Title: High-Resolution Solid-State Oxygen-17 NMR of Actinide-Bearing Compounds: An Insight into the 5f Chemistry
Authors: MARTEL LAURAMAGNANI NicolaVIGIER JEAN-FRANCOISBOSHOVEN JacobusSELFSLAG ChrisFARNAN I.GRIVEAU Jean-ChristopheSOMERS JosephFANGHAENEL Thomas
Citation: INORGANIC CHEMISTRY vol. 53 no. 13 p. 6928 - 6933
Publisher: AMER CHEMICAL SOC
Publication Year: 2014
JRC N°: JRC88514
ISSN: 0020-1669
URI: http://pubs.acs.org/doi/abs/10.1021/ic5007555
http://publications.jrc.ec.europa.eu/repository/handle/JRC88514
DOI: 10.1021/ic5007555
Type: Articles in periodicals and books
Abstract: A massive interest has been generated lately by the improvement of solid-state magic-angle spinning (MAS) NMR methods for the study of a broad range of paramagnetic organic and inorganic materials. The open-shell cations at the origin of this paramagnetism can be metals, transition metals, or rare-earth elements. Actinide-bearing compounds and their 5f unpaired electrons remain elusive in this intensive research area due to their well-known high radiotoxicity. A dedicated effort enabling the handling of these highly radioactive materials now allows their analysis using high-resolution MAS NMR (>55 kHz). Here, the study of the local structure of a series of actinide dioxides, namely, ThO2, UO2, NpO2, PuO2, and AmO2, using solid-state 17O MAS NMR is reported. An important increase of the spectral resolution is found due to the removal of the dipolar broadening proving the efficiency of this technique for structural analysis. The NMR parameters in these systems with numerous and unpaired 5f electrons were interpreted using an empirical approach. Single-ion model calculations were performed for the first time to determine the z component of electron spin on each of the actinide atoms, which is proportional to the shifts. A similar variation thereof was observed only for the heavier actinides of this study.
JRC Directorate:Nuclear Safety and Security

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