Direct water treatment by APGD with rotating electrodes

The APGD with rotating star-shaped electrodes was applied directly to the surface of liquid as a counter electrode. It was shown that the rotation of electrodes enables the stabilization of the discharged. A high concentration of H₂O₂ and nitrates were measured. The high level of microbial reduction...

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Veröffentlicht in:Problems of Atomic Science and Technology
Datum:2023
Hauptverfasser: Golota, V., Mohanty, P., Zavada, L.
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Zitieren:Direct water treatment by APGD with rotating electrodes / V. Golota, P. Mohanty, L. Zavada // Problems of Atomic Science and Technology. — 2023. — № 4. — С. 147-150. — Бібліогр.: 9 назв. — англ.

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Digital Library of Periodicals of National Academy of Sciences of Ukraine
id nasplib_isofts_kiev_ua-123456789-196193
record_format dspace
spelling Golota, V.
Mohanty, P.
Zavada, L.
2023-12-11T12:37:05Z
2023-12-11T12:37:05Z
2023
Direct water treatment by APGD with rotating electrodes / V. Golota, P. Mohanty, L. Zavada // Problems of Atomic Science and Technology. — 2023. — № 4. — С. 147-150. — Бібліогр.: 9 назв. — англ.
1562-6016
PACS: 52.77.−j, 52.80.−s, 52.80.Hc
DOI: https://doi.org/10.46813/2023-146-147
https://nasplib.isofts.kiev.ua/handle/123456789/196193
The APGD with rotating star-shaped electrodes was applied directly to the surface of liquid as a counter electrode. It was shown that the rotation of electrodes enables the stabilization of the discharged. A high concentration of H₂O₂ and nitrates were measured. The high level of microbial reduction was shown for inoculated deionized water treated by APGD with rotating electrodes.
Використовувався тліючий розряд атмосферного тиску (APGD) між обертовим зіркоподібним електродом і поверхнею води в якості другого електрода. Показано, що обертання електродів дозволяє стабілізувати розряд. Була зафіксована висока концентрація H₂O₂ та нітратів. Високий рівень мікробного зменшення було показано для інокульованої деіонізованої води, обробленої APGD з обертовими електродами.
en
Національний науковий центр «Харківський фізико-технічний інститут» НАН України
Problems of Atomic Science and Technology
Gas discharge, plasma-beam discharge and their applications
Direct water treatment by APGD with rotating electrodes
Безпосередня обробка води APGD з обертовими електродами
Article
published earlier
institution Digital Library of Periodicals of National Academy of Sciences of Ukraine
collection DSpace DC
title Direct water treatment by APGD with rotating electrodes
spellingShingle Direct water treatment by APGD with rotating electrodes
Golota, V.
Mohanty, P.
Zavada, L.
Gas discharge, plasma-beam discharge and their applications
title_short Direct water treatment by APGD with rotating electrodes
title_full Direct water treatment by APGD with rotating electrodes
title_fullStr Direct water treatment by APGD with rotating electrodes
title_full_unstemmed Direct water treatment by APGD with rotating electrodes
title_sort direct water treatment by apgd with rotating electrodes
author Golota, V.
Mohanty, P.
Zavada, L.
author_facet Golota, V.
Mohanty, P.
Zavada, L.
topic Gas discharge, plasma-beam discharge and their applications
topic_facet Gas discharge, plasma-beam discharge and their applications
publishDate 2023
language English
container_title Problems of Atomic Science and Technology
publisher Національний науковий центр «Харківський фізико-технічний інститут» НАН України
format Article
title_alt Безпосередня обробка води APGD з обертовими електродами
description The APGD with rotating star-shaped electrodes was applied directly to the surface of liquid as a counter electrode. It was shown that the rotation of electrodes enables the stabilization of the discharged. A high concentration of H₂O₂ and nitrates were measured. The high level of microbial reduction was shown for inoculated deionized water treated by APGD with rotating electrodes. Використовувався тліючий розряд атмосферного тиску (APGD) між обертовим зіркоподібним електродом і поверхнею води в якості другого електрода. Показано, що обертання електродів дозволяє стабілізувати розряд. Була зафіксована висока концентрація H₂O₂ та нітратів. Високий рівень мікробного зменшення було показано для інокульованої деіонізованої води, обробленої APGD з обертовими електродами.
issn 1562-6016
url https://nasplib.isofts.kiev.ua/handle/123456789/196193
citation_txt Direct water treatment by APGD with rotating electrodes / V. Golota, P. Mohanty, L. Zavada // Problems of Atomic Science and Technology. — 2023. — № 4. — С. 147-150. — Бібліогр.: 9 назв. — англ.
