An efficient route for the synthesis of 5-substituted 1H-tetrazole via [2＋3] cycloaddition of nitriles and sodium azide is reported using Fe3O4/ZnS hollow nanospheres as a magnetic separable heterogeneous catalyst. T...An efficient route for the synthesis of 5-substituted 1H-tetrazole via [2＋3] cycloaddition of nitriles and sodium azide is reported using Fe3O4/ZnS hollow nanospheres as a magnetic separable heterogeneous catalyst. The catalyst is very efficient, affording excellent yields and can be reused for several circles. In addition, the Fe3O4 inner shell exhibits magnetism, making the catalyst easily separated by a magnet.展开更多
The relationship between the activity and the precursor phase composition of the molten iron catalyst for ammonia synthesis has been studied with high pressure testing equipment and XRD. A humped curve between the act...The relationship between the activity and the precursor phase composition of the molten iron catalyst for ammonia synthesis has been studied with high pressure testing equipment and XRD. A humped curve between the activity and Fe2+/Fe3+ has been obtained. It is found that the unicity of the iron oxidate phase in precursor is an essential condition of the high activity of the iron catalyst and that the uniform distribution of the adominant phase and the promoters is the key to preparing a catalyst with better performance The humped curve is interpreted using the ratio f of the phase compositions in precursor. A new idea has been obtained that the activity change of the molten iron catalyst depends essentially on the molecule ratio of the different iron oxidates in precursor under the certain promoters, and it is found that the FeO based catalyst for ammonia synthesis with Wustite phase structure (Fe1-xO, 0.04≤x≤0.10) has the highest activity of all the molten iron catalysts for ammonia synthesis.展开更多
A series of Fe2O3/Al2O3, Fe2O3/CeO2, Ce0.7Zr0.3O2, and Fe2O3/Ce1-xZrxO2（x = 0.1–0.4） oxides was prepared and their physicochemical features were investigated by X-ray diffraction（XRD）, transmission electron micro...A series of Fe2O3/Al2O3, Fe2O3/CeO2, Ce0.7Zr0.3O2, and Fe2O3/Ce1-xZrxO2（x = 0.1–0.4） oxides was prepared and their physicochemical features were investigated by X-ray diffraction（XRD）, transmission electron microscope（TEM）, and H2-temperature-programmed reduction（H2-TPR） techniques. The gas–solid reactions between these oxides and methane for syngas generation as well as the catalytic performance for selective oxidation of carbon deposition in O2-enriched atmosphere were investigated in detail. The results show that the samples with the presence of Fe2O3show much higher activity for methane oxidation compared with the Ce0.7Zr0.3O2solid solution,while the CeO2-contained samples represent higher CO selectively in methane oxidation than the Fe2O3/Al2O3sample. This suggests that the iron species should be the active sites for methane activation, and the cerium oxides provide the oxygen source for the selective oxidation of the activated methane to syngas during the reaction between methane and Fe2O3/Ce0.7Zr0.3O2. For the oxidation process of the carbon deposition, the CeO2-containing samples show much higher CO selectivity than the Fe2O3/Al2O3sample, which indicates that the cerium species should play a very important role in catalyzing the carbon selective oxidation to CO. The presence of the Ce–Zr–O solid solution could induce the growth direction of the carbonfilament, resulting in a loose contact between the carbon filament and the catalyst. This results in abundant exposed active sites for catalyzing carbon oxidation, strongly improving the oxidation rate of the carbon deposition over this sample. In addition, the Fe2O3/Ce0.7Zr0.3O2also represents much higher selectivity（ca. 97 %） for the conversion of carbon to CO than the Fe2O3/CeO2sample, which can be attributed to the higher concentration of reduced cerium sites on this sample. The increase of the Zr content in the Fe2O3/Ce1-xZrxO2samples could improve the reactivity of the materials for methane oxidation, but it also reduces the selectivity for CO formation.展开更多
文摘An efficient route for the synthesis of 5-substituted 1H-tetrazole via [2＋3] cycloaddition of nitriles and sodium azide is reported using Fe3O4/ZnS hollow nanospheres as a magnetic separable heterogeneous catalyst. The catalyst is very efficient, affording excellent yields and can be reused for several circles. In addition, the Fe3O4 inner shell exhibits magnetism, making the catalyst easily separated by a magnet.
基金Project supported by the Provincial Natural Science Foundation of Zhejiang.
文摘The relationship between the activity and the precursor phase composition of the molten iron catalyst for ammonia synthesis has been studied with high pressure testing equipment and XRD. A humped curve between the activity and Fe2+/Fe3+ has been obtained. It is found that the unicity of the iron oxidate phase in precursor is an essential condition of the high activity of the iron catalyst and that the uniform distribution of the adominant phase and the promoters is the key to preparing a catalyst with better performance The humped curve is interpreted using the ratio f of the phase compositions in precursor. A new idea has been obtained that the activity change of the molten iron catalyst depends essentially on the molecule ratio of the different iron oxidates in precursor under the certain promoters, and it is found that the FeO based catalyst for ammonia synthesis with Wustite phase structure (Fe1-xO, 0.04≤x≤0.10) has the highest activity of all the molten iron catalysts for ammonia synthesis.
基金financially supported by the National Natural Science Foundation of China (Nos. 51004060, 51104074, and 51174105)the Natural Science Foundation of Yunnan Province (No. 2010ZC018)
文摘A series of Fe2O3/Al2O3, Fe2O3/CeO2, Ce0.7Zr0.3O2, and Fe2O3/Ce1-xZrxO2（x = 0.1–0.4） oxides was prepared and their physicochemical features were investigated by X-ray diffraction（XRD）, transmission electron microscope（TEM）, and H2-temperature-programmed reduction（H2-TPR） techniques. The gas–solid reactions between these oxides and methane for syngas generation as well as the catalytic performance for selective oxidation of carbon deposition in O2-enriched atmosphere were investigated in detail. The results show that the samples with the presence of Fe2O3show much higher activity for methane oxidation compared with the Ce0.7Zr0.3O2solid solution,while the CeO2-contained samples represent higher CO selectively in methane oxidation than the Fe2O3/Al2O3sample. This suggests that the iron species should be the active sites for methane activation, and the cerium oxides provide the oxygen source for the selective oxidation of the activated methane to syngas during the reaction between methane and Fe2O3/Ce0.7Zr0.3O2. For the oxidation process of the carbon deposition, the CeO2-containing samples show much higher CO selectivity than the Fe2O3/Al2O3sample, which indicates that the cerium species should play a very important role in catalyzing the carbon selective oxidation to CO. The presence of the Ce–Zr–O solid solution could induce the growth direction of the carbonfilament, resulting in a loose contact between the carbon filament and the catalyst. This results in abundant exposed active sites for catalyzing carbon oxidation, strongly improving the oxidation rate of the carbon deposition over this sample. In addition, the Fe2O3/Ce0.7Zr0.3O2also represents much higher selectivity（ca. 97 %） for the conversion of carbon to CO than the Fe2O3/CeO2sample, which can be attributed to the higher concentration of reduced cerium sites on this sample. The increase of the Zr content in the Fe2O3/Ce1-xZrxO2samples could improve the reactivity of the materials for methane oxidation, but it also reduces the selectivity for CO formation.
