The reaction kinetics of SO 2 oxidation on Cs Rb V series sulfuric acid catalyst promoted by alkali salts such as cesium and rubidium was studied. A three step reaction mechanism of SO 2 oxidation was proposed, in whi...The reaction kinetics of SO 2 oxidation on Cs Rb V series sulfuric acid catalyst promoted by alkali salts such as cesium and rubidium was studied. A three step reaction mechanism of SO 2 oxidation was proposed, in which it was assumed that oxidation of quadrivalent vanadium complex was a controlling step. Then, a mechanism model equation was concluded according to the three step reaction mechanism. The SO 2 oxidation rate was measured with a non gradient reactor under the conditions of temperature of 380~520?℃ and space velocity of 3?600~7?200?h -1 . Through calculating with Powell nonlinear regression method, the parameters of model equation were obtained: K 1=0.152?exp(-62?073/ (RT) ), K 2=8.18?exp(-2?384/ (RT) ), K 3=0.221?exp(-18?949/ (RT) ). It was found that the model equation could fit with all the experimental reaction rate data very well. [展开更多
The use of non-noble nickel-based catalysts for low temperature CO methanation has been a challenge in recent years.Herein,MgAl layered double oxides sample with high dispersion synthesized by a facile N-(2-Hydroxyeth...The use of non-noble nickel-based catalysts for low temperature CO methanation has been a challenge in recent years.Herein,MgAl layered double oxides sample with high dispersion synthesized by a facile N-(2-Hydroxyethyl)ethylenediaminetriacetic acid assisted wetness impregnation approach,demonstrates much superior catalytic activity and exceptional stability for CO methanation in comparison with the classical Ni/MgAl-LDO catalyst prepared by the ordinary wetness impregnation method.HRTEM results showed that N-(2-Hydroxyethyl)ethylenediaminetriacetic acid played a positive role in the dispersion of Ni,as well as Ni-support interaction.Well-dispersed Ni particles with a size of about 5 nm were formed in the presence of N-(2-Hydroxyethyl)ethylenediaminetriacetic acid.Compared to the Ni/MgAl-LDO prepared by conventional impregnation method,the NH-Ni/MgAl-LDO exhibited superior catalytic performance,especially excellent thermal stability.The NH-Ni30/MgAl-LDO catalyst was found to keep a 70%CO conversion even at 160◦C which demonstrates its good low temperature performance.From the in situ FTIR observations,this good performance at low temperatures may be linked to the delocalization of electrons around CO caused by surface hydroxyl groups.展开更多
Selective catalytic reduction technology using NH3 as a reducing agent(NH3-SCR) is an effective control method to remove nitrogen oxides. TiO2-supported vanadium oxide catalysts with different levels of Ce and Sb mo...Selective catalytic reduction technology using NH3 as a reducing agent(NH3-SCR) is an effective control method to remove nitrogen oxides. TiO2-supported vanadium oxide catalysts with different levels of Ce and Sb modification were prepared by an impregnation method and were characterized by X-ray diffractometer(XRD), Brunauer-Emmett-Teller(BET), Transmission electron microscopy(TEM), Fourier transform infrared spectroscopy(FT-IR), UV-Vis diffuse reflectance spectroscopy(UV-Vis DRS), Raman and Hydrogen temperature-programmed reduction(H2-TPR). The catalytic activities of V5 CexS by/TiO2 catalysts for denitration were investigated in a fixed bed flow microreactor. The results showed that cerium, vanadium and antimony oxide as the active components were well dispersed on TiO2, and the catalysts exhibited a large number of d-d electronic transitions, which were helpful to strengthen SCR reactivity. The V5 CexS by/TiO2 catalysts exhibited a good low temperature NH3-SCR catalytic activity. In the temperature range of 210 to 400℃, the V5 CexS by/TiO2 catalysts gave NO conversion rates above 90%. For the best V5Ce35Sb2/TiO2 catalyst, at a reaction temperature of 210℃, the NO conversion rate had already reached 90%. The catalysts had different catalytic activity with different Ce loadings. With the increase of Ce loading, the NO conversion rate also increased.展开更多
A homogeneous catalyst [Cp*Rh(NH3)(H2O)2]-(3+) has been found for the clean conversion of methanol and water to hydrogen and carbon dioxide. The simple and easily available reaction steps can circumvent the fo...A homogeneous catalyst [Cp*Rh(NH3)(H2O)2]-(3+) has been found for the clean conversion of methanol and water to hydrogen and carbon dioxide. The simple and easily available reaction steps can circumvent the formation of CO, therefore, making it possible to avoid inactivating catalysts and contaminating the hydrogen fuel. Different from conventional reforming method for hydrogen production, no additional alkaline or organic substances are required in this method. Valuable hydrogen can be obtained under ambient pressure at 70 C, corresponding TOF is 83.2 h 1. This is an unprecedented success in reforming methanol to hydrogen. Effects of reaction conditions, such as reaction temperature, initial methanol concentration and the initial p H value of buffer solution on the hydrogen evolution are all systematically investigated. In a certain range, higher reaction temperature will accelerate reaction rate. The slightly acidic condition is conducive to rapid hydrogen production. These findings are of great significance to the present establishment of the carbon-neutral methanol economy.展开更多
文摘The reaction kinetics of SO 2 oxidation on Cs Rb V series sulfuric acid catalyst promoted by alkali salts such as cesium and rubidium was studied. A three step reaction mechanism of SO 2 oxidation was proposed, in which it was assumed that oxidation of quadrivalent vanadium complex was a controlling step. Then, a mechanism model equation was concluded according to the three step reaction mechanism. The SO 2 oxidation rate was measured with a non gradient reactor under the conditions of temperature of 380~520?℃ and space velocity of 3?600~7?200?h -1 . Through calculating with Powell nonlinear regression method, the parameters of model equation were obtained: K 1=0.152?exp(-62?073/ (RT) ), K 2=8.18?exp(-2?384/ (RT) ), K 3=0.221?exp(-18?949/ (RT) ). It was found that the model equation could fit with all the experimental reaction rate data very well. [
基金National Natural Science Foundation of China(No.22068034)International Science and Technology Cooperation Project of Shihezi University(No.GJHZ201804)+1 种基金International Science and Technology Cooperation Project of Bingtuan(No.2018BC002)Science and Technology Innovation Talents Program of Bingtuan(No.2019CB025).
