Granular CuO-CeO2-MnOx/γ-Al2O3 catalysts were synthesized by the sol-gel method. The performance of the CuO-CeO2-MnOx/γ-Al2O3 catalysts for the selective catalytic reduction (SCR) was studied in a fixed bed system. ...Granular CuO-CeO2-MnOx/γ-Al2O3 catalysts were synthesized by the sol-gel method. The performance of the CuO-CeO2-MnOx/γ-Al2O3 catalysts for the selective catalytic reduction (SCR) was studied in a fixed bed system. Preliminary tests were carried out to analyze the behavior of NH3 and NO over catalyst in the presence of oxygen. The optimum temperature range for SCR over the CuO-CeO2-MnOx/γ-Al2O3 catalysts is 300-400 ℃ . The catalysts maintain nearly 100% NO conversion at 350 ℃. The NH3 oxidation experiments show that both NO and N2O are produced gradually with the increase of temperature. The catalysts in this experiment have a stronger oxidation property on NH3, which improves the denitrification activity at low temperature. The over-oxidation of NH3 at high temperature is the main cause leading to a decrease in the NO conversion. The NH3 and NO desorption experiments show that NH3 and NO can be adsorbed on CuO-CeO2-MnOx/γ-Al2O3 granular catalysts. The transient response of NH3 and NO indicates that the SCR reaction proceeds in accordance with the Eley-Rideal mechanism. The adsorbed NO has little influence on the denitrification activity in SCR process.展开更多
The selective catalytic reduction reaction belongs to the gas-solid multiphase reaction, and the adsorption of NH3 and NO on CuO/γ-Al2O3 catalysts plays an important role in the reaction. Performance of the CuO/γ-Al...The selective catalytic reduction reaction belongs to the gas-solid multiphase reaction, and the adsorption of NH3 and NO on CuO/γ-Al2O3 catalysts plays an important role in the reaction. Performance of the CuO/γ-Al2O3 catalysts was explored in a fixed bed adsorption system. The catalysts maintain nearly 100% NO conversion efficiency at 350℃. Comprehensive tests were carried out to study the adsorption behavior of NH3 and NO over the catalysts. The desorption experiments prove that NH3 and NO are adsorbed on CuO/γ-Al2O3 catalysts. The adsorption behaviors of NH3 and NO were also studied with the in-situ diffusion reflectance infrared Fourier transform spectroscopy methods. The results show that NH3 could be strongly adsorbed on the catalysts, resulting in coordinated NH3 and NH4＋. NO adsorption leads to the formation of bridging bidentate nitrate, chelating bidentate nitrate, and chelating nitro. The interaction of NH3 and NO molecules with the Cu2＋ present on the CAl2O3 （100） surface was investigated by using a periodic density functional theory. The results show that the adsorption of all the molecules on the Cu2＋ site is energetically favorable, whereas NO bound is stronger than that of NH3 with the adsorption site, and key information about the structural and energetic properties was also addressed.展开更多
基金Projects (50776037,50721005) supported by the National Natural Science Foundation of China
文摘Granular CuO-CeO2-MnOx/γ-Al2O3 catalysts were synthesized by the sol-gel method. The performance of the CuO-CeO2-MnOx/γ-Al2O3 catalysts for the selective catalytic reduction (SCR) was studied in a fixed bed system. Preliminary tests were carried out to analyze the behavior of NH3 and NO over catalyst in the presence of oxygen. The optimum temperature range for SCR over the CuO-CeO2-MnOx/γ-Al2O3 catalysts is 300-400 ℃ . The catalysts maintain nearly 100% NO conversion at 350 ℃. The NH3 oxidation experiments show that both NO and N2O are produced gradually with the increase of temperature. The catalysts in this experiment have a stronger oxidation property on NH3, which improves the denitrification activity at low temperature. The over-oxidation of NH3 at high temperature is the main cause leading to a decrease in the NO conversion. The NH3 and NO desorption experiments show that NH3 and NO can be adsorbed on CuO-CeO2-MnOx/γ-Al2O3 granular catalysts. The transient response of NH3 and NO indicates that the SCR reaction proceeds in accordance with the Eley-Rideal mechanism. The adsorbed NO has little influence on the denitrification activity in SCR process.
基金Projects(50806025, 51021065, 50976038) supported by the National Natural Science Foundation of ChinaProject(20100480893) supported by the China Postdoctoral Science FoundationProject(1001022B) supported by the Postdoctoral Research Fund of Jiangsu Province, China
文摘The selective catalytic reduction reaction belongs to the gas-solid multiphase reaction, and the adsorption of NH3 and NO on CuO/γ-Al2O3 catalysts plays an important role in the reaction. Performance of the CuO/γ-Al2O3 catalysts was explored in a fixed bed adsorption system. The catalysts maintain nearly 100% NO conversion efficiency at 350℃. Comprehensive tests were carried out to study the adsorption behavior of NH3 and NO over the catalysts. The desorption experiments prove that NH3 and NO are adsorbed on CuO/γ-Al2O3 catalysts. The adsorption behaviors of NH3 and NO were also studied with the in-situ diffusion reflectance infrared Fourier transform spectroscopy methods. The results show that NH3 could be strongly adsorbed on the catalysts, resulting in coordinated NH3 and NH4＋. NO adsorption leads to the formation of bridging bidentate nitrate, chelating bidentate nitrate, and chelating nitro. The interaction of NH3 and NO molecules with the Cu2＋ present on the CAl2O3 （100） surface was investigated by using a periodic density functional theory. The results show that the adsorption of all the molecules on the Cu2＋ site is energetically favorable, whereas NO bound is stronger than that of NH3 with the adsorption site, and key information about the structural and energetic properties was also addressed.
