摘要
The catalysts Ni/Al2O3, Ni/ZrO2-CeO2-Al2O3 and Ni/CuO-ZrO2-CeO2-Al2O3 were prepared by the co-precipitation method at a pH of 9 using Na2CO3 as the precipitant. The Ni loading(mass fraction) of the catalysts was 10%. The ignition process on the catalysts for the autothermal reforming of methane to hydrogen was investigated and the surface properties of the catalysts were characterized by XPS. The results showed that the Ni/Al2O3 catalyst could not ignite the process of autothermal reforming of methane to hydrogen. However, the Ni/CuO-ZrO2-CeO2-Al2O3 catalyst could ignite the process of autothermal reforming of methane to hydrogen at lower reaction temperature(650 ℃) with the conversion of methane reaching 76%. The result of XPS analysis indicated that the promoters could change the binding energy(BE) of Ni2p3/2 obviously. The species of Cu in the Ni/CuO-ZrO2-CeO2-Al2O3 catalyst comprised Cu2 O and Cu2+. The formation of ZrO2-CeO2 solid solution and a large amount of Cu2 O might be the reason leading to good oxygen storage capacity and mobility of lattice oxygen of the Ni/CuO-ZrO2-CeO2-Al2O3 catalyst, which could ignite the process of autothermal reforming of methane to hydrogen at lower reaction temperature.
The catalysts Ni/Al2O3, Ni/ZrO2-CeO2-Al2O3 and Ni/CuO-ZrO2-CeO2-Al2O3 were prepared by the co-precipitationmethod at a pH of 9 using Na2CO3 as the precipitant. The Ni loading (mass fraction) of the catalysts was 10%. The ignitionprocess on the catalysts for the autothermal reforming of methane to hydrogen was investigated and the surface properties ofthe catalysts were characterized by XPS. The results showed that the Ni/Al2O3 catalyst could not ignite the process of autothermalreforming of methane to hydrogen. However, the Ni/CuO-ZrO2-CeO2-Al2O3 catalyst could ignite the process of autothermalreforming of methane to hydrogen at lower reaction temperature (650 ℃) with the conversion of methane reaching76%. The result of XPS analysis indicated that the promoters could change the binding energy (BE) of Ni2p3/2 obviously. Thespecies of Cu in the Ni/CuO-ZrO2-CeO2-Al2O3 catalyst comprised Cu2O and Cu2+. The formation of ZrO2-CeO2 solid solutionand a large amount of Cu2O might be the reason leading to good oxygen storage capacity and mobility of lattice oxygenof the Ni/CuO-ZrO2-CeO2-Al2O3 catalyst, which could ignite the process of autothermal reforming of methane to hydrogenat lower reaction temperature.
基金
supported by the Guangdong Provincial Natural Science Foundation (030514)
the Science and Technology Plan of Guangdong Province of China (2004B33401006)
the Doctoral Startup Foundation of Guangdong Pharmaceutical University