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首页> 外文期刊>Chemistry: A European journal >Ru-II, Os-II, and Ir-III Complexes with Chelating Pyridyl-Mesoionic Carbene Ligands: Structural Characterization and Applications in Transfer Hydrogenation Catalysis
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Ru-II, Os-II, and Ir-III Complexes with Chelating Pyridyl-Mesoionic Carbene Ligands: Structural Characterization and Applications in Transfer Hydrogenation Catalysis

机译：Ru-II，Os-II和Ir-III配合物与螯合的吡啶基-中型碳原子配体：结构表征及其在转移加氢催化中的应用

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Chelating ligands with one pyridine donor and one mesoionic carbene donor are fast establishing themselves as privileged ligands in homogeneous catalysis. The synthesis of several new Ir-III-Cp*- and Os-II-Cym complexes (Cp*=pentamethylcyclopentadienyl, Cym=p-cymene=4-isopropyl-toluene) derived from chelating pyridyltriazolylidenes where the additional pyridine donor was incorporated via the azide part of the triazole is presented. Furthermore, different 4-substituted phenylacetylene building blocks have been used to introduce electronic fine-tuning in the ligands. The ligands thus can be generally described as 4-(4-R-pphenyl)-3-methyl-1-(pyridin-2-yl)-1H-1,2,3-triazol-5-ylidene (with R being H (L-1), Me (L-2), OMe (L-3), CN (L-4), CF3 (L-5), Br (L-6) or NO2 (L-7)). The corresponding complexes (Ir-1 to Ir-7 and Os-1 to Os-7) were characterized by standard spectroscopic methods, and the expected three-legged, piano-stool type coordination was unambiguously confirmed by X-ray diffraction analysis of selected compounds. Together with Ru-II analogues previously reported by us, a total of 21 complexes were tested as (pre) catalysts for the transfer hydrogenation of carbonyl groups, showing a remarkable reactivity even at very low catalyst loadings. The electronic effects of the ligands as well as different substrates were investigated. Some mechanistic elucidations are also presented.
机译：具有一个吡啶供体和一个内消旋卡宾供体的螯合配体在均相催化中迅速确立了自己的特权配体。几种新的Ir-III-Cp *-和Os-II-Cym配合物（Cp * =五甲基环戊二烯基，Cym = p-丁烯基= 4-异丙基-甲苯）的合成，螯合吡啶基三唑基亚烷基，通过介绍了三唑的叠氮化物部分。此外，已经使用了不同的4-取代的苯乙炔结构单元来在配体中引入电子微调。因此，配体通常可以描述为4-（4-R-对苯基）-3-甲基-1-（吡啶-2-基）-1H-1,2,3-三唑-5-亚基（R为H （L-1），Me（L-2），OMe（L-3），CN（L-4），CF3（L-5），Br（L-6）或NO2（L-7））。相应的配合物（Ir-1至Ir-7和Os-1至Os-7）通过标准光谱法进行了表征，并通过X射线衍射分析明确地确认了预期的三足钢琴凳式配位化合物。与我们先前报道的Ru-II类似物一起，总共测试了21种配合物作为羰基转移加氢的（预）催化剂，即使在非常低的催化剂负载量下也显示出显着的反应活性。研究了配体以及不同底物的电子效应。还介绍了一些机械方法。

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