Probing the Local Structure of Nanoscaled Actinide Oxides: A Comparison between PuO2 and ThO2 Nanoparticles Rules out PuO2+x Hypothesis

Autor: Thierry Wiss, Laurent Venault, Philippe Moisy, Thomas Dumas, Adel Mesbah, Oliver Dieste Blanco, Matthieu Virot, Damien Prieur, Laura Bonato, Xavier F. Le Goff, Sergey I. Nikitenko, Elodie Dalodière, Michael Odorico, Nicolas Dacheux, André Rossberg
Přispěvatelé: CEA, Contributeur MAP, Sonochimie dans les Fluides Complexes (LSFC), Institut de Chimie Séparative de Marcoule (ICSM - UMR 5257), Centre National de la Recherche Scientifique (CNRS)-Institut de Chimie du CNRS (INC)-Université de Montpellier (UM)-Ecole Nationale Supérieure de Chimie de Montpellier (ENSCM)-Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Centre National de la Recherche Scientifique (CNRS)-Institut de Chimie du CNRS (INC)-Université de Montpellier (UM)-Ecole Nationale Supérieure de Chimie de Montpellier (ENSCM)-Commissariat à l'énergie atomique et aux énergies alternatives (CEA), Commissariat à l'énergie atomique et aux énergies alternatives (CEA), Northwestern University [Evanston], European Commission - Joint Research Centre [Karlsruhe] (JRC), Etude de la Matière en Mode Environnemental (L2ME), European Synchrotron Radiation Facility (ESRF), Département RadioChimie et Procédés (DRCP), CEA-Direction des Energies (ex-Direction de l'Energie Nucléaire) (CEA-DES (ex-DEN)), Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Commissariat à l'énergie atomique et aux énergies alternatives (CEA), Interfaces de Matériaux en Evolution (LIME), Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Ecole Nationale Supérieure de Chimie de Montpellier (ENSCM)-Institut de Chimie du CNRS (INC)-Université de Montpellier (UM)-Centre National de la Recherche Scientifique (CNRS)-Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Ecole Nationale Supérieure de Chimie de Montpellier (ENSCM)-Institut de Chimie du CNRS (INC)-Université de Montpellier (UM)-Centre National de la Recherche Scientifique (CNRS), Institut des Sciences et technologies pour une Economie Circulaire des énergies bas carbone (ISEC)
Jazyk: angličtina
Rok vydání: 2019
Předmět:
[CHIM.INOR] Chemical Sciences/Inorganic chemistry
Materials science
Oxide
Nanoparticle
Bioengineering
02 engineering and technology
[CHIM.INOR]Chemical Sciences/Inorganic chemistry
010402 general chemistry
01 natural sciences
Colloid
chemistry.chemical_compound
[CHIM.RADIO] Chemical Sciences/Radiochemistry
[CHIM.CRIS]Chemical Sciences/Cristallography
General Materials Science
Reactivity (chemistry)
[CHIM.CRIS] Chemical Sciences/Cristallography
ComputingMilieux_MISCELLANEOUS
[CHIM.MATE] Chemical Sciences/Material chemistry
Extended X-ray absorption fine structure
General Engineering
[CHIM.MATE]Chemical Sciences/Material chemistry
General Chemistry
Actinide
021001 nanoscience & nanotechnology
Atomic and Molecular Physics
and Optics

0104 chemical sciences
Characterization (materials science)
Nanocrystal
chemistry
Chemical physics
0210 nano-technology
[CHIM.RADIO]Chemical Sciences/Radiochemistry
Zdroj: Nanoscale Advances
Nanoscale Advances, RSC, 2020, 2 (1), pp.214-224. ⟨10.1039/c9na00662a⟩
Nanoscale Advances, 2019, pp.214-224. ⟨10.1039/C9NA00662A⟩
Nanoscale Advances, 2020, 2 (1), pp.214-224. ⟨10.1039/c9na00662a⟩
Nanoscale Advances 2(2020)1, 214-224
ISSN: 2516-0230
DOI: 10.1039/c9na00662a⟩
Popis: International audience; Actinide research at the nanoscale is gaining fundamental interest due to environmental and industrial issues. The knowledge of the local structure and speciation of actinide nanoparticles, which possibly exhibit specific physico-chemical properties in comparison to bulk materials, would help in a better and reliable description of their behaviour and reactivity. Herein, the synthesis and relevant characterization of PuO2 and ThO2 nanoparticles displayed as dispersed colloids, nanopowders or nanostructured oxide powders, allow to establish a clear relationship between the size of the nanocrystals composing these oxides and their corresponding An(IV) local structure investigated by EXAFS spectroscopy. Particularly, the probed An(IV) first oxygen shell evidences an analogous behaviour for both Pu and Th oxides. This observation suggests that the often observed and controversial splitting of the Pu-O shell on the Fourier transformed EXAFS signal of PuO2 samples is attributed to a local structural disorder driven by a nanoparticle surface effect rather than to the presence of PuO2+x species.
Databáze: OpenAIRE