亚苯胺基偶联锰卟啉聚合物的合成及对醇的催化氧化研究
首发时间:2015-06-08
摘要:本文基于Buchwald-Hartwing芳胺化反应,以卡宾钯配合物作为催化剂,首次合成了一系列以亚苯胺基桥联的,具有稳定多孔结构的共轭金属卟啉聚合物MnP-AMP。得到的聚合物具有网状超共轭结构,卟啉环中的锰离子得到进一步的活化。通过SEM、TEM以及BET表征发现该类聚合物具有均一的孔径结构和较大的比表面积。实验发现,大量C-N桥键的引入使得聚合物极性增大,与醇化合物的亲和性强,在催化空气氧化醇化合物的反应中表现出很高催化活性。在乙腈溶剂中非均相催化空气氧化苯甲醇的过程中,底物完全转化,醛选择性达到98%。催化剂重复利用多次依然具有很好的催化效果。
关键词: 工业催化 含氮杂环卡宾 芳胺化反应 金属卟啉共轭聚合物 醇类催化氧化
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Synthesis of Conjugated Mn Porphyrin Polymers with PPD building blocks and Research on Catalytic Oxidation of alcohols
Abstract:This article discribed the synthesis of a series of conjugated metalloporphyrin polymers (MnP-AMP) based on Buchwald-Hartwing aromatic amination with p-phenylenediamine buliding blocks and used N-heterocyclic carbene-palladium complex as catalyst. MnP-AMP has stable porous and super reticular conjugated structure which further activates the manganese ions in porphyrin ring. The test result of FT IR, SEM, and TEM showed that the polymers have large surface area and uniform pore size. Experiments found that the introduction of C-N adds polymer polarity and affinity for alcohols. MnP-AMP exhibited excellent catalytic activity when applied to aerobic oxidation of alcohols and catalysed the selective oxidation of benzyl alcohol to benzaldehyde by air and pivaladehyde, conversation up to 100% and aldehyde selectivity up to 98%, under mild condition in acetonitrile at 40℃. MnP-AMP also has high catalytic activity after several recycles.
Keywords: industrial catalysis N-heterocyclic carbene aromatic amination conjugated metalloporphyrin polymer catalytic oxidation of alcohols
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亚苯胺基偶联锰卟啉聚合物的合成及对醇的催化氧化研究
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