CN102593469B - Method for accelerating reduction decolorization of azo dyes wastewater at microbial fuel cell cathode - Google Patents
Method for accelerating reduction decolorization of azo dyes wastewater at microbial fuel cell cathode Download PDFInfo
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- CN102593469B CN102593469B CN201210041468.6A CN201210041468A CN102593469B CN 102593469 B CN102593469 B CN 102593469B CN 201210041468 A CN201210041468 A CN 201210041468A CN 102593469 B CN102593469 B CN 102593469B
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- polypyrrole
- anthraquinone
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- carbon felt
- sodium disulfonate
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- 239000000446 fuel Substances 0.000 title claims abstract description 42
- 239000000987 azo dye Substances 0.000 title claims abstract description 30
- 238000000034 method Methods 0.000 title claims abstract description 21
- 230000000813 microbial effect Effects 0.000 title claims abstract description 20
- 230000009467 reduction Effects 0.000 title claims abstract description 17
- 239000002351 wastewater Substances 0.000 title claims abstract description 15
- 238000004042 decolorization Methods 0.000 title claims abstract description 8
- 229920000128 polypyrrole Polymers 0.000 claims abstract description 73
- 229910052708 sodium Inorganic materials 0.000 claims abstract description 67
- 239000011734 sodium Substances 0.000 claims abstract description 67
- OKTJSMMVPCPJKN-UHFFFAOYSA-N Carbon Chemical compound [C] OKTJSMMVPCPJKN-UHFFFAOYSA-N 0.000 claims abstract description 63
- 229910052799 carbon Inorganic materials 0.000 claims abstract description 63
- 238000006243 chemical reaction Methods 0.000 claims abstract description 8
- 239000000758 substrate Substances 0.000 claims abstract description 8
- 230000002906 microbiologic effect Effects 0.000 claims description 26
- 239000012528 membrane Substances 0.000 claims description 10
- 238000005868 electrolysis reaction Methods 0.000 claims description 8
- 238000006116 polymerization reaction Methods 0.000 claims description 5
- 230000005540 biological transmission Effects 0.000 claims description 3
- 239000007788 liquid Substances 0.000 claims description 2
- 238000002156 mixing Methods 0.000 claims description 2
- DGAQECJNVWCQMB-PUAWFVPOSA-M Ilexoside XXIX Chemical compound C[C@@H]1CC[C@@]2(CC[C@@]3(C(=CC[C@H]4[C@]3(CC[C@@H]5[C@@]4(CC[C@@H](C5(C)C)OS(=O)(=O)[O-])C)C)[C@@H]2[C@]1(C)O)C)C(=O)O[C@H]6[C@@H]([C@H]([C@@H]([C@H](O6)CO)O)O)O.[Na+] DGAQECJNVWCQMB-PUAWFVPOSA-M 0.000 abstract 1
- 238000002845 discoloration Methods 0.000 abstract 1
- 239000011259 mixed solution Substances 0.000 abstract 1
- 230000027756 respiratory electron transport chain Effects 0.000 abstract 1
- 238000006722 reduction reaction Methods 0.000 description 14
- STZCRXQWRGQSJD-GEEYTBSJSA-M methyl orange Chemical compound [Na+].C1=CC(N(C)C)=CC=C1\N=N\C1=CC=C(S([O-])(=O)=O)C=C1 STZCRXQWRGQSJD-GEEYTBSJSA-M 0.000 description 10
- 229940012189 methyl orange Drugs 0.000 description 10
- 239000000463 material Substances 0.000 description 7
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- 230000000052 comparative effect Effects 0.000 description 5
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- 239000000243 solution Substances 0.000 description 5
- 238000005516 engineering process Methods 0.000 description 4
- BASFCYQUMIYNBI-UHFFFAOYSA-N platinum Chemical compound [Pt] BASFCYQUMIYNBI-UHFFFAOYSA-N 0.000 description 4
- RTAQQCXQSZGOHL-UHFFFAOYSA-N Titanium Chemical compound [Ti] RTAQQCXQSZGOHL-UHFFFAOYSA-N 0.000 description 3
- 230000007547 defect Effects 0.000 description 3
- 239000000975 dye Substances 0.000 description 3
