CN1931735A - Gas-liquid mixed discharge process and apparatus for degrading organic pollutant in water - Google Patents
Gas-liquid mixed discharge process and apparatus for degrading organic pollutant in water Download PDFInfo
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- CN1931735A CN1931735A CN 200610068995 CN200610068995A CN1931735A CN 1931735 A CN1931735 A CN 1931735A CN 200610068995 CN200610068995 CN 200610068995 CN 200610068995 A CN200610068995 A CN 200610068995A CN 1931735 A CN1931735 A CN 1931735A
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Abstract
The present invention belongs to the application of low temperature plasma technology in the field of controlling environmental pollution, and is especially high voltage pulse discharge apparatus and process to generate high chemically active particle degrading organic pollutant in water. The technological scheme includes using sand core to make the solution distributed homogeneously in the lower layer inside the reactor, applying high voltage pulse across The high voltage electrode in the liquid phase and the earth electrode in the gas phase, acting the liquid phase generated low temperature plasma and the gas phase generated ozone directly on the organic pollutant under the action of high strength electric field, using the baffling metal net in the solution to raise ozone utilization rate, adding active carbon fiber and ferrous ion into solution to raise the organic pollutant treating effect.
Description
Technical field
The invention belongs to the application of lower temperature plasma technology, relate to the method and the device of organic pollutant in the high reactivity chemical particle degradation water of utilizing the high pressure pulse discharge generation in environmental pollution control field.
Background technology
Industries such as pharmacy at present, printing and dyeing, chemical industry, oil have caused a large amount of trade effluents, and this class wastewater discharge is big, water quality is complicated, hazardous contaminant content height, have a very wide distribution, and have proposed new test for traditional water technology.Over nearly 30 years, risen some new water technologies at the waste water of these difficult degradations, wherein high pressure pulse discharge is because the exergonic diversity of its electronic transmission process and its application aspect environmental pollution improvement have caused widely pays close attention to.
Liquid phase high pressure pulse discharge, the high voltage pulse by applying steep-front, spike pulse make the extra light electronics of quality moment obtain energy and quicken between nonequilibrium earth polar and high voltage electrode, ion since its bigger quality be difficult to obtain acceleration in moment.Electronics obtains to become the high energy unbound electron behind the energy, with other molecular impact, makes molecular dissociation in moving process, causes a series of chemical processes, causes active substance such as H
2O
2, OH, O, HO
2Deng generation.These active substances and organic pollutant collision, making the organic pollutant degradation in the water is carbonic acid gas, water and nontoxic byproduct.In these processes, because the ionization of molecule, transition etc. can produce some physical influences such as UV-light, ultrasonic, shockwave, localized hyperthermia etc., these physical processes also can be impelled the degraded of organic pollutant.
Liquid phase high pressure pulse discharge blasting under the air or oxygen condition can also produce ozone except that above chemical process and physical influence, improve the degradation rate of organic pollutant.But air-flow velocity is fast, bubble is big, and the little and residence time weak point of organic pollutant contact area causes the utilization ratio of ozone low in ozone and the water.
Summary of the invention
The objective of the invention is the problem that exists at prior art, the method and the device of organic pollutant in the high gas-liquid mixed discharge degradation water of a kind of degradation rate with organic pollutant is provided.
Concrete technical scheme comprises:
The method of organic pollutant is in the gas-liquid mixed discharge degradation water: at the reactor bottom injecting gas, make the gas uniform distribution in lower floor's solution, applying high-voltage pulse between parallel corresponding high voltage electrode that is provided with and the ground electrode between lower floor's solution and the upper solution, under the high-strength electric field effect, utilize the low-temperature plasma of liquid phase generation and the ozone of gas phase generation to directly act on organic pollutant.In upper solution, the metal barrier net is set, in solution, add active carbon fibre peacekeeping ferrous ion, the add-on of gac, active carbon fibre peacekeeping ferrous ion is respectively 3-20g/L, 1-15g/L and 0.1-10g/L, and the adsorption catalysis of activated carbon fiber, Fenton reagent and high pressure pulse discharge form synergistic effect.
