The IR emission spectra of methane were measured under DC glow discharge conditions. The distinct difference in time between methane decomposition and C2 hydrocarbons formation was specially pointed out. C2 hydrocarbo...The IR emission spectra of methane were measured under DC glow discharge conditions. The distinct difference in time between methane decomposition and C2 hydrocarbons formation was specially pointed out. C2 hydrocarbons formed at the end of methane decomposition. The optimum condition for C2 hydrocarbon formation was studied and the optimum combination between electric current density and methane input quantity was suggested. The appropriate reaction conditions for methane decomposition and C2 hydrocarbons formation are different, so high yield of C2 hydrocarbons will be probably obtained when different conditions are taken.展开更多
Methane conversion has been studied using gliding arc plasma in the presence of argon.The process was conducted at atmospheric pressure and ambient temperature.The focus of this research was to develop a process of co...Methane conversion has been studied using gliding arc plasma in the presence of argon.The process was conducted at atmospheric pressure and ambient temperature.The focus of this research was to develop a process of converting methane to C2 hydrocarbons and hydrogen. The main parameters,including the CH4/Ar mole ratio,the CH4 flow rate,the input voltage,and the minimum electrode gap,were varied to investigate their effects on methane conversion rate, product distribution,energy consumption,carbon deposit,and reaction stability.The specific energy requirement（SER） was used to express the energy utilization efficiency of the process and provided a practical guidance for optimizing reaction conditions for improving energy efficiency. It was found that the carbon deposition was not conducive to methane conversion,and the gliding arc plasma discharge reached a stable state twelve minutes later.Optimum conditions for methane conversion were suggested.The maximum methane conversion rate of 43.39%was obtained under the optimum conditions.Also,C2 hydrocarbons selectivity,C2 hydrocarbons yield,H2 selectivity, H2 yield and SER were 87.20%,37.83%,81.28%,35.27%,and 2.09 MJ/mol,respectively.展开更多
The plasma technology served as a tool in unconventional catalysis has been used in natural gas conversion,because the traditional catalytic methane oxidative coupling reaction must be performed at high temperature on...The plasma technology served as a tool in unconventional catalysis has been used in natural gas conversion,because the traditional catalytic methane oxidative coupling reaction must be performed at high temperature on account of the stability of methane molecule.The focus of this research is to develop a process of converting methane to C2 hydrocarbons with non-equilibrium plasma technology at room temperature and atmospheric pressure.It was found that methane conversion increased and the selectivity of C2 hydrocarbons decreased with the voltage.The optimum input voltage range was 40-80 V corresponding to high yield of C2 hydrocarbons.Methane conversion decreased and the selectivity of C2 hydrocarbons increased with the inlet flow rate of methane.The proper methane flow rate was 20-40 ml/min （corresponding residence time 10-20 s）.The experimental results show that methane conversion was 47% and the selectivity of C2 hydrocarbons was 40% under the proper condition using atmospheric DBD cold plasma technology.It was found that the breakdown voltage of methane VB was determined by the type of electrode and the discharge gap width in this glow discharge reactor.The breakdown voltage of methane VB,min derived from the Paschen law equation was established.展开更多
Adsorptive separation of light hydrocarbons by porous solids provides an energy-efficient alternative to state-of-the-art cryogenic distillation.However,an optimal balance between the cost,performance and stability of...Adsorptive separation of light hydrocarbons by porous solids provides an energy-efficient alternative to state-of-the-art cryogenic distillation.However,an optimal balance between the cost,performance and stability of the sorbent material is yet to be achieved for industrial applications.Here,we report the efficient separation of C2 and C3 hydrocarbons by a faujasite zeolite(Na-X,Si/Al=1.23).A tandem configuration of two fixed-beds packed with Na-X affords complete dynamic separation of the ternary mixture of C_(2)H_(2)/C_(2)H_(4)/C_(2)H_(6)(1/49.5/49.5;v/v/v)under ambient conditions.Pressure-swing desorption on the latter fixed-bed gives ethylene(>99.50%,1.80 mmol g^(-1))and ethane(>99.99%,1.41 mmol g^(-1)).In situ synchrotron X-ray powder diffraction revealed the binding sites for C_(2)H_(2)and C_(2)H_(4)in Na-X.This study highlights the potential application of commercial zeolites for challenging industrial separations.展开更多
