摘要
随着全球石油资源重质化程度不断加深,常规石油加氢工艺正面临愈发严重的挑战。低温等离子体技术为缓解加氢工艺中高温、高压、催化剂失活等难题提供了新思路。选择1-甲基萘作为重质油模型化合物,在无催化剂的温和条件下研究脉冲介质阻挡放电等离子体加氢的转化规律和反应机理。结果表明:甲基萘在氢气等离子体中容易发生饱和加氢反应,而在甲烷等离子体中则更易发生不饱和加氢反应;增大脉冲电压与脉冲重复频率有利于等离子体甲基萘加氢,但过高会导致加氢反应向裂解反应转变。获得了等离子体甲基萘加氢反应的发射光谱和Hα谱线演化过程,估算气体温度约为350 K,结合密度泛函计算结果推测等离子体甲基萘加氢是H自由基引发的芳香环逐步加氢反应。研究结果为后续等离子体加氢研究提供了参考。
At present,the increasingly inferior quality of global petroleum resources has posed great challenges to the traditional petroleum hydrogenation process.Low-temperature plasma technology provides a new idea for alleviating difficulties such as high temperature,high pressure and catalyst deactivation in the hydrogenation process.In this study,1-methylnaphthalene was selected as the model compound of heavy oil to study the conversion law and reaction mechanism of pulsed dielectric barrier discharge plasma hydrogenation under mild conditions without catalyst.Experimental results show that it is easier for methylnaphthalene to achieve saturation hydrogenation in hydrogen plasma than in methane plasma.Increasing the pulse voltage and pulse repetition frequency is conductive to the methylnaphthalene hydrogenation with plasma,but too high voltage and frequency may convert hydrogenation into cracking reaction.The evolution of emission spectra and Hαspectra line of the methylnaphthalene hydrogenation with plasma was acquired,and the gas temperature was estimated as being about 350 K.In combination with density functional calculations,it is inferred that methylnaphthalene hydrogenation with plasma is a stepwise aromatic ring hydrogenation reaction enabled by H radicals.In conclusion,The research result provides a reference for further plasma hydrogenation research.
作者
范喆
孙昊
张帅
窦立广
韩伟
杨清河
邵涛
FAN Zhe;SUN Hao;ZHANG Shuai;DOU Liguang;HAN Wei;YANG Qinghe;SHAO Tao(Beijing International S&T Cooperation Base for Plasma Science and Energy Conversion,Institute of Electrical Engineering,Chinese Academy of Sciences,Beijing 100190,China;School of Electronic,Electrical and Communication Engineering,University of Chinese Academy of Sciences,Beijing 100049,China;SINOPEC Research Institute of Petroleum Processing Co.,Ltd.,Beijing 100083,China)
出处
《石油学报（石油加工）》
EI
CAS
CSCD
北大核心
2023年第5期1133-1141,共9页
Acta Petrolei Sinica(Petroleum Processing Section)
基金
国家自然科学基金重点项目(51637010)
国家自然科学基金青年项目(52007179)资助
国家杰出青年科学基金项目(51925703)。
关键词
脉冲放电
低温等离子体
加氢
重质油
甲基萘
pulsed discharge
low-temperature plasma
hydrogenation
heavy oil
methylnaphthalene
作者简介
第一作者:范喆,男,博士研究生,从事等离子体重油加工研究,Tel:010-82547193,E-mail:fanzhe@mail.iee.ac.cn;通讯联系人:孙昊,男,助理研究员,博士,从事等离子体能源转化研究,Tel:010-82547193,E-mail:sunhao@mail.iee.ac.cn。
