Effect of ligands on Pa5+ and PaO3+ relative stabilities: A computational study

Shaaban, Tamara; Vallet, Valérie; Réal, Florent; Maurice, Rémi

Document type :

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

Title :

Effect of ligands on Pa5+ and PaO3+ relative stabilities: A computational study

Author(s) :

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

Physico-Chimie Moléculaire Théorique [PCMT]
Réal, Florent [Auteur]

Physico-Chimie Moléculaire Théorique [PCMT]
Maurice, Rémi [Auteur]
Institut des Sciences Chimiques de Rennes [ISCR]

Conference title :

53rd Journées des Actinides international conference

City :

Lille

Country :

France

Start date of the conference :

2024-04-15

Publication date :

2024-04-15

HAL domain(s) :

Chimie/Chimie théorique et/ou physique

English abstract : [en]

The physical and chemical properties of solvated actinide complexes, including their speciation, bond nature with the surrounding environment, and thermodynamics and spectroscopic properties, hold significant implications ...
Show more >The physical and chemical properties of solvated actinide complexes, including their speciation, bond nature with the surrounding environment, and thermodynamics and spectroscopic properties, hold significant implications for societal and industrial applications. The coordination of the actinides with ligands [1] affects these properties. Researchers, both experimental and theoretical, are interested in the coordination and properties exhibited by the f-elements with ligands. Among the actinides, protactinium (Z=91) keeps on being specific because, depending on its oxidation state it can behave as ‘’f element” (Pa(VI)) or “d element” (Pa(V)). In solution, Pa(V) is dominating because Pa(IV) is unstable and can be directly oxidized to Pa(V) unless a strong reducing agent is present [2]. Pa(V) can exist in solution as Pa5+ and in some specific solutions it will form PaO3+ [3], but apparently it does not form the actinyl moiety PaO2+ which is not the case of their heavier neighbour’s uranium, neptunium and plutonium. In this work, with the use of the state-of-the-art quantum calculations, we investigate the two possible forms of Pa(V), namely PaO3+ and Pa5+ and the influence of coordinated ligands in order to determine the suitable experimental conditions to tune their relative stability. For that we consider two different stoichiometrically equivalent complexes PaO(OH)2(X)(H2O) and Pa(OH)4(X) where X=OH- , F- (see Fig. 1), Cl-, Br-, I-, NO3-, NCS-, C2O42- and SO42- and compare their relative stabilities [4]. It was supported by grants funded the French National Agency for Research (ANR-21-CE29-0027, LABEX CaPPA/ANR-11-LABX-0005-01 and I-SITE ULNE/ANR-16-IDEX-0004 ULNE). References [1]K. Binnemans et al., Chem. Rev., 107, 2592 (2007). (DOI: 10.1021/cr050979c) [2]N. Banik et al., Dalton Trans., 45, 453 (2016). (DOI: 10.1039/C5DT03560K) [3]C. Le Naour et al., Inorg. Chem., 44, 9542 (2005). (DOI: 10.1021/ic0512330) [4]T. Shaaban et al, Chemistry - A Eur. Journal, In press (2024). (DOI: 10.1002/chem.202304068)Show less >

Language :

Anglais

Peer reviewed article :

Oui

Audience :

Internationale

Popular science :

Non

ANR Project :

Chimie, spectroscopie et spéciation du protactinium
Physiques et Chimie de l'Environnement Atmosphérique
ULNE

Collections :

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

Source :

Harvested from HAL

Effect of ligands on Pa<sup>5+</sup> and ... BibTeX CSV Excel RIS

Effect of ligands on Pa<sup>5+</sup> and ...

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