Computational insights into the lattice dynamics of Pu(IV) oxalates
Source abstract
Abstract
Despite its use in PuO 2 production, the structure of anhydrous Pu(C 2O 4) 2 is still not completely understood. Recently, two candidate structures for Pu(C 2O 4) 2 were proposed via density functional theory (DFT), after which the first experimental optical vibrational spectra were reported. Here, we calculated the lattice dynamics of the candidate structures using DFT and found that the primary difference between them is the presence of a vibrational mode near 1380 cm −1 in one structure. The frequency and optical activity of this mode agree well with the published experimental results, providing strong support for this calculated structure as that of anhydrous Pu(C 2O 4) 2.
Source: expertdata · Quality: candidate unverified · Source record ↗
Research context
OpenAlex topics: Radioactive element chemistry and processing · Nuclear Materials and Properties · Nuclear materials and radiation effects
SciVX discovery tags are terminology-based. OpenAlex topics are source-provided classifications.
References (21)
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1. Crowder, M. L.; Pierce, R. A.; Scogin, J. H.; Daniel, W. E.; King, W. D. Small-Scale Testing of Plutionium(IV) Oxalate Precipitation and Calcination to Plutonium Oxide to Support the MOX Feed Mission (SRNL-STI-2012-00338); 2012.10.2172/1044791 ↗
2. Myser, M. N. Thermal decomposition of plutionium (IV) Oxalate and Hydrofluorination of Plutonium (IV) Oxalate and Oxide; 1956.10.2172/4181389 ↗
3. Thermal decomposition of tetravalent and trivalent plutonium oxalates10.1007/BF01505392 ↗
4. Thermal decomposition of plutonium oxalates10.1016/0022-1902(63)80395-4 ↗
5. Remarks on the thermal decomposition of plutonium (IV) Oxalates10.1016/0022-1902(64)80142-1 ↗
6. The thermal decomposition of hydrated plutonium(IV) oxalates10.1016/0022-1902(64)80239-6 ↗
7. The thermal decomposition of plutionium (IV) Oxalate Hexahydrate10.1007/BF01909457 ↗
8. Thermal Decomposition of Np(IV) and Pu(III, IV) Oxalates10.1007/BF02117565 ↗
9. Insights into the thermal decomposition of plutonium(IV) Oxalate – a DFT study of the intermediate structures10.1016/j.jnucmat.2021.152864 ↗
10. Reaction Mechanisms of the Thermal Conversion of Pu(IV) Oxalate into Plutonium Oxide10.1016/j.jallcom.2007.01.057 ↗
11. A review of plutonium oxalate decomposition reactions and effects of decomposition temperature on the surface area of the plutonium dioxide product10.1016/j.jnucmat.2015.06.058 ↗
12. Raman and infrared spectra of plutonium (IV) oxalate and its thermal degradation products10.1016/j.jnucmat.2022.153574 ↗
13. Ab initio molecular dynamics for liquid metals10.1103/PhysRevB.47.558 ↗
14. Efficient iterative schemes for ab initio total-energy calculations using a plane-wave basis set10.1103/PhysRevB.54.11169 ↗
15. Efficiency of Ab-initio total energy calculations for metals and semiconductors using a plane-wave basis set10.1016/0927-0256(96)00008-0 ↗
16. Assessing the performance of recent density functionals for bulk solids10.1103/PhysRevB.79.155107 ↗
17. Generalized gradient approximation made simple10.1103/PhysRevLett.77.3865 ↗
18. DFT+U study of the structures and properties of the actinide dioxides10.1016/j.jnucmat.2017.05.025 ↗
19. Hidden magnetic order in plutonium dioxide nuclear fuel10.1039/C8CP03583K ↗
20. Distributions of phonon lifetimes in brillouin zones10.1103/PhysRevB.91.094306 ↗
21. VESTA 3 for three-dimensional visualization of crystal, volumetric and morphology data10.1107/S0021889811038970 ↗