WO2021113901A1 - Plasma water treatment - Google Patents
Plasma water treatment Download PDFInfo
- Publication number
- WO2021113901A1 WO2021113901A1 PCT/AU2020/051323 AU2020051323W WO2021113901A1 WO 2021113901 A1 WO2021113901 A1 WO 2021113901A1 AU 2020051323 W AU2020051323 W AU 2020051323W WO 2021113901 A1 WO2021113901 A1 WO 2021113901A1
- Authority
- WO
- WIPO (PCT)
- Prior art keywords
- gas
- dielectric barrier
- discharge zone
- liquid
- plasma
- Prior art date
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- HNPSIPDUKPIQMN-UHFFFAOYSA-N dioxosilane;oxo(oxoalumanyloxy)alumane Chemical compound O=[Si]=O.O=[Al]O[Al]=O HNPSIPDUKPIQMN-UHFFFAOYSA-N 0.000 description 1
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Classifications
-
- H—ELECTRICITY
- H01—ELECTRIC ELEMENTS
- H01J—ELECTRIC DISCHARGE TUBES OR DISCHARGE LAMPS
- H01J37/00—Discharge tubes with provision for introducing objects or material to be exposed to the discharge, e.g. for the purpose of examination or processing thereof
- H01J37/32—Gas-filled discharge tubes
- H01J37/32009—Arrangements for generation of plasma specially adapted for examination or treatment of objects, e.g. plasma sources
- H01J37/32348—Dielectric barrier discharge
-
- C—CHEMISTRY; METALLURGY
- C02—TREATMENT OF WATER, WASTE WATER, SEWAGE, OR SLUDGE
- C02F—TREATMENT OF WATER, WASTE WATER, SEWAGE, OR SLUDGE
- C02F1/00—Treatment of water, waste water, or sewage
- C02F1/46—Treatment of water, waste water, or sewage by electrochemical methods
- C02F1/4608—Treatment of water, waste water, or sewage by electrochemical methods using electrical discharges
-
- H—ELECTRICITY
- H01—ELECTRIC ELEMENTS
- H01J—ELECTRIC DISCHARGE TUBES OR DISCHARGE LAMPS
- H01J37/00—Discharge tubes with provision for introducing objects or material to be exposed to the discharge, e.g. for the purpose of examination or processing thereof
- H01J37/32—Gas-filled discharge tubes
- H01J37/32009—Arrangements for generation of plasma specially adapted for examination or treatment of objects, e.g. plasma sources
-
- C—CHEMISTRY; METALLURGY
- C02—TREATMENT OF WATER, WASTE WATER, SEWAGE, OR SLUDGE
- C02F—TREATMENT OF WATER, WASTE WATER, SEWAGE, OR SLUDGE
- C02F1/00—Treatment of water, waste water, or sewage
- C02F1/48—Treatment of water, waste water, or sewage with magnetic or electric fields
-
- H—ELECTRICITY
- H05—ELECTRIC TECHNIQUES NOT OTHERWISE PROVIDED FOR
- H05H—PLASMA TECHNIQUE; PRODUCTION OF ACCELERATED ELECTRICALLY-CHARGED PARTICLES OR OF NEUTRONS; PRODUCTION OR ACCELERATION OF NEUTRAL MOLECULAR OR ATOMIC BEAMS
- H05H1/00—Generating plasma; Handling plasma
- H05H1/24—Generating plasma
- H05H1/2406—Generating plasma using dielectric barrier discharges, i.e. with a dielectric interposed between the electrodes
- H05H1/2441—Generating plasma using dielectric barrier discharges, i.e. with a dielectric interposed between the electrodes characterised by the physical-chemical properties of the dielectric, e.g. porous dielectric
-
- H—ELECTRICITY
- H05—ELECTRIC TECHNIQUES NOT OTHERWISE PROVIDED FOR
- H05H—PLASMA TECHNIQUE; PRODUCTION OF ACCELERATED ELECTRICALLY-CHARGED PARTICLES OR OF NEUTRONS; PRODUCTION OR ACCELERATION OF NEUTRAL MOLECULAR OR ATOMIC BEAMS
- H05H1/00—Generating plasma; Handling plasma
- H05H1/24—Generating plasma
- H05H1/2406—Generating plasma using dielectric barrier discharges, i.e. with a dielectric interposed between the electrodes
- H05H1/2443—Generating plasma using dielectric barrier discharges, i.e. with a dielectric interposed between the electrodes the plasma fluid flowing through a dielectric tube
- H05H1/245—Generating plasma using dielectric barrier discharges, i.e. with a dielectric interposed between the electrodes the plasma fluid flowing through a dielectric tube the plasma being activated using internal electrodes
-
- H—ELECTRICITY
- H05—ELECTRIC TECHNIQUES NOT OTHERWISE PROVIDED FOR
- H05H—PLASMA TECHNIQUE; PRODUCTION OF ACCELERATED ELECTRICALLY-CHARGED PARTICLES OR OF NEUTRONS; PRODUCTION OR ACCELERATION OF NEUTRAL MOLECULAR OR ATOMIC BEAMS
- H05H1/00—Generating plasma; Handling plasma
- H05H1/24—Generating plasma
- H05H1/247—Generating plasma using discharges in liquid media
