Production of Methyl Radicals in Atmospheric Pressure Microreactors for Up-Conversion to High Values Hydrocarbons

S. Kerketta, K. Wolf, R. Hartman, M. Kushner
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Abstract

The on-site up-conversion of methane (CH 4 ) to higher value hydrocarbons is being investigated as a means to minimize the emission of global warming methane during oil production. One proposed method is production of methyl (CH 3 ) radials by a low temperature plasma, followed by reaction with organic metallic complexes in solution. Production of CH 3 radicals using dielectric barrier discharge (DBD) plasma microreactors is being computationally and experimentally investigated. A typical microreactor consists of a 500 μm gap etched on a Si substrate and covered with borosilicate glass as the dielectric. Nanosecond high voltage pulses of up to 10 kV operating at frequencies of 1-10 kHz were used to generate atmospheric pressure plasma in the feed gas consisting of mixtures of Ar and CH 4 . nonPDPSIM , a 2D plasma hydrodynamics model was used to simulate the plasma generation and subsequent plasma chemistry initiated by electron impact dissociation of CH 4 . The spatial and temporal evolution of CH 3 radicals will be discussed as a function of reactor geometry, gas mixture, and solvent location (e.g., along walls or in droplets). Although methyl radicals can be efficiently produced, there is also rapid formation of ethylene (C 2 H 6 ) in the gas phase. The location of CH 3 formation with respect to the solvent is therefore important in maximizing the solvation of the CH 3 radicals for further up-conversion.
常压微反应器上转化高值烃甲基自由基的产生
目前正在研究将甲烷(ch4)就地转化为更高价值的碳氢化合物,以减少石油生产过程中温室气体甲烷的排放。提出的一种方法是通过低温等离子体生产甲基(ch3)径向,然后在溶液中与有机金属配合物反应。利用介质阻挡放电(DBD)等离子体微反应器对ch3自由基的产生进行了计算和实验研究。典型的微反应器是在硅衬底上蚀刻一个500 μm的缝隙,并用硼硅酸盐玻璃作为介质覆盖。利用频率为1-10 kHz的高达10 kV的纳秒高压脉冲,在由Ar和ch4组成的原料气中产生大气压等离子体。利用二维等离子体流体动力学模型nonPDPSIM模拟了ch4电子冲击解离引发的等离子体生成和随后的等离子体化学过程。ch3自由基的时空演变将作为反应器几何形状、气体混合物和溶剂位置(例如,沿壁或在液滴中)的函数进行讨论。虽然甲基自由基可以有效地产生,但在气相中也会迅速形成乙烯(c2h6)。因此,相对于溶剂,ch3形成的位置对于最大化ch3自由基的溶剂化以进一步上转化是很重要的。
本文章由计算机程序翻译,如有差异,请以英文原文为准。
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