首页> 外文期刊>Chemistry: A European journal >Catalytic and mechanistic insights of the low-temperature selective oxidation of methane over Cu-promoted Fe-ZSM-5
【24h】

Catalytic and mechanistic insights of the low-temperature selective oxidation of methane over Cu-promoted Fe-ZSM-5

机译:铜促进的Fe-ZSM-5上甲烷的低温选择性氧化的催化和机理研究

获取原文
获取原文并翻译 | 示例
           

摘要

The partial oxidation of methane to methanol presents one of the most challenging targets in catalysis. Although this is the focus of much research, until recently, approaches had proceeded at low catalytic rates (<10 h ~(-1)), not resulted in a closed catalytic cycle, or were unable to produce methanol with a reasonable selectivity. Recent research has demonstrated, however, that a system composed of an iron- and copper-containing zeolite is able to catalytically convert methane to methanol with turnover frequencies (TOFs) of over 14 000 h~(-1) by using H_2O _2 as terminal oxidant. However, the precise roles of the catalyst and the full mechanistic cycle remain unclear. We hereby report a systematic study of the kinetic parameters and mechanistic features of the process, and present a reaction network consisting of the activation of methane, the formation of an activated hydroperoxy species, and the by-production of hydroxyl radicals. The catalytic system in question results in a low-energy methane activation route, and allows selective C_1-oxidation to proceed under intrinsically mild reaction conditions. Activate methane! A reaction network consisting of the activation of methane, the formation of an activated hydroperoxy species, and the by-production of hydroxyl radicals is presented (see scheme). The catalytic system results in a low-energy methane activation route, and allows selective C_1-oxidation to proceed under intrinsically mild reaction conditions.
机译:甲烷部分氧化为甲醇是催化中最具挑战性的目标之一。尽管这是许多研究的重点,但直到最近,方法仍以低催化速率(<10 h〜(-1))进行,未导致封闭的催化循环或无法以合理的选择性生产甲醇。然而,最近的研究表明,由含铁和铜的沸石组成的系统能够通过以H_2O _2为末端,将甲烷转化为周转频率(TOF)超过14000 h〜(-1)的甲醇。氧化剂。然而,催化剂的确切作用和整个机械循环仍然不清楚。我们在此报告该过程的动力学参数和力学特征的系统研究,并提出了一个由甲烷的活化,活化的氢过氧物质的形成以及羟基自由基的副产物组成的反应网络。所讨论的催化系统导致低能的甲烷活化路线,并允许在固有的温和反应条件下进行选择性的C_1氧化。激活甲烷!提出了一种由甲烷的活化,活化的氢过氧物质的形成以及羟基自由基的副产物组成的反应网络(参见方案)。催化系统产生低能的甲烷活化路线,并允许在固有的温和反应条件下进行选择性C_1氧化。

著录项

相似文献

  • 外文文献
  • 中文文献
  • 专利
获取原文

客服邮箱:kefu@zhangqiaokeyan.com

京公网安备:11010802029741号 ICP备案号:京ICP备15016152号-6 六维联合信息科技 (北京) 有限公司©版权所有
  • 客服微信

  • 服务号