CN103864183B - A kind of neutrality electricity Fenton oxidation water treatment method of coupled molecule oxygen activation - Google Patents
A kind of neutrality electricity Fenton oxidation water treatment method of coupled molecule oxygen activation Download PDFInfo
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- CN103864183B CN103864183B CN201410107965.0A CN201410107965A CN103864183B CN 103864183 B CN103864183 B CN 103864183B CN 201410107965 A CN201410107965 A CN 201410107965A CN 103864183 B CN103864183 B CN 103864183B
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Abstract
The invention provides a kind of efficient neutral electricity Fenton oxidation water treatment method of coupled molecule oxygen activation, it is in the pending waste water system of 5-9 in pH preconditioning, with the material containing fe for anode, porous carbon electrodes is negative electrode, polyphosphoric acid salt is supporting electrolyte, forms electric Fenton-like system, is then energized, continue to provide air or oxygen to negative electrode place simultaneously, electric Fenton oxidation process is carried out to pending waste water.Ionogen polyphosphoric acid salt used in the present invention significantly can not only improve the clearance of Organic Pollutants in Wastewater, the COD clearance of actual waste water, can also avoid a large amount of iron mud produced due to iron ion hydrolysis simultaneously, simplify subsequent processes.The present invention is applicable to the process of various organic waste water.
Description
Technical field
The invention belongs to technical field of water pollution control, be specifically related to a kind of efficient neutral electricity Fenton oxidation water treatment method of coupled molecule oxygen activation, be applicable to the process of the organic wastewater with difficult degradation thereby such as printing and dyeing, chemical industry, agriculture field.
Background technology
1894, under french chemist Fenton Late Cambrian acidic conditions, Fe
2+and H
2o
2mixing solutions (Fenton reagent) can the efficient oxidation tartrate.Fenton reagent is mainly used in the investigation and application of enzyme reaction, organic synthesis and cell injury mechanism at first.Within 1964, Fenton reagent is applied in wastewater treatment by Canadian scientist Eisenhaner first.Research shows, Fenton reagent energy the efficient oxidation removes the Persistent organic pollutants that conventional waste water treatment technology cannot be removed.Fenton reagent both as the pre-treatment of waste water, also as final advanced treatment, can have a wide range of applications.But traditional Fenton reagent exists shortcomings such as hydrogen peroxide utilization ratio is low, processing cost is high, oxidation operation is not thorough, therefore the method for Fenton reagent and other technologies combination treatment waste water is arisen at the historic moment.Mainly containing of current research: ultrasonic Fenton process, light Fenton process, electro-fenton process, photoelectricity Fenton process etc.Wherein electro-fenton process is widely studied due to advantages such as processing efficiency is high, treatment cycle is short, equipment is simple, mild conditions, has been proved feasible in the process of the pollutents such as organic chloride and benzene class, and has obtained good result.
The essence of electro-fenton process is the Fe produced with electrochemical process
2+and (or) H
2o
2as the constant source of Fenton reagent, degradation of contaminant.According to Fe
2+and H
2o
2the difference of producing method, electro-fenton process can be divided into cathode electro-Fenton method, sacrificial anode protection, bipolar electric Fenton process etc.Bipolar electric Fenton process without the need to outer adding medicine, Fe
2+and H
2o
2can be produced by electrode reaction.Wherein Fe
2+can be produced in anodic oxidation by Fe, H
2o
2by O
2produce in cathodic reduction.The device of the method is anode mainly with dull and stereotyped iron or iron net, and porous carbon electrodes is negative electrode, and sodium sulfate is that supporting electrolyte is formed.Air is passed at negative electrode in reaction process.In order to improve the current efficiency that negative electrode hydrogen peroxide generates, avoid the Fe that anode produces simultaneously
2+be oxidized to Fe (OH)
3precipitation, the pH value of solution generally should not be greater than 3.5.In order to maintain lower pH value requirement, need acid adding to regulate in reaction process, acid adding not only increases the processing cost of waste water, is unfavorable for discharge of wastewater, simultaneously also can etching apparatus.
Summary of the invention
Technical problem to be solved by this invention is the deficiency that exists for above-mentioned prior art and provides a kind of efficient neutral electricity Fenton oxidation water treatment method of coupled molecule oxygen activation, it uses polyphosphoric acid salt as supporting electrolyte, within the scope of wider pH, all significantly can improve clearance, the COD clearance of Organic Pollutants in Wastewater, iron ion can also be avoided simultaneously to be hydrolyzed and produce a large amount of iron mud.