The device of organic pollutant comprises two kinds of schemes in the gas-liquid mixed discharge degradation water:
Scheme 1 is: comprise reactor, high voltage electrode in the cooling sandwith layer of reactor ectosome and the reactor, ground electrode and outside high-voltage pulse power source, the bottom of reactor is provided with core, high voltage electrode is positioned at the upper surface of core, by being connected with high-voltage pulse power source by lead after several apicule needle parallel connections, the prong diameter is less than 0.25mm, ground electrode is on the interface of gas phase and upper solution, by fixed link and wiring nut ground connection, the thickness of ground electrode is 0.3～2mm, its diameter is than the little 1～4mm of reactor inner diameter of steel flue, distance between high voltage electrode 1 and the ground electrode 2 is less than 200mm, and the distance between ground electrode 2 and the liquid-gas interface 7 is less than 2mm.
Scheme 2 is: comprise reactor, high voltage electrode in the cooling sandwith layer of reactor ectosome and the reactor, ground electrode and outside high-voltage pulse power source, it is characterized in that: the bottom of reactor is provided with core, ground electrode is positioned at the upper surface of core, the thickness of ground electrode is 0.3～2mm, its diameter is than the little 1～4mm of reactor inner diameter of steel flue, high voltage electrode is on the interface of gas phase and upper solution, by fixed link and wiring nut ground connection, by being connected with high-voltage pulse power source by lead after several apicule needle parallel connections, the prong diameter is less than 0.25mm, distance between high voltage electrode 1 and the ground electrode 2 is less than 200mm, and the distance between ground electrode 2 and the liquid-gas interface 7 is less than 2mm.
More than the improvement project of two kinds of schemes also comprise: vertical direction is provided with the several layers of metal barrier net that is parallel to each other in upper solution, and the metal barrier net is fixed on the fixed link, is uniformly distributed in the upper solution; The polarity of high voltage needle electrode can be changed, and as changing the setting of high-voltage pulse power source, when applying the negative high voltage pulse, the polarity of high voltage needle electrode becomes the negative high voltage pulse by original positive high voltage pulse; When applying the positive or negative high voltage pulse, the polarity of high voltage needle electrode changes from the positive high voltage pulse to the negative high voltage pulse cycle.
The invention has the beneficial effects as follows that the gentle phase discharge reactor of a Liquid-phase reactor combines, simple in structure, easy to make.
1. the core gas distribution has reduced discharge inception voltage and has made discharge evenly.
Maximum using the chemically-active particle of discharge generation, particularly gasiform ozone, through after the stopping of multiple layer metal net, utilization ratio is higher.
3. the adsorption catalysis of activated carbon fiber, Fenton reagent and high pressure pulse discharge form synergistic effect, improve the degradation efficiency of organic pollutant.
Description of drawings
Accompanying drawing 1 is the structural representation of device; Accompanying drawing 2 is the performance comparison diagrams with pre-existing reactors; Accompanying drawing 3 is to add gac and the activated carbon fiber comparison diagram that influences to degradation rate; Accompanying drawing 4 is the comparison diagrams that influence that add foundary weight ion pair degradation rate.
Embodiment
The invention will be further elaborated below by example, but the present invention is not constituted any qualification.
The method particular embodiment of organic pollutant is the gas uniform distribution in the reactor lower floor solution in the gas-liquid mixed discharge degradation water, high-voltage pulse power source in liquid phase high voltage electrode and the ground electrode in the gas phase apply high-voltage pulse, under the high-strength electric field effect, utilize the low-temperature plasma of liquid phase generation and the ozone of gas phase generation to directly act on organic pollutant, the stainless steel metal in the upper solution stops that net can improve the utilization ratio of ozone.In solution, add active carbon fibre peacekeeping ferrous ion, the add-on of gac, active carbon fibre peacekeeping ferrous ion is respectively 3-20g/L, 1-15g/L and 0.1-10g/L, the adsorption catalysis of activated carbon fiber, Fenton reagent and high pressure pulse discharge form synergistic effect, have increased substantially the degradation rate of organic pollutant.
