Kinetic Modeling of Ozone Generation via Dielectric Barrier Discharges

A mathematical model combining chemical kinetic and reactor geometry is developed for ozone synthesis in dry O₂ streams with a wire-tube dielectric barrier discharge (DBD) reactor. Good agreement is found between the predicted ozone concentrations and experimental data. Sensitivity analysis is conducted to elucidate the relative importance of individual reactions. Results indicate that the ground-state oxygen atom is the most important species for O₃ generation; however, ozone generation will be inhibited if the O atom is overdosed. The excited species, that is, O(¹ D) and O₂(b ¹Σ), can decompose O₃ and suppress ozone synthesis. The model developed is then applied to modify the original DBD reactor design for the enhancement of ozone yield. With a thinner dielectric thickness, more than 10% increase of ozone concentration is achieved.     

On the Performance of Ozone Generators Working with Dielectric Barrier Discharges

The parameters, which determine the performance of ozone generators, are efficiency and maximum ozone concentration. The efficiency from oxygen has been found to be nearly independent on the kind of barrier discharge arrangement (volume, surface, coplanar), while the ozone concentration saturation level depends on the specific design of the generator. These phenomena are explained with features of the discharge process and the properties of chemical reactions, respectively. The importance of a limit in the energy density of the discharge is highlighted.     

Optimizing Factors on High Concentration of Ozone Production with Dielectric Barrier Discharge

The gap distance, electrode material, voltage and gas flow velocity were optimized with gas pressure variation of dielectric barrier discharge (DBD) for producing high concentration of ozone. There exists an optimum gas pressure at which the highest ozone concentration is produced with other parameters being fixed. This optimum gas pressure value changes accordingly as the other parameters changed. As the discharge continues at the optimum pressure, the ozone concentration could increase or decrease slowly. This aging effect has different characteristics with the metal electrode material and the impurity level of the oxygen gas used for ozone generation. The aging effect is supposed to be related with the catalytic effect of metal oxide, which is generated in the discharge zone. The change in the characteristic of optimum pressure by the other parameters, indicate that the ozone concentration is deeply related with the filament self-organization characteristics of DBD. At the final optimized condition, the ozone concentration was higher than 22.5 wt.%.     

Ozone Production in a High Frequency Dielectric Barrier Discharge Generator

Factors that affect the performance of an expanded-mesh dielectric barrier discharge ozone cell were investigated. A gas feed pf 94% O₂, 4% Ar and 1% N₂ was used. An improvement in the productivity (g ozone/kWh) of about 20 % was achieved by doubling the gas flow rate through the cell. Decreasing the cell operating frequency (in the range 72 kHz to 19 kHz) increased the productivity of the ozone generator at constant power. The ozone production increased approximately in proportion to the input power; however productivity did not vary significantly with power above a minimum level. As the cell voltage was increased the dependence of productivity on power or frequency was reduced. Changing the feed gas temperature between ? 5^°C and + 42^°C had no effect on productivity. Finer meshes drew more power than coarser ones for a given voltage. Using a thinner mesh for the centre electrode increased productivity. The best results were obtained with a 6 × 3 × 1.86 mm titanium mesh giving a productivity of 110 g ozone/kWhr at 30–60 W, 1500–1900V and 23 KHz.     

Ozone Production in a Dielectric Barrier Discharge with Ultrasonic Irradiation

Ozone production has been investigated using an atmospheric pressure dielectric barrier discharge in pure O₂ at room temperature with and without ultrasonic irradiation. It was driven at a frequency of either 15 kHz or ～40 kHz. The ozone production was highly dependent on the O₂ flow rate and the discharge power. Furthermore, powerful ultrasonic irradiation at a fundamental frequency of ～30 kHz with the sound pressure level of ～150 dB into the discharge can improve the ozone production efficiency, particularly when operated at the frequency of 15 kHz at the flow rate of 15 L/min.     

Influence of Field Strength and Energy Distribution of Different Barrier Discharge Arrangements on Ozone Generation

Because of different field strength and energy density distributions in volume (VD), surface (SD) and coplanar discharge (CD) arrangements the ozone yield will differ in general. While in VD configurations the initial field strength distribution is rather uniform, the situation is quite different in CD and especially SD devices. The distributions change during discharge development as well as the energy density in the discharge region and by this the ozone yields. The situation in SD arrangements is discussed in detail and is compared with those in VD and CD configurations.     

