A range of 2,5-dihydro-1H-1,2,4-triazol-2-yl radicals 2b-p has been pr
epared by dehydrogenation of the corresponding 4,5-dihydro-1H-1,2,4-tr
iazoles 5b-p which have been synthesized using various methods. EPR, E
NDOR and NMR studies have led to a complete analysis and full assignme
nt of all hyperfine coupling constants. The pi-SOMO, having a node at
the C(3) methine carbon, is mainly confined to the nitrogens of the fi
ve-membered ring, particularly to those of the hydrazyl moiety.