CN112058195A - Liquid-phase plasma reaction device and treatment method based on radio-frequency discharge plasma - Google Patents
Liquid-phase plasma reaction device and treatment method based on radio-frequency discharge plasma Download PDFInfo
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- CN112058195A CN112058195A CN201911334430.6A CN201911334430A CN112058195A CN 112058195 A CN112058195 A CN 112058195A CN 201911334430 A CN201911334430 A CN 201911334430A CN 112058195 A CN112058195 A CN 112058195A
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- B01J19/00—Chemical, physical or physico-chemical processes in general; Their relevant apparatus
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- B01J19/00—Chemical, physical or physico-chemical processes in general; Their relevant apparatus
- B01J19/08—Processes employing the direct application of electric or wave energy, or particle radiation; Apparatus therefor
- B01J19/087—Processes employing the direct application of electric or wave energy, or particle radiation; Apparatus therefor employing electric or magnetic energy
- B01J19/088—Processes employing the direct application of electric or wave energy, or particle radiation; Apparatus therefor employing electric or magnetic energy giving rise to electric discharges
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- 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
- H05H1/46—Generating plasma using applied electromagnetic fields, e.g. high frequency or microwave energy
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- H—ELECTRICITY
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- H05H1/00—Generating plasma; Handling plasma
- H05H1/24—Generating plasma
- H05H1/46—Generating plasma using applied electromagnetic fields, e.g. high frequency or microwave energy
- H05H1/4645—Radiofrequency discharges
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- B—PERFORMING OPERATIONS; TRANSPORTING
- B01—PHYSICAL OR CHEMICAL PROCESSES OR APPARATUS IN GENERAL
- B01J—CHEMICAL OR PHYSICAL PROCESSES, e.g. CATALYSIS OR COLLOID CHEMISTRY; THEIR RELEVANT APPARATUS
- B01J2219/00—Chemical, physical or physico-chemical processes in general; Their relevant apparatus
- B01J2219/08—Processes employing the direct application of electric or wave energy, or particle radiation; Apparatus therefor
- B01J2219/0894—Processes carried out in the presence of a plasma
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- H—ELECTRICITY
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- H05H—PLASMA TECHNIQUE; PRODUCTION OF ACCELERATED ELECTRICALLY-CHARGED PARTICLES OR OF NEUTRONS; PRODUCTION OR ACCELERATION OF NEUTRAL MOLECULAR OR ATOMIC BEAMS
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Abstract
The invention relates to a liquid-phase plasma reaction device based on radio-frequency discharge plasma and a processing method. The gas supply system is respectively connected with a second connecting pipe and a third connecting pipe through a first connecting pipe, the second connecting pipe is connected with a second radio-frequency discharge plasma generating system, the third connecting pipe is connected with the first radio-frequency discharge plasma generating system, a gas outlet of the first radio-frequency discharge plasma generating system is connected with a gas inlet of the first stirring reaction tank, a gas outlet of the second radio-frequency discharge plasma generating system is connected with a gas inlet of the second stirring reaction tank, and the gas inlet of the first stirring reaction tank and the gas inlet of the second stirring reaction tank are arranged at the lower part of the tank wall of the stirring reaction tank. Has the advantages of no pollution and large treatment capacity.
Description
Technical Field
The present invention relates to a plasma reaction apparatus and a processing method thereof, and more particularly, to a liquid phase plasma reaction apparatus and a processing method thereof based on a radio frequency discharge plasma.
Background
The discharge plasma processing technology is an advanced oxidation technology, and has the advantages of high efficiency, low temperature, low energy consumption, no by-product and the like, so the discharge plasma processing technology is widely applied to a plurality of fields of water treatment, food sterilization, biomacromolecule modification and the like. However, in the existing liquid phase plasma reaction device, the metal discharge electrode plate is directly contacted with the material, so that the material pollution is caused by the dissolution of metal ions. The method adopts a treatment mode of dielectric barrier discharge plasma, namely, a discharge polar plate is embedded in a plastic material, so that metal ions are prevented from dissolving out. However, the processing space of the dielectric barrier discharge plasma is very narrow, which limits the processing capacity and cannot realize industrial production. Therefore, it is an urgent need to solve the technical problem for those skilled in the art to develop a plasma processing apparatus and method suitable for industrial production.
