CN104817169B - Microbial fuel cell (MFC) coupling electrolysis device and process method for processing PPCPs - Google Patents
Microbial fuel cell (MFC) coupling electrolysis device and process method for processing PPCPs Download PDFInfo
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- CN104817169B CN104817169B CN201510236788.0A CN201510236788A CN104817169B CN 104817169 B CN104817169 B CN 104817169B CN 201510236788 A CN201510236788 A CN 201510236788A CN 104817169 B CN104817169 B CN 104817169B
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- 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
- Y02W—CLIMATE CHANGE MITIGATION TECHNOLOGIES RELATED TO WASTEWATER TREATMENT OR WASTE MANAGEMENT
- Y02W10/00—Technologies for wastewater treatment
- Y02W10/10—Biological treatment of water, waste water, or sewage
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Abstract
The invention discloses a microbial fuel cell (MFC) coupling electrolysis device and a process for processing PPCPs, belonging to the technical field of water treatment. According to the invention, electric energy generated by an MFC is utilized to be introduced into an electric field in a biological treatment process, so that the problems that the degradation to certain PPCPs caused by the existing activated sludge process is poor and the effluent concentration is high are solved; moreover, an extra electric field does not need to be added, so that the problem of high electrolysis cost can be solved; a new concept is found for the practical application of the electric energy generated by the MFC.
Description
Technical field
The invention belongs to water-treatment technology field, relate to device and technique side that PPCPs processes
Method, especially microbiological fuel cell coupling electrolysis process the process of PPCPs.
Background technology
Utilize the pollutant in electrochemical method process waste water early to have to study widely, this type of side
The features such as it is high that method has treatment effeciency, easy to operate, and equipment is simple, great advantage is can be right
Organic substance for bio-refractory carries out degradable.It is a kind of cleaning, efficient sewage disposal
Method.But uniquely deficiency needs persistently to put into electric energy exactly, operating cost is excessive, hinders
Large-scale application in water treatment technology.Microbiological fuel cell (microbial fuel
Cell, MFC), by the effect of microorganism, by the organic matter degradation in waste water, produce simultaneously
Electric energy, is that the most promising a kind of bioelectrochemical learns a skill.But, the product electricity effect of MFC
Rate is relatively low, and when external resistance is 1000 Ω, its voltage produced is generally 0.3-0.7V, far away
Demand to reality application.
Medicine and personal care articles (pharmaceuticals and personal care products,
PPCPs) it is the class newcooperative medical system using and having potential ecological effect the most in a large number
Learning material, medicine for animals including people, agricultural and personal care articles, wherein medicine is broadly divided into
Antibiotic, steroid, anti-inflammation analgesic, mental medicine, developing agent, contraceptive and appetrol
Deng；Personal care articles is mainly Moschus compounds, disinfection sanitizer, sunscreen, cosmetics
Deng.In the nineties, in water system, PPCPs just detected, along with living standard and doctor
The raising for the treatment of level, PPCPs is shown by substantial amounts of use, monitoring result, and PPCPs can enter
Enter natural environment, cause source water pollute and ecosystem causes potential negative effect.
PPCPs has the features such as stronger persistency and bioaccumulation, and it is exposed in environment for a long time
Potential risk will be brought to human health, cause the common concern of countries in the world.With biography
System pollutant are different, and PPCPs continues reduced levels (such as μ g/L) even at one, also can
Cause significant eco-toxicity.Research shows, some PPCPs can interfere with in organism
Hormonal system, affect its normal function.
The most conventional water treatment technology is not for PPCPs design, some PPCPs
Can effectively be removed, other removal efficiency is the most relatively low, in some sewage treatment plant
In also can be through halogenide sterilization process before water outlet, the PPCPs in water can send out with chlorine, bromine
Raw reaction produces multiple halogenated by-products, and these novel halogenated by-products are almost without known
Toxicologic properties, these materials enter natural water along with water outlet, increase the potential wind to environment
Danger.Particularly some medicines, owing to its structure is through specialized designs, have specific biology
Effect, has potential, cumulative harmful effect to nontarget organism body.Find after testing,
In the sample of swimming-pool water, the PPCPs of several low concentration detected, show swimming pool after deliberation
In PPCPs volatilize hardly, and can carry out the most anti-with the chlorine that used of sterilization
Should, produce multiple secondary species.These materials all can enter internal along with the metabolism of people,
The health of people is had a huge impact.