The technical scheme that the problem that the present invention is the above-mentioned proposition of solution adopts is:
A kind of efficient neutral electricity Fenton oxidation water treatment method of coupled molecule oxygen activation, it is in the pending waste water system of 5-9 in pH preconditioning, with the material containing fe for anode, porous carbon electrodes is negative electrode, polyphosphoric acid salt is supporting electrolyte, forms electric Fenton-like system, is then energized, continue to provide air or oxygen to negative electrode place simultaneously, electric Fenton oxidation process is carried out to pending waste water.
By such scheme, the reagent of described preconditioning pH is conventional acid or alkali, and described acid can select the mineral acids such as hydrochloric acid, sulfuric acid, acetic acid, and described alkali can select the mineral alkali such as sodium hydroxide, potassium hydroxide.
By such scheme, the concentration of described polyphosphoric acid salt in waste water system is 0.1 ~ 1 mM/l.
By such scheme, the described material containing fe can be the iron compounds such as iron wire, iron plate, stainless steel substrates, stainless (steel) wire.
By such scheme, described porous carbon electrodes can be the porous carbon electrodes such as activated carbon fiber, charcoal felt.
By such scheme, described polyphosphoric acid salt is four poly-phosphate or tri-polyphosphate, and four described poly-phosphate are selected from sodium tetrapolyphosphate, four Rapisols, four ammonium polyphosphates etc.; Described tri-polyphosphate is selected from tripoly phosphate sodium STPP, Potassium tripolyphosphate, tripolyphosphate ammonium etc.
By such scheme, described electric Fenton oxidation treating processes is carried out under constant current conditions, and range of current controls as 0.3-1.0 milliampere.
By such scheme, described electric Fenton oxidation treating processes Anodic current density control for 2-10 pacify/square metre.
By such scheme, described negative electrode place air or oxygen flow velocity is 40 ~ 100 ml/min.
Know-why of the present invention: during energising, oxygen passes through 2e at negative electrode
-reduction produces hydrogen peroxide, and fe generates ferrous ion in anodic oxidation.Ferrous ion and ionogen polyphosphoric acid salt generation coordination reaction form Fe
2+l title complex (L represents polyphosphoric acid salt), this title complex both can directly and the hydrogen peroxide generation Fenton's reaction that produces of negative electrode produce hydroxyl radical free radical, also can produce hydroxyl radical free radical with dissolved oxygen by series reaction, concrete reaction formula is as follows:
Anodic reaction: Fe-2e
-=Fe
2+
Cathodic reaction: O
2+ 2H
++ 2e
-=H
2o
2
Reaction Fe in solution
2++ L=Fe
2+l(L represents polyphosphoric acid salt)
O
2+Fe
2+L=·O
2 -+Fe
3+L
·O
2 -+Fe
2+L+2H
+=H
2O
2+Fe
3+L
Fe
2+L+H
2O
2=Fe
3+L+OH
-+·OH
The hydroxyl radical free radical that above-mentioned reaction produces has very high oxidation activity, can with the organic pollutant reaction in water, organic pollutant in degrading waste water, forms corresponding oxidation products, and oxidation products is again through generating carbonic acid gas and water and inorganic salt further with hydroxyl radical reaction.
Compared with prior art, the invention has the beneficial effects as follows:
1. the present invention uses polyphosphoric acid salt to make supporting electrolyte significantly can not only to improve the clearance of Organic Pollutants in Wastewater and the COD clearance of waste water, another compared with traditional electrolyte matter sodium sulfate, use polyphosphoric acid salt can also obtain good wastewater treatment efficiency within the scope of wider pH as supporting electrolyte, be applicable to the process of various organic waste water;
2. polyphosphoric acid salt is more stable, not easily decomposes, and therefore compares the facilitation effect of other organic ligands to electric Fenton process organic waste water more lasting;
3. the method for the invention can be avoided due to iron ion hydrolysis and a large amount of iron mud of generation, simplifies subsequent processes;
4. polyphosphoric acid salt is often used as foodstuff additive, belongs to environmentally friendly additive, to human non-toxic.
Accompanying drawing explanation
Fig. 1 is that embodiment 1 adopts sodium tetrapolyphosphate to be that supporting electrolyte and comparative example adopt sodium sulfate to be that supporting electrolyte administers rhodamine B effect contrast figure in sewage;
Fig. 2 is that embodiment 2 adopts tripoly phosphate sodium STPP to be that supporting electrolyte administers G-30027 design sketch in sewage;
Fig. 3 is that embodiment 3 adopts sodium tetrapolyphosphate to be supporting electrolyte G-30027 design sketch in pollution administration water under different initial pH value condition;
Fig. 4 is that embodiment 4 adopts sodium tetrapolyphosphate to be that supporting electrolyte administers waste water design sketch of soaping.
