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Metal-free mesoporous carbon nitride catalyze the Friedel-Crafts reaction by activation of benzene

机译:无金属介孔碳氮化物通过活化苯催化Friedel-Crafts反应

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摘要

Mesoporous graphitic carbon nitride (mpg-C3N4) was synthesized and studied as a metal-free catalyst for Friedel-Crafts acylation of benzene. The synthesis was done by a template method using SiO2 as template and organic chemicals including guanidine hydrochloride (GndCl), dicyandiamide and urea as precursors. Characterizations by XRD, FT-IR, XPS, N-2 physisorption and TEM indicated that the assumed mpg-C3N4 is synthesized irrespective of the precursor used. However, the surface chemistry of mpg-C3N4, evaluated from TGA and CO2-TPD, varied with the precursors and the mass ratio (r) of SiO2 to precursor. Catalytic results showed that the sample prepared using GndCl as precursor and at mass ratio of SiO2 to GndCl equals to 0.7, defined as mpg-C3N4_G((0.7)), exhibits the best activity for the reactions, due to its rich surface basic sites and high surface area. Thus 89% conversion was obtained within 30 min using hexanoyl chloride as electrophile at 90 degrees C. Even at room temperature (27 degrees C), 75% conversion can be observed within 30 min. The catalyst is also reusable with ca. 80% activities recoverable after washing with ethanol. The excellent catalytic performances, as well as its low cost, straightforward synthesis and metal-free characters, make mpg-C3N4_G((0.7)) a potential catalyst for Friedel-Crafts acylation of benzene in industry with a "green" route.
机译:合成介孔的石墨碳碳氮化物(MPG-C3N4)并研究作为苯的Friedel-Crafts酰化的无金属催化剂。该合成通过使用SiO 2作为模板和有机化学品,包括盐酸胍(GNDCl),双氰胺和尿素作为前体的模板和有机化学品来完成。 XRD,FT-IR,XPS,N-2理由和TEM的特征表明,不管使用的前体如何合成假定的MPG-C3N4。然而,MPG-C3N4的表面化学,由TGA和CO2-TPD评价,与前体和SiO 2的质量比(R)变化至前体。催化结果表明,使用GNDCl作为前体和SiO 2至GndCl的质量比等于0.7的样品,其定义为MPG-C3N4_G((0.7)),由于其富含表面碱性基本位点,表现出反应的最佳活性。高表面积。因此,在30分钟内使用六氧酰氯在30分钟内得到89%转化率,即使在室温(27℃)下,可以在30分钟内观察75%转化。催化剂也可与CA重复使用。用乙醇洗涤后80%的活性可恢复。优异的催化性能以及其低成本,直接合成和无金属特征,使MPG-C3N4_G((0.7))具有“绿色”途径的Friedel-Crafts苯并处理的潜在催化剂。

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  • 来源
    《RSC Advances》 |2015年第68期|共7页
  • 作者单位

    South Cent Univ Nationalities Key Lab Catalysis &

    Mat Sci State Ethn Affairs &

    Minist Educ Wuhan 430074 Peoples R China;

    South Cent Univ Nationalities Key Lab Catalysis &

    Mat Sci State Ethn Affairs &

    Minist Educ Wuhan 430074 Peoples R China;

    South Cent Univ Nationalities Key Lab Catalysis &

    Mat Sci State Ethn Affairs &

    Minist Educ Wuhan 430074 Peoples R China;

    South Cent Univ Nationalities Key Lab Catalysis &

    Mat Sci State Ethn Affairs &

    Minist Educ Wuhan 430074 Peoples R China;

    Heilongjiang Univ Sch Chem &

    Mat Key Lab Funct Inorgan Mat Chem Minist Educ Harbin 150080 Peoples R China;

    South Cent Univ Nationalities Key Lab Catalysis &

    Mat Sci State Ethn Affairs &

    Minist Educ Wuhan 430074 Peoples R China;

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  • 正文语种 eng
  • 中图分类 化学;
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