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Epoxidation of propylene in the gas phase

机译:气相中丙烯的环氧化

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摘要

The gas-phase epoxidation of propylene using N2O, air and air-ammonia mixture as an oxidants was studied. Propylene can be epoxidized by nitrous oxide with a yield as high as 13.3% over silica supported iron oxide catalysts modified by amines. The iron oxide dispersion, the acidity of the support and the nitrogen-containing modifiers are the key factors determining the catalytic performance. We suggest a reaction pathway involving two concurrent mechanisms: the radical oxidation of propylene to acroleine, hexanediene, etc., and a non-radical oxidation leading to epoxide. Propylene is epoxidized with air over silica-supported iron oxide catalysts at a conversion of about 0.2%. Using air as an oxidizing agent, the presence of gaseous ammonia improves the propylene conversion by 10-fold preserving the considerable selectivity (up to 60%). This observation suggests a reaction mechanism involving the oxidation of ammonia to nitrous oxide in the first step, which subsequently produces active oxygen species, which selectively oxidize propylene to propylene oxide (PO).
机译:研究了以N2O,空气和气氨混合物为氧化剂的丙烯气相环氧化反应。丙烯可以被一氧化二氮环氧化,其产率比经胺改性的二氧化硅负载的氧化铁催化剂高13.3%。氧化铁分散体,载体的酸度和含氮改性剂是决定催化性能的关键因素。我们提出了一种反应途径,该途径涉及两个同时发生的机理:丙烯自由基氧化为丙烯醛,己二烯等,以及非自由基氧化导致环氧化物。丙烯在二氧化硅负载的氧化铁催化剂上用空气环氧化,转化率为约0.2%。使用空气作为氧化剂,气态氨的存在将丙烯转化率提高了10倍,同时保留了相当高的选择性(最高60%)。该观察结果表明在第一步中涉及将氨氧化为一氧化二氮的反应机理,其随后产生活性氧,其将丙烯选择性氧化为环氧丙烷(PO)。

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  • 来源
    《Topics in Catalysis》 |2007年第2期|129-135|共7页
  • 作者单位

    Department of Organic Technology Slovak University of Technology Radlinského 9 Bratislava 81237 Slovak Republic;

    Department of Organic Technology Slovak University of Technology Radlinského 9 Bratislava 81237 Slovak Republic;

    Institut für Anorganische Chemie Rheinische Friedrich-Wilhelms-Universität Gerhard-Domagk-Str. 1 Bonn D-53121 Germany;

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  • 原文格式 PDF
  • 正文语种 eng
  • 中图分类
  • 关键词

    epoxidation; propylene; iron oxide; nitrous oxide; oxygen;

    机译:环氧化;丙烯;氧化铁;一氧化二氮;氧气;

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