Embodiment
Describe summary of the invention of the present invention in detail below by specific embodiment, described specific embodiment only in order to explain the present invention, is not intended to limit the present invention.
embodiment 1administer the sewage containing dye, rhodamine B
For the electric Fenton reparation at dye discoloration water source, this example adopts the rhodamine B aqueous solution prepared voluntarily to be the efficient neutral electricity Fenton process experiment that experimental subjects carries out coupled molecule oxygen activation.
Be that the rhodamine B aqueous solution of 10mg/L makes simulated wastewater with concentration, the pH value of the rhodamine B aqueous solution is that 6.6(is without the need to adding acid-alkali accommodation pH).Get simulated wastewater 25mL, add sodium tetrapolyphosphate wherein and make its concentration be 0.3mmol/L.Take iron wire as anode, activated carbon fiber is negative electrode, continuous current 0.6mA, anodic current density be 6 peaces/square metre, blast air by aerating apparatus at negative electrode, air-flow velocity is 40mL/min, carries out electric Fenton oxidation process to simulated wastewater.As shown in Figure 1, after electric Fenton oxidation processing reaction 1h, in waste water, the percent of decolourization of rhodamine B reaches 89%, and namely degradation rate reaches 89%.
Comparative example: adopt sodium sulfate to be that the supporting electrolyte tripoly phosphate sodium STPP come in alternative above-mentioned experiment carries out electric Fenton oxidation process, other experiment conditions are all identical with above-mentioned experiment condition.The results are shown in Figure 1, as shown in Figure 1: the percent of decolourization of its rhodamine B only can reach 20%.
embodiment 2administer the sewage containing atrazine
For the electric Fenton reparation at pesticidal contamination water source, this example adopts the G-30027 aqueous solution prepared voluntarily to be the efficient neutral electricity Fenton improvement experiment that experimental subjects carries out coupled molecule oxygen activation.
Take concentration as the G-30027 aqueous solution of 15mg/L be simulated wastewater, the pH value of G-30027 aqueous solution is that 6.8(is without the need to adding acid-alkali accommodation pH).Get simulated wastewater 25mL, add tripoly phosphate sodium STPP wherein and make its concentration be 0.5mmol/L.Take iron wire as anode, activated carbon fiber is negative electrode, continuous current 0.5mA, anodic current density be 5 peaces/square metre, blast air by aerating apparatus at negative electrode, gas velocity is 60mL/min, carries out electric Fenton oxidation process to simulated wastewater.As shown in Figure 2, after electric Fenton oxidation processing reaction 1h, in water, the degradation rate of G-30027 reaches more than 97%.
embodiment 3the sewage containing atrazine is administered under different pH condition
This example adopts the G-30027 aqueous solution prepared voluntarily to be the efficient neutral electricity Fenton improvement experiment that experimental subjects carries out coupled molecule oxygen activation.
Take concentration as the G-30027 aqueous solution of 15mg/L be simulated wastewater, the concentration adding sodium tetrapolyphosphate is wherein 0.5mmol/L, is respectively 5.3,6.3,7.3,8.3,9.3 with the initial pH of NaOH or HCl solution regulator solution.Get the simulated wastewater 25mL of different initial pH respectively, take iron wire as anode, activated carbon fiber is negative electrode, continuous current 0.5mA, anodic current density be 5 peaces/square metre, blast air by aerating apparatus at negative electrode, gas velocity is 60mL/min, carries out electric Fenton oxidation process to simulated wastewater.As shown in Figure 3, after electric Fenton oxidation processing reaction 1h, under different pH condition, in water, the degradation rate of G-30027 all reaches more than 80%.
embodiment 4administer printing and dyeing mill to soap waste water
This example adopt printing and dyeing mill soap waste water be experimental subjects carry out coupled molecule oxygen activation efficient neutral electricity Fenton administer experiment.
