Plasma Devices and Operations

Vol. 14, No. 1, March 2006, 15–26

Discharge characteristics of a gliding-arc plasma in

chlorinated methanes diluted in atmospheric air
ANTONIUS INDARTO†, JAE-WOOK CHOI†, HWAUNG LEE†, HYUNG KEUN
SONG*† and NOWARAT COOWANITWONG‡
†Korea Institute of Science and Technology, Clean Technology Research Center, PO Box 131,
Cheongryang, Seoul 130-650, South Korea
‡School of Environment, Resources, and Development Asian Institute of Technology, PO Box 4,
Klong Luang, Pathumthani 12120, Thailand

(Received 18 October 2004)

Plasma processing of the chloromethane compounds (methylene chloride (CH2 Cl2 ), chloroform
(CHCl3 ) and carbon tetrachloride (CCl4 )) diluted in atmospheric air using a gliding arc has been
studied. Various injected initial chloromethane concentrations, total gas flow rates and power
frequencies were used as the variables to investigate the discharge characteristics. This paper evaluates
the phenomenon of chloromethane processing by gliding-arc plasma.

Keywords: Plasma; Gliding arc; Chloromethanes;Alternating-current waveform; Equilibrium voltage;

Voltage breakdown

1. Introduction

The plasma of a gliding arc is widely used now to destroy toxic materials. Many dangerous
emissions, such as H2 S [1], N2 O [2], CHCl3 and CCl4 [3, 4], have been investigated and
studied. Usually, a high destruction efficiency can be achieved by using this method.
The device for the generation of a gliding arc consists of a pair of flat electrodes, which
are connected to a power supply. In operation, the arc is ignited at the narrowest part of the
gap between the electrodes immediately after breakdown. Breakdown takes place when the
electric field in the gap is high enough to ignite the arc. The current of the arc increases very
rapidly at moderate voltages sufficient to create a powerful arc that expands upwards along
the surface of electrodes and elongates until it can no longer be maintained. At this point, the
arc is extinguished and the process is repeated [5].
The number of arcs that will be produced depends on many factors, such as the frequency
of the power supply applied, the species of flowing gas and the total gas flow rate. During
this arc movement, the destruction of the molecules of hazardous materials simultaneously

*Corresponding author. Email: hksong@kist.re.kr

Plasma Devices and Operations

ISSN 1051-9998 print/ISSN 1029-4929 online © 2006 Taylor & Francis
http://www.tandf.co.uk/journals
DOI: 10.1080/10519990500494898
16 A. Indarto et al.

occurs. Plasma arcs usually have an energy high enough to break strong molecular bonds or
to initiate a reaction of stable gas material owing to the high temperature of the flame, high
electron density, etc.
However, there have been only a few papers that have discussed the behaviour of a gliding
arc. The results of theoretical and numerical studies performed using many mathematical
equations describing a gliding arc have been published in the literature [6–10].
In this paper, we try to explain the physical characteristics of a plasma of compressed
air with chloromethane compounds diluted in it. The experiment was carried out with two
triangular stainless steel electrodes, which were electrically charged from an alternating-
current (AC) power supply. According to a report by the US Environmental Protection Agency,
the chloromethane to be destroyed was categorized as a compound of high thermal stability
[11]. An analysis was carried out, which was focused on the discharge parameters, such as
the equilibrium voltage, breakdown voltage and voltage–current–power (V –I–W ) profile as
functions of the chloromethane concentration, total gas flow rate and power frequency.

2. Experimental set-up

A schematic diagram of the experimental set-up is shown in figure 1. Chloromethane com-

pounds and atmospheric air were used as input gases. The system and the components of the
set-up are described in detail in the following sections.

2.1 Plasma reactor and power supply

The reactor was made from a quartz-glass tube of inner diameter 45 mm and length 300 mm.
The upper part and the bottom of the reactor equipped with Teflon seals consisted of two
electrodes made of stainless steel. The electrodes were 150 mm in length. The separation
of electrodes in the narrowest section was 1.5 mm. The gas mixture was injected between
the electrodes through a capillary (a nozzle tube) of 0.8 mm inner diameter. A thermocouple,
located 10 cm above the electrodes, was provided to measure the temperature of the outlet gas.
A high-frequency AC power supply (Autoelectric A1831) with a maximum voltage of 10 kV
and a maximum current of 100 mA was connected to the gliding-arc electrode to generate a
plasma. The frequency of the power supply could be adjusted from 10 to 20 kHz.

