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Thermodynamic and crystallographic model for anion uptake by hydrated calcium aluminate (AFm): an example of molybdenum
Amongst all cement phases, hydrated calcium aluminate (AFm) plays a major role in the retention of anionic species. Molybdenum (Mo), whose (93)Mo isotope is considered a major steel activation product, will be released mainly under the form of MoO(4)(2−) in a radioactive waste repository. Understand...
Autores principales: | , , , , , |
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Formato: | Online Artículo Texto |
Lenguaje: | English |
Publicado: |
Nature Publishing Group UK
2018
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Materias: | |
Acceso en línea: | https://www.ncbi.nlm.nih.gov/pmc/articles/PMC5962639/ https://www.ncbi.nlm.nih.gov/pubmed/29784983 http://dx.doi.org/10.1038/s41598-018-26211-z |
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author | Marty, Nicolas C. M. Grangeon, Sylvain Elkaïm, Erik Tournassat, Christophe Fauchet, Clémence Claret, Francis |
author_facet | Marty, Nicolas C. M. Grangeon, Sylvain Elkaïm, Erik Tournassat, Christophe Fauchet, Clémence Claret, Francis |
author_sort | Marty, Nicolas C. M. |
collection | PubMed |
description | Amongst all cement phases, hydrated calcium aluminate (AFm) plays a major role in the retention of anionic species. Molybdenum (Mo), whose (93)Mo isotope is considered a major steel activation product, will be released mainly under the form of MoO(4)(2−) in a radioactive waste repository. Understanding its fate is of primary importance in a safety analysis of such disposal. This necessitates models that can both predict quantitatively the sorption of Mo by AFm and determine the nature of the sorption process (i.e., reversible adsorption or incorporation). This study investigated the Cl(−)/MoO(4)(2−) exchange processes occurring in an AFm initially containing interlayer Cl in alkaline conditions using flow-through experiments. The evolution of the solid phase was characterized using an electron probe microanalyzer and synchrotron high-energy X-ray scattering. All data, together with their quantitative modeling, coherently indicated that Mo replaced Cl in the AFm interlayer. The structure of the interlayer is described with unprecedented atomic-scale detail based on a combination of real- and reciprocal-space analyses of total X-ray scattering data. In addition, modeling of several independent chemical experiments elucidated that Cl(−)/OH(−) exchange processes occur together with Cl(−)/MoO(4)(2−) exchange. This competitive effect must be considered when determining the Cl(−)/MoO(4)(2−) selectivity constant. |
format | Online Article Text |
id | pubmed-5962639 |
institution | National Center for Biotechnology Information |
language | English |
publishDate | 2018 |
publisher | Nature Publishing Group UK |
record_format | MEDLINE/PubMed |
spelling | pubmed-59626392018-05-24 Thermodynamic and crystallographic model for anion uptake by hydrated calcium aluminate (AFm): an example of molybdenum Marty, Nicolas C. M. Grangeon, Sylvain Elkaïm, Erik Tournassat, Christophe Fauchet, Clémence Claret, Francis Sci Rep Article Amongst all cement phases, hydrated calcium aluminate (AFm) plays a major role in the retention of anionic species. Molybdenum (Mo), whose (93)Mo isotope is considered a major steel activation product, will be released mainly under the form of MoO(4)(2−) in a radioactive waste repository. Understanding its fate is of primary importance in a safety analysis of such disposal. This necessitates models that can both predict quantitatively the sorption of Mo by AFm and determine the nature of the sorption process (i.e., reversible adsorption or incorporation). This study investigated the Cl(−)/MoO(4)(2−) exchange processes occurring in an AFm initially containing interlayer Cl in alkaline conditions using flow-through experiments. The evolution of the solid phase was characterized using an electron probe microanalyzer and synchrotron high-energy X-ray scattering. All data, together with their quantitative modeling, coherently indicated that Mo replaced Cl in the AFm interlayer. The structure of the interlayer is described with unprecedented atomic-scale detail based on a combination of real- and reciprocal-space analyses of total X-ray scattering data. In addition, modeling of several independent chemical experiments elucidated that Cl(−)/OH(−) exchange processes occur together with Cl(−)/MoO(4)(2−) exchange. This competitive effect must be considered when determining the Cl(−)/MoO(4)(2−) selectivity constant. Nature Publishing Group UK 2018-05-21 /pmc/articles/PMC5962639/ /pubmed/29784983 http://dx.doi.org/10.1038/s41598-018-26211-z Text en © The Author(s) 2018 Open Access This article is licensed under a Creative Commons Attribution 4.0 International License, which permits use, sharing, adaptation, distribution and reproduction in any medium or format, as long as you give appropriate credit to the original author(s) and the source, provide a link to the Creative Commons license, and indicate if changes were made. The images or other third party material in this article are included in the article’s Creative Commons license, unless indicated otherwise in a credit line to the material. If material is not included in the article’s Creative Commons license and your intended use is not permitted by statutory regulation or exceeds the permitted use, you will need to obtain permission directly from the copyright holder. To view a copy of this license, visit http://creativecommons.org/licenses/by/4.0/. |
spellingShingle | Article Marty, Nicolas C. M. Grangeon, Sylvain Elkaïm, Erik Tournassat, Christophe Fauchet, Clémence Claret, Francis Thermodynamic and crystallographic model for anion uptake by hydrated calcium aluminate (AFm): an example of molybdenum |
title | Thermodynamic and crystallographic model for anion uptake by hydrated calcium aluminate (AFm): an example of molybdenum |
title_full | Thermodynamic and crystallographic model for anion uptake by hydrated calcium aluminate (AFm): an example of molybdenum |
title_fullStr | Thermodynamic and crystallographic model for anion uptake by hydrated calcium aluminate (AFm): an example of molybdenum |
title_full_unstemmed | Thermodynamic and crystallographic model for anion uptake by hydrated calcium aluminate (AFm): an example of molybdenum |
title_short | Thermodynamic and crystallographic model for anion uptake by hydrated calcium aluminate (AFm): an example of molybdenum |
title_sort | thermodynamic and crystallographic model for anion uptake by hydrated calcium aluminate (afm): an example of molybdenum |
topic | Article |
url | https://www.ncbi.nlm.nih.gov/pmc/articles/PMC5962639/ https://www.ncbi.nlm.nih.gov/pubmed/29784983 http://dx.doi.org/10.1038/s41598-018-26211-z |
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