Quantitative behavior of non-equilibrium excitation by direct electron impact in low-temperature dry reforming of methane was investigated by integrated studies of experimental validation and kinetic modeling.A plasma...Quantitative behavior of non-equilibrium excitation by direct electron impact in low-temperature dry reforming of methane was investigated by integrated studies of experimental validation and kinetic modeling.A plasma chemistry kinetic mechanism incorporating the reactions involving vibrational excitation of CH4,CO2,H2 and CO molecules as well as the low temperature He/CH4/CO2 conversion pathways was developed and validated.The calculation results showed that at lower E/N values(<150 Td)large population of energized electrons generated in a He/CH4/CO2 discharge resulted in an intensification of vibrational excitation.Despite the large generation of vibration,the vibrationally excited molecules in a 0.5/0.25/0.25 of He/CH4/CO2 discharge mixture were easy to relax,due to the strong coupling of the vibration of different molecules in a gas mixture.The results showed that the moderate levels of the vibrational excitation,such as CO2(v10,11,...,18)and CO(v9,10),presented most efficient in the stimulation of species generation including CO,CH2 O,CH3 OH,C2 H4 and C2 H6.Specifically,under conditions of E/N of 108 Td,14.9%of CO formation was estimated from the recombination of CO2(v)with CH3 and H,CO2(v)+CH3→CH3 O+CO,CO2(v)+H→CO+OH.Also,4.8%of C2 H4 formation was from the recombination reaction CH4(v)+CH→C2 H4+H.These results highlight the strong roles of vibrational states in a complex plasma chemistry system.展开更多
基金supported by the National Natural Science Foundation of China(Grant No.21676024)the Beijing Natural Science Foundation(Grant No.3182029)。
文摘Quantitative behavior of non-equilibrium excitation by direct electron impact in low-temperature dry reforming of methane was investigated by integrated studies of experimental validation and kinetic modeling.A plasma chemistry kinetic mechanism incorporating the reactions involving vibrational excitation of CH4,CO2,H2 and CO molecules as well as the low temperature He/CH4/CO2 conversion pathways was developed and validated.The calculation results showed that at lower E/N values(<150 Td)large population of energized electrons generated in a He/CH4/CO2 discharge resulted in an intensification of vibrational excitation.Despite the large generation of vibration,the vibrationally excited molecules in a 0.5/0.25/0.25 of He/CH4/CO2 discharge mixture were easy to relax,due to the strong coupling of the vibration of different molecules in a gas mixture.The results showed that the moderate levels of the vibrational excitation,such as CO2(v10,11,...,18)and CO(v9,10),presented most efficient in the stimulation of species generation including CO,CH2 O,CH3 OH,C2 H4 and C2 H6.Specifically,under conditions of E/N of 108 Td,14.9%of CO formation was estimated from the recombination of CO2(v)with CH3 and H,CO2(v)+CH3→CH3 O+CO,CO2(v)+H→CO+OH.Also,4.8%of C2 H4 formation was from the recombination reaction CH4(v)+CH→C2 H4+H.These results highlight the strong roles of vibrational states in a complex plasma chemistry system.