- 239000003344 environmental pollutant Substances 0.000 description 3
- 231100000719 pollutant Toxicity 0.000 description 3
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- 229910052719 titanium Inorganic materials 0.000 description 3
- 239000010936 titanium Substances 0.000 description 3
- XLYOFNOQVPJJNP-UHFFFAOYSA-N water Substances O XLYOFNOQVPJJNP-UHFFFAOYSA-N 0.000 description 3
- QGZKDVFQNNGYKY-UHFFFAOYSA-N Ammonia Chemical compound N QGZKDVFQNNGYKY-UHFFFAOYSA-N 0.000 description 2
- IJGRMHOSHXDMSA-UHFFFAOYSA-N Atomic nitrogen Chemical compound N#N IJGRMHOSHXDMSA-UHFFFAOYSA-N 0.000 description 2
- BZORFPDSXLZWJF-UHFFFAOYSA-N N,N-dimethyl-1,4-phenylenediamine Chemical compound CN(C)C1=CC=C(N)C=C1 BZORFPDSXLZWJF-UHFFFAOYSA-N 0.000 description 2
- 150000001412 amines Chemical class 0.000 description 2
- 230000015572 biosynthetic process Effects 0.000 description 2
- 230000007613 environmental effect Effects 0.000 description 2
- 238000011049 filling Methods 0.000 description 2
- 125000002496 methyl group Chemical group [H]C([H])([H])* 0.000 description 2
- 239000008055 phosphate buffer solution Substances 0.000 description 2
- 229910052697 platinum Inorganic materials 0.000 description 2
- 229920001296 polysiloxane Polymers 0.000 description 2
- 238000002360 preparation method Methods 0.000 description 2
- STZCRXQWRGQSJD-UHFFFAOYSA-M sodium;4-[[4-(dimethylamino)phenyl]diazenyl]benzenesulfonate Chemical compound [Na+].C1=CC(N(C)C)=CC=C1N=NC1=CC=C(S([O-])(=O)=O)C=C1 STZCRXQWRGQSJD-UHFFFAOYSA-M 0.000 description 2
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- WQZGKKKJIJFFOK-GASJEMHNSA-N Glucose Natural products OC[C@H]1OC(O)[C@H](O)[C@@H](O)[C@@H]1O WQZGKKKJIJFFOK-GASJEMHNSA-N 0.000 description 1
- PEDCQBHIVMGVHV-UHFFFAOYSA-N Glycerine Chemical compound OCC(O)CO PEDCQBHIVMGVHV-UHFFFAOYSA-N 0.000 description 1
- CBENFWSGALASAD-UHFFFAOYSA-N Ozone Chemical compound [O-][O+]=O CBENFWSGALASAD-UHFFFAOYSA-N 0.000 description 1
- 208000031320 Teratogenesis Diseases 0.000 description 1
- 239000003513 alkali Substances 0.000 description 1
- 229910021529 ammonia Inorganic materials 0.000 description 1
- 230000003321 amplification Effects 0.000 description 1
- 230000001458 anti-acid effect Effects 0.000 description 1
- 230000000845 anti-microbial effect Effects 0.000 description 1
- QVGXLLKOCUKJST-UHFFFAOYSA-N atomic oxygen Chemical compound [O] QVGXLLKOCUKJST-UHFFFAOYSA-N 0.000 description 1
- 230000009286 beneficial effect Effects 0.000 description 1
- 238000007664 blowing Methods 0.000 description 1
- 230000000711 cancerogenic effect Effects 0.000 description 1
- 231100000315 carcinogenic Toxicity 0.000 description 1
- 239000003054 catalyst Substances 0.000 description 1
- 238000005341 cation exchange Methods 0.000 description 1
- 230000008859 change Effects 0.000 description 1
- 230000007812 deficiency Effects 0.000 description 1
- 239000008367 deionised water Substances 0.000 description 1
- 229910021641 deionized water Inorganic materials 0.000 description 1
- ZOMNIUBKTOKEHS-UHFFFAOYSA-L dimercury dichloride Chemical class Cl[Hg][Hg]Cl ZOMNIUBKTOKEHS-UHFFFAOYSA-L 0.000 description 1
- 239000012153 distilled water Substances 0.000 description 1
- 238000004043 dyeing Methods 0.000 description 1
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Classifications
-
- Y—GENERAL TAGGING OF NEW TECHNOLOGICAL DEVELOPMENTS; GENERAL TAGGING OF CROSS-SECTIONAL TECHNOLOGIES SPANNING OVER SEVERAL SECTIONS OF THE IPC; TECHNICAL SUBJECTS COVERED BY FORMER USPC CROSS-REFERENCE ART COLLECTIONS [XRACs] AND DIGESTS
- Y02—TECHNOLOGIES OR APPLICATIONS FOR MITIGATION OR ADAPTATION AGAINST CLIMATE CHANGE
- Y02E—REDUCTION OF GREENHOUSE GAS [GHG] EMISSIONS, RELATED TO ENERGY GENERATION, TRANSMISSION OR DISTRIBUTION