-
- C—CHEMISTRY; METALLURGY
- C02—TREATMENT OF WATER, WASTE WATER, SEWAGE, OR SLUDGE
- C02F—TREATMENT OF WATER, WASTE WATER, SEWAGE, OR SLUDGE
- C02F2101/00—Nature of the contaminant
- C02F2101/30—Organic compounds
- C02F2101/305—Endocrine disruptive agents
-
- C—CHEMISTRY; METALLURGY
- C02—TREATMENT OF WATER, WASTE WATER, SEWAGE, OR SLUDGE
- C02F—TREATMENT OF WATER, WASTE WATER, SEWAGE, OR SLUDGE
- C02F2101/00—Nature of the contaminant
- C02F2101/30—Organic compounds
- C02F2101/36—Organic compounds containing halogen
-
- C—CHEMISTRY; METALLURGY
- C02—TREATMENT OF WATER, WASTE WATER, SEWAGE, OR SLUDGE
- C02F—TREATMENT OF WATER, WASTE WATER, SEWAGE, OR SLUDGE
- C02F2201/00—Apparatus for treatment of water, waste water or sewage
- C02F2201/002—Construction details of the apparatus
- C02F2201/003—Coaxial constructions, e.g. a cartridge located coaxially within another
-
- C—CHEMISTRY; METALLURGY
- C02—TREATMENT OF WATER, WASTE WATER, SEWAGE, OR SLUDGE
- C02F—TREATMENT OF WATER, WASTE WATER, SEWAGE, OR SLUDGE
- C02F2201/00—Apparatus for treatment of water, waste water or sewage
- C02F2201/46—Apparatus for electrochemical processes
-
- C—CHEMISTRY; METALLURGY
- C02—TREATMENT OF WATER, WASTE WATER, SEWAGE, OR SLUDGE
- C02F—TREATMENT OF WATER, WASTE WATER, SEWAGE, OR SLUDGE
- C02F2201/00—Apparatus for treatment of water, waste water or sewage
- C02F2201/46—Apparatus for electrochemical processes
- C02F2201/461—Electrolysis apparatus
- C02F2201/46105—Details relating to the electrolytic devices
- C02F2201/46115—Electrolytic cell with membranes or diaphragms
-
- C—CHEMISTRY; METALLURGY
- C02—TREATMENT OF WATER, WASTE WATER, SEWAGE, OR SLUDGE
- C02F—TREATMENT OF WATER, WASTE WATER, SEWAGE, OR SLUDGE
- C02F2201/00—Apparatus for treatment of water, waste water or sewage
- C02F2201/46—Apparatus for electrochemical processes
- C02F2201/461—Electrolysis apparatus
- C02F2201/46105—Details relating to the electrolytic devices
- C02F2201/4612—Controlling or monitoring
- C02F2201/46125—Electrical variables
- C02F2201/46135—Voltage
-
- C—CHEMISTRY; METALLURGY
- C02—TREATMENT OF WATER, WASTE WATER, SEWAGE, OR SLUDGE
- C02F—TREATMENT OF WATER, WASTE WATER, SEWAGE, OR SLUDGE
- C02F2201/00—Apparatus for treatment of water, waste water or sewage
- C02F2201/46—Apparatus for electrochemical processes
- C02F2201/461—Electrolysis apparatus
- C02F2201/46105—Details relating to the electrolytic devices
- C02F2201/4619—Supplying gas to the electrolyte
-
- C—CHEMISTRY; METALLURGY
- C02—TREATMENT OF WATER, WASTE WATER, SEWAGE, OR SLUDGE
- C02F—TREATMENT OF WATER, WASTE WATER, SEWAGE, OR SLUDGE
- C02F2201/00—Apparatus for treatment of water, waste water or sewage
- C02F2201/48—Devices for applying magnetic or electric fields
-
- C—CHEMISTRY; METALLURGY
- C02—TREATMENT OF WATER, WASTE WATER, SEWAGE, OR SLUDGE
- C02F—TREATMENT OF WATER, WASTE WATER, SEWAGE, OR SLUDGE
- C02F2303/00—Specific treatment goals
- C02F2303/04—Disinfection
-
- C—CHEMISTRY; METALLURGY
- C02—TREATMENT OF WATER, WASTE WATER, SEWAGE, OR SLUDGE
- C02F—TREATMENT OF WATER, WASTE WATER, SEWAGE, OR SLUDGE
- C02F2305/00—Use of specific compounds during water treatment
- C02F2305/02—Specific form of oxidant
- C02F2305/023—Reactive oxygen species, singlet oxygen, OH radical
-
- H—ELECTRICITY
- H05—ELECTRIC TECHNIQUES NOT OTHERWISE PROVIDED FOR
- H05H—PLASMA TECHNIQUE; PRODUCTION OF ACCELERATED ELECTRICALLY-CHARGED PARTICLES OR OF NEUTRONS; PRODUCTION OR ACCELERATION OF NEUTRAL MOLECULAR OR ATOMIC BEAMS
- H05H2245/00—Applications of plasma devices
- H05H2245/20—Treatment of liquids
-
- H—ELECTRICITY
- H05—ELECTRIC TECHNIQUES NOT OTHERWISE PROVIDED FOR
- H05H—PLASMA TECHNIQUE; PRODUCTION OF ACCELERATED ELECTRICALLY-CHARGED PARTICLES OR OF NEUTRONS; PRODUCTION OR ACCELERATION OF NEUTRAL MOLECULAR OR ATOMIC BEAMS
- H05H2245/00—Applications of plasma devices
- H05H2245/30—Medical applications
- H05H2245/36—Sterilisation of objects, liquids, volumes or surfaces
Definitions
- the present invention relates to an apparatus and a method for treating water with a plasma, to water treated with a plasma and to methods of using the plasma treated water.
