The effects of CeO2 contents and silica carrier porosity with their pore diameters ranging from 5.2 nm to 12.5 nm of CuO-CeO2/SiO2 cata-lysts in CO oxidation were investigated.The catalysts were characterized by N2 ad...The effects of CeO2 contents and silica carrier porosity with their pore diameters ranging from 5.2 nm to 12.5 nm of CuO-CeO2/SiO2 cata-lysts in CO oxidation were investigated.The catalysts were characterized by N2 adsorption/desorption at low temperature,X-ray diffraction （XRD）,temperature-programmed reduction by H2 （H2-TPR）,oxygen temperature programmed desorption （O2-TPD） and X-ray photoelectron spectroscopy （XPS）.The results suggested that,the ceria content and the porosity of SiO2 carrier possessed great impacts on the structures and catalytic performances of CuO-CeO2/SiO2 catalysts.When appropriate content of CeO2 （Ce content 8 wt%） was added,the catalytic activity was greatly enhanced.In the catalyst supported on silica carrier with larger pore diameter,higher dispersion of CuO was observed,better agglomeration-resistant capacity was displayed and more lattice oxygen could be found,thus the CuO-CeO2 supported on Si-1 showed higher catalytic activity for low-temperature CO oxidation.展开更多
Two-step steam reforming of methane (SRM) is a novel chemical looping process towards the production of pure hydrogen and syngas (synthesis gas), consisting of a syngas production step and a water-splitting step. Rene...Two-step steam reforming of methane (SRM) is a novel chemical looping process towards the production of pure hydrogen and syngas (synthesis gas), consisting of a syngas production step and a water-splitting step. Renewable energy can be used to drive this process for hydrogen production, especially solar energy. CeO2-Fe2O3 complex oxide oxygen carrier was prepared by the impregnation method and characterized by means of X-ray diffractometer (XRD), Raman spectroscopy (Raman) and hydrogen programmed reduction (H2-TPR). CH4 temperature programmed and isothermal reactions were adopted to test syngas production reactivity, and water splitting reaction was employed to investigate water-splitting activity. Moreover, two-step SRM performance was evaluated by a successive redox cycle. The results showed that CO-uncontaminated H2 and highly selective syngas (with H2/CO ratio close to 2) could be respectively obtained from two steps, and CeFeO3 formation was found in the first redox cycle and proved to be enhanced by the redox treatment. After 10 successive cycles, obvious CeFeO3 phase was detected, which may be responsible for favorable successive redox cycle performances.展开更多
Effects of carrier gas composition（N2/air） on NH3 production, energy efficiency regarding NH3 production and byproducts formation from plasma-catalytic decomposition of urea were systematically investigated using an...Effects of carrier gas composition（N2/air） on NH3 production, energy efficiency regarding NH3 production and byproducts formation from plasma-catalytic decomposition of urea were systematically investigated using an Al2 O3-packed dielectric barrier discharge（DBD） reactor at room temperature. Results show that the presence of O2 in the carrier gas accelerates the conversion of urea but leads to less generation of NH3. The final yield of NH3 in the gas phase decreased from 70.5%, 78.7%, 66.6% and 67.2% to 54.1%, 51.7%, 49.6% and 53.4% for applied voltages of 17, 19, 21 and 23 kV, respectively when air was used as the carrier gas instead of N2.From the viewpoint of energy savings, however, air carrier gas is better than N2 due to reduced energy consumption and increased energy efficiency for decomposition of a fixed amount of urea. Carrier gas composition has little influence on the major decomposition pathways of urea under the synergetic effects of plasma and Al2 O3 catalyst to give NH3 and CO2 as the main products. Compared to a small amount of N2 O formed with N2 as the carrier gas, however,more byproducts including N2O and NO2 in the gas phase and NH4 NO3 in solid deposits were produced with air as the carrier gas, probably due to the unproductive consumption of NH3, the possible intermediate HNCO and even urea by the abundant active oxygen species and nitrogen oxides generated in air-DBD plasma.展开更多
基金supported by the National Natural Science Foundation of China(20590360)New Century Excellent Talent Project of China(NCET-05-0783)
文摘The effects of CeO2 contents and silica carrier porosity with their pore diameters ranging from 5.2 nm to 12.5 nm of CuO-CeO2/SiO2 cata-lysts in CO oxidation were investigated.The catalysts were characterized by N2 adsorption/desorption at low temperature,X-ray diffraction （XRD）,temperature-programmed reduction by H2 （H2-TPR）,oxygen temperature programmed desorption （O2-TPD） and X-ray photoelectron spectroscopy （XPS）.The results suggested that,the ceria content and the porosity of SiO2 carrier possessed great impacts on the structures and catalytic performances of CuO-CeO2/SiO2 catalysts.When appropriate content of CeO2 （Ce content 8 wt%） was added,the catalytic activity was greatly enhanced.In the catalyst supported on silica carrier with larger pore diameter,higher dispersion of CuO was observed,better agglomeration-resistant capacity was displayed and more lattice oxygen could be found,thus the CuO-CeO2 supported on Si-1 showed higher catalytic activity for low-temperature CO oxidation.
