title: Gas-Phase Reactivity of Cesium-Containing Species by Quantum Chemistry.
abstract: Thermodynamics and kinetics of cesium species reactions have been studied by using high-level quantum chemical tools. A systematic theoretical study has been done to find suitable methodology for calculation of reliable thermodynamic properties, allowing us to determine bimolecular rate constants with appropriate kinetic theories of gas-phase reactions. Four different reactions have been studied in this work: CsO + H2 = CsOH + H (R1), Cs + HI = CsI + H (R2), CsI + H2O = CsOH + HI (R3), and CsI + OH = CsOH + I (R4). All reactions involve steam, hydrogen, and iodine in addition of cesium. Most of the reactions are fast and (R3) and (R4) proceed even without energetic barrier. In terms of chemical reactivity in the reactor coolant system (RCS) in the case of severe accident, it can be expected that there will be no kinetic limitations for main cesium species (CsOH and CsI) transported along the RCS. Cs chemical speciation inside the RCS should be governed by the thermodynamics.
authors.affiliation: Institut de Radioprotection et de Sûreté Nucléaire (IRSN), PSN-RES, SAG, LETR, St Paul Lez Durance 13115, France.
authors.forename: Katarína
authors.initials: K
authors.lastname: Šulková
authors.affiliation: Institut de Radioprotection et de Sûreté Nucléaire (IRSN), PSN-RES, SAG, LETR, St Paul Lez Durance 13115, France.|Laboratoire de Recherche Commun IRSN-CNRS-Lille1 "Cinétique Chimique, Combustion, Réactivité" (C3R), Centre de Cadarache, BP3, St Paul Lez Durance 13115, France.
authors.forename: Laurent
authors.initials: L
authors.lastname: Cantrel
authors.affiliation: PhysicoChimie des Processus de Combustion et de l'Atmosphère (PC2A), UMR CNRS 8522, Université Lille 1 Sciences et Technologies, 59655 Villeneuve d'Ascq Cedex, France.|Laboratoire de Recherche Commun IRSN-CNRS-Lille1 "Cinétique Chimique, Combustion, Réactivité" (C3R), Centre de Cadarache, BP3, St Paul Lez Durance 13115, France.
authors.forename: Florent
authors.initials: F
authors.lastname: Louis
mesh_terms: D002586:Cesium / Q000737:chemistry*; D007700:Kinetics; D011789:Quantum Theory; D013816:Thermodynamics
chemical_list: D002586:Cesium