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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U2 - 10.1021/ja063510n
DO - 10.1021/ja063510n
M3 - Article
C2 - 17031968
AN - SCOPUS:33750050270
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 -