The device of organic pollutant as shown in Figure 1 in the gas-liquid mixed discharge degradation water, among the figure, liquid phase high voltage electrode 1, gas phase ground electrode 2, stainless steel metal stops net 3, core 4, gas phase 5, add the organic waste water solution (liquid phase) 6 of active carbon fibre peacekeeping ferrous ion, liquid-gas interface 8, fixed link 9, set screw nut 10, wiring nut 11, grounding wire 12, reactor inner core (synthetic glass) 13, reactor (synthetic glass) urceolus 14, cooling water sandwich 15, cooling water inlet 16, cooling water outlet 17, stopple coupon 18, air outlet 19, inlet mouth 20, high-voltage pulse power source lead-in wire 21, bubble 22, gas-bearing formation 23, time 24, air chamber 25.
Core 4 is positioned at the bottom of lower floor's solution, makes from air chamber 25 and blasts air filled cavity uniform distribution the reactor lower floor solution 6, and bubble diameter reduces discharge inception voltage and makes discharge evenly about 2mm.Core can be selected G
1～G
6Different model (G
1～G
6Represent its pore size distribution size), pore size distribution is more little, and the bubble diameter of generation is little and even more, specific surface area is big, helps surface reaction and active particle to Liquid Phase Diffusion.Core also can replace with other porous material, as porous ceramics etc.The gas that blasts can be that air, oxygen, hydrogen, nitrogen, argon gas etc. also can be the mixed gass of two or more gas, as blasts oxygen, can produce O at liquid and gas
3, O, O
2 -Equimolecular, active particle and ion; Blast the mixed gas of oxygen and other gases, remove at liquid and gas and produce O
3, O, O
2 -, can also produce other molecules, active particle and ion outward, thereby improve the degradation rate of organic pollutant.
High voltage electrode 1 in the liquid phase is positioned at the upper surface of core 4,21 is connected with high-voltage pulse power source (not drawing) by going between by five acupuncture needles (also can be less than or more than five) back in parallel, and the diameter of every pin is 0.25mm.Needle tip insulate as much as possible with the lower section, makes the loss of energy be reduced to minimum, also can be on-insulated, there is no strict demand.Needle point is point possibly, so that produce concentration of local and very strong electric field around needle point, makes electronics obtain higher energy.High voltage electrode also can be other metals, and as filaments such as stainless steel, silver, platinum, tungsten, nichromes, diameter is less than 0.25mm.
The polarity of high voltage needle electrode 1 can be changed, and as changing the setting of high-voltage pulse power source, when applying the negative high voltage pulse, the polarity of high voltage needle electrode 1 becomes negative high voltage by original positive high voltage; When applying the positive or negative high voltage pulse, the polarity one-period of high voltage needle electrode 1 changes twice.
Stainless steel disk ground electrode 2 is on the interface of gas phase 5 and upper solution 6, by stainless steel fixed link 9 and wiring nut 11 direct ground connection.The thickness of stainless steel disk is 2mm, and its diameter is than the little 1mm of synthetic glass inner diameter of steel flue, and the slit of gas between stainless steel disk and synthetic glass inner core enters the upper solution, and upper solution 6 can flow down the solution 6 formation circulations with lower floor along inner tube wall again.
Distance between high voltage electrode 1 and the stainless steel disk ground electrode 2 is adjusted up and down by stainless steel fixed link 9 and set screw nut 10, can change in less than the 200mm scope; Distance between stainless steel disk ground electrode 2 and the liquid-gas interface 7 by reconciling the gap size adjustment between air input and stainless steel disk and the synthetic glass inner core, can change in less than the 2mm scope.In the present invention, the distance between high voltage needle electrode 1 and the stainless steel disk ground electrode 2 is 17mm, and the optimum distance between stainless steel disk ground electrode 2 and the liquid-gas interface 7 is 16mm.
Ground electrode can be other electric good conductor material, also can be that the poor conductor of electricity plates metal (as platinum, palladium, rhodium etc.), can also be the porous electro-conductive material.
The polarity of high voltage needle electrode 1 and stainless steel disk ground electrode 2 can be put upside down, and pin electrode 1 is done the earth polar, and stainless steel disk electrode 2 is made high voltage electrode.
