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Reversibility in radionuclide/bentonite bulk and colloidal ternary systems

Published online by Cambridge University Press:  02 January 2018

Nick Sherriff ,
Ragiab Issa ,
Katherine Morris ,
Francis Livens ,
Sarah Heath  and
Nick Bryan
Nick Sherriff
Affiliation:
Centre for Radiochemistry Research, School of Chemistry, University of Manchester, Manchester M13 9PL, UK
Ragiab Issa
Affiliation:
Centre for Radiochemistry Research, School of Chemistry, University of Manchester, Manchester M13 9PL, UK
Katherine Morris
Affiliation:
Research Centre for Radwaste and Decommissioning, School of Earth, Atmospheric and Environmental Sciences, University of Manchester, Manchester M13 9PL, UK
Francis Livens
Affiliation:
Centre for Radiochemistry Research, School of Chemistry, University of Manchester, Manchester M13 9PL, UK Research Centre for Radwaste and Decommissioning, School of Earth, Atmospheric and Environmental Sciences, University of Manchester, Manchester M13 9PL, UK
Sarah Heath
Affiliation:
Centre for Radiochemistry Research, School of Chemistry, University of Manchester, Manchester M13 9PL, UK
Nick Bryan*
Affiliation:
National Nuclear Laboratory, 5th Floor, Chadwick House, Birchwood, Warrington WA3 6AE, UK
*
*E-mail: nick.bryan@nnl.co.uk
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Abstract

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Ternary systems of 152Eu(III), bulk bentonite and ethylenediaminetetraacetic acid (EDTA) ([Eu] = 7.9 × 10–10 M; pH = 6.0–7.0) have been studied. Without EDTA, there was slow uptake in a two-stage process, with initial rapid sorption of Eu(III) (96%), followed by slower uptake of a much smaller fraction (3.0% over a period of one month). The reversibility of Eu(III) binding was tested by allowing Eu(III) to sorb to bentonite for 1–322 days. EDTA was added to the pre-equilibrated Eu bentonite systems at 0.01 M, a concentration that was sufficient to suppress sorption in a system where EDTA was present prior to the contact of Eu(III) with bentonite. A fraction of the Eu was released instantaneously (30–50%), but a significant amount remained bound. With time, the amount of Eu(III) retained by the bentonite reduced, with a slow fraction dissociation rate constant of approximately 4.3 × 10–8 s–1 (values in the range 2.2 × 10–8 – 1.0 × 10–7 s–1) for pre-equilibration times ≥7 days. Eventually, the amount of Eu(III) remaining bound to the bentonite was within error of that when EDTA was present prior to contact (4.5% ± 0.6), although in systems with pre-equilibration times >100 days, full release took up to 500 days. Europium interactions with colloidal bentonite were also studied, and the dissociation rate constant measured by a resin competition method. For the colloids, more Eu was found in the slowly dissociating fraction (60–70%), but the first-order dissociation rate constant was faster, with an average rate constant of 8.8 × 10–7 s–1 and a range of 7.7 × 10–7 –9.5 × 10–7 s–1. For both bulk and colloidal bentonite, although slow dissociation was observed for Eu(III), there was no convincing evidence for 'irreversible' binding.

Keywords

ternary systemsbentoniteethylenediaminetetraacetic acidEDTAeuropium152Eu(III)reversibilitydissociation rate constant
Type
Research Article
Information
Mineralogical Magazine , Volume 79 , Issue 6 , November 2015 , pp. 1307 - 1315
Creative Commons
Creative Common License - CCCreative Common License - BY
Copyright © The Mineralogical Society of Great Britain and Ireland 2015. This is an open access article, distributed under the terms of the Creative Commons Attribution (CC BY) license (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 2015

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