Discharge Characteristics of Chlorinated Methanes Diluted in

Atmospheric Air on Gliding Arc Plasma

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)

Please, give an additional shortened running title (not more than 35 characters including
spaces) For example: Arc Plasma in Chlorinated Methanes

Abstract

Plasma processing of the chloromethane compounds (methylene chloride (CH2Cl2), chloroform

(CHCl3), and carbon tetrachloride (CCl4)) diluted in the atmospheric air using gliding arc have 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 characteristic. This

paper evaluates the plasma process phenomena of chloromethane by gliding arc plasma??. the

phenomena of chloromethane processing by gliding arc plasma

Key words: Plasma, Gliding Arc, chloromethane, AC wave form, equilibrium voltage, voltage

breakdown

1. Introduction

The applications of gliding arc for destructing toxic materials are widely used now. 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
†
Corresponding author: E-mail:indarto_antonius@yahoo.com, Tel:+82-19-352-1981
investigated and studied. Usually, high percentage of destruction efficiency could can be achieved

by using this method.

The gliding arc creates arcs (please, clarify. Does it mean, that initial arc is splitted?), which

were started are initiated at the shortest distance from the electrodes, and arcs move together with

gas flow at the same direction. and move in the same direction with the gas flow.

The number of arcs that would will/can (please, choose the correct word) be produced is

dependent depends on many factors, such as the frequency of the power supply applied, flowing gas

(sort of gas? Gas species ?), and the total gas flow rate. During this movement, plasma reaction (?)

(reactions in plasma?) is occurred simultaneously occurs. Plasma arcs usually has have powerful

energy high enough to destruct strong molecule bond or initiate the a reaction of stable gas material

due to many advanced characteristics (high plasma parameters?) such as high temperature of flame,

higher electron density, and etc.

However, not many the papers that discuss on the discharge behaviour of gliding arc plasma.

the behaviour of gliding arc are few in number. Theoretical and numerical study of gliding arc to

describe it has been published with showing many mathematical equations [5-9]. (Does it mean:

The results of the theoretical and numerical studies performed with the use of many mathematical

equations describing gliding arc have been published in literature [5-9].)

In this paper, the physical plasma characteristic of chloromethane compounds diluted in

compressed air was tried to be explained. In this paper, we tried to explain physical characteristics

of the plasma of compressed air with the chloromethane compounds diluted in it. The experiment

was carried out with two triangular stainless steel electrodes, which were electrically charged by AC

power supply from an AC power supply. According to an EPA (Please, spell out the abbreviation)

report, the chloromethane to be destructed has been was categorized as high thermal stability

compound a compound of high thermal stability to be destructed [10]. An analysis was focusing

carried out, which was focused on discharge phenomena parameters, such as the equilibrium

voltage, breakdown voltage, and voltage-current-power (V-I-W) profile as the influence of various
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 have been were used as an input gas. The details of each part of the

setup system are described in the following section. Each system and component of the setup are

described in detail in the following section.

2.1. Plasma reactor and applied 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 supplied equipped with a teflon seal comprised

two electrodes made of stainless steel. The length of the electrodes was 150 mm. The separation of

the electrodes in the narrowest section was 1.5 mm. The gas mixture was introduced fed between

the electrodes through a capillary (nozzle tube) of 0.8 mm inner diameter. A thermocouple, located

10 cm above the electrode, has been 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 ampere current of 100 mA was connected to the gliding arc electrode to generate plasma.

The frequency could be adjusted from 10 to 20 kHz.

2.2. Input gas

Chlorinated methanes, used as the starting initial material, are:

a. Methylene chloride: CH2Cl2, molecular weight 84.93, purity 99.0%, purchased from the Junsei

Chemical Co., Ltd., concentration 1, 2, 3, 4 % volume/volume (?) (volume percent ?)

b. Chloroform: CHCl3, molecular weight 119.38, purity 99.0%, purchased from the Junsei

Chemical Co., Ltd., concentration 1, 3, 5, 8 % v/v. (Does it mean: 1, 3, 5, 8 volume percent ? or

1, 3, 5, 8 % chloroform by volume ?)
c. Carbon tetrachloride: CCl4, molecular weight 153.82, purity 99.5%, purchased from the Kanto

Chemical Co., Inc., concentration 1, 3, 5, 8 % v/v. (volume percent?)

