AC Plasmas Directly Excited in Liquid-Phase Hydrocarbons for H<sub>2</sub> and Unsaturated C<sub>2</sub> Hydrocarbon Production

AC plasmas directly excited within liquid hydrocarbons were investigated for the production of hydrogen and unsaturated C<sub>2</sub> hydrocarbon in a recirculating liquid "jet" flow configuration. Arc discharges were excited at two different frequencies (60 Hz and 17.3 kHz) in C<sub>6</sub>-C<sub>8</sub> hydrocarbons (hexane, cyclohexane, benzene, toluene, and xylene) to produce H<sub>2</sub>, C<sub>2</sub>H<sub>4</sub>, C<sub>2</sub>H<sub>2</sub>, and CH<sub>4</sub>, along with liquid and solid carbon byproducts. AC frequency was seen to modify the plasma properties and gas bubble formation dynamics, significantly influencing the efficiency and reaction pathway. Higher discharge frequency increased energy efficiency more than 2-fold by minimizing thermal losses and favored the production of hydrogenated compounds due to shorter reactant-plasma contact times. Further optimization of hexane conversion was achieved by introducing fluid flow around the plasma electrodes, which led to competitively low specific energy requirements (SERs) of 3.2 kWh/kg C<sub>2</sub>H<sub>4</sub>, 4.9 kWh/kg C<sub>2</sub>H<sub>2</sub>, and 24.3 kWh/kg H<sub>2</sub>. The effect of hydrocarbon feed chemistry was analyzed, showing that hexane and cyclohexane are preferable for C<sub>2</sub> hydrocarbon syntheses, whereas aromatic hydrocarbons produce more H<sub>2</sub>. Gas bubble dynamics and liquid/solid products were analyzed using high-speed imaging, optical emission spectroscopy (OES), gas chromatography-mass spectrometry (GC-MS), scanning electron microscopy/transmission electron microscopy (SEM/TEM), and Raman spectroscopy. This work contributes to the understanding of plasma conversion mechanisms within liquids and demonstrates the potential for the energy-efficient transformation of hydrocarbons with plasma in unique reaction environments.

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Publication Details

Journal
Journal of the American Chemical Society
Published
2024-12-20
DOI
https://doi.org/10.1021/jacs.4c11174
Citations
5
Primary Topic
Electrohydrodynamics and Fluid Dynamics
Type
article
Field-Weighted Citation Impact
1.04

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article

AC Plasmas Directly Excited in Liquid-Phase Hydrocarbons for H2 and Unsaturated C2 Hydrocarbon Production

Norleakvisoth Lim, Michael J. Gordon, Eric W. McFarland
5 citations
Journal of the American Chemical Society
Electrohydrodynamics and Fluid Dynamics
1.04
article

AC Plasmas Directly Excited in Liquid-Phase Hydrocarbons for H2 and Unsaturated C2 Hydrocarbon Production

Norleakvisoth Lim, Michael J. Gordon, Eric W. McFarland
article en
5 citations

Abstract

AC plasmas directly excited within liquid hydrocarbons were investigated for the production of hydrogen and unsaturated C<sub>2</sub> hydrocarbon in a recirculating liquid "jet" flow configuration. Arc discharges were excited at two different frequencies (60 Hz and 17.3 kHz) in C<sub>6</sub>-C<sub>8</sub> hydrocarbons (hexane, cyclohexane, benzene, toluene, and xylene) to produce H<sub>2</sub>, C<sub>2</sub>H<sub>4</sub>, C<sub>2</sub>H<sub>2</sub>, and CH<sub>4</sub>, along with liquid and solid carbon byproducts. AC frequency was seen to modify the plasma properties and gas bubble formation dynamics, significantly influencing the efficiency and reaction pathway. Higher discharge frequency increased energy efficiency more than 2-fold by minimizing thermal losses and favored the production of hydrogenated compounds due to shorter reactant-plasma contact times. Further optimization of hexane conversion was achieved by introducing fluid flow around the plasma electrodes, which led to competitively low specific energy requirements (SERs) of 3.2 kWh/kg C<sub>2</sub>H<sub>4</sub>, 4.9 kWh/kg C<sub>2</sub>H<sub>2</sub>, and 24.3 kWh/kg H<sub>2</sub>. The effect of hydrocarbon feed chemistry was analyzed, showing that hexane and cyclohexane are preferable for C<sub>2</sub> hydrocarbon syntheses, whereas aromatic hydrocarbons produce more H<sub>2</sub>. Gas bubble dynamics and liquid/solid products were analyzed using high-speed imaging, optical emission spectroscopy (OES), gas chromatography-mass spectrometry (GC-MS), scanning electron microscopy/transmission electron microscopy (SEM/TEM), and Raman spectroscopy. This work contributes to the understanding of plasma conversion mechanisms within liquids and demonstrates the potential for the energy-efficient transformation of hydrocarbons with plasma in unique reaction environments.

Journal of the American Chemical SocietyVol. 147(1)
University of California, Santa Barbara (US)
National Science Foundation, University of California, Santa Barbara
Openalex Percentile: Top 22%
Electrohydrodynamics and Fluid Dynamics
1.04
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