The glass transition and the non-Arrhenian viscosity of carbonate melts

D.B. Dingwell, Kai-Uwe Hess*, Martin C. Wilding, Richard A Brooker, Danilo Di Genova, James W E Drewitt , Mark Wilson, Daniel Weidendorfer

*Corresponding author for this work

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Abstract

We report the first calorimetric observation of the glass transition for a carbonate melt. A carbonate glass [55K2CO3–45MgCO3 (molar)] was quenched from 780 °C at 0.1 GPa. The activation energy of structural relaxation close to the glass transition was derived through a series of thermal treatments comprising excursions across the glass transition at different heating rates. Viscosities just above the glass transition temperature were obtained by applying a shift factor to the calorimetric results. These viscosity measurements (in the range of 109 Pa·s) at supercooled temperatures (ca. 230 °C) dramatically extend the temperature range of data for carbonates, which were previously restricted to super-liquidus viscosities well below 1 Pa·s. Combining our calorimetrically derived results with published alkaline-earth carbonate melt viscosities at high temperatures yields a highly non-Arrhenian viscosity-temperature relationship and confirms that carbonate liquids are “fragile.” Based on simulations, fragile behavior is also exhibited by Na2CO3 melt. In both cases, the fragility presumably relates to the formation of temperature-dependent low-dimensional structures and Vogel-Fulcher-Tammann (VFT) curves adequately describe the viscosity-temperature relationships of carbonate melts below 1000 °C.
Original languageEnglish
Pages (from-to)1053-1064
Number of pages12
JournalAmerican Mineralogist
Volume107
Issue number6
Early online date31 May 2022
DOIs
Publication statusE-pub ahead of print - 31 May 2022

Bibliographical note

Funding Information:
We thank Fabrice Gaillard and Rodolphe Vuilleumier for fruitful suggestions that greatly improved the manuscript. R.A.B was funded by the NERC Thematic Grant consortium NE/M000419/1. J.W.E.D acknowledges support from NERC under Grant NE/P002951/1. D.B.D. acknowledges the support of ERC 2018 ADV Grant 834255 (EAVESDROP).

Publisher Copyright:
© 2022 Donald B. Dingwell, Kai-Uwe Hess, Martin C. Wilding, Richard A. Brooker, Danilo Di Genova, James W.E. Drewitt, Mark Wilson, and Daniel Weidendorfer, published by Mineralogical Society of America.

Keywords

  • Viscosity
  • glass transition
  • fragility
  • carbonate melt
  • carbonatite
  • shift factor

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