A novel multi-tube photoreactor with 0.0188m3 valid reaction volume was constructed in pilot-scale. This rectangular reactor consisted of 13 regularly distributed silica glass tubes coating with TiO2 thin film photo-c...A novel multi-tube photoreactor with 0.0188m3 valid reaction volume was constructed in pilot-scale. This rectangular reactor consisted of 13 regularly distributed silica glass tubes coating with TiO2 thin film photo-catalyst. Total active area of TiO2 thin film is 0.3916m2. The ratio of surface area to volume achieves 20.8m-1. Photocatalytic experiment of phenol red demonstrates that the apparent reaction rate constant (k) is 0.074 65 h-1 and 0.16502h-1 for reaction system with and without micro-bubbles mixing. The corresponding apparent quantum efficiency (a) is 8.1771 X 10-7g.J-1 and 4.9036 x 10-7g-J-1, respectively. COD value of reactant could decrease to 17mg.L-1 and high performance liquid chromatography (HPLC) only shows two absorption peaks in 24 h pho-tocatalytic process time, so this photoreactor has good photomineralization effect. Experimental results reveal that photocatalytic destruction of organics is possible by using the multi-tube photoreactor.展开更多
Liquid phase oxidation of toluene is an environmental benign route for the production of benzoic acid.In a φ48mm bubble column reactor,the commercial process of toluene liquid phase oxidation was conducted with Co(CH...Liquid phase oxidation of toluene is an environmental benign route for the production of benzoic acid.In a φ48mm bubble column reactor,the commercial process of toluene liquid phase oxidation was conducted with Co(CH3COO)2.4H2O as catalyst.The Co2+ concentration [Co2+] was determined by extraction spectrophotometry and hereby the Co3+ concentration [Co3+] was obtained by mass balance.The results showed that [Co3+] reached the maximum at about 25-30min.[Co3+] increased with increasing Co catalyst amount at total Co concentration<150 mg.L-1 of toluene.The conversion of toluene,yield and selectivity of benzoic acid increased with the increasing [Co3+/Co2+] max.A high [Co3+] and a high [Co3+]/[Co2+] ratio are beneficial to the reaction.展开更多
Using catalytic oxidative absorption for H_2S removal is of great interest due to its distinct advantages. However,traditional scrubbing process faces a great limitation in the confined space. Therefore, there is an u...Using catalytic oxidative absorption for H_2S removal is of great interest due to its distinct advantages. However,traditional scrubbing process faces a great limitation in the confined space. Therefore, there is an urgent demand to develop high-efficiency process intensification technology for such a system. In this article, H_2S absorption experimental research was conducted in a rotating packed bed(RPB) reactor with ferric chelate absorbent and a mixture of N_2 and H_2S, which was used to simulate natural gas. The effects of absorbent p H value, gas–liquid ratio, gravity level of RPB, absorption temperature and character of the packing on the desulfurization efficiency were investigated. The results showed that H_2S removal efficiency could reach above 99.6% under the most of the experimental condition and above 99.9% under the optimal condition. A long-time continuous experiment was conducted to investigate the stability of the whole process combining absorption and regeneration. The result showed that the process could well realize simultaneous desulfurization and absorbent regeneration, and the H_2S removal efficiency kept relatively stable in the whole duration of 72 h. It can be clearly seen that high gravity technology desulfurization process, which is simple, high-efficiency, and space intensive, has a good prospect for industrial application of H_2S removal in confined space.展开更多
The performance characteristics of isothermal fluidized bed syngas methanation for substitute natural gas are investigated over a self-made Ni–Mg/Al2O3 catalyst. Via atmospheric methanation in a laboratory fluidized ...The performance characteristics of isothermal fluidized bed syngas methanation for substitute natural gas are investigated over a self-made Ni–Mg/Al2O3 catalyst. Via atmospheric methanation in a laboratory fluidized bed reactor it was clarified that the CO conversion varied in 5% when changing the space velocity in 40–120 L·g-1·h-1but the conversion increased obviously by raising the superficial gas velocity from 4 to12.4 cm·s-1. The temperature at 823 K is suitable for syngas methanation while obvious deposition of uneasyoxidizing Cγoccurs on the catalyst at temperatures around 873 K. From a kinetic aspect, the lowest reaction temperature is suggested to be 750 K when the space velocity is 60 L·g-1·h-1. Raising the H2/CO