The influences of CeO2-ZrO2 and γ-Al2O3 mixing methods on the catalytic activity and stability of partial oxidation of methane （POM） were investigated over Ni/Ce0.7Zr0.3O2-Al2O3 catalysts. The catalysts were charac...The influences of CeO2-ZrO2 and γ-Al2O3 mixing methods on the catalytic activity and stability of partial oxidation of methane （POM） were investigated over Ni/Ce0.7Zr0.3O2-Al2O3 catalysts. The catalysts were characterized by XRD, TPR, H2-chemsorption, and TG-DTA. For fresh catalysts, the results showed that the salt precursor mixing catalyst （ATOM） presented better performance than the catalysts prepared by the precipitator mixing method （MOL） and the powder mechanically mixing method （MECH）. The result of XRD suggested that the interaction between CeO2-ZrO2 and Al2O3 in ATOM sample was stronger than the others, which led to more lattice defects and thereby better initial activity. Moreover, the MECH sample had the best stability and the least coke deposition in 24 h stability tests. The results of TPR and H2-chemsorption indicated that the intimate contact of Ni-Al in MECH sample enhanced the ability of resisting coke deposition and metal sintering.展开更多
This study focused on measurement of the autothermal reforming of biogas over a Ni based monolithic catalyst. The effects of the steam/CH4 （S/C） ratio, O2/CH4 （O2/C） ratio and temperature were investigated. The CH...This study focused on measurement of the autothermal reforming of biogas over a Ni based monolithic catalyst. The effects of the steam/CH4 （S/C） ratio, O2/CH4 （O2/C） ratio and temperature were investigated. The CH4 conversions were higher under all examined temperatures than the equilibrium conversion calculated using the blank outlet temperature, because the catalyst layer was heated by the exothermic catalytic partial oxidation reaction. The CH 4conversion increased with increasing O2/C ratio. Moreover, the CH4 conversion was higher than the equilibrium conversion calculated using the blank outlet temperature for O2/C〉0.42 and reached about 100% at O2/C=0.55. However, the hydrogen concentration decreased for O2/C〉0.45 because hydrogen was combusted to steam in the presence of excess oxygen. On the other hand, the hydrogen and CO2 concentrations increased and the CO concentration decreased with increasing SIC ratio. As a result, it was found that the highest hydrogen concentrations and CH4 conversions were attained at the O2/C ratios of 0.45-0.55 and the SIC ratios of 1.5-2.5. Moreover, the H2/CO ratio could also be controlled in the range from about 2 to 3.5 to give at least 90% CH4 conversion, by regulating the O2/C or S/C ratios.展开更多
基金973 Program (2004CB719503)Key Program of Natural Science Foundation of Tianjin (07JCZDJC01600)Program for New Century Excellent Talents in University (NCET-06-0243)
文摘The influences of CeO2-ZrO2 and γ-Al2O3 mixing methods on the catalytic activity and stability of partial oxidation of methane （POM） were investigated over Ni/Ce0.7Zr0.3O2-Al2O3 catalysts. The catalysts were characterized by XRD, TPR, H2-chemsorption, and TG-DTA. For fresh catalysts, the results showed that the salt precursor mixing catalyst （ATOM） presented better performance than the catalysts prepared by the precipitator mixing method （MOL） and the powder mechanically mixing method （MECH）. The result of XRD suggested that the interaction between CeO2-ZrO2 and Al2O3 in ATOM sample was stronger than the others, which led to more lattice defects and thereby better initial activity. Moreover, the MECH sample had the best stability and the least coke deposition in 24 h stability tests. The results of TPR and H2-chemsorption indicated that the intimate contact of Ni-Al in MECH sample enhanced the ability of resisting coke deposition and metal sintering.
基金supported by the greenhouse gas mitigation technology development program"Technology Developments on Hydrogen Production from Biomass and Waste"organized by the National Institute for Environmental Studies(NIES)for 2002~2008 in trust from the Ministry of the Environment(MOE)
文摘This study focused on measurement of the autothermal reforming of biogas over a Ni based monolithic catalyst. The effects of the steam/CH4 （S/C） ratio, O2/CH4 （O2/C） ratio and temperature were investigated. The CH4 conversions were higher under all examined temperatures than the equilibrium conversion calculated using the blank outlet temperature, because the catalyst layer was heated by the exothermic catalytic partial oxidation reaction. The CH 4conversion increased with increasing O2/C ratio. Moreover, the CH4 conversion was higher than the equilibrium conversion calculated using the blank outlet temperature for O2/C〉0.42 and reached about 100% at O2/C=0.55. However, the hydrogen concentration decreased for O2/C〉0.45 because hydrogen was combusted to steam in the presence of excess oxygen. On the other hand, the hydrogen and CO2 concentrations increased and the CO concentration decreased with increasing SIC ratio. As a result, it was found that the highest hydrogen concentrations and CH4 conversions were attained at the O2/C ratios of 0.45-0.55 and the SIC ratios of 1.5-2.5. Moreover, the H2/CO ratio could also be controlled in the range from about 2 to 3.5 to give at least 90% CH4 conversion, by regulating the O2/C or S/C ratios.
