A carbon-based sulfonated catalyst was prepared by direct sulfonation and carbonization （in moderate conditions：200 ＆#176;C, 12 h） of red liquor solids, a by-product of paper-making process. The prepared sulfonate...A carbon-based sulfonated catalyst was prepared by direct sulfonation and carbonization （in moderate conditions：200 ＆#176;C, 12 h） of red liquor solids, a by-product of paper-making process. The prepared sulfonated cata-lyst （SC） had aromatic structure, composed of carbon enriched inner core, and oxygen-containing （SO3H, COOH, OH） groups enriched surface. The SO3H, COOH, OH groups amounted to 0.74 mmol·g^-1, 0.78 mmol·g^-1, 2.18 mmol·g^-1, respectively. The fresh SC showed much higher catalytic activity than that of the traditional solid acid catalysts （strong-acid 732 cation exchange resin, hydrogen type zeolite socony mobile-five （HZSM-5）, sulfated zir-conia） in esterification of oleic acid. SC was deactivated during the reactions, through the mechanisms of leaching of sulfonated species and formation of sulfonate esters. Two regeneration methods were developed, and the catalytic activity can be mostly regenerated by regeneration Method 1 and be fully regenerated by regeneration Method 2, respectively.展开更多
Nickel catalysts supported on CeO2-ZrO2-CeO2,ZrO2-Al2O3 and Al2O3 were prepared and characterized by means of X-ray diffraction（XRD）,BET areas,H2 temperature-programmed reduction（H2-TPR）,and X-ray photoelectron sp...Nickel catalysts supported on CeO2-ZrO2-CeO2,ZrO2-Al2O3 and Al2O3 were prepared and characterized by means of X-ray diffraction（XRD）,BET areas,H2 temperature-programmed reduction（H2-TPR）,and X-ray photoelectron spectroscopy（XPS）.Through the test of catalytic partial oxidation of methane（CPOM）,Ni/CeO2-ZrO2-Al2O3 displayed the highest activity,which resulted from its largest BET area and best NiO dispersion.Furthermore,Ni/CeO2-ZrO2-Al2O3 maintained a long-time stability in CPOM,which was attributed to its best coking resistance among all the prepared catalysts.展开更多
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
Ni/α-Al2O3 catalysts were found to be active in the temperature range 600 ～ 900℃ for both CO2 reforming and partial oxidation of methane.The effects of Ni loading,reaction temperature and feed gas ratio for the com...Ni/α-Al2O3 catalysts were found to be active in the temperature range 600 ～ 900℃ for both CO2 reforming and partial oxidation of methane.The effects of Ni loading,reaction temperature and feed gas ratio for the combination of CO2 reforming and partial oxidation of CH4 over Ni/α-Al2O3 were investigated.Catalysts of xwt%Ni/α-Al2O3（x=2.5,5,8 and 12） were prepared by wet impregnating the calcined support with a solution of nickel nitrate.XRD patterns and activity tests have verified that the 5wt%Ni/α-Al2O3 was the most active catalyst,as compared with the other prepared catalyst samples.An increase of the Ni loading to more than 5wt% led to a reduction in the Ni dispersion.In addition,by combining the endothermic carbon dioxide reforming reaction with the exothermic partial oxidation reaction,the loss of catalyst activity with time on stream was reduced with the amount of oxygen added to the feed.展开更多
Y2O3-Al2O3 with different mole ratios of Y：Al were prepared by co-precipitation method. Catalysts Ni/Y2O3, Ni/Al2O3 and Ni/ Y2O3-Al2O3 were prepared by impregnation method. The result of BET showed that Al2O3 with re...Y2O3-Al2O3 with different mole ratios of Y：Al were prepared by co-precipitation method. Catalysts Ni/Y2O3, Ni/Al2O3 and Ni/ Y2O3-Al2O3 were prepared by impregnation method. The result of BET showed that Al2O3 with relative high surface area was in favor of Ni distribution, whilst the TPR test demonstrated that composite support had appropriate synergistic effect between active constituent and sup-port, and NiO could be reduced more easily than loaded on the single support. H2-TPD test indicated that the catalyst NYA11 had lots of ac-tivity sites where H could be desorbed easily, which led to hydrogen-rich production over the catalyst. Composite support catalysts exhibited high activity for ethanol steam reforming （SRE）, and the supported catalyst with composite of 1：1 mole ratio of Y：Al exhibited the optimum catalytic properties for SRE. Ethanol could be completely converted over catalyst NYA11 even at 450 °C, and there had no inactivation after 60 h continuous reaction, hydrogen yield appeared maximum 35.9% at 400 ℃, and tended to increase with increasing H2O/EtOH molar ratio and feed flow rate.展开更多
Supported nickel-based catalysts were prepared by the incipient wetness impregnation method for the selective hydrogenation of methyl isobutyl ketone to methyl isobutyl carbinol in a fixed-bed reactor. The effects of ...Supported nickel-based catalysts were prepared by the incipient wetness impregnation method for the selective hydrogenation of methyl isobutyl ketone to methyl isobutyl carbinol in a fixed-bed reactor. The effects of the nickel source,Ni loading, calcination time, and calcination temperature on the hydrogenation performance were studied. The experimental results showed that the Ni/γ-Al_2O_3 catalyst demonstrated the highest catalytic performance under the preparation conditions by using nickel nitrate as the nickel source with a NiO loading of 20%, followed by calcination at 440°C for 5h. In addition,this catalyst showed the largest specific surface area, best crystal structure, highest active component content, smallest particle size, and uniform distribution of NiO on the surface of the carrier. The nickel-based catalyst prepared using the optimized conditions exhibited a 96.1% conversion of methyl isobutyl ketone, with a methyl isobutyl carbinol selectivity of 99.6%. The described procedure is very effective for the preparation of methyl isobutyl carbinol using methyl isobutyl ketone as the feedstock.展开更多
基金Supported by the National Natural Science Foundation of China(21276076)the Fundamental Research Funds for the Central Universities of China(WA1014003)State Key Laboratory of Chemical Engineering(SKL-ChE-10C06)
文摘A carbon-based sulfonated catalyst was prepared by direct sulfonation and carbonization （in moderate conditions：200 ＆#176;C, 12 h） of red liquor solids, a by-product of paper-making process. The prepared sulfonated cata-lyst （SC） had aromatic structure, composed of carbon enriched inner core, and oxygen-containing （SO3H, COOH, OH） groups enriched surface. The SO3H, COOH, OH groups amounted to 0.74 mmol·g^-1, 0.78 mmol·g^-1, 2.18 mmol·g^-1, respectively. The fresh SC showed much higher catalytic activity than that of the traditional solid acid catalysts （strong-acid 732 cation exchange resin, hydrogen type zeolite socony mobile-five （HZSM-5）, sulfated zir-conia） in esterification of oleic acid. SC was deactivated during the reactions, through the mechanisms of leaching of sulfonated species and formation of sulfonate esters. Two regeneration methods were developed, and the catalytic activity can be mostly regenerated by regeneration Method 1 and be fully regenerated by regeneration Method 2, respectively.
