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Effect of water on the glass transition of a potassium-magnesium carbonate melt

  • Daniel Weidendorfer*
  • , Kai Uwe Hess
  • , Ruben M. Ruhekenya
  • , Jürgen E.K. Schawe
  • , Martin C. Wilding
  • , Donald B. Dingwell
  • *Corresponding author for this work
  • Ludwig Maximilian University of Munich
  • Mettler-Toledo
  • ETH Zurich - Institute for Particle Physics and Astrophysics (IPA)
  • UK Catalysis Hub

Research output: Contribution to journalArticlepeer-review

Abstract

Calorimetric measurements of the glass transition temperatures (T g) of hydrous carbonate melts are reported on a near-eutectic composition of 55 mol% K 2 CO 3 -45 mol% MgCO 3 with up to 42 mol% bulk H 2 O dissolved in the carbonate melt. Hydrous melts were quenched from 750°C to transparent and crystal-free glasses and were subsequently analysed for water content before and after measuring T g by high-sensitivity differential scanning calorimetry. The glass transition and limited fictive temperatures as a function of the water content were determined at 10 K/min cooling/heating rates resulting in T g ranging from 245°C at nominally anhydrous conditions to 83°C in the presence of 42 mol% H 2 O in the glass. Through a generalized Gordon-Taylor analysis, the factors k (7.27), k 0 (3.2) and the interaction parameter A x (0.49) were derived. The limited fictive temperature of a hypothetically, zero water containing 55 mol% K 2 CO 3 -45 mol% MgCO 3 glass is 232 ± 5°C (505 K). The high value of the interaction parameter A indicates strong specific molecular interactions between water and the carbonates in the glassy state and a large decrease in the excess enthalpy of mixing during the conversion of the glassy into the liquid state at the glass transition. This article is part of the theme issue 'Exploring the length scales, timescales and chemistry of challenging materials (Part 1)'.

Original languageEnglish
Article number20220355
JournalPhilosophical transactions. Series A, Mathematical, physical, and engineering sciences
Volume381
Issue number2258
DOIs
StatePublished - 16 Oct 2023
Externally publishedYes

Keywords

  • Gordon-Taylor analysis
  • differential scanning calorimetry
  • glass transition temperature
  • potassium-magnesium carbonate
  • water

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