纳秒脉冲介质阻挡放电等离子体驱动CH<sub>4</sub>-CH<sub>3</sub>OH转化制备液态化学品的特性研究

doi:10.19595/j.cnki.1000-6753.tces.210679

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摘要开发非合成气路线的CH₄-CH₃OH直接制取高碳液态化学品转化技术可有效规避传统工业中面临的高危反应条件、废水排放、原子经济性低等问题。该文以CH₄、CH₃OH为原料,采用纳秒脉冲放电等离子体驱动CH₄-CH₃OH直接合成C₂-C₄液态产品,主要探究了Ar添加和脉冲上升沿、下降沿对CH₄-CH₃OH放电中电学特性和转化特性的影响,并进行机理探究。实验结果表明,CH₄-CH₃OH-H₂O体系实验的主要气态产品为H₂、CO、C₂H₆和C₃H₈,主要液态产品为C₂H₅OH、C₃H₇OH。总流速固定时,Ar添加后产生的彭宁电离有利于液态产品的生成,总液体选择性最高为16.4%;在电压和频率固定时,变化六种不同的上升沿、下降沿条件,发现较大的上升沿、下降沿有利于液态产品的生成,当上升沿、下降沿为500ns时,总液体选择性为14.7%。

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关键词 ：纳秒脉冲, 介质阻挡放电, 甲烷转化, 等离子体化学

Abstract：The direct one-step conversion of CH₃OH with CH₄ into value-added liquid chemicals could avoid the problems (harsh reaction conditions, industrial effluent and low atomic economy) that are usually engaged in industrial production. In this paper, CH₄ and CH₃OH are used to directly synthesize C₂-C₄ liquid products by nanosecond pulsed dielectric barrier discharge.The effects of Ar dilution, pulse rising and falling time on the electrical characteristics and conversion are investigated, and the reaction mechanism is also discussed.The results show that the main gaseous products are H₂, CO, C₂H₆, C₃H₈, while the main liquid products are C₂H₅OH and C₃H₇OH. Penning ionization induced by Ar dilution is favorable for the liquid formation, which the highest total liquid selectivity is 16.4%.It is found that the larger rising&falling time could enhance the liquid formation with the fixed voltage and frequency. When the rising&falling timeare 500ns, the total liquid selectivity achieves 14.7%.

Key words： Nanosecond pulse dielectric barrier discharge (DBD) methane conversion plasma chemistry

收稿日期: 2021-05-14

PACS:	O461
	O461.2+5
	O646.9

基金资助:国家自然科学基金资助项目（51925703, 51637010, 51807190, 21908219）

通讯作者: 高远男,1991年生,博士研究生,助理研究员,研究方向为等离子体能源转化。E-mail：gaoyuan@mail.iee.ac.cn

作者简介: 黑雪婷女,1997年生,硕士研究生,研究方向为高压放电与等离子体技术应用。E-mail：heixueting@mail.iee.ac.cn

引用本文:

黑雪婷, 高远, 窦立广, 李江伟, 陈根永, 邵涛. 纳秒脉冲介质阻挡放电等离子体驱动CH₄-CH₃OH转化制备液态化学品的特性研究[J]. 电工技术学报, 2022, 37(15): 3941-3950. Hei Xueting, Gao Yuan, Dou Liguang, Li Jiangwei, Chen Genyong, Shao Tao. Study on Plasma Enhanced CH₄-CH₃OH Conversion to Liquid Chemicals by Nanosecond Pulsed Dielectric Barrier Discharge. Transactions of China Electrotechnical Society, 2022, 37(15): 3941-3950.

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