Capture of Gaseous Iodine in Isoreticular ...
Type de document :
Article dans une revue scientifique: Article original
DOI :
URL permanente :
Titre :
Capture of Gaseous Iodine in Isoreticular Zirconium‐Based UiO‐n Metal‐Organic Frameworks: Influence of Amino Functionalization, DFT Calculations, Raman and EPR Spectroscopic Investigation
Auteur(s) :
Leloire, Maeva [Auteur]
Unité de Catalyse et de Chimie du Solide (UCCS) - UMR 8181
Walshe, Catherine [Auteur]
Unité de Catalyse et Chimie du Solide - UMR 8181 [UCCS]
Devaux, Philippe [Auteur]
Unité de Catalyse et Chimie du Solide (UCCS) - UMR 8181
Giovine, Raynald [Auteur]
Unité de Catalyse et Chimie du Solide - UMR 8181 [UCCS]
Duval, Sylvain [Auteur]
Unité de Catalyse et Chimie du Solide (UCCS) - UMR 8181
Bousquet, Till [Auteur]
Unité de Catalyse et Chimie du Solide (UCCS) - UMR 8181
Chibani, Siwar [Auteur]
Unité de Catalyse et Chimie du Solide - UMR 8181 [UCCS]
Paul, Jean-Francois [Auteur]
Unité de Catalyse et Chimie du Solide (UCCS) - UMR 8181
Moissette, Alain [Auteur]
Laboratoire Avancé de Spectroscopie pour les Intéractions la Réactivité et l'Environnement (LASIRE) - UMR 8516
Vezin, Herve [Auteur]
Laboratoire Avancé de Spectroscopie pour les Intéractions la Réactivité et l'Environnement - UMR 8516 [LASIRE]
Nerisson, Philippe [Auteur]
Cantrel, Laurent [Auteur]
Volkringer, Christophe [Auteur]
Unité de Catalyse et Chimie du Solide (UCCS) - UMR 8181
Loiseau, Thierry [Auteur]
Unité de Catalyse et Chimie du Solide (UCCS) - UMR 8181
Unité de Catalyse et de Chimie du Solide (UCCS) - UMR 8181
Walshe, Catherine [Auteur]
Unité de Catalyse et Chimie du Solide - UMR 8181 [UCCS]
Devaux, Philippe [Auteur]
Unité de Catalyse et Chimie du Solide (UCCS) - UMR 8181
Giovine, Raynald [Auteur]
Unité de Catalyse et Chimie du Solide - UMR 8181 [UCCS]
Duval, Sylvain [Auteur]
Unité de Catalyse et Chimie du Solide (UCCS) - UMR 8181
Bousquet, Till [Auteur]
Unité de Catalyse et Chimie du Solide (UCCS) - UMR 8181
Chibani, Siwar [Auteur]
Unité de Catalyse et Chimie du Solide - UMR 8181 [UCCS]
Paul, Jean-Francois [Auteur]
Unité de Catalyse et Chimie du Solide (UCCS) - UMR 8181
Moissette, Alain [Auteur]
Laboratoire Avancé de Spectroscopie pour les Intéractions la Réactivité et l'Environnement (LASIRE) - UMR 8516
Vezin, Herve [Auteur]
Laboratoire Avancé de Spectroscopie pour les Intéractions la Réactivité et l'Environnement - UMR 8516 [LASIRE]
Nerisson, Philippe [Auteur]
Cantrel, Laurent [Auteur]
Volkringer, Christophe [Auteur]
Unité de Catalyse et Chimie du Solide (UCCS) - UMR 8181
Loiseau, Thierry [Auteur]
Unité de Catalyse et Chimie du Solide (UCCS) - UMR 8181
Titre de la revue :
Chemistry – A European Journal
Nom court de la revue :
Chemistry A European J
Éditeur :
Wiley
Date de publication :
2022-02-10
ISSN :
0947-6539
Mot(s)-clé(s) en anglais :
DFT calculations
EPR spectroscopy
gaseous iodine adsorption
kinetics
Raman spectroscopy
UiO-n MOF materials
EPR spectroscopy
gaseous iodine adsorption
kinetics
Raman spectroscopy
UiO-n MOF materials
Discipline(s) HAL :
Chimie
Résumé en anglais : [en]
A series of Zr-based UiO-n MOF materials (n=66, 67, 68) have been studied for iodine capture. Gaseous iodine adsorption was collected kinetically from a home-made set-up allowing the continuous measurement of iodine content ...
