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首页> 外文期刊>Chemistry: A European journal >Group IV organometallic compounds based on dianionic 'pincer' ligands: Synthesis, characterization, and catalytic activity in intramolecular hydroamination reactions
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Group IV organometallic compounds based on dianionic 'pincer' ligands: Synthesis, characterization, and catalytic activity in intramolecular hydroamination reactions

机译：基于二价“钳子”配体的第四族有机金属化合物：分子内加氢胺化反应的合成，表征和催化活性

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摘要

Neutral Zr~(IV) and Hf~(IV) diamido complexes stabilized by unsymmetrical dianionic N,C,N′ pincer ligands have been prepared through the simplest and convenient direct metal-induced C_(aryl)-H bond activation. Simple ligand modification has contributed to highlight the non-innocent role played by the donor atom set in the control of the cyclometallation kinetics. The as-prepared bis-amido catalysts were found to be good candidates for the intramolecular hydroamination/cyclization of primary aminoalkenes. The ability of these compounds to promote such a catalytic transformation efficiently (by providing, in some cases, fast and complete substrate conversion at room temperature) constitutes a remarkable step forward toward catalytic systems that can operate at relatively low catalyst loading and under milder reaction conditions. Kinetic studies and substrate-scope investigations, in conjunction with preliminary DFT calculations on the real systems, were used to elucidate the effects of the substrate substitution on the catalyst performance and to support the most reliable mechanistic path operative in the hydroamination reaction. Changing the order of the "factors" can (somehow) change the result! Neutral Zr~(IV) and Hf~(IV) diamido complexes stabilized by unsymmetrical dianionic N,C,N′-pincer ligands have been prepared (see picture) and successfully employed as good catalyst candidates for the efficient and mild intramolecular hydroamination/cyclization of primary aminoalkenes.
机译：通过最简单方便的直接金属诱导的C_（芳基）-H键活化作用，制备了由不对称双阴离子N，C，N'钳型配体稳定的中性Zr〜（IV）和Hf〜（IV）二氨基配合物。简单的配体修饰有助于突出供体原子在控制环金属化动力学中发挥的非无害作用。发现所制备的双-酰胺催化剂是伯氨基烯烃的分子内加氢胺化/环化的良好候选者。这些化合物有效地促进这种催化转化的能力（通过在某些情况下提供快速和完全的底物转化）构成了朝着催化体系迈出的重要一步，该催化体系可以在相对较低的催化剂负载量和较温和的反应条件下运行。动力学研究和底物范围研究，结合对实际系统的初步DFT计算，被用来阐明底物替代对催化剂性能的影响，并支持加氢胺化反应中最可靠的机理。更改“因素”的顺序可以（以某种方式）更改结果！制备了由不对称双阴离子N，C，N'-钳位配体稳定的中性Zr〜（IV）和Hf〜（IV）二酰胺配合物（见图），已成功地用作有效且温和的分子内加氢胺化/环化的良好催化剂候选物伯氨基烯烃。

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