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fulltext ISSN 1562-6016. Problems of Atomic Science and Technology. 2023. № 4(146) 147 https://doi.org/10.46813/2023-146-147 DIRECT WATER TREATMENT BY APGD WITH ROTATING ELECTRODES V. Golota 1 , P. Mohanty 1 , L. Zavada 2 1 University of Michigan, Deaborn, MI, USA; 2 National Science Center “Kharkov Institute of Physics and Technology”, Kharkiv, Ukraine E-mail: golota@umich.edu The APGD with rotating star-shaped electrodes was applied directly to the surface of liquid as a counter elec- trode. It was shown that the rotation of electrodes enables the stabilization of the discharged. A high concentration of H2O2 and nitrates were measured. The high level of microbial reduction was shown for inoculated deionized water treated by APGD with rotating electrodes. PACS: 52.77.−j, 52.80.−s, 52.80.Hc INTRODUCTION The Atmospheric Pressure Glow Discharge (APGD) is one of the most widely used sources of Low- Temperature Nonequilibrium Plasma, which has found broad industrial applications including gas and water treatment, chemical conversion and materials synthesis, food processing and medicine [1]. Visually APGD di- vides into two zones: bright – ionization layer and glow- ing – diffuse/drift zone [2]. Near a sharp electrode, a strong electric field forms a narrow ionization layer, in which enough charged particles are generated for the self-sustaining development of the discharge. The dif- fuse zone with a relatively low electric field covers the remaining (biggest) part of the discharge gap. The com- plex plasma-chemical processes, as well as the transpor- tation of charged particles to the electrode, occur in the diffuse zone. APGD has attracted the attention of many researchers [3] because the entire discharge gap oper- ates as a plasma-chemical reactor and provides chemical reactivity at low gas temperature. However, APGD has one significant weakness, it is an uncontrollable transi- tion/contraction of the discharge from the volume dis- charge mode to the spark mode with a thin hot discharge channel. Such a transition to the spark has a destructive effect on the electrodes, changes the variety of generat- ed reactive species and remains an exceptional chal- lenge both for experimental studies and for many emerging applications. There are three common practices to control early transition to the spark. They are: (i) ballast resistors in discharge circuit, (ii) high speed gas flow, and (iii) very short pulse duration of applied HV. Ballast resistors are used to prevent sparks by reducing the voltage across the discharge gap when the discharge current exceeds a predetermined limit. Laroussi et al. [4] realized stable APGD by using suitable material with resistivity in the range of 10 9 …10 10 Ω instead of using dielectric layer normally used in Dielectric Barrier Discharge. The high-speed gas flow has a more complex effect on the discharge. Akishev et al. [5] used point-to-sphere elec- trode geometry and a fast gas flow to produce APGD by DC negative corona discharge. They studied in detail the effect of the electrode geometry and gas flow veloci- ty on the transition of corona-to-glow and glow-to-spark mode in ambient air. They demonstrated that a high- speed gas flow disperses the charged cloud formed in the discharge gap and reduces its shielding effect; addi- tionally, the gas and the electrode surface are cooled down by the gas flow, helping to keep the ionization rate at its lowest level. Typically, the APGD with high- speed gas flow works for applications requiring large volumes of gas to be treated with a relatively low con- centration of active species. The short HV pulse dura- tion (usually a range of nanoseconds) with the short voltage rising time is a relatively new and very effective method to generate APGD, however this technic re- quires a complex HV pulsed power supply with pulses of nanoseconds range which has a poor power efficien- cy (usually less than 50%). Moreover, EMI shielding is a challenge for these HV short pulse power generators. All these three methods for the discharge stabiliza- tion are currently being used in a broad range of practi- cal applications. However, as highlighted in