In Fischer-Tropsch synthesis reaction, methane formation is one of the side reactions which must be suppressed in order to get better catalytic selectivity for light olefins. In the present study, we have modified cob...In Fischer-Tropsch synthesis reaction, methane formation is one of the side reactions which must be suppressed in order to get better catalytic selectivity for light olefins. In the present study, we have modified cobalt based Fischer-Tropsch catalyst and developed a process to minimize methane production, consequently to produce maximum yield of light olefins. Manganese-cobalt oxide supported on H-5A zeolite catalyst was synthesized using modified H-5A zeolite, to increase its surface acid sites. Increased acidity of zeolite plays a major part in the suppression of methane formation during the Fischer-Tropsch reaction. The modified zeolite results in the electronic modification of catalyst surface by creating new active catalytic sites. The results are compared with other supported catalysts along with unmodified zeolite. Appreciable reduction in methane formation is achieved on modified zeolite supported catalyst in comparison with unsupported catalyst.展开更多
We modeled and studied the permeability of methane hydrate bearing formations as a function of methane hydrate concentration by artificially varying the T2 distribution as well as using a tube-sphere model.We varied t...We modeled and studied the permeability of methane hydrate bearing formations as a function of methane hydrate concentration by artificially varying the T2 distribution as well as using a tube-sphere model.We varied the proportion of irreducible and movable water as well as the total porosity associated with the T2 distribution and found the normalized permeability as a function of methane hydrate concentration is dependent of these variations.Using a tube-sphere model,we increased the methane hydrate concentration by randomly placing methane hydrate crystals in the pore spaces and computed the permeability using either the Schlumberger T2 relaxation time formula or a direct calculation based on Darcy's law assuming Poiseuille flow.Earlier experimental measurements reported in the literature show there is a methane hydrate concentration range where the permeability remains relatively constant.We found that when the Schlumberger T2 relaxation time formula is used the simulation results show a curve of normalized permeability versus methane hydrate concentration quite close to that predicted by the Masuda model with N = 15.When the permeability was directly calculated based on Darcy's law,the simulation results show a much higher normalized permeability and only show a trend consistent with the experimental results,i.e.,with a permeability plateau,when the methane hydrate crystals are preferentially placed in the tubes,and the higher the preferential probability,the larger the range where the permeability has a plateau.展开更多
Primary formation of methane and secondary formation of ethylene in methanol conversion are evidenced by temperature-programmed-surface- reaction of adsorbed methanol on HZSM-5 catalyst.A reaction mechanism accounts f...Primary formation of methane and secondary formation of ethylene in methanol conversion are evidenced by temperature-programmed-surface- reaction of adsorbed methanol on HZSM-5 catalyst.A reaction mechanism accounts for the observed results is described.展开更多
Biological characteristics of methane emission were compared among Oryza sativa, Panicum crus-galli andCyperus difformis grown on paddy soil. The order of the amounts of methane emitted was P. crus-galli > O. sativ...Biological characteristics of methane emission were compared among Oryza sativa, Panicum crus-galli andCyperus difformis grown on paddy soil. The order of the amounts of methane emitted was P. crus-galli > O. sativa >C. difformis, with the former two 11 and 8 times as much as that of the latter, respectively. And it was just opposite tothat of the methane-forming activities of roots of the three plants. The diurnal changes of methane emission of thethree plants were relatively consistent with valleys during 11:00-14:00 and midnight and peaks during 8:00-11: 00,14:00- 20:00 and about 5:00 early morning. The methanogenic activites in rhizospheric soils were higher than those innonrhizospheric soils with P. crus-galli and O. sativa, but not with C. difformis. The pathways of methane release ofP. crus-galli and O . sativa were probably through the top gaps near the junctions of nodal plate and leaf sheath, how-ever in C. difformistopgaps from which methane could escape into atmosphere were not found.展开更多
Extensive work on a Cu-modified TiO_(2) photocatalyst for CO_(2) reduction under visible light irradiation was conducted. The structure of the copper cocatalyst was established using UV-vis diff use refl ectance spect...Extensive work on a Cu-modified TiO_(2) photocatalyst for CO_(2) reduction under visible light irradiation was conducted. The structure of the copper cocatalyst was established using UV-vis diff use refl ectance spectroscopy, high-resolution transmis- sion electron microscopy, X-ray absorption spectroscopy, and X-ray photoelectron spectroscopy. It was found that copper exists in different states (Cu 0 , Cu^(+) , and Cu^(2+) ), the content of which depends on the TiO_(2) calcination temperature and copper loading. The optimum composition of the cocatalyst has a photocatalyst based on TiO_(2) calcined at 700℃ and modified with 5 wt% copper, the activity of which is 22 μmol/(h·g cat ) (409 nm). Analysis of the photocatalysts after the photocatalytic reaction disclosed that the copper metal on the surface of the calcined TiO_(2) was gradually converted into Cu_(2) O during the photocatalytic reaction. Meanwhile, the metallic copper on the surface of the noncalcined TiO_(2) did not undergo any trans- formation during the reaction.展开更多
Crystalline TiO(P25) and isolated titanate species in a ZSM-5 structure(TS-1) were modified with Au and Ag, respectively, and tested in the gas-phase photocatalytic COreduction under high purity conditions. The no...Crystalline TiO(P25) and isolated titanate species in a ZSM-5 structure(TS-1) were modified with Au and Ag, respectively, and tested in the gas-phase photocatalytic COreduction under high purity conditions. The noble metal modification was performed by photodeposition. Light absorbance properties of the catalysts are examined with UV–Vis spectroscopy before and after the activity test. In the gas-phase photocatalytic COreduction, it was observed that the catalysts with Ag nanostructures are more active than those with Au nanostructures. It is thus found that the energetic difference between the band gap energy of the semiconductor and the position of the plasmon is influencing the photocatalytic activity.Potentially, plasmon excitation due to visible light absorption results in plasmon resonance energy, which affects the excitation of the semiconductor positively. Therefore, an overlap between band gap energy of the semiconductor and metal plasmon is needed.展开更多
文摘In Fischer-Tropsch synthesis reaction, methane formation is one of the side reactions which must be suppressed in order to get better catalytic selectivity for light olefins. In the present study, we have modified cobalt based Fischer-Tropsch catalyst and developed a process to minimize methane production, consequently to produce maximum yield of light olefins. Manganese-cobalt oxide supported on H-5A zeolite catalyst was synthesized using modified H-5A zeolite, to increase its surface acid sites. Increased acidity of zeolite plays a major part in the suppression of methane formation during the Fischer-Tropsch reaction. The modified zeolite results in the electronic modification of catalyst surface by creating new active catalytic sites. The results are compared with other supported catalysts along with unmodified zeolite. Appreciable reduction in methane formation is achieved on modified zeolite supported catalyst in comparison with unsupported catalyst.
