Bray, AW, Benning, LG, Bonneville, S et al. (1 more author) (2014) Biotite surface chemistry as a function of aqueous fluid composition. Geochimica et Cosmochimica Acta, 128. 58 - 70. ISSN 0016-7037
Abstract
The chemical composition and charge of the biotite near-surface, in contact with NaCl bearing aqueous solutions at 25°C from pH 1 to 12, have been derived via zeta potential measurements and potentiometric titrations performed for 20 and 60min in batch reactors. Zeta potential measurements yielded an isoelectric point of pH 3.0 (±0.2) and batch potentiometric titrations yielded a pH of immersion of 9.66 (S.D. 0.24). From batch potentiometric titrations we determined both the proton consumption and the metal release from the biotite surface as a function of pH. Potassium removal from the near-surface of biotite is only slightly dependent on pH with a minimum of ~6atomsnm removed at the immersion pH, corresponding to an average depletion depth of ~1.5nm. In contrast, the release of Mg, Al and Fe is strongly pH-dependent as those metals are preferentially removed from the biotite surface at pH less than 9 (Mg) and 4 (Al, Fe). The average depletion depth of Mg, Al, and Fe increases with decreasing pH, reaching on average ~2nm at pH ~1. The removal of K, Mg, Al, and Fe is not charge conservative, resulting in a relative negative charge in the biotite near-surface. Taken together, our results indicate that the composition of the biotite surface varies dramatically as a function of pH. At basic conditions, the biotite near-surface is K depleted and likely hydrogen enriched. At near-neutral conditions, the biotite near-surface is comprised of only the Si and Al tetrahedral, and the Fe(II) octahedral framework, following the removal of both alkali metals and Mg. Finally, at acidic conditions, the biotite near-surface is comprised exclusively of a remnant Si, O and H framework. The results of these experiments give an indication of the composition and charge of the biotite surface in the natural environment, following contact with water, for example in the vadose zone, and can help us understand weathering reactions in these systems.
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Item Type: | Article |
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Authors/Creators: |
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Copyright, Publisher and Additional Information: | (c) 2013 Published by Elsevier Ltd. Uploaded in accordance with the publisher's self-archiving policy. NOTICE: this is the author’s version of a work that was accepted for publication in Geochimica et Cosmochimica Acta. Changes resulting from the publishing process, such as peer review, editing, corrections, structural formatting, and other quality control mechanisms may not be reflected in this document. Changes may have been made to this work since it was submitted for publication. A definitive version was subsequently published in Geochimica et Cosmochimica Acta, 128, (2014) DOI 10.1016/j.gca.2013.12.002 |
Dates: |
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Institution: | The University of Leeds |
Academic Units: | The University of Leeds > Faculty of Environment (Leeds) > School of Earth and Environment (Leeds) |
Depositing User: | Symplectic Publications |
Date Deposited: | 14 Aug 2014 14:35 |
Last Modified: | 18 Jan 2018 05:12 |
Published Version: | http://dx.doi.org/10.1016/j.gca.2013.12.002 |
Status: | Published |
Publisher: | Elsevier |
Identification Number: | 10.1016/j.gca.2013.12.002 |
Related URLs: | |
Open Archives Initiative ID (OAI ID): | oai:eprints.whiterose.ac.uk:79959 |