DISCHARGE CHARACTERISTICS OF GLIDING ARC PLASMA IN

CHLORINATED METHANES DILUTED IN ATMOSPHERIC AIR

Antonius Indarto†, Jae-Wook Choi, Hwaung Lee and Hyung Keun Song
Korea Institute of Science & Technology, Clean Technology Research Center,
P.O. Box 131, Cheongryang, Seoul 130-650, Korea

(Received 17 October 2004)

Shortened title: GLIDING ARC IN CHLORINATED METHANE

Abstract
Plasma processing of the chloromethane compounds (methylene chloride (CH2Cl2), chloroform
(CHCl3), and carbon tetrachloride (CCl4) diluted in the atmospheric air using gliding arc has
been studied. Various values of injected initial chloromethane concentrations, total gas flow
rates, and power frequency were used as the variables to investigate their discharge
characteristics. This paper evaluates the phenomena of chloromethane processing by gliding arc
plasma.

Key words: Plasma; Gliding Arc, Chloromethane; AC wave form; Equilibrium voltage; Voltage
breakdown

†
Corresponding author: E-mail:indarto_antonius@yahoo.com
1. Introduction
The plasma of gliding arc is widely used now to destruct toxic materials. Many dangerous
emissions, such as H2S [1], N2O[2], CHCl3 and CCl4 [3-4] have been investigated and studied.
Usually, high destruction efficiency can be achieved by using this method.
The device for the generation 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 electrodes immediately after breakdown. Breakdown takes place when the electric field
in the gap is high enough to ignite arc. The current of the arc increases very fast at moderate
voltage sufficient to create a powerful arc that expands upward along the surface of electrodes
and elongates until it can no longer be maintained. At this point, the arc goes out, 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, species of flowing gas, and the total gas flow rate. During this arc
movement, the destruction of the molecules of hazardous materials simultaneously occurs.
Plasma arcs usually have energy high enough to break strong molecular bonds or initiate a
reaction of stable gas material due to high temperature of flame, high electron density, etc.
However, the papers that discuss the behaviour of gliding arc are few in number. The
results of the theoretical and numerical studies performed with the use of many mathematical
equations describing gliding arc have been published in literature [6-10].
In this paper, we tried to explain the physical characteristics of the 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 AC power supply.
According to the report of the US Environmental Protection Agency (EPA), the chloromethane to
be destructed was categorized as a compound of high thermal stability [11]. An analysis was
carried out, which was focused on discharge parameters, such as equilibrium voltage, breakdown
voltage, and voltage-current-power (V-I-W) profile as functions of different concentrations of
chloromethane, total gas flow rate, and power frequency.

2. Experimental setup
The schematic diagram of the experimental setup is shown in Fig.1. Chloromethane compounds
and atmospheric air were used as an input gas. Each system and component of the setup are
described in detail in the following section.

2.1. Plasma reactor and power supply

 Figure 1
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 a teflon seal comprised two electrodes
made of stainless steel. The electrodes were of 150 mm length. The separation of electrodes in
the narrowest section was 1.5 mm. The gas mixture was injected between the electrodes through
a capillary (nozzle tube) of 0.8 mm inner diameter. A thermocouple, located 10 cm above the
electrodes, was provided to measure the temperature of outlet gas. A high-frequency AC power
supply (the Auto electric, A1831) with a maximum voltage of 10 kV and a maximum current of
100 mA was connected to the gliding arc electrode to generate plasma. The frequency of power
supply could be adjusted from 10 to 20 kHz.

2.2. Input gas

The following chlorinated methanes were used as the initial material:
a. Methylene chloride: CH2Cl2, molecular weight 84.93, purity 99.0%, purchased from the
Junsei Chemical Co., Ltd., concentration 1, 2, 3, 4 volume percent.
b. Chloroform: CHCl3, molecular weight 119.38, purity 99.0%, purchased from the Junsei
Chemical Co., Ltd., concentration 1, 3, 5, 8 volume percent.
c. Carbon tetrachloride: CCl4, molecular weight 153.82, purity 99.5%, purchased from the
Kanto Chemical Co., Inc., concentration 1, 3, 5, 8 volume percent.
Atmospheric air was used as a carrier gas and controlled by a calibrated mass flow controller
(the Tylan, FC-280S). The flow rates were 3, 4, and 5 l/min. Before entering the reactor,
atmospheric air first passed through a scrubber and then was mixed with chloromethane
compound. Chloromethane compounds were injected by a syringe pump (the KD Scientific,
Model 100). The temperature of input stream was maintained higher than the temperature of
compounds vaporization by means of heating tape surrounding the stream line.