- Y02E60/00—Enabling technologies; Technologies with a potential or indirect contribution to GHG emissions mitigation
- Y02E60/30—Hydrogen technology
- Y02E60/50—Fuel cells
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Abstract
The invention discloses a method for accelerating reduction decolorization of azo dyes wastewater at a microbial fuel cell cathode. The method comprises the following steps: adopting a carbon felt as a working electrode, adding a uniformly mixed solution of 100mL sodium anthraquinonc-2,6-disulfonate of concentration 0.029mol/L and 20mL polypyrrole of concentration 0.12mol/L into a working electrode chamber, forming a polypyrrole/anthraquinonc-2,6-disulfonate thin layer on the surface of the working electrode, preparing carbon felt/polypyrrole/anthraquinonc-2,6-disulfonate cathode and anode, inserting the cathode and the anode into a cathode chamber and an anode chamber and connecting with an external circuit. The oxidized substrate in the anode chamber generates electrons and protons, the electrons are transferred to the surface of the anode and then reach the cathode through the external circuit, the protons disperse to the cathode through a proton exchange film, the azo dyes, the protons and the electrons in the cathode chamber reach the electrons of the cathode and take reduction half-reaction on the surface of the cathode, and then the azo dyes are reduced and decolorized. The increase of the anode electron transfer rate greatly increases the reduction discoloration rate of the azo dyes wastewater, with no need of additional input power and no secondary pollution.
Description
Technical field
The present invention relates to a kind of method accelerating reduction decolorization of azo dyes wastewater at microbial fuel cell cathode, belong to technical field of sewage in environmental protection.
Background technology
Azo dyes is the azo-compound of Prof. Du Yucang, and its molecule principal character is containing one or more azo bond (-N=N-).Azo dye wastewater is mainly derived from DYE PRODUCTION and dyeing process, has the characteristics such as antiacid, alkali resistant, antimicrobial, long demurrage, and " three cause " of its precursor and catabolite thereof (carcinogenic, teratogenesis, mutagenesis) effect is very large to environmental hazard.At home and abroad in azo dye wastewater processing technology field, treatment effeciency is higher, non-secondary pollution, do not need the advantages such as additional electrical energy input to utilize microbiological fuel cell (MFC) cathodic reduction treatment technology to have.Microbiological fuel cell is a kind of electrogenesis device chemical energy being converted into electric energy, and azo dyes itself has higher oxidation-reduction potential, effectively can not be degraded under anodised condition.
For solving the problem, Yang Mu(
environ.Sci. Technol.2009,43,5137 – 5143) etc. propose the external power supply when microbiological fuel cell does not add electron mediator and participate in cathodic reduction reaction with degrade azo dyestuff, but its defect needs additionally to input electric energy.M.C.Costa(
bioresource Technology101. 2010,105 – 110) etc. propose microbiological fuel cell under anaerobic add catalyst anthraquinone-2,6-sodium disulfonate (AQDS) degrade azo dyestuff, but its defect be anthraquinone-2,6-sodium disulfonate easily with water outlet run off cause secondary pollution.Rong-Hua Liu{
appl Microbiol Biotechnol, 18 September 2010} etc. propose cathode surface plating anthraquinone-2, the 6-sodium disulfonate thin layer at microbiological fuel cell, but its defect is slower to methyl orange (MO) degradation rate.
