纳秒脉冲火花放电高效转化甲烷的实验研究

doi:10.19595/j.cnki.1000-6753.tces.180032

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摘要火花放电是一种气体温度介于电弧放电和介质阻挡放电（DBD）之间的放电形式,具有设备简单、成本较低、转化率高和能量利用效率高等优点,是存在工业化潜力的甲烷高效转化技术。纳秒脉冲放电具有窄脉宽和上升沿,能够提高火花放电等离子体的不平衡程度,降低气体温度,进一步提高甲烷转化能量利用效率。本文研究纳秒脉冲甲烷放电的放电特性和产物分布,实验结果表明在输入能量为170kJ/mol的条件下,甲烷转化率可达60%、氢气选择性和产率分别为44.4%和26.6%、乙炔选择性和产率分别为28.8%和16.8%、总能量利用效率为33.9%、氢气能量利用效率为23%。获得了350~700nm的甲烷等离子发射光谱（OES）,包括H_α、H_β、H_γ氢原子等Balmer谱线和CH、C⁺、C₂等谱线,并利用H_α的Stark展宽效应估算了电子密度约为10¹⁷cm^-3量级。利用ICCD和单色仪获得了电子密度和CH、C₂发射光谱演变过程,实验结果表明电子密度随时间逐渐减少;C⁺几乎仅在外加脉冲时存在,CH仅在外加脉冲结束后出现,说明C⁺主要是由电子碰撞产生的,而C⁺在放电结束后与H发生反应生成CH,CH进一步复合生成C₂H₂。

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关键词 ：甲烷无氧转化, 纳秒脉冲放电, 发射光谱, 电子密度

Abstract：The spark discharge, in which the gas temperature is between arc discharge and dielectric barrier discharge, has a potential for industrial methane conversion due to its high conversion rate, high conversion efficiency and low requirements. Nano-second pulse power source is able to enhance spark performance by short duration and rapid rising time, making plasma more efficient and colder. In this paper, an overall study of nanosecond pulsed spark discharge in methane has been conducted. The results show that the conversion rate of methane is 60%. The selectivity and yield of hydrogen is 44.4% and 26.6%, while those of acetylene are 28.8% and 16.8%, respectively. The total energy efficiency and hydrogen production efficiency are calculated as high as 33.9% and 23% at SEI of 170kJ/mol. Optical emission spectrum (OES) at range of 350~700nm has been recorded, in which H Balmer profiles (such as H_α, H_β, H_γ), CH, C⁺ and C₂ are detected. The electron density has been estimated about 10¹⁷cm^-3 by the Stark effect of H_α. The evolutions of H_α, CH and C₂have been acquired by ICCD and monochromator. The electrons density decreases along with reaction time. C⁺ shows up as long as pulses are exerted, while CH starts to be generated at the end of pulse, which indicates C₂H₂ comes from recombination of CH that derives from H and C⁺.

Key words： Methane non-oxidative conversion nanosecond pulsed spark discharge optical emission spectrum electron density

收稿日期: 2018-01-08 出版日期: 2019-03-01

PACS:	O461
	O539
	O646.9

基金资助:石油化工催化材料与反应工程国家重点实验室（中国石油化工股份有限公司石油化工科学研究院）开放基金课题（33600000-15-zc0607-0001）、国家自然科学基金重点基金（51637010）、青年基金（51507169）、中英人才基金（51561130156）和牛顿高级学者基金（NA140303）资助项目

通讯作者: 邵涛,男,1977年生,研究员,岗位教授,博士生导师,研究方向为高电压技术、脉冲功率技术及放电等离子体应用等。 E-mail: st@mail.iee.ac.cn

作者简介: 孙昊,男,1989年生,博士研究生,研究方向为气体放电与等离子体应用。E-mail: sunhao@mail.iee.ac.cn

引用本文:

孙昊, 张帅, 韩伟, 高远, 王瑞雪, 邵涛. 纳秒脉冲火花放电高效转化甲烷的实验研究[J]. 电工技术学报, 2019, 34(4): 880-888. Sun Hao, Zhang Shuai, Han Wei, Gao Yuan, Wang Ruixue, Shao Tao. An Experimental Investigation of Nanosecond Pulsed Spark Discharge for High-Efficient Methane Conversion. Transactions of China Electrotechnical Society, 2019, 34(4): 880-888.

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