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Spectroscopic characterization of neptunium(VI), plutonium(VI), americium(VI) and neptunium(V) encapsulated in uranyl nitrate hexahydrate.
- Source :
-
Physical chemistry chemical physics : PCCP [Phys Chem Chem Phys] 2021 Jun 16; Vol. 23 (23), pp. 13228-13241. - Publication Year :
- 2021
-
Abstract
- The coordination of crystalline products resulting from the co-crystallization of Np(vi), Pu(vi), Am(vi), and Np(v) with uranyl nitrate hexahydrate (UNH) has been revealed through solid-state spectroscopic characterization via diffuse reflectance UV-Vis-NIR spectroscopy, SEM-EDS, and extended X-ray absorption fine structure (EXAFS) spectroscopy. Density functional and multireference wavefunction calculations were performed to analyze the An(vi/v)O2(NO3)2·2H2O electronic structures and to help assign the observed transitions in the absorption spectra. EXAFS show a similar coordination between the U(VI) in UNH and Np(vi) and Pu(vi); while Am resulted in a similar coordination to Am(iii), as reduction of Am(vi) occurred prior to EXAFS data being obtained. The co-crystallization of the oxidized transuranic species-penta- and hexavalent-with UNH, represents a significant advance from not only a practical standpoint in providing an elegant solution for used nuclear fuel recycle, but also as an avenue to expand the fundamental understanding of the 5f electronic behavior in the solid-state.
Details
- Language :
- English
- ISSN :
- 1463-9084
- Volume :
- 23
- Issue :
- 23
- Database :
- MEDLINE
- Journal :
- Physical chemistry chemical physics : PCCP
- Publication Type :
- Academic Journal
- Accession number :
- 34086024
- Full Text :
- https://doi.org/10.1039/d1cp01047f