A series of CexPr1-xO2-δ (x=0, 0.5, 0.9, 1.0) mixed oxide calcined at different temperatures were synthesized by sol-gel method and characterized by Raman, XRD and O2-TPD techniques. When x=0.9, only a cubic phase Ce...A series of CexPr1-xO2-δ (x=0, 0.5, 0.9, 1.0) mixed oxide calcined at different temperatures were synthesized by sol-gel method and characterized by Raman, XRD and O2-TPD techniques. When x=0.9, only a cubic phase CeO2 is observed. When x=0.5, the compound was combined by Pr6O11 and CeO2 mixed oxides. For CexPr1-xO2-δ (x=0.5, 0.9)samples 465 cm-1 Raman peak is attributed to the Raman active F2g mode of CeO2. The broad peak at about 570 cm-1 can be linked to lattice defects resulting in oxygen vacancies. The crystallite size of the samples increased as increasing the calcined temperature. But the increased value of Ce0.9Pr0.1O2-δ and Ce0.5Pr0.5O2-δ is smaller than single CeO2 and Pr6O11 obviously. It reveals that the insertion of Pr atom into the ceria lattice could enhance the sintering resistance and thermal stability of the mixed oxides. Calcination temperatures had great effect on the peak intensity for CeO2 but less effect on Ce0.8Pr0.2O2-δ in Raman spectra, and it may be caused by the colors transformation of the mixed oxides. The result of O2-TPD experiment indicates that the formation of solid solution has elevation the stabilization and thermal stability of the mixed oxides.展开更多
Ce x Ti 1- x O 2 mixed oxides of different mole ratios ( x =0, 0.1, 0.2～0.9, 1.0) were prepared by co precipitation of TiCl 4 with Ce(NO 3) 3 and then loaded with different amounts of CuO. The effe...Ce x Ti 1- x O 2 mixed oxides of different mole ratios ( x =0, 0.1, 0.2～0.9, 1.0) were prepared by co precipitation of TiCl 4 with Ce(NO 3) 3 and then loaded with different amounts of CuO. The effects of CuO on NO+CO reaction were investigated, and the structure and reductive properties of various CuO/Ce x Ti 1- x O 2 were characterized by the methodologies of BET, TPR and XRD. The results show that different Ce/Ti mole ratios and calcination temperatures induce changes of structure and reductive properties of the Ce x Ti 1- x O 2 mixed oxides. When x =0.1～0.5, amorphous CeTi 2O 6 phase mainly forms at 650 ℃ compared to the formation of CeTi 2O 6 which crystallizes at 800 ℃. When x >0.6, some TiO 2 enters the CeO 2 lattice and a CeO 2 TiO 2 solid solution is formed. The activity of 6%CuO/Ce x Ti 1- x O 2 calcined at 650 ℃ is largely affected by the x values, which is the highest when x =0.3, 0.4 and 0.9. The NO conversion reaches 70% at a reaction temperature of 150 ℃. By comparison, the x values have little effect on the activity of 6%CuO/Ce x Ti 1- x O 2 calcined at 800 ℃ . There are strong interactions between CuO and CeTi 2O 6, i.e., formation of the CeTi 2O 6 phase shifts the CuO reduction peak temperature from 380 to 200 ℃, and CuO, in turn, shifts the CeTi 2O 6 reduction peak temperature from 600 to 300 ℃.展开更多
Using SnxTi1-xO2 as carriers, CuO/Sn0.9Zi0.1O2 and CuO/Sn0.7Ti0.3O2 catalysts with different loading amounts of copper oxide （CuO） were prepared by an impregnation method. The catalytic properties of CuO/Sn0.9Ti0.1O...Using SnxTi1-xO2 as carriers, CuO/Sn0.9Zi0.1O2 and CuO/Sn0.7Ti0.3O2 catalysts with different loading amounts of copper oxide （CuO） were prepared by an impregnation method. The catalytic properties of CuO/Sn0.9Ti0.1O2 and CuO/Sn0.7Zi0.3O2 were examined using a microreactor-gas chromatography （GC） NO＋CO reaction system and the methods of BET （Brun- auer-Emmett-Teller）, TG-DTA （themogravimetric and differential thermal analysis）, X-ray diffraction （XRD） and H2-temperature programmed reduction （TPR）. The results showed that NO conversions of Sn0.9Zi0.1O2 and Sn0.7Ti0.3O2 were 47.2% and 43.6% respectively, which increased to 95.3% and 90.9% at 6 wt% CuO loading. However, further increase in CuO loading caused a decrease in the catalytic activity. The nitrogen adsorption-desorption isotherm and pore-size distribution curve of Sn0.9Zi0.1O2 and Sn0.7Ti0.3O2 represented type IV of the BDDT （Brunauer, Deming, Deming and Teller） system and a typical mesoporous sample. There were two CuO diffraction peaks （2θ 35.5° and 38.7°）, and the diffraction peak areas increased with increasing CuO loading. TPR analysis also detected three peaks （α, β and γ） from the CuO-loaded catalysts, suggesting that the α peak was the reduction of the highly dispersed copper oxide, the β peak was the reduction of the isolated copper oxide, and the y peak was the reduction of crystal phase copper oxide. In addition, a fourth peak （5） of the catalysts meant that the SnxTi1-xO2 mixed oxides could be reductive.展开更多