Summary of the invention
The object of the invention is to for the deficiencies in the prior art, a kind of method accelerating reduction decolorization of azo dyes wastewater at microbial fuel cell cathode is provided, adopt carbon felt/polypyrrole/anthraquinone-2,6-sodium disulfonate yin, yang electrode, to increase the speed that anode current transmits, improve the speed of reduction decolorization of azo dyes wastewater at microbial fuel cell cathode.
The technical solution used in the present invention is: be substrate oxidized under microbial action in the anode chamber of microbiological fuel cell, it is azo dye wastewater in cathode chamber, first adopt three electrode diaphragm formula H type electrolysis tanks, using carbon felt as work electrode, the anthraquinone-2 that 100 mL concentration are 0.029 mol/L is added in work electrode indoor, 6-sodium disulfonate and 20mL concentration are the Homogeneous phase mixing liquid of the polypyrrole of 0.12 mol/L, are 1.83 ~ 1.86 mA/cm in current density
2, temperature is 10.0 ~ 10.2 DEG C, polymerization time is form one deck polypyrrole/anthraquinone-2 at working electrode surface under the condition of 3600 ~ 3800s, 6-sodium disulfonate thin layer, obtained carbon felt/polypyrrole/anthraquinone-2,6-sodium disulfonate anode and carbon felt/polypyrrole/anthraquinone-2,6-sodium disulfonate negative electrode; Again by carbon felt/polypyrrole/anthraquinone-2,6-sodium disulfonate anode and carbon felt/polypyrrole/anthraquinone-2,6-sodium disulfonate negative electrode inserts in the equal and anode chamber that is that be separated by with proton exchange membrane of volume and cathode chamber therebetween respectively as anode and the negative electrode of microbiological fuel cell, and by carbon felt/polypyrrole/anthraquinone-2,6-sodium disulfonate anode and carbon felt/polypyrrole/anthraquinone-2,6-sodium disulfonate negative electrode access external circuit; Finally, oxidized substrate in anode chamber produces electronics, proton, electron transmission is to carbon felt/polypyrrole/anthraquinone-2,6-sodium disulfonate anode surface, carbon felt/polypyrrole/anthraquinone-2 is arrived via external circuit, 6-sodium disulfonate negative electrode, proton diffuses to cathode chamber through proton exchange membrane, azo dyes in cathode chamber, proton and arrive carbon felt/polypyrrole/anthraquinone-2 through external circuit, the electronics of 6-sodium disulfonate negative electrode is at carbon felt/polypyrrole/anthraquinone-2, there is reduction half-reaction in 6-sodium disulfonate cathode surface, makes azo dyes be reduced decolouring.
The beneficial effect that the present invention has after adopting technique scheme is:
1, the present invention adopts electropolymerization-doping techniques to prepare carbon felt/polypyrrole/anthraquinone-2,6-sodium disulfonate (CF/PPy/AQDS) electrode, adopt CF/PPy/AQDS electrode at microbiological fuel cell yin, yang electrode simultaneously, increase the speed (namely electronics is delivered to the process of anode of fuel cell in microbial cell) that anode current transmits, significantly improve the speed of reduction decolorization of azo dyes wastewater at microbial fuel cell cathode, azo dye wastewater can be processed quickly and efficiently.
2, the present invention does not need additionally to input electric energy.The electronics that anode of microbial fuel cell room produces is passed to anode surface from microbial cell and arrives cathode electrode via external circuit, and electronics constantly produces, transmit, flow formation electric current, completes electricity generation process.Meanwhile, yin, yang electrode adopts CF/PPy/AQDS electrode to improve electricity generation performance of microbial fuel cell simultaneously.
3, the present invention can not cause secondary pollution.Negative electrode azo dyes there occurs the reduction reaction of four electronics, and azo bond fracture generates amine substance, and reaction equation is:
.Amine substance has a lot of application in real life, as the reduzate of methyl orange
n,N-dimethyl-p-phenylenediamine (PPD) is applied to H
2the removal of S.
4, the degradation rate of the present invention to pollutants such as methyl oranges is very fast.Cathodic reduction reaction is for removing the difficult degradation azo dyes pollutant itself with higher oxygen reduction potential, yin, yang electrode adopts CF/PPy/AQDS electrode to add the speed of anode current transmission simultaneously, accelerate cathode surface and reduction half-reaction occurs, improve the degradation rate to pollutants such as methyl oranges.
