CN1789150A - Method and apparatus for highly efficient removal of water organisms by utilizing photoelectric Fenton reaction - Google Patents
Method and apparatus for highly efficient removal of water organisms by utilizing photoelectric Fenton reaction Download PDFInfo
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- CN1789150A CN1789150A CN 200410098592 CN200410098592A CN1789150A CN 1789150 A CN1789150 A CN 1789150A CN 200410098592 CN200410098592 CN 200410098592 CN 200410098592 A CN200410098592 A CN 200410098592A CN 1789150 A CN1789150 A CN 1789150A
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Abstract
The invention provides a photoelectrical FenDun method for removing the non-degradable organic substance in water, which combines photochemistry reaction and electrical FenDun reaction to co-treat the organic substance effectively with multiple actions. The invention also provides a device applying the photoelectrical FenDUN reaction to remove organic substance in water, which comprises: the reactor employing shape stable electrode (DSA) as anode, employing activated charcoal as cathode, putting the low pressure mercury vapor lamp closed in the quartz glass tube vertically between the anode and cathode and venting a certain quantity of oxygen to the cathode surface, adding marginal ferrous salt into the organic wastewater with pH being about 3 as catalyst and importing current flow for electrolysis to remove pollutant. The invention oxides and degrades organic substance by using the hydroxyl free radical generated by photochemical reaction and electrical FenDun reaction, the hydroxyl free radical possesses strong oxidability which can oxide organic substance without selection, and is characterized by the complete, fast and effective oxidation and no secondary pollution.
Description
Technical field
The present invention relates to a kind of efficient water treatment process and the device of water and wastewater treatment, purify waste water and waste water thereby utilize light to help electro-Fenton reaction to be used in the degradation water organism.Specifically be to utilize the activated carbon fiber of high-specific surface area as negative electrode, the steady electrode of shape is as anode, ultraviolet lamp places airtight silica tube vertically to be positioned between the anodic-cathodic, at cathode surface aerating oxygen or air, oxygen molecule can generate hydrogen peroxide in the reduction of activated carbon fiber cathode surface effectively, a certain amount of ferrous ion that adds in hydrogen peroxide and the solution or iron ion generation Fenton's reaction, simultaneously the reduction reaction can take place at cathode surface with under UV-irradiation and generates ferrous ion and continue to participate in organism in the Fenton's reaction degradation water in iron ion, and the hydrogen peroxide that produces of electrochemistry can issue estranged separating in the ultraviolet light irradiation and generate the hydroxyl radical free radical degradation of organic substances simultaneously.At anode electrochemical oxidation, electric Fenton, UV/H
2O
2The acting in conjunction of reaction is issued to the organic purpose of efficient removal.
Technical background
The treatment technology of bio-refractory organic waste water is a difficult point in the environmental improvement always in the environment for a long time, also is the important topic of puzzlement home and abroad environment scientific circles.Common concern organic contamination problem in countries in the world has proposed the priority pollutants list one after another.These preferential control organic pollutants have following characteristics mostly: 1. be difficult to degraded or not degraded, progressively enrichment in environment has certain residual level; 2. has biological accumulation; 3. have " three cause " effect or toxicity, HUMAN HEALTH and ecotope are constituted potential threat.Traditional biological process seems powerless when handling this type organic.Widely used now method has coagulating sedimentation, absorption, chemical oxidation, ion-exchange etc., but all needs to consume more pharmaceutical chemicals and starting material, and expense is higher, complicated operation, and have the secondary pollution problem.
