Assembled Multinuclear Ruthenium(II)–NNNN Complexes: Synthesis, Catalytic Properties, and DFT Calculations,Organometallics

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Assembled Multinuclear Ruthenium(II)–NNNN Complexes: Synthesis, Catalytic Properties, and DFT Calculations
Organometallics ( IF 2.5 ) Pub Date : 2019-12-19 , DOI: 10.1021/acs.organomet.9b00669
Tingting Liu _{1,

2,

3} , Kaikai Wu ₁ , Liandi Wang ₁ , Hongjun Fan _{1,

4} , Yong-Gui Zhou ₁ , Zhengkun Yu _{1,

5}

Affiliation

Using a coordinatively unsaturated 16-electron mononuclear ruthenium(II)-pyrazolyl-imidazolyl-pyridine complex [Ru(II)–NNN] as the building block and oligopyridines as the polydentate ligands, pincer-type tri- and hexanuclear ruthenium(II) complexes [Ru(II)–NNNN]_n were efficiently assembled. These complexes were characterized by elemental analyses, NMR, IR, and MALDI-TOF mass spectroscopies. In refluxing 2-propanol, the multinuclear ruthenium(II)–NNNN complexes exhibited exceptionally high catalytic activity for the transfer hydrogenation of ketones at very low concentrations and reached turnover frequencies (TOFs) up to 7.1 × 10⁶ h^–1, featuring a remarkable cooperative effect from the multiple Ru(II)–NNNN functionalities. DFT calculations have revealed the origin of the high catalytic activities of these Ru(II)–NNNN complexes.

中文翻译：

组装的多核钌（II）–NNNN配合物：合成，催化性能和DFT计算

使用配位不饱和的16电子单核钌（II）-吡唑基-咪唑基-吡啶复合物[Ru（II）–NNN]作为结构单元，并以低聚吡啶为多齿配体，夹型三和六核钌（II）配合物[Ru（II）–NNNN] _n被有效地组装。这些配合物的特征在于元素分析，NMR，IR和MALDI-TOF质谱。在回流的2-丙醇中，多核钌（II）-NNNN络合物在极低的浓度下对酮的转移加氢显示出异常高的催化活性，并达到高达7.1×10 ⁶ h ^–1的周转频率（TOF）。具有多种Ru（II）-NNNN功能的显着协同作用。DFT计算揭示了这些Ru（II）-NNNN配合物具有高催化活性的起源。

更新日期：2019-12-20

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