This work synthesized a series of Ni/CeO_(2)/Al_(2)O_(3) catalysts with varying CeO_(2) doping amounts to enhance low-temperature CO_(2) methanation.The introduction of CeO_(2) weakens the interaction between Ni and A...This work synthesized a series of Ni/CeO_(2)/Al_(2)O_(3) catalysts with varying CeO_(2) doping amounts to enhance low-temperature CO_(2) methanation.The introduction of CeO_(2) weakens the interaction between Ni and Al_(2)O_(3),leading to the formation of Ni-CeO_(2) active sites.This results in a high dispersion of Ni and CeO_(2),improved catalyst reducibility,increased number of active sites,and enhanced the CO_(2) methanation.This work further investigated the impact of WHSV and catalyst stacking configuration to enhance the reaction.When the catalyst is stacked into three segments with a temperature gradient of 330℃,300℃,and 250℃under WHSV=9000 ml·h^(-1)·g^(-1),the CO_(2) conversion significantly increases to 95%,which is remarkably close to the thermodynamic equilibrium(96%).展开更多
Catalytic decomposition of methane using a Fe-based catalyst for hydrogen production has been studied in this work. A Fe/Al2O3 catalyst previously developed by our research group has been tested in a fluidized bed rea...Catalytic decomposition of methane using a Fe-based catalyst for hydrogen production has been studied in this work. A Fe/Al2O3 catalyst previously developed by our research group has been tested in a fluidized bed reactor （FBR）. A parametric study ot the effects of some process variables, including reaction temperature and space velocity, is undertaken. The operating conditions strongly affect the catalyst performance. Methane conversion was increased by increasing the temperature and lowering the space velocity. Using temperatures between 700 and 900℃ and space velocities between 3 and 6 LN/（gcat·h）, a methane conversion in the range of 25%-40% for the gas exiting the reactor could be obtained during a 6 h run. In addition, carbon was deposited in the form of nanofilaments （chain like nanofibers and multiwall nanotubes） with similar properties to those obtained in a fixed bed reactor.展开更多
A novel particle/metal-based monolithic catalysts dual-bed reactor with beds-interspace supplementary oxygen is constructed comprising of the upper-layer 5 wt%Na2WO4-2 wt%Mn/SiO2 particle catalyst and the under-layer ...A novel particle/metal-based monolithic catalysts dual-bed reactor with beds-interspace supplementary oxygen is constructed comprising of the upper-layer 5 wt%Na2WO4-2 wt%Mn/SiO2 particle catalyst and the under-layer 3 wt%Ce-5 wt%Na2WO4-2 wt%Mn/SBA-15/Al2O3/FeCrA1 metal-based monolithic catalyst as well as a side tube in the interspaces of two layers for supplementing 02. The reaction performance of oxidative coupling of methane （OCM） in the dual-bed reactor system is evaluated. The effects of the reaction parameters such as feed CH4/O2 ratio, reaction temperature and side tube feed 02 flowrate on the catalytic performance are investigated. The results indicate that the suggested mode of dual-bed reactor exhibits an excellent performance for OCM. CH4 conversion of 33.2%, C2H4 selectivity of 46.5% and C2 yield of 22.5% could be obtained, which have been increased by 6.4%, 4.1% and 5.5%, respectively, as compared with 5 wt%Na2WO4-2 wt%Mn/SiO2 particle catalyst in a single-bed reactor and increased by 10.7%, 31.9% and 17.7%, respectively, as compared with 3 wt%Ce-5 wt%Na2WO4-2 wt%Mn/SBA-15/Al2O3/FeCrA1 metal-based monolithic catalyst in a single-bed reactor. The effective promotion of OCM performance in the reactor would supply a valuable reference for the industrialization of OCM process.展开更多
A dual-bed reactor was constructed comprising of a 5%Na2WO4-2%Mn/SiO2 particle catalyst and a 4%Ce-5%Na2WO4-2%Mn/SiO2 /cordierite monolithic catalyst.The reaction performance of the oxidative coupling of methane （OCM...A dual-bed reactor was constructed comprising of a 5%Na2WO4-2%Mn/SiO2 particle catalyst and a 4%Ce-5%Na2WO4-2%Mn/SiO2 /cordierite monolithic catalyst.The reaction performance of the oxidative coupling of methane （OCM） over the dual-bed reactor system was evaluated.The effects of the bed height and operation mode,as well as the reaction parameters such as reaction temperature,CH4/O2 ratio and flowrate of feed gas,on the catalytic performance were investigated.The results indicated that the suggested dual-bed reactor exhibited a good performance for the OCM reaction when the feed gases firstly passed through the particle catalyst bed and then to the monolithic catalyst bed.A CH4 conversion of 38.2% and a C2H4 selectivity of 43.3% could be obtained using the dual-bed reactor with a particle catalyst bed height of 10 mm and a monolithic catalyst bed height of 50 mm.Both the CH4 conversion and C2H4 selectivity have increased by 2.5% and 12.8%,respectively,as compared with the 5%Na2WO4-2%Mn/SiO2 particle catalyst in a conventional single-bed reactor and by 12.9% and 23.0%,respectively,as compared with the 4%Ce-5%Na2WO4-2%Mn/SiO2 /cordierite monolithic catalyst in a single-bed reactor.The catalytic performance of the OCM in the dual-bed reactor system has been improved remarkably.展开更多
