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Reaction Enhancement Mechanism Of The Nonthermal Discharge And Catalyst Hybrid Reaction For Methane Reforming

机译:甲烷重整用非热放电与催化剂混合反应的反应增强机理

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摘要

The reaction enhancement mechanism of methane steam reforming (MSR) in the nonthermal discharge and catalyst hybrid reaction is presented. Coke deposited on Al_2O_3-supported Ni catalyst was investigated using temperature-programmed oxidation (TPO) analysis and micro-Raman spectroscopy. Although methane conversion in the hybrid reaction is greater than that of normal catalytic reforming, the normal reaction deposited 5 times more coke than the hybrid reaction. Raman spectroscopy revealed that the superposition of the nonthermal discharge on catalysts produced less graphitized coke compared to the normal catalytic reaction, by which it is easily removed by H_2O during steam reforming. Excited species produced by nonthermal discharge are so reactive that their reaction is completed only on the pellet surface: coke formation in the catalyst pore was only slightly detectable. In contrast, large amounts of coke were detected from the surface and catalyst pores in the normal reaction. In the hybrid reaction, CH4 and H_2O are primarily excited by electron impact. Therefore, methane dehydrogenation followed by coke oxidation is promoted, resulting in a small amount of coke formation with greater methane conversion than in the normal reaction. The results are well-correlated with Arrhenius plot analysis of the overall forward rate constant for MSR in the hybrid reaction.
机译:提出了甲烷在非热排放和催化剂混合反应中蒸汽重整反应的机理。使用程序升温氧化(TPO)分析和显微拉曼光谱研究了沉积在Al_2O_3负载的Ni催化剂上的焦炭。尽管杂化反应中的甲烷转化率比常规催化重整的甲烷转化率大,但常规反应沉积的焦炭是杂化反应的5倍。拉曼光谱法显示,与常规催化反应相比,催化剂上非热放电的叠加产生的石墨化焦炭较少,因此在蒸汽重整过程中很容易被H_2O去除。通过非热放电产生的兴奋物质具有很高的反应性,以至于它们的反应仅在颗粒表面完成:仅轻微检测到催化剂孔中焦炭的形成。相反,在正常反应中从表面和催化剂孔中检测到大量焦炭。在杂化反应中,CH4和H_2O主要被电子撞击激发。因此,与常规反应相比,促进了甲烷脱氢和焦炭氧化,导致形成少量的焦炭,并且甲烷转化率更高。结果与杂化反应中MSR的总正向速率常数的Arrhenius图分析非常相关。

著录项

  • 来源
    《Energy & fuels》 |2008年第6期|p.3600-3604|共5页
  • 作者单位

    Department of Mechanical and Control Engineering, Tokyo Institute of Technology, 2-12-1 O-okayama, Meguro, Tokyo 1528552, Japan;

  • 收录信息 美国《科学引文索引》(SCI);美国《工程索引》(EI);美国《生物学医学文摘》(MEDLINE);
  • 原文格式 PDF
  • 正文语种 eng
  • 中图分类 TK-;
  • 关键词

  • 入库时间 2022-08-18 00:42:40

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