Numerical Study of Reactive Radical Species Formation in Methane
Plasma Discharge
Khawla MOKRANI1, Ziane KECHIDI2, Abdelatif TAHRAOUI1.
1Quantum Electronics Laboratory, Faculty of Physics, USTHB, Bp, 32 El Alia Bab Ezzouar.
2Laboratory of Electrical Engineering and Automatics, University of Medea, Medea 26000.
khawla.mokranii@gmail.com
Abstract — A unidimensional self-consistent fluid
model for radio-frequency plasma discharges,
capacitively coupled in methane, used as a chemical
reactor for gas conversion, is developed. Poisson’s
equation for the electric field is coupled to the first
moments of the Boltzmann equation (continuity
equation, drift-diffusion equation and energy
equation). Transport and reaction coefficients are
obtained from the mean energy of the electrons. The
model is applied to a reduced methane (CH4) system,
considering the main ionization and excitation
processes, to generate reactive species such as
CH4+ , CH3+ , H, CH3 and CH2 . The detailed discharge
characteristics of the plasma are simulated using the
COMSOL software, which employs multi-physics
field coupling.
Keywords— Reactive species production, RF
plasma modeling, hydrocarbon, atmospheric
pressure, CH4, CH3, H, electron energy distribution.
I. INTRODUCTION
O ver the past few years, non-equilibrium cold
plasmas at atmospheric pressure and relatively
low pressure have become very useful devices for
the production of reactive species[1]–[3]. There are
many applications that benefit from the possibility of
their low temperature. For instance, depollution,
sterilization, medical interventions, and more
recently, flow control or combustion control[4].
Methane, as a primary hydrocarbon, has garnered
significant attention in studies exploring electron-
induced fragmentation processes. It serves as an
important model for more complex hydrocarbons.
Numerous experimental[5]–[27] and theoretical[28]–
[35] investigations have been conducted to
understand the collisions between methane
molecules and electrons. Non-equilibrium discharge
plasma has the ability to convert methane into
valuable chemical reactive components, such as
ions, radicals, and excited species[36], [37].
While previous studies have primarily focused on
elastic processes, providing insights into total and
elastic cross sections, our knowledge regarding
inelastic processes remains incomplete. Limited
reports exist on cross sections related to vibrational
and rotational excitation, and dissociation,
ionization, and electron attachment cross sections
have received relatively less attention.
Therefore, a more comprehensive understanding
of the inelastic processes involved in methane-
electron collisions is still needed. In our project, we
aim to address this gap by focusing on understanding
the properties of non-equilibrium plasmas and the
mechanisms of power transfer from the excitation
source to establish and maintain a homogeneous
discharge, within the context of various applications.
To achieve this objective, we present a one-
dimensional fluid model and report the obtained
results. The discharge is generated between two
electrodes separated by a distance d. We derive a set
of governing equations related to the transport of
charged and neutral species, drift-diffusion
approximation, electron energy equation, and
Poisson's equation from the well-known fluid
approach.
 II. THEORETICAL MODEL 𝜕𝑛𝑝
⃗ ∙ 𝛤⃗ 𝑝 = 𝑆𝑝
+𝛻 (1)
𝜕𝑡
The paper adopts a one-dimensional fluid model
that was originally developed for modeling Silane In these equations, 𝑛𝑝 , 𝛤𝑝 and 𝑆𝑝 stand for the
plasmas[38], [39] and subsequently modified for density, flux and the source term as function of time
methane plasmas[40]. The model employs a particle- and space, is obtained by considering the volume
in-cell method and incorporates the temporal reactions in which species p are produced or lost.
evolution of the electron energy distribution
function, along with its correlation to hydrogen The flux 𝛤𝑝 of each type species p is given by
radical generation. Additionally, the model accounts using the drift-diffusion approximation, in terms of
for the spatial distribution of electron energy and its the mobility and diffusion coefficient:
electron-methane reaction rates. The simulations are
⃗ 𝑝 = ±𝜇𝑝 𝐸
𝛤 ⃗ 𝑛 𝑝 − 𝐷𝑝 𝛻
⃗ 𝑛𝑝 (2)
conducted at a discharge frequency of 13.56 MHz.
For the electrons, the assumption that the energy
Description of the model
is directly related to the local electric field is invalid
The model incorporates mass balance equations because they have much lower mass compared to
for each species, the Poisson equation, and the heavy particles. Its parameters are expressed as a
electron energy equation. The electric field is function of the average energy 𝜀, a balance equation
derived from the Poisson equation, and an effective is solved:
field is utilized since ions are unable to precisely 𝜕(𝑛𝑒 𝜀)
follow the actual RF field[38]. The average electron ⃗ ∙ 𝛤⃗ 𝜀 = 𝑆𝜀
+𝛻 (3)
𝜕𝑡
energy is determined by combining the electron
energy equation and the electron density balance The source term Sε is based on energy gain from the
equation, which vary spatially and temporally within electric field and energy loss due to collisions, in the
the RF cycle. various reactions. It given by:

