聚卟啉的制备及其在光氧化催化反应中的应用
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国家自然科学基金项目(面上项目,重点项目,重大项目)


Preparation of polyporphyrin and its application in photocatalysis
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The National Natural Science Foundation of China (General Program, Key Program, Major Research Plan)

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    摘要:

    通过Sonogashira偶联聚合制备了一系列具有多孔结构的网状交联聚卟啉作为光催化剂,解决单体卟啉在光催化过程中的分离、循环利用及产物纯化困难等问题,具体工作如下:设计了两种结构的卟啉单体,双溴双炔卟啉和四溴卟啉,通过双溴双炔卟啉自聚得到多孔有机聚卟啉(PPOP-1),通过四溴卟啉与含双炔基的单体(1,7-辛二炔、对苯二炔、联苯二炔)共聚得到聚卟啉PPOP-2、PPOP-3和PPOP-4。通过扫描电镜和物理吸附仪观测聚合物的表面形貌和表征孔结构,结果显示这四种聚合物均具有均匀颗粒的形态和微孔结构。以PPOPs为异相光催化剂,通过可见光诱导二苄胺、缩硫酮、二苄基硫醚的有氧氧化证实了其对C-N和C-S键的氧化均具有优于单体催化剂的催化活性,且经过五次循环催化后,PPOPs依然保持较高的催化活性。

    Abstract:

    A library of cross-linked poly-porphyrins with porous and network structures were prepared via the Sonogashira polymerization method to address the issues of the porphyrin monomers in separation, recycling and purification during the photocatalytic process. Two types of porphyrin monomers (dibromodiacetylenic porphyrin and tetrabromoporphyrin) were designed and the porphyrin-based porous organic polymer (PPOP-1) was obtained through self-polymerization of dibromodiacetylenic porphyrin and three poyporphyrins were obtained through the copolymerization of tetrabromoporphyrin and various linkers containing dialkynes (1, 7-octadiyne, p-phenylenediyne, and biphenyl). The surface morphology and pore structure of the polymers are characterized by scanning electron microscopy and physical adsorption. All four polymers had uniform ellipsoid morphology and microporous structures. PPOPs were used as metal-free heterogeneous photocatalysts and the photocatalytic activity for C-N and C-S bonds were confirmed through the visible light-induced oxidation of dibenzylamine, bisaminothioketal and dibenzyl sulfide. The PPOPs maintained excellent catalytic activity after five cycles.

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马卉,徐翔,郑玉斌,宋汪泽.聚卟啉的制备及其在光氧化催化反应中的应用[J].精细化工,2021,38(9):

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  • 收稿日期:2021-02-17
  • 最后修改日期:2021-04-29
  • 录用日期:2021-04-29
  • 在线发布日期: 2021-08-05
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