| 大气压非平衡等离子体甲烷干法重整零维数值模拟 |
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| 引用本文： | 钟旺燊,陈野力,钱沐杨,刘三秋,张家良,王德真.大气压非平衡等离子体甲烷干法重整零维数值模拟[J].物理学报,2021(7):246-258. |
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| 作者姓名： | 钟旺燊 陈野力 钱沐杨 刘三秋 张家良 王德真 |
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| 作者单位： | 南昌大学物理系;大连理工大学物理学院 |
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| 基金项目： | 国家自然科学基金(批准号:12065019,11705080)资助的课题. |
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| 摘 要： | 大气压非平衡等离子体由于其独特的非平衡特性,可为甲烷和二氧化碳稳定温室气体分子活化和重整提供非热平衡和活化环境.本文采用了零维等离子体化学反应动力学模型,考虑了详细的CH4/CO2等离子体化学反应集,重点研究了反应气体CH4/CO2摩尔分数(5%—95%)对大气压非平衡等离子体甲烷干法重整制合成气和重要含氧化合物的影响.首先,给出了进料气体不同体积比时电子密度和温度随时间的演化规律,结果表明初始甲烷摩尔分数的提高有利于获得较高的电子密度和电子温度.随后,讨论了主要自由基和离子数密度在不同的甲烷摩尔分数下随着时间的变化规律,并给出了反应气体的转化率、合成气体和重要含氧化合物的选择性.此外,还明确了合成气和含氧化合物主要生成和损耗的化学反应路径,发现甲基和羟基是合成含氧化合物的关键中间体.最后,归纳总结给出了主要等离子体粒子之间的总体等离子体化学反应流程图.
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| 关 键 词： | 大气压非平衡等离子体 甲烷干法重整 零维等离子体化学反应动力学模型 反应机理 |
Zero-dimensional numerical simulation of dry reforming of methane in atmospheric pressure non-equilibrium plasma |
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| Zhong Wang-Shen,Chen Ye-Li,Qian Mu-Yang,Liu San-Qiu,Zhang Jia-Liang,Wang De-Zhen.Zero-dimensional numerical simulation of dry reforming of methane in atmospheric pressure non-equilibrium plasma[J].Acta Physica Sinica,2021(7):246-258. |
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| Authors: | Zhong Wang-Shen Chen Ye-Li Qian Mu-Yang Liu San-Qiu Zhang Jia-Liang Wang De-Zhen |
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| Affiliation: | (Department of Physics,Nanchang University,Nanchang 330031,China;School of Physics,Dalian University of Technology,Dalian 116024,China) |
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| Abstract: | Recently,atmospheric non-equilibrium plasma has been proposed as a potential and novel type of“reaction carrier”for the activation and conversion of greenhouse gases(methane and carbon dioxide)into value-added chemicals,due to its unique non-equilibrium characteristics.In this paper,a zero-dimensional plasma chemical reaction kinetic model in CH4/CO2 gas mixture is constructed,with an emphasis on reaction mechanism for plasma dry reforming of methane to syngas and oxygenates.Especially,the effect of the CH4 molar fraction(5%–95%)on plasma dry reforming of methane is investigated.First,the time evolution of electron temperature and density with initial methane content is presented,and the results show that both the electron temperature and electron density vary periodically with the applied triangular power density pulse,and the higher initial methane content in gas mixture is favored for a larger electron temperature and density.Subsequently,the time evolution of number densities of free radicals,ions and molecules at different CH4/CO2 molar fraction are given.The higher the initial methane content,the greater the number densities of H,H–,H2,and CH3,leading to insufficient oxygen atoms to participate in the reaction for oxygenates synthesis.The conversions of inlet gases,the selectivities of syngas and important oxygenates are also calculated.The conversion rate of carbon dioxide increases with the increasing methane content,but the conversion rate of methane is insensitive to the variation of methane content.As methane mole fraction is increased from 5%to 95%,the selectivities of important oxygenates(CH3OH and CH2O)are relatively low(<5%),and the selectivity of H2 gradually increases from 13.0%to 24.6%,while the selectivity of CO significantly decreases from 58.9%to 9.7%.Moreover,the dominant reaction pathways governing production and destruction of H2,CO,CH2O and CH3OH are determined,and CH3 and OH radicals are found to be the key intermediate for the production of valuable oxygenates.Finally,a schematic overview of the transformation relationship between dominant plasma species is summarized and shown to clearly reveal intrinsic reaction mechanism of dry reforming of methane in atmospheric nonequilibrium plasma. |
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| Keywords: | atmospheric pressure non-equilibrium plasma dry reforming of methane zero-dimensional chemical reaction kinetic model reaction mechanism |
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