CN103304018B - Method and device for enhanced ozone oxidation wastewater treatment of ozone tail gas - Google Patents
Method and device for enhanced ozone oxidation wastewater treatment of ozone tail gas Download PDFInfo
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- CN103304018B CN103304018B CN201310236853.0A CN201310236853A CN103304018B CN 103304018 B CN103304018 B CN 103304018B CN 201310236853 A CN201310236853 A CN 201310236853A CN 103304018 B CN103304018 B CN 103304018B
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Abstract
The invention relates to a method and a device for enhanced ozone oxidation wastewater treatment of ozone tail gas. According to the method, ozone and oxygen in ozone oxidation reaction tail gas are subjected to electrocatalytic reduction to obtain hydrogen peroxide; the hydrogen peroxide catalyzes the ozone to generate hydroxyl radicals; and organic matters in wastewater are mineralized and decomposed. The device comprises a pre-electrolysis unit and an ozone oxidation unit, wherein a tail gas outlet of the ozone oxidation unit is connected to the pre-electrolysis unit. According to the method and the device, oxygen and ozone resources in the tail gas are fully utilized; destroying treatment is not needed; and an ozone oxidation treatment effect is enhanced.
Description
Technical field
The invention belongs to field of waste water treatment, relate in particular to method and the device of the wastewater treatment of a kind of ozone tail gas strengthening ozone oxidation.
Background technology
After biological wastewater treatment, residual organic substances is difficult to biological degradation usually.These organism have carcinogenic, teratogenesis and mutagenic " three cause " effect, very harmful, must give deep removal.For the hardly degraded organic substance of these lower concentrations, feasible technology is mainly adsorption and oxidation.Absorption method adopts gac etc. as sorbent material usually, and the loading capacity of gac is limited, and saturated rear regeneration cost is very high, and hardly degraded organic substance adsorbs saturated waste carbon simultaneously becomes dangerous solid waste and brings secondary pollution.Oxidation technology mainly adopts high-level oxidation technology.In numerous high-level oxidation technologies, the technical finesse costs such as photochemical catalysis, catalytic wet oxidation, electrocatalysis and ultrasonic cavitation are higher, and current primary limitation is in the laboratory study stage.Possesses the high-level oxidation technology high-level oxidation technology that mainly Fenton is relevant with ozone of industrial applications prospect at present.Fenton oxidation technical risk is little, reliable, but cost is higher, particularly adds iron ion and soda acid adjustment introduces a large amount of salt and is unfavorable for waste water recycling toward waste water in, generation iron mud secondary pollution simultaneously.The high-level oxidation technology that ozone is correlated with, except homogeneous phase ozone catalytic, does not usually need to add soda acid, does not produce secondary pollution.Particularly along with the industrialization of Large Efficient rate ozone machine, ozone oxidation is made to have more technology competition.Simple ozone oxidation has selectivity, better to the treatment effect of some unsaturated compoundses and aromatic compound, but be difficult to organism permineralization, simultaneously very poor to organism treatment effects such as some small molecules lipid acid, so generally ozone oxidation and additive method are used in conjunction, make it to produce the stronger hydroxyl radical free radical of oxidation capacity, thus by mineralization of organic material, improve treatment effect, if catalytic ozonation technology utilizes catalyst ozone decomposition to produce hydroxyl radical free radical.But homogeneous catalyst often brings heavy metal secondary pollution, and oxide compound heterogeneous catalyst efficiency is not high, easy inactivation in waste water simultaneously; Ozone-hydrogen peroxide (O
3/ H
2o
2) technology, utilize hydrogen peroxide catalyzed ozone generation hydroxyl radical free radical, do not introduce catalyst ion, do not have secondary pollution, but the hydrogen peroxide cost added is higher, hydrogen peroxide accumulating danger is high.
Particularly based on wastewater treatment, generally adopt source of oxygen, obtain higher ozone concn.Because ozone is difficult to absorb completely and react, still contain certain density ozone in tail gas after process, if directly enter air, can air environmental pollution be caused, need to carry out harmless treatment.In tail gas, main component is oxygen, and other are containing a small amount of ozone, water vapor, carbonic acid gas etc., and cost is higher on the one hand to carry out destroying process up to standard, wastes oxygen and ozone resource on the other hand.