Abdelmelek et al. utilizes reverse osmosis technology to remove the PPCPs in water, and utilizes high-order
Oxidation technology is thoroughly degraded these Organic substances being trapped.Utilize continuous ultrasonic and impulse ultrasound
Ripple is also used to the PPCPs that degrades.It has been investigated that, for the compound arteries and veins that molecular structure is less
The degradation rate rushing ultrasound wave is bigger than continuous ultrasonic, and the compound for macromole surpasses continuously
The degradation rate of sound wave is better.Also have and utilize in adsorbing material absorption water
PPCPs, as SWCN, graphene oxide, multi-walled carbon nano-tubes, Graphene,
Graphite etc..
These methods are required for putting into the energy or chemical reagent, not only invest huge, and operate
Loaded down with trivial details.The water yield that municipal sewage even surface water faced by and is the biggest, these methods are either
The biggest difficulty is had from practical operation or economic investment.
Summary of the invention
It is an object of the invention to provide a kind of bio electrochemistry technique, in conjunction with microbial treatments and electricity
The feature of chemistry, the process unit of the PPCPs that the most well degrades and method.
Further with MFC produce electric energy, in biological treatment on introduce electric field, with
Solving existing activated sludge process poor to some PPCPs degradation property, aqueous concentration is high, and
And need not extra electric field, solve electrolysis costly, and be the actual application of MFC electric energy
Have found a kind of new approaches.
The present invention solves that above-mentioned technical problem adopts the technical scheme that.
Microbiological fuel cell coupling electrolysis unit, it is characterised in that at least include elevated tank
(1), the first valve (2), sbr reactor device (3), mud valve (4), Microbial fuel electricity
Pond group (5), wire (6), titanium silk (7), battery lead plate (8), elevated tank (1) passes through
Valve (2) connects with the water inlet of sbr reactor device (3), microbiological fuel cell group (5)
Yin, yang the two poles of the earth be connected with two electrode plate (8) through wire (6), titanium silk (7) respectively,
Battery lead plate (8) inserts in sbr reactor device (3), and the largest face of two electrode plate (8) is put down
Row relatively and keeps certain distance, and after sbr reactor device (3) has been intake, liquid level need to be higher than
Battery lead plate (8), sbr reactor device (3) bottom is additionally provided with aeration head (16), air compressor
(13) it is connected with aeration head (16) by gas flowmeter (14) and the second valve (15),
Sbr reactor device (3) is provided with mud valve (4)；
Wherein preferred microorganism fuel cell unit (5) is single chamber air cathode microbial fuel electricity
Pond, single chamber air cathode microbial fuel cell includes anode (9), negative electrode (10), container
(11), its Anodic (9) is positioned in container (11), and negative electrode (10) is container (11)
Sidewall, side, outside directly and air contact, sets between (10) at anode (9), negative electrode
Change the mouth of a river (12).
The present invention preferably selects microbiological fuel cell group (5) by multiple micro-lifes of single chamber air cathode
Thing fuel cell series forms.
Method: be seeded to by anaerobic sludge in container (11), MFC water inlet is waste water or people
Work simulated wastewater, tames, and constantly changes water, until the voltage stabilization produced；By two blocks of electricity
Pole plate (8) inserts in SBR sewage sludge reactor, connects microbiological fuel cell group (5), SBR
After reactor has been intake, liquid level need to be higher than battery lead plate；Sbr reactor device uses activated sludge work
Skill is with sequencing batch operation, i.e. through fill phase, aeration phase, subsidence stage, bleeding stage,
It is once a cycle that four stages were sequentially completed.
MFC can be converted into electric energy Organic substance degradable in waste water, but it produces electricity relatively
Little；Although traditional activated sludge process operating cost is relatively low but process effect to the PPCPs of trace
The most little, after the present invention couples MFC with activated Sludge System, the electric field the highest by these,
Add in activated Sludge System, it is possible to some traces in effective removal waste water, the most highly toxic
PPCPs.Along with going deep into of research, the raising of MFC electricity generation performance, this technology theory and practicality
Value all will highlight.
Preferred pin is not less than 1V to oxytetracycline, the voltage of MFC.
