CN103864183A - Molecular oxygen activation-coupled water treatment method employing high-efficiency neutral electro-fenton oxidation - Google Patents
Molecular oxygen activation-coupled water treatment method employing high-efficiency neutral electro-fenton oxidation Download PDFInfo
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- CN103864183A CN103864183A CN201410107965.0A CN201410107965A CN103864183A CN 103864183 A CN103864183 A CN 103864183A CN 201410107965 A CN201410107965 A CN 201410107965A CN 103864183 A CN103864183 A CN 103864183A
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Abstract
The invention provides a molecular oxygen activation-coupled water treatment method employing high-efficiency neutral electro-fenton oxidation. The method comprises the following steps: in a to-be-processed wastewater system of which the pH is adjusted to 5-9 in advance, taking a substance containing zero-valent iron as an anode, a porous carbon electrode as a cathode and polyphosphate as supporting electrolyte to form an electro-fenton system; electrifying, and simultaneously providing air or oxygen to the cathode lastingly; and carrying out electro-fenton oxidation treatment on the to-be-processed wastewater. By adopting the electrolyte polyphosphate used by the method, not only can the removal rate of organic pollutants in the wastewater and the actual chemical oxygen demand (COD) removal rate of the wastewater be greatly improved, but also a lot of iron cement generated by iron ion hydrolysis can be avoided, and the subsequence treatment process is simplified. Thus, the molecular oxygen activation-coupled water treatment method is applicable to treatment of various organic wastewater.
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 processing of the organic wastewater with difficult degradation thereby such as printing and dyeing, chemical industry, agriculture field.
Background technology
1894, french chemist Fenton found under acidic conditions first, Fe
2+and H
2o
2mixing solutions (Fenton reagent) can the efficient oxidation tartrate.Fenton reagent is mainly used in research and the application of enzyme reaction, organic synthesis and cell injury mechanism at first.Within 1964, Canadian scientist Eisenhaner is applied to Fenton reagent in wastewater treatment first.Research shows, Fenton reagent energy the efficient oxidation is removed the Persistent organic pollutants that traditional wastewater processing technology cannot be removed.Fenton reagent both can be used as the pre-treatment of waste water, also can be used as final advanced treatment, had a wide range of applications.But therefore traditional Fenton reagent exists shortcomings such as hydrogen peroxide utilization ratio is low, processing cost is high, oxidation operation is not thorough arise at the historic moment the method for Fenton reagent and other technologies combination treatment waste water.Mainly containing of research at present: ultrasonic Fenton process, light Fenton process, electro-fenton process, photoelectricity Fenton process etc.Wherein electro-fenton process is because the advantages such as processing efficiency is high, treatment cycle is short, equipment is simple, mild condition are widely studied, and in the processing of the pollutents such as organic chloride and benzene class, has been proved feasiblely, and obtains good result.
The essence of electro-fenton process is the Fe producing with electrochemical process
2+and (or) H
2o
2as the lasting 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 cathodic electricity Fenton process, sacrificial anode protection, bipolar electric Fenton process etc.Bipolar electric Fenton process is without outer adding medicine, Fe
2+and H
2o
2can produce by electrode reaction.Wherein Fe
2+can be produced by Fe H in anodic oxidation
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 forms.In reaction process, pass to air at negative electrode.The current efficiency generating in order to improve negative electrode hydrogen peroxide, the Fe that simultaneously avoids anode to produce
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, in reaction process, need acid adding to regulate, acid adding has not only increased 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 efficient neutral electricity Fenton oxidation water treatment method that a kind of coupled molecule oxygen activation is provided for the deficiency of above-mentioned prior art existence, it uses polyphosphoric acid salt as supporting electrolyte, within the scope of wider pH, all can significantly improve clearance, the COD clearance of Organic Pollutants in Wastewater, can also avoid iron ion hydrolysis to produce a large amount of iron mud simultaneously.
The present invention for the technical scheme that the problem of the above-mentioned proposition of solution adopts is:
A kind of efficient neutral electricity Fenton oxidation water treatment method of coupled molecule oxygen activation, in the pending waste water system that it is is 5-9 in pH preconditioning, take the material containing fe as anode, porous carbon electrodes is negative electrode, polyphosphoric acid salt is supporting electrolyte, forms electric Fenton system, then energising, continue to provide air or oxygen to negative electrode place, pending waste water is carried out to electric Fenton oxidation processing simultaneously.
Press such scheme, the reagent of described preconditioning pH is conventional acid or alkali, and described acid can be selected the mineral acids such as hydrochloric acid, sulfuric acid, acetic acid, and described alkali can be selected the mineral alkali such as sodium hydroxide, potassium hydroxide.