- Reactive species produced by plasma are known to be effective for the breakdown of certain biological and chemical materials that may be present in water. Water exposed to plasma derived reactive species may also be “activated” by introducing a range of reactive metastable species into the water.
- This Plasma Activated Water (PAW) may be used to treat materials exposed to it, so as to provide product decontamination including microbial, fungal, viral and chemical.
- the PAW may be used as a fertilizer or as a fuel.
- the plasma may be interfaced with the water via direct discharge to its surface, underwater discharge, discharge within submerged gas bubbles or via introduction of the reactive gas species as bubbles to the water bulk.
- the present invention seeks to provide an apparatus which will overcome or substantially ameliorate at least some of the deficiencies of the prior art, or to at least provide an alternative.
- an apparatus for treating a liquid with a plasma comprising a first dielectric barrier and a second dielectric barrier, said first and second dielectric barriers defining a discharge zone therebetween, and a high voltage electrode which is electrically insulated from the discharge zone by the first dielectric barrier.
- the second dielectric barrier is gas-permeable and the discharge zone is configured to accept a gas flow therethrough.
- the apparatus may additionally comprise an earthed electrode.
- the earthed electrode may be separated from the discharge zone by at least the second dielectric barrier.
- the earthed electrode and the discharge zone may be on opposite sides of the second dielectric barrier.
- the apparatus may additionally comprise a vessel for containing a liquid.
- the liquid in the vessel may be in contact with the second dielectric barrier.
- the liquid may be separated from the discharge zone by the second dielectric barrier.
- the term “separated from ... by”, for example “A is separated from B by C”, indicates that at least a portion of C is disposed between A and B such that A does not contact B. It does not imply that C is the only integer between A and B, although in certain instances it may be.
- the vessel comprises a dielectric material
- the apparatus comprises an earthed electrode in contact with the dielectric material.
- the earthed electrode may be disposed such that, in use, said dielectric material separates the liquid in the vessel from the earthed electrode.
- the earthed electrode may be disposed on the outside of the vessel. In this instance, in use, the liquid would be contained inside the vessel.
- the apparatus comprises an earthed electrode, which is disposed such that, in use, said earthed electrode is in electrical contact with the liquid in the vessel.
- the vessel is electrically conducting and comprises or forms the earthed electrode.
- a separate metallic earthed electrode is disposed within the liquid in the vessel, optionally disposed on an inside surface of the vessel.
- the high voltage electrode may be disposed within the first dielectric barrier. It may be surrounded by, enclosed in, or encased in, the first dielectric barrier. In one configuration, the high voltage electrode, the first dielectric barrier, the discharge zone and the second dielectric barrier are concentric. The high voltage electrode may be surrounded by the first dielectric barrier, which is surrounded by the discharge zone, which is in turn surrounded by the second dielectric barrier.
- the first dielectric barrier may be gas-impermeable. It may be impermeable to a gas used in the discharge zone. It may be impermeable to the liquid.
- the second dielectric barrier may be porous. It may be microporous. It may be permeable to any one or more of a gas in the discharge zone, the plasma species and the discharge itself. It may be hydrophobic. Alternatively it may be hydrophilic. It may have non-porous and/or gas impermeable regions, provided that at least part thereof is porous and/or gas permeable.
- the apparatus may comprise a gas inlet. This may enable a gas or gas mixture to enter the discharge zone. In some instances the discharge zone has a gas outlet but in other instances the second (gas-permeable) dielectric barrier serves as the only gas outlet.
- the apparatus may comprise a gas propulsion device, e.g. a pump, for passing a gas into the discharge zone through the gas inlet. In some instances, all of the gas entering the discharge zone exits the discharge zone through the outer dielectric barrier.
- the apparatus may comprise a high voltage generator. This may be capable of applying a voltage to the high voltage electrode sufficient to generate a plasma in a gas in the discharge zone.
- the voltage may be between about lkV RMS (root mean square) and about 150kV RMS.
- the high voltage generator may be electrically coupled to, and/or in electrical contact with, the high voltage electrode.
- an apparatus for treating a liquid with a plasma comprising a first dielectric barrier which is gas impermeable and a second dielectric barrier which is porous, said first and second dielectric barriers defining a discharge zone therebetween, and a high voltage electrode which is electrically insulated from the discharge zone by the first dielectric barrier.
- the discharge zone is configured to accept a gas flow therethrough.
- an apparatus for treating a liquid with a plasma comprising: a first dielectric barrier which is gas impermeable and a second dielectric barrier which is porous, said first and second dielectric barriers defining a discharge zone therebetween, a high voltage electrode which is electrically insulated from the discharge zone by the first dielectric barrier and encased therein, and a high voltage generator capable of applying a voltage to the high voltage electrode sufficient to generate a plasma in a gas in the discharge zone, said voltage commonly being between about lkV RMS and about 150kV RMS.
- the discharge zone is configured to accept a gas flow therethrough
- a method for treating a liquid with a plasma comprises providing an apparatus according to the first aspect, passing a gas through the discharge zone, exposing a side of the second dielectric barrier away from the discharge zone to the liquid; and applying a voltage to the high voltage electrode sufficient to generate a plasma in the gas in the discharge zone.
