CN107043168A - Accelerate the method for the electric Fenton fuel battery negative pole degraded Polyester wastewater of microorganism - Google Patents
Accelerate the method for the electric Fenton fuel battery negative pole degraded Polyester wastewater of microorganism Download PDFInfo
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- CN107043168A CN107043168A CN201710041522.XA CN201710041522A CN107043168A CN 107043168 A CN107043168 A CN 107043168A CN 201710041522 A CN201710041522 A CN 201710041522A CN 107043168 A CN107043168 A CN 107043168A
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- carbon felt
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- laccase
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- C—CHEMISTRY; METALLURGY
- C02—TREATMENT OF WATER, WASTE WATER, SEWAGE, OR SLUDGE
- C02F—TREATMENT OF WATER, WASTE WATER, SEWAGE, OR SLUDGE
- C02F3/00—Biological treatment of water, waste water, or sewage
- C02F3/34—Biological treatment of water, waste water, or sewage characterised by the microorganisms used
- C02F3/342—Biological treatment of water, waste water, or sewage characterised by the microorganisms used characterised by the enzymes used
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- C—CHEMISTRY; METALLURGY
- C02—TREATMENT OF WATER, WASTE WATER, SEWAGE, OR SLUDGE
- C02F—TREATMENT OF WATER, WASTE WATER, SEWAGE, OR SLUDGE
- C02F3/00—Biological treatment of water, waste water, or sewage
- C02F3/005—Combined electrochemical biological processes
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- C—CHEMISTRY; METALLURGY
- C02—TREATMENT OF WATER, WASTE WATER, SEWAGE, OR SLUDGE
- C02F—TREATMENT OF WATER, WASTE WATER, SEWAGE, OR SLUDGE
- C02F2101/00—Nature of the contaminant
- C02F2101/30—Organic compounds
- C02F2101/34—Organic compounds containing oxygen
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- C—CHEMISTRY; METALLURGY
- C02—TREATMENT OF WATER, WASTE WATER, SEWAGE, OR SLUDGE
- C02F—TREATMENT OF WATER, WASTE WATER, SEWAGE, OR SLUDGE
- C02F2101/00—Nature of the contaminant
- C02F2101/30—Organic compounds
- C02F2101/38—Organic compounds containing nitrogen
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- C—CHEMISTRY; METALLURGY
- C02—TREATMENT OF WATER, WASTE WATER, SEWAGE, OR SLUDGE
- C02F—TREATMENT OF WATER, WASTE WATER, SEWAGE, OR SLUDGE
- C02F2305/00—Use of specific compounds during water treatment
- C02F2305/02—Specific form of oxidant
- C02F2305/026—Fenton's reagent
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Abstract
A kind of method for accelerating the electric Fenton fuel battery negative pole degraded Polyester wastewater of microorganism of the present invention includes making carbon felt electrode, prepares γ FeooH, laccase modified electrode and starts battery.Laccase and γ FeooH embeddings are fixed on cathode carbon felt using sodium alginate, negative electrode is modified.Using laccase electro transfer to oxygen molecule, oxidation base is formed, along with the OH of Fenton formation, Cathodic oxygen reduction is improved, improves the COD degradation rate of Polyester wastewater.Laccase is the oxidoreducing enzyme that copper is contained at a kind of center simultaneously, and the output voltage of system can be improved using this modification negative electrode.
Description
Technical field
The present invention relates to the field of sewage disposal technology, and in particular to one kind accelerates the electric Fenton fuel battery negative pole of microorganism
The method for Polyester wastewater of degrading.
