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Performance Evaluation of Nonthermal Plasma Reactors for NO Oxidation in Diesel Engine Exhaust Gas Treatment

T. Yamamoto, B.S. Rajanikanth*, M. Okubo, T. Kuroki and M. Nishino Dept. of Energy Systems Engineering, Osaka Prefecture University 1-1 Gakuen-cho, Sakai-city, Osaka 599-8531, JAPAN Phone and Fax: 81-722-54-9230 E-mail: yamamoto@energy.oskafu-u.ac.jp *Dept. of High Voltage Engineering, Indian Institute of Science, Bangalore 560012, India

Abstract- The discharge plasma-chemical hybrid process for NOx removal from the flue gas emissions is an extremely effective and economical approach in comparison with the conventional selective catalytic reduction system. In this paper we bring out a relative comparison of several discharge plasma reactors from the point of NO removal efficiency. The reactors were either energized by AC or by repetitive pulses. Ferroelectric pellets were used to study the effect of pellet assisted discharges on gas cleaning. Diesel engine exhaust, at different loads, is used to approximately simulate the flue gas composition. Investigations were carried out at room temperature with respect to the variation of reaction products against the discharge power. Main emphasis is laid on the oxidation of NO to NO 2 , without reducing NOx concentration (i.e., minimum reaction byproducts), with least power consumption. The produced NO 2 will be totally converted to N 2 and Na 2 SO 4 using Na 2 SO 3 . The AC packed bed reactor and pelletless pulsed corona reactor showed better performance, with minimum reaction products for a given power, when the NO concentration was low (~100 ppm). At high engine loads (NO > 300ppm) there was not much decrease in NO x reduction and more or less all the reactors performed equally. The paper discusses these observations in detail.

I. INTRODUCTION

Flue gas emissions and automobile emissions are chief contributors to the ever-increasing environmental problems like global warming, acid rain, smog etc. The governing laws are becoming more and more severe and in order to meet the tougher emission regulations continuous development is being taken place in the pollution abatement technology all over the globe. Among the major air pollutants, the NOx

removal from flue gases and CO removal from auto emissions are of chief concern today. In this paper, we focus our attention on the NO abatement in diesel engine exhaust gas treatment. At present, several catalytic based conventional techniques, like selective catalytic reduction process (SCR), DeNOx burners etc., exist for NO abatement. Improved NO reduction techniques like fuel injection timing, exhaust gas recirculation etc., have also been investigated. These conventional techniques, however, hardly meet the future stringent emission regulations. Therefore, the establishment of a low, cost-effective, NO/NO x after treatment technology is desired. One of the promising ways to control NO x is by using electrical discharge plasma-chemical hybrid process, which is extremely effective and economical approach in comparison with the conventional selective catalytic reduction system [1-3].

Literature is abound with many innovative nonthermal plasma techniques which have proved to be successful in controlling various air borne pollutants [1-18]. Researchers have reported several designs of plasma reactors for gas treatment. Each reactor has its own advantages depending on the gas conditions and electrical parameters. In the present paper, three commonly used nonthermal plasma reactors namely, AC energized pellet bed reactor and pulse energized reactor with/without pellets, were studied for their performance evaluation. In order to approximate the flue gas emission the real exhaust of a small-scale diesel engine was used. Experiments were carried out at room temperature and at different engine load conditions.

II. EXPERIMENTAL S ETUP AND PROCEDURE

Figure 1 shows the schematic of experimental setup. A 2 kW diesel generator (3600 rpm, single cylinder, direct fuel injection, Yammer diesel Co., YDG200SS-6E) was used as the source to closely simulate flue gas emissions. The load on engine was adjusted by changing the resistance of an electric

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Diesel engine Silica gel Glass filter Drain pot Pump Flow meter Power supply Probe Heater
Diesel engine
Silica gel
Glass filter
Drain pot
Pump
Flow meter
Power
supply
Probe
Heater
Thermometer
Plasma
Exhaust
reactor
Gas
Oscilloscope
analyzer

Fig. 1 Experimental setup for gas treatment

(a) Rising portion of the pulse for two reactors: (a) no pellets and (b) with
(a)
Rising portion of the pulse for two reactors: (a)
no pellets and (b) with BaTiO 3 pellets

Fig. 2

heater. A part of the exhaust gas was sampled with a vacuum diaphragm pump and coarse particles, such as carbon soot, were removed by a glass-wool filter. Smaller particles were then removed using a series of drain pots containing hollow-fiber membrane filters (0.01mm pore diameter). Moisture content in the gas is minimized using a silica gel suspension. As a result, an absolute humidity of about 0.4 mg/L (relative humidity, 2.6%) was obtained at the room temperature.