- the gas may be any one of air, nitrogen, oxygen, carbon dioxide, helium, neon, argon, xenon or it may be a mixture of any two or more of these.
- the gas may be air.
- the liquid may be an aqueous liquid. It may be water.
- the pressure difference across the second dielectric barrier may be sufficient to cause the gas to pass from the discharge zone into the liquid.
- the voltage may be between about lkV RMS and about 150kV RMS.
- the liquid may comprise one or more contaminants.
- the method may at least partially remove and/or destroy the contaminant(s).
- the contaminant(s) may be microorganisms or may be viruses or may be chemical contaminants, or the water may have any two or more of viral, microbial and chemical contaminants.
- the contaminant comprises PFAS (per- and/or poly-fluoroalkyl substances).
- PFAS per- and/or poly-fluoroalkyl substances
- it comprises one or more of pharmaceuticals, endocrine disruptors and PFAS.
- the method comprises: providing an apparatus for treating a liquid with a plasma, said apparatus comprising a first dielectric barrier and a second dielectric barrier, said first and second dielectric barriers defining a discharge zone therebetween, and a high voltage electrode which is electrically insulated from the discharge zone by the first dielectric barrier, wherein the second dielectric barrier is gas-permeable and the discharge zone is configured to accept a gas flow therethrough; passing a gas through the discharge zone, exposing a side of the second dielectric barrier away from the discharge zone to the liquid; and applying a voltage to the high voltage electrode sufficient to generate a plasma in the gas in the discharge zone.
- the method treats water which contains a microbial and/or chemical contaminant, the method comprising: providing an apparatus for treating the water with a plasma, said apparatus comprising a first dielectric barrier which is gas-impermeable and a second dielectric barrier which is porous, said first and second dielectric barriers defining a discharge zone therebetween, and a high voltage electrode which is electrically insulated from the discharge zone by the first dielectric barrier, wherein discharge zone is configured to accept a gas flow therethrough; passing a gas through the discharge zone and through the second dielectric barrier, exposing a side of the second dielectric barrier away from the discharge zone to the water; and applying a voltage of between about 1 and about 150kV RMS to the high voltage electrode.
- the method comprises: providing an apparatus for treating a liquid with a plasma, said apparatus comprising a first dielectric barrier and a second dielectric barrier, said first and second dielectric barriers defining a discharge zone therebetween, and a high voltage electrode which is electrically insulated from the discharge zone by the first dielectric barrier, wherein the second dielectric barrier is gas-permeable and the discharge zone is configured to accept a gas flow therethrough; passing a gas through the discharge zone, exposing a side of the second dielectric barrier away from the discharge zone to the liquid; and applying a voltage to the high voltage electrode sufficient to generate a plasma in the gas in the discharge zone; wherein the pressure difference across the second dielectric barrier is sufficient to cause the gas to pass from the discharge zone into the liquid.
- a third aspect of the invention there is provided use of water treated using the apparatus of the first aspect, or treated using the method of the second aspect, for human consumption.
- a process for preparing potable water comprising applying the method of the second aspect to contaminated water.
- a fifth aspect of the invention there is provided use of water treated using the apparatus of the first aspect, or treated using the method of the second aspect, for irrigating seeds, crops or other plants or for creating chemistry to be used as a fuel.
- a method for irrigating seeds, crops or other plants comprising treating water using the apparatus of the first aspect, or treating water using the method of the second aspect, and applying the water so treated to the seeds, crops or other plants or to soil in which the seeds, crops or other plants are disposed or are growing.
- the gas may be a nitrogen containing gas, or may be nitrogen itself, whereby the method of the second aspect generates nitrogenous species in the water which are beneficial to plant growth.
- plant growth nutrients and/or hormones and/or essential minerals may be added to the treated water subsequent to applying the method of the second aspect so as to further enhance the beneficial properties of the water.
- This invention may also be said broadly to consist in the parts, elements and features referred to or indicated in the specification of the application, individually or collectively, and any or all combinations of any two or more of said parts, elements or features, and where specific integers are mentioned herein which have known equivalents in the art to which this invention relates, such known equivalents are deemed to be incorporated herein as if individually set forth.
- Fig. 1 is an apparatus in accordance with one embodiment of the present invention.
- Fig. 2 is an apparatus in accordance with another embodiment of the present invention.
- Fig. 3 is a graph showing the production of reactive oxygen species (OH ⁇ , H2O2, O3) generated using the method of the present invention. Data curves show hydrogen peroxide (H2O2) [o]; ozone (O 3 ) [ ⁇ ]; hydroxyl radical (OH ⁇ ) [ ⁇ ] generation overtime [mg/L]
- the gas used is atmospheric air.
- the liquid is water.
- Fig. 4 shows graphs of: (a) nitrite production as a function of gas flowrate (SLM: standard litres per minute) employing the design from Fig. 1 with ground (i.e. an earthed electrode [IN]) directly in the water at 20° C; and (b) the effect of water temperature on nitrite generation under the conditions of (a) with a gas flowrate of 0.5 SLM.
- SLM gas flowrate
- Fig. 5 shows an example of the plasma gas excitation spectrum for air inside the reactor, showing the presence of excited nitrogen and oxygen species.