Atmospheric air was used as the a carrier gas and was controlled by a calibrated mass flow
controller (the Tylan, FC-280S). The flow rates were 3, 4, and 5 Nl/min. (Does Nl mean 'normal
litre'?) Before entering the reactor, atmospheric air was first passed through a scrubber first and
directly then was mixed with chloromethane compound. The chloromethane compounds were
introduced injected by a syringe pump (the KD Scientific, Model 100). Heater tape has been
attached surrounding the line stream to maintain the input stream temperature higher than vaporized
temperature of compounds. 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. Measurement system System of Measurements

The supplied power supplied and AC voltage-current (V-I) waveform were measured
registered by a digital oscilloscope (the Agilent 54641A) with a high-voltage probe (the Tektronix
P6015A) having analogue bandwidth of 350 MHz through a high voltage probe (the Tektronix
P6015A) and a current monitor (the Pearson 4997). The consumed power consumed was also
calculated by a wattmeter (the Metex M-3860M). The oscilloscope value is the real power used in
the reactor only and defined as: 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 Watt (1)

In this study, each data of experiment was taken after 30 minutes from the start of gliding

plasma operation refers to the stability of bulk gas outlet temperature which has been measured by

thermocouple. 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 special characteristic of gliding arc is the initial breakdown of the moving gas will
begin the cycle of the gliding arc production. The specific characteristic of the gliding arc is the

initial breakdown of the moving gas, which initiates this arc. Initial breakdown voltage was higher

than equilibrium voltage. Figure 2 shows the arc movement along the electrode plates. The number

of produced arcs produced could be easily detected found from the equilibrium waveform of the

voltage and current. As is shown in Figure 3, arcs were produced by over-current value (please,

explain. Does it mean that arc was was registered when over current peaks were observed?). In this

study, the applied AC power supply voltage applied and current were determined by gliding system

(please, explain what is the gliding system? Is it the system in which the gliding arc was initiated?).

After On achieving initial breakdown, power supply voltage and current were decreased in the

equilibrium state to a stationary value which those variables could not be adjusted or changed by

varying the parameter of the power supply controller. The frequency of the power supply was the

only the adjustable independent variable parameter. The frequency gave played the an important

role in the amount of arcs production. produced.

3.1. Influence of chloromethane compounds

Figure 4

Figure 5

The power consumed or applied power has plays the main important role to hold in holding

the stability or instability of gliding plasma. Although the concentration and flow rate were kept the

same, but difference different compounds of injected material gives gave different power

consumption. Figure 4 shows the comparison of the oscilloscope result of the measurements of

average voltage carried out by oscilloscope (recording) for different gases. Slightly different Slight

differences in of voltage area and positions of maxima peak voltage have been occurred With

increasing rising concentration of chloromethane in the inlet stream, the difference was getting

more and more, which It is clearly shown by in Figure 5. From Figure 5, it can be concluded that

the compound containing CCl4 consumed the highest discharge power. Amount number of
consumed discharged the discharge power consumed follows: . The power consumed by different

compounds was as follows (in descending order):

CCl4 > CH2Cl2 > CHCl3

A good analytical explanation could can be found following 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 [11].

V = f ( p, d ) (2)

In this experiment the gap distance of electrode the interelectrode gap was kept constant,

and the pressure could also be assumed constant also. Although it the potential was mainly the

function of p and d, in the real experiment, some coefficient must be added introduced to match the

results between of the experiment and mathematical calculations [12]. Extended The extension of

Eq. 1 gives: (please, clarify, what you mean writing 'extension')

B pd
V=
 A pd  (3)
ln  
 ln(1 / γ ) 

where γ is the Townsend secondary emission coefficient of electrons of Townsend and

followed, which is written as follows :

1
=∈αd (4)
γ

Differentiating 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 of A and B constants is available under?? in the case of
gliding arc plasma. The parameters A and B must be experimentally determined determined

experimentally [13].

Routing From Eqs. 3 and 6, it could can be said seen that there is a relation of between V to

the and Vbd. Experiment result got the different value of Vbd when the chloromethane compounds

were injected in the different ratio of concentration. When chloromethane compounds were injected

with different concentrations, the values of Vbd obtained from the experiment was were different.

