The catalytic behaviors of Pd(1.4 wt%)catalysts supported on CeO2-ZrO2-La2O3 mixed oxides with different Ce/Zr molar ratios were investigated for methanol decomposition.Nitrogen adsorption-desorption(BET),X-ray photoe...The catalytic behaviors of Pd(1.4 wt%)catalysts supported on CeO2-ZrO2-La2O3 mixed oxides with different Ce/Zr molar ratios were investigated for methanol decomposition.Nitrogen adsorption-desorption(BET),X-ray photoelectron spectroscopy(XPS),H2 temperature-programmed reduction(H2-TPR),X-ray diffraction(XRD)and Pd dispersion analysis were used for their characterization.Pd/Cc0.76Zro.18 La0.06O1.97 catalyst showed the highest BET surface area,best Pd dispersion capability and strongest metal-support interaction.Moreover,XPS showed that there was lattice defect oxygen or mobile oxygen.According to the result of O 1s measurements the lattice defect oxygen or mobile oxygen helped to maintain Pd in a partly oxidized state and increased the activity for methanol decomposition.The Pd/Ce0.76Zr0.18La0.0601.97 catalyst exhibited the best activity.A 100%conversion of methanol was achieved at around 260°C,which was about 20-40°C lower than other catalysts.展开更多
SO4^2- / TiO2-La2O3, a novel solid superacid, was prepared and its catalytic activities at different synthetic conditions are discussed with esterification of n-butanoic acid and n-butyl alcohol as probing reaction. T...SO4^2- / TiO2-La2O3, a novel solid superacid, was prepared and its catalytic activities at different synthetic conditions are discussed with esterification of n-butanoic acid and n-butyl alcohol as probing reaction. The optimum conditions have also been found, mole ratio of n(La^3+):n(Ti^4+) is 1:34, the soaked consistency of H2SO4 is 0.8 tool/L, the soaked time of HESO4 is 24 h, the calcining temperature is 480 ℃, the calcining time is 3 h. Then it was applied in the catalytic synthesis often important ketals and acetals as catalyst and revealed high catalytic activity. Under these conditions on which the molar ratio of aldehyde/ketone to glycol is l: 1.5, the mass ratio of the catalyst used in the reactants is 0.5%, and the reaction time is 1.0 h, the yields of ketals and acetals can reach 41.4%-95.8%.展开更多
Sulfated zirconia-lanthana (SO4^2-/ZrO2-La2O3) precursors were prepared by ultrasonic coprecipitation method and followed by aging at different temperature. The precursors were treated by 0.5 mol/L H2SO4. Samples of...Sulfated zirconia-lanthana (SO4^2-/ZrO2-La2O3) precursors were prepared by ultrasonic coprecipitation method and followed by aging at different temperature. The precursors were treated by 0.5 mol/L H2SO4. Samples of SO4^2-/ZrO2-La2O3 nano-crystalline catalysts were obtained by baking the treated precursors at different temperatures. The acidic properties of SO4^2-/ZrO2-La2O3 were tested by the Hammett indicator method. The phase composition, specific area, particle structure, and surface state were characterized by X-ray diffraction, BET, transmission electron microscopy, infrared spectrum, and X-ray photoelectron spec- troscopy. The catalytic activities were estimated by esterification of acetic acid with glycerin. It was shown that the catalyst prepared by ultrasonic stirring and low temperature (-15 ℃) exhibited highly active sites and high catalytic property.展开更多
基金the National Natural Science Foundation of China(20773090)the Specialized Research Fund for the Doctoral Program of Higher Education of China(20070610026,200806100009)
摘要The catalytic behaviors of Pd(1.4 wt%)catalysts supported on CeO2-ZrO2-La2O3 mixed oxides with different Ce/Zr molar ratios were investigated for methanol decomposition.Nitrogen adsorption-desorption(BET),X-ray photoelectron spectroscopy(XPS),H2 temperature-programmed reduction(H2-TPR),X-ray diffraction(XRD)and Pd dispersion analysis were used for their characterization.Pd/Cc0.76Zro.18 La0.06O1.97 catalyst showed the highest BET surface area,best Pd dispersion capability and strongest metal-support interaction.Moreover,XPS showed that there was lattice defect oxygen or mobile oxygen.According to the result of O 1s measurements the lattice defect oxygen or mobile oxygen helped to maintain Pd in a partly oxidized state and increased the activity for methanol decomposition.The Pd/Ce0.76Zr0.18La0.0601.97 catalyst exhibited the best activity.A 100%conversion of methanol was achieved at around 260°C,which was about 20-40°C lower than other catalysts.
基金Project supported by the National Natural Science Foundation of China (No. 20471044), and the Natural Science Foundation of Hubei Province (No. 2005ABA053), China
摘要SO4^2- / TiO2-La2O3, a novel solid superacid, was prepared and its catalytic activities at different synthetic conditions are discussed with esterification of n-butanoic acid and n-butyl alcohol as probing reaction. The optimum conditions have also been found, mole ratio of n(La^3+):n(Ti^4+) is 1:34, the soaked consistency of H2SO4 is 0.8 tool/L, the soaked time of HESO4 is 24 h, the calcining temperature is 480 ℃, the calcining time is 3 h. Then it was applied in the catalytic synthesis often important ketals and acetals as catalyst and revealed high catalytic activity. Under these conditions on which the molar ratio of aldehyde/ketone to glycol is l: 1.5, the mass ratio of the catalyst used in the reactants is 0.5%, and the reaction time is 1.0 h, the yields of ketals and acetals can reach 41.4%-95.8%.
摘要Sulfated zirconia-lanthana (SO4^2-/ZrO2-La2O3) precursors were prepared by ultrasonic coprecipitation method and followed by aging at different temperature. The precursors were treated by 0.5 mol/L H2SO4. Samples of SO4^2-/ZrO2-La2O3 nano-crystalline catalysts were obtained by baking the treated precursors at different temperatures. The acidic properties of SO4^2-/ZrO2-La2O3 were tested by the Hammett indicator method. The phase composition, specific area, particle structure, and surface state were characterized by X-ray diffraction, BET, transmission electron microscopy, infrared spectrum, and X-ray photoelectron spec- troscopy. The catalytic activities were estimated by esterification of acetic acid with glycerin. It was shown that the catalyst prepared by ultrasonic stirring and low temperature (-15 ℃) exhibited highly active sites and high catalytic property.