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首页> 外文期刊>Dalton transactions: An international journal of inorganic chemistry >Synthesis and catalytic alcohol oxidation and ketone transfer hydrogenation activity of donor-functionalized mesoionic triazolylidene ruthenium(II) complexes?
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Synthesis and catalytic alcohol oxidation and ketone transfer hydrogenation activity of donor-functionalized mesoionic triazolylidene ruthenium(II) complexes?

机译：供体官能化的中离子型三氮亚甲基钌（II）配合物的合成及其催化醇氧化和酮转移加氢活性？

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摘要

We report on the synthesis of a variety of C,E-bidentate triazolylidene ruthenium complexes that comprise different donor substituents E (E = C: phenyl anion; E = O: carboxylate, alkoxide; E = N: pyridine at heterocyclic carbon or nitrogen). Introduction of these donor functionalities is greatly facilitated by the synthetic versatility of triazoles, and their facile preparation routes. Five different complexes featuring a C,E-coordinated ruthenium center with chloride/cymene spectator ligands and three analogous solvento complexes with MeCN spectator ligands were prepared and evaluated as catalyst precursors for direct base- and oxidant-free alcohol dehydrogenation, and for transfer hydrogenation using basic iPrOH as a source of dihydrogen. In both catalytic reactions, the neutral/mono-cationic complexes with chloride/ cymene spectator ligands performed better than the solvento ruthenium complexes. The donor functionality had a further profound impact on catalytic activity. For alcohol dehydrogenation, the C,C-bidentate phenyl-triazolylidene ligand induced highest conversions, while carboxylate or pyridine donor sites gave only moderate activity or none at all. In contrast, transfer hydrogenation is most efficient when a pyridyl donor group is linked to the triazolylidene via the heterocyclic carbon atom, providing turnover frequencies as high as 1400 h~(?1) for cyclohexanone transfer hydrogenation. The role of the donor group is discussed in mechanistic terms.
机译：我们报告了包含不同供体取代基E（E = C：苯基阴离子; E = O：羧酸根，醇盐; E = N：杂环碳或氮上的吡啶）的各种C，E-二齿三唑基钌络合物的合成。这些供体功能的引入极大地促进了三唑的合成多功能性及其简便的制备途径。制备了五种不同的配合物，这些配合物具有C，E配位的钌中心和氯/苏木精配体，还有三种类似的溶剂配体具有MeCN配体，并被评估为直接无碱和无醇醇脱氢的催化剂前体，并使用碱性iPrOH作为氢的来源。在这两种催化反应中，具有氯离子/次甲基苯并咪基配位体的中性/单阳离子配合物的性能均优于溶剂钌配合物。供体的功能性对催化活性有更深远的影响。对于醇脱氢，C，C齿状的苯基三氮杂亚烷基配体诱导了最高的转化率，而羧酸盐或吡啶供体位点仅给出中等活性，或根本没有。相反，当吡啶基供体基团通过杂环碳原子与三唑基亚烷基相连时，转移氢化是最有效的，为环己酮转移氢化提供了高达1400h〜（？1）的周转频率。用机械的方式讨论了供体的作用。

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