Oxidative coupling of methane is a direct way to obtain C2 hydrocarbon, and Mn-Na-W/SiO2 catalyst is the most promising among all the catalysts. The 2%Mn/5%Na2WO4/SiO2 catalyst was prepared by the incipient wetness im...Oxidative coupling of methane is a direct way to obtain C2 hydrocarbon, and Mn-Na-W/SiO2 catalyst is the most promising among all the catalysts. The 2%Mn/5%Na2WO4/SiO2 catalyst was prepared by the incipient wetness impregnation method. A 7-step heterogeneous reaction model of the oxidative coupling of methane to C2 hydrocarbons was conducted by co-feeding methane and oxygen at a total pressure of 1 bar over the catalyst. The kinetic measurements were carried out in a micro-catalytic fixed bed reactor. The kinetic data were obtained at the appropriate range of reaction conditions （4 kPa〈Po2 〈20 kPa, 20 kPa〈PcH4〈80 kPa, 800 ℃〈T〈900℃）. The proposed reaction kinetic scheme consists of three primary and four consecutive reaction steps. The conversions of hydrocarbons and carbon oxides were evaluated by applying Langmuir-Hinshelwood type rate equations. Power-law rate equation was applied only for the water-gas shift reaction. In addition, the effects of operating conditions on the reaction rate were studied. The proposed kinetic model can predict the conversion of methane and oxygen as well as the yield of C2 hydrocarbons and carbon oxides with an average accuracy of ± 15%.展开更多
In this work the effects of the contents of nickel （5, 7.5, 10 wt%） and copper （0, 1, 2 wt%） and reac- tion temperature （650, 700, 750 ℃） on the catalytic performance of Ni-Cu/Al_2O_3 catalyst in methane dry re...In this work the effects of the contents of nickel （5, 7.5, 10 wt%） and copper （0, 1, 2 wt%） and reac- tion temperature （650, 700, 750 ℃） on the catalytic performance of Ni-Cu/Al_2O_3 catalyst in methane dry reforming were evaluated using Box-Behnken design in order to optimize methane conversion, H_2/CO ratio and the catalyst deactivation. Different catalysts were prepared by co-impregnation method and characterized by XRD, BET, H_2-TPR, FESEM and TG/DTA analyses. The results revealed that copper addi- tion improved the catalyst reducibility. Promoted catalyst with low amounts of Cu gave higher activity and stability with high resistance to coke deposition and agglomeration of active phase especially during the reaction. However catalysts with high amounts of Cu were less active and rather deactivated due to the active sites sintering as well as Ni covering by Cu-enriched phase. The optimal conditions were de- termined by desirability function approach as 10 wt% of Ni, 0.83 wt% of Cu at 750℃. CH_4 conversion of 95.1%, H_2/CO ratio of 1 and deactivation of 1.4% were obtained experimentally under optimum conditions, which were in close agreement with the values oredicted hv the developed model.展开更多
基金This work was financially supported by the Research Department of Iran University of Science and Technology
文摘Oxidative coupling of methane is a direct way to obtain C2 hydrocarbon, and Mn-Na-W/SiO2 catalyst is the most promising among all the catalysts. The 2%Mn/5%Na2WO4/SiO2 catalyst was prepared by the incipient wetness impregnation method. A 7-step heterogeneous reaction model of the oxidative coupling of methane to C2 hydrocarbons was conducted by co-feeding methane and oxygen at a total pressure of 1 bar over the catalyst. The kinetic measurements were carried out in a micro-catalytic fixed bed reactor. The kinetic data were obtained at the appropriate range of reaction conditions （4 kPa〈Po2 〈20 kPa, 20 kPa〈PcH4〈80 kPa, 800 ℃〈T〈900℃）. The proposed reaction kinetic scheme consists of three primary and four consecutive reaction steps. The conversions of hydrocarbons and carbon oxides were evaluated by applying Langmuir-Hinshelwood type rate equations. Power-law rate equation was applied only for the water-gas shift reaction. In addition, the effects of operating conditions on the reaction rate were studied. The proposed kinetic model can predict the conversion of methane and oxygen as well as the yield of C2 hydrocarbons and carbon oxides with an average accuracy of ± 15%.
文摘In this work the effects of the contents of nickel （5, 7.5, 10 wt%） and copper （0, 1, 2 wt%） and reac- tion temperature （650, 700, 750 ℃） on the catalytic performance of Ni-Cu/Al_2O_3 catalyst in methane dry reforming were evaluated using Box-Behnken design in order to optimize methane conversion, H_2/CO ratio and the catalyst deactivation. Different catalysts were prepared by co-impregnation method and characterized by XRD, BET, H_2-TPR, FESEM and TG/DTA analyses. The results revealed that copper addi- tion improved the catalyst reducibility. Promoted catalyst with low amounts of Cu gave higher activity and stability with high resistance to coke deposition and agglomeration of active phase especially during the reaction. However catalysts with high amounts of Cu were less active and rather deactivated due to the active sites sintering as well as Ni covering by Cu-enriched phase. The optimal conditions were de- termined by desirability function approach as 10 wt% of Ni, 0.83 wt% of Cu at 750℃. CH_4 conversion of 95.1%, H_2/CO ratio of 1 and deactivation of 1.4% were obtained experimentally under optimum conditions, which were in close agreement with the values oredicted hv the developed model.