Summary of the invention
The weak effect and the tail gas that the present invention is directed to existing simple ozone oxidation existence need to destroy the problems such as process, propose method and the device of the wastewater treatment of a kind of ozone tail gas strengthening ozone oxidation.
For reaching this object, the present invention by the following technical solutions:
An object of the present invention is to provide a kind of ozone tail gas to strengthen the method for ozone oxidation wastewater treatment, and described method makes the ozone in ozone oxidation reaction tail gas and oxygen electrical catalyze reduction be hydrogen peroxide; Described hydrogen peroxide catalyzed ozone generation hydroxyl radical free radical, decomposes the mineralization of organic material in waste water.
The method of the invention utilizes ozone in ozone oxidation reaction tail gas and oxygen resource, makes it be converted into hydrogen peroxide, the treatment effect of strengthening waste water by ozone oxidation.Electrocatalysis of the present invention and produce the operation of hydroxyl radical free radical and all belong to and well known to a person skilled in the art operation.
Particularly, described method makes waste water first enter preelectrolysis unit to carry out electrolytic reaction, and the waste water after electrolytic reaction flows into ozone oxidation unit; In ozone oxidation unit, pass into ozone react, aeration in the ozone tail gas access preelectrolysis unit that ozone oxidation unit produces.
Waste water after electrolytic reaction enters ozone oxidation unit through pump or from high head gravity flow.
In described electrolytic reaction, control electrolysis voltage is 2 ~ 7V, preferred 4V.
Two of object of the present invention is to provide a kind of ozone tail gas to strengthen ozone oxidation wastewater treatment equipment, and described treatment unit comprises preelectrolysis unit and the ozone oxidation unit of connection; The offgas outlet of described ozone oxidation unit is connected into preelectrolysis unit.
Described preelectrolysis unit comprises electric catalysis reactor, is wherein provided with anode and negative electrode; Described anode is titanium base ruthenium dioxide or titanium-based titanium dioxide; Described negative electrode is the powder electrode of graphite felt, activated carbon fiber, gac or carbon nanotube and ptfe emulsion adhering and pressing.The typical but non-limiting example of described negative electrode is: graphite felt, activated carbon fiber, the powder electrode of gac and ptfe emulsion adhering and pressing, the powder electrode of carbon nanotube and ptfe emulsion adhering and pressing.
Electric catalysis reactor of the present invention comprises reactor shell, and described anode and negative electrode are positioned at reactor shell internal space; Aerating apparatus is provided with bottom reactor shell.
Described reactor shell is provided with waste water inlet, wastewater outlet and tail gas discharging pipe.The concrete setting of described waste water inlet, wastewater outlet and tail gas discharging pipe can be selected by those skilled in the art, and the present invention there is no particular restriction.Preferably, waste water inlet is located at the bottom of reactor shell, wastewater outlet is located at the middle part of reactor shell, and tail gas discharging pipe is located at the top of reactor shell.
The aeration head of described aerating apparatus is pure titanium micro porous aeration head or silica gel micro porous aeration head.Described aeration head is arranged in the below of described negative electrode; Described aerating apparatus air inlet is the ozone tail gas that ozone oxidation unit produces.
Ozone oxidation unit of the present invention comprises ozone oxidation reaction device; Be provided with ozone entrance and ozonation aerated device bottom described ozone oxidation reaction device, top is provided with water-distributing device, and top is provided with ozone oxidation tail gas discharging pipe and vacuum pressure valves; Described ozone oxidation tail gas discharging pipe is connected into the aerating apparatus of electric catalysis reactor.
The ozone of described ozone oxidation reaction device is oxygen source ozone.