2.3. System of Measurements

The power supplied and AC voltage-current (V-I) waveform were registered by a digital
oscilloscope (the Agilent 54641A) with a high-voltage probe (the Tektronix P6015A) having
analogue bandwidth of 350 MHz and a current monitor (the Pearson 4997). The power
consumed was also registered by a wattmeter (the Metex M-3860M). The power measured with
oscilloscope was the real value absorbed in the reactor only and was defined as:
Discharge power = ∫ (V (t ) × I (t ) ) dt × frequency Watt (1)
 In this study the experimental data were taken 30 minutes after the initiation of the
plasma of gliding arc referred to the onset outlet temperature of the bulk gas measured by
thermocouple.

3. Results and Discussion

3.1. Characteristics of Power Supplies
Figure 2
Figure 3
The specific characteristic of gliding arc is the initial breakdown of the moving gas that initiates
this arc. Initial breakdown voltage was higher than 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 voltage and current (Figure 3). Following [12], the breakdown at arc ignition
results from over-current at the shortest distance between the pair of electrodes. In this study, the
AC supply voltage applied and the current at breakdown and in equilibrium state were
determined by some parameters, such as the distance between electrodes, material of electrodes,
gas flow rate, etc, and could not be manually adjusted by varying the parameters of power
supply.
On achieving initial breakdown, supply voltage and current decreased in the equilibrium
state to a stationary value which could not be adjusted or changed by varying the parameters of
the power supply. The frequency of power supply was the only adjustable independent
parameter. However, this frequency played an important role in the amount of arcs produced.

3.2. Influence of chloromethane compounds

Figure 4
Figure 5
The power consumed or applied played the main role in holding the stability or instability of
gliding plasma. Although the concentration and flow rate were kept the same, different
compounds of injected material gave different power consumption. Figure 4 shows the result of
the measurements of voltage carried out by oscilloscope for different gases. Slight differences in
voltage and positions of maxima occurred. With rising concentration of the chloromethane in
inlet stream, the difference was getting more and more, which is clearly shown in Figure 5. From
Figure 5, it can be concluded that the compound containing CCl4 consumed the highest discharge
power. The power consumed by different compounds was as follows (in descending order):
CCl4 > CH2Cl2 > CHCl3
 A good analytical explanation can be given on the base of the Paschen’s 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 the function of p and d, in the real experiment,
some coefficient must be introduced to match the results of the experiment and mathematical
calculations [14]. By rearranging Eq. 2 and inserting some coefficients, we will have:
B pd
V=
 A pd  (3)
ln  
 ln(1 / γ ) 
where γ is the Townsend secondary emission coefficient of electrons, which is written as follows
:
1
=∈αd (4)
γ
By differentiating Eq. 2 and setting the derivation equal to zero, we will have:
The differentiation of Eq. 2 and setting the derivation equal to zero will give:
e 1 2.718 1
( pd ) m = ln = ln (5)
A γ A γ
The minimum/ maximum voltage was obtained by substituting Eq. 5 into Eq. 3:
B 1
Vm = 2.718 ln (6)
A γ
The voltage given in Eq. 6 is usually called as a voltage of breakdown (Vbd). In case of
gliding arc, Vm > V. Less information about A and B constants is available in the case of gliding
arc plasma. Parameters A and B must be determined experimentally [15].
From Eqs. 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 Eq. (6) to the form:
2.718 1
A= B ln (7)
Vm γ
and substituting it into Eq. (3) we will have:
B pd
V=
 2.718 B  (8)
ln  
 Vm 
For two different concentrations of chloromethane compounds, we have:
B1 p1 d 1
 2.718 B1 
ln  
V1  V m1 
= (9)
V2 B2 p 2 d 2
 2.718 B 2 
ln  
 Vm 2 
The experiment was carried out under the same pressure and gap distance: p1 = p2 and d1 =
d2. Parameter B is the function of effective ionization potential (V*) and pressure. This potential
ensures the transport electrons through the gap and thus ionization is produced. As we used the
same gap distance, the pressure and concentrations of chloromethane compounds differed only
slightly, it could be assumed that B1 ≈ B2.
In this case Eq. (9) can be written in the form:
1 
ln
V 
 V
 1  = m2
(10)
 1  V m1
ln
V 

 2 
Figure 6
The 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
different concentrations, the results were close. The satisfactory result was also achieved when
the experiment was carried out with different total gas flow rates and fixed concentration and
chloromethane species. However, this result could not be obtained when we applied the same
rates with different chloromethane compounds. This means that 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 breakdown process Radu et.al. have studied and
mentioned in their work the effect of electrons on the initiation of breakdown. Lack of free
electrons that are necessary to initiate the breakdown will lead to the over-voltage across the
electrodes gap, which will result in higher voltage and current and more rapid rising times [16-
19]. Taylor et al. have compared these compounds and graded these compounds in stability under
the conditions of oxidation [20]:
CCl4 = CH2Cl2 > CHCl3
and in the absence of oxygen:
CCl4 > CH2Cl2 > CHCl3
 Stability depends on the structure and chemical bonds of compounds. High chemical
bond stability compared to other chlorinated methanes could explain why CCl4 gave the highest
value of V and Vbd. This result also matched with other experimental results testifying that CCl4
has higher energy consumption than CHCl3 [4].