Accompanying drawing explanation
Fig. 1 is the structural representation of microbiological fuel cell;
Fig. 2 be yin, yang electrode all adopt carbon felt/polypyrrole/anthraquinone-2,6-sodium disulfonate (CF/PPy/AQDS) electrode do the output voltage variation relation curve chart in time of microbiological fuel cell;
Fig. 3 be four groups by Different electrodes material form yin, yang electrode do power density and the current density graph of relation of microbiological fuel cell;
Fig. 4 be four groups by Different electrodes material form yin, yang electrode do methyl orange residual concentration and the initial concentration percentage change curve of microbiological fuel cell;
In Fig. 1,1. electrode jack; 2. silicone gasket and pad; 3. anode chamber; 4. cathode chamber; 5. carbon felt/polypyrrole/anthraquinone-2,6-sodium disulfonate anode; 6. carbon felt/polypyrrole/anthraquinone-2,6-sodium disulfonate negative electrode; 7. proton exchange membrane; 8. backing plate.
Embodiment
First prepare carbon felt/polypyrrole/anthraquinone-2,6-sodium disulfonate (CF/PPy/AQDS) electrode, method is: be first placed in thermal reaction furnace by carbon felt, take ammonia as gas medium, temperature be 600 DEG C, the time be the condition of 30 s under react, to increase carbon felt specific area.Then utilize conventional electropolymerization-doping techniques, adopting three electrode diaphragm formula H type electrolysis tanks, is 3.0 × 3.0 cm by surface area
2carbon felt as work electrode, mix after the work electrode indoor of three electrode diaphragm formula H type electrolysis tanks add anthraquinone-2,6-sodium disulfonate (AQDS) that 100 mL concentration are 0.029 mol/L and 20mL concentration is the polypyrrole (ppy) of 0.12 mol/L.The auxiliary electrode of the auxiliary electrode indoor in three electrode diaphragm formula H type electrolysis tanks is platinized platinum, and platinized platinum surface area is 1.0 × 1.0 cm
2, auxiliary electrode room is connected with work electrode room by cation-exchange membrane.At indoor filling 120 mL of auxiliary electrode, concentration is the H of 0.1 mol/L
2sO
4.Reference electrode in three electrode diaphragm formula H type electrolysis tanks adopts saturated calomel electrode, and prepare 3 mol/L by secondary deionized water, temperature is KCl saturated solution 120 mL of 20 DEG C, and reference electrode is connected with work electrode room by salt bridge.The working current density using constant potential/galvanostat to control three electrode diaphragm formula H type electrolysis tanks is 1.83 ~ 1.86 mA/cm
2, preparation temperature is 10.0 ~ 10.2 DEG C, and polymerization time is 3600 ~ 3800s.One deck polypyrrole/anthraquinone-2 is formed at working electrode surface, 6-sodium disulfonate thin layer, obtained carbon felt/polypyrrole/anthraquinone-2,6-sodium disulfonate anode and carbon felt/polypyrrole/anthraquinone-2,6-sodium disulfonate negative electrode, carbon felt/polypyrrole/anthraquinone-2,6-sodium disulfonate anode and carbon felt/these two electrodes of polypyrrole/anthraquinone-2,6-sodium disulfonate negative electrode are kept at and are filled with in the distilled water of High Purity Nitrogen.
The structure of microbiological fuel cell as shown in Figure 1, adopt two pool structure, there is the equal anode chamber of volume 3 and cathode chamber 4, separate by proton exchange membrane 7 between anode chamber 3 and cathode chamber 4, the top of proton exchange membrane 7 and bottom are sealed by silicone gasket and pad 2, anode chamber 3 be fixedly connected with one piece of backing plate 8 bottom cathode chamber 4, there is in anode chamber 3 substrate (as glucose etc.), substrate is oxidized under microbial action, is azo dye wastewater in cathode chamber 4.Anode chamber 3 is all connected an electrode jack 1 with the top of cathode chamber 4, by above-mentioned obtained carbon felt/polypyrrole/anthraquinone-2,6-sodium disulfonate anode 5 inserts in anode chamber 3 by the electrode jack 1 at top, anode chamber 3, above-mentioned obtained carbon felt/polypyrrole/anthraquinone-2,6-sodium disulfonate negative electrode 6 is inserted in cathode chamber 4 by the electrode jack 1 at cathode chamber 4 top.Carbon felt/polypyrrole/anthraquinone-2,6-sodium disulfonate negative electrode 6 and carbon felt/polypyrrole/anthraquinone-2,6-sodium disulfonate anode 5 are accessed external circuit.