- the discharge is dominated by the excited nitrogen molecules and the first negative N2+ transition induced by the energetic electron collisions with O2 and N 2 molecules. Hydroxyl and atomic oxygen radicals are also evident.
- Fig. 6 is a photograph showing the apparatus in operation using CO2 as the supply gas, with the plasma discharge evident within the forming bubbles leaving the reactors.
- the setup consists of two reactors with 12 microholes of 200pm diameter.
- Fig. 7 is a photograph showing plasma discharges within forming bubbles leaving the porous reactor.
- the gas is argon.
- operating parameters may be appropriate for different gases used in the apparatus, and these may also be readily determined by the skilled person by reference to common general knowledge and/or by routine trial and error as well as to the guidance provided herein.
- Operating parameters that may need to be adjusted include gas flow rate, pressure across the second dielectric barrier, voltage supplied to the high voltage electrode, whether the earthed electrode is in electrical contact with the liquid or is electrically insulated therefrom etc. Some or all of these parameters may also be adjusted to accommodate different scales of the apparatus. For example an apparatus according to the invention which is designed to treat 1 L/minute of water may require different operating parameters (voltage, gas flow rate etc.) to an apparatus designed to treat 1 m 3 /minute. Also, as will be well understood, the dimensions of these two apparatuses will be different. Appropriate sizing can be readily determined without inventive input.
- dielectric barrier refers to an entity which separates two regions electrically, i.e. it divides one region from another and has high electrical resistivity. It may be physically permeable or may be physically impermeable or may be physically selectively permeable.
- the method may be employed to treat water or create plasma-activated water (PAW) for material decontamination, sterilization and plant growth promotion.
- the reactor i.e. the portion of the apparatus consisting of the first and second dielectric barriers, the discharge zone therebetween and the high voltage electrode
- the reactor is designed to be at least partially submerged in a liquid to be treated.
- This liquid may act as the earth, or a separate earth electrode may be provided.
- the separate earth electrode if present, may be in electrical contact with the liquid, either in the form of a discrete electrode in electrical contact with the liquid or in the form of an earthed vessel in which the liquid is contained, or else it may be electrically insulated from the liquid by means of a dielectric material.
- dielectric may be considered to refer to a substance with an electrical resistivity of between 0.01 and 10 15 Q.m.
- Suitable dielectrics for any or all of the first dielectric barrier, the second dielectric barrier and the dielectric material (if present) include ceramics, glasses and polymeric materials, e.g. glass, quartz, silica, aluminosilicate, polyolefins, fluoropolymers, polyamides, polyimides etc.
- any of the dielectrics used in the present invention may, independently, have a resistivity of from about 0.01 to aboutlO 15 Q.m, or about 1 to 10 15 , 10 3 to 10 15 , 10 7 to 10 15 , 10 10 to 10 15 , 0.01 to 10 10 , 0.01 to 10 5 , 0.01 to 10, 0.01 to 1, 1 to 10 10 , 10 5 to 10 10 or 100 to 10 7 Q.m, e.g. about 0.01, 0.1, 1, 10, 100, 1000, 10 4 10 5 , 10 6 , 10 7 , 10 8 , 10 9 , 10 10 , 10 11 , 10 12 , 10 13 , 10 14 or 10 15 Q.m.
- the second dielectric barrier is permeable to the gas and or plasma discharge.
- the second dielectric barrier may be hydrophobic, so as to prevent or inhibit an aqueous liquid from penetrating through it to the discharge zone and/or to facilitate passage of gas from the discharge zone through the second dielectric barrier. Alternatively it may be hydrophilic. In the event that the second dielectric barrier is porous, the pore size may be such as to prevent or inhibit leakage of the liquid into the discharge zone. A suitable gas pressure within the discharge zone may also serve to inhibit such leakage.
- Suitable pore sizes are from about 0.1 to about 2000 microns, or from about 0.1 to 1000, 0.1 to 500, 0.1 to 100, 0.1 to 50, 0.1 to 10, 1 to 2000, 10 to 2000, 100 to 2000, 500 to 2000, 500 to 1000, 1 to 1000, 1 to 100, 10 to 1000, 10 to 100 or 10 to 500 microns, e.g. about 0.1, 0.5, 1, 2, 5, 10 15, 20, 25, 30, 35, 40, 45, 50, 60, 70, 80, 90, 100, 150, 200, 250, 300, 350, 400, 450, 500, 600, 700, 800, 900, 1000, 1100, 1200, 1300, 1400, 1500, 1600, 1700, 1800, 1900 or 2000 microns.
- Suitable pressure differences across the second dielectric barrier are at least about lOkPa, or at least about 20, 30, 40, 50, 60, 70, 80, 90 or lOOkPa, or from about 10 to about lOOkPa, or about 10 to 50 10 to 20, 20 to 100, 50 to 100 or 20 to 50kPa, e.g. about 10, 15, 20, 25, 30, 34, 40, 45, 50, 60, 70, 80, 90 or lOOkPa.
- This pressure may be generated by adjusting the flow rate of the gas through the discharge zone and/or by constricting the outlet (if present) from the discharge zone. In some instances there is no outlet from the discharge zone other than the porous second dielectric barrier.
- the pressure difference across the second dielectric barrier is sufficient to cause gas and/or plasma to pass from the discharge zone into the liquid. This causes bubbles to form in the liquid. Plasma and/or plasma byproducts can then pass across the gas liquid barrier into the liquid so as to treat the liquid.
