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An experimental study of tremolite dissolution rates as a function of pH and temperature: Implications for tremolite toxicity and its use in carbon storage

Published online by Cambridge University Press:  05 July 2018

Tamara Diedrich ,
Jacques Schott  and
Eric H. Oelkers
Tamara Diedrich
Affiliation:
GET-Université de Toulouse-CNRS-IRD-OMP, 14 Avenue Edouard Belin, 31400 Toulouse, France
Jacques Schott
Affiliation:
GET-Université de Toulouse-CNRS-IRD-OMP, 14 Avenue Edouard Belin, 31400 Toulouse, France
Eric H. Oelkers*
Affiliation:
GET-Université de Toulouse-CNRS-IRD-OMP, 14 Avenue Edouard Belin, 31400 Toulouse, France Earth Sciences, University College London, Gower Street, London WC1E 6BT, UK
*
* E-mail: Oelkers@get.obs-mip.fr
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Abstract

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Steady-state tremolite dissolution rates, at far-from-equilibrium conditions, were measured as a function of aqueous silica and magnesium activity, pH from 1.9 to 6.7, and temperature from 25 to 150ºC. Calcium is released from tremolite faster than either Mg or Si throughout most of the experiments even after these latter elements attained steady-state release rates. The preferential removal of Ca releases fine Mg-Si rich needle-like fibres from the tremolite, probably promoting its toxicity. In contrast, Mg was released in stoichiometric or near to stoichiometric proportion to Si once steady-state was attained. Measured steady-state tremolite dissolution rates based on Si release can be described using

where r+ signifies the BET surface area-normalized forward tremolite steady-state dissolution rate, AA refers to a pre-exponential factor = 6610–3 mol cm–2 s–1, EA designates an activation energy equal to 80 kJ mol–1, R represents the gas constant, T denotes absolute temperature, and ai refers to the activity of the subscripted aqueous species. This rate expression is consistent with tremolite dissolution rates at acidic pH being controlled by the detachment of partially liberated silica tetrahedra formed from the exchange of Mg2+ for two protons near the mineral surface after the near-surface Ca has been removed. Nevertheless, Mg release rates from tremolite are ~3 orders of magnitude slower than those from forsterite and enstatite suggesting that tremolite carbonation will be far less efficient than the carbonation of these other Mg-silicate minerals.

Keywords

tremolitedissolution ratesbiodurabilitymineral carbonation
Type
Research Article
Information
Mineralogical Magazine , Volume 78 , Issue 6 , November 2014 , pp. 1449 - 1464
Creative Commons
Creative Common License - CCCreative Common License - BY
© [2014] 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 2014

Footnotes

§

Present address: Barr Consulting, Duluth MN, USA

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