The research that utilizes high-level oxidation technology to handle organic wastewater with difficult degradation thereby has in recent years obtained significant progress.(Advanced Oxidation Processes AOPs) is called the deep oxidation technology again to high-level oxidation technology, and this process can produce oxide of high activity intermediate hydroxyl radical free radical, and it has very high redox potential (E
0=+2.80V) can not have the selective oxidation organism, makes its degraded even inorganicization.Wherein the most representative with Fenton's reaction.It utilizes hydrogen peroxide and ferrous ion reaction to produce hydroxyl radical free radical, can remove the hardly degraded organic substance that traditional wastewater processing technology can't be removed by the efficient oxidation.Advantages such as this method is simple to operate because of it, reaction is quick enjoy favor.Along with going deep into of research,, in the technology introduction Fenton methods such as electrochemistry, light Fenton and electro-Fenton reaction have been formed again UV-light UV.Wherein electric Fenton technology is in the weakly acidic solution system (optimum response pH is about 3.0), utilize oxygen molecule to generate hydrogen peroxide at the cathode surface electrochemical reduction, the ferrous ion generation Fenton's reaction with catalytic capability in it and the water produces the process of hydroxyl radical free radical degradation of organic substances.Wherein ferrous ion plays catalyzer in reaction, and after promptly it and hydroperoxidation generated ferric ion, iron ion can regenerate ferrous ion with hydrogen peroxide generation reduction reaction, continues to participate in Fenton's reaction.The iron ion that generates in electro-Fenton reaction also can generate ferrous ion in negative electrode generation reduction reaction.And under UV-irradiation, photoreduction also can take place and generate ferrous ion in iron ion.And studies show that wavelength can make the hydrogen peroxide photodissociation less than the ultraviolet radiation of 380nm, promptly hydrogen peroxide decomposition generates hydroxyl radical free radical, therefore, introduces UV-irradiation and can improve method to organic palliating degradation degree in electro-Fenton reaction.
Summary of the invention
The objective of the invention is: it is in the electro-Fenton reaction of negative electrode that ultraviolet radiation is introduced with the high-specific surface area activated carbon fiber, photochemical reaction and electrochemical reaction are combined becomes an advantages of simplicity and high efficiency equipment, make full use of the iron ion photoreduction, the synergy of hydrogen peroxide optical radiation decomposition and electro-Fenton reaction is purified water quality.
The present invention adopts the activated carbon fiber of high-specific surface area as negative electrode, oxygen molecule can generate hydrogen peroxide in its surperficial high-efficiency electrochemical reduction, and, utilize UV-light to promote the reduction of iron ion and the optical radiation of hydrogen peroxide to decompose because electro-Fenton reactor is introduced low pressure mercury lamp.The synergy that electro-Fenton reaction decomposes owing to the photoreduction and the hydrogen peroxide optical radiation of iron ion under the effect of UV-light makes the organic efficient degraded, thereby improves the efficient of electrochemical oxidation.
Reaction unit of the present invention as shown in drawings.Positive plate 1 and negative plate 2 be at certain intervals in the fixed reactor 3, and low pressure mercury lamp 5 is placed airtight silica tube 4, and reaction soln is by magnetic agitation 6 circulations, and the electric current of D.C. regulated power supply 7 is applied on positive plate 1 and the negative plate 2.Instrument 10 is trip switchs of ultraviolet source, and oxygen is fed by airway 8, and whole reactor places airtight reaction box 11.The voltage and current of electrochemical reaction is by voltage stabilized source 7 controls.Sample regularly takes out analytical solution TOC and color removal by thief hole 9;
Concrete grammar of the present invention is as follows:
Positive plate 1 and negative plate 2 are fixed in the circular reactor 3 with certain spacing, and silica tube 5 vertical fixing that will place airtight low pressure mercury lamp 4 connect the circuit of power supply and light source simultaneously between two-plate.The finite concentration organic wastewater that contains about pH3 is injected in the reactor 3, adds a certain amount of supporting electrolyte and use magnetic stirring apparatus 6 stirred solutions.The off-response chamber door, aerating oxygen 5 minutes before reaction beginning so that in the solution dissolved oxygen saturated.With control open the light 10 and power supply 7 connect respectively, by regulating D.C. regulated power supply 7 electrochemical reaction is carried out under certain current density, by regulating conditions such as strength of current, oxygen flow, pH, ferrous ion concentration electrochemical reaction and organism are fully reacted, to reach the highest removal efficient.