The soap pH value of waste water of printing and dyeing mill is that 8.5(is without the need to adding acid-alkali accommodation pH), initial COD is 450mg/L, adding sodium tetrapolyphosphate wherein makes its concentration be 1mmol/L, then samples 100mL, take iron wire as anode, activated carbon fiber is negative electrode, continuous current 1.0mA, anodic current density be 10 peaces/square metre, blast air by aerating apparatus at negative electrode, gas velocity is 100mL/min, carries out electric Fenton oxidation process to waste water.As shown in Figure 4, after electric Fenton oxidation processing reaction 1h, the COD of waste water is 95mg/L, and namely printing and dyeing mill's waste water COD clearance of soaping is 79%.
Claims (7)
1. the neutrality electricity Fenton oxidation water treatment method of a coupled molecule oxygen activation, it is characterized in that: it is in the pending waste water system of 5-9 in pH preconditioning, with the material containing fe for anode, porous carbon electrodes is negative electrode, polyphosphoric acid salt is supporting electrolyte, forms electric Fenton-like system, is then energized, continue to provide air or oxygen to negative electrode place simultaneously, electric Fenton oxidation process is carried out to pending waste water; The concentration of described polyphosphoric acid salt in waste water system is 0.1 ~ 1 mM/l, and described electric Fenton oxidation treating processes is carried out under constant current conditions, and range of current controls as 0.3-1.0 milliampere.
2. the neutrality electricity Fenton oxidation water treatment method of a kind of coupled molecule oxygen activation according to claim 1, is characterized in that: the described material containing fe is the one in iron wire, iron plate, stainless steel substrates, stainless (steel) wire.
3. the neutrality electricity Fenton oxidation water treatment method of a kind of coupled molecule oxygen activation according to claim 1, is characterized in that: described porous carbon electrodes is the one in activated carbon fiber, charcoal felt.
4. the neutrality electricity Fenton oxidation water treatment method of a kind of coupled molecule oxygen activation according to claim 1, is characterized in that: described polyphosphoric acid salt is a kind of in four poly-phosphate or tri-polyphosphate.
5. the neutrality electricity Fenton oxidation water treatment method of a kind of coupled molecule oxygen activation according to claim 4, is characterized in that: four described poly-phosphate are selected from sodium tetrapolyphosphate, four Rapisols, four ammonium polyphosphates; Described tri-polyphosphate is selected from tripoly phosphate sodium STPP, Potassium tripolyphosphate, tripolyphosphate ammonium.
6. the neutrality electricity Fenton oxidation water treatment method of a kind of coupled molecule oxygen activation according to claim 1, is characterized in that: described electric Fenton oxidation treating processes Anodic current density control for 2-10 pacify/square metre.
7. the neutrality electricity Fenton oxidation water treatment method of a kind of coupled molecule oxygen activation according to claim 1, is characterized in that: described negative electrode place air or oxygen flow velocity is 30 ~ 100 ml/min.
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| CN104478073B (en) * | 2014-12-10 | 2016-07-06 | 广西师范大学 | A kind of device utilizing ABR-bio electricity Fenton coupling technique to process difficult for biological degradation industrial wastewater |
| CN104692567B (en) * | 2015-03-09 | 2016-09-14 | 中国海洋石油总公司 | Organic wastewater with difficult degradation thereby advanced treatment system based on photoelectrocatalysis and processing method |
| CN105692971A (en) * | 2016-03-18 | 2016-06-22 | 沈阳飞机工业（集团）有限公司 | Method for treating aluminum alloy chemical milling cleaning liquid through electro-Fenton oxidization |
| CN105753111A (en) * | 2016-04-05 | 2016-07-13 | 南开大学 | Method for treating organic wastewater by efficient peroxide flocculation technology |
| CN106517443A (en) * | 2016-11-23 | 2017-03-22 | 西安工业大学 | Novel electro-Fenton system |
| CN107879429A (en) * | 2017-11-09 | 2018-04-06 | 中国恩菲工程技术有限公司 | Electric Fenton device |
| CN110182934A (en) * | 2019-06-03 | 2019-08-30 | 东莞理工学院 | The method and application of nano zero-valence aluminium activate molecular oxygen are utilized under a kind of alkaline condition |
| CN113087208A (en) * | 2021-02-03 | 2021-07-09 | 南京水滴智能环保装备研究院有限公司 | Method for degrading copper ore wastewater by using synergistic catalytic oxidation system |
| CN113023839A (en) * | 2021-04-28 | 2021-06-25 | 辽宁科技学院 | Micro-electrolysis Fenton oxidation water treatment method activated by polyphosphate |
| CN114956299B (en) * | 2022-07-04 | 2023-07-14 | 吉林大学 | Method for regulating and controlling oxidation/reduction degradation pollutant of ferrous/polyphosphate system |
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