Stainless steel metal stops that net 3 is fixed on the stainless steel fixed link 9, be uniformly distributed in the upper solution 6, gaseous ozone is obstructed in uphill process, lower surface at Stainless Steel Wire Mesh 3 forms gas-bearing formation, be increased in the residence time in the solution 6, solution forms liquid film on Stainless Steel Wire Mesh 3 simultaneously, has increased the contact area of ozone and organic pollutant, organic pollutant in ozone and the upper solution 6 is fully reacted, improve the utilization ratio of ozone.In addition, also may play katalysis in the organic pollutant reaction process of Stainless Steel Wire Mesh 3 in ozone and solution 6.
The two-layer spacing size of net that stops can be regulated, and according to handling liquid measure, also can suitably increase the number of plies that stops net.In the present invention, be provided with 5 layers and stop net, two-layerly stop that the spacing of net is 20mm.Stop that net can replace with other porous material, as porous ceramics, molecular sieve etc., pore size can be selected as required.
In the cooling water sandwich 15 between synthetic glass inner core 13 and the synthetic glass urceolus 14 water coolant is housed, it also can be other cooling fluid, with peristaltic pump (not drawing) make water coolant (liquid) in the cooling water inlet 16 and cooling water outlet 17 constitute circulation, keep isothermal reaction, prevent reactor overheated (the overheated solubleness of ozone that makes reduces).
Gas enters air outlet 19 after by gas meter (not drawing), so that control and measurement gas flow connect the gaseous ozone analysers in escape pipe 19 backs, so that the ozone content in the analysis combustion gas.The reactor inner/outer tube can be with silica glass or other transparent material, or other insulating material leaves transparent fenestra, so that connect spectral analysis apparatus.
Reactor of the present invention is powered with high-voltage pulse power source as far as possible.In steep-front, spike pulse discharge process, liquid phase produces H
2O
2, OH, O
3, O, H
2, H, O
2 -And other molecule, ion and active particle; Gas phase produces O
3, O, OH and other molecule, ion and active particle.Owing to increased O
3, O, OH and other excited state particle, thereby improve the degradation efficiency of organic pollutant.
Can significantly improve degradation rate after in solution 6, adding active carbon fibre peacekeeping ferrous ion.Activated carbon fiber plays adsorption on the one hand, and katalysis is also played on porous activated carbon fiber surface on the other hand, makes the organic pollutant accelerated degradation that is adsorbed on the activated carbon fiber surface.The H that produces in ferrous ion and the discharge process
2O
2As Fenton reagent, fast reaction speed is with the adsorption catalysis formation synergistic effect of high pressure pulse discharge and activated carbon fiber.In the present invention, the best dosage of ferrous sulfate is 1.4g/L.Can be on activated carbon fiber loaded optic catalyst, utilize the UV-light in the discharge process to produce photocatalysis, further improve degradation rate.
Application example 1, the validity of gas-liquid mixed discharge reactor degraded tropeolin-D.
By gas-liquid mixed discharge reactor and the contrast of traditional liquid phase reference reaction device of not adding active carbon fibre peacekeeping ferrous sulfate, the validity of tropeolin-D is separated in publicly price-reduction, and the synthetic glass inner diameter of steel flue of these two kinds of reactors all is 40mm.The high voltage electrode of gas-liquid mixed discharge reactor is made up of the acupuncture needle of five diameter 0.25mm, and pin spacing 12mm, pin exceed core surface 16mm.The ground electrode diameter is the thick stainless steel plate of 38mm, 2mm, and two distance between electrodes are 17mm, and ground electrode is 16mm to the spacing of liquid-gas interface.The high voltage electrode of reference reaction device is made up of five No. 9 entry needles, and the ground electrode diameter is the thick stainless steel plate of 30mm, 2mm, and two distance between electrodes are 17mm.All with the high-voltage pulse power source power supply, crest voltage is 40KV to these two kinds of reactors, and frequency is 50Hz, and the concentration of methyl orange aqueous solution is 40ppm, handles liquid measure 150ml, air flow quantity 0.08m
3/ h, the treatment time is 30 minutes, and sampling interval is 6 minutes, repeats 3 times, averages, and surveys solution absorbency with the UV762 ultraviolet-visible spectrophotometer, and error is less than 3%.
Fig. 2 has shown the degradation rate of gas-liquid mixed discharge reactor and reference reaction device.Gas-liquid mixed discharge reactor degradation rate is 74.65%, and the degradation rate of reference reaction device is 63.58%, and the degradation rate of gas-liquid mixed discharge reactor is higher 11 percentage points than reference reaction device, illustrates that the performance of gas-liquid mixed discharge reactor is better than the reference reaction device.