An AC driven pellet-bed reactor, pulse driven pellet-bed reactor and a pulse driven pelletless reactor, were investigated for NO oxidation. The pellet bed consists of 1.7~2.0 mm diameter barium titanate (BaTiO 3 ) ferroelectric pellets (relative dielectric constant of 10,000 at room

10 9 60 Hz AC 8 210 Hz Pulse (no pellets) 7 210 Hz Pulse
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Discharge power variation of the reactors

temperature). The reactor was Pyrex glass tube of 20 mm diameter with a 1.5 mm corona electrode placed co-axially. The effective length of the tube is 26 cm. The tube is wrapped with a copper mesh forming the ground electrode. For energization, a 60 Hz AC supply or a 210 Hz pulse supply (supplied through a rotary spark gap switch) was used. The applied voltage was measured by an oscilloscope (Sony Tektronix TDS380P-2GS/s) through a voltage divider (Sony Tektronix P6015A).

The gas flow was controlled using a valve and a float-type flow meter. The treated gas, before being fed into the analyzer, was made to pass through a heater to remove ozone. The heater temperature was maintained at 300 °C. The NO in the exhaust gas was effectively oxidized to NO 2 with moderate plasma power. The concentration of gas components such as CO, NO, and NO x was measured using a gas analyzer (Horiba Co., VIA-50). The concentrations of

CO 2 and humidity were measured using gas detection tubes

(Gastec Co.).

III. RESULTS AND DISCUSSION

At first, without any energization, the gas concentrations from the diesel engine were measured at different engine loads (K). NO concentration increases from 92 to 560 ppm and NO x concentration increases from 145 to 600 ppm when

K varies from 0 to 100%. On the other hand, NO 2

concentration was in the range of 40~60 ppm, irrespective of

K.

Figure 2 shows the pulsed voltage waveforms for the reactor with and without pellets. The pulse rise time was 6.1 ns for the pelletless reactor and 13.7 ns for that with pellets. The applied voltage was about 26 kV. The pulse duration

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NO,
NO 2 , NO x , CO
concentrations
(ppm)
CO 2 , O 2 concentrations (%)

Fig.4

Load (%)

Initial Gas concentrations of diesel engine exhaust at different loads

was 1.2 ms in both the cases. The voltage and current wave forms for the AC packed-bed reactor was already reported in

[4].

Figure 3 shows the power consumption of the three plasma reactors. It is clear that the pulsed corona without pellets showed the lowest power consumption, followed by the pulsed corona with BaTiO 3 pellets and 60 Hz AC packed-bed plasma reactor.

Figure 4 shows the concentrations of the diesel emission plotted against the engine load K. The concentration of NO x , NO, NO 2 and CO were shown in the left Y-axis and the concentration of CO 2 and O 2 , in volume %, is shown on the right Y-axis. When the load K changed from 0 to 100 %, NO concentration increases from 92 to 560 ppm and NOx concentration increases from 145 to 600 ppm which is almost proportional to the load factor K. On the other hand, NO 2 concentration was in the range of 40~60 ppm. The concentration of CO becomes 1,080 ppm at K=0%, decreases with increase in K and becomes minimum value of 360 ppm at K=75 %. It increases again to reach 460 ppm at K=100 %. The concentration of CO 2 increases from 2.0 % to 5.3 % with increasing K. The concentration of O 2 decreases from 16.7 % to 10.4 % with increasing K.

Figure 5(a) shows the gas concentration plotted against the discharge power at the reactor for AC packed-bed plasma reactor when K=0%. The flow rate and the absolute humidity were set at 3.0 L/min and 0.4 mg/L, respectively, throughout the experiments. The initial NO concentration of 105 ppm was effectively oxidized to NO 2 at 0.4 W. It is important to note that the plasma reactor should operate at 0.4 W, which gives least NO x reduction, indicating minimum byproducts formation such as N 2 O, HNO 2 and HNO 3 . The concentration

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Fig. 5

(c)

Gas concentrations at different discharge powers for 0% load on diesel engine : (a) AC (b) pulse with no pellets (c) pulse with pellets

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of CO remained the same at any discharge power.

Figure 5(b) shows the gas concentration for the pulsed

NO

concentration was about 135 ppm but almost complete NO

oxidation was achieved

concentration compared with the initial NO x concentration was attributed to the oxidation of air. The concentration of CO increased with the power. This may be attributed to the oxidation of residual carbon soot in the reactor and/or plasma reduction of CO 2 .

corona

without

pellets

when

at

K=0%.

1.0

W.

The

The

initial

higher

NO x

Figure 5(c) shows the gas concentration for the pulsed

corona

concentration of 125 ppm was totally converted to NO 2 at 5.0 W. The AC packed-bed reactor and the pulsed corona pelletless reactor achieved the best NO reduction for a given power (0.4W) while treating the low NO concentration (<130 ppm). The produced NO 2 was totally converted to N 2 and sodium sulfate (Na 2 SO 4 ) using an aqueous solution of sodium sulfite (Na 2 SO 3 ) [1-3]. The Na 2 SO 4 solution is water soluble and a nontoxic compound. The trace amount of reaction byproducts such as HNO 2 and HNO 3 can be easily neutralized by NaOH scrubbing [2,3].

