Abstract
The 1H and 13C n.m.r. spectra of 15 substituted benzylidenemalononitriles (IIa–o) are reported in detail. The 1H chemical shift of the vinylic hydrogen changes by 0.67 p.p.m. over the range of substituents and may be correlated with either σ or σ+ substituent constants with almost the same degree of confidence (r0.989 for σ and 0.994 for σ+). The 13C chemical shift of the β-vinylic carbon is, however, much more sensitive to substituent effects (range of δ= 17.2 p.p.m.) and shows a clear correlation with the σ+ substituent constants (r 0.996) rather than the corresponding σ values (r 0.968). Three hitherto unreported σ+ values are derived from the data.

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