The three way catalysts (TWCs) promoters (Ce Zr)O 2, (Pr Ce Zr)O 2 and (Pr Zr)O 2 were prepared by sol gel like method. They were characterized by XRD, EXAFS and BET surface area determination. The reduction ...The three way catalysts (TWCs) promoters (Ce Zr)O 2, (Pr Ce Zr)O 2 and (Pr Zr)O 2 were prepared by sol gel like method. They were characterized by XRD, EXAFS and BET surface area determination. The reduction features of the promoters were measured by temperature programmed reduction (TPR) of H 2 to access the potential for the promoters containing praseodymia as oxygen storage component in three way catalyst. The (Pr Zr)O 2 cubic solid solution is formed at high temperature up to 800 ℃, which makes it more reducible than the (Ce Zr)O 2 solid solution. For the (Pr Ce Zr)O 2 samples, the ternary solid solution plays an important role in the reduction process. The performance of the three way catalysts with fully formulated Pt, Pd and Rh is proceeded by using both light off temperature under a stoichiometric gas composition and the conversion of CO, C 3H 6 and NO under changing air/fuel ratio at a constant reaction temperature 400 ℃ . The results indicate that a small amount of praseodymia doping into (Ce Zr)O 2 favors the light off temperature of C 3H 6 and NO, and all the catalysts containing praseodymia obviously exhibits enhanced width of S value for NO conversion at lean region ( S ≥1.00).展开更多
The Ce0.7Zr0.3O2 solid solution and CeO2 were prepared using the sol-gel method. The phase structure, crystallite sizes and the reducibility of the catalysts were characterized by XRD and H2-TPR techniques. XRD result...The Ce0.7Zr0.3O2 solid solution and CeO2 were prepared using the sol-gel method. The phase structure, crystallite sizes and the reducibility of the catalysts were characterized by XRD and H2-TPR techniques. XRD results indicated that Zr^4+ had replaced part of Ce^4+ to form a fluorite-like solid solution, which was favorable to obtain ultrafine nanoparticles. The ratio of main HE consumption for Ce0.7Zr0.3O2:CeO2 was 4.4:1.0, implying that the solid solution could improve the reducibility compared to the single CeO2. The Ce0.7Zr0.3O2 solid solution catalyst showed a sharp combustion peak at 397 ℃, which was 200 ℃ lower than that of the single soot. The good catalytic activity of the Ce0.7Zr0.3O2 was attributed to the formation of nano-CeO2-based solid solution, which enhanced the reducibility and then improved the combustion activity. As Ce0.7Zr0.3O2 could be easily reduced to Ce0.7Zr0.3O2-x meanwhile, after oxygenation, the Ce0.7Zr0.3O2.x was recovered to Ce0.7Zr0.3O2 completely. A catalytic combustion reaction mechanism was proposed: the Ce0.7Zr0.3O2 was reduced to Ce0.7Zr0.3O2-x by the reaction with carbon and then it was recovered to Ce0.7Zr0.3O2-x by the interaction with O2.展开更多
Ce Zr O solid solution was prepared by four different methods, i.e., decomposition of nitrate, coprecipiation, hydroxysuainic acid sol gel as well as citrate sol gel, and characterized by using X ray powder diffr...Ce Zr O solid solution was prepared by four different methods, i.e., decomposition of nitrate, coprecipiation, hydroxysuainic acid sol gel as well as citrate sol gel, and characterized by using X ray powder diffraction, Raman and temperature programmed reduction. The phase composition and the reduction properties of Ce Zr O depend on the preparation method. A cubic Ce 0.5 Zr 0.5 O 2 solid solution can be obtained by using the sol gel method. The Ce Zr O solid solution prepared by using decomposition or coprecipiation was composed of cubic Ce 0.8 Zr 0.2 O 2 and tetragonal Ce 0.2 Zr 0.8 O 2 solid solution. The Ce Zr O solid solution prepared with different methods shows the different reduction properties owing to different phase composition. Results of differential thermal analysis and XRD show that Ce 0.5 Zr 0.5 O 2 solid solution is formed during the decomposition or combustion of the gel.展开更多
