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首页> 外文期刊>Dalton transactions: An international journal of inorganic chemistry >Ruthenium(II) complexes of hemilabile pincer ligands: synthesis and catalysing the transfer hydrogenation of ketones
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Ruthenium(II) complexes of hemilabile pincer ligands: synthesis and catalysing the transfer hydrogenation of ketones

机译：半不稳定夹钳配体的钌（II）配合物：合成和催化酮的转移加氢

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摘要

A series of Ru(II) complexes were synthesised based on a hemilabile pyrazole-N-heterocyclic carbene (NHC)-pyrazole (C3N2H3)CH2(C3N2H2)CH2(C3N2H3) NCN pincer ligand 1. All complexes were fully characterised using single crystal X-ray crystallography and multinuclear NMR spectroscopy. Hemilabile ligands provide flexible coordination modes for the coordinating metal ion which can play a significant effect on the efficiency and mechanism of catalysis by the resulting complex. Here we observed and isolated mono-, bi- and tri-dentate complexes of both Ag(I) and Ru(II) with 1 in which the resultant coordination mode was controlled by careful reagent selection. The catalytic activity of the Ru(II) complexes for the transfer hydrogenation reaction of acetophenone with isopropanol was investigated. The unexpected formation of the pentaborate anion, [B5O6(OH)(4)](-), during the synthesis of complex 6a was found to have an unexpected positive effect by enhancing the catalysis rate. This work provides insights into the roles that different coordination modes, counterions and ligand hemilability play on the catalytic activity in transfer hydrogenations.
机译：基于半不稳定的吡唑-N-杂环卡宾（NHC）-吡唑（C3N2H3）CH2（C3N2H2）CH2（C3N2H3）NCN钳位配体1合成了一系列Ru（II）配合物。所有配合物均使用单晶X进行了完全表征射线晶体学和多核NMR光谱。半不稳定的配体为配位金属离子提供了灵活的配位方式，可对所得配合物催化的效率和机理产生重大影响。在这里，我们观察到并分离出了Ag（I）和Ru（II）与1的单齿，双齿和三齿配合物，其中通过谨慎的试剂选择控制了最终的配位模式。研究了Ru（II）配合物对苯乙酮与异丙醇转移氢化反应的催化活性。发现在络合物6a的合成过程中五硼酸阴离子[B5O6（OH）（4）]（-）的意外形成通过提高催化速率具有意外的积极作用。这项工作提供了对不同配位方式，抗衡离子和配体半合性在转移氢化中的催化活性中所起的作用的见解。

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