2.2 Input gas

The following chlorinated methanes were used as the initial material:

(i) methylene chloride: CH2 Cl2 ; molecular weight, 84.93; purity, 99.0%; purchased from
the Junsei Chemical Co., Ltd; concentrations, 1, 2, 3 and 4 vol.%;
(ii) chloroform: CHCl3 ; molecular weight, 119.38; purity, 99.0%; purchased from the Junsei
Chemical Co., Ltd; concentrations, 1, 3, 5 and 8 vol.%;
(iii) carbon tetrachloride: CCl4 ; molecular weight, 153.82; purity, 99.5%; purchased from the
Kanto Chemical Co., Inc.; concentrations, 1, 3, 5 and 8 vol.%.

Atmospheric air was used as the carrier gas and controlled by a calibrated mass flow
controller (Tylan FC-280S). The flow rates were 3, 4 and 5 l min−1. Before entering the reactor,
atmospheric air first passed through a scrubber and then was mixed with the chloromethane
compound. Chloromethane compounds were injected using a syringe pump (KD Scientific
 Gliding-arc plasma in chlorinated methanes 17

Figure 1. Schematic diagram of the experimental set-up: MFC, mass flow controller.

model 100). The temperature of the input stream was maintained higher than the temperature
of vaporization of the compounds by means of a heating tape surrounding the streamline.

2.3 System of measurements

The power supplied and the AC voltage–current (V –I) waveform were recorded using a digital
oscilloscope (Agilent 54641A) with a high-voltage probe (Tektronix P6015A) having an ana-
logue bandwidth of 350 MHz and a current monitor (Pearson 4997). The power consumed was
also recorded using a wattmeter (Metex M-3860M). The power measured with the oscilloscope
was the real value absorbed in the reactor only and was defined as


discharge power = [V (t) × I (t)] dt × frequency W. (1)

In this study the experimental data were taken 30 min after initiation of the plasma of
the gliding arc referred to the onset outlet temperature of the bulk gas measured with a
thermocouple.
18 A. Indarto et al.

3. Results and discussion

3.1 Characteristics of the power supply

The specific characteristic of the gliding arc is the initial breakdown of the moving gas that
initiates this arc. The initial breakdown voltage was higher than the equilibrium voltage.
Figure 2 shows the arc movement along the electrode plates. The number of arcs produced
could be easily found from the waveform of the voltage and current (figure 3). Furthermore,
the breakdown at arc ignition results from the over-current at the shortest distance between
the pair of electrodes [12]. In this study, the AC supply voltage applied and the current at
breakdown and in the equilibrium state were determined by various parameters, such as the

Figure 2. Movement of the gliding arc along the electrode plate recorded by a high-speed camera.
 Gliding-arc plasma in chlorinated methanes 19

Figure 3. Typical waveform of the AC power supply. The phenomena of arc production can be clearly seen from
the fluctuations in current waveform.

distance between the electrodes, the material of the electrodes and the gas flow rate, and could
not be manually adjusted by varying the power supply parameters.
On achieving initial breakdown, the supply voltage and current decreased in the equilibrium
state to a stationary value, which could not be adjusted or changed by varying the power supply
parameters. The frequency of the power supply was the only adjustable independent parameter.
However, this frequency played an important role in the number of arcs produced.

3.2 Influence of the chloromethane compounds

The power consumed or applied played the main role in maintaining the stability or instability
of the gliding plasma. Although the concentration and flow rate were kept the same, different
compounds of injected material gave different power consumptions. Figure 4 shows the result
of the measurements of voltage carried out using an oscilloscope for different gases. Slight
differences in the voltage and positions of the maxima occurred. With increasing concentration
of the chloromethane in the inlet stream, the difference increased rapidly, which is clearly
shown in figure 5. From figure 5, it can be concluded that the compound containing CCl4
20 A. Indarto et al.

Figure 4. Voltage profile.

consumed the highest discharge power. The power consumed by different compounds was as
follows (in descending order):

CCl4 > CH2 Cl2 > CHCl3 .

