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Temperature Inhibition of Plasma-Driven Methane Conversion in DBD Systems

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Abstract

Low-temperature non-thermal plasmas produce highly reactive chemical environments made up of electrons, ions, radicals, and vibrationally excited molecules. These reactive species, when combined with catalysts, can help drive thermodynamically unfavorable chemical reactions at low temperatures and atmospheric pressure. The conversion of methane (CH4) to produce other value-added chemicals is a good model system because of its applicability to a wide range of industries. To effectively create these plasma catalytic systems, a fundamental understanding of the plasma-phase chemistry alone is imperative. While there have been many studies on methane plasmas and how certain operating conditions (i.e., gas composition and power) affect the plasma, there is limited understanding on how changing bulk reaction temperature affects the plasma properties and ensuing plasma chemistry. In this work, we use a dielectric barrier discharge to investigate the effects of temperature on the reaction chemistry and the plasma’s electrical properties in various methane-gas mixtures. Results show that increasing temperature leads to a reduction in methane conversion as well as changes to both the gas and dielectric material pre-breakdown, which manifests itself in temperature-dependent electrical properties of the plasma. Experiments at various temperatures and power show a positive correlation between key electrical plasma properties (average charge and lifetime per filament) and the measured methane conversion as a function of temperature.

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Data Availability

All data generated during this work are available from the corresponding author upon request.

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Funding

This work was supported by the U.S. Department of Energy by National Energy Technology Laboratory under Award Number DE-FE0031862. F.V. and D.G. also acknowledge ND – UC|Chile Luksic Scholars Joint Research Award.

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Authors and Affiliations

  1. Department of Aerospace and Mechanical Engineering, University of Notre Dame, Notre Dame, IN, 46556, USA

    Ibukunoluwa Akintola, Jinyu Yang & David B. Go

  2. Department of Chemical and Biomolecular Engineering, University of Notre Dame, Notre Dame, IN, 46556, USA

    Gerardo Rivera-Castro, Jeffrey Secrist, Jason C. Hicks & David B. Go

  3. Instituto de Física, Pontificia Universidad Catolica de Chile, Santiago, Region Metropolitana, Chile

    Felipe Veloso

Authors
  1. Ibukunoluwa Akintola
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  2. Gerardo Rivera-Castro
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Contributions

IA and DG designed and analyzed the plasma experiments. JY and JS assisted in acquiring experimental data. IA and FV designed and interpreted the circuit analyses. GR and JH designed and analyzed the methane conversion experiments. IA, GR, and DG wrote the main manuscript text. All authors reviewed the manuscript.

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Correspondence to David B. Go.

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Akintola, I., Rivera-Castro, G., Yang, J. et al. Temperature Inhibition of Plasma-Driven Methane Conversion in DBD Systems. Plasma Chem Plasma Process 43, 1999–2016 (2023). https://doi.org/10.1007/s11090-023-10388-x

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