Reaction of (dpp-BIAN)Mg(THF) 3 (1) {dpp-BIAN = 1,2-bis [(2,6-diisopropylphenyl)imino]acenaphthene} with one molar equivalent of 2,2,6,6-tetramethylpiperidine-1-oxyl (TEMPO) proceeds with oxidation of the dpp-BIAN dianion in 1 to the radical-anion and affords the (dpp-BIAN)-Mg(TEMPO)(thf) (2) complex. The reaction of dpp-BIAN with an excess amount of magnesium and 0.5 molar equivalents of I 2 in Et 2 O gives (dpp-BIAN)MgI(Et 2 O) n , which then reacts in situ with (Me 3 Si) 2 NK to produce (dpp-BIAN)-Mg[N(SiMe 3 ) 2 ](Et 2 O) (3). Solvent-free magnesium amide (dpp-BIAN)Mg[N(SiMe 3 ) 2 ] (4) was synthesized by treating equimolar amounts of MgI 2 , dpp-BIAN, and sodium in tolu-