Abstract: “2+1” technetium tricarbonyl complexes [99Tc(CO)3(NN)(Ad)]ClO4 with a combination of bidentate NN heterocyclic imines [NN = 2,2'-bipyridine (bipy) or 1,10-phenanthroline (phen)] and adenine (Ad) were prepared. The complexes were isolated pure and characterized by IR and 99Tc NMR spectroscopy in solution. The solid-state structure of the complexes was determined by single crystal X-ray diffraction. Both in solution and in the solid phase, adenine is coordinated to technetium via either imidazole or pyrimidine nitrogen atom to form two coordination isomers. © Pleiades Publishing, Ltd. 2025.