Ozone Production Influenced by Increasing Gas Pressure in Multichannel Dielectric Barrier Discharge for Positive and Negative Pulse Modes

This paper describes the influence of gas pressure on the conversion of O₂ to O₃ and the ozone production efficiency in a multichannel dielectric barrier discharge (DBD) reactor utilizing positive and negative pulses. Results show that conversion of O₂ to O₃ is continuously enhanced by the increase of gas pressure (0.1–0.24 MPa) while the rising speed of oxygen conversion with the increasing gas pressure at fixed specific input energy is reduced above 0.15 MPa. The maximum ozone generation efficiency is increased with increasing gas pressure (0–0.2 MPa) while positive pulse exhibits higher energy efficiency. The maximum ozone generation efficiency is suppressed with further increase of gas pressure (0.2–0.24 MPa) while no significant difference in ozone generation efficiency is observed for two unipolar pulse modes. Results also show that 0.2 MPa is the optimal working gas pressure to obtain the maximum ozone generation efficiency and increasing gas pressure would lead to remarkable increase of ozone generation efficiency for ozone production at high energy densities in multichannel DBD.     

Enhancement of Energy Yield for Ozone Production via Packed-Bed Reactors

The present work aims to enhance the energy yield of ozone production via packed-bed reactors. It has been experimentally demonstrated that ozone concentration and corresponding energy yield achieved by packed-bed reactors are significantly higher than that achieved by DBD only. The so-called packed-bed reactor is constructed by packing granular dielectric pellets within a DBD reactor. Two kinds of dielectric materials including glass beads and Al₂O₃ pellets are tested. Experimental results indicate that an ozone generator packed with Al₂O₃ pellets results in a higher ozone production compared with one packed with glass beads. The maximum ozone production takes place when Al₂O₃ pellets with diameter of 2 mm are packed. The maximum ozone concentration, ozone production rate, and energy yield achieved in this study are 61 gO₃/m³, 3.7 gO₃/hr, and 173 gO₃/kWh, respectively. The highest ozone concentration and energy yield achieved with the packed-bed reactor are about 8 and 12 times high as those with DBD reactor, respectively. Although the packed-bed reactors have a shortcoming of high temperature, it can be solved by adding a cooling system and the ozone generation can be improved thereof. As a result, the packed-bed reactor is a promising and state-of-the-art technology for ozone generation based on this study.     

Ozone Production by an Ultra-Short Triggered Dielectric Barrier Discharge.

This work was motivated by the ozone production improvement by a dielectric barrier discharge supplied with a high voltage triggered pulsed generator. Particular attention was focused on the ozone generator cell geometry and on the type of electrical generator. A comparative parametrical analysis on two configurations of reactor was performed: an annular and a surface configuration. This study emphasizes that surface discharges coupled to ultra-short triggered high voltage generators stand out as an efficient process to produce ozone in large quantities.     

Ozone Generation from Argon-Oxygen Mixtures in Presence of Different Packing Materials within Dielectric Barrier Discharge Gap

Assessments of ozone yield and concentration in Dielectric Barrier Discharge of argon-oxygen mixtures in presence of various packing materials are discussed. These include zeolite molecular sieve 13X pellets, Pyrex beads, Pyrex wool, and porous TiO₂-beads, which presented differential reactive surfaces, nano cavities, photo-catalysis, and dissimilar ionic environments. Their utility was evaluated in conjunction with varied gas composition, flow rate, and electrical inputs. In a mixture of 3–21% O₂ in argon, the ozone concentration ranged between 16–980 ppm, simultaneous measurements of in situ energy dissipation revealed its yield, G(O₃) to change independently from 0.002 to 2.020 μmol J^?1. TiO₂ packing emerged as the most versatile material to produce O₃ in high concentration and yield.     

Effective Ozone Generation in Oxygen Using a Mesh Electrode in an Ozonizer with Variable Linear Velocity

Results of studies on ozone synthesis under discharges proceeding in a metal mesh-ceramic dielectric system have been presented. The experiments were carried out in the reactor with unique reaction space geometry, in which the reacting gas flew with consequently increasing linear velocity. The high voltage electrode was made of a metal mesh, which caused intensification of the gas mixing in the reaction space. Using a simple reactor with one-side cooling of the reaction space, high ozone maximum concentrations (100 g/Nm³) and energy efficiencies (180–200 g/kWh) were obtained at 25 °C.     

