Details

Autor(en) / Beteiligte

• Gerber, Evgeny
• Romanchuk, Anna Yu
• Pidchenko, Ivan
• Amidani, Lucia
• Rossberg, Andre
• Hennig, Christoph
• Vaughan, Gavin B. M
• Trigub, Alexander
• Egorova, Tolganay
• Bauters, Stephen
• Plakhova, Tatiana
• Hunault, Myrtille O. J. Y
• Weiss, Stephan
• Butorin, Sergei M
• Scheinost, Andreas C
• Kalmykov, Stepan N
• Kvashnina, Kristina O

Titel

The missing pieces of the PuO nanoparticle puzzle

Ist Teil von

• Nanoscale, 2020-09, Vol.12 (35), p.1839-1848

Erscheinungsjahr

2020

Quelle

Alma/SFX Local Collection

Beschreibungen/Notizen

• The nanoscience field often produces results more mystifying than any other discipline. It has been argued that changes in the plutonium dioxide (PuO 2 ) particle size from bulk to nano can have a drastic effect on PuO 2 properties. Here we report a full characterization of PuO 2 nanoparticles (NPs) at the atomic level and probe their local and electronic structures by a variety of methods available at the synchrotron, including extended X-ray absorption fine structure (EXAFS) at the Pu L 3 edge, X-ray absorption near edge structure (XANES) in high energy resolution fluorescence detection (HERFD) mode at the Pu L 3 and M 4 edges, high energy X-ray scattering (HEXS) and X-ray diffraction (XRD). The particles were synthesized from precursors with different oxidation states of plutonium (III, IV, and V) under various environmentally and waste storage relevant conditions (pH 8 and pH > 10). Our experimental results analyzed with state-of-the-art theoretical approaches demonstrate that well dispersed, crystalline NPs with a size of ∼2.5 nm in diameter are always formed in spite of diverse chemical conditions. Identical crystal structures and the presence of only the Pu( iv ) oxidation state in all NPs, reported here for the first time, indicate that the structure of PuO 2 NPs is very similar to that of the bulk PuO 2 . All methods give complementary information and show that investigated fundamental properties of PuO 2 NPs, rather than being exotic, are very similar to those of the bulk PuO 2 . We report a full characterization of PuO 2 nanoparticles at the atomic level and probe their local and electronic structure by a variety of methods available at the synchrotron and theoretical approaches.