Disclosure of Invention
The invention provides a liquid-phase plasma reaction device and a treatment method based on radio-frequency discharge plasma, aiming at solving the technical problems that materials are prevented from being in direct contact with a discharge polar plate and the generation of the liquid-phase plasma is increased.
In order to achieve the above object, the technical solution of the present invention is as follows: a liquid phase plasma reaction device based on radio frequency discharge plasma is composed of an air supply system, a first radio frequency discharge plasma generation system, a second radio frequency discharge plasma generation system and a stirring reaction tank, wherein the air supply system is respectively connected with a second connecting pipe and a third connecting pipe through a first connecting pipe, the second connecting pipe is connected with the second radio frequency discharge plasma generation system, the third connecting pipe is connected with the first radio frequency discharge plasma generation system, an air outlet of the first radio frequency discharge plasma generation system is connected with an air inlet of a first stirring reaction tank, an air outlet of the second radio frequency discharge plasma generation system is connected with an air inlet of a second stirring reaction tank, and the air inlet of the first stirring reaction tank and the air inlet of the second stirring reaction tank are arranged on the lower portion of the tank wall of the stirring reaction tank.
The gas supply system supplies gas by a gas cylinder and/or a gas pump; when the gas cylinder supplies gas, the outlet of the gas cylinder is connected with a gas mixer, the gas mixer is connected with a first connecting pipe, and the outlet of the gas cylinder is provided with a valve; when the air pump supplies air, the air inlet end of the air pump is connected with the air filter, and a fourth valve is arranged on the air outlet pipe of the air pump; at least 2 gas cylinders are provided.
The first radio frequency discharge plasma generating system has the following structure: the gas supply device is composed of a first radio frequency discharge tube and a first high pulse power supply generator, wherein the gas inlet of the first radio frequency discharge tube is communicated with a gas supply system through a third connecting tube, and the gas outlet of the first radio frequency discharge tube is directly communicated with the gas inlet of a first stirring reaction tank.
And a first one-way valve is arranged between the air outlet of the first radio-frequency discharge tube and the air inlet of the first stirring reaction tank.
The structure of the second radio frequency discharge plasma generating system is as follows: the gas inlet of the second radio-frequency discharge tube is communicated with a gas supply system through a second connecting tube, and the gas outlet of the second radio-frequency discharge tube is directly communicated with the gas inlet of the second stirring reaction tank.
And a second one-way valve is arranged between the air outlet of the second radio-frequency discharge tube and the air inlet of the second stirring reaction tank.
The structure of the stirring reaction tank is as follows: stirring retort is high-pressure vessel, and first stirring retort air inlet and second stirring retort air inlet are established and are symmetrical tangential direction at stirring retort tank body lower part and distribute, and stirring retort bottom head is the toper, is equipped with dog-house and inlet at stirring retort's top, is equipped with stirring paddle leaf in the stirring retort, and stirring paddle leaf is connected with the agitator motor at stirring retort top.
A processing method of a liquid phase plasma reaction device based on radio frequency discharge plasma comprises the steps that after materials are dissolved and blended in a stirring reaction tank, gas is conveyed to a first radio frequency discharge tube and a second radio frequency discharge tube through a gas supply system, the gas is ionized by radio frequency discharge in the process of passing through the first radio frequency discharge tube and the second radio frequency discharge tube to generate plasma gas substances, the plasma gas substances are discharged from outlets of the first radio frequency discharge tube and the second radio frequency discharge tube, are directly injected into the stirring reaction tank, are directly mixed with the materials, are subjected to liquid phase plasma processing, and are discharged from a liquid outlet of the stirring reaction tank after the processing requirements are met.
The plasma gas substances enter the stirring reaction tank in a symmetrical tangential direction, and are beneficial to fully stirring and mixing the plasma gas substances and the materials.
The air supply system adopts an air pump as an air supply source, and air is air; selecting a gas cylinder as a gas supply source, wherein the gas is oxygen, nitrogen and argon; the pressure of the stirring reaction tank is 0.5-2 MPa; the oxidant may be added while the stirred tank reactor is stirring.