The electron impact reaction rate coefficients and ⃗𝑒∙𝐸

𝑆𝜀 = −𝑒𝛤 ⃗ − 𝑄𝑒𝑙 − 𝑄𝑖𝑛𝑒𝑙 (4)
electron mobility are parameters that depend on the
electron mean energy. These dependencies are For the so-called heavy particles (ions,
calculated using the BOLSIG+ Boltzmann molecules, radicals) no energy balance equation
solver[41], which obtains electron transport needs to be.
coefficients and collision rate coefficients from more − The electron energy flux can be obtained from:
fundamental cross-section data. The transport
coefficients are then used to calculate the fluxes of 5 5
⃗𝛤𝜀 = − 𝜇𝑒 ⃗𝐸𝑛𝑒 𝜀 − 𝑛𝑒 𝐷𝑒 ⃗𝛻𝜀 (5)
different species (neutrals, radicals, and ions) in the 3 3
drift-diffusion approximation[42]–[44], following Where the first term is the hydrodynamic flux of
equations described in detail in reference[38]–[40]. enthalpy, and the second term is the heat conduction
To compute the electron energy distribution flux.
function (EEDF), a range of electric field values is
− For the charged ions (+ positive or – negative
considered, given a specific density and composition
ions):
of the background gas. This results in combinations
of average electron energies and their corresponding ⃗ 𝑖 = ±𝑛𝑖 𝜇𝑖 𝐸
𝛤 ⃗ − 𝐷𝑖 𝛻
⃗ 𝑛𝑖 (6)
coefficients. The main control equations of this
dynamic plasma model are listed as follows: − For the neutrals:

The particle continuity equation describes the ⃗ 𝑛 = −𝐷𝑛 𝛻

𝛤 ⃗ 𝑛𝑛 (7)
continuity of each type species p:
 These partial differential equations are coupled to Species Included in the Model
the Poisson equation, to obtain the electric field
distribution in the plasma: To characterize the chemical reactions occurring
in a pure methane plasma, our model considers a
⃗ ∙ (𝜀0 𝛻
𝛻 ⃗ 𝜑) = −𝛻
⃗ ∙ (𝜀0 𝐸
⃗ ) = − ∑ 𝑞𝑝 𝑛𝑝 (8) comprehensive set of 35 species, including
𝑝 electrons, molecules, ions, and radicals. The
selection of these species is based on previous
Where 𝜑 is the electric potential as function of modeling investigations of methane discharges
time and space, 𝜀0 is the vacuum permittivity, and conducted under diverse conditions[40], [45], [46].
𝑞𝑝 is the charge of species p. These specific species are chosen because they are
considered relevant and significant in the observed
For all the species described in the model, the
chemistry of such systems. By including this wide
diffusion coefficients and the mobility coefficients
range of species, our model aims to provide a
(only for the charged species) have to be calculated
comprehensive representation of the complex
using the external Boltzmann solver BOLSIG+. The
chemical dynamics that occur within a methane
diffusion coefficients 𝐷𝑖𝑗 for neutral species,
plasma.
including radicals and background neutrals, are
determined using the generalized Einstein relation: TABLE 1-OVERVIEW OF THE DIFFERENT PLASMA SPECIES INCLUDED IN
THE FLUID MODEL FOR A CH4 GAS, BESIDES THE ELECTRONS.

𝑘𝑏 𝑇𝑖 𝑘𝑏 𝑇𝑖
𝐷𝑖 = = 𝜇𝑖 (9) Molecules Ions Radicals
𝑚𝑖 𝜈𝑖 𝑒 CH5+ , CH4+,

In the aforementioned equation, 𝑘𝑏 denotes the 𝐂𝐇𝟒 CH3+ , CH2+, CH3 , CH2 , CH, C

Boltzmann constant, and 𝑇𝑖 , 𝑚𝑖 , 𝜈𝑖 and 𝜇𝑖 denote the CH + , C+

ion temperature, which assumed to be identical to the
C2 H6+ , C2 H5+ ,
temperature of the background gas, mass, ion-
𝑪𝟐 𝐇𝟔, 𝐂𝟐𝐇𝟒, C2 H5 , C2 H3 ,
neutral collision frequency and the ions mobility, C2 H4+ , C2 H3+ ,
respectively. 𝐂𝟐 𝐇 𝟐 , 𝐂𝟐 , 𝐂𝟑 𝐇 𝟖 , 𝐂𝟑 𝐇 𝟔 C2 H, C3 H7 , C3 H5
C2 H2+ , C2 H + , C2+
𝐂𝟒 𝐇 𝟐
Boundary conditions 𝐇𝟐 H3+ , H2+, H + H