This paper deals with thermodynamic chemical equilibrium analysis using the method of direct minimization of Gibbs free energy for all possible CH4 and CO2 reactions. The effects of CO2/CH4 feed ratio, reaction temper...This paper deals with thermodynamic chemical equilibrium analysis using the method of direct minimization of Gibbs free energy for all possible CH4 and CO2 reactions. The effects of CO2/CH4 feed ratio, reaction temperature, and system pressure on equilibrium composition, conversion, selectivity and yield were studied. In addition, carbon and no carbon formation regions were also considered at various reaction temperatures and CO2/CH4 feed ratios in the reaction system at equilibrium. It was found that the reaction temperature above 1100 K and CO2/CH4 ratio=1 were favourable for synthesis gas production with H2/CO ratio unity, while carbon dioxide oxidative coupling of methane （CO2 OCM） reaction to produce ethane and ethylene is less favourable thermodynamically. Numerical results indicated that the no carbon formation region was at temperatures above 1000 K and CO2/CH4 ratio larger than 1.展开更多
The infrared emission spectra of methane, H, CH and C2 hydrocarbons in natural gas were measured. The process of methane decomposition and C2 hydrocarbons formation was investigated. The experiment showed that the tim...The infrared emission spectra of methane, H, CH and C2 hydrocarbons in natural gas were measured. The process of methane decomposition and C2 hydrocarbons formation was investigated. The experiment showed that the time and conditions of methane decomposition and C2 hydrocarbons formation were different. Methane conversion rate increased with the increase in the current and decrease in the amount of methane. Furthermore, an examination of the reaction mechanisms revealed that free radicals played an important role in the chain reaction.展开更多
The catalyst screening tests for carbon dioxide oxidative coupling of methane (CO2-OCM) have been investigated over ternary and binary metal oxide catalysts. The catalysts are prepared by doping MgO- and CeO2-based so...The catalyst screening tests for carbon dioxide oxidative coupling of methane (CO2-OCM) have been investigated over ternary and binary metal oxide catalysts. The catalysts are prepared by doping MgO- and CeO2-based solids with oxides from alkali (Li2O), alkaline earth (CaO), and transition metal groups (WO3 or MnO). The presence of the peroxide (O2-2) active sites on the Li2O2, revealed by Raman spectroscopy, may be the key factor in the enhanced performance of some of the Li2O/MgO catalysts. The high reducibility of the CeO2 catalyst, an important factor in the CO2-OCM catalyst activity, may be enhanced by the presence of manganese oxide species. The manganese oxide species increases oxygen mobility and oxygen vacancies in the CeO2 catalyst. Raman and Fourier Transform Infra Red (FT-IR) spectroscopies revealed the presence of lattice vibrations of metal-oxygen bondings and active sites in which the peaks corresponding to the bulk crystalline structures of Li2O, CaO, WO3 and MnO are detected. The performance of 5%MnO/15%CaO/CeO2 catalyst is the most potential among the CeO2-based catalysts, although lower than the 2%Li2O/MgO catalyst. The 2%Li2O/MgO catalyst showed the most promising C2+ hydrocarbons selectivity and yield at 98.0% and 5.7%, respectively.展开更多
基金Supported by the Special Fund of the Education Committee of Shaanxi Province (No. 2000K13-G19 and No. 2002K09-G21).
文摘The IR emission spectra of methane were measured under DC glow discharge conditions. The distinct difference in time between methane decomposition and C2 hydrocarbons formation was specially pointed out. C2 hydrocarbons formed at the end of methane decomposition. The optimum condition for C2 hydrocarbon formation was studied and the optimum combination between electric current density and methane input quantity was suggested. The appropriate reaction conditions for methane decomposition and C2 hydrocarbons formation are different, so high yield of C2 hydrocarbons will be probably obtained when different conditions are taken.
基金supported by National Natural Science Foundation of China(Nos.21176175,- 20606023)
文摘Methane conversion has been studied using gliding arc plasma in the presence of argon.The process was conducted at atmospheric pressure and ambient temperature.The focus of this research was to develop a process of converting methane to C2 hydrocarbons and hydrogen. The main parameters,including the CH4/Ar mole ratio,the CH4 flow rate,the input voltage,and the minimum electrode gap,were varied to investigate their effects on methane conversion rate, product distribution,energy consumption,carbon deposit,and reaction stability.The specific energy requirement（SER） was used to express the energy utilization efficiency of the process and provided a practical guidance for optimizing reaction conditions for improving energy efficiency. It was found that the carbon deposition was not conducive to methane conversion,and the gliding arc plasma discharge reached a stable state twelve minutes later.Optimum conditions for methane conversion were suggested.The maximum methane conversion rate of 43.39%was obtained under the optimum conditions.Also,C2 hydrocarbons selectivity,C2 hydrocarbons yield,H2 selectivity, H2 yield and SER were 87.20%,37.83%,81.28%,35.27%,and 2.09 MJ/mol,respectively.