Technical background
Polyester wastewater is production polyurethane foam plastics, foam stabiliser, paper industry defoamer, crude oil demulsifier and height
Imitate the industry such as low-foaming detergent and produce industrial wastewater, mainly comprising polyethers (also known as PPG), diethylene glycol (DEG), dimethylamine, sweet
Oil, oxirane, expoxy propane, sucrose etc..Not only COD in waste waterCrVery high (general 10~30g/L), and biodegradability pole
Difference (BOD5/CODCr<0.05), it is difficult to directly carry out biochemical treatment.According to single processing method, it is difficult to reach country
Discharge standard.If the Polyester wastewater organic matter for being discharged into water body exceedes allowance, anaerobism phenomenon occurs in water body, to animals and plants and
River ecological has undesirable effect.At home and abroad in Polyester wastewater processing technology field, microorganism electricity Fenton fuel battery negative pole
Redox treatment technology has higher treatment effeciency, non-secondary pollution, is not required to the advantages such as additional power source, causes domestic and international scientific research
Great concern.
Microorganism electricity Fenton technology obtains electric energy using microorganism anode anaerobic degradation organic matter, and electron-proton is delivered to
Negative electrode, along with the air and ferrous ion of cathode chamber, forms Fenton reagent, has Strong oxdiative ability OH useless to aoxidize
Water.But the characteristics of being due to the low electric Fenton fuel cell output power of microorganism and Polyester wastewater difficult degradation, microorganism electricity Fenton
Fuel cell technology is not high to Polyester wastewater degradation rate.
The content of the invention
The technical problem to be solved in the present invention is:The present invention provides a kind of acceleration microorganism electric Fenton fuel battery negative pole drop
The method for solving Polyester wastewater, among the wastewater treatments such as polyethers.
The technical solution adopted for the present invention to solve the technical problems is:Laccase and Υ-FeOOH are wrapped using sodium alginate
It is embedded in cathode chamber carbon felt, oxygen is continually provided while being aerated always.There are a large amount of oxygen while Fenton reagent is formed
In the presence of gas, using laccase electro transfer to oxygen molecule, oxidation base is formed, Cathodic oxygen reduction is improved.Simultaneously
Laccase is the oxidoreducing enzyme that copper is contained at a kind of center, can improve the output voltage of system.
A kind of method of the electric Fenton fuel battery negative pole degraded Polyester wastewater of acceleration microorganism of the present invention, including make carbon
Felt pole, prepares γ-FeooH, laccase modified electrode and startup battery.
Described making carbon felt electrode is by 2 pieces of 5*5cm2Carbon felt is placed in thermal reaction furnace, using ammonia as gas medium,
600 DEG C of temperature, time are reaction under conditions of 30s, to increase carbon felt specific surface area.Then it is interspersed in copper conductor in carbon felt,
Carbon felt electrode is made.
Described γ-the FeooH that prepare are the accurate 0.1mol/LFeSO for measuring 100mL4Solution is placed in beaker, in magnetic force
Under stirring, 100mL 5*10 is added-4mol/L EDTA-Na2Solution, controls CEDTA-Na2/CFe2+=5 × 10- 3Within the scope of,
It is 8.64 with the pH of 6mol/L NaOH solution regulation systems, then passing to air, (air supply uses bubbler, and flow is
0.11m3/ h), with general lighting light according to (illumination 300lux) and controlling reaction temperature (14~25 DEG C).With the progress of reaction,
The color of reaction system by initial canescence rapidly go to it is thick it is blackish green be finally yellow, final pH is about 4.8, is obtained
To predecessor γ-FeOOH.
Described laccase modified electrode is to weigh 5g sodium alginate powders and add 195mL distilled water in beaker to be positioned over
In 80 DEG C of water-baths, 2.5% solution is stirred into.0.445g γ-FeooH and 2.1g laccases are taken to be placed on 2.5% alginic acid again
Ultrasonic agitation is mixed in sodium, makes Fe in catholyte2+Concentration be 5mM and laccase concentration 1mg/mL, then 1 piece of 5*5cm2Carbon felt is soaked
Not in the solution of beaker, carbon felt is set uniformly to be stained with smearing sodium alginate/γ-FeooH/ laccase solutions.Then carbon felt is soaked again
Not in 4% Cacl215h is fixed in solution, the carbon felt then modified with distilled water flushing.