The boundary conditions for the various species

in the vicinity of the anode and cathode, are given in
Chemical reactions
the fluid as follows (at x=0, d):

⃗⃗⃗
1
⃗⃗𝑖 ∙ 𝑛) + 𝛼𝑠′ 𝑛𝑒 𝜇𝑒 𝐸,
Upon the application of RF voltage to one of the
𝛤𝑒 ∙ 𝑛 = 𝑛 𝑣 − 𝛼𝑠 ∑ 𝛾𝑖 (𝛤 (10)
4 𝑒 𝑡ℎ,𝑒 symmetrically placed electrodes, electron impact
𝑖

ionization and dissociation of CH4 occur, resulting

1
⃗⃗𝛤𝑖 ∙ 𝑛 = 𝑛 𝑣 − 𝛼𝑠′ 𝑛𝑖 𝜇𝑖 𝐸, (11) in the generation of new species such as electrons,
4 𝑖 𝑡ℎ,𝑖
ions, and radicals. The production of these new
Where i represent the positive ion, 𝛾 is the electrons and ions is crucial for sustaining the
secondary electron emission coefficient, vth,𝑒 and discharge. In RF discharges, electron impact
vth,i are the electron thermal velocity and the ion reactions are primarily responsible for the increased
thermal velocity, in the negative ion species, we formation of radicals. By increasing the RF voltage
have used the Dirichlet boundary. applied across the electrodes while maintaining a
fixed gas pressure and RF frequency, the plasma
1 (𝐸⃗. 𝑛⃗ ≥ 0) 0 (𝐸⃗. 𝑛⃗ ≥ 0)
𝛼𝑠 = { , 𝛼𝑠′ = { (12) density can be effectively increased.
0 (𝐸⃗. 𝑛⃗ < 0) 1 (𝐸⃗ . 𝑛⃗ < 0)
To comprehensively characterize the plasma
chemistry within the discharge gap, a set of 367 gas-
 phase reactions involving 35 distinct species has Dissociation e− + C2 H6 → e− + C2 H5 + H [52], [53]
e− + C2 H6 → e− + C2 H4 + H2 [52], [53]
been developed. These reactions can be classified C2 H5
into four major groups[47]: 100 electron-neutral Ionization e− + C2 H5 → 2e− + C2 H5+ [49]

reactions, 35 electron-ion reactions, 92 neutral- e− + C2 H5 → 2e− + C2 H4+ + H [49]

e− + C2 H5 → 2e− + C2 H3+ + H2 [49]
neutral reactions, and 140 ion-neutral reactions. The e− + C2 H5 → 2e− + C2 H2+ + H2 + H [49]
electron-neutral reactions encompass 6 momentum Dissociation e− + C2 H5 → e− + C2 H4 + H [52], [53]
e− + C2 H5 → e− + C2 H3 + H2
transfer reactions, 15 vibrational excitation C2 H4
reactions, 47 ionization reactions, and 32 Momentum e− + C2 H4 → e− + C2 H4 [48]
dissociation reactions. The electron-ion reactions transfer
Vibr. Exc. e− + C2 H4 → e− + C2 H4 ∗ (2) [48]
specifically involve dissociative recombination Ionization e− + C2 H4 → 2e− + C2 H4+ [49]
reactions, as volume recombination plays a e− + C2 H4 → 2e− + C2 H3+ + H [49]
e− + C2 H4 → 2e− + C2 H2+ + H2 [49]
significant role at atmospheric pressure. Dissociation e− + C2 H4 → e− + C2 H3 + H [52], [53]
e− + C2 H4 → e− + C2 H2 + H2 [52], [53]
TABLE 2- ELECTRON IMPACT REACTIONS WITH THE VARIOUS
MOLECULES AND RADICALS, CONSIDERED IN THIS PLASMA MODEL C2 H3
(VIBR. EXC. STANDS FOR VIBRATIONAL EXCITATION ). Ionization e− + C2 H3 → 2e− + C2 H3+ [49]
e− + C2 H3 → 2e− + C2 H2+ + H [49]
Reaction Chemical Reaction Ref. e− + C2 H3 → 2e− + C2 H + + H2 [49]

