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首页> 外文期刊>Chemistry: A European journal >Elusive Trimethyllanthanum: Snapshots of Extensive Methyl Group Degradation in La-Al Heterobimetallic Complexes
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Elusive Trimethyllanthanum: Snapshots of Extensive Methyl Group Degradation in La-Al Heterobimetallic Complexes

机译：难以捉摸的三甲基镧：La-Al异双金属配合物中大量甲基降解的快照

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摘要

Reactions of [La(AlMe4)(3)] and [Y(AlMe4)(3)] with PMe3 show that the phosphine can cleave Ln-CH3-Al linkages, separating Me3Al(PMe3). PMe3 (3 mol equiv) reacts with [Y(AlMe4)(3)] to give [(YMe3)(n)] contaminated with by-products containing phosphorus and aluminum. The La-based analog. [(LaMe3)(n)], is not formed selectively front the reaction of [La(AlMe4)(3)] with PMe3, or Et2O, which rather yields insoluble La/Al heterobimetallic products. Three multinuclear La-based clusters were obtained from a reaction of [La(AlMe4)(3)] with PMe3 (1 equiv) and identified by X-ray structure analyses. Each cluster exhibits extensive methyl group degradation and contains methylene, methine, or carbide moieties. [La4Al8(CH)(4)(CH2)(2)(CH3)(20)(PMe3)] has a {La-4(CH)(4)} cuboid core supported by AlMe3, Me2AlCH2AlMe2, and PMe3 ligands. [La4Al8(C)(CH)(2)(CH2)(2)(CH3)(22)-(toluene)] also contains a cuboid core, {La3Al(C)(CH)(2)(CH2)}, which includes one exo cubic lanthanum atom, and is supported by AlMe3, Me3AlCH2AlMe2, (AlMe4)(-), and toluene ligands. The lanthanum atoms in [La5Al9(CH)(6)(CH3)(30)] are arranged in a trigonal bipyramidal fashion with (CH) functionalities capping each face. The {La-5(CH)(6)}(3-) core is formally balanced by three AlMe2+ moieties and is additionally supported by six AlMe3 ligands. The unit cell contains two independent La-5 clusters, one with pseudo-C-3h and the other with pseudo-D-3 symmetry, as well as two molecules of the separation co-product Me3Al(PMe3).
机译：[La（AlMe4）（3）]和[Y（AlMe4）（3）]与PMe3的反应表明，膦可以裂解Ln-CH3-Al键，从而分离Me3Al（PMe3）。 PMe3（3摩尔当量）与[Y（AlMe4）（3）]反应，得到[（YMe3）（n）]，其被含磷和铝的副产物污染。基于La的模拟物。在[La（AlMe4）（3）]与PMe3或Et2O的反应之前，没有选择性地形成[（LaMe3）（n）]，这反而会产生不溶的La / Al异双金属产物。从[La（AlMe4）（3）]与PMe3（1当量）的反应中获得了三个基于La的多核簇，并通过X射线结构分析对其进行了鉴定。每个簇显示出广泛的甲基降解，并包含亚甲基，次甲基或碳化物部分。 [La4Al8（CH）（4）（CH2）（2）（CH3）（20）（PMe3）]具有{Al-4（CH）（4）}长方体核心，由AlMe3，Me2AlCH2AlMe2和PMe3配体支撑。 [La4Al8（C）（CH）（2）（CH2）（2）（CH3）（22）-（甲苯）]也包含长方体核，{La3Al（C）（CH）（2）（CH2）}，它包含一个外立立方镧原子，并由AlMe3，Me3AlCH2AlMe2，（AlMe4）（-）和甲苯配体支撑。 [La5Al9（CH）（6）（CH3）（30）]中的镧原子以三角双锥体方式排列，并带有（CH）官能团覆盖每个面。 {La-5（CH）（6）}（3-）核芯由三个AlMe2 +部分形成正式平衡，并另外由六个AlMe3配体支撑。晶胞包含两个独立的La-5簇，一个具有伪C-3h对称性，另一个具有伪D-3对称性，以及分离副产物Me3Al（PMe3）的两个分子。

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