FeOtot) were produced under different oxygen fugacity (fO2) conditions in a CO/CO2 gas-mixing furnace. Their oxidation-state (Fe3+/Fetot) ranges from 0.44 to 0.93 (±0.05). The viscosity above the liquidus was recorded via the concentric cylinder technique at a constant temperature of 1186 ˚ C. Additionally, viscosities were measured in the interval of 107to 1011Pa swith temperatures up to 900 ˚ C at ambient pressure via a BAEHR micro-penetration viscometer. Glass transition temperatures (Tg) have been determined with a constant heating/cooling rate of 10K/min on a SETARAM Sensys evo DSC using the peak of the specific heat capacity curve. Under a constant temperature in the super-liquidus state, the viscosity increases strongly with increasing fO2. In the sub-liquidus state, the measured calorimetric Tgis shifted to lower temperatures as the ratio of ferrous/total iron decreases from 638 ˚ C to 610 ˚ C. However, there is no equivalent measurable effect of the oxidation-state on super-cooled melt viscosity at Tg, within the precision of the micro-penetration experiment (all values are scattered around 10.10 ± 0.2 Pa s). Our results show a large discrepancy of 0.5 log units compared to the predicted viscosity at Tg using the kinetic model of Gottsmann et al. (2002). We further investigate additional relatively iron-rich compositions aiming for the development of an improved model for the viscosity prediction at the glass transition. References: Cukierman, M. and Uhlmann D.R (1974) Effects of iron oxidation-state on viscosity, lunar composition 15555. Journal of Geophysical Research, 79, 1594-1598. Dingwell, D.B. and Virgo, D. (1987) The effect of oxidation-state on the viscosity of melts in the system Na2O-FeO-Fe2O3-SiO2. Geochimica et Cosmochimica Acta, 51, 195-205. Dingwell, D.B. and Webb, S.L. (1989) Structural relaxation in silicate melts and non-newtonian melt rheology in geologic processes. Physics and Chemistry of Minerals, 16, 508-516. Giordano, D.; Russel, J.K.; Dingwell, D.B. (2008) Viscosity of magmatic liquids: A model. Earth and Planetary Science Letters, 271, 123-134. Gottsmann, J.; Giordano, D.; Dingwell, D.B. (2002) Predicting shear viscosity during volcanic processes at the glass transition: a calorimetric calibration. Earth and Planetary Science Letters, 198, 417-427. Hess, K.U. and Dingwell, D.B. (1996) Viscosities of hydrous leucogranitic melts: a non-Arrhenian model. American Mineralogist, 81, 1297-1300. Hui, H. and Zhang, Y. (2007) Toward a general viscosity equation for natural anhydrous and hydrous silicate melts. Geochimica et Cosmochimica Acta, 71, 403- 416.