3.3. Influence of total gas flow rate

Figure 7
After the initial breakdown of the discharge gap, we failed to control the equilibrium voltage and
current by varying the parameters of power supply, and the setting of specified voltage and
current was difficult. In this case, the total gas flow rate also was a factor to be considered as a
variable. Figure 7 shows the effect of the total gas flow rate on power profile. It can be easily
seen that at 3 l/min, the total discharge power that was supplied to the system was higher
compared to its value at 4 and 5 l/min.
Figure 8
To study thoroughly this effect, we tried to capture the real voltage-current profile under
the conditions of equilibrium. Figure 8 shows the behavior of the voltage-current wave obtained
by experiment. The calculations both of real and average values of voltage wave gave that the
total voltage supplied would be lower at lower total gas flow rate. But this difference was not
noticeable. This phenomenon can be also explained by the Paschen’s law [14].
Usually, rising flow rate increases the pressure in the system. Rising pressure can increase the
breakdown voltage (Vb) which is higher compared to the voltage at lower pressure. Moreover,
the voltage under the equilibrium condition will be also higher compared to the voltage at lower
pressure. The effect of current waveform can be supposed to be the main reason for rising or
reducing the value of total discharge power. The comparison between Figures 8 (b), (d), and (e),
shows that at 3 l/min the number of sudden-fluctuated pulses was higher than in the two others
cases. This means that at 3 l/min the system produced more arcs compared to their number at 4
and 5 l/min. As mentioned above, the rising flow rate resulted in higher pressure, therefore, the
possibility to produce arcs was getting weaker. That is why the number of sudden-fluctuated
pulses was smaller and smaller with rising total gas flow rate. However, sudden-fluctuated pulses
also gave significant contribution to the calculated average total current fed to the system.
Compared to the average current when arc was not occurred, in case with plasma the value of the
total average current was 5 ~ 10 times higher.

3.4. Effect of frequency

 Figure 9
Figure 10
The frequency of the power supply was an adjustable factor in this experiment. Figure 9 shows
the effect of frequency on power profile. The integration of Eq. 1 shows that the total discharge
power increased linearly with rising frequency. When the conditions were kept constant, the
number of arcs also increased. Radu et. al. mentioned that a change in the frequency would
change the basic mechanism of the Townsend breakdown [16]. Rising frequency will lead to the
increase in sudden fluctuations of current and voltage peak per cycle. The integration calculation
of power waveform by using Eq.1 shows that higher number of peaks per cycle will give higher
energy supplied, see Figure 10. The measurements carried out with a wattmeter showed the same
tendency as the oscilloscope measurements but power value was a little bit higher. Oscilloscope
was used to measure only the energy that was supplied to the plasma. On the other hand,
wattmeter measured the total power needed for all instruments, including the total power to
operate the power supply.

4. Conclusion
The power discharge characteristics of gliding arc plasma have been studied using
chloromethane compounds. Different concentrations, total gas flow rate and frequency have been
used to investigate the behaviour of voltage-current-power (V-I-W) characteristic. Different
kinds of chloromethane compounds gave significantly different values of discharge power,
equilibrium voltage, and breakdown voltage; CCl4 gave their highest values. In case of different
concentrations and total gas flow rate, the behavior of chlorinated methane compounds followed
the Paschen’s law, which gave the relation between equilibrium voltage and breakdown voltage.
Higher total gas flow rate resulted in the decrease of discharge power, the number of arcs
produced and, consequently, the sudden fluctuations in the current wave. Discharge power also
increased with higher frequency.

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

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Figure captions
Figure 1. Schematic diagram of the experimental setup
Figure 2. Movement of the gliding arc along the electrode plate recorded by a high-speed
camera.
Figure 3. Typical waveform of the AC power supply. The phenomena of arc production could be
clearly seen from the fluctuations of current waveform.
Figure 4. Voltage profile.
Figure 5. Effect of injected chloromethane compounds (species, concentration, and total gas flow
rate) on discharge power.
Figure 6. Comparison between the calculation and experimental value of Vbd.
Figure 7. Power profile as a function of the total gas flow rate.
The data were obtained using 1% of CCl4 as an injected compound at a power frequency of 20
kHz.
Figure 8. Voltage-current behaviour at 1% of injected CCl4 and a power frequency of 20 kHz. (a)
V-3 L/min (b) I-3 L/min (c) V-4 L/min (d) I-4 L/min (e) V-5 L/min (f) I-5 L/min
Figure 9. Effect of the frequency of the power supply applied on the power profile. The data
were obtained using 10% of CHCl3 at a total gas flow rate of 2.5 L/min
Fig 10. Effect of the frequency of the power supply applied on the total discharge power. The
data were obtained using 8% of CHCl3 at a total gas flow rate of 2.5 L/min