Application example 2, the experiment condition of gas-liquid mixed discharge reactor add 1.5g gac and 0.5g activated carbon fiber respectively with example 1 in methyl orange solution, investigate the influence of gas-liquid mixed discharge reactor to degradable organic pollutant.
Fig. 3 shows that the degradation rate of tropeolin-D is 74.65% when not adding gac and activated carbon fiber; The degradation rate of tropeolin-D is 83.36% behind the adding 1.5g gac, improves 8.7 percentage points; The degradation rate of tropeolin-D is 92.61% after the adding 0.5g activated carbon fiber, improves 18 percentage points, illustrates that adding activated carbon fiber specific activity charcoal is more effective.
Application example 3, the experiment condition of gas-liquid mixed discharge reactor is with example 1, in methyl orange solution, add 1.5g gac and 0.14g ferrous sulfate, 0.5g active carbon fibre peacekeeping 0.14g ferrous sulfate respectively, investigate of the influence of gas-liquid mixed discharge reactor degradable organic pollutant.
Fig. 4 shows and adds that the degradation rate of tropeolin-D is 90.01% behind 1.5g gac and the 0.14g ferrous sulfate, improves 6.65 percentage points than independent adding gac; The degradation rate of tropeolin-D is 99.99% behind the adding 0.5g active carbon fibre peacekeeping 0.14g ferrous sulfate, improve 7.38 percentage points than adding activated carbon fiber separately, at this moment as seen almost all degradeds, can significantly improve the degradation rate of tropeolin-D behind the adding active carbon fibre peacekeeping ferrous sulfate.
Claims (6)
1, the method for organic pollutant in the gas-liquid mixed discharge degradation water, it is characterized in that: at the reactor bottom injecting gas, make the gas uniform distribution in lower floor's solution, applying high-voltage pulse between parallel corresponding high voltage electrode that is provided with and the ground electrode between lower floor's solution and the upper solution, under the high-strength electric field effect, utilize the low-temperature plasma of liquid phase generation and the ozone of gas phase generation to directly act on organic pollutant.
2, the method for organic pollutant in the gas-liquid mixed discharge degradation water according to claim 1, it is characterized in that: in upper solution, the metal barrier net is set, add gac, active carbon fibre peacekeeping ferrous ion in solution, the add-on of gac, active carbon fibre peacekeeping ferrous ion is respectively 3-20g/L, 1-15g/L and 0.1-10g/L.
3, the device of organic pollutant in a kind of gas-liquid mixed discharge degradation water, comprise reactor, high voltage electrode in the cooling sandwith layer of reactor ectosome and the reactor, ground electrode and outside high-voltage pulse power source, it is characterized in that: the bottom of reactor is provided with core, high voltage electrode is positioned at the upper surface of core, by being connected with high-voltage pulse power source by lead after several apicule needle parallel connections, the prong diameter is less than 0.25mm, ground electrode is on the interface of gas phase and upper solution, by fixed link and wiring nut ground connection, the thickness of ground electrode is 0.3～2mm, its diameter is than the little 1～4mm of reactor inner diameter of steel flue, distance between high voltage electrode 1 and the ground electrode 2 is less than 200mm, and the distance between ground electrode 2 and the liquid-gas interface 7 is less than 2mm.
4, the device of organic pollutant in a kind of gas-liquid mixed discharge degradation water, comprise reactor, high voltage electrode in the cooling sandwith layer of reactor ectosome and the reactor, ground electrode and outside high-voltage pulse power source, it is characterized in that: the bottom of reactor is provided with core, ground electrode is positioned at the upper surface of core, the thickness of ground electrode is 0.3～2mm, its diameter is than the little 1～4mm of reactor inner diameter of steel flue, high voltage electrode is on the interface of gas phase and upper solution, by fixed link and wiring nut ground connection, by being connected with high-voltage pulse power source by lead after several apicule needle parallel connections, the prong diameter is less than 0.25mm, distance between high voltage electrode 1 and the ground electrode 2 is less than 200mm, and the distance between ground electrode 2 and the liquid-gas interface 7 is less than 2mm.
