title: Performance of CuII-, PbII-, and HgII-Exchanged Mordenite in the Adsorption of I2, ICH3, H2O, CO, ClCH3, and Cl2: A Density Functional Study.
abstract: Periodic dispersion-corrected DFT is used to investigate the adsorption of I2and ICH3, which may be released during a severe nuclear accident, for three divalent cation (Cu2+, Pb2+and Hg2+)-exchanged mordenites with an Si/Al ratio of 23. Gases such as H2O, CO, ClCH3, and Cl2present in the containment atmosphere can inhibit the selective adsorption of iodine species. To identify the most promising adsorbents, a systematic study is performed in which all the possible cationic sites in the main channel of the mordenite structure are considered. For the energetically most stable sites, the divalent cation is located in the small rings (five- or six-membered) containing two Al atoms, while in the energetically less stable configurations, the two Al atoms are far apart (>7 Å) and the cation is close to only one Al atom. Upon adsorption of the various molecules, the coordination number of the cation decreases with increasing interaction energy, as the molecules can attract the divalent cations from the framework. Finally, the computed interaction energies show that Hg-mordenite (MOR) could be a suitable material for selective adsorption of volatile iodine species, contrary to Cu-MOR and Pb-MOR.
authors.affiliation: Laboratoire de Chimie et Physique-Approche Multi-Echelle des Milieux Complexes (LCP-A2MC, EA4632), Institut Jean Barriol FR2843 CNRS, Université de Lorraine, Rue Victor Demange, 57500, Saint-Avold, France.
authors.forename: Siwar
authors.initials: S
authors.lastname: Chibani
authors.affiliation: Laboratoire de Chimie et Physique-Approche Multi-Echelle des Milieux Complexes (LCP-A2MC, EA4632), Institut Jean Barriol FR2843 CNRS, Université de Lorraine, Rue Victor Demange, 57500, Saint-Avold, France.
authors.forename: Israa
authors.initials: I
authors.lastname: Medlej
authors.affiliation: Laboratoire de Cristallographie, Résonance Magnétique et Modélisations (CRM2, UMR CNRS 7036), Institut Jean Barriol, Université de Lorraine, BP 239, Boulevard des Aiguillettes, 54506, Vandœuvre-lès-Nancy-Cedex, France.
authors.forename: Sébastien
authors.initials: S
authors.lastname: Lebègue
authors.affiliation: Laboratoire de Cristallographie, Résonance Magnétique et Modélisations (CRM2, UMR CNRS 7036), Institut Jean Barriol, Université de Lorraine, BP 239, Boulevard des Aiguillettes, 54506, Vandœuvre-lès-Nancy-Cedex, France.
authors.forename: János G
authors.initials: JG
authors.lastname: Ángyán
authors.affiliation: Institut de Radioprotection et de Sûreté Nucléaire (IRSN), PSN-RES, Saint-Paul Lez Durance, 13115, France.
authors.forename: Laurent
authors.initials: L
authors.lastname: Cantrel
authors.affiliation: Laboratoire de Chimie et Physique-Approche Multi-Echelle des Milieux Complexes (LCP-A2MC, EA4632), Institut Jean Barriol FR2843 CNRS, Université de Lorraine, Rue Victor Demange, 57500, Saint-Avold, France.
authors.forename: Michael
authors.identifier: http://orcid.org/0000-0002-3504-4180
authors.initials: M
authors.lastname: Badawi
keywords: adsorption; density functional calculations; iodine; mercury; zeolites