A novel hydrocracking Ni-W binary catalyst was tentatively designed and prepared by means ofimpregnation on mixed supports of modified Y zeolite and amorphous aluminosilicate . The structure andproperties of catalyst ...A novel hydrocracking Ni-W binary catalyst was tentatively designed and prepared by means ofimpregnation on mixed supports of modified Y zeolite and amorphous aluminosilicate . The structure andproperties of catalyst were extensively characterized by XRD, NH3-TPD, IR and XRF techniques. The perfor-mance of catalyst was evaluated by a 100-ml hydrogenation laboratory test unit with two single-stage fixed-bedreactors connected in series. The characterization results showed that the catalyst has a developed and con-centrated mesopores distribution, suitable acid sites and acid strength distribution, and uniform and highdispersion of metal sites. Under a high conversion rate of 73.8% with the >350℃ feedstock, a 98.1m% of C5+yield and 83.5% of middle distillates selectivity were obtained. The yield of middle distillates boiling between140℃and 370℃ was 68.70m% and its quality could meet the WWFC category III specification. It means thatthis catalyst could be used to produce more high quality clean middle distillates derived from heavy oilhydrocracking. The potential aromatic content of heavy naphtha from 65℃ to 140℃ was 37.5m%. The BMCIvalue of >370℃ tail oil was 6.6. The heavy naphtha and tail oil are premium feedstocks for catalytic reformingand steam cracker units.展开更多
A series of Ni-W catalysts supported on mesoporous SBA-15 with different Ni:W ratios(NixW/SBA-15, Ni-5%, x=1, 10, 50) was prepared and fully characterized by powder X-ray diffraction(PXRD), Brunner-Emmet-Teller(BET), ...A series of Ni-W catalysts supported on mesoporous SBA-15 with different Ni:W ratios(NixW/SBA-15, Ni-5%, x=1, 10, 50) was prepared and fully characterized by powder X-ray diffraction(PXRD), Brunner-Emmet-Teller(BET), transmission electronic microscopy(TEM), H2-temperature programmed reduction(H2-TPR), and X-ray photoelectron spectroscopy(XPS). High-resolution TEM images, XPS measurements, H2-TPR experiments coupled with PXRD results determined the evolution of Ni and W species. It is found that a trace amount of W from H2WO4 can significantly improve Ni dispersion on SBA-15 (Ni50W/SBA-15) with Ni0 and non-stoichiometric WOx species as small as ca. 3.6 nm. The prepared NixW/SBA-15 was utilized for CO_(2) hydrogenation, which showed that a higher W content restrained the CO_(2) hydrogenation while a lower W ratio promoted both conversion rate and selectivity for methane compared with Ni/SBA-15. The Ni50W/SBA-15 catalyst showed the best performance with a 93.3% CO_(2) conversion rate and 99.7% selectivity for methane at 400 oC under 0.1 MPa and maintained ca. 97% initial performance for 24 h. Tracking product evolution experiments by in-situ Fourier transform infrared spectrascopy(FTIR) indicated that a small amount of W can modify the surface of Ni particles by geometric coverage and electronic modification, which facilitates the adsorption of the CO intermedia and results in the formation of CH4. This work provides a new clue to fabricating efficient CO_(2) conversion bimetallic materials.展开更多
In this work,syngas methanation over Ni-W/TiO2-SiO2catalyst was studied in a fluidized-bed reactor(FBR)and its performance was compared with a fixed-bed reactor(FIXBR).The effects of main operating variables including...In this work,syngas methanation over Ni-W/TiO2-SiO2catalyst was studied in a fluidized-bed reactor(FBR)and its performance was compared with a fixed-bed reactor(FIXBR).The effects of main operating variables including feedstock gases space velocity,coke content,bed temperature and sulfur-tolerant stability of 100 h life were investigated.The structure of the catalysts was characterized by XRD,N2adsorptiondesorption and TEM.It is found that under same space velocity from 5000 h 1to 25000 h 1FBR gave a higher CH4yield,lower coke content,and lower bed temperature than those obtained in FIXBR.Ni-W/TiO2-SiO2catalyst possessed excellent sulfur-tolerant stability on the feedstock gases less than 500 ppm H2S in FBR.The carbon deposits formed on the spent catalyst were in the form of carbon fibers in FBR,while in the form of dense accumulation distribution appearance in FIXBR.展开更多
