The CuO/γ-Al2O3/cordierite catalyst, after being sulfated by sulfur dioxide (SO2) at 673 K, exhibits high activities for selective catalytic reduction (SCR) of nitrogen oxide (NO) with ammonia (NH3) at 573-723 K. The...The CuO/γ-Al2O3/cordierite catalyst, after being sulfated by sulfur dioxide (SO2) at 673 K, exhibits high activities for selective catalytic reduction (SCR) of nitrogen oxide (NO) with ammonia (NH3) at 573-723 K. The intrinsic kinetics of SCR of NO with NH3 over CuO/γ-Al2O3/cordierite catalyst has been measured in a fixed-bed reactor in the absence of internal and external diffusions. The experimental results show that the reaction rate can be quantified by a first-order expression with activation energy Eá of 94.01 kJ·mol-1 and the corresponding p re-exponential factor A′ of 3.39×108 cm3·g-1·s-1 when NH3 is excessive. However, when NH3 is not enough, an E ley-Rideal kinetic model based on experimental data is derived with Ea of 105.79 kJ·mol-1, the corresponding A of 2 .94×109 cm3·g-1·s-1, heat of adsorption-Hads of 87.90 kJ·mol-1 and the corresponding Aads of 9.24 cm3·mol-1. The intrinsic kinetic model obtained was incorporated in a 3D mathematical model of monolithic reactor, and the agreement of the prediction with experimental data indicates that the present kinetic model is adequate for the reac-tor design and engineering scale-up.展开更多
An industrial scale propylene production via oxidative dehydrogenation of propane （ODHP） in multi-tubular re- actors was modeled. Multi-tubular fixed-bed reactor used for ODHP process, employing 10000 of small diame...An industrial scale propylene production via oxidative dehydrogenation of propane （ODHP） in multi-tubular re- actors was modeled. Multi-tubular fixed-bed reactor used for ODHP process, employing 10000 of small diameter tubes immersed in a shell through a proper coolant flows. Herein, a theory-based pseudo-homogeneous model to describe the operation of a fixed bed reactor for the ODHP to correspondence olefln over V2O5/γ-Al203 catalyst was presented. Steady state one dimensional model has been developed to identify the operation parameters and to describe the propane and oxygen conversions, gas process and coolant temperatures, as well as other pa- rameters affecting the reactor performance such as pressure. Furthermore, the applied model showed that a double-bed multitubular reactor with intermediate air injection scheme was superior to a single-bed design due to the increasing of propylene selectivity while operating under lower oxygen partial pressures resulting in propane conversion of about 37.3%. The optimized length of the reactor needed to reach 100% conversion of the oxygen was theoretically determined. For the single-bed reactor the optimized length of 11.96 m including 0.5 m of inert section at the entrance region and for the double-bed reactor design the optimized lengths of 5.72 m for the first and 7.32 m for the second reactor were calculated. Ultimately, the use of a distributed oxygen feed with limited number of injection points indicated a significant improvement on the reactor performance in terms of propane conversion and propylene selectivity. Besides, this concept could overcome the reactor run- away temperature problem and enabled operations at the wider range of conditions to obtain enhanced propyl- ene production in an industrial scale reactor.展开更多
An extensive study of Fischer-Tropsch synthesis on nanostructure supports with high surface area such as nanostructure -y-alumina, single wall carbon nanotubes （SWNTs）, and the hybrid of SWNTs/nanostructure -y-alumi...An extensive study of Fischer-Tropsch synthesis on nanostructure supports with high surface area such as nanostructure -y-alumina, single wall carbon nanotubes （SWNTs）, and the hybrid of SWNTs/nanostructure -y-alumina has been investigated. The nanostructure γ-alumina was promoted with lanthanum to obtain better performance of catalyst and 15 wt% cobalt loading was the basis of our investigation. Fischer- Tropsch synthesis was performed in a fixed bed reactor under different reaction conditions （220-240 ℃, 15-25 bar, H2/CO ratio of 2, GHSV of 900-1400） in order to study the effects of temperature, pressure and gas hourly space velocity （GHSV） changes on hydrocarbon selec- tivity and catalyst activity. The catalysts were extensively characterized by different methods including X-ray diffraction （XRD）, scanning electron microscopy （SEM）, transmission electron microscopy （TEM）, inductively coupled plasma （ICP）, hydrogen （H2） chemisorption and temperature-programmed reduction （TPR）. The results showed that the yield of hybrid supported catalyst （55.4%） is higher than that of nanos- tructure -y-alumina supported catalyst （55.0%） and lower than that of SWNTs supported cobalt catalyst （71.0%）. The hybrid supported catalyst showed higher reduction degree and dispersion of cobalt particles. The temperature, pressure and GHSV effects on hybrid supported catalyst were studied and results showed that higher pressure favors the chain growth and temperature increase leads to the increases in methane selec- tivity and CO conversion. Higher hydrocarbon selectivity and CO conversion showed positive relationship with increasing GHSV while lower hydrocarbon selectivity diminishes.展开更多
