CN102427653A - Atmospheric non-equilibrium plasma source for introducing mini-glow discharge mode - Google Patents

Atmospheric non-equilibrium plasma source for introducing mini-glow discharge mode Download PDF

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CN102427653A
CN102427653A CN2011102785455A CN201110278545A CN102427653A CN 102427653 A CN102427653 A CN 102427653A CN 2011102785455 A CN2011102785455 A CN 2011102785455A CN 201110278545 A CN201110278545 A CN 201110278545A CN 102427653 A CN102427653 A CN 102427653A
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electrode
glow discharge
dielectric layer
discharge
pin
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CN102427653B (en
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俞哲
张芝涛
白敏冬
田一平
许少杰
金忠林
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Dalian Maritime University
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Dalian Maritime University
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Abstract

The invention discloses an atmospheric non-equilibrium plasma source for introducing a mini-glow discharge mode and belongs to the technical field of gas discharge and application. A high-voltage electrode component is arranged between two parallel grounding electrode components to form a dual ionization chamber structure; a needle array electrode for an atmospheric local strong electric field induction device is arranged at any one electrode and forms a multi-needle plate discharge electrode structure with a corresponding plate electrode; and an alpha-Al2O3 dielectric layer uniformly covers the surface of the plate electrode, wherein metal Ag or Au is coated on one side in contact with a discharge electrode under the conditions of a discharging gap distance of 0.25 to 0.64mm, a working air pressure of 90 to 110kPa, a cooling water temperature of between 5 and 10 DEG C, an excitation voltage of 5 to 10kV and an excitation frequency of 5 to 50kHz. The plasma source can alternatively work in a mini-glow discharge mode and a mini-flow discharge mode, the discharging electric-field strength is effectively improved through mini-glow discharge, and richer active particles are provided for a plasma chemical reaction.

Description

A kind of atmospheric pressure nonequilibrium plasma source of introducing little glow discharge pattern
Technical field
The invention belongs to gas discharge and applied technical field, relate to a kind of gas discharge low temperature plasma source, especially a kind of atmospheric pressure nonequilibrium plasma source of introducing little glow discharge pattern take place.
Background technology
The atmospheric pressure nonequilibrium plasma and in modern times the application in fields such as industry, the energy, resource environment, national defence be the scientific and engineering that has global effect 21 century, handle at the preparation of high-efficiency activated oxygen radical, material surface, ozone is synthetic, ultraviolet source, high power CO 2Fields such as laser, Plasma Display, plasma chemistry and environmental protection obtain extensive use, have realized the unapproachable treatment effect of conventional method, have represented the nonequilibrium plasma important use and have been worth.Low pressure nonequilibrium plasma generation technique with traditional is compared; The topmost advantage of atmospheric pressure nonequilibrium plasma is that it does not need huge and complicated vacuum system and the vacuum (-tight) housing reactor with strict seal, therefore is particularly suitable for the industrial demand of continuity.At present, the method that produces the atmospheric pressure nonequilibrium plasma mainly contains corona discharge, microwave discharge and dielectric barrier discharge etc., wherein atmospheric dielectric barrier discharge simple in structure, obtain the large space nonequilibrium plasma easily, the most representative.
In the atmospheric dielectric barrier discharge system; Miniflow annotate discharge mode be main, the most common, also be the discharge mode of realization the most easily; This discharge mode is used the history in year surplus in the of existing 100 in the synthetic field of industrial ozone, but adopts the plasma chemical reaction usefulness of this discharge mode not high always so far.Annotating discharge with miniflow compares; Glow discharge has plasma chemical reaction performance more efficiently; But under atmospheric pressure realize very difficulty of large space glow discharge; Only can under He compression ring border, realize at present having limited the application of glow discharge pattern in plasma chemical reaction by Atomospheric pressure glow discharge.
