Modelling excited species and their role on kinetic pathways in the non-oxidative coupling of methane by dielectric barrier discharge

P-A Maitre; M S Bieniek; Panagiotis Kechagiopoulos

doi:10.1016/j.ces.2020.116399

Modelling excited species and their role on kinetic pathways in the non-oxidative coupling of methane by dielectric barrier discharge

P-A Maitre, M S Bieniek, Panagiotis Kechagiopoulos^* (Corresponding Author)

^*Corresponding author for this work

University of Aberdeen

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

13 Citations (Scopus)

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Abstract

A detailed kinetic scheme for non-thermal methane plasma is developed that considers the reactivity and relaxation of electronically and vibrationally excited species. An atmospheric pressure dielectric barrier discharge reactor for methane non-oxidative coupling is modelled. Via 1D fluid modelling short periods of time are investigated, while for longer periods of time, on the order of the reactor residence time, a combined 1D-0D approach is followed. Modelling results are in good qualitative agreement with literature experiments. Around 86% of the energy input is found to channel into the creation of excited species. The vibrationally excited states of methane exhibit very transient responses due to their rapid formation during electron streamers and fast quenching by VV and VT processes. The, higher energy, electronically excited states are rapidly converted, many of which essentially instantly dissociate. Over 70% of methane’s conversion proceeds via electronical excitation, while the contribution of vibrationally excited states is limited.

Original language	English
Article number	116399
Number of pages	18
Journal	Chemical Engineering Science
Volume	234
Early online date	6 Jan 2021
DOIs	https://doi.org/10.1016/j.ces.2020.116399
Publication status	Published - 28 Apr 2021

Bibliographical note

Acknowledgments
We acknowledge and greatly appreciate the assistance from Dr. Mihailova from Plasma Matters B.V. in working with the software Plasimo and from Dr Marcus Campbell Bannerman from the University of Aberdeen for providing access to the computational cluster used for carrying out the simulations in this work.
The work was supported by the UK Engineering and Physical Sciences Research Council (EPSRC) New Investigator Award, grant no. EP/R031800/1.

Keywords

non-thermal plasma
dielectric barrier discharge
non-oxidative methane coupling
excited states
kinetic modelling
energy channelling

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Accepted author manuscript, 11 MBLicence: CC BY-NC-ND

Cite this

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title = "Modelling excited species and their role on kinetic pathways in the non-oxidative coupling of methane by dielectric barrier discharge",

abstract = "A detailed kinetic scheme for non-thermal methane plasma is developed that considers the reactivity and relaxation of electronically and vibrationally excited species. An atmospheric pressure dielectric barrier discharge reactor for methane non-oxidative coupling is modelled. Via 1D fluid modelling short periods of time are investigated, while for longer periods of time, on the order of the reactor residence time, a combined 1D-0D approach is followed. Modelling results are in good qualitative agreement with literature experiments. Around 86% of the energy input is found to channel into the creation of excited species. The vibrationally excited states of methane exhibit very transient responses due to their rapid formation during electron streamers and fast quenching by VV and VT processes. The, higher energy, electronically excited states are rapidly converted, many of which essentially instantly dissociate. Over 70% of methane{\textquoteright}s conversion proceeds via electronical excitation, while the contribution of vibrationally excited states is limited.",

keywords = "non-thermal plasma, dielectric barrier discharge, non-oxidative methane coupling, excited states, kinetic modelling, energy channelling",

author = "P-A Maitre and Bieniek, {M S} and Panagiotis Kechagiopoulos",

note = "Acknowledgments We acknowledge and greatly appreciate the assistance from Dr. Mihailova from Plasma Matters B.V. in working with the software Plasimo and from Dr Marcus Campbell Bannerman from the University of Aberdeen for providing access to the computational cluster used for carrying out the simulations in this work. The work was supported by the UK Engineering and Physical Sciences Research Council (EPSRC) New Investigator Award, grant no. EP/R031800/1.",

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AU - Maitre, P-A

AU - Bieniek, M S

AU - Kechagiopoulos, Panagiotis

N1 - Acknowledgments We acknowledge and greatly appreciate the assistance from Dr. Mihailova from Plasma Matters B.V. in working with the software Plasimo and from Dr Marcus Campbell Bannerman from the University of Aberdeen for providing access to the computational cluster used for carrying out the simulations in this work. The work was supported by the UK Engineering and Physical Sciences Research Council (EPSRC) New Investigator Award, grant no. EP/R031800/1.

PY - 2021/4/28

Y1 - 2021/4/28

N2 - A detailed kinetic scheme for non-thermal methane plasma is developed that considers the reactivity and relaxation of electronically and vibrationally excited species. An atmospheric pressure dielectric barrier discharge reactor for methane non-oxidative coupling is modelled. Via 1D fluid modelling short periods of time are investigated, while for longer periods of time, on the order of the reactor residence time, a combined 1D-0D approach is followed. Modelling results are in good qualitative agreement with literature experiments. Around 86% of the energy input is found to channel into the creation of excited species. The vibrationally excited states of methane exhibit very transient responses due to their rapid formation during electron streamers and fast quenching by VV and VT processes. The, higher energy, electronically excited states are rapidly converted, many of which essentially instantly dissociate. Over 70% of methane’s conversion proceeds via electronical excitation, while the contribution of vibrationally excited states is limited.

AB - A detailed kinetic scheme for non-thermal methane plasma is developed that considers the reactivity and relaxation of electronically and vibrationally excited species. An atmospheric pressure dielectric barrier discharge reactor for methane non-oxidative coupling is modelled. Via 1D fluid modelling short periods of time are investigated, while for longer periods of time, on the order of the reactor residence time, a combined 1D-0D approach is followed. Modelling results are in good qualitative agreement with literature experiments. Around 86% of the energy input is found to channel into the creation of excited species. The vibrationally excited states of methane exhibit very transient responses due to their rapid formation during electron streamers and fast quenching by VV and VT processes. The, higher energy, electronically excited states are rapidly converted, many of which essentially instantly dissociate. Over 70% of methane’s conversion proceeds via electronical excitation, while the contribution of vibrationally excited states is limited.

KW - non-thermal plasma

KW - dielectric barrier discharge

KW - non-oxidative methane coupling

KW - excited states

KW - kinetic modelling

KW - energy channelling

U2 - 10.1016/j.ces.2020.116399

DO - 10.1016/j.ces.2020.116399

M3 - Article

SN - 0009-2509

VL - 234

JO - Chemical Engineering Science

JF - Chemical Engineering Science

M1 - 116399

ER -

Modelling excited species and their role on kinetic pathways in the non-oxidative coupling of methane by dielectric barrier discharge

Abstract

Bibliographical note

Keywords

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