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甲烷针-板放电与重油加氢耦合形成甲烷转化重油加氢，可实现重油高效加氢并增产高附加值低碳烯烃，有实践应用前景和科学研究意义.建立二维流体模型，对大气压甲烷针-板放电等离子体进行数值模拟，得到电场强度、电子温度和粒子密度的空间与轴向分布，总结反应产额并提炼生成各种带电和中性粒子的关键路径.模拟结果表明，CH3+和CH4+密度与电场强度和电子温度的轴向演化接近且密切相关；CH5+和C2H5+密度沿轴向先增大后减小；CH3与H密度的空间和轴向分布几乎相同；CH2，C2H4与C2H5的粒子密度分布在靠近阴极的区域内明显不同而在正柱区内较为相像；电子与CH4发生电子碰撞电离生成的CH3+和CH4+，CH3+和CH4+分别与CH4发生分子碰撞解离生成C2H5+和CH5+；电子与CH4间的电子碰撞分解是生成CH3，CH2，CH和H的主导反应；CH2与CH4和电子与C2H4发生的反应分别是生成C2H4和C2H2的关键路径；电子与CH4间的电子碰撞分解反应和CH2与CH4发生的反应的产额各占H2总产额的52.15%和47.85%.Methane needle-plane discharge has practical application prospect and scientific research significance since methane conversion heavy oil hydrogenation is formed by coupling methane needle-plane discharge with heavy oil hydrogenation, which can achieve high-efficient heavy oil hydrogenation and increase the yields of high value-added light olefins. In this paper, a two-dimensional fluid model is built up for numerically simulating the methane needle-plane discharge plasma at atmospheric pressure. Spatial and axial distributions of electric intensity, electron temperature and particle densities are obtained. Reaction yields are summarized and crucial pathways to produce various kinds of charged and neutral particles are found out. Simulation results indicate that axial evolutions of CH3+ and CH4+ densities, electric intensity and electron temperature are similar and closely related. The CH5+ and C2H5+ densities first increase and then decrease along the axial direction. The CH3 and H densities have nearly identical spatial and axial distributions. Particle density distributions of CH2, C2H4 and C2H5 are obviously different in the area near the cathode but comparatively resemblant in the positive column region. The CH3+ and CH4+ are produced by electron impact ionizations between electrons and CH4. The CH5+ and C2H5+ are respectively generated by molecular impact dissociations between CH3+ and CH4 and between CH4+ and CH4. Electron impact decomposition between electrons and CH4 is a dominated reaction to produce CH3, CH2, CH and H. The reactions between CH2 and CH4 and between electrons and C2H4 are critical pathways to produce C2H4 and C2H2, respectively. In addition, the yields of electron impact decomposition reactions between electrons and CH4 and reactions between CH2 and CH4 account for 52.15% and 47.85% of total yields of H2 respectively.
