Methylation of 2, 3, 4, 5-tetrahydro-1, 2, 4-triazine-3, 5-dione (I) with dimethyl sulfate afforded anhydro-3-hydroxy-1-methyl-2, 5 (4, 5)-dihydro-5-oxo-l, 2, 4-triazinium hydroxide (II), the structure of which was established by NMR spectra and chemical evidence consisting in hydrogenation to 1-methylhexahydro-1, 2, 4-triazine-3, 5-dione (IV).