文摘A series of CexPr1-xO2-δ (x=0, 0.5, 0.9, 1.0) mixed oxide calcined at different temperatures were synthesized by sol-gel method and characterized by Raman, XRD and O2-TPD techniques. When x=0.9, only a cubic phase CeO2 is observed. When x=0.5, the compound was combined by Pr6O11 and CeO2 mixed oxides. For CexPr1-xO2-δ (x=0.5, 0.9)samples 465 cm-1 Raman peak is attributed to the Raman active F2g mode of CeO2. The broad peak at about 570 cm-1 can be linked to lattice defects resulting in oxygen vacancies. The crystallite size of the samples increased as increasing the calcined temperature. But the increased value of Ce0.9Pr0.1O2-δ and Ce0.5Pr0.5O2-δ is smaller than single CeO2 and Pr6O11 obviously. It reveals that the insertion of Pr atom into the ceria lattice could enhance the sintering resistance and thermal stability of the mixed oxides. Calcination temperatures had great effect on the peak intensity for CeO2 but less effect on Ce0.8Pr0.2O2-δ in Raman spectra, and it may be caused by the colors transformation of the mixed oxides. The result of O2-TPD experiment indicates that the formation of solid solution has elevation the stabilization and thermal stability of the mixed oxides.
文摘Ce x Ti 1- x O 2 mixed oxides of different mole ratios ( x =0, 0.1, 0.2～0.9, 1.0) were prepared by co precipitation of TiCl 4 with Ce(NO 3) 3 and then loaded with different amounts of CuO. The effects of CuO on NO+CO reaction were investigated, and the structure and reductive properties of various CuO/Ce x Ti 1- x O 2 were characterized by the methodologies of BET, TPR and XRD. The results show that different Ce/Ti mole ratios and calcination temperatures induce changes of structure and reductive properties of the Ce x Ti 1- x O 2 mixed oxides. When x =0.1～0.5, amorphous CeTi 2O 6 phase mainly forms at 650 ℃ compared to the formation of CeTi 2O 6 which crystallizes at 800 ℃. When x >0.6, some TiO 2 enters the CeO 2 lattice and a CeO 2 TiO 2 solid solution is formed. The activity of 6%CuO/Ce x Ti 1- x O 2 calcined at 650 ℃ is largely affected by the x values, which is the highest when x =0.3, 0.4 and 0.9. The NO conversion reaches 70% at a reaction temperature of 150 ℃. By comparison, the x values have little effect on the activity of 6%CuO/Ce x Ti 1- x O 2 calcined at 800 ℃ . There are strong interactions between CuO and CeTi 2O 6, i.e., formation of the CeTi 2O 6 phase shifts the CuO reduction peak temperature from 380 to 200 ℃, and CuO, in turn, shifts the CeTi 2O 6 reduction peak temperature from 600 to 300 ℃.
基金Project (No. Y504131) supported by the Natural Science Foundation of Zhejiang Province, China
文摘Using SnxTi1-xO2 as carriers, CuO/Sn0.9Zi0.1O2 and CuO/Sn0.7Ti0.3O2 catalysts with different loading amounts of copper oxide （CuO） were prepared by an impregnation method. The catalytic properties of CuO/Sn0.9Ti0.1O2 and CuO/Sn0.7Zi0.3O2 were examined using a microreactor-gas chromatography （GC） NO＋CO reaction system and the methods of BET （Brun- auer-Emmett-Teller）, TG-DTA （themogravimetric and differential thermal analysis）, X-ray diffraction （XRD） and H2-temperature programmed reduction （TPR）. The results showed that NO conversions of Sn0.9Zi0.1O2 and Sn0.7Ti0.3O2 were 47.2% and 43.6% respectively, which increased to 95.3% and 90.9% at 6 wt% CuO loading. However, further increase in CuO loading caused a decrease in the catalytic activity. The nitrogen adsorption-desorption isotherm and pore-size distribution curve of Sn0.9Zi0.1O2 and Sn0.7Ti0.3O2 represented type IV of the BDDT （Brunauer, Deming, Deming and Teller） system and a typical mesoporous sample. There were two CuO diffraction peaks （2θ 35.5° and 38.7°）, and the diffraction peak areas increased with increasing CuO loading. TPR analysis also detected three peaks （α, β and γ） from the CuO-loaded catalysts, suggesting that the α peak was the reduction of the highly dispersed copper oxide, the β peak was the reduction of the isolated copper oxide, and the y peak was the reduction of crystal phase copper oxide. In addition, a fourth peak （5） of the catalysts meant that the SnxTi1-xO2 mixed oxides could be reductive.
