The catalytic hydrogenation of 2-nitro-4-acetylamino anisole(NMA)is a less-polluting and efficient method to produce 2-amino-4-acetamino anisole(AMA).However,the kinetics of catalytic hydrogenation of NMA to AMA remai...The catalytic hydrogenation of 2-nitro-4-acetylamino anisole(NMA)is a less-polluting and efficient method to produce 2-amino-4-acetamino anisole(AMA).However,the kinetics of catalytic hydrogenation of NMA to AMA remains obscure.In this work,the kinetic models including power-law model and Langmuir-Hinshelwood-Hougen-Watson(LHHW)model of NMA hydrogenation to AMA catalyzed by Raney nickel catalyst were investigated.All experiments were carried out under the elimination of mass transfer resistance within the temperature range of 70–100°C and the hydrogen pressure of 0.8–1.5 MPa.The reaction was found to follow 0.52-order kinetics with respect to the NMA concentration and 1.10-order kinetics in terms of hydrogen pressure.Based on the LHHW model,the dual-site dissociation adsorption of hydrogen was analyzed to be the rate determining step.The research of intrinsic kinetics of NMA to AMA provides the guidance for the reactor design and inspires the catalyst modification.展开更多
The intrinsic kinetics of oxidative dehydrogenation of propane with CO2 has been investigated over Cr/MSU-1 catalyst in a fixed bed reactor. Without limitations of both internal and external diffusion, intrinsic kinet...The intrinsic kinetics of oxidative dehydrogenation of propane with CO2 has been investigated over Cr/MSU-1 catalyst in a fixed bed reactor. Without limitations of both internal and external diffusion, intrinsic kinetic data were obtained under the following conditions: 490-530 °C, space velocity of 3600?6000 mL·h-1·g-1 and 3/1 molar ratio for CO2/C3H8 under normal pressure. Based on Langmuir-Hinshelwood mechanism, the kinetic models were established, and they were validated by statistical analysis. The parameters were estimated using Simplex Method combined with Universal Global Optimization Algorithm. The model, taking the surface reaction process as the rate-determining step, is the best one in agreement with the experimental data.展开更多
The intrinsic reaction kinetics of methane aromatization under non-oxidative conditions over modified Mo/HZSM-5 catalysts was studied in the quartz pipe-reactor under ordinary pressure with the temperature ranging fro...The intrinsic reaction kinetics of methane aromatization under non-oxidative conditions over modified Mo/HZSM-5 catalysts was studied in the quartz pipe-reactor under ordinary pressure with the temperature ranging from 913.15 to 973.15 K and the space velocity from 700 to 2100 ml/(g·h). The Langmuir-Hinshelwood model was chosen to describe the intrinsic kinetics while Levenberg-Marquardt method was selected to determine the parameters in the kinetic model. Statistical test and residual error distribution diagrams showed that experimental data were in good agreement with calculated data, and Langmuir-Hinshelwood model was suitable for the description of the intrinsic kinetics of methane aromatization under the reaction conditions discussed in this article.展开更多
The catalysis technology of propylene dimerization to form 4-methyl-1-pentene(4MP1)using a Cu-K/K_(2)CO_(3) solid base catalyst is a well-known heterogeneous catalytic reaction.In this study,the intrinsic kinetics of ...The catalysis technology of propylene dimerization to form 4-methyl-1-pentene(4MP1)using a Cu-K/K_(2)CO_(3) solid base catalyst is a well-known heterogeneous catalytic reaction.In this study,the intrinsic kinetics of propylene dimerization were studied in a fixed-bed continuous reactor.Internal and external diffusion during the dimerization reaction experiments were eliminated by adjusting the flow rate of the carrier gas and the particle size of the catalyst support.Then,the concentration changes of each substance at the outlet of the catalyst bed under different residence times were investigated.Moreover,the suitable reaction kinetics equations was derived using the Langmuir Hinshelwood-Hougen-Watson kinetic model.Finally,the activation energy for each reaction involved in the dimerization reaction was calculated.The activation energies of 4MP1,branched by-products,and 1-hexene were 115.0,150.8,and 177.4 kJ/mol,respectively.The effect of process conditions on propylene dimerization with solid base catalysts was studied through kinetic model simulation.By comparing the theoretical values obtained from the simulation with the experimental results,the applicability and accuracy of the kinetic model were verified.展开更多
The sulfation of CeO2/γ-Al2O3 sorbent in simulated flue gas was studied. A series of CeO2/γ-Al2O3 sorbents with different CeO2 loadings were prepared by impregnation and characterized by X-ray diffraction. Thermogra...The sulfation of CeO2/γ-Al2O3 sorbent in simulated flue gas was studied. A series of CeO2/γ-Al2O3 sorbents with different CeO2 loadings were prepared by impregnation and characterized by X-ray diffraction. Thermogravimetric technique was used to study the sulfation of CeO2/γ-Al2O3 sorbents, mainly on the CeO2 loading, sulfation cycles, and intrinsic kinetics. The study revealed that monolayer coverage of CeO2 supported on γ-Al2O3 was 0. 125 g CeO2/g (γ-Al2O3). Below monolayer coverage, CeO2 was highly dispersed on γ-Al2O3. The optimal CeO2 loading on sulfation was 0.03 g CeO2/g (γ-Al2O3). CeO2/γ-Al2O3 sorbent was recyclable by controlling sulfation time. Intrinsic kineticd equation was R = 1. 1394×10^-4×exp ( - 1,508.39/T) mg·mg^-1·s^-1 Activation energy and reaction order were 12.54 kJ·mol^-1 and first order, respectively.展开更多
基金the National Natural Science Foun-dation of China(22022802 and 22288102).