基金Project support by the National Natural Science Foundation of China (50574046, 50774038)the Natural Science Foundation of Yunnan Prov-ince (2008E030M)+1 种基金the Research Fund for the Doctoral Program of Higher Education of China (20095314120005)2010 Innovation Fund of Kunming University of Science and Technology
文摘Two-step steam reforming of methane (SRM) is a novel chemical looping process towards the production of pure hydrogen and syngas (synthesis gas), consisting of a syngas production step and a water-splitting step. Renewable energy can be used to drive this process for hydrogen production, especially solar energy. CeO2-Fe2O3 complex oxide oxygen carrier was prepared by the impregnation method and characterized by means of X-ray diffractometer (XRD), Raman spectroscopy (Raman) and hydrogen programmed reduction (H2-TPR). CH4 temperature programmed and isothermal reactions were adopted to test syngas production reactivity, and water splitting reaction was employed to investigate water-splitting activity. Moreover, two-step SRM performance was evaluated by a successive redox cycle. The results showed that CO-uncontaminated H2 and highly selective syngas (with H2/CO ratio close to 2) could be respectively obtained from two steps, and CeFeO3 formation was found in the first redox cycle and proved to be enhanced by the redox treatment. After 10 successive cycles, obvious CeFeO3 phase was detected, which may be responsible for favorable successive redox cycle performances.
基金supported by the National Natural Science Foundation of China (Nos. 21547004, 51638001)the Beijing Natural Science Foundation (No. 8152011)the Scientific Research Program of Beijing Municipal Education Commission (No. KM201510005009)
文摘Effects of carrier gas composition（N2/air） on NH3 production, energy efficiency regarding NH3 production and byproducts formation from plasma-catalytic decomposition of urea were systematically investigated using an Al2 O3-packed dielectric barrier discharge（DBD） reactor at room temperature. Results show that the presence of O2 in the carrier gas accelerates the conversion of urea but leads to less generation of NH3. The final yield of NH3 in the gas phase decreased from 70.5%, 78.7%, 66.6% and 67.2% to 54.1%, 51.7%, 49.6% and 53.4% for applied voltages of 17, 19, 21 and 23 kV, respectively when air was used as the carrier gas instead of N2.From the viewpoint of energy savings, however, air carrier gas is better than N2 due to reduced energy consumption and increased energy efficiency for decomposition of a fixed amount of urea. Carrier gas composition has little influence on the major decomposition pathways of urea under the synergetic effects of plasma and Al2 O3 catalyst to give NH3 and CO2 as the main products. Compared to a small amount of N2 O formed with N2 as the carrier gas, however,more byproducts including N2O and NO2 in the gas phase and NH4 NO3 in solid deposits were produced with air as the carrier gas, probably due to the unproductive consumption of NH3, the possible intermediate HNCO and even urea by the abundant active oxygen species and nitrogen oxides generated in air-DBD plasma.
