The reaction of N,N′-dimethylformamide azine (DMFA) or its dihydrochloride derivative (DMFA·2HCl) with o-RO(O)CC6H4NH2 (R = Me, Et) leads to co-crystallization products o-RO(O)CC6H4NH2·DMFA (R = Me, Et), while the same reaction of DMFA·2HCl with m- and p-RO(O)CC6H4NH2 (R = Me, Et) provides the corresponding 4-substituted 1,2,4-triazoles (1–4). Reaction of the same m- and p-substituted amines with DMFA has failed, while addition of a few drops of HCl or HNO3 in this reaction mixture has allowed us to obtain the corresponding triazole derivatives. Thus, the direct transamination reaction with the formation of triazoles 1–4 is catalysed by acidic catalysts. Molecular structures of DMFA, o-EtO(O)CC6H4NH2·DMFA and 3 were elucidated by X-ray diffraction.
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