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首页> 外文期刊>RSC Advances >Fabrication and catalytic properties of ordered cyclopalladated diimine monolayer : investigation on catalytic mechanism
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Fabrication and catalytic properties of ordered cyclopalladated diimine monolayer : investigation on catalytic mechanism

机译：有序环钯二嘧啶单层的制备和催化性能：催化机制研究

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摘要

Channel-like self-assembled monolayers having aliphatic and aromatic diimines (denoted as Si@1DIS, Si@2DIS and Si@3DIS) immobilized on substrates and their palladacycle monolayers (Si@1DIS-Pd, Si@2DIS-Pd and Si@3DIS-Pd) were prepared and characterized. Their catalytic performances were investigated using the Suzuki coupling reaction as a model. Si@3DIS-Pd showed the highest catalytic activity in water without ligands, and better recyclability than that of Si@2DIS-Pd and Si@1DIS-Pd. The reason was the carbon in the aliphatic diimine of Si@2DIS-Pd and Si@1DIS-Pd was easily hydrolyzed because of the active hydrogen of -C, resulting in poor recyclability. Control of the amount of catalyst could be achieved by modulating the diameter of the channel-like structure, which also affected the catalytic activity. The catalytic process and mechanism were investigated systematically and proposed based on the experimental results obtained by the water contact angle, ultraviolet spectroscopy, X-ray photoelectron spectroscopy, cyclic voltammetry and atomic force spectroscopy. Changes in the morphology of monolayer surfaces during the catalytic process with or without stirring presented a clear process from order to disorder, and indicated that the reaction was a heterogeneous catalytic process occurring on the surface of the catalyst monolayer.
机译：具有脂族和芳族二胺的频道的自组装单层（表示为Si @ 1dis，Si @ 2dis和si @ 3dis），其固定在底物上和它们的钯单层（Si @ 1dis-pd，Si @ 2dis-pd和Si @ 3dis -PD）制备并表征。使用Suzuki偶联反应作为模型研究了它们的催化性能。 SI @ 3DIS-PD在没有配体的情况下显示出最高的催化活性，比SI @ 2DIS-PD和SI @ 1DIS-PD更好的可再循环性。原因是由于-C的活性氢，Si @ 2dis-Pd的脂族二亚胺和Si @ 1dis-pd的碳容易水解，导致可回收性差。通过调节沟道状结构的直径，可以通过调节催化活性的直径来实现催化剂的量。基于通过水接触角，紫外光谱，X射线光电子能谱，环伏安法和原子力光谱获得的实验结果，对催化过程和机理进行了系统和提出。单层表面在催化过程中的变化在催化过程中或不搅拌的催化过程中呈现出澄清的方法，从顺序排序，表明反应是在催化剂单层表面上发生的非均相催化过程。

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  • 来源
    《RSC Advances》 |2018年第56期|共8页
  • 作者

    Wang Linhong; Huang Pingping; Yang Jun; Li Tiesheng; Mao Luyuan; Liu Minghua; Wu Yangjie;

  • 作者单位

    Coll Chem &

    Mol Engn Key Lab Chem Biol &

    Organ Chem Henan Prov Key Lab Nanoinformat Mat Zhengzhou Zhengzhou 450001 Henan Peoples R China;

    Coll Chem &

    Mol Engn Key Lab Chem Biol &

    Organ Chem Henan Prov Key Lab Nanoinformat Mat Zhengzhou Zhengzhou 450001 Henan Peoples R China;

    Coll Chem &

    Mol Engn Key Lab Chem Biol &

    Organ Chem Henan Prov Key Lab Nanoinformat Mat Zhengzhou Zhengzhou 450001 Henan Peoples R China;

    Coll Chem &

    Mol Engn Key Lab Chem Biol &

    Organ Chem Henan Prov Key Lab Nanoinformat Mat Zhengzhou Zhengzhou 450001 Henan Peoples R China;

    Zhengzhou Univ Coll Mat Sci &

    Engn Zhengzhou 450001 Henan Peoples R China;

    Chinese Acad Sci Inst Chem Beijing Natl Lab Mol Sci Beijing 100190 Peoples R China;

    Coll Chem &

    Mol Engn Key Lab Chem Biol &

    Organ Chem Henan Prov Key Lab Nanoinformat Mat Zhengzhou Zhengzhou 450001 Henan Peoples R China;

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  • 正文语种 eng
  • 中图分类 化学;
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