DeNOx Study in Diesel Engine Exhaust Using Barrier DischargeCorona Assisted by V2O5／TiO2 Catalyst

A plasma-assisted catalytic reactor was used to remove nitrogen oxides (NOx) from diesel engine exhaust operated under different load conditions. Initial studies were focused on plasma reactor (a dielectric barrier discharge reactor) treatment of diesel exhaust at various temperatures. The nitric oxide (NO) removal efficiency was lowered when high temperature exhaustwas treated using plasma reactor. Also, NO removal efficiency decreased when 45% load exhaust was treated. Studies were then made with plasma reactor combined with a catalytic reactor consisting of a selective catalytic reduction (SCR) catalyst, V2O5/TiO2. Ammonia was used as a reducing agent for SCR process in a ratio of 1:1 to NOx. The studies were focused on temperatures of the SCR catalytic reactor below 200℃. The plasma-assisted catalytic reactor was operated well to remove NOx under no-load and load conditions. For an energy input of 96 J/1, the NOx removal efficiencies obtained under no-load and load conditions were 90% and 72% respectively at an exhaust temperature of 100℃.     

Catalyst-Packed Non-Thermal Plasma Reactor for Removalof Nitrogen Oxides

A single-stage plasma-catalytic reactor in which catalytic materials were packed was used to remove nitrogen oxides. The packing material was scoria being made of various metal oxides including Al2O3, MgO, TiO2, etc. Scoria was able to act not only as dielectric pellets but also as a catalyst in the presence of reducing agent such as ethylene and ammonia. Without plasma discharge, scoria did not work well as a catalyst in the temperature range of 100℃ to 200℃, showing less than 10% of NOx removal efficiency. When plasma is produced inside the reactor, the NOx removal efficiency could be increased to 60% in this temperature range.     

A Cascaded Discharge plasma—Adsorbent Technique for Engine Exhaust Treatment

A cascaded system of electrical discharges(non-thermal plasma)and adsorption process was investigated for the removal of oxides of Nitrogen(NOx) and total hydrocarbons (THC) from an actual diesel engine exhaust.The non-thermal plasma and adsorption processes were separately studied first and then the casecaded procxess was studied.In this study,different types of adsorbents were used.The NOx removal efficiency processes and the removal efficiency was found almost invariant in time.When associated by plasma,among the adsorbents studied.Activated charcoal and MS-13X were more effective for NOx and THC removal respectively.The experiments were conducted at no load and at 50% load conditions.The plasma reactor was kept at room temperature throughout the experiment,while the temperature of the adsorbent reactor was varied.A relative comparison of adsorbents was discussed at the end.     

Injection of N-Radicals into Diesel Engine Exhaust Treated by Plasma for Improved NOx Removal： A Feasibility Study

Reported in this paper is a feasibility study on the injection of plasma induced N radicals for the abatement of NO and NOx present in the actual diesel exhaust. The radical laden diesel exhaust was further treated by discharge plasma in a dielectric barrier discharge reactor. N radicals were produced in a separate plasma reactor filled with BaTiO3 pellets and were then injected into the treatment zone, There was a significant improvement in the efficiency when the radicals were injected compared to that when there was no radical injection. The efficiency of NOx removal at 0 load with plasma alone was 14% whereas with the injection of N radicals it went up to 38%, The results of the experiments conducted at different loads are discussed,     

Removal of Nitrogen Oxides in Diesel Engine Exhaust by Plasma Assisted Molecular Sieves

This paper reports the studies conducted on removal of oxides of nitrogen (NOx) from diesel engine exhaust using electrical discharge plasma combined with adsorbing materials such as molecular sieves. This study is being reported for the first time. The exhaust is taken from a diesel engine of 6 kW under no load conditions. The characteristic behavior of a pulse energized dielectric barrier discharge reactor in the diesel exhaust treatment is reported. The NOx removal was not significant (36%) when the reactor without any packing was used. However, when the reactor was packed with molecular sieves (MS -3A, -4A & -13X), the NOx removal efficiency was increased to 78% particularly at a temperature of 200℃ . The studies were conducted at different temperatures and the results were discussed.     