Further, the method for association reaction principle to a kind of ozone tail gas strengthening ozone oxidation of the present invention wastewater treatment is described as follows:
1, electrocatalysis pre-treatment: ozone tail gas electrocatalysis is converted into hydrogen peroxide
Waste water is introduced into preelectrolysis unit (electric catalysis reactor), and the ozone tail gas that follow-up ozone oxidation reaction produces passes into this electric catalysis reactor, and control electrolysis voltage is 2 ~ 7V, and ozone and partial oxidation electrical catalyze reduction are hydrogen peroxide, discharge after tail gas clean-up.Following principal reaction is there is in electric catalysis reactor:
O
2+2H
2O+2e→H
2O
2+2OH
-
Cathodic reaction: 2O
3+ 6H
2o+6e → 3H
2o
2+ 6OH
-
2Cl
--2e→Cl
2
Anodic reaction: organism-ne → oxidation products
Cl
2+ organism → oxidation products+2Cl
-
Reaction in solution: H
2o
2+ organism → oxidation products
2, catalytic ozonation
Electric catalysis reactor water outlet enters ozone oxidation reaction device, and on the one hand, the organism in waste water is decomposed by ozone oxygen; On the other hand, the hydrogen peroxide catalyzed ozone generation hydroxyl radical free radical in waste water, decomposes oxidation operation.Catalytic ozonation reaction process is mainly as follows:
Ozone oxidation reaction: 2O
3+ organism → oxidation products+2O
2↑+H
2o
Catalytic ozonation reacts:
OH+ organism → mCO
2+ nH
2o
Compared with prior art scheme, the present invention has following beneficial effect:
The tail gas of ozone oxidation reaction passes in electric catalysis reactor water inlet by the present invention, ozone in tail gas and oxygen in situ electrical catalyze reduction are hydrogen peroxide, follow-uply react with ozone, produce hydroxyl radical free radical, mineralization of organic material is decomposed, thus enhances ozone oxidation effect.By the present invention, not only take full advantage of the oxygen in tail gas and ozone resource, do not need to destroy process, enhance the treatment effect of ozone oxidation simultaneously.
Accompanying drawing explanation
Fig. 1 is a kind of ozone tail gas strengthening ozone oxidation wastewater treatment equipment of the present invention.
In figure: 1-reactor shell; 2-anode; 3-negative electrode; 4-aerating apparatus; 5-tail gas discharging pipe; The ozonation aerated device of 6-; 7-water-distributing device; 8-ozone oxidation tail gas discharging pipe; 9-vacuum pressure valves; 10-waste water; Waste water after 11-electrolytic reaction; 12-ozone tail gas; 13-ozone; The water outlet of 14-ozone oxidation unit.
The present invention is described in more detail below.But following example is only simple and easy example of the present invention, and do not represent or limit the scope of the present invention, protection scope of the present invention is as the criterion with claims.
Embodiment
For better the present invention being described, be convenient to understand technical scheme of the present invention, typical but non-limiting embodiment of the present invention is as follows:
As shown in Figure 1, a kind of ozone tail gas strengthening ozone oxidation wastewater treatment equipment, described treatment unit comprises preelectrolysis unit and the ozone oxidation unit of connection; The offgas outlet of described ozone oxidation unit is connected into preelectrolysis unit.
Described preelectrolysis unit comprises electric catalysis reactor, and described electric catalysis reactor comprises reactor shell 1, and its internal space is provided with anode 2 and negative electrode 3; Described anode 2 is titanium base ruthenium dioxide or titanium-based titanium dioxide; Described negative electrode 3 is the powder electrode of graphite felt, activated carbon fiber, gac or carbon nanotube and ptfe emulsion adhering and pressing.
Aerating apparatus 4 is provided with bottom reactor shell 1; Described reactor shell 1 is provided with waste water inlet, wastewater outlet and tail gas discharging pipe 5.The aeration head of described aerating apparatus 4 is pure titanium micro porous aeration head or silica gel micro porous aeration head; Described aeration head is arranged in the below of described negative electrode 3; The air inlet of described aerating apparatus 4 is the ozone tail gas 12 that ozone oxidation unit produces.
Described ozone oxidation unit comprises ozone oxidation reaction device; Be provided with ozone entrance and ozonation aerated device 6 bottom described ozone oxidation reaction device, top is provided with water-distributing device 7, and top is provided with ozone oxidation tail gas discharging pipe 8 and vacuum pressure valves 9; Described ozone oxidation tail gas discharging pipe 8 is connected into the aerating apparatus 4 of electric catalysis reactor.
The ozone of described ozone oxidation reaction device is oxygen source ozone.
Embodiment 1
Advanced treatment object is the coking chemical waste water after biological treatment, and COD is about 150mg/L.