A good analytical explanation can be given on the basis of the Paschen law, according to
which the potential is a function of the product of pressure and gap length [13]:

V = f (p, d). (2)

In this experiment the interelectrode gap was kept constant, and the pressure could also be
assumed constant.Although the potential was a function of p and d, in the real experiment, some
coefficients must be introduced to ensure a match between the results of the experiment and

Figure 5. Effect of the injected chloromethane compounds (species, concentration and total gas flow rate) on the
discharge power.
 Gliding-arc plasma in chlorinated methanes 21

mathematical calculations [14]. By rearranging equation (2) and inserting some coefficients,
we have
Bpd
V = , (3)
ln[Apd/ ln(1/γ )]
where γ is the Townsend secondary emission coefficient of electrons, which is written as
follows:
1
= eαd . (4)
γ
By differentiating equation (2) and setting the derivative equal to zero, we have
   
e 1 2.718 1
(pd)m = ln = ln . (5)
A γ A γ
The minimum or maximum voltage was obtained by substituting equation (5) into
equation (3):
 
B 1
Vm = 2.718 ln . (6)
A γ
The voltage given in equation (6) is usually called the breakdown voltage Vbd . In the case of
a gliding arc, Vm > V . Less information about the constants A and B is available in the case
of a gliding-arc plasma. The parameters A and B must be determined experimentally [15].
From equations (3) and (6), it can be seen that there is a relation between V and Vbd . When
chloromethane compounds were injected with different concentrations, the values of Vbd
obtained from the experiment were different. In this study, to check the relationship between
V and Vbd , we used the following algorithm.
By rearranging equation (6) in the form
 
2.718 1
A= B ln (7)
Vm γ
and substituting it into equation (3) we have
Bpd
V = . (8)
ln(2.718B/Vm )
For two different concentrations of chloromethane compounds, we obtain
V1 B1 p1 d1 / ln(2.718B1 /Vm1 )
= (9)
V2 B2 p2 d2 / ln(2.718B2 /Vm2 )
The experiment was carried out under the same pressures and gap distances: p1 = p2 and
d1 = d2 . The parameter B is a function of the effective ionization potential V ∗ and pressure.
This potential ensures that the transport electrons move through the gap and thus ioniza-
tion is produced. As we used the same gap distances, the pressures and concentrations of
chloromethane compounds differed only slightly, and it could be assumed that B1 ≈ B2 .
In this case, equation (9) can be written in the form
ln(1/V1 ) Vm2
= (10)
ln(1/V2 ) Vm1
A comparison between the calculation and experimental results is shown in figure 6. When
the experiment was carried out with the same chloromethane compounds but with differ-
ent concentrations, the results were close. A satisfactory result was also achieved when the
22 A. Indarto et al.

Figure 6. Comparison between the calculation and experimental value of Vbd .

experiment was carried out with different total gas flow rates and fixed concentration and
chloromethane species. However, the result was not satisfactory when we applied the same
rates with different chloromethane compounds. This means that the parameters A and C have
specific values for each chloromethane gas and play an important role in the initiation of arc
cycle production.
The chemical stability of molecules, which determines the emission of such species as
electrons and ions, has an appreciable effect on the breakdown process. Bartnikas and
co-workers [16–19] have studied and described in their work the effect of electrons on the
initiation of breakdown. The lack of free electrons that are necessary to initiate the breakdown
will lead to an over-voltage across the electrode gap, which will result in a higher voltage
and current and shorter rise times. Taylor and Dellinger have compared these compounds and
graded these compounds with respect to stability under oxidation conditions [20] according to

CCl4 = CH2 Cl2 > CHCl3

and in the absence of oxygen according to

CCl4 > CH2 Cl2 > CHCl3 .

The stability depends on the structure and chemical bonds of the compounds. A higher
chemical bond stability than those of other chlorinated methanes could explain why CCl4
gave the highest value of V and Vbd . This result also matched other experimental results
testifying that CCl4 has a higher energy consumption than CHCl3 [4].

