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首页> 外文期刊>Chemistry: A European journal >Ruthenium(II) Complexes Containing Lutidine-Derived Pincer CNC Ligands: Synthesis, Structure, and Catalytic Hydrogenation of C=N bonds
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Ruthenium(II) Complexes Containing Lutidine-Derived Pincer CNC Ligands: Synthesis, Structure, and Catalytic Hydrogenation of C=N bonds

机译：含卢替丁衍生的钳式CNC配体的钌（II）配合物：C = N键的合成，结构和催化加氢

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摘要

A series of Ru complexes containing lutidine-derived pincer CNC ligands have been prepared by transmetalation with the corresponding silver-carbene derivatives. Characterization of these derivatives shows both mer and fac coordination of the CNC ligands depending on the wing-tips of the N-heterocyclic carbene fragments. In the presence of tBuOK, the Ru-CNC complexes are active in the hydrogenation of a series of imines. In addition, these complexes catalyze the reversible hydrogenation of phenantridine. Detailed NMR spectroscopic studies have shown the capability of the CNC ligand to be deprotonated and get involved in ligand-assisted activation of dihydrogen. More interestingly, upon deprotonation, the Ru-CNC complex 5e(BF4) is able to add aldimines to the metal-ligand framework to yield an amido complex. Finally, investigation of the mechanism of the hydrogenation of imines has been carried out by means of DFT calculations. The calculated mechanism involves outer-sphere stepwise hydrogen transfer to the C=N bond assisted either by the pincer ligand or a second coordinated H-2 molecule.
机译：通过与相应的银卡宾衍生物进行重金属化制备了一系列含卢剔啶衍生的钳式CNC配体的Ru络合物。这些衍生物的表征显示了CNC配体的mer和fac配位，这取决于N-杂环卡宾片段的翼尖。在tBuOK存在下，Ru-CNC络合物在一系列亚胺的氢化中具有活性。另外，这些络合物催化菲啶啶的可逆氢化。详细的NMR光谱研究表明CNC配体具有去质子化能力，并参与了配体辅助的二氢活化。更有趣的是，在去质子化后，Ru-CNC络合物5e（BF4）能够向金属-配体骨架中添加醛亚胺以生成酰胺基络合物。最后，通过DFT计算对亚胺的氢化机理进行了研究。计算的机理涉及通过钳形配体或第二个配位的H-2分子协助外球逐步将氢转移至C = N键。

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