基金supported by the Research Foundation of SINOPEC under the Grant No. 404003the Research Foundation of Tianjin Scientific & Technology Committee under the Grant No. 043182611
文摘The plasma technology served as a tool in unconventional catalysis has been used in natural gas conversion,because the traditional catalytic methane oxidative coupling reaction must be performed at high temperature on account of the stability of methane molecule.The focus of this research is to develop a process of converting methane to C2 hydrocarbons with non-equilibrium plasma technology at room temperature and atmospheric pressure.It was found that methane conversion increased and the selectivity of C2 hydrocarbons decreased with the voltage.The optimum input voltage range was 40-80 V corresponding to high yield of C2 hydrocarbons.Methane conversion decreased and the selectivity of C2 hydrocarbons increased with the inlet flow rate of methane.The proper methane flow rate was 20-40 ml/min （corresponding residence time 10-20 s）.The experimental results show that methane conversion was 47% and the selectivity of C2 hydrocarbons was 40% under the proper condition using atmospheric DBD cold plasma technology.It was found that the breakdown voltage of methane VB was determined by the type of electrode and the discharge gap width in this glow discharge reactor.The breakdown voltage of methane VB,min derived from the Paschen law equation was established.
基金supported by the National Natural Science Fund of China(22121005,22025203)the University of Manchester,and Haihe Laboratory of Sustainable Chemical Transformations,Tianjin。
文摘Adsorptive separation of light hydrocarbons by porous solids provides an energy-efficient alternative to state-of-the-art cryogenic distillation.However,an optimal balance between the cost,performance and stability of the sorbent material is yet to be achieved for industrial applications.Here,we report the efficient separation of C2 and C3 hydrocarbons by a faujasite zeolite(Na-X,Si/Al=1.23).A tandem configuration of two fixed-beds packed with Na-X affords complete dynamic separation of the ternary mixture of C_(2)H_(2)/C_(2)H_(4)/C_(2)H_(6)(1/49.5/49.5;v/v/v)under ambient conditions.Pressure-swing desorption on the latter fixed-bed gives ethylene(>99.50%,1.80 mmol g^(-1))and ethane(>99.99%,1.41 mmol g^(-1)).In situ synchrotron X-ray powder diffraction revealed the binding sites for C_(2)H_(2)and C_(2)H_(4)in Na-X.This study highlights the potential application of commercial zeolites for challenging industrial separations.
文摘This paper deals with thermodynamic chemical equilibrium analysis using the method of direct minimization of Gibbs free energy for all possible CH4 and CO2 reactions. The effects of CO2/CH4 feed ratio, reaction temperature, and system pressure on equilibrium composition, conversion, selectivity and yield were studied. In addition, carbon and no carbon formation regions were also considered at various reaction temperatures and CO2/CH4 feed ratios in the reaction system at equilibrium. It was found that the reaction temperature above 1100 K and CO2/CH4 ratio=1 were favourable for synthesis gas production with H2/CO ratio unity, while carbon dioxide oxidative coupling of methane （CO2 OCM） reaction to produce ethane and ethylene is less favourable thermodynamically. Numerical results indicated that the no carbon formation region was at temperatures above 1000 K and CO2/CH4 ratio larger than 1.
基金supported by National Natural Science Foundation of ChinaDoctoral Foundation of Ministry of Education(20010698007)Returned Scholars Foundation of Ministry of Education(2001[345])
文摘The infrared emission spectra of methane, H, CH and C2 hydrocarbons in natural gas were measured. The process of methane decomposition and C2 hydrocarbons formation was investigated. The experiment showed that the time and conditions of methane decomposition and C2 hydrocarbons formation were different. Methane conversion rate increased with the increase in the current and decrease in the amount of methane. Furthermore, an examination of the reaction mechanisms revealed that free radicals played an important role in the chain reaction.
文摘The catalyst screening tests for carbon dioxide oxidative coupling of methane (CO2-OCM) have been investigated over ternary and binary metal oxide catalysts. The catalysts are prepared by doping MgO- and CeO2-based solids with oxides from alkali (Li2O), alkaline earth (CaO), and transition metal groups (WO3 or MnO). The presence of the peroxide (O2-2) active sites on the Li2O2, revealed by Raman spectroscopy, may be the key factor in the enhanced performance of some of the Li2O/MgO catalysts. The high reducibility of the CeO2 catalyst, an important factor in the CO2-OCM catalyst activity, may be enhanced by the presence of manganese oxide species. The manganese oxide species increases oxygen mobility and oxygen vacancies in the CeO2 catalyst. Raman and Fourier Transform Infra Red (FT-IR) spectroscopies revealed the presence of lattice vibrations of metal-oxygen bondings and active sites in which the peaks corresponding to the bulk crystalline structures of Li2O, CaO, WO3 and MnO are detected. The performance of 5%MnO/15%CaO/CeO2 catalyst is the most potential among the CeO2-based catalysts, although lower than the 2%Li2O/MgO catalyst. The 2%Li2O/MgO catalyst showed the most promising C2+ hydrocarbons selectivity and yield at 98.0% and 5.7%, respectively.