The substrate oxidation of anode chamber 3 produces electronics, proton and metabolite, the electronics wherein produced is passed to carbon felt/polypyrrole/anthraquinone-2 from microbial cell, 6-sodium disulfonate anode 5 surface, carbon felt/polypyrrole/the anthraquinone-2 in cathode chamber 4 is arrived again through external circuit, 6-sodium disulfonate negative electrode 6, the proton produced diffuses to cathode chamber 4 from anode chamber 3 through proton exchange membrane 7, electron acceptor azo dyes in cathode chamber 4, carbon felt/polypyrrole/anthraquinone-2, 6-sodium disulfonate anode 5 transmits next proton and arrives carbon felt/polypyrrole/anthraquinone-2 through external circuit, the electronics of 6-sodium disulfonate negative electrode 6 is at carbon felt/polypyrrole/anthraquinone-2, the catalyzed generation reduction half-reaction of 6-sodium disulfonate anode 5 surface, like this, the moon of microbiological fuel cell, positive electrode adopts CF/PPy/AQDS electrode simultaneously, add the speed that anode current transmits, not only increase electricity generation performance of microbial fuel cell, also accelerate cathode surface and reduction half-reaction occurs, azo dyes is decoloured by fast restore.Meanwhile, electronics constantly produces, transmit, flow formation electric current, completes electricity generation process.
Below provide 1 embodiment of the present invention to set forth implementer's case of the present invention further:
embodiment 1
Utilize conventional electropolymerization-doping techniques, polymerization is completed in electrode diaphragm formula H type electrolysis tank at work electrode, reference electrode and auxiliary electrode three, using the carbon felt after specific area increases process as work electrode, work electrode indoor filling 100 mL concentration is the anthraquinone-2 of 0.029 mol/L, 6-sodium disulfonate (AQDS) and 20mL concentration are the mixed liquor of the polypyrrole (ppy) of 0.12 mol/L, and using constant potential/galvanostat to control working current density is 1.85 mA/cm
2, preparation temperature is 10 DEG C, polymerization time is 3800s, forms one deck polypyrrole/anthraquinone-2,6-sodium disulfonate thin layer at working electrode surface, obtained carbon felt/polypyrrole/anthraquinone-2,6-sodium disulfonate anode and carbon felt/polypyrrole/anthraquinone-2,6-sodium disulfonate negative electrode.By obtained carbon felt/polypyrrole/anthraquinone-2,6-sodium disulfonate anode 5 and carbon felt/polypyrrole/anthraquinone-2,6-sodium disulfonate negative electrode 6 accesses external circuit simultaneously, and in the anode chamber 3 inserting microbiological fuel cell respectively and cathode chamber 4, anode chamber 3 is equal with cathode chamber 4 volume and be separated by with proton exchange membrane 7 therebetween.By whole microbiological fuel cell at sterile purification operating desk ultra violet lamp 30 min, the ozone blowout that blowing about 15 min will produce after ultraviolet irradiation, has assembled the structure of the microbiological fuel cell shown in Fig. 1.Then this microbiological fuel cell is started, output voltage to be moved to reaches stable, the methyl orange solution of 0.04 mmol/L, pH=3.0 is added in cathode chamber 4, temperature controls at about 30 ± 1 DEG C, now, the open circuit voltage measuring microbiological fuel cell increases sharply, and shows carbon felt/polypyrrole/anthraquinone-2, electrical potential difference between 6-sodium disulfonate anode 5 and carbon felt/polypyrrole/anthraquinone-2,6-sodium disulfonate negative electrode 6 increases.Microbiological fuel cell is accessed load resistance, automatically gathered output voltage continuously by the 16 channel signal collectors connecting computer and stored, 1 time is recorded every 1 min, methyl orange is added continuously in cathode chamber 4, Microbial fuel is made constantly to repeat electrogenesis, external circuit accesses the resistance of 2000 Ω, and maximum output voltage is 275 mV.In a circulation, Microbial fuel produces metastable output voltage 275 ± 18 mV in 1.02 h after this; After 1.02h, because cathode electronics acceptor methyl orange has been degraded substantially, output voltage is dropped rapidly to 65 ± 15 mV.Now, the solution of estimating cathode chamber 4 is become colorless by redness.When rejoining 0.04 mmol/L methyl orange, Microbial fuel repeats electrogenesis.Draw out the time dependent graph of relation of output voltage as shown in Figure 2, as shown in Figure 2, carbon felt/polypyrrole/anthraquinone-2 of the present invention, 6-sodium disulfonate anode 5 and carbon felt/polypyrrole/anthraquinone-2,6-sodium disulfonate negative electrode 6 directly using azo dyes as electron acceptor, create the electric current of continous-stable, azo dyes is by effectively degraded fast simultaneously.
