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T. Namihiraξ, K. Shinozaki, S. Katsuki, R. Hackam* H. Akiyama and T. Sakugawa**
Department of Electrical and Computer Engineering, Kumamoto University, Kurokami 2-39-1, Kumamoto 860-8555, Japan
Recently industrial applications of ozone have increased in widely different areas including oxidation, sterilization, deodorization, bleaching and others. Ozone generation has been attained using ultra violet irradiation, electrolysis and electrical discharges. The electrical discharge technique includes silent discharge, surface discharge, pulse corona discharge and superimposed silent and surface discharges. In this study, high concentration ozone was produced by using a pulsed streamer discharge under atmospheric pressure of oxygen. A magnetic pulse compressor (MPC) which has a maximum output voltage of 60 kV, a maximum pulse repetition rate of 500 pulses per second (pps) and a pulse duration of about 130 ns was used as a pulsed power source. A spiral copper wire (1 mm in diameter, 10 mm pitch) wound on PVC tubes (26 mm and 30 mm in outside diameters) formed the central electrode in a coaxial geometry. A copper cylinder of 60 mm in internal diameter formed the outer electrode. The ozone production characteristics of three reactors having different dimensions of the gap spacing (15 mm and 17 mm) and length (500 mm and 1000 mm) were investigated. An oxygen flow rate in the range of 1 to 3 l/min at atmospheric pressure was used. It has been found that the dependence of ozone concentration on energy density (J/l) was almost the same for the three different reactors. Typically a production yield of ozone of 100 g/kWh at 30 g/m3 was attained.
be generated where it is required . Currently major efforts are being expended world wide to increase the efficiency of ozone production in order to reduce costs. Many studies on ozone production using dielectric barrier discharges were reported [1-4]. Usually ozone is generated in silent discharges using a dielectric barrier placed adjacent to the outer cylinder [1-3, 5] where micro discharges with a very short duration prevail at the surface of the dielectric. A dc voltage has also been used for ozone generation in a wire-cylinder geometry . On the other hand, there are only few studies using pulsed corona discharges without any dielectric material between the electrodes in spite of its substantial advantages [7-9]. In the present work, a pulsed corona discharge has been used in three different reactors. The effects of the pulse voltage, the pulse repetition rate, the gas flow rate and the discharge energy density (J/L) are reported.
II. EXPERIMENTAL APPARATUS AND PROCEDURE
A schematic diagram of the magnetic pulse compressor (MPC) , which was used as the pulsed power source, is shown in figure 1. The MPC consists of a high speed Gate Turn Off Thyristor (GTO: H10D33YFH, Meidensha Co., Japan) and a single stage pulse compression element. Following the charging of the capacitor C0, GTO is turned on. At the beginning, the current in GTO is reduced by the saturable inductor (SL1). After the saturation of SL1, the stored charge in C0 is stepped up to C1 through GTO, the step-up pulse transformer (PT) and the saturable transformer (ST). The ST compresses the current pulse and steps up the voltage. After the saturation of ST, the charge in C1 is transferred to the peaking capacitor (CP). Finally CP is charged to the desired voltage. The pulses obtained were directly applied to the coaxial electrodes (Load). This setup provided the voltage and current pulses with a repetition rate of up to 500 pps. A typical duration of 130 ns, defined as the full width at half maximum (FWHM) of the pulse voltage, was measured at 35 kV output voltage. Figure 2 shows the experimental set-up. This set-up consisted of a cylinder of oxygen, the discharge chamber, an ozone monitor and the MPC. The purity of the oxygen
There is a growing worldwide interest in the production of ozone for a wide range of applications. Ozone is increasingly being used as an alternative to chlorination of potable water, treatment of industrial wastes, bleaching processes, and chemical synthesis as well as processing of semiconductor devices. In addition the use of ozone has the advantage of less energy consumption compared to other alternatives, namely the chlorination process . Historically, the major application of ozone has been in the treatment of drinking water, which is known as a potent bactericide and viricide . Since ozone cannot be shipped or stored in a gaseous form due to its short lifetime, it must
*Department of Electrical and Computer Engineering, University of Windsor, Canada **Meidensha Corporation, Japan ξ E-mail: email@example.com 0-7803-7120-8/02/$17.00 © 2002 IEEE
cylinder was 99.5 % (Kumamoto Sanso, Japan). The gas flow rate and the ozone concentration were monitored by means of a flow-stat meter (FLOWLINE model SEF-1R, STEC, Japan) and ultraviolet (UV) ray absorption ozone meter (DOA 300, Ebara, Japan). The UV absorption measurements were carried out at 253.7 nm where the absorption cross-section is large at 1.14 × 10-21 m2 [1, 11]. Gas flow rates in the range of 0.5 to 3.0 l/min were used. The ozonizer constituted a discharge tube, which contained a spiral copper wire of 1 mm in diameter, made to a cylindrical configuration as shown in figure 3. The wire was coiled on vinyl chloride tubes having different diameters. In the present work, three different reactors were used. The inner diameter of the copper cylinder was 60 mm. The diameters of vinyl chloride tubes were 26 mm and 30 mm. The length of the copper cylinder was 500 mm and 1000 mm. Table 1 shows the parameters of the three different reactors. The pulsed voltage and the discharge current were measured using an oscilloscope (HP54542A, Hewlett Packard, USA) via a resistive voltage divider (1 Ω / 10 kΩ), which was connected between the inner spiral wire and the ground, and a Pearson current monitor (Model 110A, Pearson Electronics, USA). This oscilloscope with a maximum bandwidth of 500 MHz and a maximum sample rate of 2 GSamples/s recorded the signal. The power (VI) and the energy ( ∫ VIdt ) input to the discharge per pulse were determined using a computer from the digitized signals. Table 1. Parameters of three different reactors Inner electrode Outer electrode Length, L Pitch, d φout φin (mm) (mm) (mm) (mm) Type 1 26 500 10 60 Type 2 26 1000 Type 3 30 500
Figure 2. Experimental set-up for generation of ozone.