The Influence of Iron on Ammonium Ion Generation from Nitrate Ion in Liquid Phase

Flue gas cleaning in discharge plasma process has been Studied intensively and we have tried to remove the NOx and S02 using the wet-type plasma reactor. In this system, NO is oxidized to NO2 and absorbed as NO3^-, and SO2 is absorbed as SO3^2- and oxidized in the liquid to SO4^2-. But the concentration of NO3^- was saturated and the absorption of NOx and SO2 was inhibited. Then, the reduction of NO3^- in the liquid is required. We examined the reductive reaction of NO3^- to NH4^ using discharge above the liquid surface then the pH value of the liquid was changed to alkaline slightly. When the Fe plate was used as a ground electrode in the liquid, NH4^ was generated. Then, the relation between the generation of NH4^ and Fe ions (Fe^2 and Fe^3 ) was studied. When Fe^2 was presented in the liquid, NH4^ was generated and Fe^2 was oxidized to Fe^3 . Fe^2 is required to generate NH4^ from NO3^-. When NH4^ was generated from NO3^-, both the calculated pH value from NH4^ concentration and the measured pH value indicated a similar value. From these results, the discharge above the liquid surface was effective to convert NO3^- to NH4^ and the reductive reaction leads to more absorption of NO3^-. These results showed that the wet-type plasma reactor is effective for NOx and SO2 removal system.     

NO reduction using low-temperature SCR assisted by a DBD method

This paper discusses the removal of nitric oxide(NO) with low-temperature selective catalytic reduction driven by a dielectric barrier discharge with ammonia(NH_3) as a reductant. We explored the effects of NH_3, O_2, temperature and water under different applied voltage on NO removal at atmospheric pressure. The results showed that when the gas concentration ration of NH_3/NO was 0.23–0.67, the NO removal efficiency and the energy consumption was acceptable. The NO removal efficiency reached 84% under an applied voltage of 7 kV, 400 ppm NO and 90 ppm NH_3 at a temperature of 150 ℃. Water vapor had a negative effect because NO formation reactions were strengthened and NH_3 was oxidized directly rather than reduced NO molecules. The outlet gas components were observed via Fourier transform infrared spectroscopy for revealing the decomposition process and mechanism.     

NO_x storage and reduction assisted by non-thermal plasma over Co/Pt/Ba/γ-Al_2O_3 catalyst using CH_4 as reductant

N_Ox storage and reduction(NSR) technology has been regarded as one of the most promising strategies for the removal of nitric oxides(NO_x) from lean-burn engines, and the potential of the plasma catalysis method for NO_x reduction has been confirmed in the past few decades. This work reports the NSR of nitric oxide(NO) by combining non-thermal plasma(NTP) and Co/Pt/Ba/γ-Al_2O_3(Co/PBA) catalyst using methane as a reductant. The experimental results reveal that the NO_x conversion of NSR assisted by NTP is notably enhanced compared to the catalytic efficiency obtained from NSR in the range of 150 °C–350 °C, and NO_x conversion of the 8% Co/PBA catalyst reaches 96.8% at 350°C. Oxygen(O_2) has a significant effect on the removal of NO_x, and the NO_x conversion increases firstly and then decreases when the O_2 concentration ranges from 2% to 10%. Water vapor reduces the NO_x storage capacity of Co/PBA catalysts on account of the competition for adsorption sites on the surface of Co/PBA catalysts. There is a negative correlation between sulfur dioxide(SO_2) and NO_x conversion in the NTP system, and the 8% Co/PBA catalyst exhibits higher NO_x conversion compared to other catalysts, which shows that Co has a certain SO_2 resistance.     

Removal of NO and SO2 in Corona Discharge Plasma Reactor with Water Film

In this paper, a novel type of a corona discharge plasma reactor was designed, which consists of needle-plate-combined electrodes, in which a series of needle electrodes are placed in a glass container filled with flue gas, and a plate electrode is immersed in the water. Based on this model, the removal of NO and SO2 was tested experimentally. In addition, the effect of streamer polarity on the reduction of SO2 and NO was investigated in detail. The experimental results show that the corona wind formed between the high-voltage needle electrode and the water by corona discharge enhances the cleaning efficiency of the flue gas because of the presence of water, and the cleaning efficiency will increase with the increase of applied dc voltage within a definite range. The removal efficiency of SO2 up to 98%, and about 85% of NO~ removal under suitable conditions is obtained in our experiments.     