2 comparative examples are below provided:
comparative example 1
The method of carbon felt/polypyrrole/anthraquinone-2,6-sodium disulfonate anode 5 and carbon felt/polypyrrole/anthraquinone-2,6-sodium disulfonate negative electrode 6 that makes is with above-described embodiment 1.
By carbon felt/polypyrrole/anthraquinone-2,6-sodium disulfonate anode 5 and carbon felt/polypyrrole/anthraquinone-2,6-sodium disulfonate negative electrode 6 as first group of electrode, then makes another three groups of electrodes, and second group of electrode all adopts titanium silk, the anode of the 3rd group of electrode adopts carbon felt/polypyrrole/anthraquinone-2,6-sodium disulfonate, negative electrode adopts titanium silk, and the anode of the 4th group of electrode adopts titanium silk, negative electrode adopts carbon felt/polypyrrole/anthraquinone-2,6-sodium disulfonate.
Respectively the yin, yang electrode that these four groups are made up of different materials is used for four microbiological fuel cells as shown in Figure 1, start microbiological fuel cell output voltage to be moved to and reach stable, in cathode chamber 4, add PH=7.0, concentration is 0.1 mol/L phosphate buffer solution, in cathode chamber 4, air is passed into airway, after moving to output voltage stabilization, regulate the pH value of solution to 3.0 of cathode chamber 4.By changing the resistance of external circuits resistance, when output voltage reaches quasi-stable state, record power density and the current density of the yin, yang electrode that these four groups are made up of different materials, draw out relation curve as shown in Figure 3, as shown in Figure 3, yin, yang electrode all adopts carbon felt/polypyrrole/anthraquinone-2, the current density amplification of first group of electrode of 6-sodium disulfonate material is maximum, power density is maximum, and its electricity generation performance is obviously optimum, and Degradation of Azo Dyes speed is also the fastest.
comparative example 2
Adopt four groups of yin, yang electrodes be made up of different materials in comparative example 1, method is with comparative example 1.
Four microbiological fuel cells respectively in running and comparing example 1, after moving to output voltage stabilization, 0.1 mmol/L methyl orange solution is added in cathode chamber 4, and regulate the pH value of solution to 3.0 of cathode chamber 4, external circuit all connects 2000 Ω resistance, and startup microbiological fuel cell all fades to the solution of cathode chamber 4.In the methyl orange reduction-decolor process of cathode chamber 4, in chronological sequence 1ml response sample is drawn in gradation, the phosphate buffer solution identical with sample pH value is adopted to dilute, direct employing spectrophotometer method determination methyl orange residual concentration, draw out the curve chart that time as shown in Figure 4 and residual concentration and initial concentration percentage changes, as shown in Figure 4, yin, yang electrode all adopts the methyl orange degradation speed in the microorganism fuel cell cathode room of carbon felt/polypyrrole/anthraquinone-2,6-sodium disulfonate material the fastest.