A Study of Ozone Synthesis in Coaxial Cylinder Pulse Streamer Corona Discharge Reactors

Synthesis of ozone in coaxial cylinder non-thermal plasma reactors with different structures was investigated in this paper. With digital measuring technology, the absorption energy of non-thermal plasma reactors induced by pulse streamer corona was estimated. In the view of energy absorption of non-thermal plasma reactors, pulse input energy depended on reactor structures, as well as pulse parameters, such as pulse amplitude and DC bias. With coaxial cylinder reactors energized by pulse voltage, the influences on ozone generation of pulse voltage polarity, pulse amplitude, and pulse repetition rate were studied. It was found that positive pulse voltage induced higher ozone generation than negative pulse voltage and higher amplitude pulses generated more ozone. Increasing the pulse repetition rate at a low level increased ozone generation to some extent, but then leveled off with further increasing. A critical repetition rate was found at which the ozone synthesis was the most efficient. Lower pulse amplitude was associated with higher critical repetition rate. Superimposing DC bias on pulse voltage was an effective method to enhance ozone generation. Besides, discharge modes and electrode structures of reactors affect ozone generation. A mixed discharge mode of volume and surface discharges was the most effective mode to generate ozone in all of the experimental discharge modes, namely volume, surface, volume and surface mixed discharge modes. Moreover, helix-cylinder reactors were better than wire-to-cylinder reactors in generating ozone.     

Generation of Active Oxidant Species by Pulsed Dielectric Barrier Discharge in Water-Air Mixtures

Experimental research into the electrical and optical parameters of pulsed dielectric barrier discharge (PDBD) was undertaken. PDBD was applied to humid air containing water droplets as a means of water oxidative treatment with short-living species generated in the discharge zone. In spectral analysis of PDBD, only small concentrations of nitric oxides were detected at the resulting electric field strength and electron mean energy sufficient for generation of OH-radicals. The water droplets served as electric field strength concentrators: PDBD was ignited close to the water droplets' surface.     

The Effect of SF6 on Ozone Generation using Dielectric Barrier Discharge

This paper reports the results of an experimental study of effect of SF₆ on ozone generation within a Dielectric Barrier Discharge (DBD) fed by both pure oxygen and dry air. The chemical reaction mechanisms relevant to the process of ozone generation (and destruction) are discussed. The experimental results show the oxygen source should avoid the presence of SF₆ but the addition of a small amount of SF₆ in an air discharge can improve ozone concentration and ozone produce efficiency.     

Effect of MnOx/TiO2 Oxidation State on Ozone Concentration in a Nonthermal Plasma-Driven Catalysis Reactor

Manganese oxides on titanium dioxide were prepared by impregnation method at various calcination temperatures and by deposition-precipitation method and the catalysts were characterized using TG-DTA, XRD, XPS, and N₂ adsorption. Various oxidation states for manganese were obtained and activity towards ozone decomposition inside a nonthermal plasma catalysis reactor was investigated. Activity tests show that with increasing manganese oxidation state, the greater the degree of ozone decomposition inside the reactor. MnOx/TiO₂ prepared by impregnation method calcined at 350 °C showed the highest decrease in ozone concentration.     

Numerical Study of NOx Abatement Using Ozone Injection Integrated with Wet Absorption

Nitrogen oxides emitted from power plants and the chemical industry are poisonous to humans and animals, contribute to ozone depletion, and cause acid rain. More than 90% of nitrogen oxides (NO_x) consist of nitric oxide (NO), which is insoluble in water. Among the various available techniques of NO_x abatement, ozone injection is a promising method in which NO is oxidized to higher-order nitrogen oxides (NO₃, N₂O₃, N₂O₄, and N₂O₅), which can easily be absorbed in a wet scrubber. In this article, the ozone injection process integrated with an absorber column is numerically modeled and simulated at various operating conditions. The predicted results of NO_x oxidation with ozone injection and absorption in water agree with the published experimental results. The ozone injection process is modeled using a plug flow reactor, while the wet absorption is based on a rigorous rate-based RateFrac model. Detailed kinetic mechanisms of O₃-NO_x oxidation and absorption of nitrogen oxides in water are incorporated in the model to simultaneously predict the performance efficiency of the ozone reactor and absorber column. Thermodynamic properties of the components are estimated using an Electrolyte NRTL model. The influence of performance parameters (such as feed gas flow rate, inlet gas temperature, reactor configurations, ozone concentration, and NO/NO₂ molar ratio) on the oxidation efficiency of NO_x in the reactor and absorber column is investigated to predict the optimal operating conditions.     

Kinetic Modeling of Homogeneous Low-Temperature Multi-Pollutant Oxidation by Ozone

The features of the low-temperature (300–600 K) oxidation process by ozone are examined. The process is modeled employing “full” chemistry and simulated in a perfectly stirred reactor (PSR). The issues addressed include the rate of multi-pollutant of flue gas removed by the process, the critical temperature window, the range of ozone demand (if any) for high multi-pollutant removal and the impact of other species and residence time on multi-pollutant removal. The results are discussed in comparison with earlier experimental findings. For the simulated flue gas stream, the optimum temperature and ozone concentration required for high multi-pollutant removal are 400±20 K, 600–800 ppm, respectively.