ratio of the syngas increased proportionally the CO conversion and CH4 selectivity, showing that at enough high H2/CO ratios the active sites on the catalyst are sufficient for CO adsorption and in turn the reaction with H2 for forming CH4.Introducing CO2 into the syngas feed suppresses the water gas shift and Boudouard reactions and thus increased H2 consumption. The ratio of CO2/CO in syngas should be better below 0.52 because varying the ratio from 0.52 to0.92 resulted in negligible increases in the H2 conversion and CH4 selectivity but decreased the CH4 yield.Introducing steam into the feed gas affected little the CO conversion but decreased the selectivity to CH4. The tested Ni–Mg/Al2O3 catalyst manifested good stability in structure and activity even in syngas containing water vapor.展开更多
A functional electrocatalytic membrane reactor(ECMR) was performed for the electrocatalytic oxidation of2,2,3,3-tetrafluoro-l-propanol(TFP) into high value-added sodium 2,2,3,3-tetrafluoropropionate(STFP),A computatio...A functional electrocatalytic membrane reactor(ECMR) was performed for the electrocatalytic oxidation of2,2,3,3-tetrafluoro-l-propanol(TFP) into high value-added sodium 2,2,3,3-tetrafluoropropionate(STFP),A computational fluid dynamics(CFD) technique was applied to simulate the hydrodynamic distributions along a tubular ECMR so as to provide guidance for the design and optimization of ECMR Two-dimensional simulation with porous media model was employed to predict the properties of fluid dynamics in ECMR.The experimental investigation was carried to confirm the CFD simulation.Results showed that a uniform distribution of permeate velocity along the tubular reactor with short length and large diameter could be obtained.TFP conversion of97.7%,the selectivity to STFP of 99.9%and current efficiency of 40.1%were achieved from the ECMR with a length of 40 mm and an inside diameter of 53 mm.The simulations were in good agreement with the experimental results.展开更多
Hydrogen production by partial oxidation steam reforming of methanol over a Cu/ZnO/Al2 O3 catalyst has been paid more and more attention. The chemical equilibria involved in the methanol partial oxidation steam reform...Hydrogen production by partial oxidation steam reforming of methanol over a Cu/ZnO/Al2 O3 catalyst has been paid more and more attention. The chemical equilibria involved in the methanol partial oxidation steam reforming reaction network such as methanol partial oxidation, methanol steam reforming, decomposition of methanol and water-gas shift reaction have been examined over the ranges of temperature 473-1073 K under normal pressure. Based on the detailed kinetics of these reactions over a Cu/ZnO/Al2O3 catalyst, and from the basic concept of the effectiveness factor, the intraparticle diffusion limitations were taken into account. The effectiveness factors for each reaction along the bed length were calculated. Then important results were offered for the simulation of this reaction process.展开更多
By taking the surface chemical reactions as the rate-controlling step, a possible reaction mechanism for ethylene epoxidation to synthesize ethylene oxide over the A-type silver catalyst was developed, while it was as...By taking the surface chemical reactions as the rate-controlling step, a possible reaction mechanism for ethylene epoxidation to synthesize ethylene oxide over the A-type silver catalyst was developed, while it was assumed that the epoxidation reaction would take place between ethylene and the un-dissociated adsorbed oxygen O2 a on the solo active sites, while the deep oxidation would occur between ethylene and the dissociated adsorbed oxygen Oa on the adjacent multi-active sites. In order to describe the effect of 1,2-C2H4Cl2(EDC) inhibitor on the ethylene epoxidation process, the reversible reactions between EDC and vinyl chloride(VC) on the active sites of silver catalyst was introduced. According to the assumed mechanism, the hyperbolic macro-kinetic model of ethylene epoxidation over the A-type silver catalyst was established, and the macrokinetic experiments were carried out in an internal-recycle gradientless reactor operating at a pressure of 2.1 MPa and a temperature in the range of 217.8—249.0 ℃, with the gas composition(molar fraction) consisting of 15.82%—34.65% C2H4, 2.55%—7.80% O2, 0.88%—6.15% CO2, 0.15—2.61 μmol/mol of 1,2-C2H4Cl2 and 0.14—1.28 μmol/mol of C2H3 Cl. By means of the Simplex Optimal Method, the parameters of the macrokinetic models were estimated. Statistical test showed that the macrokinetic models developed for the A-type silver catalyst agree well with the experimental results.展开更多
基金Supported by the Natural Science Foundation of Jiangsu Province (JH01-010).
