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Dissolution kinetics of hydrated calcium aluminates (AFm-Cl) as a function of pH and at room temperature

Published online by Cambridge University Press:  02 January 2018

Nicolas C. M. Marty ,
Sylvain Grangeon ,
Catherine Lerouge ,
Fabienne Warmont ,
Olivier Rozenbaum ,
Thibauld Conte  and
Francis Claret
Nicolas C. M. Marty*
Affiliation:
BRGM, 45060 Orléans Cedex 2, France
Sylvain Grangeon
Affiliation:
BRGM, 45060 Orléans Cedex 2, France
Catherine Lerouge
Affiliation:
BRGM, 45060 Orléans Cedex 2, France
Fabienne Warmont
Affiliation:
ICMN – CNRS - Université d’Orléans, 1b rue de la Férollerie, 45071 Orléans Cedex 2, France
Olivier Rozenbaum
Affiliation:
Institut des Sciences de la Terre d’Orléans (ISTO), UMR 6113, 1A, rue de la Férollerie, 45071 Orléans Cedex 2, France
Thibauld Conte
Affiliation:
BRGM, 45060 Orléans Cedex 2, France
Francis Claret
Affiliation:
BRGM, 45060 Orléans Cedex 2, France
*
*E-mail: [email protected]
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Abstract

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The determination of reliable weathering/dissolution rates for cement phases is of fundamental importance for the modelling of the temporal evolution of both radioactive waste repositories and CO2 geological storage sites (e.g. waste matrix, plug in boreholes). Here, the dissolution kinetics of AFm-Cl (hydrated calcium aluminates containing interlayer Cl) has been studied using flow-through experiments conducted at pH values ranging from 9.2 to 13. Mineralogical (XRD) and chemical (EPMA, TEM) analyses have been performed to determine the evolution of the phases during the dissolution experiments. For pH values between 10 and 13, the dissolution of AFm-Cl is congruent (i.e. Ca/Al ratios close to 2 both for solids and outlet concentrations). In contrast, the precipitation of amorphous Al-phases and possibly amorphous mixed Al/Ca phases is observed at pH 9.2, leading to Ca/Al ratios in the outlet solutions higher than those of the initial solid. Therefore, at pH 9.2, even if Cl–/OH– exchange occurs, estimation of dissolution rate from released Cl appears to be the best proxy. Dissolution rates were normalized to the final specific surface areas (ranging from 6.1 to 35.4 m2 g−1). Dissolution rate appears to be pH-independent and therefore the far-from-equilibrium dissolution rate at room temperature is expressed as: logR(mol m–2 s–1) = –9.23 ± 0.18

Keywords

hydrated calcium aluminatesAFmFriedel’s saltdissolutionkinetics
Type
Research Article
Information
Mineralogical Magazine , Volume 81 , Issue 5 , October 2017 , pp. 1245 - 1259
Creative Commons
Creative Common License - CCCreative Common License - BY
© [2017] The Mineralogical Society of Great Britain and Ireland. This is an open access article distributed under the terms of the Creative Commons Attribution (CC BY) licence (http://creativecommons.org/licenses/by/4.0/), which permits unrestricted use, distribution, and reproduction in any medium, provided the original work is properly cited.
Copyright
Copyright © The Mineralogical Society of Great Britain and Ireland 2017

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