We investigated the effect of calcination temperature, reaction temperature, and different amounts of replenished lattice oxygen on the partial oxidation of methane (POM) to synthesis gas using perovskite-type LaFeO...We investigated the effect of calcination temperature, reaction temperature, and different amounts of replenished lattice oxygen on the partial oxidation of methane (POM) to synthesis gas using perovskite-type LaFeO3 oxide as oxygen donor instead of gaseous oxygen, which was prepared by the sol-gel method, and the oxides were characterized by XRD, TG/DTA, and BET. The results indicated that the particle size increased with the calcination temperature increasing, while BET and CH4 conversion declined with the calcination temperature increasing using LaFeO3 oxide as oxygen donor in the absence of gaseous oxygen. CO selectivity remained at a high level such as above 92%, and increased slightly as the calcination temperature increased. Exposure of LaFeO3 oxides to methane atmosphere enhanced the oxygen migration of in the bulk with time online owing to the loss of lattice oxygen and reduction of the oxidative stated Fe ion simultaneously, The high reaction temperature was favorable to the migration of oxygen species from the bulk toward the surface for the synthesis gas production with high CO selectivity. The product distribution and evolution for POM by sequential redox reaction was determined by amounts of replenished lattice oxygen with gaseous oxygen. The optimal process should decline the total oxidation of methane, and increase the selectivity of partial oxidation of methane.展开更多
We reported the effects of annealing temperatures on microstructure and electrochemical properties of perovskite-type oxide LaFeO3 prepared by stearic acid combustion method. X-Ray diffraction(XRD) patterns show tha...We reported the effects of annealing temperatures on microstructure and electrochemical properties of perovskite-type oxide LaFeO3 prepared by stearic acid combustion method. X-Ray diffraction(XRD) patterns show that the annealed LaFeO3 powder has orthorhombic structure. Scanning electron microscopy(SEM) and transmission electron microscopy(TEM) images show the presence of homogeneously dispersed, less aggregated, and small crystals(30--40 nm) at annealing temperatures of 500 and 600 ℃. However, as the annealing temperature was increased to 700 and 800 ℃, the crystals began to combine with each other and grew into further larger crystals(90--100 nm). The electrochemical performance of the annealed oxides was measured at 60 ℃ using chronopotentiometry, potentiodynamic polarization, and cyclic voltammetry. As the annealing temperature increased, the discharge capacity and anti-corrosion ability of the oxide electrode first increased and then decreased, reaching the optimum values at 600 ℃, with a maximum discharge capacity of 563 mA-h/g. The better electrochemical performance of LaFeO3 annealed at 600℃ could be ascribed to their smaller and more homogeneous crysals.展开更多
基金the National Natural Science Foundation of China (20306016, 20322201)
文摘We investigated the effect of calcination temperature, reaction temperature, and different amounts of replenished lattice oxygen on the partial oxidation of methane (POM) to synthesis gas using perovskite-type LaFeO3 oxide as oxygen donor instead of gaseous oxygen, which was prepared by the sol-gel method, and the oxides were characterized by XRD, TG/DTA, and BET. The results indicated that the particle size increased with the calcination temperature increasing, while BET and CH4 conversion declined with the calcination temperature increasing using LaFeO3 oxide as oxygen donor in the absence of gaseous oxygen. CO selectivity remained at a high level such as above 92%, and increased slightly as the calcination temperature increased. Exposure of LaFeO3 oxides to methane atmosphere enhanced the oxygen migration of in the bulk with time online owing to the loss of lattice oxygen and reduction of the oxidative stated Fe ion simultaneously, The high reaction temperature was favorable to the migration of oxygen species from the bulk toward the surface for the synthesis gas production with high CO selectivity. The product distribution and evolution for POM by sequential redox reaction was determined by amounts of replenished lattice oxygen with gaseous oxygen. The optimal process should decline the total oxidation of methane, and increase the selectivity of partial oxidation of methane.
基金Supported by the National Natural Science Foundation of China(Nos. 51771164, 51571173 and 51701175).
文摘We reported the effects of annealing temperatures on microstructure and electrochemical properties of perovskite-type oxide LaFeO3 prepared by stearic acid combustion method. X-Ray diffraction(XRD) patterns show that the annealed LaFeO3 powder has orthorhombic structure. Scanning electron microscopy(SEM) and transmission electron microscopy(TEM) images show the presence of homogeneously dispersed, less aggregated, and small crystals(30--40 nm) at annealing temperatures of 500 and 600 ℃. However, as the annealing temperature was increased to 700 and 800 ℃, the crystals began to combine with each other and grew into further larger crystals(90--100 nm). The electrochemical performance of the annealed oxides was measured at 60 ℃ using chronopotentiometry, potentiodynamic polarization, and cyclic voltammetry. As the annealing temperature increased, the discharge capacity and anti-corrosion ability of the oxide electrode first increased and then decreased, reaching the optimum values at 600 ℃, with a maximum discharge capacity of 563 mA-h/g. The better electrochemical performance of LaFeO3 annealed at 600℃ could be ascribed to their smaller and more homogeneous crysals.