基金Supported by the National Natural Science Foundation of China （20821004 20736001 21076008） the Research Fund for the Doctoral Program of Higher Education of China （2090010110002）
文摘The CuO/γ-Al2O3/cordierite catalyst, after being sulfated by sulfur dioxide (SO2) at 673 K, exhibits high activities for selective catalytic reduction (SCR) of nitrogen oxide (NO) with ammonia (NH3) at 573-723 K. The intrinsic kinetics of SCR of NO with NH3 over CuO/γ-Al2O3/cordierite catalyst has been measured in a fixed-bed reactor in the absence of internal and external diffusions. The experimental results show that the reaction rate can be quantified by a first-order expression with activation energy Eá of 94.01 kJ·mol-1 and the corresponding p re-exponential factor A′ of 3.39×108 cm3·g-1·s-1 when NH3 is excessive. However, when NH3 is not enough, an E ley-Rideal kinetic model based on experimental data is derived with Ea of 105.79 kJ·mol-1, the corresponding A of 2 .94×109 cm3·g-1·s-1, heat of adsorption-Hads of 87.90 kJ·mol-1 and the corresponding Aads of 9.24 cm3·mol-1. The intrinsic kinetic model obtained was incorporated in a 3D mathematical model of monolithic reactor, and the agreement of the prediction with experimental data indicates that the present kinetic model is adequate for the reac-tor design and engineering scale-up.
文摘An industrial scale propylene production via oxidative dehydrogenation of propane （ODHP） in multi-tubular re- actors was modeled. Multi-tubular fixed-bed reactor used for ODHP process, employing 10000 of small diameter tubes immersed in a shell through a proper coolant flows. Herein, a theory-based pseudo-homogeneous model to describe the operation of a fixed bed reactor for the ODHP to correspondence olefln over V2O5/γ-Al203 catalyst was presented. Steady state one dimensional model has been developed to identify the operation parameters and to describe the propane and oxygen conversions, gas process and coolant temperatures, as well as other pa- rameters affecting the reactor performance such as pressure. Furthermore, the applied model showed that a double-bed multitubular reactor with intermediate air injection scheme was superior to a single-bed design due to the increasing of propylene selectivity while operating under lower oxygen partial pressures resulting in propane conversion of about 37.3%. The optimized length of the reactor needed to reach 100% conversion of the oxygen was theoretically determined. For the single-bed reactor the optimized length of 11.96 m including 0.5 m of inert section at the entrance region and for the double-bed reactor design the optimized lengths of 5.72 m for the first and 7.32 m for the second reactor were calculated. Ultimately, the use of a distributed oxygen feed with limited number of injection points indicated a significant improvement on the reactor performance in terms of propane conversion and propylene selectivity. Besides, this concept could overcome the reactor run- away temperature problem and enabled operations at the wider range of conditions to obtain enhanced propyl- ene production in an industrial scale reactor.
基金supported by the Iran National Science Foundation (INSF) under the contract number 87040961the Iranian Nano Technology Initiative Council
文摘An extensive study of Fischer-Tropsch synthesis on nanostructure supports with high surface area such as nanostructure -y-alumina, single wall carbon nanotubes （SWNTs）, and the hybrid of SWNTs/nanostructure -y-alumina has been investigated. The nanostructure γ-alumina was promoted with lanthanum to obtain better performance of catalyst and 15 wt% cobalt loading was the basis of our investigation. Fischer- Tropsch synthesis was performed in a fixed bed reactor under different reaction conditions （220-240 ℃, 15-25 bar, H2/CO ratio of 2, GHSV of 900-1400） in order to study the effects of temperature, pressure and gas hourly space velocity （GHSV） changes on hydrocarbon selec- tivity and catalyst activity. The catalysts were extensively characterized by different methods including X-ray diffraction （XRD）, scanning electron microscopy （SEM）, transmission electron microscopy （TEM）, inductively coupled plasma （ICP）, hydrogen （H2） chemisorption and temperature-programmed reduction （TPR）. The results showed that the yield of hybrid supported catalyst （55.4%） is higher than that of nanos- tructure -y-alumina supported catalyst （55.0%） and lower than that of SWNTs supported cobalt catalyst （71.0%）. The hybrid supported catalyst showed higher reduction degree and dispersion of cobalt particles. The temperature, pressure and GHSV effects on hybrid supported catalyst were studied and results showed that higher pressure favors the chain growth and temperature increase leads to the increases in methane selec- tivity and CO conversion. Higher hydrocarbon selectivity and CO conversion showed positive relationship with increasing GHSV while lower hydrocarbon selectivity diminishes.
