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首页> 外文期刊>Dalton transactions: An international journal of inorganic chemistry >Solvent-free heterogeneous catalysis for cyanosilylation in a dynamic cobalt-MOF
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Solvent-free heterogeneous catalysis for cyanosilylation in a dynamic cobalt-MOF

机译：动态钴-MOF中氰基甲硅烷基化反应的无溶剂多相催化

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摘要

The butterfly-like tetranuclear cobalt cluster based 3D MOF [Me2NH2][Co-2(bptc)(mu(3)-OH)(H2O)(2)] (1) underwent a reversible thermally triggered single-crystal-to-single-crystal transformation via Co-O-water weakened intermediate 1a to produce a partly dehydrated phase [Me2NH2][Co-2(bptc)(mu 3-OH)(H2O)] (2), which was confirmed by single-crystal X-ray diffraction, powder X-ray diffraction, thermogravimetric analysis, and IR spectroscopy. During the dehydration course, the local coordination environment of one Co2+ ion was changed from the saturated octahedron to a coordinately unsaturated square-pyramid, accompanied by a crystal color change from red to purple. Compared with pristine hydrated 1, dehydrated 2 exhibits highly efficient and recyclable catalytic activity for cyanosilylation of carbonyl compounds with a low catalyst loading of 0.1 mol% Co at room temperature under solvent-free conditions, which due to the open Co2+ sites as catalytically activated sites played a significant role in the heterogeneous catalytic process.
机译：基于蝴蝶状四核钴簇的3D MOF [Me2NH2] [Co-2（bptc）（mu（3）-OH）（H2O）（2）]（1）经历了可逆的热触发单晶至单晶Co-O-水弱化中间体1a进行晶体转化，生成部分脱水的相[Me2NH2] [Co-2（bptc）（mu 3-OH）（H2O）]（2），这已通过单晶X确认射线衍射，粉末X射线衍射，热重分析和红外光谱。在脱水过程中，一个Co 2+离子的局部配位环境从饱和的八面体变为配位不饱和的方形金字塔，同时晶体颜色也从红色变为紫色。与原始水合1相比，脱水2在无溶剂条件下在室温下以0.1 mol％Co的低催化剂负载量对羰基化合物的氰基甲硅烷化显示出高效且可回收的催化活性，这归因于开放的Co2 +位点作为催化活化位点在非均相催化过程中起着重要作用。

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