多相催化CO2参与的炔烃C−H键羧基化反应研究进展

Advances in heterogeneous catalytic C−H bond carbonylation of alkynes with CO2

  • 摘要: 炔烃C−H键与CO2羧基化生成丙炔酸类化合物符合原子经济理念,在有机、医药中间体合成领域具有重要研究意义。在“碳达峰、碳中和”的背景下,该反应也是一种实现CO2高值化利用的有效途径。目前,该反应体系主要通过均相催化进行,但由于多相催化体系易于分离、回收等优点,多相催化炔烃C−H键与CO2羧基化也逐步引起了关注。基于C−H键和CO2的活化机制,目前,围绕铸币金属催化剂开展了相关研究,通过铸币金属与载体协同作用,促进C−C键的耦合,实现丙炔酸类化合物的合成。本工作综述了炔烃C−H键与CO2羧基化的多相催化体系,对体系活化、羧基化反应机理、催化剂的结构特性进行了分析和总结,为后期开发高效羧基化多相催化剂及相关工艺提供了研究思路。

     

    Abstract: The carboxylation of C−H bond of terminal alkyne with CO2 to propargylic acid compounds conforms to the concept of green chemistry, which plays an important role in the field of organic and pharmaceutical intermediate synthesis. Under the background of "Carbon peaking and carbon neutrality", this reaction is also an effective way to realize the high value utilization of CO2. At present, this reaction system is mainly carried out through homogeneous catalysis. However, due to the advantages of heterogeneous catalysis system such as easy separation and recovery, heterogeneous catalytic C−H bond carbonylation of alkynes with CO2 has also gradually attracted attention. Based on the activation mechanism of C−H bond and CO2, relevant research has been carried out over coin metal catalysts. Through the synergistic effect of coin metal and carrier, the coupling of C−C bond is promoted to achieve the synthesis of propargylic acid compounds. In this paper, the heterogeneous catalytic C−H bond carbonylation of alkynes with CO2 is systematically reviewed. The activation of the system, the mechanism of carboxylation reaction, and the structural characteristics of the catalyst are analyzed and summarized, which provides a research idea for the development of efficient heterogeneous catalyst for carboxylation and related processes.

     

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