Due to the adoption of the technical scheme, the invention has the following advantages and effects:
the method comprises the steps of firstly ionizing gas by radio frequency discharge, generating plasma gas substances in advance, and then mixing the plasma gas substances with materials to carry out liquid-phase plasma treatment. The material is not in direct contact with the discharge electrode plate, so that material pollution caused by dissolution of metal ions of the discharge electrode plate is avoided. Simultaneously, change the material processing space from between the discharge electrode plate to in the stirring retort, show to have increased material handling capacity.
When the liquid phase plasma reaction device based on the radio frequency discharge plasma and the treatment method thereof are used for treating the liquid phase plasma, the advantages of no pollution and large treatment capacity are achieved.
Drawings
FIG. 1 is a schematic diagram of the system of the present invention.
FIG. 2 is a schematic view of the stirred tank gas inlet arrangement.
In the figure, 1, an air supply system; 2. a first radio frequency discharge plasma generating system; 3. stirring the reaction tank; 4. a second radio frequency discharge plasma generating system; 11. a first connecting pipe; 12. a second connecting pipe; 13. a third connecting pipe; 101. a gas cylinder; 102. a first valve; 103. a second valve; 104. a third valve; 105. an air filter; 106. an air pump; 107. a fourth valve; 108. a gas mixer; 201. a first high pulse power generator; 202. a first radio frequency discharge tube; 203. a second high pulse power generator; 204. a second radio frequency discharge tube; 301. a first stirred tank reactor gas inlet; 302. an air inlet of the second stirring reaction tank; 303. a first check valve; 304. a second one-way valve; 305. a fifth valve; 306. a stirring motor; 307. a stirring paddle; 308. a feeding port; 309. and (4) a liquid inlet.
The specific implementation mode is as follows:
the present invention will be described in further detail with reference to examples. The following examples are only specific examples of the present invention, but the design concept of the present invention is not limited thereto, and any insubstantial modifications of the present invention using the design concept shall fall within the scope of infringing upon the protection of the present invention.
Example 1
As shown in the figure, the liquid phase plasma reaction device based on the radio frequency discharge plasma of the invention comprises a gas supply system 1, a first radio frequency discharge plasma generating system 2, the second radio frequency discharge plasma generating system 4 and the stirring reaction tank 3 are formed, the gas supply system 1 is respectively connected with a second connecting pipe 12 and a third connecting pipe 13 through a first connecting pipe 11, the second connecting pipe 12 is connected with the second radio frequency discharge plasma generating system 4, the third connecting pipe 13 is connected with the first radio frequency discharge plasma generating system 2, the gas outlet of the first radio frequency discharge plasma generating system 2 is connected with the gas inlet 301 of the first stirring reaction tank, the gas outlet of the second radio frequency discharge plasma generating system 4 is connected with the gas inlet 302 of the second stirring reaction tank, and the gas inlet 301 of the first stirring reaction tank and the gas inlet 302 of the second stirring reaction tank are arranged at the lower part of the tank wall of the stirring reaction tank 3.
The gas supply system 1 supplies gas by a gas cylinder 101; the outlets of the gas cylinders 101 are connected with a gas mixer 108, the gas mixer 108 is connected with a first connecting pipe 11, the number of the gas cylinders 101 is three, different gases are filled in each gas cylinder 101, the gases are respectively oxygen, nitrogen and argon, and the outlets of the three gas cylinders 101 are respectively and sequentially provided with a first valve 102, a second valve 103 and a third valve 104.
The first rf discharge plasma generating system 2 has the following structure: the gas mixing device is composed of a first radio frequency discharge tube 202 and a first high pulse power supply generator 201, wherein a gas inlet of the first radio frequency discharge tube 202 is communicated with a gas supply system 1 through a third connecting tube 13, and a gas outlet of the first radio frequency discharge tube 202 is directly communicated with a gas inlet 301 of a first stirring reaction tank. A first one-way valve 303 is arranged between the air outlet of the first radio frequency discharge tube 202 and the air inlet 301 of the first stirring reaction tank, and the first radio frequency discharge tube 202.
The structure of the second rf discharge plasma generating system 4 is as follows: the gas supply system is composed of a second radio frequency discharge tube 204 and a second high pulse power supply generator 203, wherein a gas inlet of the second radio frequency discharge tube 204 is communicated with a gas supply system 1 through a second connecting tube 12, a gas outlet of the second radio frequency discharge tube 202 is directly communicated with a gas inlet 302 of a second stirring reaction tank, a second one-way valve 304 is arranged between the gas outlet of the second radio frequency discharge tube 204 and the gas inlet 302 of the second stirring reaction tank, and the second radio frequency discharge tube 204.