文摘A novel multi-tube photoreactor with 0.0188m3 valid reaction volume was constructed in pilot-scale. This rectangular reactor consisted of 13 regularly distributed silica glass tubes coating with TiO2 thin film photo-catalyst. Total active area of TiO2 thin film is 0.3916m2. The ratio of surface area to volume achieves 20.8m-1. Photocatalytic experiment of phenol red demonstrates that the apparent reaction rate constant (k) is 0.074 65 h-1 and 0.16502h-1 for reaction system with and without micro-bubbles mixing. The corresponding apparent quantum efficiency (a) is 8.1771 X 10-7g.J-1 and 4.9036 x 10-7g-J-1, respectively. COD value of reactant could decrease to 17mg.L-1 and high performance liquid chromatography (HPLC) only shows two absorption peaks in 24 h pho-tocatalytic process time, so this photoreactor has good photomineralization effect. Experimental results reveal that photocatalytic destruction of organics is possible by using the multi-tube photoreactor.
基金Supported by the National Natural Science Foundation of China （20576081, 20736009） and the Ph.D. Programs Foundation of Ministry of Education of China （20070610128）.
文摘Liquid phase oxidation of toluene is an environmental benign route for the production of benzoic acid.In a φ48mm bubble column reactor,the commercial process of toluene liquid phase oxidation was conducted with Co(CH3COO)2.4H2O as catalyst.The Co2+ concentration [Co2+] was determined by extraction spectrophotometry and hereby the Co3+ concentration [Co3+] was obtained by mass balance.The results showed that [Co3+] reached the maximum at about 25-30min.[Co3+] increased with increasing Co catalyst amount at total Co concentration<150 mg.L-1 of toluene.The conversion of toluene,yield and selectivity of benzoic acid increased with the increasing [Co3+/Co2+] max.A high [Co3+] and a high [Co3+]/[Co2+] ratio are beneficial to the reaction.
基金Supported by the National Natural Science Foundation of China(21406008)
文摘Using catalytic oxidative absorption for H_2S removal is of great interest due to its distinct advantages. However,traditional scrubbing process faces a great limitation in the confined space. Therefore, there is an urgent demand to develop high-efficiency process intensification technology for such a system. In this article, H_2S absorption experimental research was conducted in a rotating packed bed(RPB) reactor with ferric chelate absorbent and a mixture of N_2 and H_2S, which was used to simulate natural gas. The effects of absorbent p H value, gas–liquid ratio, gravity level of RPB, absorption temperature and character of the packing on the desulfurization efficiency were investigated. The results showed that H_2S removal efficiency could reach above 99.6% under the most of the experimental condition and above 99.9% under the optimal condition. A long-time continuous experiment was conducted to investigate the stability of the whole process combining absorption and regeneration. The result showed that the process could well realize simultaneous desulfurization and absorbent regeneration, and the H_2S removal efficiency kept relatively stable in the whole duration of 72 h. It can be clearly seen that high gravity technology desulfurization process, which is simple, high-efficiency, and space intensive, has a good prospect for industrial application of H_2S removal in confined space.