In this study, to check the relationship between V and Vbd, we used the following algorithm

followed this way:

By rearrangement By rearranging Eq. (6) into in the form:

2.718 1
A= B ln (7)
Vm γ

and substituting it into Eq. (3) we will give have:

B pd
V=
 2.718 B  (8)
ln  
 Vm 

If we compare For two different amount of 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 occurred carried out at under the same conditions of pressure and gap

distance: and it can could be written that p1 = p2 and d1 = d2. Parameter B is the function of

effective ionization potential? (V*) and pressure. This potential will be used to travel ensures the

transport the of electrons through the gap to make and thus ionization is produced. Because As we

used the same gap distance, pressure, and very low concentrations different of chloromethane

compounds differ only slightly, it could be assumed that B1 ≈ B2.

 1
ln 
 V1  = Vm 2
The remaining In this case Eq. (9) will be can be written in the form:
 1  Vm1
ln 
 V2 

(10)

Figure 6

The comparison between the calculation and experimental results is shown in Figure 6.

When the experiment was done carried out as the variable but at same compound of

chloromethanes, with varying concentrations but with the same chloromethane compounds, the

result was closed each other the results were close. The satisfaction satisfactory result was also

achieved when the experiment has been done was carried out in the with different total gas flow

rates and fixed amount of concentration and chloromethane species. However, this kind of result

could not be found obtained when we applied the same flow rate in different compound of

chloromethane rates with different chloromethane compounds. This It means that the parameters A

and C have specific numbers values for each chloromethane gases and give play an important role

to initiate in the initiation of the production of arcs in gliding system (?).

Radu, et.al. and others have studied and mentioned about in their work the effect of electron

on the initiation of breakdown. Lack of free electrons those that are necessary to initiate breakdown

under ac condition (What does it mean? AC condition?) will lead to the over-voltage across the

short gap, that which will result in larger magnitude (of which value? voltage?) and more rapid

rising times [14-17]. Taylor et al. have made a comparing comparison between the stabilities of

these compounds and gave the order of stability graded these compounds in stability under
oxidative the conditions of oxidation [18]:

CCl4 = CH2Cl2 > CHCl3

and in the absence of oxygen:

CCl4 > CH2Cl2 > CHCl3

Stability is depending depends on the structure and chemical bonds of compounds. This

factor could tell the reason explain why CCl4 gave the highest value of V and Vbd. This result was

also matched with other experimental results testifying that gave CCl4 has higher energy

consumption than CHCl3 [4].

3.2. Influence of total gas flow rate

Figure 7

Un-adjustable equilibrium voltage and current by power supply controller after initial

breakdown made the experiment little bit difficult to set in the exact same supplied voltage and

current. After the initial breakdown of the discharge gap,we failed to control equilibrium voltage

and current by varying the parameters of the power supply, and setting of specified voltage and

current was difficult. In this case, the total gas flow rate also was also a factor that must to be

counted as a variable. Figure 7 shows the effect of the total gas flow rate on power profile. By

comparing, It can be easily seen that at 3 Nl/min, the total discharge power that was supplied to the

system the was higher value compared to its value at 4 and 5 Nl/min.

Figure 8

To study deeply about thoroughly this effect, we have tried to capture- the real voltage-

current profile at under the equilibrium condition conditions of equilibrium. Figure 8 shows the

behavior of voltage-current wave obtained by experiment. The calculations of both real and average

values of voltage wave gave the result that the total voltage supplied would be lower at lower total

gas flow rate. But the different this difference was not significantly high noticeable. This

phenomenon has clearly can be also explained by previous explanation the Paschen’s law [12].
Usually, increasing rising flow rate would increases the pressure in the system. Increasing pressure

could increase the breakdown-voltage (Vb) in term of producing an initial arc and equilibrium

voltage in term of stabilizing arc cycle production. (Please, explain, what does it mean 'in terms of

producing arc' and ' in term of stabilizing arc cycle production' ? Does it mean the following:

Higher pressure can increase the breakdown-voltage (Vb) by producing an initial arc and increase

equilibrium voltage by stabilizing arc production.) Current wave form effect could be suspected as

the main reason of the increasing or decreasing value of total discharge power The effect of current

waveform can be supposed to be the main reason for rising or reducing the value of total discharge

power. Comparing The comparison between Figures 8 (b), (d), and (e), it shows that at 3 Nl/min the

number of sudden-fluctuated pulses was higher that in the two others cases. It This means that at 3

Nl/min the system produced higher number of more arcs compared to 4 and 5 Nl/min. As

mentioned before above, as the effect of increasing rising flow rate refers to increasing results in

higher pressure, therefore, the possibility to produce arcs was getting decrease weaker . That is why

the number of sudden-fluctuated pulses was became lower smaller and lower smaller with an

increment rising of the total gas flow rate. However, sudden-fluctuated pulses also gave significant

contribution to the calculation of calculated average total supply current fed to the system.

Compared to the average current when there was no plasma was off, the value of the total average

current when plasma on was 5 ~ 10 times higher when plasma was on in case with plasma.

(Please, clarify. Does it mean, that without plasma you had the current? What kind of

current it was?)

3.3. Effect of frequency

Figure 9

Figure 10

Power supply frequency The frequency of the power supply was an adjustable factor in this
experiment. Figure 9 shows the effect of frequency on power profile. Integration calculations by Eq.

1 gave The integration of Eq. 1 showed that the total discharge power increased linier linearly with

increasing number of rising frequency. When the conditions was were kept constant, the number of

arcs was also increased. Radu et. al. mentioned that changing the frequency a change in the

frequency will change the basic Townsend breakdown mechanism the basic mechanism of the

Townsend breakdown [14]. Increasing Rising frequency will increase the number of sudden-

fluctuated pulsed current sudden fluctuations of current and voltage peak per cycle. Examined the

power waveform,( what does it mean? ) increasing number of peak per cycle would give more

supply of energy, Fig. 10.Higher number of peaks per cycle will give higher energy supplied, Fig.

10. Measurement using wattmeter was also giving the same trend as oscilloscope measurement but

little bit higher. The measurements carried out with a wattmeter showed the same tendency as the

oscilloscope measurements but power value was a little bit higher. Oscilloscope just measured was

used to measure only the netto energy that was supplied to the plasma system. In On the other hand,

wattmeter measured the total power that needed by for all instruments, including the total power to

operate the power supply.

4. Conclusion

The power discharge characteristic of gliding arc plasma using chloromethane compounds

has been studied. The power discharge characteristics of gliding arc plasma have been studied using

chloromethane compounds. Various 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; which CCl4 gave their highest values of them. In case

of different concentrations and total gas flow rate, the phenomena were following the behavior of

chloromethane compounds followed the Paschen’s law, which gave the relation between

equilibrium voltage and breakdown voltage. Increasing amount of Higher total gas flow rate would
degrease decreased the discharge power. It would reduced the number of production of arc of arcs

produced that, which would reduced the sudden-fluctuated pulse sudden fluctuations in the current

wave. Discharge power would also increased with the increasing value of higher frequency.

Acknowledgement

This work was supported by the National Research Laboratory of the Korea Minister

Ministry of Science and Technology of Korea.

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 Figure Captions

Fig. 1. Schematic diagram of the experimental setup

Figure 2. Gliding arc movement along the electrode plate. Captured by high-speed camera
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.
Fig 4. Voltage profile.
Figure 5. Effect of injected chloromethane compounds (species, concentration, and total gas
flow rate) on discharge power.
Figure 6. Comparison of between the calculated calculation and experimental value of Vbd.
Figure 7. Power profile as effect as a function of the total gas flow rate. The data were taken
obtained using 1% of CCl4 as an injected compound and 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 Nl/min (b) I-3 Nl/min (c) V-4 Nl/min (d) I-4 Nl/min (e) V-5 Nl/min (f) I-5 Nl/min
Fig 9. Effect of the frequency of the power supply applied frequency on the power profile.
The data were taken obtained using 10% of CHCl3 at a total gas flow rate of 2.5 Nl/min
Fig 10. Effect of the frequency of the power supply applied on the total discharge power.
The data were taken obtained using 8% of CHCl3 at a total gas flow rate of 2.5 Nl/min