- the finer the pore size of the second dielectric barrier the smaller the bubbles that will be formed in the liquid, and hence the greater the gas-liquid interfacial area. Increasing the interfacial area increases the transfer rate and hence renders the treatment more efficient.
- the flow rate through the second dielectric barrier also reduces for a particular pressure across the second dielectric barrier.
- a suitable combination of pore size and pressure should be used to achieve a desired level of treatment efficiency. This combination may readily be determined by routine experimentation. If bubbles are to form within the liquid surrounding the second dielectric barrier, it is preferable for the liquid to be in contact with, or connected to, the outer atmosphere so as to prevent a build-up of pressure in the liquid.
- a range of plasma control parameters may be controlled in the apparatus including, discharge gap (i.e the thickness of the discharge zone), discharge volume (i.e. the volume of the discharge zone), voltage and frequency to produce controlled plasma reactive species in the water.
- a suitable discharge gap is from about 1 to about 50mm, or about 1 to 40, 1 to 30, 1 to 20, 1 to 10, 10 to 50, 20 to 50, 30 to 50, 40 to 50, 10 to 30 or 20 to 40mm, e.g. about 1, 2, 3, 4, 5, 6, 7, 8, 9, 10, 15, 20, 25, 30, 35, 40, 45 or 50mm.
- the discharge volume will depend on the discharge gap and the length of the discharge zone. In general, the size of the discharge zone will depend on the desired throughput of liquid to be treated.
- a suitable discharge volume is from about 10 2 to about 10 5 cm 3 , or about 10 2 to 10 2 , 10 2 to 1, 1 to 10 5 , 10 2 to 10 5 , 10 2 to 2*10 4 , 1 to 10 3 or 10 1 to 10cm 3 , e.g. about 10 2 , 5*10 2 , 0.1, 0.5, 1, 5, 10, 50, 100, 500, 1000, 5000, 10 4 , 2*10 4 , 5*10 4 or 10 5 cm 3 .
- a suitable discharge voltage is about 1 to about 150kV, or about 1 to 100, 1 to 50, 1 to 10, 10 to 150, 50 to 150, 100 to 150 or 50 to lOOkV, e.g.
- the applied voltage may be AC, DC or rectified AC. It may have a frequency of between about 1 and about 10 12 Hz, or about 1 to 10 10 , 1 to 10 8 , 1 to 10 6 , 1 to 10 4 , 1 to 10 2 , 10 2 to 10 12 , 10 4 to 10 12 , 10 6 to 10 12 , 10 8 to 10 12 , 10 10 to 10 12 , 10 2 to 10 6 , 10 6 to 10 10 or 10 4 to 10 8 , e.g.
- the method of the invention may be used for microbial or chemical decontamination for water, wastewater, food products, medical devices, or other objects where treatment with reactive water or liquids is effective.
- the apparatus and/or method of the present invention may operate at a temperature between about 10 and about 90°C, or between about 20 and 90, 30 and 90, 40 and 90, 50 and 90, 60 and 90, 70 and 90, 80 and 90, 10 and 80, 10 and 70, 10 and 60, 10 and 50, 10 and 40, 10 and 30, 10 and 20, 20 and 50, 50 and 80 or 20 and 40°C, e.g. about 10, 15, 20, 25, 30, 35, 40, 45, 50, 55, 60, 65, 70, 75, 80, 85 or 90°C.
- the reactive species created in the plasma may include Reactive Oxygen and Nitrogen Species (RONS), which usually include long-lived species like hydrogen peroxide (H2O2), ozone (O3), nitrate (NO 3 ) and nitrite (NO 2 ), and (relatively) short lived species such as hydroxyl radical (OH ⁇ ), nitric oxide (NO ⁇ ), atomic oxygen (O), peroxynitrate (OONO 2 ) and peroxynitrites (0N0070N00H).
- ROS Reactive Oxygen and Nitrogen Species
- Fig. 5 shows an example of the gas excitation spectrum for air, showing excited nitrogen and oxygen species in-situ within the reactor discharge gap. These species can lead to a lowering of the pH of the liquid.
- PAW can be used as an antimicrobial agent against bacteria, biofilms, fungi, amoebae and viruses. Similarly, it can breakdown chemical contaminants such as pesticides, antibiotics, pharmaceuticals and per- and poly- fluoroalkyl substances (PFAS). It can also be used as a plant fertilizer by utilizing nitrogen species produced such as nitrates and subsequently applied to plants or cells. Due to the reduction in pH, it may be necessary to adjust the pH of the liquid after treatment and prior to use. It may be necessary to neutralize the liquid.
- PFAS per- and poly- fluoroalkyl substances
- An atmospheric non-thermal plasma reactor is presented herein as a means to treat water and/or generate of PAW.
- the apparatus is capable of being sized so as to treat large quantities of liquid and/or to have high liquid throughput.
- the apparatus may be readily scaled so as to treat anywhere between about 1 to about 10,000L/hour or more, or about 1 to 1000, 1 to 100, 1 to 10, 10 to 10,000, 100 to 10,000, 1000 to 10,000 or 500 to 5000L/h, e.g. about 1 5, 10, 20, 50, 100, 200, 500, 1000, 2000, 5000 or 10,000 L/h or more than 10,000L/h.