基金Supported by the National Natural Science Foundation of China(21161140329)the International Science&Technology Cooperation Program of China(2013DFG60060)the National Key Technology R&D Program(2010BAC66B01,2012BAC03B05)
文摘The performance characteristics of isothermal fluidized bed syngas methanation for substitute natural gas are investigated over a self-made Ni–Mg/Al2O3 catalyst. Via atmospheric methanation in a laboratory fluidized bed reactor it was clarified that the CO conversion varied in 5% when changing the space velocity in 40–120 L·g-1·h-1but the conversion increased obviously by raising the superficial gas velocity from 4 to12.4 cm·s-1. The temperature at 823 K is suitable for syngas methanation while obvious deposition of uneasyoxidizing Cγoccurs on the catalyst at temperatures around 873 K. From a kinetic aspect, the lowest reaction temperature is suggested to be 750 K when the space velocity is 60 L·g-1·h-1. Raising the H2/CO ratio of the syngas increased proportionally the CO conversion and CH4 selectivity, showing that at enough high H2/CO ratios the active sites on the catalyst are sufficient for CO adsorption and in turn the reaction with H2 for forming CH4.Introducing CO2 into the syngas feed suppresses the water gas shift and Boudouard reactions and thus increased H2 consumption. The ratio of CO2/CO in syngas should be better below 0.52 because varying the ratio from 0.52 to0.92 resulted in negligible increases in the H2 conversion and CH4 selectivity but decreased the CH4 yield.Introducing steam into the feed gas affected little the CO conversion but decreased the selectivity to CH4. The tested Ni–Mg/Al2O3 catalyst manifested good stability in structure and activity even in syngas containing water vapor.
基金Supported by the National Natural Science Foundation of China(21206119 and21576208)the Program for Changjiang Scholars and Innovative Research Team in University of Ministry of Education of China(IRT13084)
文摘A functional electrocatalytic membrane reactor(ECMR) was performed for the electrocatalytic oxidation of2,2,3,3-tetrafluoro-l-propanol(TFP) into high value-added sodium 2,2,3,3-tetrafluoropropionate(STFP),A computational fluid dynamics(CFD) technique was applied to simulate the hydrodynamic distributions along a tubular ECMR so as to provide guidance for the design and optimization of ECMR Two-dimensional simulation with porous media model was employed to predict the properties of fluid dynamics in ECMR.The experimental investigation was carried to confirm the CFD simulation.Results showed that a uniform distribution of permeate velocity along the tubular reactor with short length and large diameter could be obtained.TFP conversion of97.7%,the selectivity to STFP of 99.9%and current efficiency of 40.1%were achieved from the ECMR with a length of 40 mm and an inside diameter of 53 mm.The simulations were in good agreement with the experimental results.
基金the grant of Post-Doc. Program, Kyungpook National University (1999).
文摘Hydrogen production by partial oxidation steam reforming of methanol over a Cu/ZnO/Al2 O3 catalyst has been paid more and more attention. The chemical equilibria involved in the methanol partial oxidation steam reforming reaction network such as methanol partial oxidation, methanol steam reforming, decomposition of methanol and water-gas shift reaction have been examined over the ranges of temperature 473-1073 K under normal pressure. Based on the detailed kinetics of these reactions over a Cu/ZnO/Al2O3 catalyst, and from the basic concept of the effectiveness factor, the intraparticle diffusion limitations were taken into account. The effectiveness factors for each reaction along the bed length were calculated. Then important results were offered for the simulation of this reaction process.
文摘By taking the surface chemical reactions as the rate-controlling step, a possible reaction mechanism for ethylene epoxidation to synthesize ethylene oxide over the A-type silver catalyst was developed, while it was assumed that the epoxidation reaction would take place between ethylene and the un-dissociated adsorbed oxygen O2 a on the solo active sites, while the deep oxidation would occur between ethylene and the dissociated adsorbed oxygen Oa on the adjacent multi-active sites. In order to describe the effect of 1,2-C2H4Cl2(EDC) inhibitor on the ethylene epoxidation process, the reversible reactions between EDC and vinyl chloride(VC) on the active sites of silver catalyst was introduced. According to the assumed mechanism, the hyperbolic macro-kinetic model of ethylene epoxidation over the A-type silver catalyst was established, and the macrokinetic experiments were carried out in an internal-recycle gradientless reactor operating at a pressure of 2.1 MPa and a temperature in the range of 217.8—249.0 ℃, with the gas composition(molar fraction) consisting of 15.82%—34.65% C2H4, 2.55%—7.80% O2, 0.88%—6.15% CO2, 0.15—2.61 μmol/mol of 1,2-C2H4Cl2 and 0.14—1.28 μmol/mol of C2H3 Cl. By means of the Simplex Optimal Method, the parameters of the macrokinetic models were estimated. Statistical test showed that the macrokinetic models developed for the A-type silver catalyst agree well with the experimental results.