文摘A novel hydrocracking Ni-W binary catalyst was tentatively designed and prepared by means ofimpregnation on mixed supports of modified Y zeolite and amorphous aluminosilicate . The structure andproperties of catalyst were extensively characterized by XRD, NH3-TPD, IR and XRF techniques. The perfor-mance of catalyst was evaluated by a 100-ml hydrogenation laboratory test unit with two single-stage fixed-bedreactors connected in series. The characterization results showed that the catalyst has a developed and con-centrated mesopores distribution, suitable acid sites and acid strength distribution, and uniform and highdispersion of metal sites. Under a high conversion rate of 73.8% with the >350℃ feedstock, a 98.1m% of C5+yield and 83.5% of middle distillates selectivity were obtained. The yield of middle distillates boiling between140℃and 370℃ was 68.70m% and its quality could meet the WWFC category III specification. It means thatthis catalyst could be used to produce more high quality clean middle distillates derived from heavy oilhydrocracking. The potential aromatic content of heavy naphtha from 65℃ to 140℃ was 37.5m%. The BMCIvalue of >370℃ tail oil was 6.6. The heavy naphtha and tail oil are premium feedstocks for catalytic reformingand steam cracker units.
基金supported by the National Natural Science Foundation of China (No.91961110).
文摘A series of Ni-W catalysts supported on mesoporous SBA-15 with different Ni:W ratios(NixW/SBA-15, Ni-5%, x=1, 10, 50) was prepared and fully characterized by powder X-ray diffraction(PXRD), Brunner-Emmet-Teller(BET), transmission electronic microscopy(TEM), H2-temperature programmed reduction(H2-TPR), and X-ray photoelectron spectroscopy(XPS). High-resolution TEM images, XPS measurements, H2-TPR experiments coupled with PXRD results determined the evolution of Ni and W species. It is found that a trace amount of W from H2WO4 can significantly improve Ni dispersion on SBA-15 (Ni50W/SBA-15) with Ni0 and non-stoichiometric WOx species as small as ca. 3.6 nm. The prepared NixW/SBA-15 was utilized for CO_(2) hydrogenation, which showed that a higher W content restrained the CO_(2) hydrogenation while a lower W ratio promoted both conversion rate and selectivity for methane compared with Ni/SBA-15. The Ni50W/SBA-15 catalyst showed the best performance with a 93.3% CO_(2) conversion rate and 99.7% selectivity for methane at 400 oC under 0.1 MPa and maintained ca. 97% initial performance for 24 h. Tracking product evolution experiments by in-situ Fourier transform infrared spectrascopy(FTIR) indicated that a small amount of W can modify the surface of Ni particles by geometric coverage and electronic modification, which facilitates the adsorption of the CO intermedia and results in the formation of CH4. This work provides a new clue to fabricating efficient CO_(2) conversion bimetallic materials.
文摘In this work,syngas methanation over Ni-W/TiO2-SiO2catalyst was studied in a fluidized-bed reactor(FBR)and its performance was compared with a fixed-bed reactor(FIXBR).The effects of main operating variables including feedstock gases space velocity,coke content,bed temperature and sulfur-tolerant stability of 100 h life were investigated.The structure of the catalysts was characterized by XRD,N2adsorptiondesorption and TEM.It is found that under same space velocity from 5000 h 1to 25000 h 1FBR gave a higher CH4yield,lower coke content,and lower bed temperature than those obtained in FIXBR.Ni-W/TiO2-SiO2catalyst possessed excellent sulfur-tolerant stability on the feedstock gases less than 500 ppm H2S in FBR.The carbon deposits formed on the spent catalyst were in the form of carbon fibers in FBR,while in the form of dense accumulation distribution appearance in FIXBR.