Nanosized Ce^1-x)(Nd^0.5)Eu^0.5))xO^2-δ) solid solutions(x = 0.00-0.20) were synthesized by means of hydrothermal method.Then the solid solutions were ball milled with Mg2Ni and Ni powders for 20 h to get the...Nanosized Ce^1-x)(Nd^0.5)Eu^0.5))xO^2-δ) solid solutions(x = 0.00-0.20) were synthesized by means of hydrothermal method.Then the solid solutions were ball milled with Mg2Ni and Ni powders for 20 h to get the Mg2Ni–Ni–5 mol% Ce^1-x)(Nd^0.5)Eu^0.5))xO^2-δ) composites.The structures and spectrum characteristics of the Ce^1-x)(Nd^0.5)Eu^0.5))xO^2-δ) solid solutions catalysts were analyzed systemically.XRD results showed that the doped samples exhibited single phase of CeO2 fluorite structure.The cell parameters and cell volumes were increased with increasing the doped content.Raman spectrum revealed that the peak position of F^2g mode shift to higher wavenumbers and the peak corresponding to oxygen vacancies were observed distinctly for the doped samples.UV-Vis technique indicated that the absorption peaks of Eu^3+ and Nd^3+ ions appeared; the bandgap energy was decreased linearly.The electrochemical and kinetic properties of the Mg2Ni–Ni–5 mol% Ce1-x(Nd0.5Eu0.5xO2-δ composites were measured.The maximum discharge capacity was increased from 722.3 mA h/g for x = 0.00 to 819.7 mA h/g for x = 0.16,and the cycle stability S20 increased from 25.0%(x = 0.00) to 42.2%(x = 0.20).The kinetic measurement proved that the catalytic activity of composite surfaces and the hydrogen diffusion rate were improved for the composites with doped catalysts,especially for the composites with x = 0.16 and x = 0.20.The catalysis mechanism was analyzed from the point of microstructure and spectrum features of the Ce1-x(Nd0.5Eu0.5)xO2-δ solid solutions.展开更多
The three-way catalysts (TWCs) promoters Ce0.6Zr0.4- x TbxO2-y were prepared by sol-gel method. BET surface areas analysis indicated that an increase of the dopant Tb content from x = 0.05 to x = 0.15 favors an incr...The three-way catalysts (TWCs) promoters Ce0.6Zr0.4- x TbxO2-y were prepared by sol-gel method. BET surface areas analysis indicated that an increase of the dopant Tb content from x = 0.05 to x = 0.15 favors an increase of surface area from 66.8 to 80.4 m^2· g^-1 compared with the undoped sample Ce0 .6oZr0.40O2 65.1 m^2·g^- 1 after calcination at 650℃. Transmission electron microscopy (TEM) observation indicated that the doped samples have a higher thermal stability. The XRD and Raman spectra confirmed that the Ce0.6Zr0.4-xTbxO2-y cubic solid solution is formed. XPS analysis revealed that Ce and Tb mainly existed in the form of Ce^4+ and Tb^3 + , and Zr existed in the form of Zr^4+ on the surface of the samples. The doped samples were homogenous in composition ; the introduction of Tb into the CeO2-ZrO2 promoters resuited in the formation of a solid solution, and the concentration of surface lattice oxygen was increased.展开更多
文摘The three way catalysts (TWCs) promoters (Ce Zr)O 2, (Pr Ce Zr)O 2 and (Pr Zr)O 2 were prepared by sol gel like method. They were characterized by XRD, EXAFS and BET surface area determination. The reduction features of the promoters were measured by temperature programmed reduction (TPR) of H 2 to access the potential for the promoters containing praseodymia as oxygen storage component in three way catalyst. The (Pr Zr)O 2 cubic solid solution is formed at high temperature up to 800 ℃, which makes it more reducible than the (Ce Zr)O 2 solid solution. For the (Pr Ce Zr)O 2 samples, the ternary solid solution plays an important role in the reduction process. The performance of the three way catalysts with fully formulated Pt, Pd and Rh is proceeded by using both light off temperature under a stoichiometric gas composition and the conversion of CO, C 3H 6 and NO under changing air/fuel ratio at a constant reaction temperature 400 ℃ . The results indicate that a small amount of praseodymia doping into (Ce Zr)O 2 favors the light off temperature of C 3H 6 and NO, and all the catalysts containing praseodymia obviously exhibits enhanced width of S value for NO conversion at lean region ( S ≥1.00).