文摘The use of non-noble nickel-based catalysts for low temperature CO methanation has been a challenge in recent years.Herein,MgAl layered double oxides sample with high dispersion synthesized by a facile N-(2-Hydroxyethyl)ethylenediaminetriacetic acid assisted wetness impregnation approach,demonstrates much superior catalytic activity and exceptional stability for CO methanation in comparison with the classical Ni/MgAl-LDO catalyst prepared by the ordinary wetness impregnation method.HRTEM results showed that N-(2-Hydroxyethyl)ethylenediaminetriacetic acid played a positive role in the dispersion of Ni,as well as Ni-support interaction.Well-dispersed Ni particles with a size of about 5 nm were formed in the presence of N-(2-Hydroxyethyl)ethylenediaminetriacetic acid.Compared to the Ni/MgAl-LDO prepared by conventional impregnation method,the NH-Ni/MgAl-LDO exhibited superior catalytic performance,especially excellent thermal stability.The NH-Ni30/MgAl-LDO catalyst was found to keep a 70%CO conversion even at 160◦C which demonstrates its good low temperature performance.From the in situ FTIR observations,this good performance at low temperatures may be linked to the delocalization of electrons around CO caused by surface hydroxyl groups.
基金supported by the Natural Science Foundation of China (Nos. 21376261, 21173270)the Beijing Natural Science Foundation (2142027)+1 种基金Doctor select Foundation (No. 20130007110007)the National Hi-Tech Research and Development Program (863) of China (No. 2013AA065302)
文摘Selective catalytic reduction technology using NH3 as a reducing agent(NH3-SCR) is an effective control method to remove nitrogen oxides. TiO2-supported vanadium oxide catalysts with different levels of Ce and Sb modification were prepared by an impregnation method and were characterized by X-ray diffractometer(XRD), Brunauer-Emmett-Teller(BET), Transmission electron microscopy(TEM), Fourier transform infrared spectroscopy(FT-IR), UV-Vis diffuse reflectance spectroscopy(UV-Vis DRS), Raman and Hydrogen temperature-programmed reduction(H2-TPR). The catalytic activities of V5 CexS by/TiO2 catalysts for denitration were investigated in a fixed bed flow microreactor. The results showed that cerium, vanadium and antimony oxide as the active components were well dispersed on TiO2, and the catalysts exhibited a large number of d-d electronic transitions, which were helpful to strengthen SCR reactivity. The V5 CexS by/TiO2 catalysts exhibited a good low temperature NH3-SCR catalytic activity. In the temperature range of 210 to 400℃, the V5 CexS by/TiO2 catalysts gave NO conversion rates above 90%. For the best V5Ce35Sb2/TiO2 catalyst, at a reaction temperature of 210℃, the NO conversion rate had already reached 90%. The catalysts had different catalytic activity with different Ce loadings. With the increase of Ce loading, the NO conversion rate also increased.
基金financial support granted by Ministry of Science and Technology of the People's Republic of China(Nos.2016YFA0200700 and 2016YFE0105700)the National Natural Science Foundation of China(Nos.21373264 and 21573275)+2 种基金the Natural Science Foundation of Jiangsu Province(No.BK20150362)Suzhou Institute of Nano-tech and Nanobionics(No.Y3AAA11004)Thousand Youth Talents Plan(No.Y3BQA11001)
文摘A homogeneous catalyst [Cp*Rh(NH3)(H2O)2]-(3+) has been found for the clean conversion of methanol and water to hydrogen and carbon dioxide. The simple and easily available reaction steps can circumvent the formation of CO, therefore, making it possible to avoid inactivating catalysts and contaminating the hydrogen fuel. Different from conventional reforming method for hydrogen production, no additional alkaline or organic substances are required in this method. Valuable hydrogen can be obtained under ambient pressure at 70 C, corresponding TOF is 83.2 h 1. This is an unprecedented success in reforming methanol to hydrogen. Effects of reaction conditions, such as reaction temperature, initial methanol concentration and the initial p H value of buffer solution on the hydrogen evolution are all systematically investigated. In a certain range, higher reaction temperature will accelerate reaction rate. The slightly acidic condition is conducive to rapid hydrogen production. These findings are of great significance to the present establishment of the carbon-neutral methanol economy.