Described startup battery is that the unmodified electrode insertion volume with modification is equal and therebetween with PEM
In the anode chamber and cathode chamber that are separated by, and access external circuit.The agitator of anode chamber is opened, anolyte is stirred, accelerates microorganism
Anaerobic reaction, improve battery power output.The aeration of cathode chamber is then turned on, oxygen is continually supplied, accelerates Fenton
With oxidation reaction of the laccase to Polyester wastewater.Finally, the oxidized substrate in anode chamber produces electronics, proton, electron transmission
To carbon felt anode electrode surface, the negative electrode of modification is reached via external circuit, proton diffuses to cathode chamber through PEM.Constantly
Polyester wastewater, proton in the cathode chamber of aeration and the electronics through external circuit arrival laccase modification carbon felt negative electrode are in carbon felt negative electrode table
Oxidation reaction occurs for face, improves the COD degradation rate of Polyester wastewater.
The present invention has an advantageous effect in that after using above-mentioned technical proposal：
1. the present invention prepares the carbon felt cathode electrode of γ-FeooH and laccase using sodium alginate investment, laccase is electronics
Shift cathode oxygen, generation oxidation base；Fenton reagent generation simultaneously has Strong oxdiative ability OH.In the effect of two kinds of oxidation bases
Under, oxidation operation in Polyester wastewater can be improved Polyester wastewater COD degradation rate.
2. the present invention does not need additional input electric energy.The electronics that microorganism electricity Fenton anode of fuel cell room anaerobism is produced from
Microbial cell is transferred to anode surface and reaches cathode electrode via external circuit, and electronics is constantly be generated, transmitted, flowing formation electricity
Stream, completes electricity generation process, saves the energy.The negative electrode of laccase modification simultaneously, is conducive to improving the output voltage of battery.
Brief description of the drawings
The present invention is further described with reference to the accompanying drawings and examples.
Fig. 1 is the structural representation of the electric Fenton fuel cell of microorganism.
In Fig. 1：1. electrode jack, 2. silicone gaskets and pad, 3. carbon felt anodes, 4. carbon felts/sodium alginate/γ-
FeooH/ laccase negative electrodes, 5. agitators, 6. aeration heads, 7. cation exchange proton membranes, 8. anode chambers, 9. cathode chambers.
Fig. 2 is two groups and constitutes the output electricity that yin, yang electrode makees the electric Fenton fuel cell of microorganism by Different electrodes material
Press the graph of a relation with the time.
Fig. 3 is two groups and constitutes yin, yang electrode by Different electrodes material and do the polyethers of the electric Fenton fuel cell of microorganism and give up
Water COD degradation rate with the time graph of a relation；
Embodiment
In conjunction with the accompanying drawings, the present invention is further explained in detail.
As shown in FIG. 1 to 3, a kind of acceleration microorganism of the invention electric Fenton fuel battery negative pole degraded Polyester wastewater
Method, including carbon felt electrode is made, prepare γ-FeooH, laccase modified electrode and startup battery.
Described making carbon felt electrode is by 2 pieces of 5*5cm2Carbon felt is placed in thermal reaction furnace, using ammonia as gas medium,
600 DEG C of temperature, time are reaction under conditions of 30s, to increase carbon felt specific surface area.Then it is interspersed in copper conductor in carbon felt,
Carbon felt electrode is made.
Described γ-the FeooH that prepare are the accurate 0.1mol/LFeSO for measuring 100mL4Solution is placed in beaker, in magnetic force
Under stirring, 100mL 5*10 is added-4mol/L EDTA-Na2Solution, controls CEDTA-Na2/CFe2+=5 × 10- 3Within the scope of,
It is 8.64 with the pH of 6mol/L NaOH solution regulation systems, then passing to air, (air supply uses bubbler, and flow is
0.11m3/ h), with general lighting light according to (illumination 300lux) and controlling reaction temperature (14~25 DEG C).With the progress of reaction,
The color of reaction system by initial canescence rapidly go to it is thick it is blackish green be finally yellow, final pH is about 4.8, is obtained
To predecessor γ-FeOOH.