Figure 3. Reactor configuration. Wire diameter, 1 mm; Spiral pitch of wire, 10 mm; Inner diameter of outer electrode, 60 mm.
III. RESULTS AND DISCUSSION
Figure 4 shows typical waveforms of the applied voltage to and the discharge current in Type 3 reactor using 1.5 L/min flow rate of oxygen, 100 pps repetition rate and an electrodes gap length of 15 mm. The pulse voltage, which had a peak voltage of 36 kV, was applied to the reactor from the MPC. It will be observed that the FWHM of the applied voltage is 130 ns, while that of the discharge current is 70 ns. The temporal variation of the current was determined by the impedance of the reactor tube and the discharge in oxygen. The displacement current can be seen before the onset of the discharge. During the discharge the impedance became complex . Figure 5 shows the discharge power to and the input energy to the reactor. The power and the energy were calculated from the voltage and the current waveforms shown in figure 4. The energy delivered to the reactor of a single pulse was typically 173 mJ (Figure 5). Figure 6 shows the final concentrations of ozone after applying a pulse voltage as a functions of (a) pulse peak voltage, (b) pulse repetition rate and (c) gas flow rate in Type 3 reactor. The concentrations of ozone indicate the values in the steady state. It is observed from figure 6 (a)
Figure 1. Circuit diagram of the magnetic pulse compressor (MPC). GTO=Gate Turn Off Thyristor; C0, Primary energy storage capacitor; SL1, Saturable inductor; PT, Step up pulse transformer; ST, Saturable transformer; C1, Secondary capacitor; SL2, Saturable inductor; CP, Peaking capacitor.
and (b) that the concentration of ozone increased with increasing peak voltage and increasing pulse repetition rate. This is attributed to the higher electric field at the spiral wire with increasing peak voltage and to increasing the energy input into the discharge. The larger production of ozone with decreasing the gas flow rate (figure 6 (b) and (c)) is attributed to increasing residence time of the gas in the reactor. Figure 7 shows the dependence of the final concentration of ozone on the input energy density to the discharge in oxygen for three different reactors. The input energy density to the gas (Ed, in J/L) is calculated using, f × E × 60 [s/min] Ed = G where f, E and G are the pulse repetition rate [pps], the input energy to the reactor per pulse [J/pulse] and the gas flow rate [L/min], respectively. Figure 7 shows that in the low energy density region of 0 to about 2000 J/L, the final value of ozone increased with increasing the energy
30 20 Voltage Current 150 100 50 0 -50 -100 1000
density for all reactors. Above about 2000 J/L, the ozone concentration was saturated. The final concentration of ozone at a fixed energy density is almost the same for all reactors. The ozone production yield in g/kWh is shown in figure 8 as a function of the final value of ozone for all reactors. The highest yield of180 ± 40 g/kWh was obtained for ozone concentrations of 10 to 20 g/m3.
O3 concentration, g/m3
100 pps 300 pps
40 30 20 10 0 15
Peak voltage, kV
10 0 -10 -20 0 200 400 600 800
O3 concentration, g/m3
1.0 L/min 3.0 L/min
Time, ns Figure 4. Typical waveforms of the applied voltage to and the discharge current in the Type 3 reactor. Conditions: gas flow rate, 1.5 L/min; pulse repetition rate, 100 pps; a gap length of electrode, 15 mm.
3 2 1 0 -1 0 200 400 600 800 Power Energy 300
O3 concentration, g/m3
Current, A Energy / Pulse, mJ
40 30 20 10 0
50 100 150 200 250 300 350 400
Pulse repetition rate, pps
50 40 30 20 10 0
19.0 kV 23.0 kV
200 100 0
Time, ns Figure 5. Typical waveforms of the discharge power to and the input energy to Type 3 reactor. Other conditions are as in figure 4.
Gas flow rate, L/min
(c) Figure 6. Final concentrations of ozone after applying pulse voltage as a functions of (a) pulse peak voltage, (b) pulse repetition rate and (c) gas flow rate in Type 3 reactor.
35 30 25 20 15 10 5 0 0 1000 2000
Type 1 Type 2 Type 3
Discharge energy density, J/L Figure 7. Dependence of the final concentration of ozone on the input energy density to the discharge in oxygen for three different reactors. Conditions: pulse peak voltage, 18 to 31 kV; pulse repetition rate, 50 to 400 pps; gas flow rate, 0.5 to 3.0 L/min.
Type 1 Type 2 Type 3
150 100 50 0
O3 concentration, g/m3
Figure 8. Ozone production yield as a function of concentration of ozone for all reactors. Other conditions are as in figure 7.
Characteristics of ozone production using pulsed streamer discharges under a wire to cylinder in coaxial geometry was studied. We have obtained the following conclusions: 1) the dependence of ozone concentration on energy density (J/l) was almost the same for the three different reactors. 2) typically an ozone production yield of 100 g/kWh at 30 g/m3 was attained.
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O3 concentration, g/m 3