Titre :

Influence of Gallium Isomorphous Substitution in the Acidic MFI Zeolite Framework on Hole Formation, Transfer, and Trapping upon Incorporation of Anthracene

Auteur(s) :

Moissette, Alain [Auteur]
Laboratoire Avancé de Spectroscopie pour les Intéractions la Réactivité et l'Environnement (LASIRE) - UMR 8516
Lobo, Raul F. [Auteur]
University of Delaware [Newark]
Vezin, Herve [Auteur]
Laboratoire Avancé de Spectroscopie pour les Intéractions la Réactivité et l'Environnement (LASIRE) - UMR 8516
Brémard, Claude [Auteur]
Laboratoire Avancé de Spectroscopie pour les Intéractions la Réactivité et l'Environnement - UMR 8516 [LASIRE]

Titre de la revue :

The Journal of Physical Chemistry C

Nom court de la revue :

J. Phys. Chem. C

Numéro :

115

Pagination :

6635-6643

Éditeur :

American Chemical Society (ACS)

Date de publication :

2011-03-17

Statut de l’article :

Publié

ISSN :

1932-7447

Mot(s)-clé(s) en anglais :

Sorption
Zeolites
Hole transfer
Ionization
Cations

Discipline(s) HAL :

Chimie/Chimie théorique et/ou physique

Résumé en anglais : [en]

The redox behavior of ACENE-3 upon sorption within the channels of Brønsted acidic H-GaZSM-5 is followed by using diffuse reflectance UV−vis−NIR spectrometry in parallel with continuous wave EPR techniques and with Raman ...
Lire la suite >The redox behavior of ACENE-3 upon sorption within the channels of Brønsted acidic H-GaZSM-5 is followed by using diffuse reflectance UV−vis−NIR spectrometry in parallel with continuous wave EPR techniques and with Raman spectrometry. Partial spontaneous ionization is clearly observed, whereas proton transfer does not occur. The intense internal proton electrostatic field, as well as the confinement effect on the occluded molecule, are put forward to explain charge separation and the long-lived ACENE-3•+ radical cation. The compartmentalization of ACENE-3•+ and trapped electron within H-GaZSM-5 hinders charge recombination but promotes hole transfer to the inner surface of the 10-membered ring (10-MR) channel. Pulsed X-band EPR experiments using the 2D-HYSCORE sequence were carried out to investigate the structural surrounding of unpaired electrons. The observation of electron couplings with 1H, 29Si, 69Ga, and 71Ga nuclei allows clear differentiation between the two successive charge separated states. The present results for H-GaZSM-5 are compared to previous analogous experiments conducted on H-AlZSM-5 for which hole transfer from the ACENE-3 organic molecule to the silicoaluminate framework was not observed at room temperature after the ACENE-3 spontaneous ionization in H-AlZSM-5. The hole transfer ΔG0 is the key parameter in the nonadiabatic electron-transfer theory that explains the hole transfer at room temperature within H-GaZSM-5 and not within H-AlZSM-5.Lire moins >

Langue :

Anglais

Audience :

Internationale

Vulgarisation :

Non

Établissement(s) :

Université de Lille
CNRS

Collections :

• Laboratoire Avancé de Spectroscopie pour les Intéractions la Réactivité et l'Environnement (LASIRE) - UMR 8516

Date de dépôt :

2021-06-18T08:11:25Z
2021-10-08T12:37:24Z