Optimization of non-thermal plasma-assisted catalytic oxidation for methane emissions abatement as an exhaust aftertreatment technology

Rahman Gholami; Cristina Stere; Sarayute Chansai; Amit Singhania; Alexandre Goguet; Peter Hinde; Paul Millington; Christopher Hardacre

doi:10.1007/s11090-022-10253-3

Optimization of non-thermal plasma-assisted catalytic oxidation for methane emissions abatement as an exhaust aftertreatment technology

Rahman Gholami, Cristina Stere, Sarayute Chansai, Amit Singhania, Alexandre Goguet, Peter Hinde, Paul Millington, Christopher Hardacre^*

^*Corresponding author for this work

School of Chemistry and Chemical Engineering

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

2 Citations (Scopus)

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Abstract

While methane-powered vehicles produce fewer greenhouse gas emissions in comparison to conventional fuel vehicles, there is a significant amount of methane slip in their exhaust that needs to be treated. This study investigates non-thermal plasma (NTP) assisted catalytic methane oxidation as an alternative method for the low temperature methane slip abatement applicable to the exhaust of biogas methane-powered vehicles. It is concluded that high CH₄ conversion and CO₂ selectivity can be obtained using NTP-catalysis at low temperature with Pd/Al₂O₃ found to be the most promising candidate among all catalysts tested. In addition, it was found that CH₄ conversion efficiency was dependent on the feed gas components and gas hourly space velocity as well as how the activation energy is introduced. For example, a combination of plasma and external heat supply provides advantages in terms of CH₄ conversion along with lower plasma energy consumption. The presence of N₂ and O₂ in the feed gas during NTP-catalytic methane oxidation results in unfavourable NO_X formation which linearly increases with CH₄ conversion. These results conclude that the most suitable aftertreatment option involves the combination of an oxidation catalyst with plasma to target the hydrocarbon and CH₄ oxidation, followed by an ammonia-SCR system to convert the NO_X formed in plasma assisted zone.

Original language	English
Pages (from-to)	709-730
Number of pages	22
Journal	Plasma Chemistry and Plasma Processing
Volume	42
Issue number	4
Early online date	12 May 2022
DOIs	https://doi.org/10.1007/s11090-022-10253-3
Publication status	Published - Jul 2022

Bibliographical note

Funding Information:
The authors acknowledge funding from Innovate UK under grant ref: 102661. Open access data can be found via the University of Manchester research portal.

Funding Information:
The authors acknowledge funding from Innovate UK under grant ref: 102661. Open access data can be found via the University of Manchester research portal.

Publisher Copyright:
© 2022, The Author(s).

Keywords

Exhaust gas cleaning
Methane oxidation
NH-SCR
NOx
Pd/AlO
Plasma DBD

ASJC Scopus subject areas

General Chemistry
General Chemical Engineering
Condensed Matter Physics
Surfaces, Coatings and Films

UN SDGs

This output contributes to the following UN Sustainable Development Goals (SDGs)

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Optimization of non-thermal plasma-assisted catalytic oxidation for methane emissions abatement as an exhaust aftertreatment technology
Copyright 2022 the authors. This is an open access article published under a Creative Commons Attribution License (https://creativecommons.org/licenses/by/4.0/), which permits unrestricted use, distribution and reproduction in any medium, provided the author and source are cited.
Final published version, 1.26 MBLicence: CC BY

Cite this

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title = "Optimization of non-thermal plasma-assisted catalytic oxidation for methane emissions abatement as an exhaust aftertreatment technology",

abstract = "While methane-powered vehicles produce fewer greenhouse gas emissions in comparison to conventional fuel vehicles, there is a significant amount of methane slip in their exhaust that needs to be treated. This study investigates non-thermal plasma (NTP) assisted catalytic methane oxidation as an alternative method for the low temperature methane slip abatement applicable to the exhaust of biogas methane-powered vehicles. It is concluded that high CH4 conversion and CO2 selectivity can be obtained using NTP-catalysis at low temperature with Pd/Al2O3 found to be the most promising candidate among all catalysts tested. In addition, it was found that CH4 conversion efficiency was dependent on the feed gas components and gas hourly space velocity as well as how the activation energy is introduced. For example, a combination of plasma and external heat supply provides advantages in terms of CH4 conversion along with lower plasma energy consumption. The presence of N2 and O2 in the feed gas during NTP-catalytic methane oxidation results in unfavourable NOX formation which linearly increases with CH4 conversion. These results conclude that the most suitable aftertreatment option involves the combination of an oxidation catalyst with plasma to target the hydrocarbon and CH4 oxidation, followed by an ammonia-SCR system to convert the NOX formed in plasma assisted zone.",

