...
  • 主题
高级搜索  >
历史搜索 清空历史
首页> 外文期刊>Dalton transactions: An international journal of inorganic chemistry >Carbene insertion into N-H bonds with size-selectivity induced by a microporous ruthenium-porphyrin metal-organic framework
【24h】

Carbene insertion into N-H bonds with size-selectivity induced by a microporous ruthenium-porphyrin metal-organic framework

机译：卡宾插入N-H键，具有由微孔钌 - 卟啉金属 - 有机框架诱导的尺寸选择性

获取原文
获取原文并翻译 | 示例
           
页面导航
  • 摘要
  • 著录项
  • 相似文献
  • 相关主题

摘要

A stable and porous porphyrinic metal-organic framework, Ru-PMOF-1(Hf), has been prepared through the self-assembly of [5,10,15,20-tetrakis(4-carboxyphenyl)porphyrinato](monocarbonyl)ruthenium (Ru(TCPP)(CO)) and HfCl4. Single-crystal X-ray diffraction analysis reveals that Ru-PMOF-1(Hf) possesses a three-dimensional (3D) structure with orthogonal 1D open channels of 1.9 x 1.9 nm(2). The porous nature has been confirmed by gas adsorption measurements. Its catalytic activity for the carbene insertion into N-H bonds has been investigated. The catalytic results indicate that Ru-PMOF-1(Hf) is efficient for the insertion reactions of ethyl 2-diazoacetate (EDA) into a range of secondary amines with up to 92% yield, 938 TON and 2475 h(-1) TOF. As an excellent heterogeneous catalyst, Ru-PMOF-1(Hf) can be recovered and reused for at least ten runs with negligible loss of catalytic activity. Due to its uniform microporosity in three orthogonal directions, Ru-PMOF-1(Hf), of which the particle sizes were carefully controlled by sieving, can induce size selectivity regarding the amine substrates. The reactivities of different unbranched dialkylamines, such as diethylamine (NHEt2), dibutylamine (NHBu2) and dipentylamine (NHPent(2)), have been compared, and the results display an apparent decreasing trend along the chain lengthening. For comparison, the corresponding nonporous and homogeneous catalyst Ru(TMCPP)(CO) (TMCPP = tetrakis(4-methoxycarbonylphenyl)porphyrin) displays negligible difference towards the reactions with these three amines.
机译：通过[5,10,15,20-四羧基）卟啉（甘油烯基）钌（甘油基）钌（氟羰基）钌（氟碳基）钌（ Ru（TCPP）（CO））和HFCL4。单晶X射线衍射分析显示Ru-PMOF-1（HF）具有三维（3D）结构，其正交1D开放通道为1.9×1.9nm（2）。通过气体吸附测量确认多孔性质。已经研究了将Carbene插入N-H键的催化活性。催化结果表明Ru-PMOF-1（HF）是乙基2-二氮乙酸酯（EDA）进入一系列仲胺的仲胺，938吨和2475小时（-1）TOF的仲胺有效。作为优异的非均相催化剂，可以回收Ru-PMOF-1（HF）并重复使用至少10个，其​​损失损失可忽略不计的催化活性。由于其三个正交方向上的均匀微孔，Ru-PMOF-1（HF），其中通过筛分仔细控制粒度，可以诱导关于胺基材的尺寸选择性。已经比较了不同非支撑二烷基胺的反应性，例如二乙胺（NHET2），二丁胺（NHBU2）和二苯胺（NHPENT（2）），结果显示沿链延长的表观降低趋势。为了比较，相应的无孔和均相催化剂Ru（TMCPP）（CO）（TMCPP =四（4-甲氧基羰基苯基）卟啉差异显示出可忽略的差异与这三种胺的反应。

著录项

  • 来源
  • 作者

    Chen Lianfen; Cui Hao; Wang Yanhu; Liang Xiang; Zhang Li; Su Cheng-Yong;

  • 作者单位

    Sun Yat Sen Univ Sch Chem Lehn Inst Funct Mat MOE Lab Bioinorgan &

    Synthet Chem Guangzhou 510275 Guangdong Peoples R China;

    Sun Yat Sen Univ Sch Chem Lehn Inst Funct Mat MOE Lab Bioinorgan &

    Synthet Chem Guangzhou 510275 Guangdong Peoples R China;

    Sun Yat Sen Univ Sch Chem Lehn Inst Funct Mat MOE Lab Bioinorgan &

    Synthet Chem Guangzhou 510275 Guangdong Peoples R China;

    Sun Yat Sen Univ Sch Chem Lehn Inst Funct Mat MOE Lab Bioinorgan &

    Synthet Chem Guangzhou 510275 Guangdong Peoples R China;

    Sun Yat Sen Univ Sch Chem Lehn Inst Funct Mat MOE Lab Bioinorgan &

    Synthet Chem Guangzhou 510275 Guangdong Peoples R China;

    Sun Yat Sen Univ Sch Chem Lehn Inst Funct Mat MOE Lab Bioinorgan &

    Synthet Chem Guangzhou 510275 Guangdong Peoples R China;

  • 收录信息
  • 原文格式 PDF
  • 正文语种 eng
  • 中图分类 化学;无机化学;
  • 关键词

相似文献

  • 外文文献
  • 中文文献
  • 专利
获取原文

客服邮箱：kefu@zhangqiaokeyan.com

京公网安备：11010802029741号 ICP备案号：京ICP备15016152号-6 六维联合信息科技 (北京) 有限公司©版权所有

  • 客服微信

  • 服务号