5, according to the device of organic pollutant in claim 3 or the 4 described gas-liquid mixed discharge degradation water, it is characterized in that: vertical direction is provided with the several layers of metal barrier net that is parallel to each other in upper solution, the metal barrier net is fixed on the fixed link, is uniformly distributed in the upper solution.
6, according to the device of organic pollutant in claim 3 or the 4 described gas-liquid mixed discharge degradation water, it is characterized in that: the polarity of high voltage needle electrode can be changed, as change the setting of high-voltage pulse power source, when applying the negative high voltage pulse, the polarity of high voltage needle electrode becomes the negative high voltage pulse by original positive high voltage pulse; When applying the positive or negative high voltage pulse, the polarity of high voltage needle electrode changes from the positive high voltage pulse to the negative high voltage pulse cycle.
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Cited By (7)
| Publication number | Priority date | Publication date | Assignee | Title |
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| CN101935092A (en) * | 2010-07-21 | 2011-01-05 | 北京交通大学 | Water treatment device for combining low-temperature plasma and air oxidation |
| CN102190352A (en) * | 2011-04-15 | 2011-09-21 | 中国石油大学(华东) | Gas-phase high pressure pulse discharge device and method for catalytically degrading organic dyes in water by same |
| CN102351282A (en) * | 2011-08-12 | 2012-02-15 | 宁波大学 | Device and method for treating difficultly degraded organic waste water by plasma technology |
| CN107522257A (en) * | 2016-06-21 | 2017-12-29 | 江苏如意环境工程有限公司 | Ultrasonic wave and UV photodissociation Fenton towers |
| CN108383199A (en) * | 2018-03-29 | 2018-08-10 | 南京中意昂环境科技发展有限公司 | A method of utilizing corona treatment water |
| CN112374586A (en) * | 2020-10-29 | 2021-02-19 | 南京林业大学 | Method for removing organic matters in water by improving plasma-Fenton reaction |
| CN114887565A (en) * | 2022-04-15 | 2022-08-12 | 浙江理工大学 | Liquid phase discharge device and application thereof |
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2006
- 2006-09-26 CN CNB2006100689950A patent/CN100509641C/en not_active Expired - Fee Related
Cited By (11)
| Publication number | Priority date | Publication date | Assignee | Title |
|---|---|---|---|---|
| CN101935092A (en) * | 2010-07-21 | 2011-01-05 | 北京交通大学 | Water treatment device for combining low-temperature plasma and air oxidation |
| CN101935092B (en) * | 2010-07-21 | 2013-03-13 | 北京交通大学 | Water treatment device for combining low-temperature plasma and air oxidation |
| CN102190352A (en) * | 2011-04-15 | 2011-09-21 | 中国石油大学(华东) | Gas-phase high pressure pulse discharge device and method for catalytically degrading organic dyes in water by same |
| CN102190352B (en) * | 2011-04-15 | 2013-09-18 | 中国石油大学(华东) | Gas-phase high pressure pulse discharge device and method for catalytically degrading organic dyes in water by same |
| CN102351282A (en) * | 2011-08-12 | 2012-02-15 | 宁波大学 | Device and method for treating difficultly degraded organic waste water by plasma technology |
| CN102351282B (en) * | 2011-08-12 | 2013-04-24 | 宁波大学 | Device and method for treating difficultly degraded organic waste water by plasma technology |
| CN107522257A (en) * | 2016-06-21 | 2017-12-29 | 江苏如意环境工程有限公司 | Ultrasonic wave and UV photodissociation Fenton towers |
| CN108383199A (en) * | 2018-03-29 | 2018-08-10 | 南京中意昂环境科技发展有限公司 | A method of utilizing corona treatment water |
| CN112374586A (en) * | 2020-10-29 | 2021-02-19 | 南京林业大学 | Method for removing organic matters in water by improving plasma-Fenton reaction |
| CN114887565A (en) * | 2022-04-15 | 2022-08-12 | 浙江理工大学 | Liquid phase discharge device and application thereof |
| CN114887565B (en) * | 2022-04-15 | 2024-01-12 | 浙江理工大学 | Liquid phase discharge device and application thereof |
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