The copper based catalysts, CuO/T-Al2O3, CuO/y-Al2O3-cordierite (Cord) and CuO/Cord, were prepared by impregnation method. The catalytic activity of the catalysts was tested in absence and presence of water vapor,an...The copper based catalysts, CuO/T-Al2O3, CuO/y-Al2O3-cordierite (Cord) and CuO/Cord, were prepared by impregnation method. The catalytic activity of the catalysts was tested in absence and presence of water vapor,and the catalysts were characterized. Temperature program desorption (TPD) experiments or toluene and water on the catalysts were carried out. The influence of water vapor on the activity of the catalysts was discussed. Results showed that addition of the water vapor has a significant negative effect on the catalytic activity of the catalysts.The higher the concentration of the Water vapor in feed steam was, the lower the catalytic activity of the copper based catalysts became, which could be mainly ascribed to the competition of water molecules with toluene molecules for adsorption on the catalyst surfaces. TPD experiments showed that the strength of the interaction between water molecules and three catalysts followed the order: CuO/γ-Al2O3〉CuO/γ-Al2O3-Cord〉CuO/Cord. As a consequence of that, the degree of degradation in the catalytic activity of these three catalysts by the water vapor followed the order: CuO/γ-Al2O3〉CuO/y-Al2O3-Cord〉CuO/Cord. However, the negative effect of the water vapor was reversible.展开更多
The catalytic activity for the synthesis of methanol from carbon dioxide and hydrogen was measured on various binary and ternary catalysts containing copper oxide under a pressure of 10 atm. Among these samples the ca...The catalytic activity for the synthesis of methanol from carbon dioxide and hydrogen was measured on various binary and ternary catalysts containing copper oxide under a pressure of 10 atm. Among these samples the catalysts, CuO/ZnO/γ-Al_2O_3, demonstrated the highest activity and selectivity to methanol; MnO, as third component, had no promotional effect on the activity of meth- anol formation. Based on a simple power rate law the apparent activation energy estimation and par- tial pressure dependence measurement were accomplished over eight catalysts. The activation energies varied from 40 to 120 kJ / mol depending on the composition of catalysts. The rates of methanol for- mation to be 0.3 -- 0.9 order in H_2 and about 0.1 -- 0.2 order in CO_2 were reported.展开更多
Direct transformation of ethanol to ethyl acetate was investigated on a series of Cu(ZrO2)/SiO2 catalysts. Inductively coupled plasma(ICP), surface area analysis, X-ray diffraction(XRD), H2-temperature programme...Direct transformation of ethanol to ethyl acetate was investigated on a series of Cu(ZrO2)/SiO2 catalysts. Inductively coupled plasma(ICP), surface area analysis, X-ray diffraction(XRD), H2-temperature programmed reduc- tion(H2-TPR), X-ray photoelectron spectroscopy(XPS), NH3-temperature programmed desorption(NH3-TPD) and Fourier transform-infrared spectroscopy(FTIR) techniques were used to characterize the catalysts. The results reveal that ZrO2 can improve the dispersion of copper species and increase the acidity of the Cu(ZrO2)/SiO2 catalysts. The Cu0 is responsible for ethanol dehydrogenation to acetaldehyde, and both the Lewis acid and Bronsted acid sites were in favor of the selectivity to ethyl acetate. The synergistic effect of Cu0 and an appropriate amount of acidic sites played an important role in the production of ethyl acetate.展开更多
基金Supported by the National-Natural Science Foundation of China (20936001), the Natural Science Foundation of Guangdong Province, and the State Key Lab of Subtropical Building Science, South China University of Technology (x2yj C709028Z).
文摘The copper based catalysts, CuO/T-Al2O3, CuO/y-Al2O3-cordierite (Cord) and CuO/Cord, were prepared by impregnation method. The catalytic activity of the catalysts was tested in absence and presence of water vapor,and the catalysts were characterized. Temperature program desorption (TPD) experiments or toluene and water on the catalysts were carried out. The influence of water vapor on the activity of the catalysts was discussed. Results showed that addition of the water vapor has a significant negative effect on the catalytic activity of the catalysts.The higher the concentration of the Water vapor in feed steam was, the lower the catalytic activity of the copper based catalysts became, which could be mainly ascribed to the competition of water molecules with toluene molecules for adsorption on the catalyst surfaces. TPD experiments showed that the strength of the interaction between water molecules and three catalysts followed the order: CuO/γ-Al2O3〉CuO/γ-Al2O3-Cord〉CuO/Cord. As a consequence of that, the degree of degradation in the catalytic activity of these three catalysts by the water vapor followed the order: CuO/γ-Al2O3〉CuO/y-Al2O3-Cord〉CuO/Cord. However, the negative effect of the water vapor was reversible.
基金Work financially supported by the National Natural Science Foundation of China.
文摘The catalytic activity for the synthesis of methanol from carbon dioxide and hydrogen was measured on various binary and ternary catalysts containing copper oxide under a pressure of 10 atm. Among these samples the catalysts, CuO/ZnO/γ-Al_2O_3, demonstrated the highest activity and selectivity to methanol; MnO, as third component, had no promotional effect on the activity of meth- anol formation. Based on a simple power rate law the apparent activation energy estimation and par- tial pressure dependence measurement were accomplished over eight catalysts. The activation energies varied from 40 to 120 kJ / mol depending on the composition of catalysts. The rates of methanol for- mation to be 0.3 -- 0.9 order in H_2 and about 0.1 -- 0.2 order in CO_2 were reported.
基金Supported by the Natural Science Foundation of Science and Technology Department of Jilin Province, China(No.20130101015JC), the Open Project Supported by State Key Laboratory of Inorganic Synthesis and Preparative Chemistry of Jilin University, China (No.2012-15), and the Innovation Project of Frontiers of Science and New Interdiscipline of Jilin University, China.
文摘Direct transformation of ethanol to ethyl acetate was investigated on a series of Cu(ZrO2)/SiO2 catalysts. Inductively coupled plasma(ICP), surface area analysis, X-ray diffraction(XRD), H2-temperature programmed reduc- tion(H2-TPR), X-ray photoelectron spectroscopy(XPS), NH3-temperature programmed desorption(NH3-TPD) and Fourier transform-infrared spectroscopy(FTIR) techniques were used to characterize the catalysts. The results reveal that ZrO2 can improve the dispersion of copper species and increase the acidity of the Cu(ZrO2)/SiO2 catalysts. The Cu0 is responsible for ethanol dehydrogenation to acetaldehyde, and both the Lewis acid and Bronsted acid sites were in favor of the selectivity to ethyl acetate. The synergistic effect of Cu0 and an appropriate amount of acidic sites played an important role in the production of ethyl acetate.