Claims (1)
1. one kind is accelerated the method for reduction decolorization of azo dyes wastewater at microbial fuel cell cathode, substrate oxidized under microbial action in the anode chamber (3) of microbiological fuel cell, cathode chamber is azo dye wastewater in (4), it is characterized in that having following steps:
1) three electrode diaphragm formula H type electrolysis tanks are adopted, using carbon felt as work electrode, adding the Homogeneous phase mixing liquid that anthraquinone-2,6-sodium disulfonate that 100 mL concentration are 0.029 mol/L and 20mL concentration are the polypyrrole of 0.12 mol/L in work electrode indoor, is 1.83 ~ 1.86 mA/cm in current density
2, temperature is 10.0 ~ 10.2 DEG C, polymerization time is form one deck polypyrrole/anthraquinone-2 at working electrode surface under the condition of 3600 ~ 3800s, 6-sodium disulfonate thin layer, obtained carbon felt/polypyrrole/anthraquinone-2,6-sodium disulfonate anode (5) and carbon felt/polypyrrole/anthraquinone-2,6-sodium disulfonate negative electrode (6);
2) by carbon felt/polypyrrole/anthraquinone-2,6-sodium disulfonate anode (5) and carbon felt/polypyrrole/anthraquinone-2,6-sodium disulfonate negative electrode (6) inserts in the equal and anode chamber (3) that is that be separated by with proton exchange membrane (7) of volume and cathode chamber (4) therebetween respectively as anode and the negative electrode of microbiological fuel cell, and by carbon felt/polypyrrole/anthraquinone-2,6-sodium disulfonate anode (5) and carbon felt/polypyrrole/anthraquinone-2,6-sodium disulfonate negative electrode (6) access external circuit;
3) the oxidized substrate in anode chamber (3) produces electronics, proton, electron transmission is to carbon felt/polypyrrole/anthraquinone-2, 6-sodium disulfonate anode (5) surface, carbon felt/polypyrrole/anthraquinone-2 is arrived via external circuit, 6-sodium disulfonate negative electrode (6), proton diffuses to cathode chamber (4) through proton exchange membrane (7), azo dyes in cathode chamber (4), proton and arrive carbon felt/polypyrrole/anthraquinone-2 through external circuit, the electronics of 6-sodium disulfonate negative electrode (6) is at carbon felt/polypyrrole/anthraquinone-2, there is reduction half-reaction in 6-sodium disulfonate negative electrode (6) surface, azo dyes is made to be reduced decolouring.
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| Publication number | Priority date | Publication date | Assignee | Title |
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| CN107043168A (en) * | 2017-01-20 | 2017-08-15 | 常州大学 | Accelerate the method for the electric Fenton fuel battery negative pole degraded Polyester wastewater of microorganism |
| WO2022168121A1 (en) | 2021-02-08 | 2022-08-11 | Council Of Scientific & Industrial Research | Earthen membrane based two chambered constructed wetland cum micriobial fuel cell for treatment and detoxification of waste water containing azo dye |
| RU2809834C1 (en) * | 2023-07-04 | 2023-12-19 | Федеральное государственное бюджетное образовательное учреждение высшего образования "Российский химико-технологический университет имени Д.И. Менделеева" (РХТУ им. Д. И. Менделеева) | Microbial fuel cell for generating electricity from wastewater |
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| CN104900889B (en) * | 2015-04-30 | 2017-12-08 | 广东工业大学 | Polypyrrole CNT manganese AQDS combination electrode material preparation methods |
| CN107046135A (en) * | 2017-01-20 | 2017-08-15 | 常州大学 | Improve the method that microbiological fuel cell handles Polyester wastewater electricity production |
| CN108328745A (en) * | 2018-01-08 | 2018-07-27 | 厦门大学 | The discoloration method of microbiological fuel cell based on polyethylene dioxythiophene membrane electrode |
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Cited By (3)
| Publication number | Priority date | Publication date | Assignee | Title |
|---|---|---|---|---|
| CN107043168A (en) * | 2017-01-20 | 2017-08-15 | 常州大学 | Accelerate the method for the electric Fenton fuel battery negative pole degraded Polyester wastewater of microorganism |
| WO2022168121A1 (en) | 2021-02-08 | 2022-08-11 | Council Of Scientific & Industrial Research | Earthen membrane based two chambered constructed wetland cum micriobial fuel cell for treatment and detoxification of waste water containing azo dye |
| RU2809834C1 (en) * | 2023-07-04 | 2023-12-19 | Федеральное государственное бюджетное образовательное учреждение высшего образования "Российский химико-технологический университет имени Д.И. Менделеева" (РХТУ им. Д. И. Менделеева) | Microbial fuel cell for generating electricity from wastewater |
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