文摘The catalytic hydrogenation of 2-nitro-4-acetylamino anisole(NMA)is a less-polluting and efficient method to produce 2-amino-4-acetamino anisole(AMA).However,the kinetics of catalytic hydrogenation of NMA to AMA remains obscure.In this work,the kinetic models including power-law model and Langmuir-Hinshelwood-Hougen-Watson(LHHW)model of NMA hydrogenation to AMA catalyzed by Raney nickel catalyst were investigated.All experiments were carried out under the elimination of mass transfer resistance within the temperature range of 70–100°C and the hydrogen pressure of 0.8–1.5 MPa.The reaction was found to follow 0.52-order kinetics with respect to the NMA concentration and 1.10-order kinetics in terms of hydrogen pressure.Based on the LHHW model,the dual-site dissociation adsorption of hydrogen was analyzed to be the rate determining step.The research of intrinsic kinetics of NMA to AMA provides the guidance for the reactor design and inspires the catalyst modification.
基金supported by the National Natural Science Foundation of China (No. 21006109)the Postdoctoral Science Foundation of China (No. 20080430581)the CASKC Wang Post-Doctoral Fellowship
文摘The intrinsic kinetics of oxidative dehydrogenation of propane with CO2 has been investigated over Cr/MSU-1 catalyst in a fixed bed reactor. Without limitations of both internal and external diffusion, intrinsic kinetic data were obtained under the following conditions: 490-530 °C, space velocity of 3600?6000 mL·h-1·g-1 and 3/1 molar ratio for CO2/C3H8 under normal pressure. Based on Langmuir-Hinshelwood mechanism, the kinetic models were established, and they were validated by statistical analysis. The parameters were estimated using Simplex Method combined with Universal Global Optimization Algorithm. The model, taking the surface reaction process as the rate-determining step, is the best one in agreement with the experimental data.
文摘The intrinsic reaction kinetics of methane aromatization under non-oxidative conditions over modified Mo/HZSM-5 catalysts was studied in the quartz pipe-reactor under ordinary pressure with the temperature ranging from 913.15 to 973.15 K and the space velocity from 700 to 2100 ml/(g·h). The Langmuir-Hinshelwood model was chosen to describe the intrinsic kinetics while Levenberg-Marquardt method was selected to determine the parameters in the kinetic model. Statistical test and residual error distribution diagrams showed that experimental data were in good agreement with calculated data, and Langmuir-Hinshelwood model was suitable for the description of the intrinsic kinetics of methane aromatization under the reaction conditions discussed in this article.
基金supported by the National Natural Science Foundation of China under agreement number 22378026the Project of Construction of Innovative Teams and Teacher Career Development for Universities and Colleges under Beijing Municipality(IDHT20180508).
文摘The catalysis technology of propylene dimerization to form 4-methyl-1-pentene(4MP1)using a Cu-K/K_(2)CO_(3) solid base catalyst is a well-known heterogeneous catalytic reaction.In this study,the intrinsic kinetics of propylene dimerization were studied in a fixed-bed continuous reactor.Internal and external diffusion during the dimerization reaction experiments were eliminated by adjusting the flow rate of the carrier gas and the particle size of the catalyst support.Then,the concentration changes of each substance at the outlet of the catalyst bed under different residence times were investigated.Moreover,the suitable reaction kinetics equations was derived using the Langmuir Hinshelwood-Hougen-Watson kinetic model.Finally,the activation energy for each reaction involved in the dimerization reaction was calculated.The activation energies of 4MP1,branched by-products,and 1-hexene were 115.0,150.8,and 177.4 kJ/mol,respectively.The effect of process conditions on propylene dimerization with solid base catalysts was studied through kinetic model simulation.By comparing the theoretical values obtained from the simulation with the experimental results,the applicability and accuracy of the kinetic model were verified.
基金Project supported bythe National Natural Science Foundation of China (90210003) Natural Science Foundation of Bei-jing City (2012010)
文摘The sulfation of CeO2/γ-Al2O3 sorbent in simulated flue gas was studied. A series of CeO2/γ-Al2O3 sorbents with different CeO2 loadings were prepared by impregnation and characterized by X-ray diffraction. Thermogravimetric technique was used to study the sulfation of CeO2/γ-Al2O3 sorbents, mainly on the CeO2 loading, sulfation cycles, and intrinsic kinetics. The study revealed that monolayer coverage of CeO2 supported on γ-Al2O3 was 0. 125 g CeO2/g (γ-Al2O3). Below monolayer coverage, CeO2 was highly dispersed on γ-Al2O3. The optimal CeO2 loading on sulfation was 0.03 g CeO2/g (γ-Al2O3). CeO2/γ-Al2O3 sorbent was recyclable by controlling sulfation time. Intrinsic kineticd equation was R = 1. 1394×10^-4×exp ( - 1,508.39/T) mg·mg^-1·s^-1 Activation energy and reaction order were 12.54 kJ·mol^-1 and first order, respectively.