Chlorobenzene removal was investigated in a non-thermal plasma reactor using CeO2/HZSM-5catalysts.The performance of catalysts was evaluated in terms of removal and energy efficiency.The decomposition products of chlo...Chlorobenzene removal was investigated in a non-thermal plasma reactor using CeO2/HZSM-5catalysts.The performance of catalysts was evaluated in terms of removal and energy efficiency.The decomposition products of chlorobenzene were analyzed.The results show that CeO2/HZSM-5 exhibited a good catalytic activity,which resulted in enhancements of chlorobenzene removal,energy efficiency,and the formation of lower amounts of by-products.With regards to CO2 selectivity,the presence of catalysts favors the oxidation of by-products,leading to a higher CO2 selectivity.With respect to ozone,which is considered as an unavoidable by-product in air plasma reactors,a noticeable decrease in its concentration was observed in the presence of catalysts.Furthermore,the stability of the catalyst was investigated by analyzing the evolution of conversion in time.The experiment results indicated that CeO2/HZSM-5 catalysts have excellent stability：chlorobenzene conversion only decreased from 78%to 60%after 75 hr,which means that the CeO2/HZSM-5 suffered a slight deactivation.Some organic compounds and chlorinated intermediates were adsorbed or deposited on the catalysts surface as shown by the results of Fourier Transform Infrared（FT-IR） spectroscopy,scanning electron microscope（SEM） and energy dispersive X-ray spectroscopy（EDS） analyses of the catalyst before and after the reaction,revealing the cause of catalyst deactivation.展开更多
This study employed a wet impregnation method to synthesize five types of Cu/HZSM-5 adsorbents with Si/Al ratios of 25,50,85,200,and 300,used for the removal of H_(2)S in lowtemperature,low-oxygen environments.The imp...This study employed a wet impregnation method to synthesize five types of Cu/HZSM-5 adsorbents with Si/Al ratios of 25,50,85,200,and 300,used for the removal of H_(2)S in lowtemperature,low-oxygen environments.The impact of different Si/Al ratios on the adsorption oxidative performance of Cu_(30)/HZSM-5–85 adsorbents was investigated.According to the performance test results,Cu_(30)/HZSM-5–85 exhibited the highest breakthrough capacity,reaching 231.75 mg H_(2)S/g_(sorbent).Cu/HZSM-5 sorbent maintains a strong ability to remove H_(2)S even under humid conditions and shows excellent water resistance.XRD,BET,and XPS results revealed that CuO is the primary active species,with Cu_(30)/HZSM-5–85 having the largest surface area and highest CuO content,providing more active sites for H_(2)S adsorption.H_(2)-TPR and O_(2)-TPD results confirmed that Cu_(30)/HZSM-5–85 sorbent exhibits outstanding redox properties and oxygen storage capacity,contributing to excellent oxygen transferability in the molecular sieve adsorption-oxidation process.With notable characteristics such as a large surface area,high desulfurization efficiency,and water resistance,Cu_(30)/HZSM-5–85 sorbents hold significant importance for industrial applications.展开更多
CeO_2–CaO–Pd/HZSM-5 catalyst was prepared for the dimethyl ether(DME) one-step synthesis in a continuous fixed-bed micro-reactor from the sulfur-containing syngas. The catalytic stability over hybrid catalyst of Ce...CeO_2–CaO–Pd/HZSM-5 catalyst was prepared for the dimethyl ether(DME) one-step synthesis in a continuous fixed-bed micro-reactor from the sulfur-containing syngas. The catalytic stability over hybrid catalyst of CeO_2–CaO–Pd/HZSM-5 was investigated to ensure that the kinetics experimental results were not significantly influenced by induction period and catalytic deactivation. A large number of kinetic data points(40 sets) were obtained over a range of temperature(240–300 °C), pressure(3–4 MPa), gas hourly space velocity(GHSV)(2000–3000 L·kg^(-1)·h^(-1)) and H_2/CO mole ratio(2–3). Kinetic model for the methanol synthesis reaction and the dehydration of methanol were obtained separately according to reaction mechanism and Langmuir–Hinshelwood mechanism. Regression parameters were investigated by the method combining the simplex method and Runge–Kutta method. The model calculations were in appropriate accordance with the experimental data.展开更多