keywords = "Exhaust gas cleaning, Methane oxidation, NH-SCR, NOx, Pd/AlO, Plasma DBD",

author = "Rahman Gholami and Cristina Stere and Sarayute Chansai and Amit Singhania and Alexandre Goguet and Peter Hinde and Paul Millington and Christopher Hardacre",

note = "Funding Information: The authors acknowledge funding from Innovate UK under grant ref: 102661. Open access data can be found via the University of Manchester research portal. Funding Information: The authors acknowledge funding from Innovate UK under grant ref: 102661. Open access data can be found via the University of Manchester research portal. Publisher Copyright: {\textcopyright} 2022, The Author(s).",

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AU - Gholami, Rahman

AU - Stere, Cristina

AU - Chansai, Sarayute

AU - Singhania, Amit

AU - Goguet, Alexandre

AU - Hinde, Peter

AU - Millington, Paul

AU - Hardacre, Christopher

N1 - Funding Information: The authors acknowledge funding from Innovate UK under grant ref: 102661. Open access data can be found via the University of Manchester research portal. Funding Information: The authors acknowledge funding from Innovate UK under grant ref: 102661. Open access data can be found via the University of Manchester research portal. Publisher Copyright: © 2022, The Author(s).

PY - 2022/7

Y1 - 2022/7

N2 - While methane-powered vehicles produce fewer greenhouse gas emissions in comparison to conventional fuel vehicles, there is a significant amount of methane slip in their exhaust that needs to be treated. This study investigates non-thermal plasma (NTP) assisted catalytic methane oxidation as an alternative method for the low temperature methane slip abatement applicable to the exhaust of biogas methane-powered vehicles. It is concluded that high CH4 conversion and CO2 selectivity can be obtained using NTP-catalysis at low temperature with Pd/Al2O3 found to be the most promising candidate among all catalysts tested. In addition, it was found that CH4 conversion efficiency was dependent on the feed gas components and gas hourly space velocity as well as how the activation energy is introduced. For example, a combination of plasma and external heat supply provides advantages in terms of CH4 conversion along with lower plasma energy consumption. The presence of N2 and O2 in the feed gas during NTP-catalytic methane oxidation results in unfavourable NOX formation which linearly increases with CH4 conversion. These results conclude that the most suitable aftertreatment option involves the combination of an oxidation catalyst with plasma to target the hydrocarbon and CH4 oxidation, followed by an ammonia-SCR system to convert the NOX formed in plasma assisted zone.

AB - While methane-powered vehicles produce fewer greenhouse gas emissions in comparison to conventional fuel vehicles, there is a significant amount of methane slip in their exhaust that needs to be treated. This study investigates non-thermal plasma (NTP) assisted catalytic methane oxidation as an alternative method for the low temperature methane slip abatement applicable to the exhaust of biogas methane-powered vehicles. It is concluded that high CH4 conversion and CO2 selectivity can be obtained using NTP-catalysis at low temperature with Pd/Al2O3 found to be the most promising candidate among all catalysts tested. In addition, it was found that CH4 conversion efficiency was dependent on the feed gas components and gas hourly space velocity as well as how the activation energy is introduced. For example, a combination of plasma and external heat supply provides advantages in terms of CH4 conversion along with lower plasma energy consumption. The presence of N2 and O2 in the feed gas during NTP-catalytic methane oxidation results in unfavourable NOX formation which linearly increases with CH4 conversion. These results conclude that the most suitable aftertreatment option involves the combination of an oxidation catalyst with plasma to target the hydrocarbon and CH4 oxidation, followed by an ammonia-SCR system to convert the NOX formed in plasma assisted zone.

KW - Exhaust gas cleaning

KW - Methane oxidation

KW - NH-SCR

KW - NOx

KW - Pd/AlO

KW - Plasma DBD

U2 - 10.1007/s11090-022-10253-3

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VL - 42

SP - 709

EP - 730

JO - Plasma Chemistry and Plasma Processing

JF - Plasma Chemistry and Plasma Processing

IS - 4

ER -

Optimization of non-thermal plasma-assisted catalytic oxidation for methane emissions abatement as an exhaust aftertreatment technology

Abstract

Bibliographical note

Keywords

ASJC Scopus subject areas

UN SDGs

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