脉冲等离子体驱动CO_(2)加氢制备CH_(3)OH电学参数调控对转化特性的影响  

Effect of Electrical Parameters on Conversion Characteristics of CO_(2) Hydrogenation to CH_(2)OH by Pulsed Plasma

作　　者：杜军[1] 李嘉聪 高远[2] 窦立广 潘杰[1] 邵涛[2,3] DU Jun;LI Jiacong;GAO Yuan;DOU Liguang;PAN Jie;SHAO Tao(School of Physics and Electronic,Shandong Normal University,Jinan 250014,China;Beijing International S&T Cooperation Base for Plasma Science and Energy Conversion,Institute of Electrical Engineering,Chinese Academy of Sciences,Beijing 100190,China;University of Chinese Academy of Sciences,Beijing 100049,China)

机构地区：[1]山东师范大学物理与电子科学学院,济南250014 [2]中国科学院电工研究所等离子体科学和能源转化北京市国际科技合作基地,北京100190 [3]中国科学院大学,北京100049

出　　处：《高电压技术》2023年第8期3275-3285,共11页High Voltage Engineering

基　　金：国家重点研发计划(2021YFE0114700);国家自然科学基金(51925703);山东省自然科学基金(ZR2022ME037)。

摘　　要：化石燃料的大量燃烧带来的CO_(2)排放导致的极端环境问题日益严重,因此,开发温和、原位的CO_(2)转化技术路线有助于实现我国“双碳”目标。为此在无催化剂条件下利用纳秒脉冲介质阻挡放电等离子体驱动CO_(2)加氢制备CH_(3)OH,主要研究了脉冲参数,即脉宽、电压幅值、脉冲上下沿对反应体系中电学特性和转化特性的影响,并讨论了其反应机理。实验结果表明,反应物转化率和产物分布与电场变化密切相关。在缺省参数设置下,随着脉宽的增大,反应物转化率不断升高,在脉宽为2500 ns时CO_(2)、H_(2)转化率分别达到最大值6.8%、3.1%;此外,脉冲上下沿的减小有利于液体产物的生成,当脉冲上升沿从500 ns减小至100 ns,总液体选择性达到最大值38.4%;当脉冲下降沿从500 ns减小至100 ns,CH_(3)OH选择性达到最大值31.8%。该研究结果为等离子体驱动CO_(2)加氢制备CH_(3)OH的转化效果优化提供了研究借鉴。The CO_(2) emissions from the massive burning of fossil fuels result in increasingly serious environmental issues,thus the development of mild and in-situ technology routes for CO_(2) conversion will contribute to achieving China’s“Du-al-Carbon”target.In this paper,the CO_(2) hydrogenation to CH_(3)OH by nanosecond pulsed dielectric barrier discharge plasma under catalyst-free conditions are investigated,and the effects of the pulse parameters(pulse width,maximum peak voltage,rising/falling times)on electrical and conversion characteristics as well as the reaction mechanism are fo-cused on.The results show that reactant conversion and product distribution are strongly correlated with electric field variations.The reactants conversion increases with increasing pulse width under the reference condition,reaching the maximum values of 6.8%and 3.1%for CO_(2) and H_(2),respectively,at a pulse width of 2500 ns.Moreover,the reduction of rising time and falling time facilitates the generation of liquid products.The total liquid selectivity reaches a maximum of 38.4%when the rising time decreases from 500 ns to 100 ns.The maximum CH_(3)OH selectivity is 31.8%when the falling time decreases from 500 ns to 100 ns.These results provide a reference for optimizing the conversion effect of plas-ma-driven CO_(2) hydrogenation into CH_(3)OH.

关 键 词：纳秒脉冲 介质阻挡放电 CO_(2)加氢 合成醇 脉冲参数 

分 类 号：TQ223.121[化学工程—有机化工]