Figure 6(a) shows the gas concentration plotted against the power consumption for the AC packed-bed plasma reactor when K=50%. The initial NO concentration is approximately 300 ppm and was effectively oxidized to NO 2 at 5.6 W, which requires significantly greater power compared with that needed at K=0% (0.4W).

with

pellets

when

K=0%.

The

initial

NO

Figure 6(b) shows the gas concentration for the pulsed

corona

concentration was reduced by about 80%, without reducing NO x , at 2.0 W.

Figure 6(c) shows the gas concentration for the pulsed

without

pellets

when

K=50%.

The

initial

NO

corona

concentration was fully converted to NO 2 at about 4.0 W. It is clear that the AC packed-bed reactor and the pulsed corona reactor with pellets achieved the best NO reduction. However, for a given power (2.0 W), the pulsed corona without pellets performed better. Again, the reaction byproducts such as

HNO 2 and HNO 3 were minimum because of less NO x reduction. The AC packed-bed reactor and the pulsed corona reactor with pellets achieved the best NO x reduction for treating medium NO concentration (~300 ppm). However, for a given power for example at 2.0 W, the pulsed corona without pellets achieved better performance.

Figure 7(a) shows the gas concentration plotted against the reactor power for the AC packed-bed plasma reactor

with

pellets

when

K=50%.

The

initial

NO

700 600 500 400 300 NO 200 NOx NO2 100 CO 0 01234567 DischargePower(W) (a)
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Fig. 6

(c)

Gas concentrations at different discharge powers for 50% load on diesel engine : (a) AC (b) pulse with no pellets (c) pulse with pellets

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when K=100%, which gives the highest initial NO concentration (approximately 550 ppm). The NO to NO 2 conversion was about 56% at 5.6 W. Obviously, the NO oxidation is more difficult for high NO concentration. However, the reaction byproducts were minimum because of little change in NOx.

Figure 7(b) shows the gas concentration for the pulsed corona without pellets when K=100%. The NO conversion was about 40% at 2.0 W. The CO concentration was changed from 1,000 ppm to 1,280 ppm. The initial CO value contradicts with the data shown in Figure 4 (440 ppm). This was due to the change in air to fuel mixture ratio of the diesel engine itself.

Figure 7(c) shows the gas concentration for the pulsed

corona

concentration was about 40% at 5.0 W. It is clear that the all

reactors performed about the same for a given power. However, the CO concentration was significantly higher for the pulsed corona with pellets.

The NOx reduction from the diesel engine was limited up to 300 ppm of NO concentration using the nonequilibrium plasma. In order to treat higher NO concentration, the NO 2 produced must be removed to avoid the dissociation of NO 2 (NO 2 + O NO + O 2 ). In this way, we can achieve a high NOx removal efficiency plasma reactor.

Now, we estimate the power consumption for the plasma-chemical hybrid process. When the flow rate is 3.0 L/min and the power consumption is 2.0 W for the case of the pulsed corona without pellets, the specific energy density becomes 40 J/L (54 eV/molecule). The electrical cost becomes $400/ton of NO ($0.05/kW-hr was assumed). The operating cost for the chemical reactor becomes about $1,800/ton of NO 2 reduction when the NO concentration is 300 ppm ($0.48/kg was assumed for Na 2 SO 3 ). Therefore, the total operating cost of the plasma-chemical hybrid system becomes $2,200/ton of NO, which is less than 1/6 of the conventional selective catalytic reduction process.

NO

with

pellets

when

K=100%.

The

initial

IV. CONCLUSIONS

Three types of plasma reactors, AC pellet bed, pulse without pellets and pulse with pellets, were evaluated for NO oxidation using a real diesel engine emission. Both AC and pulsed corona without pellets showed the best performance with minimum reaction products for a given power when the NO concentration was low (~100 ppm). However, the NOx reduction was significant with increased NO concentration and three reactors were performed more the less the same when the the engine load was high (NO>300 ppm). Also, the

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Fig. 7 Gas concentrations at diffrent discharge powers for 100% load on diesel engine : (a) AC (b) pulse with no pellets (c) pulse with pellets

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CO concentration increased significantly when the engine load was high. In order to achieve the higher NO x reduction, the NO 2 dissociation should be minimized. The total operating cost of the plasma-chemical hybrid system becomes $2,200/ton of NO, which is less than 1/6 of the conventional selective catalytic process.

ACKNOWLEDGEMENT

This work was partially supported by Grant-in-Aid for Scientific Research (B) of the Japanese Society for the Promotion of Science

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