Theoretical according to gas discharge; In the inhomogeneous field discharging structure, if driving voltage is brought up to a certain degree, cathodic electricity corona meeting very soon by Trichel pulsed discharge mode transition to the steady glow discharge mode; The yardstick of this glow discharge is very little; When needle plate type electrode spacing was 20~40mm, the radial dimension of glow discharge also only had 0.04~0.07mm, but had the region of discharge architectural feature similar with classical low pressure glow discharge.In cycle, surpass 400/cm at a driving voltage if can produce at discharge space 2Little glow discharge, the generation efficient of active particle will significantly improve.The Yu Zhe of the Maritime Affairs University Of Dalian etc. utilized pin-plate dielectric barrier discharge structure in 2010; Adopt 10kHz, the excitation of 6kV high-frequency high-voltage; In the narrow discharging gap of 0.3~1.2mm, realized glow discharge (Maritime Affairs University Of Dalian's master thesis of minute yardstick; 2010), experimental verification utilize the atmospheric dielectric barrier discharge system also can produce little glow discharge pattern.
In dielectric barrier discharge; Utilize the ballast effect of dielectric layer to produce the micro discharge that quantity is huge, structure dimension is close, characteristic is identical in the cycle at the same driving voltage of same discharge space, in most cases this micro discharge shows as the discharge mode that miniflow is annotated.If with dull and stereotyped dielectric barrier electrode structural change is spininess-plate dielectric barrier discharge structure; Improve the structure and the performance of dielectric layer simultaneously; And improve excitation electrical field intensity, just can produce quantity at the negative half-cycle of discharge space intrinsic motivation electric field and surpass 400/cm 2Minute yardstick glow discharge; Thus little glow discharge pattern has been incorporated in the atmospheric dielectric barrier discharge system; The highfield ionization working gas that utilizes little glow-discharge cathode district to produce; In conjunction with the collective effect of little glow discharge, can effectively improve the occupation rate of high energy electron on time and space, and then the active particle that enriches more is provided for plasma chemical reaction.
Summary of the invention
The present invention has overcome the existing deficiency that is used for the atmospheric pressure nonequilibrium plasma source of plasma chemical reaction, and a kind of atmospheric pressure nonequilibrium plasma source of introducing little glow discharge pattern is provided.The present invention stops that at conventional atmosphere medium nonequilibrium plasma takes place on the basis, source; Through changing electrode structure; Improve the dielectric layer material performance; Methods such as raising excitation electrical field intensity are incorporated into multiple little glow discharge pattern in the atmospheric pressure nonequilibrium plasma source, have improved the generation efficient of active particle, have strengthened plasma chemical reaction usefulness.
Technical scheme of the present invention is:
Introduce the atmospheric pressure nonequilibrium plasma source of little glow discharge pattern, comprise high-field electrode assembly, grounding electrode assembly, α-Al 2O 3Dielectric layer, α-Al 2O 3Filler strip, unstrpped gas inlet, unstrpped gas current-sharing chamber, nonequilibrium plasma ionization chamber, reacting gas compile chamber, reaction gas outlet, cooling water inlet, coolant outlet, High-Voltage Insulation terminal, sealing side plate.It is characterized in that: the high-field electrode assembly is equipped with atmospheric pressure local highfield and brings out device pin array high-field electrode; Pin array high-field electrode is placed on and constitutes the double ioinization cavity configuration between the two parallel-plate grounding electrodes; Wherein, It is 96%~99% that parallel-plate grounding electrode surface evenly covers purity, and relative dielectric constant is α-Al of 9~10 2O 3Dielectric layer, dielectric layer thickness are 0.47~0.64mm, and the one side plating that dielectric layer contacts with grounding electrode is coated with thick metal A g of 0.1mm or Au, and the coating edge is apart from α-Al 2O 3The dielectric layer edge leaves the insulation distance of 6~8mm, and metal A g or Au coating well are connected with grounding electrode; Each pin electrode in the pin array high-field electrode all is that the bottom surface is foursquare rectangular pyramid structure; Each pin electrode is arranged in length and breadth in same plane and is formed array structure; Pin electrode length is 0.5~1.0mm; Adjacent needles pointed nose distance is 0.3~0.5mm, and comprising the pin electrode number in every square centimeter is 400~1000; Pin array high-field electrode and the α-Al that covers board joint ground electrode