Lire la suite >A series of Zr-based UiO-n MOF materials (n=66, 67, 68) have been studied for iodine capture. Gaseous iodine adsorption was collected kinetically from a home-made set-up allowing the continuous measurement of iodine content trapped within UiO-n compounds, with organic functionalities (−H, −CH3, −Cl, −Br, −(OH)2, −NO2, −NH2, (−NH2)2, −CH2 NH2) by in-situ UV-Vis spectroscopy. This study emphasizes the role of the amino groups attached to the aromatic rings of the ligands connecting the {Zr6O4(OH)4} brick. In particular, the preferential interaction of iodine with lone-pair groups, such as amino functions, has been experimentally observed and is also based on DFT calculations. Indeed, higher iodine contents were systematically measured for amino-functionalized UiO-66 or UiO-67, compared to the pristine material (up to 1211 mg/g for UiO-67-(NH2)2). However, DFT calculations revealed the highest computed interaction energies for alkylamine groups (−CH2NH2) in UiO-67 (−128.5 kJ/mol for the octahedral cavity), and pointed out the influence of this specific functionality compared with that of an aromatic amine. The encapsulation of iodine within the pore system of UiO-n materials and their amino-derivatives has been analyzed by UV-Vis and Raman spectroscopy. We showed that a systematic conversion of molecular iodine (I2) species into anionic I− ones, stabilized as I−⋅⋅⋅I2 or I3− complexes within the MOF cavities, occurs when I2@UiO-n samples are left in ambient light.Lire moins >
Lire la suite >A series of Zr-based UiO-n MOF materials (n=66, 67, 68) have been studied for iodine capture. Gaseous iodine adsorption was collected kinetically from a home-made set-up allowing the continuous measurement of iodine content trapped within UiO-n compounds, with organic functionalities (−H, −CH3, −Cl, −Br, −(OH)2, −NO2, −NH2, (−NH2)2, −CH2 NH2) by in-situ UV-Vis spectroscopy. This study emphasizes the role of the amino groups attached to the aromatic rings of the ligands connecting the {Zr6O4(OH)4} brick. In particular, the preferential interaction of iodine with lone-pair groups, such as amino functions, has been experimentally observed and is also based on DFT calculations. Indeed, higher iodine contents were systematically measured for amino-functionalized UiO-66 or UiO-67, compared to the pristine material (up to 1211 mg/g for UiO-67-(NH2)2). However, DFT calculations revealed the highest computed interaction energies for alkylamine groups (−CH2NH2) in UiO-67 (−128.5 kJ/mol for the octahedral cavity), and pointed out the influence of this specific functionality compared with that of an aromatic amine. The encapsulation of iodine within the pore system of UiO-n materials and their amino-derivatives has been analyzed by UV-Vis and Raman spectroscopy. We showed that a systematic conversion of molecular iodine (I2) species into anionic I− ones, stabilized as I−⋅⋅⋅I2 or I3− complexes within the MOF cavities, occurs when I2@UiO-n samples are left in ambient light.Lire moins >
Langue :
Anglais
Audience :
Internationale
Vulgarisation :
Non
Établissement(s) :
Université de Lille
CNRS
CNRS
Collections :
Équipe(s) de recherche :
Propriétés magnéto structurales des matériaux (PMSM)
Date de dépôt :
2022-03-03T07:04:30Z
2022-03-04T09:36:51Z
2022-03-04T09:36:51Z
Fichiers
- Chemistry A European J - 2022 - Leloire - Capture of Gaseous Iodine in Isoreticular Zirconium%u2010Based UiO%u2010n Metal%u2010Organic.pdf
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