the report “The 2022 Plasma Roadmap” [3], novel and expanding fields of applications for low-temperature plasma re- quire the development of new and unique low- temperature plasma sources with high energy efficiency, specifically, capable operated with liquid electrodes and/or in high humidity plasma-forming gases. In conventional APGD systems, when the electrodes are stationary, upon application of high voltage across the electrodes, the ionization of gases begins in vicinity of the tip of the sharp electrode, and then the ionization front propagates through the discharge gap either in the form of a streamer or in the form of an ionization wave. However, due to the weakness of the electric field at a distance from the sharp electrode, i.e., in the diffuse zone, the electrons begin to attach to molecules and atoms forming a charged cloud that shields the sharp electrode, and the ionization around the sharp electrode comes to the end until the charged cloud disperse and decay, and then the shielding effect comes to the end and the cycle will be repeated again. Because the mobil- ity of ions and charged molecules is low, the next dis- charge cycle will develop and pass along the same dis- charge channel that was formed in the previous dis- charge cycle. The repeated pass through the same chan- nel will heat the channel, the pressure in the channel will drop and ionization will increase, and, as result, the spark breakdown occurs. Although details of the spark breakdown mechanism remain unclear, the above- described mechanism of the thermal instability for a spark is well established. As the transition of APGD to 148 ISSN 1562-6016. Problems of Atomic Science and Technology. 2023. № 4(146) the spark has unpredictable behavior, a major challenge for many low-temperature plasma applications is to keep the APGD stable and operating at high specific power input. In this article, the innovative Atmospheric Pressure Glow Discharge with Rotating Electrode will be exam- ined for the direct plasma water treatment. Over the conventional stationary electrode discharge system, the rotating electrode has a significant advantage. The rota- tion of electrodes allows stabilization of the discharge, shifts the glow-to-spark transition towards higher volt- age and increases the specific energy input to the dis- charge. The physical phenomena behind these ad- vantages can be explained as follows. When the elec- trode rotation speed is higher than the ion drift velocity, the tips of the sharp electrodes surrounded by the ioni- zation layer will run away from the diffuse zone of the discharge, increasing the electrical resistance of the discharge gap and, therefore, continuing to stabilize the discharge. In addition, the tips movement will elongate and rupture the discharge channel, preventing the for- mation of a spark. Further, the electrode movement through the gas will lead to cooling down of the electrode tips and mixing of the gas in the discharge gap. Thus, a plasma system with rotating electrodes can potentially be a promising way to suppress thermal instability in a low- temperature plasma-chemical reactor. This is especially relevant for the discharge with liquid electrodes and high humidity plasma-feeding gases. EXPERIMENTAL SET-UP To study the effect of direct treatment of water by APGD, a device with rotating electrodes was built. The device includes a shaft with a set of star-like electrodes; reactor housing; overflow bath/tray; water tank; recircu- lation water pump; an electric motor with gears joined to the shaft and HV power supply unit connected to the rotating shaft. Fig. 1 shows the schematic drawing of the developed device. Fig. 1: The schematic of the experimental system with rotating electrodes The set of star-like electrodes disposed radially along the longitudinal axis of the plasma-chemical reac- tor and individual star-like electrodes separated with spacer from one another. The shaft with a set of star-like electrodes is rotationally supported in the isolated reac- tor housing by a pair of bearings, one end of the shaft joined to the electrical motor through a gearbox with 1:1 ratio. The gears are made from insulating material to provide electrical