CN1440934A - Water-treating bipolar pulse discharge process - Google Patents
Water-treating bipolar pulse discharge process Download PDFInfo
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- CN1440934A CN1440934A CN 03111418 CN03111418A CN1440934A CN 1440934 A CN1440934 A CN 1440934A CN 03111418 CN03111418 CN 03111418 CN 03111418 A CN03111418 A CN 03111418A CN 1440934 A CN1440934 A CN 1440934A
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Abstract
The present invention belongs to the field of low temperature plasma applying technology and is especially a high-grade discharging and low temperature plasma oxidizing water processing method. One in-situ bipolar pulse discharge low temperature plasma water voltage power supply, covering of the discharge electrodes with medium, filling of the gap between the electrodes by air-liquid mixture of fine bubbles and processed water. The present invention has strengthened electric field between the electrodes, protected high-voltage electrodes and long service life, and may be used in sterilizing water, decoloring waste water and catalytically degrading matters hard to degrade biologically and lasting organic pollutant.
Description
Technical field
The invention belongs to the applied technical field of low-temperature plasma, relate in particular to a kind of discharge low-temperature plasma advanced oxidation treatment process of water.
Background technology
At present, for the organic pollution materials and the persistence organic pollutant matter of difficult for biological degradation in the water, conventional treatment process such as physico-chemical process processing efficiency are low.Because compound property is stable, have even growth restriction micro-organisms, so biological method also is difficult to play a role.
High-level oxidation technology that new development is got up such as Fenton (Fenton) are though reagent method processing efficiency height is very expensive for creating the reagent that Fenton's reaction provides.Ozone and combination ozone oxidation method thereof, because of ozonizer costs an arm and a leg, and the luminous efficiency of ozone is low, and energy consumption is bigger, and energy is not fully utilized in the discharge process.Photocatalysis method equipment is simple, and is easy to operate, but its photo-quantum efficiency is low, to the requirement height of light wave.
The equipment volume of beam methods generation electron beam is huge, the generation of electron beam and acceleration equipment complexity, equipment and working cost height.
The water treatment of geseous discharge nonthermal plasma chemistry method is a kind of technology that just grows up in recent years.The electrode structure of plasma discharging body method water processing reactor commonly used has discharge type on point (pin)-plate, line-plate structure form and the liquid level in the solution.There is serious etching problem in point (pin) as high voltage electrode in the reactor of point (pin)-template electrode structure, document " Physics of Plasma " 2001,8 (5) " Pulse electrical discharges in water and their applications " report is the pin electrode of R～0.05mm for needle type radius, when mean power is 100W, the mean lifetime of electrode only is 10～20 minutes, the volume that while single needle (or point) occupies in reactor is little, and it is few to be subject to processing liquid volume.The reactor of discharge type exists the short life free radical and sees through gas-bearing formation to liquid level diffusive migration and the active specy mass transfer problem by fluid level gauge course deep layer on the liquid level, only be top layer liquid thereby limited the water that is subject to processing, make the advantage of discharge water treatment method be difficult to performance.
The generation of the active specy in the discharge process (as high-energy electron, free radical and ozone such as OH, hydrogen peroxide etc.) has significant effects for the water treatment effect.High-energy electron directly influences the generation efficient of these species.Compare with direct current, unipolar pulse power supply is beneficial to the acceleration of electronics, and heavy particle such as speeding-up ion not, treatment effect improves.Dalian University of Technology's master thesis (2001,3) " electrion plasma body water treatment research " reported that interelectrode distance is 30mm, discharge unipolar pulse voltage 25KV, handle 30min after, the percent of decolourization of indigo disulfonic acid sodium solution reaches 80%, and treatment effect is undesirable.
The improvement that the DBD discharge that is coated with dielectric on the electrode is used for the gaseous contamination material as degraded VOCs, to produce aspect research such as ozone more.With the discharge reactor power supply of unipolar pulse power supply to this form, because the existence of medium, the electric charge that accumulates on the medium is difficult to release and forms hangover, is unfavorable for the processing of discharging.This phenomenon is more obvious when being used for the processing of fluid contaminants matter.
Bipolar pulse is used for the generation of ozone, feasible discharge has the advantage of corona discharge and DBD discharge concurrently, can improve discharge in the intensity of micro discharges, increase the output of ozone, but the bipolar pulse power supply is used for online gas liquid mixture discharge water treatment, yet there are no report.
