Highly Efficient Hydroformylation of 1‐Hexene over an ortho‐Metallated Rhodium(I) Complex Anchored on a 2D‐Hexagonal Mesoporous Material

Highly Efficient Hydroformylation of 1‐Hexene over an ortho‐Metallated Rhodium(I) Complex Anchored on a 2D‐Hexagonal Mesoporous Material
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DOI:
10.1002/ejic.201000844
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发表时间:
2011
影响因子:
2.3
通讯作者:
Mahasweta Nandi;P. Mondal;Manirul Islam;A. Bhaumik
Mahasweta Nandi;P. Mondal;Manirul Islam;A. Bhaumik
中科院分区:
化学3区
文献类型:
--
作者:
Mahasweta Nandi;P. Mondal;Manirul Islam;A. Bhaumik

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加氢甲酰化反应是一类重要的反应,因为它增加了烯烃分子的碳链长度。 RhI 络合物通常用作该反应的催化剂,尽管它们在分离和回收方面具有严重的缺点。通过表面活性剂模板途径合成了苯基官能化的二维六方介孔二氧化硅材料。这种中孔材料的苯基通过硝化进行官能化,然后还原成胺衍生物。胺基团进一步进行希夫碱缩合,然后将 RhI 络合物在其表面上异质化,产生锚定在介孔二氧化硅基质上的邻位金属化络合物。这些材料已通过粉末 X 射线衍射、透射电子显微镜和氮气吸附/解吸研究进行了表征。负载RhI的介孔材料作为1-己烯加氢甲酰化反应的非常有效的催化剂,并且在50巴压力下、在H2/CO存在下、在343K下对正庚醛的形成表现出高选择性。
The hydroformylation reaction is an important class of reaction as it enhances the carbon chain length of an olefin molecule. RhI complexes are conventionally used as the catalyst for this reaction although they possess severe drawbacks with respect to separation and recycling. A phenyl-functionalised 2D-hexagonal mesoporous silica material has been synthesised by a surfactant templating pathway. The phenyl group of this mesoporous material was functionalised through nitration, followed by its reduction to the amine derivative. The amine group was further subjected to Schiff-base condensation, and the RhI complex was then heterogenised over its surface to yield the ortho-metallated complex anchored on the mesoporous silica matrix. The materials have been characterised by using powder X-ray diffraction, transmission electron microscopy and nitrogen adsorption/desorption studies. The RhI-loaded mesoporous material acts as a very efficient catalyst for the hydroformylation reaction of 1-hexene and exhibits high selectivity towards the formation of n-heptanal at 343 K in the presence of H2/CO at 50 bar pressure.