Mesoporous hybrid silica-organic materials containing homogeneously distributed stable mono- or dinitroxide radicals covalently bound to the silica surface were developed as polarization matrixes for solid-state dynamic nuclear polarization (DNP) NMR experiments. For TEMPO-containing materials impregnated with water or 1,1,2,2-tetrachloroethane, enhancement factors of up to 36 were obtained at similar to 100 K and 9.4 T without the need for a glass-forming additive. We show that the homogeneous radical distribution and the subtle balance between the concentration of radical in the material and the fraction of radicals at a sufficient inter-radical distance to promote the cross-effect are the main determinants for the DNP enhancements we obtain. The material, as well as an analogue containing the poorly soluble biradical bTUrea, is used as a polarizing matrix for DNP NMR experiments of solutions containing alanine and pyruvic acid. The analyte is separated from the polarization matrix by simple filtration.

Solid-phase polarization matrixes for dynamic nuclear polarization from homogeneously distributed radicals in mesostructured hybrid silica materials / Gajan, David; Schwarzwälder, Martin; Conley, Matthew P.; Grüning, Wolfram R.; Rossini, Aaron J.; Zagdoun, Alexandre; Lelli, Moreno; Yulikov, Maxim; Jeschke, Gunnar; Sauvée, Claire; Ouari, Olivier; Tordo, Paul; Veyre, Laurent; Lesage, Anne; Thieuleux, Chloé; Emsley, Lyndon; Copéret, Christophe. - In: JOURNAL OF THE AMERICAN CHEMICAL SOCIETY. - ISSN 0002-7863. - STAMPA. - 135:(2013), pp. 15459-15466. [10.1021/ja405822h]

Solid-phase polarization matrixes for dynamic nuclear polarization from homogeneously distributed radicals in mesostructured hybrid silica materials

LELLI, MORENO
Investigation
;
2013

Abstract

Mesoporous hybrid silica-organic materials containing homogeneously distributed stable mono- or dinitroxide radicals covalently bound to the silica surface were developed as polarization matrixes for solid-state dynamic nuclear polarization (DNP) NMR experiments. For TEMPO-containing materials impregnated with water or 1,1,2,2-tetrachloroethane, enhancement factors of up to 36 were obtained at similar to 100 K and 9.4 T without the need for a glass-forming additive. We show that the homogeneous radical distribution and the subtle balance between the concentration of radical in the material and the fraction of radicals at a sufficient inter-radical distance to promote the cross-effect are the main determinants for the DNP enhancements we obtain. The material, as well as an analogue containing the poorly soluble biradical bTUrea, is used as a polarizing matrix for DNP NMR experiments of solutions containing alanine and pyruvic acid. The analyte is separated from the polarization matrix by simple filtration.
2013
135
15459
15466
Goal 3: Good health and well-being for people
Gajan, David; Schwarzwälder, Martin; Conley, Matthew P.; Grüning, Wolfram R.; Rossini, Aaron J.; Zagdoun, Alexandre; Lelli, Moreno; Yulikov, Maxim; Jeschke, Gunnar; Sauvée, Claire; Ouari, Olivier; Tordo, Paul; Veyre, Laurent; Lesage, Anne; Thieuleux, Chloé; Emsley, Lyndon; Copéret, Christophe
File in questo prodotto:
File Dimensione Formato  
ja405822h.pdf

Accesso chiuso

Descrizione: Articolo principale
Tipologia: Pdf editoriale (Version of record)
Licenza: Tutti i diritti riservati
Dimensione 487.54 kB
Formato Adobe PDF
487.54 kB Adobe PDF   Richiedi una copia

I documenti in FLORE sono protetti da copyright e tutti i diritti sono riservati, salvo diversa indicazione.

Utilizza questo identificatore per citare o creare un link a questa risorsa: https://hdl.handle.net/2158/1086328
Citazioni
  • ???jsp.display-item.citation.pmc??? ND
  • Scopus 52
  • ???jsp.display-item.citation.isi??? 53
social impact