Analysis of sensitivity enhancement by ...
Type de document :
Article dans une revue scientifique: Article original
DOI :
URL permanente :
Titre :
Analysis of sensitivity enhancement by dynamic nuclear polarization in solid-state NMR: a case study of functionalized mesoporous materials
Auteur(s) :
Kobayashi, Takeshi [Auteur]
Lafon, Olivier [Auteur]
Unité de Catalyse et de Chimie du Solide (UCCS) - UMR 8181
Lilly Thankamony, Aany S. [Auteur]
Unité de Catalyse et Chimie du Solide - UMR 8181 [UCCS]
Slowing, Igor I. [Auteur]
Kandel, Kapil [Auteur]
Carnevale, Diego [Auteur]
Vitzthum, Veronika [Auteur]
Vezin, Herve [Auteur]
Laboratoire Avancé de Spectroscopie pour les Intéractions la Réactivité et l'Environnement (LASIRE) - UMR 8516
Amoureux, Jean-Paul [Auteur]
Unité de Catalyse et de Chimie du Solide (UCCS) - UMR 8181
Bodenhausen, Geoffrey [Auteur]
Pruski, Marek [Auteur]
Lafon, Olivier [Auteur]
Unité de Catalyse et de Chimie du Solide (UCCS) - UMR 8181
Lilly Thankamony, Aany S. [Auteur]
Unité de Catalyse et Chimie du Solide - UMR 8181 [UCCS]
Slowing, Igor I. [Auteur]
Kandel, Kapil [Auteur]
Carnevale, Diego [Auteur]
Vitzthum, Veronika [Auteur]
Vezin, Herve [Auteur]
Laboratoire Avancé de Spectroscopie pour les Intéractions la Réactivité et l'Environnement (LASIRE) - UMR 8516
Amoureux, Jean-Paul [Auteur]
Unité de Catalyse et de Chimie du Solide (UCCS) - UMR 8181
Bodenhausen, Geoffrey [Auteur]
Pruski, Marek [Auteur]
Titre de la revue :
Physical Chemistry Chemical Physics
Nom court de la revue :
Phys. Chem. Chem. Phys.
Numéro :
15
Pagination :
5553
Éditeur :
Royal Society of Chemistry (RSC)
Date de publication :
2013-02-01
ISSN :
1463-9076
Discipline(s) HAL :
Chimie/Chimie théorique et/ou physique
Chimie/Chimie organique
Chimie/Chimie organique
Résumé en anglais : [en]
We systematically studied the enhancement factor (per scan) and the sensitivity enhancement (per unit time) in 13C and 29Si cross-polarization magic angle spinning (CP-MAS) NMR boosted by dynamic nuclear polarization (DNP) ...
Lire la suite >We systematically studied the enhancement factor (per scan) and the sensitivity enhancement (per unit time) in 13C and 29Si cross-polarization magic angle spinning (CP-MAS) NMR boosted by dynamic nuclear polarization (DNP) of functionalized mesoporous silica nanoparticles (MSNs). Specifically, we separated contributions due to: (i) microwave irradiation, (ii) quenching by paramagnetic effects, (iii) the presence of frozen solvent, (iv) the temperature, as well as changes in (v) relaxation and (vi) cross-polarization behaviour. No line-broadening effects were observed for MSNs when lowering the temperature from 300 to 100 K. Notwithstanding a significant signal reduction due to quenching by TOTAPOL radicals, DNP-CP-MAS at 100 K provided global sensitivity enhancements of 23 and 45 for 13C and 29Si, respectively, relative to standard CP-MAS measurements at room temperature. The effects of DNP were also ascertained by comparing with state-of-the-art two-dimensional heteronuclear 1H{13C} and 29Si{1H} correlation spectra, using, respectively, indirect detection or Carr–Purcell–Meiboom–Gill (CPMG) refocusing to boost signal acquisition. This study highlights opportunities for further improvements through the development of high-field DNP, better polarizing agents, and improved capabilities for low-temperature MAS.Lire moins >
Lire la suite >We systematically studied the enhancement factor (per scan) and the sensitivity enhancement (per unit time) in 13C and 29Si cross-polarization magic angle spinning (CP-MAS) NMR boosted by dynamic nuclear polarization (DNP) of functionalized mesoporous silica nanoparticles (MSNs). Specifically, we separated contributions due to: (i) microwave irradiation, (ii) quenching by paramagnetic effects, (iii) the presence of frozen solvent, (iv) the temperature, as well as changes in (v) relaxation and (vi) cross-polarization behaviour. No line-broadening effects were observed for MSNs when lowering the temperature from 300 to 100 K. Notwithstanding a significant signal reduction due to quenching by TOTAPOL radicals, DNP-CP-MAS at 100 K provided global sensitivity enhancements of 23 and 45 for 13C and 29Si, respectively, relative to standard CP-MAS measurements at room temperature. The effects of DNP were also ascertained by comparing with state-of-the-art two-dimensional heteronuclear 1H{13C} and 29Si{1H} correlation spectra, using, respectively, indirect detection or Carr–Purcell–Meiboom–Gill (CPMG) refocusing to boost signal acquisition. This study highlights opportunities for further improvements through the development of high-field DNP, better polarizing agents, and improved capabilities for low-temperature MAS.Lire moins >
Langue :
Anglais
Comité de lecture :
Oui
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 :
2021-06-17T14:31:21Z
2021-10-06T16:32:46Z
2021-10-06T16:32:46Z