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Three-component coupling of thiourea/urea, various structurally diverse aromatic aldehydes and ammo- nium acetate is catalyzed by activated fly ash in dry media under microwave irradiation to give 6-aryl-1,2,4,5-tetrazinan- 3-thiones/ones in good yields. The structure of 6-aryl-1,2,4,5-tetrazinan-3-thiones/ones have been elucidated on the basis of their melting points, elemental analysis, MS, IR, H NMR, D O exchange, C NMR and two dimensional NMR spec- tral studies including Homonuclear Correlation (HOMOCOR) and Heteronuclear Single Quantum Correlation (HSQC) spectra.

Easy-to-execute 'One-pot' Synthesis of 1,2,4,5-Tetrazines Catalyzed by Activated Fly Ash