surface 2O 3Constitute the nonequilibrium plasma ionization chamber between the dielectric layer, its discharging gap optimization distance is 0.25~0.64mm; The grounding electrode assembly is provided with cooling water cavity, and cooling water is got into by the cooling water inlet, is discharged by coolant outlet, and cooling water temperature is controlled at 5~10 ℃; Front portion, double ioinization chamber is provided with unstrpped gas current-sharing chamber, guarantees that the unstrpped gas flow velocity in entering double ioinization chamber is identical, is controlled at 2~10m/s according to the different needs flow velocity; Rear portion, double ioinization chamber is provided with reacting gas and compiles the chamber, and the reaction gas that the double ioinization chamber is discharged is pooled to the same pipeline output that transports; Pin array high-field electrode is connected with the high-voltage output end of high-frequency and high-voltage power supply via the High-Voltage Insulation terminal, and in order to produce multiple little glow discharge effectively, the output voltage of high-frequency and high-voltage power supply is controlled at 5~10kV, and driving frequency is controlled at 5~50kHz; The operating air pressure of introducing the atmospheric pressure nonequilibrium plasma source of little glow discharge pattern is controlled at 90~110kPa; During work; Unstrpped gas gets into unstrpped gas current-sharing chamber by the unstrpped gas inlet; Unstrpped gas speed evenly back gets into the nonequilibrium plasma ionization chamber, in the nonequilibrium plasma ionization chamber, behind plasma chemical reaction, gets into reacting gas and compiles the chamber, discharges through reaction gas outlet again; The main material that grounding electrode and housing adopt is aluminium or stainless steel.
The atmospheric pressure nonequilibrium plasma source of introducing little glow discharge pattern also can be designed to other a kind of structure, comprises high-field electrode assembly, grounding electrode assembly, α-Al equally 2O 3Dielectric layer, α-Al 2O 3Filler strip, unstrpped gas inlet, unstrpped gas current-sharing chamber, nonequilibrium plasma ionization chamber, reacting gas compile chamber, reaction gas outlet, cooling water inlet, coolant outlet, High-Voltage Insulation terminal, sealing side plate.With the difference in the atmospheric pressure nonequilibrium plasma source of the little glow discharge pattern of aforementioned introducing be: the high-field electrode assembly is provided with flat high-field electrode, α-Al 2O 3Dielectric layer covers the two sides of flat high-field electrode, wherein α-Al respectively 2O 3The one side plating that dielectric layer contacts with high-field electrode is coated with thick metal A g of 0.1mm or Au, and the coating edge is apart from α-Al 2O 3The dielectric layer edge leaves the insulation distance of 6~8mm, and metal A g or Au coating well are connected with high-field electrode; Grounding electrode then is a needle-array electrode; Pin array high-field electrode in the atmospheric pressure nonequilibrium plasma source of pin array grounding electrode parameter and requirement and the little glow discharge pattern of aforementioned introducing is identical, and flat high-field electrode assembly is placed on and constitutes the double ioinization cavity configuration between two pin array grounding electrode assemblies that are parallel to each other.
Effect of the present invention and benefit are owing to adopt the needle-array electrode structure; Good thin dielectric layer and the high-frequency and high-voltage motivational techniques of while binding ability; In extremely narrow spininess-plate discharge system, set up the discharge of atmospheric pressure electric field; And then can produce the miniflow notes discharge that structure dimension is close, characteristic is identical, quantity is huge at the positive half period of driving voltage; Negative half-cycle at driving voltage then produces the minute yardstick glow discharge that structure dimension is close, characteristic is identical, quantity is huge, therefore little glow discharge pattern has been incorporated in the atmospheric dielectric barrier discharge system highfield ionization working gas that utilizes little glow-discharge cathode district to produce; Collective effect in conjunction with little glow discharge; Can effectively improve the occupation rate of high energy electron on time and space, and then, effectively improve the chemical reaction usefulness in atmospheric pressure nonequilibrium plasma source for plasma chemical reaction provides abundant more active particle.
Description of drawings
Accompanying drawing 1 is an atmospheric pressure nonequilibrium plasma source structure decomposing schematic representation of introducing little glow discharge pattern.
Accompanying drawing 2 is atmospheric pressure nonequilibrium plasma source spininess-plate sparking electrode theory structure sketch mapes.