3.3 Influence of the total gas flow rate

After the initial breakdown of the discharge gap, we failed to control the equilibrium voltage
and current by varying the power supply parameters, and the setting of a specified voltage
and a specified current was difficult. In this case, the total gas flow rate was also a factor to
be considered as a variable. Figure 7 shows the effect of the total gas flow rate on the power
 Gliding-arc plasma in chlorinated methanes 23

Figure 7. Power profile as a function of the total gas flow rate. The data were obtained using 1 vol.% CCl4 as the
injected compound at a power frequency of 20 kHz.

profile. It can be easily seen that, at 3 l min−1 , the total discharge power that was supplied to
the system was higher than its values at 4 and 5 l min−1 .
To study this effect thoroughly, we tried to capture the real voltage–current profile under the
conditions of equilibrium. Figure 8 shows the behaviour of the voltage–current wave obtained
by experiment. The calculations of both the real and the average values of the voltage wave
indicated that the total voltage supplied would be lower at lower total gas flow rates, but
this difference was not noticeable. This phenomenon can be also explained by the Paschen
law [14].
Usually, an increasing flow rate increases the pressure in the system. The increasing pressure
can increase the breakdown voltage Vbd , which is higher than the voltage at low pressures.
Moreover, the voltage under the equilibrium condition will also be higher than the voltage at
low pressures. The effect of the current waveform can be supposed to be the main reason for
increasing or reducing the value of the total discharge power. A comparison between figures
8(b), (d) and (e) shows that at 3 l min−1 the number of suddenly fluctuating pulses was higher
than in the other two cases. This means that at 3 l min−1 the system produced more arcs than
at 4 and 5 l min−1 . As mentioned above, the increasing flow rate resulted in a higher pressure;
therefore, the possibility of producing arcs became weaker. That is why the number of suddenly
fluctuating pulses became increasingly smaller with increasing total gas flow rate. However,
suddenly fluctuating pulses also made a significant contribution to the calculated average total
current fed to the system. Compared with the average current when no arc occurred, in the
case with a plasma the value of the total average current was five to ten times higher.

3.4 Effect of the frequency

The frequency of the power supply was an adjustable factor in this experiment. Figure 9
shows the effect of the frequency on the power profile. The integration of equation (1) shows
that the total discharge power increased linearly with increasing frequency. When the con-
ditions were kept constant, the number of arcs also increased. Radu et al. [16] mentioned
that a change in the frequency would change the basic mechanism of the Townsend break-
down. An increasing frequency will lead to an increase in the sudden fluctuations in the
24 A. Indarto et al.

Figure 8. Voltage–current behaviour using 1 vol.% CCl4 as the injected compound and a power frequency of
20 kHz: (a) V at a gas flow rate of 3 l min−1 ; (b) I at a gas flow rate of 3 l min−1 ; (c) V at a gas flow rate of 4 l min−1 ;
(d) I at a gas flow rate of 4 l min−1 ; (e) V at a gas flow rate of 5 l min−1 ; (f) I at a gas flow rate of 5 l min−1 .

current and voltage peaks per cycle. The integration calculation of the power waveform using
equation (1) shows that a larger number of peaks per cycle will result in a higher supplied
energy (figure 10). The measurements carried out with a wattmeter showed the same tendency
as the oscilloscope measurements but the power was slightly higher. An oscilloscope was used
to measure only the energy that was supplied to the plasma. On the other hand, a wattmeter
measured the total power needed for all instruments, including the total power to operate the
power supply.
 Gliding-arc plasma in chlorinated methanes 25

Figure 9. Effect of the frequency of the applied power supply on the power profile. The data were obtained using
10 vol.% CHCl3 at a total gas flow rate of 2.5 l min−1 .

Figure 10. Effect of the frequency of the applied power supply on the total discharge power. The data were obtained
using 8 vol.% CHCl3 at a total gas flow rate of 2.5 l min−1 .

4. Conclusion

The power discharge characteristics of a gliding-arc plasma have been studied using
chloromethane compounds. Different concentrations, total gas flow rates and frequencies
have been used to investigate the behaviour of the voltage–current–power (V –I–W ) charac-
teristic. Different chloromethane compounds gave significantly different values of discharge
power, equilibrium voltage and breakdown voltage; CCl4 gave the highest values. In the case
of different concentrations and total gas flow rates the behaviour of chlorinated methane com-
pounds followed the Paschen law, which gave the relation between the equilibrium voltage
and the breakdown voltage. A higher total gas flow rate resulted in a decrease in the discharge
26 A. Indarto et al.

power, a decrease in the number of arcs produced and, consequently, sudden fluctuations in
the current wave. The discharge power also increased at higher frequencies.

Acknowledgement

This work was supported by the National Research Laboratory of the Ministry of Science and
Technology of Korea.

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