Characteristics of the present invention are as follows:
1,, make two kinds of removal organism processes integrated in a reactor with photoprocess process and the integrated use of electric Fenton oxidising process.
2, adopt have high-specific surface area activated carbon fiber as negative electrode, electrochemical reduction can take place on the kind electrode surface and generate the essential hydrogen peroxide of electro-Fenton reaction in oxygen molecule.
3, adopt low pressure mercury lamp as ultraviolet source, the ultraviolet radiation of certain wavelength of necessity can be provided, what promote Fenton's reaction and hydrogen peroxide photolysis effectively carries out more abundant oxidation of organic compounds.
4, activated carbon fiber has good physicochemical property, and is relatively stable in electrochemical reaction.
5, this method adopts the Activated Carbon Fiber Electrodes with high-specific surface area as negative electrode, and kind electrode can the active adsorption organism in electrolytic process, on its surface DeR efficiently takes place.
6, working method is simple, facility compact, easy handling.
7, various parameters are controlled easily, can be as required conditioned reaction parameter at any time.
8, the anode of Cai Yonging is a dimensional stable anode, has very long work-ing life, can under very extreme condition, use, and stripping hardly in electrolytic process, can not cause secondary pollution to water.
Embodiment
Embodiment 1. different treatment processes are to organic removal
Reaction target solution volume: 450ml
Reaction target solution concentration: Acid Red B 200mg/L
Solution initial pH value: 3.00
Pole plate area: 27cm
2
Electrolyte concentration: 0.05M Na
2SO
4
Oxygen gas flow rate: 100ml/min
Reaction times: 360min
Be respectively anodic oxidation (negative electrode is a titanium ruthenium net electrode), activated carbon fiber (ACF) absorption (no power), electric Fenton oxidation (do not add light, Fe
2+1mM) and photoelectricity Fenton oxidation (Fe
2+1mM adds UV-light) handle Acid Red B solution, TOC removal situation is as shown in table 1 before and after handling.
Table 1 embodiment 1 different methods is to the clearance of TOC
| Time (min) | Handle 60min | Handle 120min | Handle 180min | Handle 360min |
| ACF absorption | 3.7％ | 5.9％ | 6.9％ | 11.1％ |
| Electrooxidation | 2.3％ | 3.2％ | 3.9％ | 13.5％ |
| The electricity Fenton | 8.6％ | 19.7％ | 30.4％ | 58.5％ |
| The photoelectricity Fenton | 14.1％ | 39.6％ | 78.7％ | 95.7％ |
From embodiment 1 as can be seen, the photoelectricity Fenton's reaction can effectively be degraded and be removed organic pollutant in the water, and it is removed efficiency ratio carbon fiber adsorption and catalytic combustion, electrooxidation and electro-Fenton reaction and all wants height.
The influence of strength of current in the embodiment 2. photoelectricity Fenton's reaction processes
Reaction target solution volume: 450ml
Reaction target solution concentration: Acid Red B 200mg/L
Solution initial pH value: 3.00
Electrolyte concentration: 0.05M Na
2SO
4
Oxygen gas flow rate: 100ml/min
Strength of current: 0.12A, 0.24A, 0.36A, 0.50A
Reaction times: 360min
It is as shown in table 2 that TOC removes situation before and after handling.
Table 2 embodiment 2 strength of current influence TOC removal situation
From embodiment 2 as can be seen, along with strength of current improves, the also corresponding raising of the clearance of TOC, this is because the cause that the hydrogen peroxide generation improves.
The photoelectricity Fenton is removed Acid Red B under the embodiment 3. gas with various situations
Reaction target solution volume: 450ml
Reaction target solution concentration: Acid Red B 200mg/L
Solution initial pH value: 3.00
Pole plate area: 27cm
2
Electrolyte concentration: 0.05M Na
2SO
4
Gaseous species: Ar, O
2
Gas flow rate: 100ml/min
Strength of current: 360mA
When feeding gas is respectively oxygen and argon gas Acid Red B solution is handled, TOC removal situation is as shown in table 3 before and after handling.
