Facile condensation of 2-acetylpyridine with ethylenediamine in a 1:1 or 2:1 molar ratio yielded two neutral ligands with different denticity: 1-amino-4-(2-pyridyl)-3-azapent-3-ene (tridentate, L 1 ) and 2,7-bis(2-pyridyl)-3,6-diazaocta-2,6-diene (tetradentate, L 3 ), respectively. Replacing the ketone with 2-pyridinecarboxaldehyde gave a similar set of condensates (