基金supported by the Program for Changjiang Scholars and Innovative Research Team in University(No.IRT13096)the International S&T Cooperation Program of China(No.2011DFA92660)+2 种基金the National Natural Science Foundation of China(No.21276239)the Zhejiang Province Natural Science Foundation of China(No.LY14E080009)the International Cooperation Program of Zhejiang province(No.2013C24003)
文摘Chlorobenzene removal was investigated in a non-thermal plasma reactor using CeO2/HZSM-5catalysts.The performance of catalysts was evaluated in terms of removal and energy efficiency.The decomposition products of chlorobenzene were analyzed.The results show that CeO2/HZSM-5 exhibited a good catalytic activity,which resulted in enhancements of chlorobenzene removal,energy efficiency,and the formation of lower amounts of by-products.With regards to CO2 selectivity,the presence of catalysts favors the oxidation of by-products,leading to a higher CO2 selectivity.With respect to ozone,which is considered as an unavoidable by-product in air plasma reactors,a noticeable decrease in its concentration was observed in the presence of catalysts.Furthermore,the stability of the catalyst was investigated by analyzing the evolution of conversion in time.The experiment results indicated that CeO2/HZSM-5 catalysts have excellent stability：chlorobenzene conversion only decreased from 78%to 60%after 75 hr,which means that the CeO2/HZSM-5 suffered a slight deactivation.Some organic compounds and chlorinated intermediates were adsorbed or deposited on the catalysts surface as shown by the results of Fourier Transform Infrared（FT-IR） spectroscopy,scanning electron microscope（SEM） and energy dispersive X-ray spectroscopy（EDS） analyses of the catalyst before and after the reaction,revealing the cause of catalyst deactivation.
基金supported by the National Natural Science Foundation of China(Nos.52270106 and 22266021)Yunnan Major Scientific and Technological Projects(No.202202AG050005)Yunnan Fundamental Research Projects(No.202201AT070116).
文摘This study employed a wet impregnation method to synthesize five types of Cu/HZSM-5 adsorbents with Si/Al ratios of 25,50,85,200,and 300,used for the removal of H_(2)S in lowtemperature,low-oxygen environments.The impact of different Si/Al ratios on the adsorption oxidative performance of Cu_(30)/HZSM-5–85 adsorbents was investigated.According to the performance test results,Cu_(30)/HZSM-5–85 exhibited the highest breakthrough capacity,reaching 231.75 mg H_(2)S/g_(sorbent).Cu/HZSM-5 sorbent maintains a strong ability to remove H_(2)S even under humid conditions and shows excellent water resistance.XRD,BET,and XPS results revealed that CuO is the primary active species,with Cu_(30)/HZSM-5–85 having the largest surface area and highest CuO content,providing more active sites for H_(2)S adsorption.H_(2)-TPR and O_(2)-TPD results confirmed that Cu_(30)/HZSM-5–85 sorbent exhibits outstanding redox properties and oxygen storage capacity,contributing to excellent oxygen transferability in the molecular sieve adsorption-oxidation process.With notable characteristics such as a large surface area,high desulfurization efficiency,and water resistance,Cu_(30)/HZSM-5–85 sorbents hold significant importance for industrial applications.
基金Supported by the National Natural Science Foundation of China(51204179,51204182,51674256)The Natural Science Foundation of Jiangsu Province,China(BK20141242)
文摘CeO_2–CaO–Pd/HZSM-5 catalyst was prepared for the dimethyl ether(DME) one-step synthesis in a continuous fixed-bed micro-reactor from the sulfur-containing syngas. The catalytic stability over hybrid catalyst of CeO_2–CaO–Pd/HZSM-5 was investigated to ensure that the kinetics experimental results were not significantly influenced by induction period and catalytic deactivation. A large number of kinetic data points(40 sets) were obtained over a range of temperature(240–300 °C), pressure(3–4 MPa), gas hourly space velocity(GHSV)(2000–3000 L·kg^(-1)·h^(-1)) and H_2/CO mole ratio(2–3). Kinetic model for the methanol synthesis reaction and the dehydration of methanol were obtained separately according to reaction mechanism and Langmuir–Hinshelwood mechanism. Regression parameters were investigated by the method combining the simplex method and Runge–Kutta method. The model calculations were in appropriate accordance with the experimental data.
