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Article Dans Une Revue Journal of Physical Chemistry A Année : 2023

Irradiation of plutonium tributyl phosphate complexes by ionizing alpha particles: a computational study

Résumé

The PUREX solvent extraction process is widely used for recovering uranium and plutonium from spent nuclear fuel, it uses an organic solvent made up of TriButyl Phosphate (TBP). The emission of ionizing particles such as alpha particles, result- ing from the decay of plutonium, make the organic solvent vulnerable to degradation. Here, we study the ultra-short time alpha irradiation of tributylphosphate (TBP) and Pu(NO3)4(TBP)2 complex formed in the PUREX process. Electron dynamics is prop- agated by Real-Time Time-Dependent Auxiliary Density Functional Theory (RT-TD- ADFT). We investigate the use of previously proposed Complex Absorbing Potentiel (CAP) in energy space to treat secondary electron emission. Basis set and exchange correlation functionals effects with CAP are reported as well as a detailed analysis of the CAP parametrisation. Preliminary results on water molecule and then on TBP show that the phenomenological nature of the CAP parameters induces an adapted choice of their values for each studied system. Irradiation of free and complexed TBP shows an influence of the ligands in the variation of atomic charges at the femtosecond time scale. An accumulation of atomic charges in the alkyl chains of TBP is observed in the case where the nitrate groups are predominantly irradiated.
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Dates et versions

cea-04662956 , version 1 (26-07-2024)

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Damien Tolu, Dominique Guillaumont, Aurélien de la Lande. Irradiation of plutonium tributyl phosphate complexes by ionizing alpha particles: a computational study. Journal of Physical Chemistry A, 2023, 127 (34), pp.7045. ⟨10.1021/acs.jpca.3c02117⟩. ⟨cea-04662956⟩
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