Solid-state NMR of a paramagnetic DIAD-FeII catalyst: Sensitivity, resolution enhancement, and structure-based assignments

Gwendal Kervern; Guido Pintacuda; Yong Zhang; Eric Oldfield; Charbel Roukoss; Emile Kuntz; Eberhardt Herdtweck; Jean Marie Basset; Sylvian Cadars; Anne Lesage; Christophe Copéret; Lyndon Emsley

doi:10.1021/ja063510n

Solid-state NMR of a paramagnetic DIAD-Fe^II catalyst: Sensitivity, resolution enhancement, and structure-based assignments

Gwendal Kervern, Guido Pintacuda, Yong Zhang, Eric Oldfield, Charbel Roukoss, Emile Kuntz, Eberhardt Herdtweck, Jean Marie Basset, Sylvian Cadars, Anne Lesage, Christophe Copéret, Lyndon Emsley^*

^*Corresponding author for this work

Research output: Contribution to journal › Article › peer-review

103 Scopus citations

Abstract

A general protocol for the structural characterization of paramagnetic molecular solids using solid-state NMR is provided and illustrated by the characterization-of a high-spin Fe^II catalyst precursor. We show how good NMR performance can be obtained on a molecular powder sample at natural abundance by using very fast (> 30 kHz) magic angle spinning (MAS), even though the individual NMR resonances have highly anisotropic shifts and very short relaxation times. The results include the optimization of broadband heteronuclear (proton-carbon) recoupling sequences for polarization transfer; the observation of single or multiple quantum correlation spectra between coupled spins as a tool for removing the inhomogeneous bulk magnetic susceptibility (BMS) broadening; and the combination of NMR experiments and density functional theory calculations, to yield assignments.

Original language	English (US)
Pages (from-to)	13545-13552
Number of pages	8
Journal	Journal of the American Chemical Society
Volume	128
Issue number	41
DOIs	https://doi.org/10.1021/ja063510n
State	Published - Oct 18 2006
Externally published	Yes

ASJC Scopus subject areas

Catalysis
General Chemistry
Biochemistry
Colloid and Surface Chemistry

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Kervern, G., Pintacuda, G., Zhang, Y., Oldfield, E., Roukoss, C., Kuntz, E., Herdtweck, E., Basset, J. M., Cadars, S., Lesage, A., Copéret, C., & Emsley, L. (2006). Solid-state NMR of a paramagnetic DIAD-Fe^II catalyst: Sensitivity, resolution enhancement, and structure-based assignments. Journal of the American Chemical Society, 128(41), 13545-13552. https://doi.org/10.1021/ja063510n

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title = "Solid-state NMR of a paramagnetic DIAD-FeII catalyst: Sensitivity, resolution enhancement, and structure-based assignments",

abstract = "A general protocol for the structural characterization of paramagnetic molecular solids using solid-state NMR is provided and illustrated by the characterization-of a high-spin FeII catalyst precursor. We show how good NMR performance can be obtained on a molecular powder sample at natural abundance by using very fast (> 30 kHz) magic angle spinning (MAS), even though the individual NMR resonances have highly anisotropic shifts and very short relaxation times. The results include the optimization of broadband heteronuclear (proton-carbon) recoupling sequences for polarization transfer; the observation of single or multiple quantum correlation spectra between coupled spins as a tool for removing the inhomogeneous bulk magnetic susceptibility (BMS) broadening; and the combination of NMR experiments and density functional theory calculations, to yield assignments.",

author = "Gwendal Kervern and Guido Pintacuda and Yong Zhang and Eric Oldfield and Charbel Roukoss and Emile Kuntz and Eberhardt Herdtweck and Basset, {Jean Marie} and Sylvian Cadars and Anne Lesage and Christophe Cop{\'e}ret and Lyndon Emsley",

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doi = "10.1021/ja063510n",

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Kervern, G, Pintacuda, G, Zhang, Y, Oldfield, E, Roukoss, C, Kuntz, E, Herdtweck, E, Basset, JM, Cadars, S, Lesage, A, Copéret, C & Emsley, L 2006, 'Solid-state NMR of a paramagnetic DIAD-Fe^II catalyst: Sensitivity, resolution enhancement, and structure-based assignments', Journal of the American Chemical Society, vol. 128, no. 41, pp. 13545-13552. https://doi.org/10.1021/ja063510n

TY - JOUR

T1 - Solid-state NMR of a paramagnetic DIAD-FeII catalyst

T2 - Sensitivity, resolution enhancement, and structure-based assignments

AU - Kervern, Gwendal

AU - Pintacuda, Guido

AU - Zhang, Yong

AU - Oldfield, Eric

AU - Roukoss, Charbel

AU - Kuntz, Emile

AU - Herdtweck, Eberhardt

AU - Basset, Jean Marie

AU - Cadars, Sylvian

AU - Lesage, Anne

AU - Copéret, Christophe

AU - Emsley, Lyndon

PY - 2006/10/18

Y1 - 2006/10/18

N2 - A general protocol for the structural characterization of paramagnetic molecular solids using solid-state NMR is provided and illustrated by the characterization-of a high-spin FeII catalyst precursor. We show how good NMR performance can be obtained on a molecular powder sample at natural abundance by using very fast (> 30 kHz) magic angle spinning (MAS), even though the individual NMR resonances have highly anisotropic shifts and very short relaxation times. The results include the optimization of broadband heteronuclear (proton-carbon) recoupling sequences for polarization transfer; the observation of single or multiple quantum correlation spectra between coupled spins as a tool for removing the inhomogeneous bulk magnetic susceptibility (BMS) broadening; and the combination of NMR experiments and density functional theory calculations, to yield assignments.

AB - A general protocol for the structural characterization of paramagnetic molecular solids using solid-state NMR is provided and illustrated by the characterization-of a high-spin FeII catalyst precursor. We show how good NMR performance can be obtained on a molecular powder sample at natural abundance by using very fast (> 30 kHz) magic angle spinning (MAS), even though the individual NMR resonances have highly anisotropic shifts and very short relaxation times. The results include the optimization of broadband heteronuclear (proton-carbon) recoupling sequences for polarization transfer; the observation of single or multiple quantum correlation spectra between coupled spins as a tool for removing the inhomogeneous bulk magnetic susceptibility (BMS) broadening; and the combination of NMR experiments and density functional theory calculations, to yield assignments.

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DO - 10.1021/ja063510n

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SN - 0002-7863

VL - 128

SP - 13545

EP - 13552

JO - Journal of the American Chemical Society

JF - Journal of the American Chemical Society

IS - 41

ER -

Solid-state NMR of a paramagnetic DIAD-Fe^II catalyst: Sensitivity, resolution enhancement, and structure-based assignments

Abstract

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