Recently,a plasma catalyst was employed to efflciently degrade antibiotic residues in the environment.In this study,the plasma generated in a packed bed dielectric barrier reactor combined with TiO_(2)catalyst is used...Recently,a plasma catalyst was employed to efflciently degrade antibiotic residues in the environment.In this study,the plasma generated in a packed bed dielectric barrier reactor combined with TiO_(2)catalyst is used to degrade the antibiotic tiamulin(TIA)loaded on the surface of simulated soil particles.The effects of applied voltage,composition of the working gas,gas flow rate and presence or absence of catalyst on the degradation effect were studied.It was found that plasma and catalyst can produce a synergistic effect under optimal conditions(applied voltage 25 k V,oxygen ratio 1%,gas flow rate 0.6 l min^(-1),treatment time 5 min).The degradation efflciency of the plasma combined with catalyst can reach 78.6%,which is 18.4%higher than that of plasma without catalyst.When the applied voltage is 30 k V,the gas flow rate is 1 l min^(-1),the oxygen ratio is 1%and the plasma combined with TiO_(2)catalyst treats the sample for 5 min the degradation efflciency of TIA reached 97%.It can be concluded that a higher applied voltage and longer processing times not only lead to more degradation but also result in a lower energy efflciency.Decreasing the oxygen ratio and gas flow rate could improve the degradation efflciency.The relative distribution and identity of the major TIA degradation product generated was determined by high-performance liquid chromatography–mass spectrometry analysis.The mechanism of TIA removal by plasma and TiO_(2)catalyst was analyzed,and the possible degradation path is discussed.展开更多
The work is devoted to the study of combustion of brown coal,pine sawdust,and their mixtures in a fluidized bed of catalyst at 600-750℃.It is shown that an increase in the content of sawdust in a mixture with brown c...The work is devoted to the study of combustion of brown coal,pine sawdust,and their mixtures in a fluidized bed of catalyst at 600-750℃.It is shown that an increase in the content of sawdust in a mixture with brown coal leads to an increase in the burnout degree of solid fuel from 94.4%to 99.9%,while the emission of greenhouse gases in the form of CO_(2)CO and NOxis reduced(CO_(2)from the biomass is not included in the balance).The high content of alkaline earth metal oxides(CaO and MgO)in the mineral part of brown coal,sawdust,and their mixtures eliminates the emission of sulfur oxides and the slagging of heat-exchange surfaces during the combustion in a fluidized bed of catalyst.The optimal temperature,when the highest burnout degree of the above fuels is achieved in the combustion is 750℃.It is also shown that the increase in temperature and the content of sawdust in the composition of the fuel mixtures has a positive effect on the economic and environmental process indicators.展开更多
For the synthesis of single-walled carbon nanotubes （SWCNTs） from CH4 over a Fe/MgO catalyst, we proposed a coupled Downer-turbulent fluidized-bed （TFB） reactor to enhance the selectivity and yield （or production...For the synthesis of single-walled carbon nanotubes （SWCNTs） from CH4 over a Fe/MgO catalyst, we proposed a coupled Downer-turbulent fluidized-bed （TFB） reactor to enhance the selectivity and yield （or production rate） of SWCNTs. By controlling a very short catalyst residence time （1-3 s） in the Downer, only part of Fe oxides can be reduced to form Fe nano particles （NPs） available for the growth of SWCNTs. The percentage of unreduced Fe oxides increased and the yield of SWCNTs decreased accordingly with the increase of catalyst feeding rate in Downer. SWCNTs were preferentially grown on the catalyst surface and inhibited the sintering of the Fe crystallites which would be formed thereafter in the downstream TFB, evidenced by TEM, Raman and TGA. The coupled Downer-turbulent fluidized-bed reactor technology allowed higher selectivity and higher production rate of SWCNTs as compared to TFB alone.展开更多
