Caveat on the actual robustness of ...
Type de document :
Article dans une revue scientifique: Article original
DOI :
URL permanente :
Titre :
Caveat on the actual robustness of heteronuclear nmr methods for probing the surface of gamma-alumina and related catalysts
Auteur(s) :
Szeto, Kai C. [Auteur]
Merle, Nicolas [Auteur]
Unité de Catalyse et Chimie du Solide (UCCS) - UMR 8181
Trebosc, Julien [Auteur]
Unité de Catalyse et Chimie du Solide (UCCS) - UMR 8181
Taoufik, Mostafa [Auteur]
Gauvin, Regis [Auteur]
Unité de Catalyse et de Chimie du Solide (UCCS) - UMR 8181
Pourpoint, Frederique [Auteur]
Unité de Catalyse et Chimie du Solide (UCCS) - UMR 8181
Delevoye, Laurent [Auteur]
Unité de Catalyse et Chimie du Solide (UCCS) - UMR 8181
Merle, Nicolas [Auteur]

Unité de Catalyse et Chimie du Solide (UCCS) - UMR 8181
Trebosc, Julien [Auteur]

Unité de Catalyse et Chimie du Solide (UCCS) - UMR 8181
Taoufik, Mostafa [Auteur]
Gauvin, Regis [Auteur]

Unité de Catalyse et de Chimie du Solide (UCCS) - UMR 8181
Pourpoint, Frederique [Auteur]

Unité de Catalyse et Chimie du Solide (UCCS) - UMR 8181
Delevoye, Laurent [Auteur]

Unité de Catalyse et Chimie du Solide (UCCS) - UMR 8181
Titre de la revue :
The journal of physical chemistry. C, Nanomaterials and interfaces
Nom court de la revue :
J. Phys. Chem. C
Numéro :
123
Pagination :
12919-12927
Date de publication :
2019-05-23
ISSN :
1932-7447
Discipline(s) HAL :
Chimie/Catalyse
Chimie/Chimie inorganique
Chimie/Chimie inorganique
Résumé en anglais : [en]
Transitional aluminas are a very important class of materials in catalysis. The detailed understanding of their surface chemistry has attracted much attention with input from spectroscopic and theoretical studies. In this ...
Lire la suite >Transitional aluminas are a very important class of materials in catalysis. The detailed understanding of their surface chemistry has attracted much attention with input from spectroscopic and theoretical studies. In this context, NMR is a key technique, which, thanks to recent methodological developments, provides insights into local structures and relative arrangements. In the present paper, we first assess two 1 H− 27 Al heteronuclear correlation NMR methods for studying the surface of γ-Al 2 O 3 dehydroxylated at 500°C. The commonly used cross-polarization (CP) transfer method is compared to the dipolar heteronuclear multiple quantum coherence (D-HMQC) experiment, revealing that the latter is significantly more robust and efficient with less signal distortion that hampers the recording of meaningful signals. Furthermore, a new MQ-D-HMQC pulse sequence is proposed to confirm the presence of sites, with a large quadrupolar coupling constant at the surface of alumina. The robustness of D-HMQC is further probed by two additional alumina-based catalysts, namely, aluminum hydrides supported on γ-Al 2 O 3 , which are active in olefin hydrogenation and polymerization, and ZrCp 2 Me 2 grafted onto γ-Al 2 O 3 , a single-site olefin polymerization catalyst. In both cases, this provides information on the configuration of surface aluminum species in the vicinity of catalytically active sites and on the residual hydroxyl networks. The present study combines advanced NMR methods and complex catalytic materials for which a critical, yet fruitful, spectroscopic approach is required for deeper understanding.Lire moins >
Lire la suite >Transitional aluminas are a very important class of materials in catalysis. The detailed understanding of their surface chemistry has attracted much attention with input from spectroscopic and theoretical studies. In this context, NMR is a key technique, which, thanks to recent methodological developments, provides insights into local structures and relative arrangements. In the present paper, we first assess two 1 H− 27 Al heteronuclear correlation NMR methods for studying the surface of γ-Al 2 O 3 dehydroxylated at 500°C. The commonly used cross-polarization (CP) transfer method is compared to the dipolar heteronuclear multiple quantum coherence (D-HMQC) experiment, revealing that the latter is significantly more robust and efficient with less signal distortion that hampers the recording of meaningful signals. Furthermore, a new MQ-D-HMQC pulse sequence is proposed to confirm the presence of sites, with a large quadrupolar coupling constant at the surface of alumina. The robustness of D-HMQC is further probed by two additional alumina-based catalysts, namely, aluminum hydrides supported on γ-Al 2 O 3 , which are active in olefin hydrogenation and polymerization, and ZrCp 2 Me 2 grafted onto γ-Al 2 O 3 , a single-site olefin polymerization catalyst. In both cases, this provides information on the configuration of surface aluminum species in the vicinity of catalytically active sites and on the residual hydroxyl networks. The present study combines advanced NMR methods and complex catalytic materials for which a critical, yet fruitful, spectroscopic approach is required for deeper understanding.Lire moins >
Langue :
Anglais
Audience :
Internationale
Vulgarisation :
Non
Établissement(s) :
CNRS
Centrale Lille
ENSCL
Univ. Artois
Université de Lille
Centrale Lille
ENSCL
Univ. Artois
Université de Lille
Collections :
Équipe(s) de recherche :
Catalyse et synthèse éco-compatible (CASECO)
RMN et matériaux inorganiques (RM2I)
RMN et matériaux inorganiques (RM2I)
Date de dépôt :
2022-03-02T07:13:23Z
2023-12-15T19:26:20Z
2023-12-15T19:26:20Z
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