isolation for the motor. The power regulator module sets the rotation speed for star-like electrodes up to 10000 RPM. The bottom part of the reactor housing is open to allow discharge above the water surface of the overflowing bath. The water over- flows to the water tank and then the recirculating pump continuously pumps water back to the overflowing bath to keep the water level stable, as well as a distance be- tween tips of rotating electrodes and water surface. The total water volume was 4.4 liters, the rate of recirculat- ing pump is 3 lpm. An electrical contact for a high volt- age supply is provided at the other end of the shaft with star-like electrodes. The adjustable DC high voltage power supply (0…20 kV, 0…5 mA) with positive polar- ity was used to power the plasma-chemical reactor. The current and voltage signals from the reactor were gathered by the high voltage probe Tektronix P6015A and current probe Tektronix CT2 and were analyzed with oscilloscope Tektronix TDS 3034. The digital power meter KUMAN KW-47 was used to con- trol the total power input to the plasma-chemical reac- tor. The electrode rotation speed was controlled with the digital laser tachometer EXTECH 461920-NIST, range 2-99.000 RPM. The temperature and humidity were measured by the thermo-hygrometer Michell Instru- ments MDM25. To test water parameters the following devices and kits were used: Thermo Scientific Orion Star A211 pH Meter with 9165BNWP Sure-Flow pH electrode and 927007MD ATC probe; Myron L Ultrapen PT1 EC/TDS 1-9999 µS or ppm; Hach Water Quality Test strips: Nitrate 0…50 ppm, Nitrite 0…3.0 ppm; Water- Works Hydrogen peroxide test strips 0.5…100 ppm (0.5-2-5-10-25-50-100 ppm); Chemetrics Dissolved Ozone Meter with Vacu-vials Kit I-2019 0-5.0ppm. RESULTS AND DISCUSSION Plasma-Liquid surface interaction is an emerging and fast-growing topic of the Low Temperature Plasma research because they offer unique conditions that ena- ble decontamination of pathogens, synthesis of nano- materials, and treat of contaminated water. Plasma- Liquid discharge makes a very complex impact on the water surface such as charged particles, UV photons, electric field, reactive species (O3, OH, NOx). Result of such interaction is the saturation of interfacial water layer with ozone, reactive oxygen species and reactive nitrogen species, hydrogen peroxide, increasing of acidity and mixing of the water, all this together give a strong effect on water contaminants, including high oxi- dative stresses on bacteria and other pathogens [6]. But the challenge with keeping a steady Plasma-Liquid Dis- charge is that the surface of the liquid is extremely unsta- ble due to the electric field and the influence of the ionic wind. Further, the water surface is also unstable due to the water flowing through the reactor. Waves on the water surface lead to fluctuations in the height of the discharge gap and an early transition of the glow-to- spark. As was mentioned above, one of the new and most promising methods to stabilize the Plasma-Liquid Dis- charge is the rotation of the electrodes. Let’s make the estimation of the threshold velocity which is required to stabilize the discharge. Because the rotation of elec- trodes should suppress the thermal instability, the rota- tion speed of electrode pins should be higher compared to the ion drift velocity. The ion mobility in air at at- mospheric pressure, μ, is estimated to be in the range of ISSN 1562-6016. Problems of Atomic Science and Technology. 2023. № 4(146) 149 1.5…2.2 cm 2 ·V −1 ·s −1 depending on the humidity [7]. The electric field in the diffusing zone of the discharge is typically in a range 3…5 kV·cm -1 . Therefore, the estima- tion for average ion drift velocity is (5…10)∙10 2 cm·s -1 . When the electrode has a diameter of 65 mm, the tips of electrodes get a velocity of 10∙10 2 cm/s if the rotation speed is 3000 RPM. For the same electrode with the diameter of 65 mm, at rotation speed 6000 RPM, the velocity of the electrode tips will be 20∙10 2 cm·s -1 , which is greater than the speed of a charged cloud decay in the diffused zone, associated with an ion drift veloci- ty of (5…10)∙10 2 cm·s -1 . New streamers or ionization waves will be