Probing functionalities and acidity of ...
Document type :
Article dans une revue scientifique: Article original
DOI :
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Title :
Probing functionalities and acidity of calcined phenylene-bridged periodic mesoporous organosilicates using dynamic nuclear polarization nmr, diffuse reflectance infrared fourier transform spectroscopy, and x-ray photoelectron spectroscopy
Author(s) :
Pirez, Cyril [Auteur]
Unité de Catalyse et Chimie du Solide - UMR 8181 [UCCS]
Nagashima, Hiroki [Auteur]
National Institute of Advanced Industrial Science and Technology [AIST]
Unité de Catalyse et Chimie du Solide - UMR 8181 [UCCS]
Dumeignil, Franck [Auteur]
Unité de Catalyse et Chimie du Solide (UCCS) - UMR 8181
Lafon, Olivier [Auteur]
Unité de Catalyse et Chimie du Solide (UCCS) - UMR 8181
Pirez, Cyril [Auteur]
Unité de Catalyse et Chimie du Solide - UMR 8181 [UCCS]
Nagashima, Hiroki [Auteur]
National Institute of Advanced Industrial Science and Technology [AIST]
Unité de Catalyse et Chimie du Solide - UMR 8181 [UCCS]
Dumeignil, Franck [Auteur]
Unité de Catalyse et Chimie du Solide (UCCS) - UMR 8181
Lafon, Olivier [Auteur]
Unité de Catalyse et Chimie du Solide (UCCS) - UMR 8181
Pirez, Cyril [Auteur]
Journal title :
Journal of Physical Chemistry C
Abbreviated title :
J. Phys. Chem. C
Volume number :
124
Pages :
6110-6120
Publication date :
2020-03-19
ISSN :
1932-7447
English keyword(s) :
periodic mesoporous organosilica
calcination
solid-state NMR
DNP
DRIFTS
XPS
calcination
solid-state NMR
DNP
DRIFTS
XPS
HAL domain(s) :
Chimie/Catalyse
English abstract : [en]
Owing to their high surface area, their high stability, and their hydrophobicity, periodic mesoporous organosilica (PMO) materials represent promising catalytic support for environmentally friendly chemical processes in ...
Show more >Owing to their high surface area, their high stability, and their hydrophobicity, periodic mesoporous organosilica (PMO) materials represent promising catalytic support for environmentally friendly chemical processes in water. We investigate here how the calcination of PMO material with benzene linkers (PMOB) allows its functionalization. Conventional and dynamic nuclear polarization (DNP)-enhanced NMR spectroscopy, diffuse reflectance infrared Fourier transform spectroscopy, and X-ray photoelectron spectroscopy prove that calcination at 450 °C results in the oxidation of phenylene bridges into (poly)phenols but also into carboxylic acids. Ketone, aldehyde, as well as allyl and aliphatic alcohol functionalities are also observed, but their amount is much lower than that of carboxylic acids. The calcination also cleaves the Si–C bonds. Nevertheless, N2 adsorption–desorption measurements, powder X-ray diffraction, and transmission electron microscopy indicate that the PMOB materials calcined up to 600 °C still exhibit ordered mesopores. We show that the phenol and carboxylic acid functionalities of PMOB calcined at 450 °C protonate the NH2 group of 1-(3-aminopropyl)imidazole (API) in water at room temperature, but no formation of a covalent bond between API and the calcined PMOB functionalities has been detected.Show less >
Show more >Owing to their high surface area, their high stability, and their hydrophobicity, periodic mesoporous organosilica (PMO) materials represent promising catalytic support for environmentally friendly chemical processes in water. We investigate here how the calcination of PMO material with benzene linkers (PMOB) allows its functionalization. Conventional and dynamic nuclear polarization (DNP)-enhanced NMR spectroscopy, diffuse reflectance infrared Fourier transform spectroscopy, and X-ray photoelectron spectroscopy prove that calcination at 450 °C results in the oxidation of phenylene bridges into (poly)phenols but also into carboxylic acids. Ketone, aldehyde, as well as allyl and aliphatic alcohol functionalities are also observed, but their amount is much lower than that of carboxylic acids. The calcination also cleaves the Si–C bonds. Nevertheless, N2 adsorption–desorption measurements, powder X-ray diffraction, and transmission electron microscopy indicate that the PMOB materials calcined up to 600 °C still exhibit ordered mesopores. We show that the phenol and carboxylic acid functionalities of PMOB calcined at 450 °C protonate the NH2 group of 1-(3-aminopropyl)imidazole (API) in water at room temperature, but no formation of a covalent bond between API and the calcined PMOB functionalities has been detected.Show less >
Language :
Anglais
Peer reviewed article :
Oui
Audience :
Internationale
Popular science :
Non
Administrative institution(s) :
CNRS
Centrale Lille
ENSCL
Univ. Artois
Université de Lille
Centrale Lille
ENSCL
Univ. Artois
Université de Lille
Collections :
Research team(s) :
RMN et matériaux inorganiques (RM2I)
Valorisation des alcanes et de la biomasse (VAALBIO)
Valorisation des alcanes et de la biomasse (VAALBIO)
Submission date :
2022-03-02T07:13:22Z
2023-10-20T08:02:27Z
2023-11-08T18:58:31Z
2023-11-24T14:56:16Z
2023-10-20T08:02:27Z
2023-11-08T18:58:31Z
2023-11-24T14:56:16Z
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