Partial oxidation of CH4, CO2 reforming of CH4, and oxidative CO2 reforming of CH4 to produce synthesis gas at 700°C over supported Ni catalysts have been studied. A Ni/Mg-Al catalyst was prepared by the solid phase crystallization (spc-) method starting from a hydrotalcite-type (HT) anionic precursor. From XRD analysis, only Ni0.5Mg2.5Al catalyst consists of the layered hydrotalcite-type structure; not Ni0.5Ca2.5Al and Ni/Al2O3 catalysts. By TPR test, the Ni0.5Mg2.5Al-HT catalyst requires a high reduction temperature than the Ni0.5Ca2.5Al catalyst. It implies that the Ni0.5Mg2.5Al-HT which has a layered structure shows the stronger interaction strength between the molecules. It might increase the resistance of coke formation on the surface of the catalyst. For the reaction tests, the Ni0.5Ca2.5Al showed the highest initial activity for synthesis gas production for all reactions; but, its activity was decreased quickly due to coke formation except during the partial oxidation of CH4. The Ni0.5Mg2.5Al-HT showed a relatively higher reactivity compared to the equilibrium level than Ni/Al2O3 catalyst; and it shows very stable reactivity than other catalysts. By TPO test, the Ni0.5Mg2.5Al-HT has the lower amount of coke formed during the reaction than the Ni0.5Ca2.5Al catalyst. It confirms that the Ni0.5Mg2.5Al-HT catalyst has stronger resistance to coke formation; and it leads to provide stable reactivity in any reforming conditions at high temperature. Therefore, the Ni0.5Mg2.5Al-HT catalyst was the most promising catalyst in terms of activity and stability for partial oxidation, CO2 reforming, and oxidative CO2 reforming of CH4.
The Ni0.5Mg2.5Al-HT catalyst was used to investigate the CO2 reforming of CH4 kinetics. With increasing CH4 partial pressures at constant CO2 partial pressure, the rates of CH4 consumption were increased. However, with increasing CO2 partial pressure at constant CH4 partial pressure, CH4 consumption rates was increased at lower CO2 partial pressure, but turned to independent at higher CO2 partial pressure. When the partial pressure of H2 was increased, the CO formation rate was decreased; it confirmed that the reverse water-gas shift (RWGS) reaction was occurring during the CO2 reforming of CH4 reaction. In addition, the reaction kinetic expression was proposed when the CH4 dissociation step was considered as a rate-limiting step.
| Identifer | oai:union.ndltd.org:WATERLOO/oai:uwspace.uwaterloo.ca:10012/5375 |
| Date | January 2010 |
| Creators | Song, Hoon Sub |
| Source Sets | University of Waterloo Electronic Theses Repository |
| Language | English |
| Detected Language | English |
| Type | Thesis or Dissertation |
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