科研之友
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摘要
The present research deals with catalyst development for the utilization of CO(2) in dry reforming of methane with the aim of reaching highest yield of the main product synthesis gas (CO, H(2)) at lowest possible temperatures. Therefore, Ni-Pd bimetallic supported catalysts were prepared by simple impregnation method usingvarious carriers. The catalytic performance of the catalysts was investigated at 500, 600 and 700 degrees C under atmospheric pressure and a CH(4) to CO(2) feed ratio of 1. Fresh, spent and regenerated catalysts were characterized by N(2) adsorption for BET surface area determination, XRD, ICP, XPS and TEM. The catalytic activity of the studied Ni-Pd catalysts depends strongly on the support used and decreases in the following ranking: ZrO(2)-La(2)O(3), La(2)O(3) > ZrO(2) > SiO(2) > Al(2)O(3) > TiO(2). The bimetallic catalysts were more active than catalysts containing Ni or Pd alone. A Ni to Pd ratio = 4 at a metal loading of 7.5 wt% revealed the best results. Higher loading lead to increased formation of coke; partly in shape of carbon nanotubes (CNT) as identified by TEM. Furthermore, the effect of different calcination temperatures was studied; 600 degrees C was found to be most favorable. No effect on the catalytic activity was observed if a fresh catalyst was pre-reduced in H(2) prior to use or spent samples were regenerated by air treatment. Ni and Pd metal species are the active components under reaction conditions. Best conversions of CO(2) of 78% and CH(4) of 73% were obtained using a 7.5 wt% NiPd (80:20) ZrO(2)-La(2)O(3) supported catalyst at a reaction temperature of 700 degrees C. CO and H(2) yields of 57% and 59%, respectively, were obtained.
- 出版日期2009-9-25
