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首页> 外文期刊>Dalton transactions: An international journal of inorganic chemistry >Synthesis, structures and catalytic activities of ruthenium(II) carbonyl chloride complexes containing pyridine-functionalised N-heterocyclic carbenes
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Synthesis, structures and catalytic activities of ruthenium(II) carbonyl chloride complexes containing pyridine-functionalised N-heterocyclic carbenes

机译：含吡啶官能化的N-杂环卡宾的钌（II）羰基氯氯化物配合物的合成，结构和催化活性

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摘要

A series of ruthenium(II) carbonyl chloride complexes with pyridine-functionalised N-heterocyclic carbenes, trans(Cl)- and cis(Cl)-[Ru(Py-NHC)(CO)(2)Cl-2] [Py-NHC = 3-tert-butyl-1-(2-pyridyl)imidazol-2-ylidene, 1a and 1b; 3-n-butyl-1-(2-pyridyl)imidazol-2-ylidene, 2a and 2b; 3-tert-butyl-1-picolylimidazol-2-ylidene, 3a and 3b; 3-n-butyl-1-picolylimidazol-2-ylidene, 4a and 4b; 3-benzyl-1-picolylimidazol-2-ylidene, 5a and 5b] have been prepared by transmetallation from the corresponding silver carbene complexes and characterised by elemental analyses, infrared and H-1 and C-13 NMR spectroscopies. The yields of trans(Cl)- and cis(Cl)-isomers could be controlled by altering the reaction conditions: the trans-isomers were kinetically formed as the main products in 60-70% yield in CH2Cl2 at ambient temperature while the thermodynamic cis-isomers were obtained as the major products in 70-80% yield in toluene at refluxing temperature. The trans-isomer was transformed into the thermodynamic cis-isomer by heating in CH2Cl2 in a Teflon-lined stainless autoclave for 24 h at 120 degrees C. The molecular structures of 1a, 1b, 2b, and 4b have been determined by single-crystal X-ray diffraction. These complexes showed catalytic activities in hydrogen transfer reactions of ketones.
机译：一系列钌（II）羰基氯与吡啶官能化的N-杂环卡宾，反式（Cl）-和顺式（Cl）-[Ru（Py-NHC）（CO）（2）Cl-2] [Py- NHC ＝ 3-叔丁基-1-（2-吡啶基）咪唑-2-亚烷基，1a和1b; 3-n-丁基-1-（2-吡啶基）咪唑-2-亚烷基，2a和2b; 3-叔丁基-1-吡啶并咪唑-2-亚烷基，3a和3b; 3-正丁基-1-甲基吡啶并咪唑-2-亚烷基，4a和4b;通过相应金属卡宾银配合物的金属转移反应，制备了3-苄基-1-吡啶基咪唑-2-亚甲基5a和5b]，并通过元素分析，红外光谱和H-1和C-13 NMR谱进行了表征。可以通过改变反应条件来控制反式（Cl）-和顺式（Cl）-异构体的收率：在环境温度下，CH2Cl2中以60-70％的收率动态形成反式异构体作为主要产物。在回流温度下，在甲苯中以70-80％的收率获得作为主要产物的β-异构体。通过在衬有特氟隆的不锈钢高压釜中于120°C下在CH2Cl2中加热24小时，可将反式异构体转变为热力学顺式异构体。1a，1b，2b和4b的分子结构已通过单晶确定X射线衍射。这些配合物在酮的氢转移反应中显示出催化活性。

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