Accompanying drawing 3 is micro-imagings of independent miniflow notes and independent little glow discharge.
Accompanying drawing 4 is discharging current and voltage waveforms of introducing the atmospheric pressure nonequilibrium plasma source of little glow discharge pattern.
Among the figure: 1 high-field electrode assembly; 2 grounding electrode assemblies; 3 unstrpped gases inlet; Unstrpped gas current-sharing chambers 4;
5 reacting gass compile the chamber; 6 reaction gas outlet; 7 cooling water inlets; 8 coolant outlets;
9 High-Voltage Insulation terminals; 10 sealing side plates; 11 pin array high-field electrodes; 12 board joint ground electrodes;
13 α-Al 2O 3Dielectric layer; 14 α-Al 2O 3Filler strip, 15 nonequilibrium plasma ionization chambers;
16 planar high voltage electrodes; 17 pin array grounding electrodes; 18 high-frequency and high-voltage power supplies.
Embodiment
Be described in detail embodiment of the present invention below in conjunction with technical scheme and accompanying drawing.
The structure in the atmospheric pressure nonequilibrium plasma source of the little glow discharge pattern of introducing of the present invention comprises high-field electrode assembly 1, grounding electrode assembly 2, α-Al shown in accompanying drawing 1 2O 3 Dielectric layer 13, α-Al 2O 3Filler strip 14, unstrpped gas inlet 3, unstrpped gas current-sharing chamber 4, nonequilibrium plasma ionization chamber 15, reacting gas compile chamber 5, reaction gas outlet 6, cooling water inlet 7, coolant outlet 8, High-Voltage Insulation terminal 9 and sealing side plate 10.Wherein, high-field electrode assembly 1 is placed on and constitutes the double ioinization cavity configuration between the two parallel grounding electrode assemblies 2.During work, at first cooling water is introduced by cooling water inlet 7, evenly flow through the cooling water cavity of grounding electrode assembly 2, discharged by coolant outlet 8, cooling water temperature is controlled at 5~10 ℃.Unstrpped gas is got into by unstrpped gas inlet 3, at first through 4 current-sharings of unstrpped gas current-sharing chamber, makes the unstrpped gas flow velocity that gets into the double ioinization chamber identical, is controlled at 2~10m/s according to the different needs gas flow rate; After unstrpped gas gets into ionization chamber, in ionization chamber, carry out the nonequilibrium plasma chemical reaction and generate target product, reacted gas gets into reacting gas and compiles chamber 5, is discharged by reaction gas outlet 6 at last.The running parameter in the atmospheric pressure nonequilibrium plasma source of the little glow discharge pattern of described introducing is driving voltage 5~10kV, driving frequency 5~50kHz, operating air pressure 90~110kPa.
The atmospheric pressure nonequilibrium plasma source spininess-plate sparking electrode theory structure of the little glow discharge pattern of introducing of the present invention is shown in accompanying drawing 2; Be divided into two kinds of structures; A kind of is that high-field electrode is the needle-array electrode structure, comprises pin array high-field electrode 11, flat grounding electrode 12, α-Al 2O 3 Dielectric layer 13, α-Al 2O 3Filler strip 14 and nonequilibrium plasma ionization chamber 15; Another kind is that grounding electrode is the needle-array electrode structure, comprises flat high-field electrode 16, pin array grounding electrode 17, α-Al 2O 3 Dielectric layer 13, α-Al 2O 3Filler strip 14 and nonequilibrium plasma ionization chamber 15.Wherein, α--Al 2O 3The material purity of dielectric layer 13 is 96%~99%, and relative dielectric constant is 9~10, α-Al 2O 3Dielectric layer thickness is 0.47~0.64mm, α-Al 2O 3The one side plating that dielectric layer contacts with metal electrode is coated with thick metal A g of 0.1mm or Au, and the coating edge is apart from α-Al 2O 3The dielectric layer edge leaves the insulation distance of 6~8mm; Each pin electrode in the needle-array electrode all is that the bottom surface is foursquare rectangular pyramid structure; Each pin electrode is arranged in length and breadth in same plane and is formed array structure; Pin electrode length is 0.5~1.0mm; Adjacent needles pointed nose distance is 0.3~0.5mm, and comprising the pin electrode number in every square centimeter is 400~1000; The nonequilibrium plasma ionization chamber is a double cavity structure, and discharging gap optimization distance is 0.25~0.64mm; The atmospheric pressure nonequilibrium plasma source spininess-plate sparking electrode of the little glow discharge pattern of described introducing is by high-frequency and high-voltage power supply 18 excitations; Driving voltage is controlled at 5~10kV; Driving frequency is controlled at 5~50kHz; Operating air pressure is controlled at 90~110kPa, can in nonequilibrium plasma ionization chamber 15, alternately produce miniflow thus and annotate and two kinds of discharge modes of little aura.