Performance of the oxidative coupling of methane in fluidized-bed reactor was experimentally investigated using Mn-Na2WO4/SiO2,La2O3/CaO and La2O3-SrO/CaO catalysts.These catalysts were found to be stable,especially M...Performance of the oxidative coupling of methane in fluidized-bed reactor was experimentally investigated using Mn-Na2WO4/SiO2,La2O3/CaO and La2O3-SrO/CaO catalysts.These catalysts were found to be stable,especially Mn-Na2WO4/SiO2 catalyst.The effect of sodium content of this catalyst was analyzed and the challenge of catalyst agglomeration was addressed using proper catalyst composition of 2%Mn2.2%Na2WO4/SiO2.For other two catalysts,the effect of Lanthanum-Strontium content was analyzed and 10%La2O 3-20%SrO/CaO catalyst was found to provide higher ethylene yield than La2O3/CaO catalyst.Furthermore,the effect of operating parameters such as temperature and methane to oxygen ratio were also reviewed.The highest ethylene and ethane （C2） yield was achieved with the lowest methane to oxygen ratio around 2.40.5% selectivity to ethylene and ethane and 41% methane conversion were achieved over La2O3-SrO/CaO catalyst while over Mn-Na2WO4 /SiO2 catalyst,40% and 48% were recorded,respectively.Moreover,the consecutive effects of nitrogen dilution,ethylene to ethane production ratio and other performance indicators on the down-stream process units were qualitatively discussed and Mn-Na2WO4/SiO2 catalyst showed a better performance in the reactor and process scale analysis.展开更多
Dimethyl ether (DME) is considered as a significant fuel alternative with a critical manufacturing process. Only a few authors have presented the kinetic analysis of attractive and alternative catalysts to Al<sub&g...Dimethyl ether (DME) is considered as a significant fuel alternative with a critical manufacturing process. Only a few authors have presented the kinetic analysis of attractive and alternative catalysts to Al<sub>2</sub>O<sub>3</sub> and/or zeolite in DME production, despite the fact that there is a large library of kinetic studies for these commercial catalysts. The purpose of this research was to contribute to this direction by conducting a catalytic test to determine kinetic parameters for methanol dehydration over sulfonic acid catalysts (resin). However, due to the relevance of the mathematical description of this process in the industry was also studied, a study of kinetics parameters and mathematical modeling of methanol dehydration in an atmospheric gas phase in a fixed bed reactor with a temperature range (90°C - 120°C) was examined. The Langmuir-Hinshelwood (L-H) model provides the best fit to experimental data, with an excellent R<sup>2</sup> = 0.9997, and the experimental results were compared to those predicted by these models with very small deviations. The kinetic parameters were found to be in good agreement with the Arrhenius equation, with acceptable straight-line graphs. The activation energy E was computed and found to be 27.66 kJ/mole, with an average variation of 0.32 percent between the predicted and calculated results. Simple mathematical continuum models (plug flow reactor PFR) showed an acceptable agreement with the experimental data.展开更多
The methane autothermal reforming in the present of oxygen was studied over cerium- and zirconium-promoted Ni/SiO2 catalysts in a fluidized bed reactor. The addition of CeZrO2 resulted in a significant improvement in ...The methane autothermal reforming in the present of oxygen was studied over cerium- and zirconium-promoted Ni/SiO2 catalysts in a fluidized bed reactor. The addition of CeZrO2 resulted in a significant improvement in the initial activity of the catalysis as well as an increase in the stability. The long-term activity of the promoted catalyst was dependent upon the rapid redox properties between the oxidative zone and the reductive zone in a fluidized bed reactor. H2 temperature-programmed reduction （H2-TPR） and face reaction （TPSR） studies demonstrated that addition of the CeZrO2 resulted in an increase in the reducibility and oxygen transfer ability of the support, Ni/Ceo.5ZrO0.5O2-SiO2 showed improved redox properties compared with Ni/SiO2 due to a low-temperature reduction. X-ray diffraction （XRD） of the fresh and spent catalysts showed that the promoter enhanced the nickel dispersion and retarded metal particle growth during reaction at high temperature, and surface Ni was gradually oxidized by remaining O2, leading to Ni deactivation.展开更多