formed in the fresh/low ionized air, which should prevent the development of thermal instability that occurs due to the propagation of multiple streamers along the same channel. The stable running APGD with rotat- ing electrodes above the water surface is shown in Fig. 2. Fig. 2. Prototype reactor with rotary electrode with liquid counter electrode As mentioned above, the APGD above the water surface is very effective in generating active particles. As an example, the variation in discharge characteristics and water parameters during the treatment of deionized water with a total volume of 4.4 l using positive polarity APGD with a rotating electrode above the water surface is shown in Table 1. The total treatment time was 360 min, measurements and samples were taken after 0, 30, 60, 90, 120, 240, and 360 min. Table 1 Plasma and water characterization during direct water treatment by APGD with rotating electrodes, rotation speed – 4400 rpm Treatment time, min 0 30 60 90 120 240 360 I, mA 0 2.4 2 2 2 2 2 V, kV 0 15.2 15.3 15.3 15.6 15.6 15.6 Power, W 0 49 47 48 47 47 46 pH 6 6 5.5 5 5 4.5 4.5 EC, uS/cm 40 120 186 240 305 496 740 H2O2, ppm 0 1 4 7 10 17 20 NO3, ppm 0 3 5 10 12 25 30 NO2, ppm 0 0 0 0 0 0 0 O3, ppm 0 0 0 <0.5 <0.5 <0.5 <0.5 Twater, °C 26 29 32 33 33 36 35 The concentration of the dissolved ozone in the plasma treated water is very low, less than 0.5 ppm (see Table 1), due to the suppression of ozone synthesis under the high humidity condition and low ozone trans- fer rate through the water surface compared to gas-water mixing system, for example, Venturi injectors. Further, the presence of strong oxidizers (H2O2 and O3) in water makes the nitrite concentration (NO2-) almost zero. The concentration of nitrates (NO3-) and hydrogen peroxide (H2O2) in treated water is given in Table 1 and shown in Fig. 3. Fig. 3. Variation of concentration H2O2 and NO2 in the deionized water exposed to APGD. Total water volume is 4.4 l. Average discharge power is around 50 W It was expected that nitrate would accumulate in the water and that the concentration of nitrates (NO3-) would increase with treatment time, but the concentra- tion of hydrogen peroxide was surprisingly high. This can be explained by the high humidity conditions in the discharge and may indicate the presence of the high concentration of OH-radicals [8]. During treatment, the temperature of the water slow- ly rises because of the heating from the discharge and submersible recirculation pump. Fig. 4 shows the varia- tion in pH and electrical conductivity EC of the treated water at different treatment time under the APGD with the rotating electrodes. Fig. 4. pH and EC measurement in the deionized water exposed to APGD with the rotating electrodes. Total water volume is 4.4 l. Average discharge power is around 50 W As expected, the pH level decreases during plasma treatment, and it correlates with an increase of NO3 con- centration. However, the rapid linear increase in electrical conductivity EC of the treated water, which is a function of the accumulation of ions in the water, cannot be ex- plained either by the concentration of nitrate ions NO3, nor by the concentration of hydrogen peroxide, because for the electrical conductivity EC of 700…800 uS/cm, the concentration of ions must be in 10 times greater com- pared to the measured concentration of nitrate ions NO3. Perhaps the rapid linear increase in electrical conductivity EC can be explained by the accumulation of hydrogen ions H+ (or hydronium H3O+) in water, which has high 150 ISSN 1562-6016. Problems of Atomic Science and Technology. 