Summary of the invention
The purpose of this invention is to provide a kind of bipolar pulse power supply that utilizes to the electrode power supply that is coated with dielectric, electric field between intensifier electrode, form more micro discharges, produce more active specy, realize water sterilization more efficiently, the decolouring of waste water is the method for catalyzed degradation difficult for biological degradation and persistence organic pollutant matter (POPs) particularly, and it is low to solve existing discharge plasma water treatment efficiency, acts on unconspicuous problem.
Technical scheme of the present invention is to utilize the discharge reactor power supply of plate-plate of being coated with dielectric on the bipolar pulse power supply counter electrode, point (pin)-plate, line-plate, line (post)-barrel structure form.
This method is according to the principle of corona discharge, ebb-flow discharge and dielectric barrier discharge, and the exoelectrical reaction treatment system of design is by the bipolar pulse power supply and have the discharge electrode system of dielectric impedance to comprise that high-voltage discharging electrode and low pressure ground electrode constitute.Dielectrics such as the high voltage electrode of reactor and/or ground electrode piece of surface covering glass, pottery.In air, oxygen, nitrogen, the argon gas one or more are through gas dispersion equipment such as gas distribution grid, micro porous aeration head, aeration flexible pipes, being dispersed in the processed water and waste water in entire electrode gap after being dispersed into tiny bubble, also can be that gas and processed water directly enter into electrode gap through formation gas liquid mixtures such as gas-liquid mixed equipment such as gas-liquid mixing pumps.Gas liquid mixture discharges under the effect of electric field outside, produces low-temperature plasma.Be rich in the active specy of strong oxidizing property such as hydroxyl radical free radical, ozone, hydrogen peroxide etc. in the discharge plasma passage, and hydrated electron (e
Aq -); Simultaneously, launch UV-light with katalysis, shockwave etc. in the discharge channel evolution.These materials and effect and electric field directly act on processed water, have realized online gas liquid mixture discharge water treatment, have improved the processing efficiency of discharge reactor.
Simultaneously, power supply can also be the high-voltage power supply of interchange, intermediate frequency, high frequency, can also be at the catalyst film that load on electrode in the water and/or the dielectric surface has photocatalytic activity and/or electro catalytic activity that is exposed to of discharge reactor, make full use of the effect of electrode and electric field and discharge, with the effect of further enhancing to water treatment.
Look actual amount of water and processing requirements, above-mentioned a plurality of reactors can plural serial stage or parallel operation, reaches the purpose of actual needs.
Effect of the present invention and benefit are:
1, the applying double pole pulse power in conjunction with the creation of gas-liquid mixed environment, has improved the intensity of discharge, thereby has improved the generation efficient of active specy in the discharge plasma greatly, has strengthened the water treatment effect.
2, the dielectric on the electrode has strengthened electric field between electrode, protects high voltage electrode simultaneously, has prolonged the life-span of electrode.
3, the discharge of gas liquid mixture, make the active specy that produces in the discharge process and effect and electric field directly act on processed water, realized online discharge process, improved the processing efficiency of discharge reactor, realize water sterilization more efficiently, the decolouring of waste water is the purpose of catalyzed degradation difficult for biological degradation and persistence organic pollutant matter (POPs) particularly.
4, the catalyzer isoreactivity material of load on the electrode materials has made full use of the UV-light of electric field and discharge generation etc., makes discharge process and katalysis in addition integrated collaborative, has improved the effect of water treatment.
Description of drawings
Fig. 1 is power supply, the discharge process system diagram of bipolar pulse discharge water treatment method.
(1) reactor shell among the figure; (2) wire netting tube; (3) high voltage electrode; (4) glass insulation medium; (5) gas inlet; (6) aeration head; (7) liquid entrance valve; (8) scupper valve; (9) venting port; (10) bipolar pulse power supply.
Fig. 2 is the example structure of reactor figure of the inventive method.
(1) reactor shell among the figure; (2) wire netting tube; (3) high voltage electrode; (4) glass insulation medium; (5) gas inlet; (6) aeration head; (7) liquid entrance valve; (8) scupper valve; (9) venting port; (11) retaining plate; (12) angle steel skeleton; (13) high-voltage connection inlet; (14) upper cover plate; (15) limited block; (16) bolt.
Embodiment
Below in conjunction with Figure of description, be described in detail most preferred embodiment of the present invention.