The micro-imaging of independent miniflow notes of the present invention and independent little glow discharge is shown in accompanying drawing 3.In the atmospheric pressure nonequilibrium plasma source of the little glow discharge pattern of described introducing; Pin electrode corresponding a micro-discharge cells independently; Along with the cyclic variation of driving voltage, each independent discharge cell all can show the micro-imaging characteristic shown in the accompanying drawing 3.When driving voltage is 5~10kV; When driving frequency is 5~50kHz; If discharge occurs in the positive half period of driving voltage; Independently micro-discharge cells produces is that miniflow is annotated discharge for each, and discharge mode work will be annotated with miniflow in the atmospheric pressure nonequilibrium plasma source of the little glow discharge pattern of described introducing; If discharge occurs in the negative half-cycle of driving voltage; Because driving voltage is very high; The Trichel pulse will carry out the transition to stable little glow discharge pattern, and little glow discharge has typical low pressure glow discharge regional structure characteristic, can clearly observe the existence of glow discharge essential characteristics such as negative glow, Faraday dark space, positive column, anode glow district and anode dark space; But space scale is much little; Be merely a millimeter magnitude, therefore in the positive negative cycle of driving voltage, discharge mode and the alternation of little glow discharge pattern will be annotated with miniflow in the atmospheric pressure nonequilibrium plasma source of the little glow discharge pattern of described introducing.
The discharging current in the atmospheric pressure nonequilibrium plasma source of the little glow discharge pattern of introducing of the present invention and voltage waveform are shown in accompanying drawing 4.At driving voltage is under the situation of sine wave; The atmospheric pressure nonequilibrium plasma source of the little glow discharge pattern of described introducing must have the discharging current characteristic shown in the accompanying drawing 4; Promptly at the positive half period of driving voltage; Discharging current has miniflow and annotates the pulse current characteristic that discharge causes, and at the negative half-cycle of driving voltage, this pulse current characteristic disappear.
The present invention is incorporated into little glow discharge pattern in the atmospheric pressure nonequilibrium plasma source; Effective enhanced discharge electric field strength; Improve the occupation rate of high energy electron on time and space; And then, effectively improve the chemical reaction usefulness in atmospheric pressure nonequilibrium plasma source for plasma chemical reaction provides abundant more active particle.