CH4 Dissociation e− + C2 H3 → e− + C2 H2 + H [52], [53]

e− + C2 H3 → e− + C2 H + H2 [52], [53]
Momentum e− + CH4 → e− + CH4 [48]
C2 H2
transfer Momentum e− + C2 H2 → e− + C2 H2 [48]
Vibr. Exc. e− + CH4 → e− + CH4∗ (2) [48]
transfer
Ionization e− + CH4 → 2e− + CH4+ [49]
Vibr. Exc. e− + C2 H2 → e− + C2 H2 ∗ (3) [48]
e− + CH4 → 2e− + H + CH3+ [49]
Ionization e− + C2 H2 → 2e− + C2 H2+ [49]
e− + CH4 → 2e− + H2 + CH2+ [49] Dissociation e− + C2 H2 → 2e− + C2 H + H [52], [53]
Dissociation e− + CH4 → e− + H + CH3 [50], [51] e− + C2 H2 → 2e− + C2 + H2 [52], [53]
e− + CH4 → e− + H2 + CH2 [50], [51] C2 H
e− + CH4 → e− + H2 + H + CH [50], [51] Ionization e− + C2 H → 2e− + C2 H + [49]
− −
Dissociation e− + C2 H → e− + C2 + H [52], [53]
e + CH4 → e + 2H2 + C [50], [51]
e− + C2 H → e− + C + CH [52], [53]
CH3 C2
Ionization e− + CH3 → 2e− + CH3+ [49] Ionization e− + C2 → 2e− + C2+ [52], [53]
e− + CH3 → 2e− + CH2+ + H [49] Dissociation e− + C2 → e− + C + C [52], [53]
C3 H8
e− + CH3 → 2e− + CH + + H2 [49]
Momentum e− + C3 H8 → e− + C3 H8 [48]
− −
Dissociation e + CH3 → e + CH2 + H [50], [51] transfer
e− + CH3 → e− + CH + H2 [50], [51] Vibr. Exc. e− + C3 H8 → e− + C3 H8∗ (2) [48]
CH2 Ionization e− + C3 H8 → 2e− + C3 H5∗ + CH3 [49]
e− + C3 H8 → 2e− + C3 H4∗ + CH4 [49]
Ionization e− + CH2 → 2e− + CH2+ [49]
Dissociation e− + C3 H8 → e− + C3 H7 + H [52], [53]
e− + CH2 → 2e− + CH + + H [49]
e− + C3 H8 → e− + C3 H6 + H2 [52], [53]
e− + CH2 → 2e− + C + + H2 [49] e− + C3 H8 → e− + C2 H4 + CH4 [52], [53]
Dissociation − −
e + CH2 → e + CH + H [50], [51] C3 H7
CH Ionization e− + C3 H7 → 2e− + C2 H5+ + CH2 [52], [53]

Ionization − −
e + CH → 2e + CH + [49] e− + C3 H7 → 2e− + C2 H4+ + CH3 [52], [53]

e− + CH → 2e− + C + + H [49] e− + C3 H7 → 2e− + C2 H3+ + CH4 [52], [53]

e− + C3 H7 → 2e− + CH3+ + C2 H4 [52], [53]
Dissociation e− + CH → e− + C + H [50], [51]
Dissociation e− + C3 H7 → e− + C3 H6 + H [52], [53]
C e− + C3 H7 → e− + C3 H5 + H2 [52], [53]
Ionization e− + C → 2e− + C + [50], [51] e− + C3 H7 → e− + C2 H4 + CH3 [52], [53]
C2 H6 e− + C3 H7 → e− + C2 H3 + CH4 [52], [53]
C3 H6
Momentum e− + C2 H6 → e− + C2 H6 [48]
transfer Ionization e− + C3 H6 → 2e− + C2 H5+ + CH [52], [53]

Vibr. Exc. −
e + C2 H6 − ∗
→ e + C2 H6 (3) [48] e− + C3 H6 → 2e− + C2 H4+ + CH2 [52], [53]

Ionization e− + C2 H6 → 2e− + C2 H6+ [49] e− + C3 H6 → 2e− + C2 H3+ + CH3 [52], [53]

e− + C2 H6 → 2e− + C2 H5+ + H [49] e− + C3 H6 → 2e− + C2 H2+ + CH4 [52], [53]

e− + C2 H6 → 2e− + C2 H4+ + H2 [49] e− + C3 H6 → 2e− + CH3+ + C2 H3 [52], [53]

e− + C2 H6 → 2e− + C2 H3+ + H2 + H [49] Dissociation e− + C3 H6 → e− + C3 H5 + H [52], [53]

e− + C2 H6 → 2e− + C2 H2+ + 2H2 [49] e− + C3 H6 → e− + C2 H2 + CH4 [52], [53]

e− + C2 H6 → 2e− + CH3+ + CH3 [49] C3 H5

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