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Direct hydroxylation of benzene to phenol with molecular oxygen over vanadium oxide nanospheres and study of its mechanism

机译:用分子氧对氧化钒纳米球的分子氧直至苯酚的直接羟基化及其机理研究

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摘要

Direct hydroxylation of benzene to phenol using molecular oxygen is a green route with high atom economy but still a great challenge when compared with the existing method of production. The activation of oxygen is necessary and reductive agents were used to activate dioxygen in a so-called “reductive activation” process. Here, nano vanadium oxides that consist mainly of low valence vanadium to activate dioxygen were prepared under different conditions via a hydrothermal method. Under the optimized conditions, an excellent phenol selectivity of 96.3% with benzene conversion of 4.2% was achieved over the VOC2O4-N-5 without reductive agents. Characterizations revealed that VOC2O4-N-5 was composed of a mesoporous nanosphere structure with medium strong acid sites and low valence vanadium species. A mechanism was proposed as follows: dioxygen was activated by low valence vanadium in VOC2O4-N-5 to produce the active oxygen species which oxidized acetic acid to peracetic acid. Then the active oxygen species was subsequently transferred from peracetic acid to benzene and inserted into the C-H bond to give phenol.
机译:使用分子氧的苯对苯酚的直接羟基化是具有高原子经济的绿色途径,但与现有的生产方法相比,仍然是一个巨大的挑战。氧气的活化是必要的,并且还原剂用于在所谓的“还原活化”过程中激活二恶英。这里,在不同的条件下,通过水热法制备主要由低价钒组成的纳米钒氧化物以激活二恶英制备。在优化条件下,在没有还原剂的情况下,在VOC 2 O 4-N-5上实现了96.3%的优异酚选择性96.3%。特征揭示了VOC2O4-N-5由中孔纳米结构组成,其中具有中强酸位点和低价钒物种。提出了如下方法:通过VOC 2 O 4-N-5中的低价钒活化DiOxygen,以产生氧化乙酸至过乙酸的活性氧物质。然后随后将活性氧物质从过乙酸转移到苯中并将其插入C-H键中以提供苯酚。

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  • 来源
    《RSC Advances》 |2015年第114期|共7页
  • 作者单位

    School of Chemistry and Material Science College of Chemistry Chemical Engineering and Environmental Engineering Liaoning Shihua University Liaoning Fushun 113001 China.;

    School of Chemistry and Material Science College of Chemistry Chemical Engineering and Environmental Engineering Liaoning Shihua University Liaoning Fushun 113001 China.;

    School of Chemistry and Material Science College of Chemistry Chemical Engineering and Environmental Engineering Liaoning Shihua University Liaoning Fushun 113001 China.;

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  • 原文格式 PDF
  • 正文语种 eng
  • 中图分类 化学;
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