Challenges in relativistic electronic ...
Type de document :
Autre communication scientifique (congrès sans actes - poster - séminaire...): Communication dans un congrès avec actes: Conférence invitée
Titre :
Challenges in relativistic electronic structure calculations of gas-phase reactivity and thermodynamics of actinide species
Auteur(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]
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]
Titre de la manifestation scientifique :
Plutonium Futures: The Science 2022
Ville :
Avignon
Pays :
France
Date de début de la manifestation scientifique :
2022-09-26
Date de publication :
2022-09-26
Discipline(s) HAL :
Chimie/Chimie théorique et/ou physique
Physique [physics]/Physique [physics]/Chimie-Physique [physics.chem-ph]
Physique [physics]/Physique [physics]/Chimie-Physique [physics.chem-ph]
Résumé en anglais : [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 ...
Lire la suite >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 AnO<sub>2</sub><sup>(V)</sup> sulfinate complexes [(An<sup>V</sup>O<sub>2</sub>)(CH<sub>3</sub>SO<sub>2</sub>)<sub>2</sub>]<sup>-</sup> or [(An<sup>V</sup>O<sub>2</sub>)(C<sub>6</sub>H<sub>5</sub>SO<sub>2</sub>)<sub>2</sub>]<sup>-</sup> 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, PuO<sub>2</sub>, PuO<sub>3</sub>, and PuO<sub>2</sub>(OH)<sub>2</sub>, 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].<br>[1] V. Vallet, Y. Gong, M. Saab, F. Réal, J. K. Gibson, submitted to Dalton Trans.<br>[2] K. Boguslawski, F. Réal, P. Tecmer, C. Duperrouzel, A. S. P. Gomes, Ö. Legeza, P. W. Ayers, and V. Vallet, <i>Phys. Chem. Chem. Phys.</i> <b>19</b>, 4317 (2017)<br>[3] S. Kervazo, F. Réal, F. Virot, A. S. P. Gomes, V. Vallet, <i>Inorg. Chem.</i> <b>58</b>, 14507–14521 (2019).Lire moins >
Lire la suite >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 AnO<sub>2</sub><sup>(V)</sup> sulfinate complexes [(An<sup>V</sup>O<sub>2</sub>)(CH<sub>3</sub>SO<sub>2</sub>)<sub>2</sub>]<sup>-</sup> or [(An<sup>V</sup>O<sub>2</sub>)(C<sub>6</sub>H<sub>5</sub>SO<sub>2</sub>)<sub>2</sub>]<sup>-</sup> 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, PuO<sub>2</sub>, PuO<sub>3</sub>, and PuO<sub>2</sub>(OH)<sub>2</sub>, 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].<br>[1] V. Vallet, Y. Gong, M. Saab, F. Réal, J. K. Gibson, submitted to Dalton Trans.<br>[2] K. Boguslawski, F. Réal, P. Tecmer, C. Duperrouzel, A. S. P. Gomes, Ö. Legeza, P. W. Ayers, and V. Vallet, <i>Phys. Chem. Chem. Phys.</i> <b>19</b>, 4317 (2017)<br>[3] S. Kervazo, F. Réal, F. Virot, A. S. P. Gomes, V. Vallet, <i>Inorg. Chem.</i> <b>58</b>, 14507–14521 (2019).Lire moins >
Langue :
Anglais
Comité de lecture :
Oui
Audience :
Internationale
Vulgarisation :
Non
Projet ANR :
Source :