The invention have the advantages that
The electric field of MFC output is coupled by the present invention with activated Sludge System, effectively raises
To the removal of PPCPs in water body, compared with traditional activated sludge process, at other treatment effects
In the case of basically identical, the PPCPs of higher concentration can be tolerated；And with other electrochemistry sides
Method is compared, and maximum advantage is not required to additionally consume electric energy exactly, will be had by MFC in waste water
Machine thing is converted into electric energy, adds activated Sludge System by battery lead plate, by the organic contamination of trace
Thing is removed, and improves effluent quality, and the most also the utilization for MFC provides an approach.
The mud of traditional activated Sludge System (in the case of the most not powered) can produce substantial amounts of
Filamentous bacteria, mud is difficult to settle, and technique is difficult to run.Observe under microorganism scanning electron microscope, micro-
Biofacies such as Fig. 3, has substantial amounts of filamentous bacteria to produce.And bio electrochemistry process system of the present invention
Oxytetracycline clearance be maintained at more than 95%, hyphomycetic expansion can be suppressed after powering up,
Activated sludge can normally be settled, and microorganism electromicroscopic photograph is shown in Fig. 4.Bio electrochemistry work
Process system is adapted to higher oxytetracycline load.
Accompanying drawing explanation
Fig. 1 is the process schematic representation of patent of the present invention；
Fig. 2 is microbiological fuel cell schematic diagram；
Fig. 3 is microorganism electromicroscopic photograph in traditional activated sludge process；
Fig. 4 is microorganism electromicroscopic photograph in biological electrochemical process system；
Fig. 5 is the embodiment 1 waste water COD clearance containing different oxytetracycline concentration；
Fig. 6 is the embodiment 1 ammonia nitrogen in waste water clearance containing different oxytetracycline concentration；
Fig. 7 is the embodiment 1 waste water nitrogen removal rate containing different oxytetracycline concentration；
Fig. 8 is the embodiment 1 waste water oxytetracycline clearance containing different oxytetracycline concentration；
Fig. 9 is the embodiment 2 waste water COD clearance containing different COD concentration；
Figure 10 is the embodiment 2 ammonia nitrogen in waste water clearance containing different COD concentration；
Figure 11 is the embodiment 2 waste water nitrogen removal rate containing different COD concentration；
Figure 12 is the embodiment 2 waste water oxytetracycline clearance containing different COD concentration；
Figure 13 is the waste water COD clearance that should stay the time in the different water of embodiment 3；
Figure 14 is should to stay time ammonia nitrogen in waste water clearance in the different water of embodiment 3；
Figure 15 is should to stay time waste water nitrogen removal rate in the different water of embodiment 3；
Figure 16 is should to stay time waste water oxytetracycline clearance in the different water of embodiment 3.
1 elevated tank, 2 first valves, 3SBR reactor, 4 mud valves, 5 Microbial fuel electricity
Pond group, 6 wires, 7 titanium silks, 8 battery lead plate 9 anodes, 10 negative electrodes, 11 containers, 12 change water
Mouth, 13 air compressors, 14 gas flowmeters, 15 second valves, 16 aeration heads.
Detailed description of the invention
Below in conjunction with embodiment, the invention will be further described, but the present invention is not limited to following
Embodiment.Device is shown in Fig. 1.
MFC startup domestication is cultivated after producing electric stablizing, and within every 12 hours, changes a simulated wastewater,
3 stable MFC are together in series, and series voltage is connected by wire and titanium silk after reaching 1V
Battery lead plate is (after SBR sewage sludge reactor stable operation and do not accessing microbiological fuel cell group
When 5, the resistance recorded between two electrode plate 8 with circuit tester is about 900 Ω, battery lead plate
Material is graphite, and one side effective area is 3cm × 4cm, and thickness is 0.4cm, before use
After washing, alkali cleaning, pickling, coarse with sand papering.Insert SBR sewage sludge reactor
In, polar plate spacing is 2cm, and after having intake, liquid level need to be higher than battery lead plate.Connect SBR
Reactor use activated sludge process with sequencing batch operation, i.e. through fill phase, aeration phase,
Subsidence stage, bleeding stage, it is once a cycle that four stages were sequentially completed.Water inlet is for manually to join
The simulated wastewater containing low concentration oxytetracycline of system.Every day or every two days, discharge once remained dirt
Mud, holding sludge concentration is 3000-4000mg/L, controls aeration intensity, and holding dissolved oxygen amount is
About 2mg/L.