In order better to quicken the unbound electron in the discharge process, and speeding-up ion not, to produce more active specy, power supply adopts bipolar pulse power supply (10), its power parameter is: 1～200 kilovolt of peak-to-peak value voltage, 30～300 nanoseconds of rise time of a pulse, 1～2000 hertz of pulse-repetition frequency.
Reactor adopts the barrel type reactor of post-tubular electrode structure, the surface of high voltage electrode (3) and gas liquid mixture contact part are evenly covered by glass insulation medium (4) fully, metal high voltage electrode (3) and gas liquid mixture are kept apart, guarantee that simultaneously dielectric does not have obvious edges and corners and projection, avoids the generation of intensive shelf depreciation.The existence of dielectric has strengthened interelectrode electric field, is beneficial to the acceleration of the electronics in the bubble, has improved the efficient of water treatment.
Reactor shell shown in Figure 2 (1) is a round shape synthetic glass tube, the high 1000mm of synthetic glass cylindrical shell (1), internal diameter 70mm, the tight lining metal net of inwall tube (2) is made ground electrode, high voltage electrode (3) is made for the metal iron staff, links to each other by the output terminal of high-voltage connection through high-voltage connection inlet (13) and bipolar pulse power supply (10).The metal iron staff is close to one deck insulating glass medium (4) outward, the complex body that dielectric (4) and metal high voltage electrode (3) are formed is guaranteed to place with one heart with synthetic glass tube (1) and wire netting tube (2) by the upper cover plate (14) of reactor and limited block (15) the restriction location of bottom.The distance of electrode gap has considerable influence for the treatment effect of reality, and its characteristic and electrode shape of neglecting power supply is greatly determined.
Air from the bottom of reactor by inlet (5) after aeration head (6) is dispersed into tiny microbubble, enter into the exoelectrical reaction space of electrode gap, be distributed in the processed water, form gas liquid mixture, the gas after the discharge is discharged through venting port (9); Liquid enters reactor by inlet valve (7), and is processed after water discharge valve (8) outflow.The flow of gas has certain influence for the effect of experiment, and for the reactor of a fixed structure, this flow has an optimal value, and for this reactor, when liquid was 650ml in the cylindrical shell, optimization tolerance was 0.75m
3/ h.
Aeration head (6) is positioned between the retaining plate (11) and angle steel skeleton (12) of reactor shell (1), and firmly fixed with bolt (16) bolt.
The power supply system shown in figure (1), (2) and the actual effect of reactor are: power supply is the bipolar pulse power supply: 1～200 kilovolt of peak-to-peak value voltage, 30～300 nanoseconds of rise time of a pulse, 1～2000 hertz of pulse-repetition frequency.Adopting air in the experiment is source of the gas, and tolerance 0.75m is being optimized in the flow control of gas
3/ h.Service voltage is controlled under the condition that is lower than sparking voltage and carries out, and all adopting Vpp=19 kilovolt, reactor electrodes spacing in this experiment is 5mm.For absorbancy (Abs) is 1.406, specific conductivity 220 μ s/cm, the 650ml indigo disulfonic acid sodium solution of pH7.27, the processing of process discharge reactor 2.5 minutes, the solution decolorizing efficiency can reach 80.37%, handles 5 minutes, percent of decolourization reaches 98.72%, the specific conductivity of sodium indigotindisulfonate waste water rises simultaneously, and pH descends, and decolorizing effect is obvious.
Claims (2)
1, a kind of bipolar pulse discharge water treatment method is to utilize the bipolar pulse power supply to the electrode power supply that is coated with dielectric, and the electric field between intensifier electrode on the gas liquid mixture forms more micro discharges, it is characterized in that:
A) power supply adopts the bipolar pulse high-voltage power supply;
B) high voltage electrode of discharge reactor and/or low-field electrode are covered by dielectrics such as glass, potteries;
C) gas liquid mixture discharges under the effect of electric field outside; Wherein said gas is one or more in air, oxygen, nitrogen, the argon gas; Gas can be through gas dispersion equipment such as gas distribution grid, micro porous aeration head, aeration flexible pipes, being dispersed in the processed water in entire electrode gap after being dispersed into tiny bubble, also can be that gas and water directly enter into electrode gap through gas-liquid mixed equipment formation gas liquid mixture.
2, bipolar pulse discharge water treatment method according to claim 1, its feature is that also power supply can also be the high-voltage power supply of interchange, intermediate frequency, high frequency; Also can be at dielectric and/or the catalyst film that has catalytic activity with the direct electrodes in contact area load of water one deck.
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