Recently, as a direct consequence of the dwindling world oil reserves and the growing awareness of the environmental problems associated with the use of coal as energy source, there is growing interest in cheaper, abu...Recently, as a direct consequence of the dwindling world oil reserves and the growing awareness of the environmental problems associated with the use of coal as energy source, there is growing interest in cheaper, abundant and cleaner burning methane. The Gas-to-Liquid technology offers perhaps the most attractive routes for the exploitation of the world huge and growing natural gas resources. Using this process the erstwhile stranded gas is converted to premium grade liquid fuels and chemicals that are easily transported. However, a widespread application of the GTL process is being hampered by economical and technical challenges. The high cost of synthesis gas, for instance, weighs heavily on the economics and competitiveness of the process limiting its wider application. This work presented a modified Gas-to-Liquid process that eliminates the costly synthesis gas production step. The proposed process utilized an alternative pathway for methane activation via the production of chloromethane derivatives which are then converted to hydrocarbons. It established that hydrocarbons mainly olefins can be economically produced from di- and tri-chloro- methanes over a typical iron-based Fischer Tropsch catalysts in a moving bed reactor at industrially relevant conditions. Some of the attractions of the proposed process include a) the elimination of the costly air separation plant requirement b) high process selectivity and c) significant reduction of carbon dioxide emissions thereby saving on feedstock loss and the costly CO2 removal and isolation processes.展开更多
Thermal treatment either in the presence of oxygen (calcination) or of a reducing agent (reduction) result is all the time a key issue within the preparation of a catalyst. In this work, a microwave plasma treatment w...Thermal treatment either in the presence of oxygen (calcination) or of a reducing agent (reduction) result is all the time a key issue within the preparation of a catalyst. In this work, a microwave plasma treatment was chosen as an alternative to typical calcinations, because it is a more energy efficient process. Thus, a Microwave Fluidized Bed Plasma reactor (MFBP) was employed in catalyst synthesis process under different gas compositions, such as argon and argon/oxygen mixtures over g-alumina supported silver catalysts, which are generally used for selective reduction of NOx by ethanol. After the first catalytic tests performed in the presence of plasma treated catalyst, it can be concluded that plasma treatment process represents an interesting alternative to conventional calcination during catalyst synthesis, resulting in a more sustainable process, moreover in view of its industrial application. In order to understand the particular effect of plasma treatment, the catalysts submitted to this treatment were carefully characterized by means of thermo gravimetric analysis (TGA), differential thermal analysis (DTA) and UV-VIS-NIR.展开更多
基金financial support of the National Natural Science Foundation of China(22178265)Tianjin Science and Technology Project(21JCYBJC00400)Open Project for Ningbo Key Laboratory of Green Petrochemical Carbon Emission Reduction Technology and Equipment(ZITJU2023-ZYDK001).
文摘This work synthesized a series of Ni/CeO_(2)/Al_(2)O_(3) catalysts with varying CeO_(2) doping amounts to enhance low-temperature CO_(2) methanation.The introduction of CeO_(2) weakens the interaction between Ni and Al_(2)O_(3),leading to the formation of Ni-CeO_(2) active sites.This results in a high dispersion of Ni and CeO_(2),improved catalyst reducibility,increased number of active sites,and enhanced the CO_(2) methanation.This work further investigated the impact of WHSV and catalyst stacking configuration to enhance the reaction.When the catalyst is stacked into three segments with a temperature gradient of 330℃,300℃,and 250℃under WHSV=9000 ml·h^(-1)·g^(-1),the CO_(2) conversion significantly increases to 95%,which is remarkably close to the thermodynamic equilibrium(96%).
基金the Spanish Science and InnovationMinistry for the financial support of Project ENE2008-06516-C03-01
文摘Catalytic decomposition of methane using a Fe-based catalyst for hydrogen production has been studied in this work. A Fe/Al2O3 catalyst previously developed by our research group has been tested in a fluidized bed reactor （FBR）. A parametric study ot the effects of some process variables, including reaction temperature and space velocity, is undertaken. The operating conditions strongly affect the catalyst performance. Methane conversion was increased by increasing the temperature and lowering the space velocity. Using temperatures between 700 and 900℃ and space velocities between 3 and 6 LN/（gcat·h）, a methane conversion in the range of 25%-40% for the gas exiting the reactor could be obtained during a 6 h run. In addition, carbon was deposited in the form of nanofilaments （chain like nanofibers and multiwall nanotubes） with similar properties to those obtained in a fixed bed reactor.
