Oxidative ammonolysis of 3,4-dimethylpyridine on an individual vanadium oxide (V 2 O 5 ) catalyst and binary vanadium oxide catalysts, modified by additions of SnO 2 and ZrO 2 , has been studied. A connection between СНacidity of the methyl groups of the substrate in the gaseous phase and in the chemosorbed state and the sequence of their transformation into a cyano group has been established. It has been shown that nucleophilicity of vanadyl oxygen, calculated by the Density Functional Theory method, increases with V 2 O 5 modification by SnO 2 and ZrO 2 additions. Herewith, an increasing yield of 3methyl-4-cyanopyridine and imide of pyridine-3,4-dicarboxylic acid was observed. A proposed mechanism of the imide of pyridine-3,4-dicarboxylic acid formation has been discussed