介质阻挡放电等离子体催化甲烷无氧偶联的影响因素优化研究

梁惠民; 张荣斌; 叶闰平; 冯刚

doi:10.12434/j.issn.2097-2547.20250057

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介质阻挡放电等离子体催化甲烷无氧偶联的影响因素优化研究

C1化学与催化转化 | 更新时间：2025-11-25

- 介质阻挡放电等离子体催化甲烷无氧偶联的影响因素优化研究
- Study on optimization of influencing factors of anaerobic methane coupling catalyzed by dielectric barrier discharge plasma
- 低碳化学与化工 2025, 50(11): 1-12.
- 作者机构：
  
  1.南昌大学化学化工学院，江西南昌 330031
  2.南通大学纺织服装学院，江苏南通 226019
- 作者简介：
  
  梁惠民（1997—），硕士研究生，研究方向为工业催化，E-mail： 402800220140@email.ncu.edu.cn。
  叶闰平（1990—），博士，教授，研究方向为多相催化，E-mail： rye@ncu.edu.cn；
  冯刚（1982—），博士，教授，研究方向为工业催化，E-mail： fenggang@ncu.edu.cn。
- 基金信息：
  
  国家自然科学基金(22362022;52267001);江西省“双高”和“赣鄱俊才”项目(20232BCJ25082);江西省“双千计划”(jxsq2023101072)
- DOI：10.12434/j.issn.2097-2547.20250057
  中图分类号： TQ032;TQ039
- 收稿：2025-02-16，
  
  修回：2025-03-12，
  
  纸质出版：2025-11-25
- 稿件说明：
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梁惠民,张荣斌,叶闰平等.介质阻挡放电等离子体催化甲烷无氧偶联的影响因素优化研究[J].低碳化学与化工,2025,50(11):1-12.

LIANG Huimin,ZHANG Rongbin,YE Runping,et al.Study on optimization of influencing factors of anaerobic methane coupling catalyzed by dielectric barrier discharge plasma[J].Low-Carbon Chemistry and Chemical Engineering,2025,50(11):1-12.
梁惠民,张荣斌,叶闰平等.介质阻挡放电等离子体催化甲烷无氧偶联的影响因素优化研究[J].低碳化学与化工,2025,50(11):1-12. DOI： 10.12434/j.issn.2097-2547.20250057.

LIANG Huimin,ZHANG Rongbin,YE Runping,et al.Study on optimization of influencing factors of anaerobic methane coupling catalyzed by dielectric barrier discharge plasma[J].Low-Carbon Chemistry and Chemical Engineering,2025,50(11):1-12. DOI： 10.12434/j.issn.2097-2547.20250057.

摘要

介质阻挡放电（DBD）等离子体催化甲烷（CH

）无氧偶联是实现CH

高效转化制备高附加值碳氢化合物（如C

烃类）的重要途径，但其反应效率受到多因素影响。通过设计系列实验，系统探究了放电功率、温度、气体总流速、辅助气种类和含量（体积分数）等关键参数对CH

转化率及C

烃类选择性的影响规律。实验结果表明，气体总流速是调控反应物停留时间的关键参数，气体总流速增大时，气体在等离子体区的停留时间缩短，导致CH

转化率减小。辅助气种类对反应路径具有显著调控作用，N

作为辅助气时，通过激发高能电子使CH

转化率显著增大，C

烃类产物选择性最大可达40%，而H

作为辅助气时，CH

转化率减小，但通过氢自由基介导的加氢反应使C

选择性增大至90%以上。电极表面微观形貌直接影响放电特性，0.10 mol/L赖氨酸溶液处理电极表面1.0 d后，CH

转化率相比未处理明显增大。上述多参数协同优化机制将为等离子体催化CH

转化反应器

的工程放大提供关键设计准则，深化研究人员对等离子体催化体系作用机制的理论认知。

Abstract

Anaerobic methane (CH

) coupling catalyzed by dielectric barrier discharge (DBD) plasma is a significant pathway for the efficient conversion of CH

into high-value hydrocarbons (such as C

hydrocarbons). However

its reaction efficiency is influenced by multiple factors. Through a series of experiments

the effects of key parameters such as discharge power

temperatures

total gas flow rates

auxiliary gas types and contents (volume fraction

the same below) on CH

conversion rates and C

hydrocarbon selectivities were systematically investigated. The experimental results indicate that total gas flow rate is a critical parameter for controlling the residence time of reactants. When the total gas flow rate increases

the average residence time of the gas in the plasma region shortens

leading to a decrease in CH

conversion rate. Auxiliary gas types significantly regulate the reaction pathway. When N

is used as an auxiliary gas

the CH

conversion rate is significantly increased by exciting high-energy electrons

and the C

hydrocarbon selectivity can reach up to 40%. When H

is used as an auxiliary gas

the CH

conversion rate decreases

but the C

selectivity increases to more than 90% due to hydrogen radical-mediated hydrogenation reactions. The microscopic morphology of the electrode surface directly affects discharge characteristics. After treating the electrode surface with the 0.10 mol/L lysine solution for one day

the CH

conversion rate significantly increases compared to untreated electrodes. The synergistic optimization mechanism of these multiple parameters will provide critical design guidelines for the scale-up of plasma-catalytic CH

conversion reactors and deepen the theoretical understanding of the mechanism in plasma-

catalytic systems.

关键词

Keywords

references

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