- Parameters to be scaled in order to adjust the throughput include the diameter of the discharge zone, the discharge gap, the length of the discharge zone, the gas flow rate, the volume of the vessel containing the liquid etc.
- more than one reactor e.g. 2, 3, 4, 5, 6, 7, 8, 9 or 10, or more than 10 (a reactor being, as discussed earlier, the assembly of high voltage electrode, first and second dielectric barriers and the discharge zone between these barriers) may be immersed in the same body of liquid so as to increase the rate of treatment of the liquid.
- These may have the same dimensions and may operate at the same voltage, or may be different dimensions and/or may operate at different voltage.
- the liquid is treated batchwise. In other embodiments, the liquid is treated continuously. In such embodiments, the flow rate of the liquid through the apparatus may be controlled so as to provide effective treatment. If the flow rate is too high, insufficient plasma/plasma byproducts will contact the water to provide effective treatment.
- the reactor includes a high voltage electrode and a plasma discharge zone in the form of a Dielectric Barrier Discharge (DBD) with a gas inlet to the discharge zone.
- DBD Dielectric Barrier Discharge
- the DBD comprises (or consists of) a first and a second dielectric barrier and the discharge zone therebetween.
- the first, commonly inner, dielectric barrier which covers or surrounds the high voltage electrode for the DBD, may be made of quartz, glass, ceramic or polymeric material.
- the second, commonly outer, dielectric barrier surrounds the first dielectric barrier, so as to define the discharge zone between the first and second dielectric barriers.
- the reactor is submerged in water, with the water acting as the ground electrode, and is earthed either directly with a submerged electrode or electrically conductive water vessel or indirectly on the outside of a non-conductive water vessel.
- the direct insertion of the ground metal into the water changes the resulting chemistry of the reactor, with it acting as an electrochemical electrode.
- the second, commonly outer, dielectric barrier is porous to the flowing inducer gas, which acts as the gas outlet and the mechanism for introducing the plasma species to the water.
- the water is part of the apparatus, acting as the ground electrode for the DBD.
- the means by which this circuit is completed is important to the resultant chemistry. At least two options are considered. The first option is to use a remote electrode to the DBD which is submerged in the water to complete the electrical circuit. The second is to complete the circuit by grounding the wall of a non-metallic water vessel. For the first approach electrochemical reactions can take place at the electrode, which will be governed by its construction material and surface area.
- the outer barrier of the DBD may act not only as the outer wall of the discharge zone, maintaining the gas gap and a dielectric layer facilitating a stable plasma discharge, but also as the means for interfacing the plasma with the water.
- the controlled porosity of the second dielectric barrier means that gas plasma species can exit the DBD reactor.
- the pore size is designed to be sufficiently small to prevent an influx of water to the discharge gap.
- the pore size is also important in governing the size distribution of the bubbles formed.
- the porous DBD design minimises the time taken to introduce the reactive species formed into the liquid. However, the design permits more than merely the reactive gas species (plasma afterglow) formed in the discharge zone to be introduced. As the inducer gas passes through the pores, the plasma itself can exit and interface with the surrounding water. This approach not only increases the likelihood of introducing the short-lived species to the water but also may introduce solvated electrons into the water.
- UV light can also pass from the discharge zone through the outer dielectric barrier if it is constructed from a UV transmissive material such as quartz. The UV light may be generated by the plasma. It may assist in destroying contaminants in the water, in particular microorganisms and viruses.
- the DBD design can be scaled by the use of concentric tubes, where the annular gap of the discharge zone is dictated by the gas and discharge voltage gas input.
- the discharge volume per unit length can be increased by employing larger diameter inner and outer dielectric barriers for the DBD whilst maintaining the same gap between them.
- the discharge gap can therefore remain constant as the radii of both the inner and outer tubes are similarly increased. This design facilitates large volumes of gas breakdown without increasing the discharge gap, i.e. the distance between the two dielectric barriers.
- the apparatus By submerging the DBD reactor in the water, the apparatus has an effective heat sink to remove possible build-up of thermal energy by using natural forced convection. This may be enhanced if the apparatus is used in a continuous mode, i.e. if the water flows past the second dielectric barrier, thereby removing the heat from the overall system.
- the use of mixer elements can be used to increase convective heat transfer, but also governs the quantity of meta-stable and/or unstable species from the plasma in the bulk solution through mixing of the species with the bulk fluid.
- Suitable mixer elements may be present in the liquid, including active elements such as powered mixer blades and passive elements such as baffles.
- the apparatus may comprise a gas flow controller to control the volume of gas introduced to the discharge zone, the residence time of the gas in the discharge zone, the partial pressure in the discharge zone and the size of the bubbles which form in the liquid.
- a gas flow controller to control the volume of gas introduced to the discharge zone, the residence time of the gas in the discharge zone, the partial pressure in the discharge zone and the size of the bubbles which form in the liquid.
- a gas mixer for mixing the gases in a desired proportion. This may be located before the gas inlet so that the gases are mixed before entering the discharge zone. Alternatively, a supply of suitably mixed gases may be used.
- the apparatus may be powered by a pulsed AC voltage, a positive or negative DC voltage, or pulsed Radio Frequency voltage.