Below it is not powered on referring at identical conditions, selects microbiological fuel cell group 5 not connect
Enter sbr reactor device.Negative electrode and the anode material of each microbiological fuel cell are carbon cloth,
Anode carbon cloth has loaded 1.6mg/cm2CNT, negative electrode carbon cloth scribbles 0.25mg/cm2Platinum and
4 layers of polytetrafluoroethylene (PTFE), experimental strain is taken from sewage treatment plant's anaerobic sludge, is being detested
As seed sludge after dextrose broth domestication is cultivated under the conditions of oxygen.After producing electric stablizing,
Have a rest operation.
Wherein MFC water inlet main component:
Sbr reactor device is cylindrical, a diameter of 10cm, a height of 10cm, muddy water mixing during high water level
Liquid amasss as 400mL, and during low water level, volume is 150mL.
Embodiment 1
Manual simulation waste water with glucose as carbon source, influent COD is 574 ± 52mg/L, ammonia
Nitrogen is 30mg/L, and phosphorus is 6mg/L, and oxytetracycline is 0.5mg/L-3mg/L, 250ml of intaking
After, aeration 5 and a half hours, keeping the dissolved oxygen in reactor is about 2mg/L, precipitation
After half an hour, water outlet, i.e. hydraulic detention time are 9.6h, enter next cycle.Due to micro-life
Thing is required for adapting to for some time for different process conditions, so for every kind of work
Condition the most at least needs to stablize more than 5 days, the most continuously monitoring 4-6 the cycle of effluent quality.
Its experimental result data is shown in accompanying drawing 5-8, from above figure can be seen that oxytetracycline concentration from
0.5mg/L changes to 3mg/L, bioelectrochemical system and traditional activated Sludge System water outlet
COD clearance more than 90%, ammonia nitrogen average removal rate is all more than 85%.It is right to illustrate
Microorganism can adapt to the waste water of the oxytetracycline containing low concentration, and keeps mud well to live
Property.And, along with oxytetracycline concentration increases, the clearance of traditional active sludge system COD
Can slightly raise and reach a peak value at 1.5mg/L and 2.5mg/L respectively.Can deduce certain
The oxytetracycline of concentration stimulates microbial metabolism.When adding the concentration of oxytetracycline more than 0.5mg/L
Time, the oxytetracycline clearance of bioelectrochemical system improves than traditional activated Sludge System
5-10%, and the clearance of bioelectrochemical system oxytetracycline of the present invention is more than 97%,
The water outlet oxytetracycline clearance in some cycle can reach more than 99%.When the concentration of oxytetracycline increases
To 2.5mg/L, traditional activated Sludge System filamentary discharges, settling property extreme difference.COD,
Ammonia nitrogen, the clearance of total nitrogen has risen and has become positive correlation, can deduce all of nutrient
Matter is all used to synthesize filamentous bacteria thalline, and filamentous bacteria forms the bacterium of diameter several millimeters to a centimetre
Group, and smooth in appearance, glossy, thus it is speculated that they bondings to be made agglomerating for hyphomycetic secretions.
As can be seen from Figure 3, for traditional activated Sludge System water inlet oxytetracycline concentration more than 2mg/L
Time, sludge bulking will be produced, substantial amounts of filamentous bacteria occurs, mud is difficult to settle down, work
Skill is difficult to continue to run with.And for bioelectrochemical system, the clearance of oxytetracycline is all 97%
Above.When oxytetracycline concentration of intaking is 3mg/L, the average removal rate of oxytetracycline can reach
98.5%.Illustrate that bioelectrochemical system has good treatment effect to the oxytetracycline of low concentration,
And oxytetracycline load can be deduced and can also improve further, can preferably adapt to various waste water special
It not containing the material that microorganism is had inhibitory action.
Embodiment 2
COD in simulated wastewater, being mainly made up of a part two parts is glucose, another portion
It is divided into oxytetracycline.It is known that glucose is degradable Organic substance, can be easy to micro-
Biological utilisation.Although and oxytetracycline concentration is relatively low, but microorganism being had inhibitory action.In experiment
The concentration of water inlet oxytetracycline is fixed as 2mg/L, and the COD value changed all is contributed by glucose.
Other conditions are the most same as in Example 1.