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Keywords:
- discharge plasma at atmospheric pressure /
- methane discharge plasma /
- needle-plane discharge /
- fluid model
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[1] Liu C, Chernets I, Ji H, Smith J, Rabinovich A, Dobrynin D, Fridman A 2017 IEEE Trans. Plasma Sci. 45 683
[2] Kang H, Lee D, Kim K, Jo S, Pyun S, Song Y, Yu S 2016 Fuel Process. Technol. 148 209
[3] Bie C D, van Dijk J, Bogaerts A 2015 J. Phys. Chem. C 119 22331
[4] Xu Y, Zhang X, Yang C, Zhang Y, Yin Y 2016 Plasma Sci. Technol. 18 1012
[5] Wang C, Zhang Z, Cui H, Xia W, Xia W 2017 Chin. Phys. B 26 085207
[6] Liu J L, Park H W, Chung W J, Park D W 2016 Plasma Chem. Plasma Proc. 36 437
[7] Zhang Z B, Wu Y, Jia M, Song H M, Sun Z Z, Li Y H 2017 Chin. Phys. B 26 065204
[8] Wang W, Snoeckx R, Zhang X, Cha M S, Bogaerts A Bi Z H, Hong Y, Lei G J, Wang S, Wang Y N, Liu D P 2017 Chin. Phys. B 26 075203
[9] Bi Z H, Hong Y, Lei G J, Wang S, Wang Y N, Liu D P 2017 Chin. Phys. B 26 075203
[10] Zhang D Z, Wang Y H, Wang D Z 2017 Chin. Phys. B 26 065206
[11] Shao T, Wang R X, Zhang C, Yan P 2018 High Voltage 3 14
[12] Gao Y, Zhang S, Liu F, Wang R X, Wang T L, Shao T 2017 Trans. China Electrotechnical Soc. 32 61 (in Chinese)[高远, 张帅, 刘峰, 王瑞雪, 汪铁林, 邵涛 2017 电工技术学报 32 61]
[13] Snoeckx R, Setareh M, Aerts R, Simon P, Maghari A, Bogaerts A 2013 Int. J. Hydrogen Energy 38 16098
[14] Pan J, Li L 2015 J. Phys. D:Appl. Phys. 48 055204
[15] Sun A B, Li H W, Xu P, Zhang G J 2017 Acta Phys. Sin. 66 195101 (in Chinese)[孙安邦, 李晗蔚, 许鹏, 张冠军 2017 物理学报 66 195101]
[16] Pan J, Li L, Wang Y, Xiu X, Wang C, Song Y 2016 Plasma Sci. Technol. 18 1081
[17] Niu Z T, Zhang C, Ma Y F, Wang R X, Chen G Y, Yan P, Shao T 2015 Acta Phys. Sin. 64 195204 (in Chinese)[牛宗涛, 章程, 马云飞, 王瑞雪, 陈根永, 严萍, 邵涛 2015 物理学报 64 195204]
[18] Pan J, Li L, Chen B, Song Y, Zhao Y, Xiu X 2016 Eur. Phys. J. D 70 136
[19] Babaeva N Y, Zhang C, Qiu J, Hou X, Tarasenko V F, Shao T 2017 Plasma Sources Sci. Technol. 26 085008
[20] Yang D P, Li S Y, Jiang Y F, Chen A M, Jin M X 2017 Acta Phys. Sin. 66 115201 (in Chinese)[杨大鹏, 李苏宇, 姜远飞, 陈安民, 金明星 2017 物理学报 66 115201]
[21] Yang W B, Zhou J N, Li B C, Xing T W 2017 Acta Phys. Sin. 66 095201 (in Chinese)[杨文斌, 周江宁, 李斌成, 邢廷文 2017 物理学报 66 095201]
[22] Wang B, Yan W, Ge W, Duan X 2013 Chem. Eng. J. 234 354
[23] Levko D, Raja L L 2017 Plasma Sources Sci. Technol. 26 035003
[24] Yin Z Q, Wang Y, Zhang P P, Zhang Q, Li X C 2016 Chin. Phys. B 25 125203
[25] Wang Q, Yu X L, Wang D Z 2017 Chin. Phys. B 26 035201
[26] Herrebout D, Bogaerts A, Yan M, Gijbels R, Goedheer W, Dekempeneer E 2001 J. Appl. Phys. 90 570
[27] Lefkowitz J K, Guo P, Rousso A, Ju Y 2015 Phil. Trans. R. Soc. 373 20140333
[28] Adamovich I V, Li T, Lempert W R 2015 Phil. Trans. R. Soc. 373 20140336
[29] Takana H, Nishiyama H 2014 Plasma Sources Sci. Technol. 23 034001
[30] Nikiforov A Y, Leys C, Gonzalez M A, Walsh J L 2015 Plasma Sources Sci. Technol. 24 034001
[31] Yao C W, Ma H C, Chang Z S, Li P, Mu H B, Zhang G J 2017 Acta Phys. Sin. 66 025203 (in Chinese)[姚聪伟, 马恒驰, 常正实, 李平, 穆海宝, 张冠军 2017 物理学报 66 025203]
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