- the second dielectric barrier interfacing the gas and liquid, may be actively vibrated through ultrasonic waves, e.g. from about 20 kHz to about 1MHz (or from about 20 to 500, 20 to 100, 20 to 50, 50 to 1000, 100 to 1000, 500 to 1000, 100 to 500 or 200 to 700kHz, e.g. about 20, 30, 40, 50, 60, 70, 80, 90, 100, 150, 200, 250, 300, 350, 400, 450, 500, 600, 700, 800, 900 or lOOOkHz) to produce controlled bubbles in the nano- or micro-meter range. Small diameter bubbles are known to be more stable than larger ones and also to provide a larger interfacial surface area. This therefore may facilitate transfer of plasma and/or plasma byproducts into the liquid.
- ultrasonic waves e.g. from about 20 kHz to about 1MHz (or from about 20 to 500, 20 to 100, 20 to 50, 50 to 1000, 100 to 1000, 500 to 1000, 100 to 500 or 200 to 700kHz, e.g
- the first dielectric barrier is absent.
- the discharge zone is defined between the high voltage electrode and the second dielectric barrier. The high voltage electrode is therefore in contact with a gas in and/or passing through the discharge zone.
- the second dielectric barrier is non-porous and/or impermeable to a gas in and/or passing through the discharge zone.
- an outlet from the discharge zone is distinct from, although commonly in contact with, the second dielectric barrier.
- the outlet is disposed and designed to allow gas and/or discharge products to pass from the discharge zone into a liquid. This may therefore lead to treatment of the liquid by the gas and/or discharge products.
- the present invention provides a system for treating or activating optionally large volumes of water or liquids, comprising an apparatus configured to create an atmospheric plasma while submerged in water, the apparatus typically having: a high voltage electrode, an inner dielectric barrier surrounding the high voltage electrode, a discharge zone for flowing gas and a gas -permeable, generally porous, dielectric outer barrier interfacing the plasma and the water.
- the bulk water may act as the ground electrode. It may additionally or alternatively act as a heat sink.
- the discharge gap may therefore be maintained between non-porous and porous dielectric barriers.
- the working gas may be air or it may comprise at least two gases selected from air, nitrogen, oxygen, carbon dioxide and a noble gas.
- the plasma discharges may be directly contacted with water through the porous outer dielectric barrier. Plasma induced reactive gas species may be directly contacted with water through the porous second dielectric barrier.
- the voltage applied to the high voltage electrode may be at least about lkV RMS and a maximum of about 150kV RMS.
- the invention also provides a method of sterilizing or breaking down contaminants in water comprising immersing the apparatus described earlier herein in a volume of water to be treated, flowing a working gas or gases into the discharge zone of the apparatus; and inducing a plasma in the working gas using a high voltage differential between the high voltage electrode and the grounded water.
- the invention further provides a method of producing plasma activated water (PAW) comprising immersing the apparatus in a volume of water to be treated; flowing a working gas or gases into the discharge zone of the apparatus; and inducing a plasma in the working gas using a high voltage differential between the high voltage electrode and the grounded water;
- PAW plasma activated water
- Figs. 1 and 2 show diagrammatic representations of the apparatus of the present invention.
- a high voltage generator (not shown) is connected to high voltage metallic electrode 10.
- First dielectric barrier 20 surrounds high voltage electrode 10 to form a sheathed electrode. The effect of dielectric barrier 20 is to limit the current flowing between electrode 10 and earth and to prevent the formation of arcs.
- Dielectric barrier 20 also physically separates high voltage electrode 10 from discharge zone 30, which surrounds dielectric barrier 20 and prevents contact between high voltage electrode 10 and any water which may enter discharge zone 30 due to insufficient pressure within discharge zone 30.
- Discharge zone 30 is maintained between the outer surface of inner dielectric barrier 20 and the inner surface of outer dielectric barrier 40. The distance of the gap between inner dielectric barrier 20 and outer dielectric barrier 40 (i.e.
- Outer dielectric barrier 40 is porous in order to allow gas and/or plasma to pass from discharge zone 30, where plasma is generated, to water in contact with outer dielectric barrier 40.
- the water in contact with outer dielectric barrier 40 is earthed by means of metallic earth connection 50, whereas in Fig. 2 earth connection 50 is coupled to non-metallic vessel 60 which contains the water.
- inducer gas enters discharge zone 30 through an inlet valve and exits through porous outer dielectric barrier 40.
- Porous dielectric barrier 40 acts as both a means of maintaining the gap of discharge zone 30 and of interfacing the plasma discharge and its reactive species into the surrounding water.
- a plasma is formed in the inducer gas flowing through discharge zone 30.
- the inducer gas passes into the water surrounding outer dielectric barrier 40, it takes with it plasma and/or plasma byproducts which treat the water. These may serve to kill microorganisms in the water and/or destroy or degrade noxious chemicals therein They may also be used as chemicals such as fertilizers and fuels.
- Figure 6 shows the apparatus in operation using CO2 as the supply gas, with the plasma discharge evident within the forming bubbles leaving the reactor’s microholes.
- Figure 7 shows plasma discharges within forming bubbles leaving the porous reactor.
- plastic shall be construed to mean a general term for a wide range of synthetic or semisynthetic polymerization products, and generally consisting of a hydrocarbon-based polymer.
Abstract
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KR20090054483A (en) * | 2007-11-27 | 2009-06-01 | 주식회사 에스디알앤디 | Underwater plasma producing apparatus and method using thereof |
KR20090097340A (en) * | 2008-03-11 | 2009-09-16 | 주식회사 다원시스 | Sewage purify method using dbd plasma discharge |
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