基金funded by National Basic Research Program of China(973Program,No.2009CB219505)
文摘We modeled and studied the permeability of methane hydrate bearing formations as a function of methane hydrate concentration by artificially varying the T2 distribution as well as using a tube-sphere model.We varied the proportion of irreducible and movable water as well as the total porosity associated with the T2 distribution and found the normalized permeability as a function of methane hydrate concentration is dependent of these variations.Using a tube-sphere model,we increased the methane hydrate concentration by randomly placing methane hydrate crystals in the pore spaces and computed the permeability using either the Schlumberger T2 relaxation time formula or a direct calculation based on Darcy's law assuming Poiseuille flow.Earlier experimental measurements reported in the literature show there is a methane hydrate concentration range where the permeability remains relatively constant.We found that when the Schlumberger T2 relaxation time formula is used the simulation results show a curve of normalized permeability versus methane hydrate concentration quite close to that predicted by the Masuda model with N = 15.When the permeability was directly calculated based on Darcy's law,the simulation results show a much higher normalized permeability and only show a trend consistent with the experimental results,i.e.,with a permeability plateau,when the methane hydrate crystals are preferentially placed in the tubes,and the higher the preferential probability,the larger the range where the permeability has a plateau.
文摘Primary formation of methane and secondary formation of ethylene in methanol conversion are evidenced by temperature-programmed-surface- reaction of adsorbed methanol on HZSM-5 catalyst.A reaction mechanism accounts for the observed results is described.
文摘Biological characteristics of methane emission were compared among Oryza sativa, Panicum crus-galli andCyperus difformis grown on paddy soil. The order of the amounts of methane emitted was P. crus-galli > O. sativa >C. difformis, with the former two 11 and 8 times as much as that of the latter, respectively. And it was just opposite tothat of the methane-forming activities of roots of the three plants. The diurnal changes of methane emission of thethree plants were relatively consistent with valleys during 11:00-14:00 and midnight and peaks during 8:00-11: 00,14:00- 20:00 and about 5:00 early morning. The methanogenic activites in rhizospheric soils were higher than those innonrhizospheric soils with P. crus-galli and O. sativa, but not with C. difformis. The pathways of methane release ofP. crus-galli and O . sativa were probably through the top gaps near the junctions of nodal plate and leaf sheath, how-ever in C. difformistopgaps from which methane could escape into atmosphere were not found.
基金supported by Russian Science Foundation (No.#21-73-10235)
文摘Extensive work on a Cu-modified TiO_(2) photocatalyst for CO_(2) reduction under visible light irradiation was conducted. The structure of the copper cocatalyst was established using UV-vis diff use refl ectance spectroscopy, high-resolution transmis- sion electron microscopy, X-ray absorption spectroscopy, and X-ray photoelectron spectroscopy. It was found that copper exists in different states (Cu 0 , Cu^(+) , and Cu^(2+) ), the content of which depends on the TiO_(2) calcination temperature and copper loading. The optimum composition of the cocatalyst has a photocatalyst based on TiO_(2) calcined at 700℃ and modified with 5 wt% copper, the activity of which is 22 μmol/(h·g cat ) (409 nm). Analysis of the photocatalysts after the photocatalytic reaction disclosed that the copper metal on the surface of the calcined TiO_(2) was gradually converted into Cu_(2) O during the photocatalytic reaction. Meanwhile, the metallic copper on the surface of the noncalcined TiO_(2) did not undergo any trans- formation during the reaction.
文摘Crystalline TiO(P25) and isolated titanate species in a ZSM-5 structure(TS-1) were modified with Au and Ag, respectively, and tested in the gas-phase photocatalytic COreduction under high purity conditions. The noble metal modification was performed by photodeposition. Light absorbance properties of the catalysts are examined with UV–Vis spectroscopy before and after the activity test. In the gas-phase photocatalytic COreduction, it was observed that the catalysts with Ag nanostructures are more active than those with Au nanostructures. It is thus found that the energetic difference between the band gap energy of the semiconductor and the position of the plasmon is influencing the photocatalytic activity.Potentially, plasmon excitation due to visible light absorption results in plasmon resonance energy, which affects the excitation of the semiconductor positively. Therefore, an overlap between band gap energy of the semiconductor and metal plasmon is needed.