基金supported by the National Basic Research Program of China (Project No. 2005CB221405)
文摘A novel particle/metal-based monolithic catalysts dual-bed reactor with beds-interspace supplementary oxygen is constructed comprising of the upper-layer 5 wt%Na2WO4-2 wt%Mn/SiO2 particle catalyst and the under-layer 3 wt%Ce-5 wt%Na2WO4-2 wt%Mn/SBA-15/Al2O3/FeCrA1 metal-based monolithic catalyst as well as a side tube in the interspaces of two layers for supplementing 02. The reaction performance of oxidative coupling of methane （OCM） in the dual-bed reactor system is evaluated. The effects of the reaction parameters such as feed CH4/O2 ratio, reaction temperature and side tube feed 02 flowrate on the catalytic performance are investigated. The results indicate that the suggested mode of dual-bed reactor exhibits an excellent performance for OCM. CH4 conversion of 33.2%, C2H4 selectivity of 46.5% and C2 yield of 22.5% could be obtained, which have been increased by 6.4%, 4.1% and 5.5%, respectively, as compared with 5 wt%Na2WO4-2 wt%Mn/SiO2 particle catalyst in a single-bed reactor and increased by 10.7%, 31.9% and 17.7%, respectively, as compared with 3 wt%Ce-5 wt%Na2WO4-2 wt%Mn/SBA-15/Al2O3/FeCrA1 metal-based monolithic catalyst in a single-bed reactor. The effective promotion of OCM performance in the reactor would supply a valuable reference for the industrialization of OCM process.
基金supported by the National Basic Research Program of China(Project No. 2005CB221405)
文摘A dual-bed reactor was constructed comprising of a 5%Na2WO4-2%Mn/SiO2 particle catalyst and a 4%Ce-5%Na2WO4-2%Mn/SiO2 /cordierite monolithic catalyst.The reaction performance of the oxidative coupling of methane （OCM） over the dual-bed reactor system was evaluated.The effects of the bed height and operation mode,as well as the reaction parameters such as reaction temperature,CH4/O2 ratio and flowrate of feed gas,on the catalytic performance were investigated.The results indicated that the suggested dual-bed reactor exhibited a good performance for the OCM reaction when the feed gases firstly passed through the particle catalyst bed and then to the monolithic catalyst bed.A CH4 conversion of 38.2% and a C2H4 selectivity of 43.3% could be obtained using the dual-bed reactor with a particle catalyst bed height of 10 mm and a monolithic catalyst bed height of 50 mm.Both the CH4 conversion and C2H4 selectivity have increased by 2.5% and 12.8%,respectively,as compared with the 5%Na2WO4-2%Mn/SiO2 particle catalyst in a conventional single-bed reactor and by 12.9% and 23.0%,respectively,as compared with the 4%Ce-5%Na2WO4-2%Mn/SiO2 /cordierite monolithic catalyst in a single-bed reactor.The catalytic performance of the OCM in the dual-bed reactor system has been improved remarkably.
基金supported by National Natural Science Foundation of China(Nos.51967018,11965018 and 51967017)the Science and Technology Development Fund of Xinjiang Production and Construction(No.2019BC009)the Innovation and Development Special Project of Shihezi University(No.CXFZ202105)。
文摘Recently,a plasma catalyst was employed to efflciently degrade antibiotic residues in the environment.In this study,the plasma generated in a packed bed dielectric barrier reactor combined with TiO_(2)catalyst is used to degrade the antibiotic tiamulin(TIA)loaded on the surface of simulated soil particles.The effects of applied voltage,composition of the working gas,gas flow rate and presence or absence of catalyst on the degradation effect were studied.It was found that plasma and catalyst can produce a synergistic effect under optimal conditions(applied voltage 25 k V,oxygen ratio 1%,gas flow rate 0.6 l min^(-1),treatment time 5 min).The degradation efflciency of the plasma combined with catalyst can reach 78.6%,which is 18.4%higher than that of plasma without catalyst.When the applied voltage is 30 k V,the gas flow rate is 1 l min^(-1),the oxygen ratio is 1%and the plasma combined with TiO_(2)catalyst treats the sample for 5 min the degradation efflciency of TIA reached 97%.It can be concluded that a higher applied voltage and longer processing times not only lead to more degradation but also result in a lower energy efflciency.Decreasing the oxygen ratio and gas flow rate could improve the degradation efflciency.The relative distribution and identity of the major TIA degradation product generated was determined by high-performance liquid chromatography–mass spectrometry analysis.The mechanism of TIA removal by plasma and TiO_(2)catalyst was analyzed,and the possible degradation path is discussed.
