Tautomerism of 4-iminobarbiturates depends upon the presence of a substituent on the N (3) atom. The ultraviolet, infrared, proton nuclear magnetic resonance, 13 C-nuclear magnetic resonance and mass spectrum data show that 3-alkylated compounds present an imido system while 3-unalkylated ones are characterized by an amidinoketone system. The electrochemical bahavior of these two groups was studied by polarography, cyclic ...