Its experimental result, is shown in accompanying drawing 9-12, from the graph it can be seen that influent COD is from 400mg/L
Changing to 1200mg/L, the COD of bioelectrochemical system and traditional active sludge system is average
Clearance is all more than 90%.Ammonia nitrogen removal frank is all more than 70%, along with influent COD
Rising, the removal efficiency of ammonia nitrogen declines.When glucose is the most sufficient, microorganism is readily available
These degradable substrate, can consume oxygen in a large number.Competitive relation, nitrification is formed with nitrobacteria
Process can be affected, and ammonia nitrogen removal efficiency can reduce.Going of bioelectrochemical system oxytetracycline
Except rate improves 8-16%, going of bioelectrochemical system oxytetracycline than traditional activated Sludge System
Except rate is held at more than 94%.When COD is more than 400mg/L, the soil of traditional sludge system
Mycin clearance maintain 87% after downward trend.Show when in system when degradable substrate
As, during glucose abundance, the utilization rate of activated sludge difficult degradation this kind of to oxytetracycline substrate can drop
Low.When COD is 400mg/L, there is filamentary discharges in traditional activated Sludge System.
The clearance of oxytetracycline can reduce, and this shows when degradable substrate is inadequate, microbes profit
With this kind of material that microorganism is had inhibitory action of oxytetracycline.But this kind of thing to there being inhibitory action
Matter, can cause the change of microbial morphology and group, thus affect treatment effect.
Embodiment 3
The hydraulic detention time impact on treatment effect, other are same as in Example 1；Its experiment
Data are shown in accompanying drawing 13-16, it can be seen that under different hydraulic detention times, COD puts down
All clearances are all more than 90%.Along with hydraulic detention time rises, the removal efficiency of ammonia nitrogen is first
More than 80% it is held at after rising.The clearance ratio of bioelectrochemical system oxytetracycline is traditional
Activated Sludge System improve 9-25%, the clearance of bioelectrochemical system oxytetracycline 85% with
On.When hydraulic detention time is 9.6, traditional activated Sludge System and bioelectrochemical system
Oxytetracycline clearance difference minimum.When hydraulic detention time continues to increase, oxytetracycline
Clearance also will not raise again.
Claims (4)
1. microbiological fuel cell coupling electrolysis unit, it is characterised in that at least include elevated tank (1),
First valve (2), sbr reactor device (3), mud valve (4), microbiological fuel cell group (5), wire
(6), titanium silk (7), battery lead plate (8), elevated tank (1) is by valve (2) and sbr reactor device (3)
Water inlet connection, yin, yang the two poles of the earth of microbiological fuel cell group (5) are respectively through wire (6), titanium silk (7)
Being connected with two electrode plate (8), battery lead plate (8) inserts in sbr reactor device (3), two electrode plate (8)
Largest face parallel relatively and keep certain distance, after sbr reactor device (3) has been intake, liquid level need to be higher than
Battery lead plate (8), sbr reactor device (3) bottom is additionally provided with aeration head (16), and air compressor (13) leads to
Cross gas flowmeter (14) and the second valve (15) is connected with aeration head (16), sbr reactor device (3)
It is provided with mud valve (4)；
Wherein microbiological fuel cell group (5) is single chamber air cathode microbial fuel cell, and single chamber air is cloudy
Atomic biological fuel cell includes anode (9), negative electrode (10), container (11), and its Anodic (9) is positioned at
In container (11), negative electrode (10) is the sidewall of container (11), side, outside directly and air contact,
It is provided with between anode (9), negative electrode (10) and changes the mouth of a river (12).
2. couple electrolysis unit according to the microbiological fuel cell described in claim 1, it is characterised in that micro-
Biological fuel cell group (5) is in series by multiple single chamber air cathode microbial fuel cells.
3. utilize the device described in claim 1 or 2 to process the process of PPCPs, it is characterised in that
Being seeded to by anaerobic sludge in container (11), MFC water inlet is waste water or manual simulation waste water, tames,
Constantly change water, until the voltage stabilization produced；Two electrode plate (8) are inserted in SBR sewage sludge reactor,
Connecting microbiological fuel cell group (5), after sbr reactor device has been intake, liquid level need to be higher than battery lead plate；SBR
Reactor employing activated sludge process is with sequencing batch operation, i.e. through fill phase, aeration phase, sedimentation rank
Section, bleeding stage, it is once a cycle that four stages were sequentially completed.
4. according to the method for claim 3, it is characterised in that for oxytetracycline, the voltage of MFC is not less than 1V.
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