Abstract
Free energies of activation, ΔG, have been calculated for isomerisation about the CN bond in a series of 2,6-dimethyl-4-aryliminopyrans (1), and their hydro-[(2) and (3)] and metho-[(4) and (5)] salts. Independent values were measured from coalescence of two different sets of 1H n.m.r. signals in each compound. The effects of temperature, solvent, and aryl substituent X on ΔG indicate that the metho-salts isomerise by CN bond rotation, the imines by inversion or a mechanism intermediate between inversion and rotation, and the hydro-salts by the previously unreported deprotonation–imine isomerisation–reprotonation mechanism. Hydro-salts (3) having a –M substituent in the aryl para-position give anomalous results for ΔG at the lower coalescence temperature.

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