Described laccase modified electrode is to weigh 5g sodium alginate powders and add 195mL distilled water in beaker to be positioned over
In 80 DEG C of water-baths, 2.5% solution is stirred into.0.445g γ-FeooH and 2.1g laccases are taken to be placed on 2.5% alginic acid again
Ultrasonic agitation is mixed in sodium, makes Fe in catholyte2+Concentration be 5mM and laccase concentration 1mg/mL, then 1 piece of 5*5cm2Carbon felt is soaked
Not in the solution of beaker, carbon felt is set uniformly to be stained with smearing sodium alginate/γ-FeooH/ laccase solutions.Then carbon felt is soaked again
Not in 4% Cacl215h is fixed in solution, the carbon felt then modified with distilled water flushing.
Described startup battery is to build the electric Fenton fuel cell of microorganism by Fig. 1, using the double pool structures of H, with body
The equal anode chamber 8 of product and cathode chamber 9, are spaced, PEM 7 between anode chamber 8 and cathode chamber 9 with PEM 7
Top and bottom sealed by silicone gasket and pad 2.Anode chamber 8 and the top of cathode chamber 9 are all connected with an electrode jack
1, carbon felt pole plate is inserted into anode chamber 8, while placing agitator 5.The carbon felt electrode 4 of modification is inserted into cathode chamber 9, together
When place aeration head 6.By the electric Fenton fuel cell of the microorganism put up in sterile purification operating desk ultra violet lamp
30min, blowing about 15min blows out the ozone produced after ultraviolet irradiation.Have in anode chamber 8 methanol and Polyester wastewater substrate and
Microorganism liquid, temperature control is at 30 ± 1 DEG C or so, while starting agitator, methanol and Polyester wastewater are acted in microbiological anaerobic
It is lower to be oxidized release electronics and proton.It is Polyester wastewater in cathode chamber 9, the pH for starting to adjust cathode chamber Polyester wastewater is 3, then
Starting aerator simultaneously, there is provided oxygen.Voltmeter data gradually rise, and illustrate start battery success.By the electric Fenton combustion of microorganism
Expect battery access load resistance, by connection computer the continuous automatic data collection output voltage of 16 channel signal collectors and store,
Recorded 1 time every 1min, external circuit accesses 1000 Ω resistance, and maximum output voltage is 624mV.It is oxidized in anode chamber
Substrate produces electronics, proton, and electron transmission to carbon felt electrode surface reaches the negative electrode of modification via external circuit, proton is through proton
Exchange membrane diffuses to cathode chamber, the Polyester wastewater of the cathode chamber being constantly aerated, proton and reaches laccase modification carbon felt through external circuit
In carbon felt cathode surface oxidation reaction occurs for the electronics of negative electrode, improves 20% COD degradation rate of Polyester wastewater, reaches
55.7%.Meanwhile, electronics is constantly be generated, transmits, flows and forms electric current, completes electricity generation process.
1 comparative example presented below：
Comparative example：Make carbon felt anode 3, carbon felt/sodium alginate/γ-FeooH/ laccases negative electrode 4 and carbon felt anode 5, carbon
Felt/polytetrafluoroethylene (PTFE) (PTFE)/γ-FeooH negative electrodes 6, the COD degradation rate to Polyester wastewater is compared.Make carbon felt/poly- four
PVF (PTFE)/γ-FeooH negative electrodes 6：0.445g γ-FeooH are added and stirred in 5g PTFE, it is then uniform to apply
It is put on carbon felt pole plate, re-dry fixes 15h.The yin, yang electrode that this two groups are made from a different material respectively is used for such as Fig. 1 institutes
The electric Fenton fuel cell of two microorganisms showing, the pH of regulation cathode chamber Polyester wastewater is 3, temperature control at 30 ± 1 DEG C or so,
Then the electric Fenton fuel cell of the microorganism is started, after operation to output voltage stabilization, external circuit connects 1000 Ω resistance, then
10ml water samples are taken when being segmented in 24h, COD is carried out and quickly determines, compares two groups of different negative electrodes and cell voltage is exported and right
The COD degradation rate of Polyester wastewater.
