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Size and structure of hexanuclear plutonium oxo-hydroxo clusters in aqueous solution from synchrotron analysis
The size and shape of a water-soluble hexanuclear plutonium cluster were probed by combining synchrotron small-angle X-ray scattering (SAXS) and extended X-ray absorption fine structure (EXAFS). A specific setup coupling both techniques and dedicated to radioactive samples on the MARS beamline endst...
Autores principales: | , , , , , , |
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Formato: | Online Artículo Texto |
Lenguaje: | English |
Publicado: |
International Union of Crystallography
2022
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Materias: | |
Acceso en línea: | https://www.ncbi.nlm.nih.gov/pmc/articles/PMC8733971/ https://www.ncbi.nlm.nih.gov/pubmed/34985420 http://dx.doi.org/10.1107/S1600577521012005 |
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author | Dumas, Thomas Virot, Matthieu Menut, Denis Tamain, Christelle Micheau, Cyril Dourdain, Sandrine Diat, Olivier |
author_facet | Dumas, Thomas Virot, Matthieu Menut, Denis Tamain, Christelle Micheau, Cyril Dourdain, Sandrine Diat, Olivier |
author_sort | Dumas, Thomas |
collection | PubMed |
description | The size and shape of a water-soluble hexanuclear plutonium cluster were probed by combining synchrotron small-angle X-ray scattering (SAXS) and extended X-ray absorption fine structure (EXAFS). A specific setup coupling both techniques and dedicated to radioactive samples on the MARS beamline endstation at Synchrotron SOLEIL is described. The plutonium hexanuclear cores are well stabilized by the 1,4,7,10-tetraazacyclododecane-1,4,7,10-tetraacetic acid ligands and this allows a good evaluation of the setup to probe the very small plutonium core. The results show that, in spite of the constrained conditions required to avoid any risk of sample dispersion, the flux and the sample environment are optimized to obtain a very good signal-to-noise ratio, allowing the detection of small plutonium aggregates in an aqueous phase. The structure of the well defined hexanuclear cluster has been confirmed by EXAFS measurements in solution and correlated with SAXS data processing and modelling. An iterative comparison of classical fit models (Guinier or sphere form factor) with the experimental results allowed a better interpretation of the SAXS signal that will be relevant for future work under environmentally relevant conditions. |
format | Online Article Text |
id | pubmed-8733971 |
institution | National Center for Biotechnology Information |
language | English |
publishDate | 2022 |
publisher | International Union of Crystallography |
record_format | MEDLINE/PubMed |
spelling | pubmed-87339712022-01-19 Size and structure of hexanuclear plutonium oxo-hydroxo clusters in aqueous solution from synchrotron analysis Dumas, Thomas Virot, Matthieu Menut, Denis Tamain, Christelle Micheau, Cyril Dourdain, Sandrine Diat, Olivier J Synchrotron Radiat Actinide Physics and Chemistry The size and shape of a water-soluble hexanuclear plutonium cluster were probed by combining synchrotron small-angle X-ray scattering (SAXS) and extended X-ray absorption fine structure (EXAFS). A specific setup coupling both techniques and dedicated to radioactive samples on the MARS beamline endstation at Synchrotron SOLEIL is described. The plutonium hexanuclear cores are well stabilized by the 1,4,7,10-tetraazacyclododecane-1,4,7,10-tetraacetic acid ligands and this allows a good evaluation of the setup to probe the very small plutonium core. The results show that, in spite of the constrained conditions required to avoid any risk of sample dispersion, the flux and the sample environment are optimized to obtain a very good signal-to-noise ratio, allowing the detection of small plutonium aggregates in an aqueous phase. The structure of the well defined hexanuclear cluster has been confirmed by EXAFS measurements in solution and correlated with SAXS data processing and modelling. An iterative comparison of classical fit models (Guinier or sphere form factor) with the experimental results allowed a better interpretation of the SAXS signal that will be relevant for future work under environmentally relevant conditions. International Union of Crystallography 2022-01-01 /pmc/articles/PMC8733971/ /pubmed/34985420 http://dx.doi.org/10.1107/S1600577521012005 Text en © Thomas Dumas et al. 2022 https://creativecommons.org/licenses/by/4.0/This is an open-access article distributed under the terms of the Creative Commons Attribution (CC-BY) Licence, which permits unrestricted use, distribution, and reproduction in any medium, provided the original authors and source are cited. |
spellingShingle | Actinide Physics and Chemistry Dumas, Thomas Virot, Matthieu Menut, Denis Tamain, Christelle Micheau, Cyril Dourdain, Sandrine Diat, Olivier Size and structure of hexanuclear plutonium oxo-hydroxo clusters in aqueous solution from synchrotron analysis |
title | Size and structure of hexanuclear plutonium oxo-hydroxo clusters in aqueous solution from synchrotron analysis |
title_full | Size and structure of hexanuclear plutonium oxo-hydroxo clusters in aqueous solution from synchrotron analysis |
title_fullStr | Size and structure of hexanuclear plutonium oxo-hydroxo clusters in aqueous solution from synchrotron analysis |
title_full_unstemmed | Size and structure of hexanuclear plutonium oxo-hydroxo clusters in aqueous solution from synchrotron analysis |
title_short | Size and structure of hexanuclear plutonium oxo-hydroxo clusters in aqueous solution from synchrotron analysis |
title_sort | size and structure of hexanuclear plutonium oxo-hydroxo clusters in aqueous solution from synchrotron analysis |
topic | Actinide Physics and Chemistry |
url | https://www.ncbi.nlm.nih.gov/pmc/articles/PMC8733971/ https://www.ncbi.nlm.nih.gov/pubmed/34985420 http://dx.doi.org/10.1107/S1600577521012005 |
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