In Situ Fourier Transform Infrared (FTIR) Study of Nonthermal-Plasma-Assisted Methane Oxidative Conversion
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  • 作者:S. A. Nair ; Tomohiro Nozaki ; Ken Okazaki
  • 刊名:Industrial & Engineering Chemistry Research
  • 出版年:2007
  • 出版时间:May 23, 2007
  • 年:2007
  • 卷:46
  • 期:11
  • 页码:3486 - 3496
  • 全文大小:809K
  • 年卷期:v.46,no.11(May 23, 2007)
  • ISSN:1520-5045
文摘
Nonthermal plasma-assisted methane conversion has been widely investigated as a potential low-temperatureprocess. The desired end objective is synthesis gas production, one-step production of liquid oxygenates, orcoupling products. Either oxygen or steam or both is used as a second reactant or reactants, to provide additionalO atoms and initiate plasma-assisted radical processing. The present paper intends to investigate the variouspossible products/reactive species that are formed during plasma processing. In situ Fourier transform infrared(FTIR) absorption spectrometry is used to monitor the products/reactive groups. Experiments are performedat room temperature and at low energy inputs (50 kJ/(mol CH4)) in a gas mixture of CH4/O2/N2/H2O(atmospheric humidity). In the absence of oxygen, alkane, alkene, and alkyne groups are formed as the products,which indicates termination reactions. With increasing oxygen concentration (11, 15, and 33%) a gradualshift from alkane to a -CHO group is observed. In addition, alcohol group formation is detected withoxygen input, which indicates coupling between the CH4 dissociation products and the O radicals as a primarystep. The effect of higher energy input and the presence of catalytic surfaces such as platinum also areinvestigated.

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