Press such scheme, the concentration of described polyphosphoric acid salt in waste water system is 0.1～1 mM/l.
Press such scheme, the described material containing fe can be the iron compounds such as iron wire, iron plate, stainless steel substrates, stainless (steel) wire.
Press such scheme, described porous carbon electrodes can be the porous carbon electrodes such as activated carbon fiber, charcoal felt.
Press 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.
Press such scheme, described electric Fenton oxidation treating processes is carried out under constant current conditions, and range of current control is 0.3-1.0 milliampere.
Press such scheme, the control of described electric Fenton oxidation treating processes Anodic current density be 2-10 peace/square metre.
Press such scheme, described negative electrode place air or oxygen flow velocity is 40～100 ml/min.
Know-why of the present invention: when 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 be 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 by series reaction with dissolved oxygen, 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 water in organic pollutant reaction, organic pollutant in degrading waste water, forms corresponding oxidation products, and oxidation products is again through further generating carbonic acid gas and water and inorganic salt 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 can not only significantly to improve the clearance of Organic Pollutants in Wastewater and the COD clearance of waste water, separately compared with traditional ionogen sodium sulfate, use polyphosphoric acid salt can also within the scope of wider pH, obtain good wastewater treatment efficiency as supporting electrolyte, be applicable to the processing of various organic waste waters;
2. polyphosphoric acid salt is more stable, is difficult for decomposing, and therefore compares other organic ligands more lasting to the facilitation effect of electric Fenton processing organic waste water;
3. the method for the invention can be avoided, because iron ion is hydrolyzed a large amount of iron mud that produce, having simplified subsequent processes;
4. polyphosphoric acid salt is often used as foodstuff additive, belongs to environmentally friendly additive, nontoxic to human body.
Accompanying drawing explanation
Fig. 1 is that to adopt sodium tetrapolyphosphate be that to adopt sodium sulfate be that supporting electrolyte is administered rhodamine B effect contrast figure in sewage for supporting electrolyte and comparative example to embodiment 1;
Fig. 2 is that to adopt tripoly phosphate sodium STPP be that supporting electrolyte is administered G-30027 design sketch in sewage to embodiment 2;
Fig. 3 is that to adopt sodium tetrapolyphosphate be G-30027 design sketch during supporting electrolyte is administered polluted water under different initial pH value conditions to embodiment 3;
Fig. 4 is that to adopt sodium tetrapolyphosphate be that supporting electrolyte is administered the waste water design sketch of soaping to embodiment 4.
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.
The sewage that embodiment 1 administers containing dyestuff rhodamine B
For the electric Fenton reparation at dye discoloration water source, it is the efficient neutral electricity Fenton processing experiment that experimental subjects is carried out coupled molecule oxygen activation that this example adopts the rhodamine B aqueous solution of preparation voluntarily.
The rhodamine B aqueous solution take concentration as 10mg/L is made simulated wastewater, and the pH value of the rhodamine B aqueous solution is for 6.6(is without adding acid-alkali accommodation pH).Get simulated wastewater 25mL, adding wherein sodium tetrapolyphosphate to make its concentration is 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, and simulated wastewater is carried out to electric Fenton oxidation processing.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 degradation rate reaches 89%.
Comparative example: adopting sodium sulfate is that the tripoly phosphate sodium STPP that supporting electrolyte substitutes in above-mentioned experiment carries out electric Fenton oxidation processing, and 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%.
The sewage that embodiment 2 administers containing atrazine
For the electric Fenton reparation at pesticidal contamination water source, it is the efficient neutral electricity Fenton improvement experiment that experimental subjects is carried out coupled molecule oxygen activation that this example adopts the G-30027 aqueous solution of preparation voluntarily.
The G-30027 aqueous solution take concentration as 15mg/L is simulated wastewater, and the pH value of G-30027 aqueous solution solution is for 6.8(is without adding acid-alkali accommodation pH).Get simulated wastewater 25mL, adding wherein tripoly phosphate sodium STPP to make its concentration is 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, and simulated wastewater is carried out to electric Fenton oxidation processing.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 3 administers the sewage containing atrazine under different pH condition
It is the efficient neutral electricity Fenton improvement experiment that experimental subjects is carried out coupled molecule oxygen activation that this example adopts the G-30027 aqueous solution of preparation voluntarily.
