Rheology of a sodium‐molybdenum borosilicate melt undergoing phase separation

Author:

Pereira Luiz1ORCID,Schuller Sophie2ORCID,Wadsworth Fabian B.3ORCID,Vasseur Jérémie1ORCID,Lancelotti Ricardo F.4ORCID,Hess Kai‐Uwe1,Gossé Stéphane5ORCID,Dingwell Donald B.1ORCID

Affiliation:

1. Department of Earth and Environmental Sciences Ludwig‐Maximilians‐Universität München Munich Germany

2. CEA, DES, ISEC, DPME University of Montpellier Marcoule France

3. Department of Earth Sciences Durham University Durham UK

4. Department of Materials Engineering (DEMa) Federal University of São Carlos (UFSCar) São Carlos São Paulo Brazil

5. Université Paris‐Saclay, CEA Service de Recherche en Corrosion et Comportement des Matériaux Gif‐sur‐Yvette France

Abstract

AbstractDuring glass production, phase separation can result in the formation of suspended liquid droplets, which can cause changes in the system rheology. In nuclear waste vitrification context, some new glassy matrices may present this phase separation matter, but the mechanisms controlling the viscosity changes have not yet been determined. Here, we measure the viscosity of a sodium‐borosilicate melt containing dissolved MoO3 at different temperatures and subject to different applied shear strain rates. We observe that (i) the viscosity increases sharply as the temperature decreases and (ii) at any constant temperature below 1000°C, the system presents non‐Newtonian response. Using transmission electron microscope observations coupled with viscosity calculations, we interpret the cause of the observed changes as the result of phase separation. We show that the viscosity increase on cooling is in excess of the predicted temperature dependence for a homogeneous melt of the starting composition. The increase is due to the formation of a second phase and is controlled by chemical and structural modifications of the matrix during the loss of the elements that form the droplets. This work provides insights into the rheology of a system composed of two composition sets due to a miscibility gap.

Funder

Alexander von Humboldt-Stiftung

Publisher

Wiley

Subject

General Materials Science

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