基金funded by the Ministry of Science and Higher Education of the Russian Federation,within the governmental order for the Boreskov Institute of Catalysis(project AAAA-A21-121011390007-7)The economic assessment and Environmental impact calculation were performed as part of the Tyumen University state assignment[project No.FEWZ2021–0014(Scientific and technical foundations and applied solutions for integrated energy and thermal processing of biomass to ensure environmentally friendly technologies in energy industry and metallurgy)]。
文摘The work is devoted to the study of combustion of brown coal,pine sawdust,and their mixtures in a fluidized bed of catalyst at 600-750℃.It is shown that an increase in the content of sawdust in a mixture with brown coal leads to an increase in the burnout degree of solid fuel from 94.4%to 99.9%,while the emission of greenhouse gases in the form of CO_(2)CO and NOxis reduced(CO_(2)from the biomass is not included in the balance).The high content of alkaline earth metal oxides(CaO and MgO)in the mineral part of brown coal,sawdust,and their mixtures eliminates the emission of sulfur oxides and the slagging of heat-exchange surfaces during the combustion in a fluidized bed of catalyst.The optimal temperature,when the highest burnout degree of the above fuels is achieved in the combustion is 750℃.It is also shown that the increase in temperature and the content of sawdust in the composition of the fuel mixtures has a positive effect on the economic and environmental process indicators.
基金supported by the Chinese National Key Program (Grant No. 2011CB932602)Natural Science Foundation of China (Key Program, 51236004)the Beijing Key Scientific Program (D12110300160000)
文摘For the synthesis of single-walled carbon nanotubes （SWCNTs） from CH4 over a Fe/MgO catalyst, we proposed a coupled Downer-turbulent fluidized-bed （TFB） reactor to enhance the selectivity and yield （or production rate） of SWCNTs. By controlling a very short catalyst residence time （1-3 s） in the Downer, only part of Fe oxides can be reduced to form Fe nano particles （NPs） available for the growth of SWCNTs. The percentage of unreduced Fe oxides increased and the yield of SWCNTs decreased accordingly with the increase of catalyst feeding rate in Downer. SWCNTs were preferentially grown on the catalyst surface and inhibited the sintering of the Fe crystallites which would be formed thereafter in the downstream TFB, evidenced by TEM, Raman and TGA. The coupled Downer-turbulent fluidized-bed reactor technology allowed higher selectivity and higher production rate of SWCNTs as compared to TFB alone.
基金supported by the Deutsche Forschungsgemeinschaft (DFG)
文摘Performance of the oxidative coupling of methane in fluidized-bed reactor was experimentally investigated using Mn-Na2WO4/SiO2,La2O3/CaO and La2O3-SrO/CaO catalysts.These catalysts were found to be stable,especially Mn-Na2WO4/SiO2 catalyst.The effect of sodium content of this catalyst was analyzed and the challenge of catalyst agglomeration was addressed using proper catalyst composition of 2%Mn2.2%Na2WO4/SiO2.For other two catalysts,the effect of Lanthanum-Strontium content was analyzed and 10%La2O 3-20%SrO/CaO catalyst was found to provide higher ethylene yield than La2O3/CaO catalyst.Furthermore,the effect of operating parameters such as temperature and methane to oxygen ratio were also reviewed.The highest ethylene and ethane （C2） yield was achieved with the lowest methane to oxygen ratio around 2.40.5% selectivity to ethylene and ethane and 41% methane conversion were achieved over La2O3-SrO/CaO catalyst while over Mn-Na2WO4 /SiO2 catalyst,40% and 48% were recorded,respectively.Moreover,the consecutive effects of nitrogen dilution,ethylene to ethane production ratio and other performance indicators on the down-stream process units were qualitatively discussed and Mn-Na2WO4/SiO2 catalyst showed a better performance in the reactor and process scale analysis.
