Investigation of the Mechanisms Underpinning Plasma-Catalyst Interaction for the Conversion of Methane to Oxygenates

Jingkai Jiang; Peter J. Bruggeman

doi:10.1007/s11090-022-10251-5

Investigation of the Mechanisms Underpinning Plasma-Catalyst Interaction for the Conversion of Methane to Oxygenates

Jingkai Jiang
, Peter J. Bruggeman

Mechanical Engineering

Research output: Contribution to journal › Article › peer-review

3 Scopus citations

Abstract

Plasma catalysis is a promising approach to further enhance the conversion of methane into value-added products such as methanol. In this work, the mechanisms enabling the conversion of methane to CO, CO₂ and methanol enabled by plasma-enhanced catalysis were investigated. A catalyst reactor was incorporated downstream of the plasma jet to enable the separation between plasma generation and the catalyst bed. An enhancement in CH₃OH and CO₂ production was observed for the shortest distance between the plasma and catalyst compared to the plasma-only case. Plasma-enabled gas heating was shown not to be responsible for the observed synergy while a gas temperature increase as low as 30–40 K significantly impacted desorption rates of CH₃OH/C₂H₅OH on alumina particles. Correlations between molecular beam mass spectrometry (MBMS) measurements at the inlet and outlet of the catalytic reactor suggest that the observed synergistic effect was caused by radical species most likely the CH₃O₂ radical. This study shows that surface reactions induced by radicals such as alkylperoxy radicals might play an important role in surface reactions in plasma-catalysis.

Original language	English (US)
Pages (from-to)	689-707
Number of pages	19
Journal	Plasma Chemistry and Plasma Processing
Volume	42
Issue number	4
DOIs	https://doi.org/10.1007/s11090-022-10251-5
State	Published - Jul 2022

Bibliographical note

Funding Information:
This material is based upon work supported by the National Science Foundation (CBET 1703439). The work has significantly benefited from methods and techniques developed in the framework of work supported by the US Department of Energy, Office of Science, Office of Fusion Energy Sciences General Plasma Science program under Award Number DE-SC0020232 and DE-SC0001939.

Publisher Copyright:
© 2022, The Author(s), under exclusive licence to Springer Science+Business Media, LLC, part of Springer Nature.

Keywords

APPJ
Molecular beam mass spectrometry
Oxygenates
Partial oxidation of methane

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title = "Investigation of the Mechanisms Underpinning Plasma-Catalyst Interaction for the Conversion of Methane to Oxygenates",

abstract = "Plasma catalysis is a promising approach to further enhance the conversion of methane into value-added products such as methanol. In this work, the mechanisms enabling the conversion of methane to CO, CO2 and methanol enabled by plasma-enhanced catalysis were investigated. A catalyst reactor was incorporated downstream of the plasma jet to enable the separation between plasma generation and the catalyst bed. An enhancement in CH3OH and CO2 production was observed for the shortest distance between the plasma and catalyst compared to the plasma-only case. Plasma-enabled gas heating was shown not to be responsible for the observed synergy while a gas temperature increase as low as 30–40 K significantly impacted desorption rates of CH3OH/C2H5OH on alumina particles. Correlations between molecular beam mass spectrometry (MBMS) measurements at the inlet and outlet of the catalytic reactor suggest that the observed synergistic effect was caused by radical species most likely the CH3O2 radical. This study shows that surface reactions induced by radicals such as alkylperoxy radicals might play an important role in surface reactions in plasma-catalysis.",

keywords = "APPJ, Molecular beam mass spectrometry, Oxygenates, Partial oxidation of methane",

author = "Jingkai Jiang and Bruggeman, \{Peter J.\}",

note = "Funding Information: This material is based upon work supported by the National Science Foundation (CBET 1703439). The work has significantly benefited from methods and techniques developed in the framework of work supported by the US Department of Energy, Office of Science, Office of Fusion Energy Sciences General Plasma Science program under Award Number DE-SC0020232 and DE-SC0001939. Publisher Copyright: {\textcopyright} 2022, The Author(s), under exclusive licence to Springer Science+Business Media, LLC, part of Springer Nature.",

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doi = "10.1007/s11090-022-10251-5",

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T1 - Investigation of the Mechanisms Underpinning Plasma-Catalyst Interaction for the Conversion of Methane to Oxygenates

AU - Jiang, Jingkai

AU - Bruggeman, Peter J.

N1 - Funding Information: This material is based upon work supported by the National Science Foundation (CBET 1703439). The work has significantly benefited from methods and techniques developed in the framework of work supported by the US Department of Energy, Office of Science, Office of Fusion Energy Sciences General Plasma Science program under Award Number DE-SC0020232 and DE-SC0001939. Publisher Copyright: © 2022, The Author(s), under exclusive licence to Springer Science+Business Media, LLC, part of Springer Nature.

PY - 2022/7

Y1 - 2022/7

N2 - Plasma catalysis is a promising approach to further enhance the conversion of methane into value-added products such as methanol. In this work, the mechanisms enabling the conversion of methane to CO, CO2 and methanol enabled by plasma-enhanced catalysis were investigated. A catalyst reactor was incorporated downstream of the plasma jet to enable the separation between plasma generation and the catalyst bed. An enhancement in CH3OH and CO2 production was observed for the shortest distance between the plasma and catalyst compared to the plasma-only case. Plasma-enabled gas heating was shown not to be responsible for the observed synergy while a gas temperature increase as low as 30–40 K significantly impacted desorption rates of CH3OH/C2H5OH on alumina particles. Correlations between molecular beam mass spectrometry (MBMS) measurements at the inlet and outlet of the catalytic reactor suggest that the observed synergistic effect was caused by radical species most likely the CH3O2 radical. This study shows that surface reactions induced by radicals such as alkylperoxy radicals might play an important role in surface reactions in plasma-catalysis.

AB - Plasma catalysis is a promising approach to further enhance the conversion of methane into value-added products such as methanol. In this work, the mechanisms enabling the conversion of methane to CO, CO2 and methanol enabled by plasma-enhanced catalysis were investigated. A catalyst reactor was incorporated downstream of the plasma jet to enable the separation between plasma generation and the catalyst bed. An enhancement in CH3OH and CO2 production was observed for the shortest distance between the plasma and catalyst compared to the plasma-only case. Plasma-enabled gas heating was shown not to be responsible for the observed synergy while a gas temperature increase as low as 30–40 K significantly impacted desorption rates of CH3OH/C2H5OH on alumina particles. Correlations between molecular beam mass spectrometry (MBMS) measurements at the inlet and outlet of the catalytic reactor suggest that the observed synergistic effect was caused by radical species most likely the CH3O2 radical. This study shows that surface reactions induced by radicals such as alkylperoxy radicals might play an important role in surface reactions in plasma-catalysis.

KW - APPJ

KW - Molecular beam mass spectrometry

KW - Oxygenates

KW - Partial oxidation of methane

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Investigation of the Mechanisms Underpinning Plasma-Catalyst Interaction for the Conversion of Methane to Oxygenates

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