The G-30027 aqueous solution take concentration as 15mg/L is simulated wastewater, and the concentration that adds wherein sodium tetrapolyphosphate is 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.The simulated wastewater 25mL that gets respectively different initial pH, 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, and simulated wastewater is carried out to electric Fenton oxidation processing.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 4 administers printing and dyeing mill's waste water of soaping
It is that the efficient neutral electricity Fenton that experimental subjects is carried out coupled molecule oxygen activation is administered experiment that this example adopts printing and dyeing mill's waste water of soaping.
Printing and dyeing mill soap waste water pH value for 8.5(without adding acid-alkali accommodation pH), initial COD is 450mg/L, adding wherein sodium tetrapolyphosphate to make its concentration is 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, and waste water is carried out to electric Fenton oxidation processing.As shown in Figure 4, after electric Fenton oxidation processing reaction 1h, the COD of waste water is 95mg/L, and printing and dyeing mill's waste water COD clearance of soaping is 79%.
Claims (9)
1. the efficient neutral of coupled molecule oxygen activation electricity Fenton oxidation water treatment method, it is characterized in that: in the pending waste water system that it is is 5-9 in pH preconditioning, take the material containing fe as anode, porous carbon electrodes is negative electrode, polyphosphoric acid salt is supporting electrolyte, forms electric Fenton system, then energising, continue to provide air or oxygen to negative electrode place, pending waste water is carried out to electric Fenton oxidation processing simultaneously.
2. the efficient neutral of a kind of coupled molecule oxygen activation according to claim 1 electricity Fenton oxidation water treatment method, is characterized in that: the concentration of described polyphosphoric acid salt in waste water system is 0.1～1 mM/l.
3. the efficient neutral of a kind of coupled molecule oxygen activation according to claim 1 electricity Fenton oxidation water treatment method, is characterized in that: the described material containing fe is the one in iron wire, iron plate, stainless steel substrates, stainless (steel) wire.
4. the efficient neutral of a kind of coupled molecule oxygen activation according to claim 1 electricity Fenton oxidation water treatment method, is characterized in that: described porous carbon electrodes is the one in activated carbon fiber, charcoal felt.
5. the efficient neutral of a kind of coupled molecule oxygen activation according to claim 1 electricity Fenton oxidation water treatment method, is characterized in that: described polyphosphoric acid salt is a kind of in four poly-phosphate or tri-polyphosphate.
6. the efficient neutral of a kind of coupled molecule oxygen activation according to claim 5 electricity Fenton oxidation water treatment method, 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.
7. the efficient neutral of a kind of coupled molecule oxygen activation according to claim 1 electricity Fenton oxidation water treatment method, is characterized in that: described electric Fenton oxidation treating processes is carried out under constant current conditions, and range of current control is 0.3-1.0 milliampere.
8. the efficient neutral of a kind of coupled molecule oxygen activation according to claim 7 electricity Fenton oxidation water treatment method, is characterized in that: the control of described electric Fenton oxidation treating processes Anodic current density be 2-10 peace/square metre.
9. the efficient neutral of a kind of coupled molecule oxygen activation according to claim 1 electricity Fenton oxidation water treatment method, is characterized in that: described negative electrode place air or oxygen flow velocity is 30～100 ml/min.
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Cited By (10)
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| CN104478073A (en) * | 2014-12-10 | 2015-04-01 | 广西师范大学 | Device for treating industrial wastewater difficult to biodegrade by virtue of ABR-bioelectric Fenton coupling technique |
| CN104692567A (en) * | 2015-03-09 | 2015-06-10 | 中国海洋石油总公司 | Degradation-resistant organic wastewater depth treatment system based on photoelectrocatalysis and treatment 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 |
| CN113023839A (en) * | 2021-04-28 | 2021-06-25 | 辽宁科技学院 | Micro-electrolysis Fenton oxidation water treatment method activated by polyphosphate |
| 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 |
| CN114956299A (en) * | 2022-07-04 | 2022-08-30 | 吉林大学 | Method for regulating and controlling oxidation/reduction degradation of pollutants by ferrous/polyphosphate system |
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Cited By (10)
| Publication number | Priority date | Publication date | Assignee | Title |
|---|---|---|---|---|
| CN104478073A (en) * | 2014-12-10 | 2015-04-01 | 广西师范大学 | Device for treating industrial wastewater difficult to biodegrade by virtue of ABR-bioelectric Fenton coupling technique |
| CN104692567A (en) * | 2015-03-09 | 2015-06-10 | 中国海洋石油总公司 | Degradation-resistant organic wastewater depth treatment system based on photoelectrocatalysis and treatment 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 |
| CN114956299A (en) * | 2022-07-04 | 2022-08-30 | 吉林大学 | Method for regulating and controlling oxidation/reduction degradation of pollutants by ferrous/polyphosphate system |
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