...
  • 主题
高级搜索  >
历史搜索 清空历史
首页> 外文期刊>Catalysis science & technology >Reaction mechanism of dimethyl ether carbonylation to methyl acetate over mordenite a combined DFT/experimental study
【24h】

Reaction mechanism of dimethyl ether carbonylation to methyl acetate over mordenite a combined DFT/experimental study

机译：二甲醚羰基化反应的反应机理对乙酸甲酯在丝光沸石的总和DFT /实验研究

获取原文
获取原文并翻译 | 示例
           
页面导航
  • 摘要
  • 著录项
  • 相似文献
  • 相关主题

摘要

The reaction mechanism of dimethyl ether carbonylation to methyl acetate over mordenite was studied theoretically with periodic density functional theory calculations including dispersion forces and experimentally in a fixed bed flow reactor at pressures between 10 and 100 bar, dimethyl ether concentrations in CO between 0.2 and 2.0%, and at a temperature of 438 K. The theoretical study showed that the reaction of CO with surface methyl groups, the rate-limiting step, is faster in the eight-membered side pockets than in the twelve-membered main channel of the zeolite; the subsequent reaction of dimethyl ether with surface acetyl to form methyl acetate was demonstrated to occur with low energy barriers in both the side pockets and in the main channel. The present analysis has thus identified a path, where the entire reaction occurs favourably on a single site within the side pocket, in good agreement with previous experimental studies. The experimental study of the reaction kinetics was consistent with the theoretically derived mechanism and in addition revealed that the methyl acetate product inhibits the reaction - possibly by sterically hindering the attack of CO on the methyl groups in the side pockets.
机译：二甲醚的反应机理羰基化反应在丝光沸石乙酸甲酯从理论上研究了周期性的密度功能理论计算包括色散力,在一个固定的实验床流反应堆压力介于10到100之间酒吧,二甲醚浓度之间的有限公司2.0%和0.2,在温度为438 K。理论研究表明,公司的反应表面甲基,病原一步,更快的8人口袋比十二主要通道沸石;二甲醚与表面乙酰甲基形式醋酸发生了较低的能量障碍在侧袋和在主通道。一个路径,整个反应发生看好一个站点内的一面与先前的口袋,在良好的协议实验研究。反应动力学是一致的从理论上推导出机制,此外透露,乙酸甲酯产品抑制反应——可能sterically阻碍有限公司在甲基的攻击口袋。

著录项

相似文献

  • 外文文献
  • 中文文献
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