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Study of Unusually High Rotational Barriers about SN Bonds in Nonafluorobutane-1-sulfonamides: The Electronic Nature of the Torsional Effect

✍ Scribed by Ilya M. Lyapkalo; Hans-Ulrich Reissig; Andreas Schäfer; Armin Wagner


Publisher
John Wiley and Sons
Year
2002
Tongue
German
Weight
144 KB
Volume
85
Category
Article
ISSN
0018-019X

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✦ Synopsis


Abstract

Slow rotation about the SN bond in N,N‐disubstituted nonafluorobutane‐1‐sulfonamides 1 can easily be detected by NMR measurements at room temperature. This effect causes magnetic nonequivalence of otherwise identical geminal substituents in symmetrical staggered ground‐state conformation A. The torsional barriers determined (62–71 kJ⋅mol^−1^) proved to be the highest ever observed for sulfonamide moieties. They are comparable to the values routinely measured for carboxylic acid amides or carbamates. The restricted rotation is interpreted as result (n~N~d~S~)‐π and of n~N~__σ__ interactions, which develop substantial S,N double‐bond character in sulfonamides 1. The S,N binding interaction is increased by the highly electron‐withdrawing effect of the perfluorobutyl group. The anticipated symmetry of the ground‐state conformation A and the considerable shortening of the SN bond (1.59 Å) compared to the mean value in sulfonamides (1.63 Å) are confirmed by single‐crystal X‐ray study of N,N‐dibenzylnonafluorobutane‐1‐sulfonamide (1c).