Claims (1)

1. an atmospheric pressure nonequilibrium plasma source of introducing little glow discharge pattern comprises high-field electrode assembly (1), grounding electrode assembly (2), α-Al 2O 3Dielectric layer (13), α-Al 2O 3Filler strip (14), unstrpped gas inlet (3), unstrpped gas current-sharing chamber (4), nonequilibrium plasma ionization chamber (15), reacting gas compile chamber (5), reaction gas outlet (6), cooling water inlet (7), coolant outlet (8), High-Voltage Insulation terminal (9) and sealing side plate (10), it is characterized in that:
High-field electrode assembly (1) is placed on and constitutes the double ioinization cavity configuration between the two parallel grounding electrode assemblies (2); High-field electrode assembly (1) or grounding electrode assembly (2) are equipped with atmospheric pressure local highfield and bring out the device needle-array electrode, and and corresponding plate electrode between constitute spininess-plate discharge electrode structure; The plate electrode surface evenly covers α-Al 2O 3Dielectric layer (13), the discharging gap distance of nonequilibrium plasma ionization chamber (15) is 0.25~0.64mm, grounding electrode assembly (2) is provided with cooling water cavity;
Wherein, Needle-array electrode is divided into pin array high-field electrode (11) and pin array grounding electrode (17); Each pin electrode in pin array high-field electrode (11) and the pin array grounding electrode (17) all is that the bottom surface is foursquare rectangular pyramid structure, and each pin electrode is arranged in length and breadth in same plane and formed array structure, and pin electrode length is 0.5~1.0mm; Adjacent needles pointed nose distance is 0.3~0.5mm, and comprising the pin electrode number in every square centimeter is 400~1000;
α-Al 2O 3Dielectric layer (13) is 96%~99% by purity, and relative dielectric constant is α-Al of 9~10 2O 3Material is processed, and thickness is 0.47~0.64mm; α-Al 2O 3The one side plating that dielectric layer (13) contacts with board joint ground electrode (12) and planar high voltage electrode (16) is coated with thick metal A g of 0.1mm or Au, and the coating edge is apart from α-Al 2O 3Dielectric layer (13) edge leaves the insulation distance of 6~8mm, and metal A g or Au coating are connected with board joint ground electrode (12) the peaceful plate hight piezoelectricity utmost point (16);
This introduces 5~10 ℃ of driving voltage 5~10kV, driving frequency 5~50kHz, operating air pressure 90~110kPa, the cooling water temperatures in the atmospheric pressure nonequilibrium plasma source of little glow discharge pattern, the flow velocity 2~10m/s of unstrpped gas in nonequilibrium plasma ionization chamber (15).
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CN103442509A (en) * 2013-08-24 2013-12-11 大连海事大学 Reciprocating type multi-ionization-cavity atmospheric-pressure unbalance plasma reactor
CN103458601A (en) * 2013-09-12 2013-12-18 大连民族学院 Plasma generation device
CN106686872A (en) * 2017-02-09 2017-05-17 江苏升元菲尔科技发展有限公司 Panel tip discharge type plasma generator
CN107135597A (en) * 2017-06-26 2017-09-05 大连理工大学 Wide arc gap, the device of large area Uniform Discharge plasma and application method are produced in a kind of atmospheric air
CN108601191A (en) * 2018-05-21 2018-09-28 王逸人 Array double-dielectric barrier discharge device
CN109345927A (en) * 2018-11-23 2019-02-15 北京理工大学 A kind of device for realizing gas discharge homogenization using extra electric field
CN110708851A (en) * 2019-09-29 2020-01-17 上海交通大学 Large-gap uniform dielectric barrier discharge plasma surface treatment device under atmospheric pressure
CN113636622A (en) * 2021-07-01 2021-11-12 东莞市双平电源技术有限公司 Glow discharge circuit and dot-matrix glow discharge water treatment device

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CN103442509A (en) * 2013-08-24 2013-12-11 大连海事大学 Reciprocating type multi-ionization-cavity atmospheric-pressure unbalance plasma reactor
CN103458601A (en) * 2013-09-12 2013-12-18 大连民族学院 Plasma generation device
CN106686872A (en) * 2017-02-09 2017-05-17 江苏升元菲尔科技发展有限公司 Panel tip discharge type plasma generator
CN107135597A (en) * 2017-06-26 2017-09-05 大连理工大学 Wide arc gap, the device of large area Uniform Discharge plasma and application method are produced in a kind of atmospheric air
CN107135597B (en) * 2017-06-26 2023-05-12 大连理工大学 Device for generating large-gap and large-area uniform discharge plasma in atmospheric air and use method
CN108601191A (en) * 2018-05-21 2018-09-28 王逸人 Array double-dielectric barrier discharge device
CN109345927A (en) * 2018-11-23 2019-02-15 北京理工大学 A kind of device for realizing gas discharge homogenization using extra electric field
CN110708851A (en) * 2019-09-29 2020-01-17 上海交通大学 Large-gap uniform dielectric barrier discharge plasma surface treatment device under atmospheric pressure
CN113636622A (en) * 2021-07-01 2021-11-12 东莞市双平电源技术有限公司 Glow discharge circuit and dot-matrix glow discharge water treatment device

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