Using the above-mentioned desirable embodiment according to the present invention as enlightenment, by above-mentioned description, relevant staff is complete
Various changes and amendments can be carried out without departing from the scope of the technological thought of the present invention' entirely.The technology of this invention
Property scope is not limited to the content on specification, it is necessary to its technical scope is determined according to right.
Claims (2)
1. a kind of electric Fenton fuel-cell device of microorganism, it is characterised in that：It is equal with volume using the double pool structures of H
Anode chamber (8) and cathode chamber (9), are spaced, PEM between anode chamber (8) and cathode chamber (9) with PEM (7)
(7) top and bottom is sealed by silicone gasket and pad (2)；One is all connected with the top of anode chamber (8) and cathode chamber (9)
Electrode jack (1), carbon felt pole plate is inserted into anode chamber (8), while placing agitator (5), the carbon felt electrode (4) of modification is inserted
It is put into cathode chamber (9), while placing aeration head (6).
Accelerate the method for the electric Fenton fuel battery negative pole degraded Polyester wastewater of microorganism 2. a kind of, including make carbon felt electrode, system
Standby γ-FeooH, laccase modified electrode and startup battery, it is characterised in that：With following steps；
Described making carbon felt electrode is by 2 pieces of 5*5cm2Carbon felt is placed in thermal reaction furnace, using ammonia as gas medium, in temperature
600 DEG C, the time be 30s under conditions of react, to increase carbon felt specific surface area；Then it is interspersed in carbon felt, is made with copper conductor
Carbon felt electrode；
Described γ-the FeooH that prepare are the accurate 0.1mol/LFeSO for measuring 100mL4Solution is placed in beaker, in magnetic agitation
Under, add 100mL 5*10-4mol/LEDTA-Na2Solution, controls CEDTA-Na2/CFe2+=5 × 10- 3, use 6mol/L NaOH
The pH of solution regulation system is 8.64, and then passing to air, (air supply uses bubbler, and flow is 0.11m3/ h), with common
Houselights is according to (illumination 300lux) and controlling reaction temperature (14~25 DEG C)；With the progress of reaction, the color of reaction system by
Initial canescence rapidly go to it is thick it is blackish green be finally yellow, final pH is 4.8, obtains predecessor γ-FeOOH；
Described laccase modified electrode is to weigh 5g sodium alginate powders and add 195mL distilled water in beaker to be positioned over 80 DEG C
In water-bath, 2.5% solution is stirred into；0.445g γ-FeooH and 2.1g laccases are taken to be placed in 2.5% sodium alginate again
Ultrasonic agitation is mixed, and makes Fe in catholyte2+Concentration be 5mM and laccase concentration 1mg/mL, then 1 piece of 5*5cm2 carbon felt is immersed in
In the solution of beaker, carbon felt is set uniformly to be stained with smearing sodium alginate/γ-FeooH/ laccase solutions；Then carbon felt is immersed in again
4% Cacl215h is fixed in solution, the carbon felt then modified with distilled water flushing；
Described startup battery is to build the electric Fenton fuel cell of microorganism, using the double pool structures of H, with the equal sun of volume
Pole room (8) and cathode chamber (9), are spaced, PEM between anode chamber (8) and cathode chamber (9) with PEM (7)
(7) top and bottom is sealed by silicone gasket and pad (2)；One is all connected with the top of anode chamber (8) and cathode chamber (9)
Electrode jack (1), carbon felt pole plate is inserted into anode chamber (8), while placing agitator (5), the carbon felt electrode (4) of modification is inserted
It is put into cathode chamber (9), while placing aeration head (6)；The electric Fenton fuel cell of the microorganism put up is grasped in sterile purification
Make platform ultra violet lamp 30min, dried 15min, and the ozone produced after ultraviolet irradiation is blown out；There is first in anode chamber (8)
Alcohol and Polyester wastewater substrate and microorganism liquid, temperature control is at 30 ± 1 DEG C, while starting agitator (5), methanol and Polyester wastewater
Release electronics and proton are oxidized under microbiological anaerobic effect；Cathode chamber is Polyester wastewater in (9), starts regulation cathode chamber and gathers
The pH of ether wastewater is 3, and then starting aerator simultaneously, there is provided oxygen；Voltmeter data gradually rise, illustrate start battery into
Work(；The electric Fenton fuel cell of microorganism is accessed into load resistance, it is continuously automatic by 16 channel signal collectors of connection computer
Collection output voltage is simultaneously stored, and is recorded 1 time every 1min, and external circuit accesses 1000 Ω resistance, and maximum output voltage is
624mV；Oxidized substrate in anode chamber produces electronics, proton, and electron transmission is arrived to carbon felt electrode surface via external circuit
Up to the negative electrode of modification, proton diffuses to cathode chamber through PEM, Polyester wastewater, proton and the warp of the cathode chamber being constantly aerated
In carbon felt cathode surface oxidation reaction occurs for the electronics that external circuit reaches laccase modification carbon felt negative electrode, improves the COD of Polyester wastewater
Degradation rate；Meanwhile, electronics is constantly be generated, transmits, flows and forms electric current, completes electricity generation process.
