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首页> 外文期刊>Dalton transactions: An international journal of inorganic chemistry >An uncoordinated tertiary nitrogen based tricarboxylate calcium network with Lewis acid-base dual catalytic sites for cyanosilylation of aldehydes
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An uncoordinated tertiary nitrogen based tricarboxylate calcium network with Lewis acid-base dual catalytic sites for cyanosilylation of aldehydes

机译：具有Lewis酸碱双催化位点的未计算的叔氮基基三羧酸钙网，用于醛甲硅烷化甲硅烷化酶

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摘要

The design and utilization of dual sites for synergistic catalysts has been recognised as an efficient method towards high-efficiency catalysis in the cyanosilylation of aldehydes, which gives key intermediates for the synthesis of a number of valuable natural and pharmaceutical compounds. However, most of the reported dual-site catalysts for this reaction were homogeneous, accompanied by potential deactivation through internal complexation of the dual sites. Herein, by the rational selection of an uncoordinated tertiary nitrogen based tricarboxylic ligand (tris[(4-carboxyl)-phenylduryl]amine, H(3)TCBPA), a new three-dimensional calcium-based metal-organic framework (MOF), Ca-3(TCBPA)(2)(DMA)(2)(H2O)(2) (1, where TCBPA = ionized tris[(4-carboxyl)-phenylduryl]amine and DMA = N,N-dimethylacetamide), possessing accessible dual catalytic sites, Lewis-basic N and Lewis-acidic Ca, has been designed and constructed by a one-pot solvothermal reaction. As expected, 1 is capable of dually and heterogeneously catalysing the cyanosilylation of aldehydes at room temperature, and can be reused for at least 6 runs with a maximum turnover number (TON) of 1301, which is superior to most reported cases. Additionally, 1 shows CO2 adsorption ability and conversion with epoxides, which is beneficial for the establishment of a sustainable society.
机译：设计和利用双位点协同催化剂已被公认为是实现醛氰合反应高效催化的有效方法，该方法为合成许多有价值的天然和药物化合物提供了关键中间体。然而，大多数报道的用于该反应的双中心催化剂是均相的，伴随着通过双中心的内部络合而可能失活。在此，通过合理选择非配位的第三氮基三羧酸配体（tris[（4-羧基）-苯基杜伦基]胺，H（3）TCBPA），一种新的三维钙基金属有机骨架（MOF），Ca-3（TCBPA）（2）（DMA）（2）（H2O）（2）（1，其中TCBPA=电离的三[（4-羧基）-苯杜伦基]胺，DMA=N，N-二甲基乙酰胺），具有可访问的双催化位点，路易斯碱性N和路易斯酸性Ca是通过一锅溶剂热反应设计和构建的。正如预期的那样，1能够在室温下对醛的氰基化反应进行双重和非均相催化，并且可以重复使用至少6次，最大周转数（吨）为1301，这优于大多数报告的情况。此外，1显示了CO2吸附能力和与环氧化物的转化，这有利于建立可持续社会。

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    Wang Ying-Xia; Wang Hui-Min; Meng Pan; Song Dong-Xia; Hou Juan-Juan; Zhang Xian-Ming;

  • 作者单位

    Shanxi Normal Univ Minist Educ Key Lab Magnet Mol &

    Magnet Informat Mat Inst Chem &

    Culture Sch Chem &

    Mat Sci Linfen 041004 Shanxi Peoples R China;

    Shanxi Normal Univ Minist Educ Key Lab Magnet Mol &

    Magnet Informat Mat Inst Chem &

    Culture Sch Chem &

    Mat Sci Linfen 041004 Shanxi Peoples R China;

    Shanxi Normal Univ Minist Educ Key Lab Magnet Mol &

    Magnet Informat Mat Inst Chem &

    Culture Sch Chem &

    Mat Sci Linfen 041004 Shanxi Peoples R China;

    Shanxi Normal Univ Minist Educ Key Lab Magnet Mol &

    Magnet Informat Mat Inst Chem &

    Culture Sch Chem &

    Mat Sci Linfen 041004 Shanxi Peoples R China;

    Shanxi Normal Univ Minist Educ Key Lab Magnet Mol &

    Magnet Informat Mat Inst Chem &

    Culture Sch Chem &

    Mat Sci Linfen 041004 Shanxi Peoples R China;

    Shanxi Normal Univ Minist Educ Key Lab Magnet Mol &

    Magnet Informat Mat Inst Chem &

    Culture Sch Chem &

    Mat Sci Linfen 041004 Shanxi Peoples R China;

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  • 正文语种 eng
  • 中图分类 化学;无机化学;
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