Conversion of NO with a catalytic packed-bed dielectric barrier discharge reactor

This paper discusses the conversion of nitric oxide (NO) with a low-temperature plasma induced by a catalytic packed-bed dielectric barrier discharge (DBD) reactor.Alumina oxide (Al2O3),glass (SiO2) and zirconium oxide (ZrO2),three different spherical packed materials of the same size,were each present in the DBD reactor.The NO conversion under varying input voltage and specific energy density,and the effects of catalysts (titanium dioxide (TiO2) and manganese oxide (MnOx) coated on Al2O3) on NO conversion were investigated.The experimental results showed that NO conversion was greatly enhanced in the presence of packed materials in the reactor,and the catalytic packed bed of MnOx/Al2O3 showed better performance than that of TiO2/Al2O3.The surface and crystal structures of the materials and catalysts were characterized through scanning electron microscopy analysis.The final products were clearly observed by a Fourier transform infrared spectrometer and provided a better understanding of NO conversion.     

High-efficiency removal of NO_x using dielectric barrier discharge nonthermal plasma with water as an outer electrode

With the rapid increase in the number of cars and the development of industry, nitrogen oxide(NO_x)emissions have become a serious and pressing problem. This work reports on the development of a water-cooled dielectric barrier discharge reactor for gaseous NOxremoval at low temperature. The characteristics of the reactor are evaluated with and without packing of the reaction tube with 2 mm diameter dielectric beads composed of glass, ZnO, MnO_2, ZrO_2, or Fe_2O_3. It is found that the use of a water-cooled tube reduces the temperature, which stabilizes the reaction, and provides a much greater NO conversion efficiency(28.8%) than that obtained using quartz tube(14.1%) at a frequency of 8 k Hz with an input voltage of 6.8 k V. Furthermore,under equivalent conditions, packing the reactor tube with glass beads greatly increases the NO conversion efficiency to 95.85%. This is because the dielectric beads alter the distribution of the electric field due to the influence of polarization at the glass bead surfaces, which ultimately enhances the plasma discharge intensity. The presence of the dielectric beads increases the gas residence time within the reactor. Experimental verification and a theoretical basis are provided for the industrial application of the proposed plasma NO removal process employing dielectric bead packing.     

A comparative study on the activity of TiO2 in pulsed plasma under different discharge conditions

In the present study,a combination of pulsed discharge plasma and TiO_2(plasma/TiO_2)has been developed in order to study the activity of TiO_2by varying the discharge conditions of pulsed voltage,discharge mode,air flow rate and solution conductivity.Phenol was used as the chemical probe to characterize the activity of TiO_2in a pulsed discharge system.The experimental results showed that the phenol removal efficiency could be improved by about 10%by increasing the applied voltage.The phenol removal efficiency for three discharge modes in the plasma-discharge-alone system was found to be highest in the spark mode,followed by the spark–streamer mode and finally the streamer mode.In the plasma/TiO_2system,the highest catalytic effect of TiO_2was observed in the spark–streamer discharge mode,which may be attributed to the favorable chemical and physical effects from the spark–streamer discharge mode,such as ultraviolet light,O_3,H_2O_2,pyrolysis,shockwaves and high-energy electrons.Meanwhile,the optimal flow rate and conductivity were 0.05 m~3l~(-1)and 10μS cm~(-1),respectively.The main phenolic intermediates were hydroquinone,catechol,and p-benzoquinone during the discharge treatment process.A different phenol degradation pathway was observed in the plasma/TiO_2system as compared to plasma alone.Analysis of the reaction intermediates demonstrated that p-benzoquinone reduction was selectively catalyzed on the TiO_2surface.The effective decomposition of phenol constant(D_e)increased from 74.11%to 79.16%when TiO_2was added,indicating that higher phenol mineralization was achieved in the plasma/TiO_2system.     

Unfiltered Diesel Engine Exhaust Treatment by Discharge Plasma：Effect of Soot Oxidation

A cascaded system of electrical discharges (Non-thermal plasma), catalyst and adsorption process was investigated for the removal of oxides of nitrogen (NOx) and carbon monoxide (CO) from a Diesel engine raw exhaust. The three processes were separately studied first, and then the cascaded processes, namely plasma-catalyst and plasma-adsorbent, were investigated. In this paper main emphasis was laid on the effect of carbonaceous soot oxidation on the plasma treatment process. While the cascaded plasma-catalyst process exhibits a higher CO removal,the cascaded plasma-adsorbent process exhibits a higher NOx removal. The experiments were conducted under no-load. The plasma and adsorbent reactors were kept at room temperature throughout the experiment while the catalyst reactor was kept at 200℃ / 300℃.     