2023. № 4(146) ion mobility, and many other reactive ions that were not measured in the current tests. More importantly, these reactive species in plasma- activated water, namely reactive oxygen species and reactive nitrogen species, such as nitric oxide radicals, nitrite, nitrate, atomic oxygen and ozone, can provide the strong antimicrobial effect [9] by inducing high oxidative stress on bacteria and other pathogens. To examine the microbial reduction ability of APGD with the rotating electrode, 1.5 l of deionized water was inoculated with 1 ml E. coli test cultures. The initial concentration of E. coli in the bulk water averaged be- tween 7.05E5 to 1.88E6 CFU/ml. The water was then circulated through the system without plasma discharge. The 0-minute sample was collected immediately before the start of plasma treatment. The electrode rotation and plasma power supply were then started, and water sam- ples were collected every 15 min thereon. The average power of the plasma was ~50 W, in positive polarity. The treated water samples were serial diluted (1:10, 1:10 2 , 1:10 3 , 1:10 4 , 1:10 5 ), plated and incubated for enumeration. Images of Petri dishes with samples of different dilution after incubation 36 hours are shown in Fig. 5. Table 2 shows the test data of water samples taken from inoculated water treated by APGD for 0, 15, 30, 45, and 60 min. Fig. 5. Images of Petri dishes with water samples treat- ed by APGD for 0, 15-, 30-, 45- and 60-min. Dilution 1:10, 1:10 2 , 1:10 3 , 1:10 4 , 1:10 5 Table 2 Microbial reduction during direct water treatment by APGD with rotating electrodes (TNC – Too Numerous to Count) Sample, min 0 15 30 45 60 pH 6 6 6 5.5 5.5 H2O2, ppm 0 1.5 5 5 7 Bacteria counts 1:10 TNC TNC 400+ 8 0 1:10 2 TNC TNC 387 0 0 1:10 3 400+ 385 52 0 0 1:10 4 133 28 1 1 0 1:10 5 19 5 1 0 0 The data presented in Table 2 is a composite of 3 repetition tests. As shown, a greater than 4 log reduction of E. coli was observed after 45 min of APGD treatment of the inoculated deionized water. CONCLUSIONS The innovative Atmospheric Pressure Glow Dis- charge with Rotating Electrode was tested for direct plasma discharge treatment of water. It demonstrated both the high level of microbial reduction and the high concentration of hydrogen peroxide in plasma treated water. Over the conventional stationary electrode dis- charge system, the rotating electrode enables the im- proving of the long-term stability of discharge, sup- pressing thermal instability, and increasing the specific power consumption of the discharge. REFERENCES 1. A. Fridman. Plasma Chemistry. Cambridge Univer- sity Press. 2008, p. 978. 2. V.I. Karas’, V.I. Golota, O.V. Bolotov, B.B. Kadolin, D.V. Kudin. Specific Features of Ra- diation from a Negative Air Corona Operating in the Trichel-Pulse Mode // Plasma Physics Reports. 2008, v. 34, № 10, p. 879-884. 3. I. Adamovich et al. The 2022 Plasma Roadmap: low temperature plasma science and technology // J. Phys. D: Appl. Phys. 2022, v. 55, p. 373001. 4. M. Laroussi, I. Alexeff, J.P. Richardson, F.F. Dyer. The resistive barrier discharge // IEEE Trans. Plas- ma Sci. 2002, v. 30 (1), p. 158-159. 5. Yu. Akishev, O. Goossens, T. Callebaut, C. Leys, A. Napartovich, N. Trushkin. The influence of elec- trode geometry and gas flow on corona-to-glow and glow-to-spark threshold currents in air // J. Phys. D. 2001, v. 34, p. 2875-2882. 6. P.J. Bruggeman, A. Bogaerts, J.M. Pouvesle, E. Robert, and E.J. Szili. Plasma-liquid interactions // J. Appl. Phys. 2021, v. 130, p. 200401. 7. Y. Liu, S. Huang, and L. Zhu. Influence of Humidity and Air Pressure on the Ion Mobility Based on Drift Tube Method // CSEE Journal of Power and Energy Systems. September 2015, v. 1, № 3, p. 37-41. 8. P.J. Bruggeman, R.R. Frontiera, U.R. Kortshagen, M.J. Kushner, S. Linic, G.C. Schatz, H. Andaraar- achchi, S. Exarhos, L.O. Jones, C.M. Mueller, C.C. Rich, C. Xu, Y. Yue, and Y. Zhang. Plasma- driven Solution Electrolysis // J. Appl. Phys. 2021, v. 129, p. 200902. 9. D. Laroque, S. Seo, G. Valencia, J. Laurindo, B. Carciofi. Cold plasma in food processing: Design, mechanisms, and application // Journal of Food En- gineering. 2022, v. 312, p. 110748. Article received 10.07.2023 БЕЗПОСЕРЕДНЯ ОБРОБКА ВОДИ APGD З ОБЕРТОВИМИ ЕЛЕКТРОДАМИ В. Голота, П. Моханті, Л. Завада Використовувався тліючий розряд атмосферного тиску (APGD) між обертовим зіркоподібним електро- дом і поверхнею води в якості другого електрода. Показано, що обертання електродів дозволяє стабілізувати розряд. Була зафіксована висока концентрація H2O2 та нітратів. Високий рівень мікробного зменшення було показано для інокульованої деіонізованої води, обробленої APGD з обертовими електродами. https://uigelz.eecs.umich.edu/pub/articles/JAP_129_200902_2021.pdf https://uigelz.eecs.umich.edu/pub/articles/JAP_129_200902_2021.pdf