A series of H3PO4-modified CeO2 samples were prepared by impregnation of CeO2 with H3PO4solution,and evaluated for the selective catalytic reduction of NOx by NH3.The samples were characterized by X-ray diffraction,N2...A series of H3PO4-modified CeO2 samples were prepared by impregnation of CeO2 with H3PO4solution,and evaluated for the selective catalytic reduction of NOx by NH3.The samples were characterized by X-ray diffraction,N2 adsorption-desorption,infrared spectroscopy,Raman spectroscopy,X-ray photoelectron spectroscopy,temperature-programmed desorption of NH3,and temperature-programmed reduction of H2.The results showed that more than 80%NO conversion was achieved in the temperature range 250-550℃ over the H3PO4-CeO2 catalyst.The enhanced catalytic performance could be ascribed to the increase in acidic strength,especially Bronsted acidity,and reduction in redox properties of the CeO2 after H3PO4 modification.展开更多
This work tries to identify the relationship between geometric configuration of monolith catalysts, and transfer and reaction performances for selective catalytic reduction of N2O with CO. Monolith catalysts with five...This work tries to identify the relationship between geometric configuration of monolith catalysts, and transfer and reaction performances for selective catalytic reduction of N2O with CO. Monolith catalysts with five different channel shapes (circle, regular triangle, rectangle, square and hexagon), was investigated to make a comprehensive comparison of their pressure drop, heat transfer Nu number, mass transfer Sh number and N2O conversion. It was found that monolith catalysts have a much lower pressure drop than that of traditional packed bed, and for monolith catalysts with different channel shapes, pressure drop decreases in the order of regular triangle > rectangle > square > hexagon > circle. The order of Nu is in regular triangle > rectangle ≈ square > hexagon > circle, similar to that of Sh. N2O conversion follows the order of regular triangle > rectangular ≈ square ≈ circle > hexagon. The results indicate that chemical reaction including internal diffusion is the controlling step in the selective catalytic reduction of N2O removal with CO. In addition, channel size and gas velocity also have influence on N2O conversion and pressure drop.展开更多
Diesel emission fluid （DEF） soaking and urea deposits on selective catalytic reduction （SCR） catalysts are critical issues for real diesel engine NH3-SCR systems. To investigate the impact of DEF soaking and urea ...Diesel emission fluid （DEF） soaking and urea deposits on selective catalytic reduction （SCR） catalysts are critical issues for real diesel engine NH3-SCR systems. To investigate the impact of DEF soaking and urea deposits on SCR catalyst performance, fresh Cu-zeolite catalyst samples were drilled from a full-size SCR catalyst. Those samples were impregnated with DEF solutions and subsequently hydrothermally treated to simulate DEF soaking and urea deposits on real SCR catalysts during diesel engine operations. Their SCR performance was then evaluated in a flow reactor with a four-step test protocol. Test results show that the DEF soaking leached some Cu from the SCR catalysts and slightly reduced their Cu loadings. The loss of Cu and associated metal sites on the catalysts weakened their catalytic oxidation abilities and caused lower NO/NI-I3 oxidation and lower high-temperature N20 selectivity. Lower Cu loading also made the catalysts less active to the decomposition of surface ammonium nitrates and decreased low-temperature N20 selectivity. Cu loss during DEF impregnation released more acid sites on the surface of the catalysts and increased their acidities, and more NH3 was able to be adsorbed and involved in SCR reactions at medium and high temperatures. Due to lower NH3 oxidation and higher NH3 storage, the DEF-impregnated SCR catalyst samples showed higher NOx conversion above 400 ℃ compared with the non-soaked one. The negative impact of urea deposits during DEF impregnation was not clearly observed, because the high-temperature hydrothermal treatment helped to remove the urea deposits.展开更多
基金supported by the National Natural Science Foundation of China(21177120)the Open Fund of Key Laboratory of Functional Inorganic Material Chemistry(Heilongjiang University),Ministry of Education~~
文摘A series of H3PO4-modified CeO2 samples were prepared by impregnation of CeO2 with H3PO4solution,and evaluated for the selective catalytic reduction of NOx by NH3.The samples were characterized by X-ray diffraction,N2 adsorption-desorption,infrared spectroscopy,Raman spectroscopy,X-ray photoelectron spectroscopy,temperature-programmed desorption of NH3,and temperature-programmed reduction of H2.The results showed that more than 80%NO conversion was achieved in the temperature range 250-550℃ over the H3PO4-CeO2 catalyst.The enhanced catalytic performance could be ascribed to the increase in acidic strength,especially Bronsted acidity,and reduction in redox properties of the CeO2 after H3PO4 modification.
基金Supported by the National Natural Science Foundation of China （21121064, 21076008） the Projects in the National Science ＆ Technology Pillar Program During the 12th Five-Year Plan Period （2011BAC06B04）
文摘This work tries to identify the relationship between geometric configuration of monolith catalysts, and transfer and reaction performances for selective catalytic reduction of N2O with CO. Monolith catalysts with five different channel shapes (circle, regular triangle, rectangle, square and hexagon), was investigated to make a comprehensive comparison of their pressure drop, heat transfer Nu number, mass transfer Sh number and N2O conversion. It was found that monolith catalysts have a much lower pressure drop than that of traditional packed bed, and for monolith catalysts with different channel shapes, pressure drop decreases in the order of regular triangle > rectangle > square > hexagon > circle. The order of Nu is in regular triangle > rectangle ≈ square > hexagon > circle, similar to that of Sh. N2O conversion follows the order of regular triangle > rectangular ≈ square ≈ circle > hexagon. The results indicate that chemical reaction including internal diffusion is the controlling step in the selective catalytic reduction of N2O removal with CO. In addition, channel size and gas velocity also have influence on N2O conversion and pressure drop.
基金Project supported by the National High-Tech R&D Program(863 Program)of China(No.2013AA065301)the Fundamental Research Funds for the Central Universities,and the State Key Laboratory of Clean Energy Utilization at Zhejiang University(No.ZJUCEU2016006),China
文摘Diesel emission fluid （DEF） soaking and urea deposits on selective catalytic reduction （SCR） catalysts are critical issues for real diesel engine NH3-SCR systems. To investigate the impact of DEF soaking and urea deposits on SCR catalyst performance, fresh Cu-zeolite catalyst samples were drilled from a full-size SCR catalyst. Those samples were impregnated with DEF solutions and subsequently hydrothermally treated to simulate DEF soaking and urea deposits on real SCR catalysts during diesel engine operations. Their SCR performance was then evaluated in a flow reactor with a four-step test protocol. Test results show that the DEF soaking leached some Cu from the SCR catalysts and slightly reduced their Cu loadings. The loss of Cu and associated metal sites on the catalysts weakened their catalytic oxidation abilities and caused lower NO/NI-I3 oxidation and lower high-temperature N20 selectivity. Lower Cu loading also made the catalysts less active to the decomposition of surface ammonium nitrates and decreased low-temperature N20 selectivity. Cu loss during DEF impregnation released more acid sites on the surface of the catalysts and increased their acidities, and more NH3 was able to be adsorbed and involved in SCR reactions at medium and high temperatures. Due to lower NH3 oxidation and higher NH3 storage, the DEF-impregnated SCR catalyst samples showed higher NOx conversion above 400 ℃ compared with the non-soaked one. The negative impact of urea deposits during DEF impregnation was not clearly observed, because the high-temperature hydrothermal treatment helped to remove the urea deposits.