Experimental study on toluene removal by a two-stage plasma-biofilter system

Volatile organic compounds (VOCs) are typical pollutants that affect air quality. Discharge plasma is thought to be a potential method that can remove VOCs from flue gas. In this experiment, pulsed corona discharge plasma combined with a biological tower was carried out to remove the benzene series, and toluene was selected as the typical VOC. The results indicated that the removal efficiency of toluene by pulsed corona plasma was slightly higher than that of direct current (DC) corona plasma, while its energy efficiency was much higher than DC corona plasma. Under the optimal experimental conditions of pulse voltage 8.5 kV, initial toluene concentration 1400 mg m−3, and toluene flow rate of 12 l h−1, the toluene removal efficiency reached 77.11% by the single method of pulsed corona discharge plasma, and the energy efficiency was up to 1.515 g/(kW·h) under the pulse voltage of 4.0 kV. The trickling biofilter was constructed by using the screened and domesticated Acinetobacter baumannii, and the highest toluene removal efficiency by the pulsed corona discharge plasma combined with the trickling biofilter rose up to 97.84%. Part of the toluene was degraded into CO2, H2O, and some intermediate products such as o-diphenol under the influence of Acinetobacter baumannii. When the remaining waste gas passed through the discharge plasma reactor, the benzene ring structure could be directly destroyed by the collision between toluene and plasma. Meanwhile, O·, OH·, and some other oxidizing radicals generated by the discharge also join into the oxidative decomposition of toluene and its intermediate products, thereby further improving the removal efficiency of toluene. Therefore, the two-stage plasma-biofilter system not only showed a high toluene removal efficiency, but also had a good energy efficiency. The results of this study will provide theoretical support and technical reference for industrial VOC treatment.     

Novel electrode structure in a DBD reactor applied to the degradation of phenol in aqueous solution

Phenol degradation experimental results are presented in a similar wastewater aqueous solution using a non-thermal plasma reactor in a coaxial dielectric barrier discharge. The novelty of the work is that one of the electrodes of the reactor has the shape of a hollow screw which shows an enhanced efficiency compared with a traditional smooth structure. The experimentation was carried out with gas mixtures of 90% Ar–10% O_2, 80% Ar–20% O_2 and 0% Ar–100% O_2. After one hour of treatment the removal efficiency was 76%, 92%, and 97%, respectively, assessed with a gas chromatographic mass spectrometry technique. For both reactors used, the ozone concentration was measured. The screw electrode required less energy, for all gas mixtures, than the smooth electrode, to maintain the same ozone concentration. On the other hand, it was also observed that in both electrodes the electrical conductivity of the solution changed slightly from~0.0115 S m~(-1) up to ~0.0430 S m~(-1) after one hour of treatment. The advantages of using the hollow screw electrode structure compared with the smooth electrode were:(1) lower typical power consumption,(2) the generation of a uniform plasma throughout the reactor benefiting the phenol degradation,(3) a relatively lower temperature of the aqueous solution during the process, and(4) the plasma generation length is larger.     

Plasma-catalytic degradation of tetracycline hydrochloride over Mn/γ-Al2O3 catalysts in a dielectric barrier discharge reactor

A coaxial dielectric barrier discharge (DBD) reactor was used for plasma-catalytic degradation of tetracycline hydrochloride over a series ofMn/γ-Al₂O₃ catalysts prepared by the incipient wetness impregnation method. The combination of plasma and theMn/γ-Al₂O₃ catalysts significantly enhanced the degradation efficiency of tetracycline hydrochloride compared to the plasma process alone, with the 10%Mn/γ-Al₂O₃ catalyst exhibiting the best tetracycline hydrochloride degradation efficiency. A maximum degradation efficiency of 99.3% can be achieved after 5 min oxidation and a discharge power of 1.3 W, with only 69.7% by a single plasma process. The highest energy yield of the plasma-catalytic process is 91.7 gkWh⁻¹. Probable reaction mechanisms of the plasma-catalytic removal of tetracycline hydrochloride were also proposed.     

