Аннотация:New zwitterionic bisulfite compounds of aldehydes, such as pyridine-2-carbaldehyde (1) and qunoline-2-carbaldehydes (2), were for the first time spectroscopically characterized and structurally studied. In the crystal structures, molecules 1 and 2 are connected via intermolecular OH⋯−O3S and NH+⋯−O3S interactions to form hydrogen-bonded chains. The oxidation of a solution of 2 in dimethyl sulfoxide with atmospheric air afforded quinaldil (3) and quinaldoin (4). In the crystalline state, compound 4 exists as the enediol tautomer formed by strong intramolecular hydrogen bonds.