Challenges in relativistic electronic structure calculations of gas-phase reactivity and thermodynamics of actinide species

Réal, Florent; Vallet, Valérie; Severo Pereira Gomes, Andre; Kervazo, Sophie; Saab, Mohamad; Virot, François; Gong, Yu; Gibson, John K.

Document type :

Autre communication scientifique (congrès sans actes - poster - séminaire...): Communication dans un congrès avec actes: Conférence invitée

Title :

Challenges in relativistic electronic structure calculations of gas-phase reactivity and thermodynamics of actinide species

Author(s) :

Réal, Florent [Orateur]

Physico-Chimie Moléculaire Théorique [PCMT]
Vallet, Valérie [Auteur]

Physico-Chimie Moléculaire Théorique [PCMT]
Severo Pereira Gomes, Andre [Auteur]

Physico-Chimie Moléculaire Théorique [PCMT]
Kervazo, Sophie [Auteur]
Physico-Chimie Moléculaire Théorique [PCMT]
Saab, Mohamad [Auteur]
Physico-Chimie Moléculaire Théorique [PCMT]
Virot, François [Auteur]
Pôle Sûreté Nucléaire - Recherche en sûreté [IRSN/PSN-RES]
Gong, Yu [Auteur]
Chemical Sciences Division [LBNL Berkeley] [CSD]
Gibson, John K. [Auteur]
Chemical Sciences Division [LBNL Berkeley] [CSD]

Conference title :

Plutonium Futures: The Science 2022

City :

Avignon

Country :

France

Start date of the conference :

2022-09-26

Publication date :

2022-09-26

HAL domain(s) :

Chimie/Chimie théorique et/ou physique
Physique [physics]/Physique [physics]/Chimie-Physique [physics.chem-ph]

English abstract : [en]

Probing the electronic structures, reactivity and thermodynamics properties of early actinide (U, Np, Pu) elements is a key fundamental aspect of actinide physical-chemistry, in order to elucidate to which extent their ...
Show more >Probing the electronic structures, reactivity and thermodynamics properties of early actinide (U, Np, Pu) elements is a key fundamental aspect of actinide physical-chemistry, in order to elucidate to which extent their properties differ from one element to the other. When studied in the gas phase, it is possible to probe oxidation states that might not be readily accessible in condensed phase.In this presentation, we will first discuss the reactivity of pentavalent actinyl AnO2(V) sulfinate complexes [(AnVO2)(CH3SO2)2]- or [(AnVO2)(C6H5SO2)2]- to investigate on the one side how Np and Pu complexes might differ from U ones, and on the other side, how the relative strengths of C-S bond in methanesulfinate and benzesulftinate impact the fragmentation pathways. To answer these question, we have confronted the results of collision induced dissociation experiments to relativistic multi-reference electronic structure calculations [1].The second focus will be on the thermodynamics properties of gas-phase volatile plutonium species, PuO2, PuO3, and PuO2(OH)2, in their neutral and ionic forms. We showcase the use of relativistic quantum chemical methods to predict the forms and quantities of the released plutonium species under accidental conditions [2, 3]. [1] V. Vallet, Y. Gong, M. Saab, F. Réal, J. K. Gibson, submitted to Dalton Trans. [2] K. Boguslawski, F. Réal, P. Tecmer, C. Duperrouzel, A. S. P. Gomes, Ö. Legeza, P. W. Ayers, and V. Vallet, Phys. Chem. Chem. Phys. 19, 4317 (2017) [3] S. Kervazo, F. Réal, F. Virot, A. S. P. Gomes, V. Vallet, Inorg. Chem. 58, 14507–14521 (2019).Show less >

Language :

Anglais

Peer reviewed article :

Oui

Audience :

Internationale

Popular science :

Non

ANR Project :

Physiques et Chimie de l'Environnement Atmosphérique
ULNE

Collections :

Laboratoire de Physique des Lasers, Atomes et Molécules (PhLAM) - UMR 8523

Source :

Harvested from HAL

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