Synthesis and properties of new 2-[2-(N-alkyl)-pyridinium]-4,4,5,5-tetramethylimidazoline-1-oxyl-3-oxide iodide radicals

2-(2-pyridyl)-4,4,5,5-tetramethylimidazoline-1-oxyl-3-oxide radical 2 and t he 2-[2-(N-alkyl)-pyridinium] derivatives (3a and 3b) were synthesized and characterized by elemental analysis, melting points, and spectroscopy. The density functional theory (DFT) was used in order to obtain the structures and electronic properties of the new nitronyl nitroxide radicals. Modified reaction procedures of the intermediates are described with better yield an d purity of the find products. The magnetic properties of the compounds 2, 3a, and 3b are predicted for the first time using a simple model of charge transference, in the framework of the molecular orbital calculations. The o btained results show that the substituent at the central carbon atom of the imidazoline is important to determine the spin distribution and consequent ly the nature of the magnetic interaction.