Despite of considerable efforts on the MnO2-based catalytic combustion,the different structural and component requirements of MnO2 for gas-phase selective oxidation and complete oxidation largely remain unknown.By com...Despite of considerable efforts on the MnO2-based catalytic combustion,the different structural and component requirements of MnO2 for gas-phase selective oxidation and complete oxidation largely remain unknown.By comparing four types of MnO2 with different crystal structures(α,β,γandδ),γ-MnO2 was found to be the most efficient catalyst for both aerobic selective oxidation of ethanol and CO oxidation.The structural effect ofγ-MnO2 was further investigated by doping metal ions into the framework and by comparing the catalytic performance in the gas-phase aerobic oxidation of CO and ethanol.Among ten M-γ-MnO2 catalysts,Zn-γ-MnO2 showed the lowest temperature(160°C)for achieving 90%CO conversion.The CO oxidation activity of the M-γ-MnO2 catalysts was found to be more relevant to the surface acidity-basicity than the reducibility.In contrast,surface reducibility has been demonstrated to be more crucial in the gas-phase ethanol oxidation.Cu-γ-MnO2 with higher reducibility and more oxygen vacancies of Mn^2+/Mn^3+species exhibited higher catalytic activity in the selective ethanol oxidation.Cu-γ-MnO2 achieved the highest acetaldehyde yield(75%)and space-time-yield(5.4 g gcat^-1 h^-1)at 200°C,which are even comparable to the results obtained by the state-of-the-art silver and gold-containing catalysts.Characterization results and kinetic studies further suggest that the CO oxidation follows the lattice oxygen-based Mars-van Krevelen mechanism,whereas both surface lattice oxygen and adsorbed oxygen species involve in the ethanol activation.展开更多
Mn/Ni composite oxides as active electrode materials for supercapacitors were prepared by solid-state reaction through the reduction of KMnO4 with manganese acetate and nickel acetate at low temperature. The products ...Mn/Ni composite oxides as active electrode materials for supercapacitors were prepared by solid-state reaction through the reduction of KMnO4 with manganese acetate and nickel acetate at low temperature. The products were characterized by X-ray diffractometry(XRD) and transmission electron microscopy(TEM). The electrochemical characterizations were performed by cyclic voltammetry (CV) and constant current charge-discharge in a three-electrode system. The effects of different potential windows, scan rates, and cycle numbers on the capacitance behavior of Mn0.8Ni0.2Ox composite oxide were also investigated. The results show that the composite oxides are of nano-size and amorphous structure. With increasing the molar ratio of Ni, the specific capacitance goes through a maximum at molar fraction of Ni of 20%. The specific capacitance of Mn0.8Ni0.2Ox composite oxide is 194.5 F/g at constant current discharge of 5 mA.展开更多
文摘Despite of considerable efforts on the MnO2-based catalytic combustion,the different structural and component requirements of MnO2 for gas-phase selective oxidation and complete oxidation largely remain unknown.By comparing four types of MnO2 with different crystal structures(α,β,γandδ),γ-MnO2 was found to be the most efficient catalyst for both aerobic selective oxidation of ethanol and CO oxidation.The structural effect ofγ-MnO2 was further investigated by doping metal ions into the framework and by comparing the catalytic performance in the gas-phase aerobic oxidation of CO and ethanol.Among ten M-γ-MnO2 catalysts,Zn-γ-MnO2 showed the lowest temperature(160°C)for achieving 90%CO conversion.The CO oxidation activity of the M-γ-MnO2 catalysts was found to be more relevant to the surface acidity-basicity than the reducibility.In contrast,surface reducibility has been demonstrated to be more crucial in the gas-phase ethanol oxidation.Cu-γ-MnO2 with higher reducibility and more oxygen vacancies of Mn^2+/Mn^3+species exhibited higher catalytic activity in the selective ethanol oxidation.Cu-γ-MnO2 achieved the highest acetaldehyde yield(75%)and space-time-yield(5.4 g gcat^-1 h^-1)at 200°C,which are even comparable to the results obtained by the state-of-the-art silver and gold-containing catalysts.Characterization results and kinetic studies further suggest that the CO oxidation follows the lattice oxygen-based Mars-van Krevelen mechanism,whereas both surface lattice oxygen and adsorbed oxygen species involve in the ethanol activation.
基金Project(20060390889) supported by China Postdoctoral Science FoundationProject (2006FJ4236) supported by Hunan Postdoctoral Scientific Program
文摘Mn/Ni composite oxides as active electrode materials for supercapacitors were prepared by solid-state reaction through the reduction of KMnO4 with manganese acetate and nickel acetate at low temperature. The products were characterized by X-ray diffractometry(XRD) and transmission electron microscopy(TEM). The electrochemical characterizations were performed by cyclic voltammetry (CV) and constant current charge-discharge in a three-electrode system. The effects of different potential windows, scan rates, and cycle numbers on the capacitance behavior of Mn0.8Ni0.2Ox composite oxide were also investigated. The results show that the composite oxides are of nano-size and amorphous structure. With increasing the molar ratio of Ni, the specific capacitance goes through a maximum at molar fraction of Ni of 20%. The specific capacitance of Mn0.8Ni0.2Ox composite oxide is 194.5 F/g at constant current discharge of 5 mA.
