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The syntheses and crystal structures of a series of heterobimetallic Li/Mg and Li/Al complexes prepared from an N,N,O-tridentate ligand are described. The ligand HOC­(CH2)5CH2N­(Me)­CH2CH2NMe2 (LH) and nBu2Mg were used to synthesize the homometallic magnesium alkoxide [{LMgOC­(CH2)5CH2 N­(Me)­CH2CH2 NMe2}2] (1), which was reacted with nBuLi to afford the lithium alkylmagnesiate [{Bu2Mg­{LiOC­(CH2)5CH2 N­(Me)­CH2CH2 NMe2}}2] (2). Complex 2 was then hydrolyzed to produce [{BuMgOLi­{LiOC­(CH2)5CH2 N­(Me)­CH2CH2 NMe2}2}2] (3). The sequential reaction of LH in diethyl ether with RAlMe2 (R = Me, Cl) and nBuLi aforded two lithium aluminate complexes containing a polymeric structure of one-dimensional chains [{−LiOC­(CH2)5CH2 N­(Me)­CH2CH2 NMe2}­Al­(Me)­(n-Bu)­CH3−} n ] (4) and [{−LiOC­(CH2)5CH2 N­(Me)­CH2CH2 NMe2}­Al­(n-Bu)2CH2−} n ] (5), respectively. Each of the complexes 1–5 was structurally characterized and tested for its capability to catalyze Meerwein–Ponndorf–Verley (MPV) reactions. Heterobimetallic complexes 2 and 3 exhibited catalytic activities better than those of homometallic magnesium complex 1 and heterobimetallic lithium aluminate complexes 4 and 5 for MPV reactions.

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Dimeric anilidolithium (ArHNLi·Et2O)2 (Ar=2,6-iPr2C6H3) reacted with zirconium tetrachloride in THF to give the heterometallic zirconium–lithium complex [(Et2O)2Li(μ-Cl)2(ArHN)(ArN=)Zr(μ-Cl)]2 (C1) and with titanium tetrachloride in toluene to give the titanium complex [(ArN=)TiCl2·(Et2O)2] (C2) each in good isolated yields. Their molecular structures in the solid state were confirmed by X-ray diffraction analysis. Upon activation with methylaluminoxane, both arylimido zirconium and titanium complexes exhibited good catalytic activities toward ethylene polymerization.