基金the Natural Science Foundation of Zhejiang Province (Z404383)
文摘The Ce0.7Zr0.3O2 solid solution and CeO2 were prepared using the sol-gel method. The phase structure, crystallite sizes and the reducibility of the catalysts were characterized by XRD and H2-TPR techniques. XRD results indicated that Zr^4+ had replaced part of Ce^4+ to form a fluorite-like solid solution, which was favorable to obtain ultrafine nanoparticles. The ratio of main HE consumption for Ce0.7Zr0.3O2:CeO2 was 4.4:1.0, implying that the solid solution could improve the reducibility compared to the single CeO2. The Ce0.7Zr0.3O2 solid solution catalyst showed a sharp combustion peak at 397 ℃, which was 200 ℃ lower than that of the single soot. The good catalytic activity of the Ce0.7Zr0.3O2 was attributed to the formation of nano-CeO2-based solid solution, which enhanced the reducibility and then improved the combustion activity. As Ce0.7Zr0.3O2 could be easily reduced to Ce0.7Zr0.3O2-x meanwhile, after oxygenation, the Ce0.7Zr0.3O2.x was recovered to Ce0.7Zr0.3O2 completely. A catalytic combustion reaction mechanism was proposed: the Ce0.7Zr0.3O2 was reduced to Ce0.7Zr0.3O2-x by the reaction with carbon and then it was recovered to Ce0.7Zr0.3O2-x by the interaction with O2.
文摘Ce Zr O solid solution was prepared by four different methods, i.e., decomposition of nitrate, coprecipiation, hydroxysuainic acid sol gel as well as citrate sol gel, and characterized by using X ray powder diffraction, Raman and temperature programmed reduction. The phase composition and the reduction properties of Ce Zr O depend on the preparation method. A cubic Ce 0.5 Zr 0.5 O 2 solid solution can be obtained by using the sol gel method. The Ce Zr O solid solution prepared by using decomposition or coprecipiation was composed of cubic Ce 0.8 Zr 0.2 O 2 and tetragonal Ce 0.2 Zr 0.8 O 2 solid solution. The Ce Zr O solid solution prepared with different methods shows the different reduction properties owing to different phase composition. Results of differential thermal analysis and XRD show that Ce 0.5 Zr 0.5 O 2 solid solution is formed during the decomposition or combustion of the gel.
基金supported by the National Natural Science Foundations of China(51501095,51371094)the Natural Science Foundation of Inner Mongolia(2017MS(LH)0516)
文摘Nanosized Ce^1-x)(Nd^0.5)Eu^0.5))xO^2-δ) solid solutions(x = 0.00-0.20) were synthesized by means of hydrothermal method.Then the solid solutions were ball milled with Mg2Ni and Ni powders for 20 h to get the Mg2Ni–Ni–5 mol% Ce^1-x)(Nd^0.5)Eu^0.5))xO^2-δ) composites.The structures and spectrum characteristics of the Ce^1-x)(Nd^0.5)Eu^0.5))xO^2-δ) solid solutions catalysts were analyzed systemically.XRD results showed that the doped samples exhibited single phase of CeO2 fluorite structure.The cell parameters and cell volumes were increased with increasing the doped content.Raman spectrum revealed that the peak position of F^2g mode shift to higher wavenumbers and the peak corresponding to oxygen vacancies were observed distinctly for the doped samples.UV-Vis technique indicated that the absorption peaks of Eu^3+ and Nd^3+ ions appeared; the bandgap energy was decreased linearly.The electrochemical and kinetic properties of the Mg2Ni–Ni–5 mol% Ce1-x(Nd0.5Eu0.5xO2-δ composites were measured.The maximum discharge capacity was increased from 722.3 mA h/g for x = 0.00 to 819.7 mA h/g for x = 0.16,and the cycle stability S20 increased from 25.0%(x = 0.00) to 42.2%(x = 0.20).The kinetic measurement proved that the catalytic activity of composite surfaces and the hydrogen diffusion rate were improved for the composites with doped catalysts,especially for the composites with x = 0.16 and x = 0.20.The catalysis mechanism was analyzed from the point of microstructure and spectrum features of the Ce1-x(Nd0.5Eu0.5)xO2-δ solid solutions.
基金Project supported by the Natural Science Basic Research Plan in Shaanxi Province of China (2004B13)
文摘The three-way catalysts (TWCs) promoters Ce0.6Zr0.4- x TbxO2-y were prepared by sol-gel method. BET surface areas analysis indicated that an increase of the dopant Tb content from x = 0.05 to x = 0.15 favors an increase of surface area from 66.8 to 80.4 m^2· g^-1 compared with the undoped sample Ce0 .6oZr0.40O2 65.1 m^2·g^- 1 after calcination at 650℃. Transmission electron microscopy (TEM) observation indicated that the doped samples have a higher thermal stability. The XRD and Raman spectra confirmed that the Ce0.6Zr0.4-xTbxO2-y cubic solid solution is formed. XPS analysis revealed that Ce and Tb mainly existed in the form of Ce^4+ and Tb^3 + , and Zr existed in the form of Zr^4+ on the surface of the samples. The doped samples were homogenous in composition ; the introduction of Tb into the CeO2-ZrO2 promoters resuited in the formation of a solid solution, and the concentration of surface lattice oxygen was increased.