The preparation and characterization of a series of neutral rare-earth metal complexes [Ln(Me(3)TACD)(η(3)-C(3)H(5))(2)] (Ln=Y, La, Ce, Pr, Nd, Sm) supported by the 1,4,7-trimethyl-1,4,7,10-tetraazacyclododecane anion (Me(3)TACD(-)) are reported. Upon treatment of the neutral allyl complexes [Ln(Me(3)TACD)(η(3)-C(3)H(5))(2)] with Brønsted acids, monocationic allyl complexes [Ln(Me(3)TACD)(η(3)-C(3)H(5))(thf)(2)][B(C(6)X(5))(4)] (Ln=La, Ce, Nd, X=H, F) were isolated and characterized. Hydrogenolysis gave the hydride complexes [Ln(Me(3)TACD)H(2)](n) (Ln=Y, n=3; La, n=4; Sm). X-ray crystallography showed the lanthanum hydride to be tetranuclear. Reactivity studies of [Ln(Me(3)TACD)R(2)](n) (R=η(3)-C(3)H(5), n=0; R=H, n=3,4) towards furan derivatives includes hydrosilylation and deoxygenation under ring-opening conditions.
Neutral, cationic and anionic allyl compounds of scandium contain highly fluxional allyl ligands in solution, whilst in the solid state both η(1)- and η(3)-binding modes are detected.
Cyclic polyamine 1,4,7‐trimethyl‐1,4,7,10‐tetraazacyclododecane, (Me3TACD)H (1), was metalated with n‐butyllithium in pentane to give [Li2(Me3TACD)2] (2). The structure of this compound is dimeric in the solid state as shown by single‐crystal X‐ray diffraction. With an excess of nBuLi, nBuLi is incorporated into the product. Depending on the stoichiometry, the compounds [Li3(nBu)(Me3TACD)2] (3) or [Li4(nBu)2(Me3TACD)2] (4) are formed. As shown by single‐crystal X‐ray diffraction, both molecular structures show a ladder motif. (Me3TACD)H reacted with NaI/Na2CO3 in acetonitrile to give benzene‐soluble [NaI(Me3TACD)H] (5).
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