基金Project supported by State Key Fundamental Research Project(G1999022400)
文摘Nickel catalysts supported on CeO2-ZrO2-CeO2,ZrO2-Al2O3 and Al2O3 were prepared and characterized by means of X-ray diffraction（XRD）,BET areas,H2 temperature-programmed reduction（H2-TPR）,and X-ray photoelectron spectroscopy（XPS）.Through the test of catalytic partial oxidation of methane（CPOM）,Ni/CeO2-ZrO2-Al2O3 displayed the highest activity,which resulted from its largest BET area and best NiO dispersion.Furthermore,Ni/CeO2-ZrO2-Al2O3 maintained a long-time stability in CPOM,which was attributed to its best coking resistance among all the prepared catalysts.
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.
文摘Ni/α-Al2O3 catalysts were found to be active in the temperature range 600 ～ 900℃ for both CO2 reforming and partial oxidation of methane.The effects of Ni loading,reaction temperature and feed gas ratio for the combination of CO2 reforming and partial oxidation of CH4 over Ni/α-Al2O3 were investigated.Catalysts of xwt%Ni/α-Al2O3（x=2.5,5,8 and 12） were prepared by wet impregnating the calcined support with a solution of nickel nitrate.XRD patterns and activity tests have verified that the 5wt%Ni/α-Al2O3 was the most active catalyst,as compared with the other prepared catalyst samples.An increase of the Ni loading to more than 5wt% led to a reduction in the Ni dispersion.In addition,by combining the endothermic carbon dioxide reforming reaction with the exothermic partial oxidation reaction,the loss of catalyst activity with time on stream was reduced with the amount of oxygen added to the feed.
基金Project supported by National Natural Science Foundation of China (20863006,21166018)Natural Science Foundation committee of Jiangxi Province,China (0620042)Department of Education of Jiangxi Province (GJJ09078)
文摘Y2O3-Al2O3 with different mole ratios of Y：Al were prepared by co-precipitation method. Catalysts Ni/Y2O3, Ni/Al2O3 and Ni/ Y2O3-Al2O3 were prepared by impregnation method. The result of BET showed that Al2O3 with relative high surface area was in favor of Ni distribution, whilst the TPR test demonstrated that composite support had appropriate synergistic effect between active constituent and sup-port, and NiO could be reduced more easily than loaded on the single support. H2-TPD test indicated that the catalyst NYA11 had lots of ac-tivity sites where H could be desorbed easily, which led to hydrogen-rich production over the catalyst. Composite support catalysts exhibited high activity for ethanol steam reforming （SRE）, and the supported catalyst with composite of 1：1 mole ratio of Y：Al exhibited the optimum catalytic properties for SRE. Ethanol could be completely converted over catalyst NYA11 even at 450 °C, and there had no inactivation after 60 h continuous reaction, hydrogen yield appeared maximum 35.9% at 400 ℃, and tended to increase with increasing H2O/EtOH molar ratio and feed flow rate.
基金financially supported by the National Natural Science Foundation of China (91634101)the Project on Construction of Innovative Teams and Teacher Career Development for Universities and Colleges under Beijing Municipality (IDHT20180508)
文摘Supported nickel-based catalysts were prepared by the incipient wetness impregnation method for the selective hydrogenation of methyl isobutyl ketone to methyl isobutyl carbinol in a fixed-bed reactor. The effects of the nickel source,Ni loading, calcination time, and calcination temperature on the hydrogenation performance were studied. The experimental results showed that the Ni/γ-Al_2O_3 catalyst demonstrated the highest catalytic performance under the preparation conditions by using nickel nitrate as the nickel source with a NiO loading of 20%, followed by calcination at 440°C for 5h. In addition,this catalyst showed the largest specific surface area, best crystal structure, highest active component content, smallest particle size, and uniform distribution of NiO on the surface of the carrier. The nickel-based catalyst prepared using the optimized conditions exhibited a 96.1% conversion of methyl isobutyl ketone, with a methyl isobutyl carbinol selectivity of 99.6%. The described procedure is very effective for the preparation of methyl isobutyl carbinol using methyl isobutyl ketone as the feedstock.