The table 3 embodiment 3 different gases that feed are removed influence to TOC
| Time (min) | TOC removes situation | |||
| 60 | 120 | 180 | 360 | |
| O 2 | 14.1％ | 39.6％ | 78.7％ | 95.7％ |
| Ar | 12.1％ | 37.5％ | 59.8％ | 87.8％ |
By embodiment 3 as can be seen, the kind that feeds gas has certain influence to photoelectricity Fenton degraded Acid Red B, the feeding of oxygen helps organic better mineralising removes, but removal effect is preferably also arranged when argon gas feeds, and this is to separate out owing to anode in the electrolytic process has oxygen.
Claims (10)
1. photoelectricity Fenton method of removing organic pollutant in the water, it is characterized in that UV-light is introduced electro-Fenton reaction, oxygen in water produces hydrogen peroxide at the carbon cathode surface reduction can produce hydroxyl radical free radical with the ferrous ion reaction in the water, also can under ultraviolet radiation, produce hydroxyl radical free radical, the synergistic oxidation degradable organic pollutant, and UV-light can promote the iron ion photoreduction to generate ferrous ion, promotes the carrying out of Fenton's reaction.
2. the method for claim 1, wherein electro-Fenton reaction as negative electrode, is used SnO with activated carbon fiber, graphite, carbon fiber felt etc.
2/ Ti, PbO
2/ Ti, titanium-ruthenium electrode etc. are as anode.
3. the method for claim 1 wherein adopts activated carbon fiber as negative electrode, and this electrode has conduction, and characteristics such as high-specific surface area have very strong adsorptive power, have the character of accurate three-diemsnional electrode, therefore has higher reaction efficiency.
4. the method for claim 1, wherein ultraviolet source adopts low pressure mercury lamp, also can adopt medium pressure mercury lamp.
5. in accordance with the method for claim 1, wherein utilize ferrous ion or iron ion as catalyzer, their concentration is in 0.5mM～3mM scope.
6. in accordance with the method for claim 1, wherein being reflected at pH carries out under the acidic conditions about 2-5.
7. device that utilizes the photoelectricity Fenton's reaction to remove hardly degraded organic substance in the water, it is characterized in that, UV-light is introduced in the electro-Fenton reactor, use the charcoal base electrode, as activated carbon fiber, as negative electrode, dimensional stable anode (DSA) is made anode, the electrochemical reactor that the cathodic area has oxygen to feed, the pH value of solution value wherein adds ferrous ion or iron ion as catalyzer about 2-5, open light source and feed electric current reaction is carried out, the intensity of light source by the control reaction, strength of current, iron ion or ferrous ion concentration, electrolyte concentration, pH values etc. realize the organic effective removal in the water.
8. according to the described device of claim 6, it is characterized in that anti-activated carbon fiber, graphite, the carbon felt etc. of adopting of photoelectricity Fenton are used SnO as negative electrode
2/ Ti, PbO
2The steady electrode of shape such as/Ti, titanium-ruthenium electrode is as anode.
9. according to the described device of claim 6, it is characterized in that having oxygen to inject in the cathodic area, the oxygen that also can directly utilize anode electrolysis water to generate perhaps injects air so that solution reaches higher dissolved oxygen concentration, more helps producing hydrogen peroxide.
10. according to the described device of claim 6, it is characterized in that, in reactor, adopt low pressure mercury lamp, medium pressure mercury lamp etc. as ultraviolet source.
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| CN101798130A (en) * | 2010-04-02 | 2010-08-11 | 中国科学院苏州纳米技术与纳米仿生研究所 | Wastewater treatment method based on electro-Fenton reaction |
| CN102070230A (en) * | 2010-12-10 | 2011-05-25 | 华中师范大学 | Method for removing organic matters in water by utilizing three-dimensional electrode electro-fenton and device thereof |
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| CN112429801A (en) * | 2020-09-30 | 2021-03-02 | 南昌航空大学 | Method for treating high-concentration organic wastewater by ultraviolet light in cooperation with electrochemical oxidation |
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