文摘Dimethyl ether (DME) is considered as a significant fuel alternative with a critical manufacturing process. Only a few authors have presented the kinetic analysis of attractive and alternative catalysts to Al<sub>2</sub>O<sub>3</sub> and/or zeolite in DME production, despite the fact that there is a large library of kinetic studies for these commercial catalysts. The purpose of this research was to contribute to this direction by conducting a catalytic test to determine kinetic parameters for methanol dehydration over sulfonic acid catalysts (resin). However, due to the relevance of the mathematical description of this process in the industry was also studied, a study of kinetics parameters and mathematical modeling of methanol dehydration in an atmospheric gas phase in a fixed bed reactor with a temperature range (90°C - 120°C) was examined. The Langmuir-Hinshelwood (L-H) model provides the best fit to experimental data, with an excellent R<sup>2</sup> = 0.9997, and the experimental results were compared to those predicted by these models with very small deviations. The kinetic parameters were found to be in good agreement with the Arrhenius equation, with acceptable straight-line graphs. The activation energy E was computed and found to be 27.66 kJ/mole, with an average variation of 0.32 percent between the predicted and calculated results. Simple mathematical continuum models (plug flow reactor PFR) showed an acceptable agreement with the experimental data.
基金supported by the New Century Excellent Talents in University of Henan Province (2006HANCET-20)the National Natural Science Foundation of China (20433030)
文摘The methane autothermal reforming in the present of oxygen was studied over cerium- and zirconium-promoted Ni/SiO2 catalysts in a fluidized bed reactor. The addition of CeZrO2 resulted in a significant improvement in the initial activity of the catalysis as well as an increase in the stability. The long-term activity of the promoted catalyst was dependent upon the rapid redox properties between the oxidative zone and the reductive zone in a fluidized bed reactor. H2 temperature-programmed reduction （H2-TPR） and face reaction （TPSR） studies demonstrated that addition of the CeZrO2 resulted in an increase in the reducibility and oxygen transfer ability of the support, Ni/Ceo.5ZrO0.5O2-SiO2 showed improved redox properties compared with Ni/SiO2 due to a low-temperature reduction. X-ray diffraction （XRD） of the fresh and spent catalysts showed that the promoter enhanced the nickel dispersion and retarded metal particle growth during reaction at high temperature, and surface Ni was gradually oxidized by remaining O2, leading to Ni deactivation.
文摘Recently, as a direct consequence of the dwindling world oil reserves and the growing awareness of the environmental problems associated with the use of coal as energy source, there is growing interest in cheaper, abundant and cleaner burning methane. The Gas-to-Liquid technology offers perhaps the most attractive routes for the exploitation of the world huge and growing natural gas resources. Using this process the erstwhile stranded gas is converted to premium grade liquid fuels and chemicals that are easily transported. However, a widespread application of the GTL process is being hampered by economical and technical challenges. The high cost of synthesis gas, for instance, weighs heavily on the economics and competitiveness of the process limiting its wider application. This work presented a modified Gas-to-Liquid process that eliminates the costly synthesis gas production step. The proposed process utilized an alternative pathway for methane activation via the production of chloromethane derivatives which are then converted to hydrocarbons. It established that hydrocarbons mainly olefins can be economically produced from di- and tri-chloro- methanes over a typical iron-based Fischer Tropsch catalysts in a moving bed reactor at industrially relevant conditions. Some of the attractions of the proposed process include a) the elimination of the costly air separation plant requirement b) high process selectivity and c) significant reduction of carbon dioxide emissions thereby saving on feedstock loss and the costly CO2 removal and isolation processes.
文摘Thermal treatment either in the presence of oxygen (calcination) or of a reducing agent (reduction) result is all the time a key issue within the preparation of a catalyst. In this work, a microwave plasma treatment was chosen as an alternative to typical calcinations, because it is a more energy efficient process. Thus, a Microwave Fluidized Bed Plasma reactor (MFBP) was employed in catalyst synthesis process under different gas compositions, such as argon and argon/oxygen mixtures over g-alumina supported silver catalysts, which are generally used for selective reduction of NOx by ethanol. After the first catalytic tests performed in the presence of plasma treated catalyst, it can be concluded that plasma treatment process represents an interesting alternative to conventional calcination during catalyst synthesis, resulting in a more sustainable process, moreover in view of its industrial application. In order to understand the particular effect of plasma treatment, the catalysts submitted to this treatment were carefully characterized by means of thermo gravimetric analysis (TGA), differential thermal analysis (DTA) and UV-VIS-NIR.
