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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...

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Autores principales: Dumas, Thomas, Virot, Matthieu, Menut, Denis, Tamain, Christelle, Micheau, Cyril, Dourdain, Sandrine, Diat, Olivier
Formato: Online Artículo Texto
Lenguaje:English
Publicado: International Union of Crystallography 2022
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.
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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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