First waste water 10 enter preelectrolysis unit and carry out electrolytic reaction, control electrolysis voltage is 2V, and the ozone tail gas 12 that follow-up ozone reaction produces passes into this electric catalysis reactor simultaneously, and anode 2 adopts titanium base ruthenium dioxide plate, negative electrode 3 is graphite felt, and aerating apparatus 4 is pure titanium aeration head.Waste water 11(after electrolytic reaction contains hydrogen peroxide) squeeze into ozone oxidation unit through pump, in ozone oxidation reaction device, pass into ozone 13 react, the ozone that ozone 13 produces for source of oxygen, ozone dosage is 100mg/L.The ozone tail gas 12 that ozone oxidation unit produces accesses the aerating apparatus 4 in preelectrolysis unit.Finally obtaining ozone oxidation unit water outlet 14, COD is 20 ~ 50mg/L, and in the tail gas of preelectrolysis unit discharge, ozone is lower than 0.5ppm.
Embodiment 2
Advanced treatment object is the lincomycin wastewater after biological treatment, and COD is about 300mg/L.
First waste water 10 enter preelectrolysis unit and carry out electrolytic reaction, control electrolysis voltage is 7V, the ozone tail gas 12 that follow-up ozone reaction produces passes into this electric catalysis reactor simultaneously, anode 2 adopts titanium-based titanium dioxide plate, negative electrode 3 is the powder electrode of gac and ptfe emulsion adhering and pressing, and aerating apparatus 4 is pure titanium aeration head.Waste water 11(after electrolytic reaction contains hydrogen peroxide) squeeze into ozone oxidation unit through pump, in ozone oxidation reaction device, pass into ozone 13 react, the ozone that ozone 13 produces for source of oxygen, ozone dosage is 200mg/L.The ozone tail gas 12 that ozone oxidation unit produces accesses the aerating apparatus 4 in preelectrolysis unit.Finally obtaining ozone oxidation unit water outlet 14, COD is 100 ~ 150mg/L, and in the tail gas of preelectrolysis unit discharge, ozone is lower than 0.5ppm.
Embodiment 3
Advanced treatment object is the dyeing waste water after biological treatment, and COD is about 250mg/L.
First waste water 10 enter preelectrolysis unit and carry out electrolytic reaction, control electrolysis voltage is 4V, and the ozone tail gas 12 that follow-up ozone reaction produces passes into this electric catalysis reactor simultaneously, and anode 2 adopts titanium-based titanium dioxide plate, negative electrode 3 is activated carbon fiber, and aerating apparatus 4 is silica gel aeration head.Waste water 11(after electrolytic reaction contains hydrogen peroxide) squeeze into ozone oxidation unit through pump, in ozone oxidation reaction device, pass into ozone 13 react, the ozone that ozone 13 produces for source of oxygen, ozone dosage is 150mg/L.The ozone tail gas 12 that ozone oxidation unit produces accesses the aerating apparatus 4 in preelectrolysis unit.Finally obtaining ozone oxidation unit water outlet 14, COD is 80 ~ 100mg/L, and in the tail gas of preelectrolysis unit discharge, ozone is lower than 0.5ppm.
Embodiment 4
Advanced treatment object is the paper waste after biological treatment, and COD is about 300mg/L.
First waste water 10 enter preelectrolysis unit and carry out electrolytic reaction, control electrolysis voltage is 3V, the ozone tail gas 12 that follow-up ozone reaction produces passes into this electric catalysis reactor simultaneously, anode 2 adopts titanium-based titanium dioxide plate, negative electrode 3 is the powder electrode of carbon nanotube and ptfe emulsion adhering and pressing, and aerating apparatus 4 is silica gel aeration head.Waste water 11(after electrolytic reaction contains hydrogen peroxide) squeeze into ozone oxidation unit through pump, in ozone oxidation unit, carry out passing into ozone 13 react, the ozone that ozone 13 produces for source of oxygen, ozone dosage is 300mg/L.The ozone tail gas 12 that ozone oxidation unit produces accesses the aerating apparatus 4 in preelectrolysis unit.Finally obtaining ozone oxidation unit water outlet 14, COD is 100 ~ 150mg/L, and in the tail gas of preelectrolysis unit discharge, ozone is lower than 0.5ppm.