The structure of the stirring reaction tank 3 is as follows: stirring retort 3 is high-pressure vessel, first stirring retort air inlet 301 and second stirring retort air inlet 302 are established and are symmetrical tangential direction at 3 ladle body lower parts of stirring retort and distribute, 3 bottom heads of stirring retort are the toper, 3 bottoms of stirring retort are equipped with the liquid outlet, be equipped with fifth valve 305 on the liquid outlet, conveniently arrange the material, top at stirring retort 3 is equipped with dog-house 308 and inlet 309, be equipped with stirring paddle blade 307 in the stirring retort 3, stirring paddle blade 307 is connected with the agitator motor 306 at stirring retort 3 top.
A treatment method of a liquid phase plasma reaction device based on radio frequency discharge plasma is characterized in that solid materials and liquid materials can respectively enter a stirring reaction tank 3 from a feeding port 308 and a liquid inlet 309 of the stirring reaction tank 3, the solid materials and the liquid materials are dissolved and mixed under the stirring action of a stirring motor 306 and a stirring paddle 307, after the materials are dissolved and mixed in the stirring reaction tank 3, gas is conveyed to a first radio frequency discharge tube 202 and a second radio frequency discharge tube 204 through a gas supply system 1, a first high pulse power supply generator 201 and a second high pulse power supply generator 203 are started, the gas is ionized by radio frequency discharge in the process of passing through the first radio frequency discharge tube 202 and the second radio frequency discharge tube 204 to generate plasma gas substances, the plasma gas substances are discharged from outlets of the first radio frequency discharge tube 202 and the second radio frequency discharge tube 204, are directly injected into the stirring reaction tank 3, are directly mixed with the materials to carry out liquid phase plasma treatment, after the treatment requirement is met, discharging from a liquid outlet of the stirring reaction tank 3. The pressure of the stirring reaction tank 3 is 0.5-2MPa, which is beneficial to mixing the materials with the plasma gas substances.
The plasma gas substance enters the stirring reaction tank 3 in a symmetrical tangential direction, and is beneficial to fully stirring and mixing the plasma gas substance and the materials.
Example 2
When the air supply system 1 in embodiment 1 supplies air by the air pump 106, the air inlet end of the air pump 106 is connected to the air filter 105, and the air outlet pipe of the air pump 106 is provided with the fourth valve 107. When solid materials and liquid materials respectively enter the stirring reaction tank 3 from the feeding port 308 and the liquid inlet 309 of the stirring reaction tank 3, an oxidant is added, so that the synergistic measure treatment of the liquid phase plasma and the oxidant is realized, and the treatment effect is enhanced. Otherwise, the same procedure as in example 1 was repeated.
Example 3
The gas supply system 1 in embodiment 1 uses the gas pump 106 and the gas cylinder 101 to supply gas together, and adjusts the gas flow rate by adjusting the first valve 102, the second valve 103, the third valve 104, or the fourth valve 107, so as to control the concentration of the generated plasma gas species, thereby achieving the purpose of controlling the liquid phase plasma processing effect. Otherwise, the same procedure as in example 1 was repeated.
Claims (10)
1. A liquid phase plasma reaction device based on radio frequency discharge plasma is characterized by comprising an air supply system (1), a first radio frequency discharge plasma generation system (2), a second radio frequency discharge plasma generation system (4) and a stirring reaction tank (3), wherein the air supply system (1) is respectively connected with a second connecting pipe (12) and a third connecting pipe (13) through a first connecting pipe (11), the second connecting pipe (12) is connected with the second radio frequency discharge plasma generation system (4), the third connecting pipe (13) is connected with the first radio frequency discharge plasma generation system (2), an air outlet of the first radio frequency discharge plasma generation system (2) is connected with an air inlet (301) of the first stirring reaction tank, an air outlet of the second radio frequency discharge plasma generation system (4) is connected with an air inlet (302) of the second stirring reaction tank, the gas inlet (301) of the first stirring reaction tank and the gas inlet (302) of the second stirring reaction tank are arranged at the lower part of the tank wall of the stirring reaction tank (3).