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Cited By (6)
| Publication number | Priority date | Publication date | Assignee | Title |
|---|---|---|---|---|
| CN107265629A (en) * | 2017-06-09 | 2017-10-20 | 常州大学 | The method for Polyester wastewater of being degraded using the electric Fenton fuel cell of microorganism |
| CN108640255A (en) * | 2018-05-09 | 2018-10-12 | 南开大学 | A kind of method that carbon black FeOOH cathode bioelectricity Fenton handles Typical Aromatic class waste water and synchronous electrogenesis |
| CN109713328A (en) * | 2019-02-19 | 2019-05-03 | 东华大学 | A kind of carbon felt load iron oxide electrode and its preparation and application |
| CN112811525A (en) * | 2020-12-31 | 2021-05-18 | 同济大学 | Carbon felt loaded cerium-doped alpha-FeOOH nanosheet array electrode and preparation method and application thereof |
| CN113121071A (en) * | 2021-05-27 | 2021-07-16 | 江苏大学 | Micro-electricity-assisted immobilized laccase device, preparation method thereof and wastewater degradation method |
| CN113279011A (en) * | 2021-04-28 | 2021-08-20 | 东北电力大学 | Carbon felt electrode material with high conductivity |
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| Publication number | Priority date | Publication date | Assignee | Title |
|---|---|---|---|---|
| CN107265629A (en) * | 2017-06-09 | 2017-10-20 | 常州大学 | The method for Polyester wastewater of being degraded using the electric Fenton fuel cell of microorganism |
| CN108640255A (en) * | 2018-05-09 | 2018-10-12 | 南开大学 | A kind of method that carbon black FeOOH cathode bioelectricity Fenton handles Typical Aromatic class waste water and synchronous electrogenesis |
| CN108640255B (en) * | 2018-05-09 | 2021-01-08 | 南开大学 | Method for treating typical aromatic wastewater and synchronously generating electricity by carbon black hydroxyl ferric oxide cathode bioelectricity Fenton |
| CN109713328A (en) * | 2019-02-19 | 2019-05-03 | 东华大学 | A kind of carbon felt load iron oxide electrode and its preparation and application |
| CN112811525A (en) * | 2020-12-31 | 2021-05-18 | 同济大学 | Carbon felt loaded cerium-doped alpha-FeOOH nanosheet array electrode and preparation method and application thereof |
| CN112811525B (en) * | 2020-12-31 | 2022-08-26 | 同济大学 | Carbon felt loaded cerium-doped alpha-FeOOH nanosheet array electrode and preparation method and application thereof |
| CN113279011A (en) * | 2021-04-28 | 2021-08-20 | 东北电力大学 | Carbon felt electrode material with high conductivity |
| CN113121071A (en) * | 2021-05-27 | 2021-07-16 | 江苏大学 | Micro-electricity-assisted immobilized laccase device, preparation method thereof and wastewater degradation method |
| CN113121071B (en) * | 2021-05-27 | 2022-08-19 | 江苏大学 | Micro-electricity-assisted immobilized laccase device, preparation method thereof and wastewater degradation method |
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