Application of dielectric barrier discharge (DBD) plasma packed with glass and ceramic pellets for SO2 removal at ambient temperature: optimization and modeling using response surface methodology

Air pollution is a major health problem in developing countries and has adverse effects on human health and the environment. Non-thermal plasma is an effective air pollution treatment technology. In this research, the performance of a dielectric barrier discharge (DBD) plasma reactor packed with glass and ceramic pellets was evaluated in the removal of SO₂ as a major air pollutant from air in ambient temperature. The response surface methodology was used to evaluate the effect of three key parameters (concentration of gas, gas flow rate, and voltage) as well as their simultaneous effects and interactions on the SO₂ removal process. Reduced cubic models were derived to predict the SO₂ removal efficiency (RE) and energy yield (EY). Analysis of variance results showed that the packed-bed reactors (PBRs) studied were more energy efficient and had a high SO₂ RE which was at least four times more than that of the non-packed reactor. Moreover, the results showed that the performance of ceramic pellets was better than that of glass pellets in PBRs. This may be due to the porous surface of ceramic pellets which allows the formation of microdischarges in the fine cavities of a porous surface when placed in a plasma discharge zone. The maximum SO₂ RE and EY were obtained at 94% and 0.81 g kWh⁻¹, respectively under the optimal conditions of a concentration of gas of 750 ppm, a gas flow rate of 2 l min⁻¹, and a voltage of 18 kV, which were achieved by the DBD plasma packed with ceramic pellets. Finally, the results of the model's predictions and the experiments showed good agreement.     

The Degradation of Organic Pollutants by Bubble Discharge in Water

Organic pollutants could be degraded by using bubble discharge in water with gas aeration in the discharge reactor and more plasma can be generated in the discharge process.When pulsed high voltage was applied between electrodes with gas aerated into the reactor,it showed that bubbles were broken,which meant that breakdown took place.It could also be observed that the removal rate of phenol increased with increasing discharge voltage or pulse frequency,and with reducing initial phenol concentration or solution electric conductivity.It could remove more amount of phenol by oxygen aeration.With increasing oxygen flow rate,the removal rate increased.There was little difference with air or nitrogen aeration for phenol removal.The solution temperature after discharge increased to a great extent.However,this part of energy consumption did not contribute to the reaction,which led to a reduction in the energy utilization efficiency.     

Regulation characteristics of oxide generation and formaldehyde removal by using volume DBD reactor

Discharge plasmas in air can be accompanied by ultraviolet(UV) radiation and electron impact,which can produce large numbers of reactive species such as hydroxyl radical(OH·),oxygen radical(O·),ozone(O3),and nitrogen oxides(NOx),etc.The composition and dosage of reactive species usually play an important role in the case of volatile organic compounds(VOCs) treatment with the discharge plasmas.In this paper,we propose a volume discharge setup used to purify formaldehyde in air,which is configured by a plate-to-plate dielectric barrier discharge(DBD) channel and excited by an AC high voltage source.The results show that the relative spectral-intensity from DBD cell without formaldehyde is stronger than the case with formaldehyde.The energy efficiency ratios(EERs) of both oxides yield and formaldehyde removal can be regulated by the gas flow velocity in DBD channel,and the most desirable processing effect is the gas flow velocity within the range from2.50 to 3.33 m s-1.Moreover,the EERs of both the generated dosages of oxides(O3 and NO2) and the amount of removed formaldehyde can also be regulated by both of the applied voltage and power density loaded on the DBD cell.Additionally,the EERs of both oxides generation and formaldehyde removal present as a function of normal distribution with increasing the applied power density,and the peak of the function is appeared in the range from 273.5 to 400.0 W l-1.This work clearly demonstrates the regulation characteristic of both the formaldehyde removal and oxides yield by using volume DBD,and it is helpful in the applications of VOCs removal by using discharge plasma.     

Evaluation of trans-ferulic acid degradation by dielectric barrier discharge plasma combined with ozone in wastewater with different water quality conditions

In this study, dielectric barrier discharge plasma and ozone(O_3) were combined to synergistically degrade trans-ferulic acid(FA), and the effect of water quality on FA degradation was studied. The results showed that 96.9% of FA was degraded after 40 min treatment by the plasma/O_3 process. FA degradation efficiency increased with the p H values. The presence of suspended solid and humic acid inhibited FA degradation. FA degradation efficiency increased as the water temperature increased to 30 °C. However, the further increase in water temperature was adverse for FA degradation. Effects of common inorganic ions on FA degradation were also investigated. The addition of Cl~- inhibited the FA degradation, whileCO_3~(2-) had both negative and positive influences on FA degradation.NO_3~- andSO_4~(2-) did not have significant effect on FA degradation. Fe~(3+)and Cu~(2+)benefited FA degradation through the Fenton-like and catalytic ozonation reactions.