Applicant states, the present invention illustrates detailed construction feature of the present invention and treatment process by above-described embodiment, but the present invention is not limited to above-mentioned detailed construction feature and treatment process, namely do not mean that the present invention must rely on above-mentioned detailed construction feature and treatment process could be implemented.Person of ordinary skill in the field should understand, any improvement in the present invention, to equivalence replacement and the increase of accessory, the concrete way choice etc. of parts selected by the present invention, all drops within protection scope of the present invention and open scope.
Claims (8)
1. a device for ozone tail gas strengthening ozone oxidation wastewater treatment, it is characterized in that, described treatment unit comprises preelectrolysis unit and the ozone oxidation unit of connection; The offgas outlet of described ozone oxidation unit is connected into preelectrolysis unit;
Described preelectrolysis unit comprises electric catalysis reactor, is wherein provided with anode (2) and negative electrode (3); Described anode (2) is titanium base ruthenium dioxide or titanium-based titanium dioxide; Described negative electrode (3) is graphite felt, the powder electrode of activated carbon fiber, gac or carbon nanotube and ptfe emulsion adhering and pressing;
Described electric catalysis reactor comprises reactor shell (1), and described anode (2) and negative electrode (3) are positioned at reactor shell (1) internal space; Reactor shell (1) bottom is provided with aerating apparatus (4); Described reactor shell (1) is provided with waste water inlet, wastewater outlet and tail gas discharging pipe (5); The aeration head of described aerating apparatus (4) is pure titanium micro porous aeration head or silica gel micro porous aeration head; Described aeration head is arranged in the below of described negative electrode (3);
Described ozone oxidation unit comprises ozone oxidation reaction device; Be provided with ozone entrance and ozonation aerated device (6) bottom described ozone oxidation reaction device, top is provided with water-distributing device (7), and top is provided with ozone oxidation tail gas discharging pipe (8) and vacuum pressure valves (9); Described ozone oxidation tail gas discharging pipe (8) is connected into the aerating apparatus (4) of electric catalysis reactor.
2. treatment unit as claimed in claim 1, is characterized in that, described aerating apparatus (4) air inlet is the ozone tail gas (12) that ozone oxidation unit produces.
3. treatment unit as claimed in claim 1, it is characterized in that, the ozone of described ozone oxidation reaction device is oxygen source ozone.
4. utilize the described treatment unit of one of claim 1-3 to carry out a method for ozone tail gas strengthening ozone oxidation wastewater treatment, it is characterized in that, described method makes the ozone in ozone oxidation reaction tail gas and oxygen electrical catalyze reduction be hydrogen peroxide; Described hydrogen peroxide catalyzed ozone generation hydroxyl radical free radical, decomposes the mineralization of organic material in waste water.
5. method as claimed in claim 4, is characterized in that, described method makes waste water (10) first enter preelectrolysis unit to carry out electrolytic reaction, and the waste water (11) after electrolytic reaction flows into ozone oxidation unit; In ozone oxidation unit, pass into ozone react, aeration in ozone tail gas (12) the access preelectrolysis unit that ozone oxidation unit produces.
6. method as claimed in claim 5, it is characterized in that, the waste water (11) after electrolytic reaction enters ozone oxidation unit through pump or from high head gravity flow.
7. the method as described in claim 5 or 6, is characterized in that, in described electrolytic reaction, control electrolysis voltage is 2 ~ 7V.
8. method as claimed in claim 7, it is characterized in that, in described electrolytic reaction, control electrolysis voltage is 4V.
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| CN106882866A (en) * | 2017-02-24 | 2017-06-23 | 河北科技大学 | The method that hydrogen peroxide synergy ozone heterogeneous catalytic oxidation processes waste water |
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| JPWO2005049502A1 (en) * | 2003-11-19 | 2007-08-23 | 安斉 節 | Wastewater treatment system after biogas generation |
| CN101417835A (en) * | 2008-11-24 | 2009-04-29 | 浙江大学 | Ozone/electrochemistry integrated processing apparatus and method for organic wastewater |
| CN102701496B (en) * | 2012-06-25 | 2013-08-21 | 重庆地质矿产研究院 | Process for treating high-concentration degradation-resistant organic wastewater |
| CN202924812U (en) * | 2012-11-14 | 2013-05-08 | 北京赛科康仑环保科技有限公司 | Organic wastewater ozone catalytic oxidation treatment device |
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