脉冲介质阻挡放电等离子体催化CH<sub>4</sub>直接转化

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摘要研究了微秒脉冲和纳秒脉冲介质阻挡放电等离子体CH₄转化过程。对比了两种脉冲电源激励的CH₄介质阻挡放电等离子体特性,考察了不同脉冲电源激励时重复频率、流速和输入功率对CH₄转化效率及气态产物分布的影响,并对不同实验条件下CH₄转化反应路径的选择进行了分析。实验结果发现,CH₄转化气态产物均以H₂、C₂H₆为主,CH₄转化率和H₂产率随着重复频率的上升而下降,但随流速的增大而减小。相同重复频率和流速条件下,微秒脉冲电源激励时CH₄转化率和H₂产率较高,而纳秒脉冲电源激励时具有能量利用率高的优势。在高重复频率、低流速条件下,在石英管内壁和金属电极上会产生更多的积炭和液态烃,因此导致反应的碳氢平衡降低。微秒脉冲电源激励时,随着输入功率的升高氢气和乙烷选择性下降,纳秒脉冲电源激励时呈现出相反的趋势。

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关键词 ：纳秒脉冲放电, 微秒脉冲放电, 介质阻挡放电, CH4转化, 氢气产率

Abstract：In this paper, plasma catalytic reforming of CH₄ is carried out by both microsecond- pulse and nanosecond-pulse dielectric barrier discharges (DBDs). Characteristics of DBD plasma for microsecond-pulse and nanosecond-pulse had been compared. Effects of pulse repetition rate, CH₄ flow rate and input power on the convention rate of CH₄ and distribution of gaseous products are investigated. Moreover, the corresponding selection of chemical reaction paths is analyzed. The results show that main parts of the gaseous products are H₂ and C₂H₆. The conversion rate of CH₄ and the yield of hydrogen increase with the pulse repetition rate, but they decrease with the CH₄ flow rate. Furthermore, the conversion rate of CH₄ and the yield of hydrogen are high for microsecond-pulse DBD when the pulse repetition rate and the CH₄ flow rate are fixed. The energy efficiency in the case of nanosecond-pulse DBD is higher than that in the case of microsecond-pulse DBD. In addition, coking and liquid hydrocarbons appear on the quartz tube and inner electrode at the conditions of high pulse repetition rate and low CH₄ flow rate, leading to the reduction of C&H balance. The selectivities of H₂ and C₂H₆ decreases with the increase of the input power in the case of microsecond-pulse DBD, while they increase with the input power in the case of nanosecond-pulse DBD.

Key words： Nanosecond pulsed discharge microsecond pulsed discharge dielectric barrier discharge methane conversion hydrogen production rate

收稿日期: 2016-06-03 出版日期: 2017-02-08

PACS:

O461

基金资助:国家自然科学基金中英人才基金（51561130156）、青年基金（51507169）和英国皇家学会牛顿高级学者基金（NA140303）资助项目

作者简介: 高远男,1991年生,硕士,研究方向为化学工艺。E-mail: gaoyuan@mail.iee.ac.cn;邵涛男,1977年生,博士,研究员,博士生导师,研究方向为高电压技术、放电等离子体应用等。E-mail: st@mail.iee.ac.cn（通信作者）

引用本文:

高远, 张帅, 刘峰, 王瑞雪, 汪铁林, 邵涛. 脉冲介质阻挡放电等离子体催化CH₄直接转化[J]. 电工技术学报, 2017, 32(2): 61-69. Gao Yuan, Zhang Shuai, Liu Feng, Wang Ruixue, Wang Tielin, Shao Tao. Plasma Enhanced CH₄ Direct Conversion in Pulsed Dielectric Barrier Discharges. Transactions of China Electrotechnical Society, 2017, 32(2): 61-69.

链接本文:

https://dgjsxb.ces-transaction.com/CN/Y2017/V32/I2/61

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