2. The rf discharge plasma-based liquid phase plasma reaction device according to claim 1, wherein the gas supply system (1) is supplied with gas from a gas cylinder (101) and/or a gas pump (106); when the gas cylinder (101) supplies gas, the outlet of the gas cylinder (101) is connected with a gas mixer (108), the gas mixer (108) is connected with a first connecting pipe (11), and the outlet of the gas cylinder (101) is provided with a valve; when the air pump (106) supplies air, the air inlet end of the air pump (106) is connected with the air filter (105), and the air outlet pipe of the air pump (106) is provided with a fourth valve (107); at least 2 gas cylinders (101).
3. A liquid-phase plasma reaction apparatus based on rf discharge plasma according to claim 1, wherein the first rf discharge plasma generating system (2) is constructed as follows: the gas mixing device is composed of a first radio frequency discharge tube 202 and a first high pulse power supply generator (201), wherein a gas inlet of the first radio frequency discharge tube (202) is communicated with a gas supply system (1) through a third connecting tube (13), and a gas outlet of the first radio frequency discharge tube (202) is directly communicated with a gas inlet (301) of a first stirring reaction tank.
4. A radio frequency discharge plasma based liquid phase plasma reaction device according to claim 3, wherein a first one-way valve (303) is installed between the gas outlet of the first radio frequency discharge tube (202) and the gas inlet (301) of the first stirring reaction tank.
5. A liquid-phase plasma reaction apparatus based on rf discharge plasma according to claim 1, wherein the second rf discharge plasma generating system (4) is constructed as follows: the gas supply device is composed of a second radio frequency discharge tube (204) and a second high pulse power supply generator (203), wherein a gas inlet of the second radio frequency discharge tube (204) is communicated with a gas supply system (1) through a second connecting tube (12), and a gas outlet of the second radio frequency discharge tube (202) is directly communicated with a gas inlet (302) of a second stirring reaction tank.
6. A liquid phase plasma reaction device based on radio frequency discharge plasma according to claim 5, characterized in that a second one-way valve (304) is installed between the gas outlet of the second radio frequency discharge tube (204) and the gas inlet (302) of the second stirring reaction tank.
7. A liquid-phase plasma reaction apparatus based on rf discharge plasma according to claim 1, wherein the structure of the agitation reaction tank (3) is as follows: stirring retort (3) is high-pressure vessel, first stirring retort air inlet (301) and second stirring retort air inlet (302) are established and are symmetrical tangential direction at stirring retort (3) ladle lower part and distribute, stirring retort (3) bottom head is the toper, top at stirring retort (3) is equipped with dog-house (308) and inlet (309), be equipped with stirring paddle leaf (307) in stirring retort (3), stirring paddle leaf (307) are connected with agitator motor (306) at stirring retort (3) top.
8. The processing method of the liquid phase plasma reaction device based on the radio frequency discharge plasma according to claim 1, characterized in that after the materials are dissolved and blended in the stirring reaction tank (3), the gas is delivered to the first radio frequency discharge tube (202) and the second radio frequency discharge tube (204) by the gas supply system (1), the gas is ionized by the radio frequency discharge in the process of passing through the first radio frequency discharge tube (202) and the second radio frequency discharge tube (204) to generate plasma gas substances, the plasma gas substances are discharged from the outlets of the first radio frequency discharge tube (202) and the second radio frequency discharge tube (204), the plasma gas substances are directly injected into the stirring reaction tank (3) to be directly mixed with the materials for the liquid phase plasma treatment, and the liquid phase plasma substances are discharged from the outlet of the stirring reaction tank (3) after the treatment requirements are met.
9. The processing method of the liquid phase plasma reaction device based on the radio frequency discharge plasma as claimed in claim 8, wherein the plasma gas substance enters the stirring reaction tank (3) in a symmetrical tangential direction, which is beneficial to fully stirring and mixing the plasma gas substance and the material.
10. The processing method of the liquid phase plasma reaction device based on the radio frequency discharge plasma according to claim 8, characterized in that the gas supply system (1) is a gas pump (106) as a gas supply source, and the gas is air; selecting a gas cylinder (101) as a gas supply source, wherein the gas is oxygen, nitrogen and argon; the pressure of the stirring reaction tank (3) is 0.5-2 MPa; adding an oxidant while stirring in the stirring reaction tank (3).
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