CN106957102A - A kind of girdle type biological membrane electrode electrochemical appliance and its application - Google Patents
A kind of girdle type biological membrane electrode electrochemical appliance and its application Download PDFInfo
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- CN106957102A CN106957102A CN201710257355.2A CN201710257355A CN106957102A CN 106957102 A CN106957102 A CN 106957102A CN 201710257355 A CN201710257355 A CN 201710257355A CN 106957102 A CN106957102 A CN 106957102A
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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
- C02F3/00—Biological treatment of water, waste water, or sewage
- C02F3/30—Aerobic and anaerobic processes
- C02F3/301—Aerobic and anaerobic treatment in the same reactor
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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
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- H—ELECTRICITY
- H01—ELECTRIC ELEMENTS
- H01M—PROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
- H01M8/00—Fuel cells; Manufacture thereof
- H01M8/16—Biochemical fuel cells, i.e. cells in which microorganisms function as catalysts
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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
- C02F2101/10—Inorganic compounds
- C02F2101/16—Nitrogen compounds, e.g. ammonia
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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
- C02F2101/10—Inorganic compounds
- C02F2101/20—Heavy metals or heavy metal compounds
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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
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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
- C02F2103/00—Nature of the water, waste water, sewage or sludge to be treated
- C02F2103/20—Nature of the water, waste water, sewage or sludge to be treated from animal husbandry
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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
- C02F2203/00—Apparatus and plants for the biological treatment of water, waste water or sewage
- C02F2203/006—Apparatus and plants for the biological treatment of water, waste water or sewage details of construction, e.g. specially adapted seals, modules, connections
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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
- 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
Abstract
The invention provides a kind of girdle type biological membrane electrode electrochemical appliance and its application, device includes cylindrical reaction chamber：The girdle type membrane electrode inside reative cell is arranged at, girdle type membrane electrode includes anode, barrier film and the negative electrode contacted successively；Reative cell is divided into anode chamber and cathode chamber by girdle type membrane electrode；Cathode surface adheres to alga-bacteria biofilm；Anode surface adheres to electrically-active bacterium biomembrane；The annular fixed frame of fixed girdle type membrane electrode；It is arranged at the anode posts of anode compartment；It is arranged at the cathode separator inside cathode chamber；It is arranged at the anode clapboard of anode compartment；Anode chamber bottom, which is provided with the top of anode water inlet, anode chamber, is provided with anode delivery port；Provided with the negative electrode water inlet communicated with anode delivery port at the top of cathode chamber, cathode chamber bottom is provided with negative electrode delivery port；The adjustable resistor and potentiostat being connected with cathode and anode.The device integrated level is high, and energy consumption and operating cost are low, and can strengthen organic pollution, nitrogen compound and heavy metal in removal breeding wastewater.
Description
Technical field
The present invention relates to bioelectrochemistry and field of environment engineering technology, more particularly to a kind of girdle type biological membrane electrode electricity
Chemical devices and its application.
Background technology
With economic fast development and the continuous improvement of living standard, demand of the people to food such as meat, milk, eggs
It is growing day by day so that thus livestock and poultry breeding industry causes to produce substantial amounts of livestock and poultry towards intensive and scale direction fast development
Breeding wastewater.Livestock breeding wastewater is a kind of typical high nitrogenous organic wastewater, simultaneously containing a certain amount of antibiotic and a huge sum of money
Belong to ion, serious environmental pollution will be caused by being discharged into environment, threaten ecological safety and human health.
At present, it is common to use good/anaerobic microbial conversion (A/O techniques) handles breeding wastewater.Spread out based on this principle
Raw technology mainly includes：Oxidation pond, oxidation ditch, UASB and SBR methods etc., these technologies are each in terms of livestock breeding wastewater is handled
Tool advantage, but not high there is also treatment effeciency, the defect such as floor space is big, energy consumption and operating cost height.
In recent years, bioelectrochemistry technology shows great application potential in field of waste water treatment, its distinctive cathode and anode
Bioelectrochemistry environment provides diversified approach and condition for the removal of each pollutant and recycling in waste water.In view of raw
Thing electrochemical techniques production capacity is relatively low, is at present generally combined it for handling waste water with traditional good/Anaerobic Biotechnology.Build
Integration degree height, the small area that takes up space, energy consumption and operating cost it is low and be easy to amplification application system and device be promote life
The key of thing electrochemical techniques practical application.
The content of the invention
In view of this, it is an object of the invention to provide a kind of girdle type biological membrane electrode electrochemical appliance and its application,
The electrochemical appliance integrated level is high, and the position that takes up space is small, and can strengthen the organic pollution and ammonia nitrogen removed in breeding wastewater.
The invention provides a kind of girdle type biological membrane electrode electrochemical appliance, include the reative cell of cylinder：
The girdle type membrane electrode inside the reative cell is arranged at, the girdle type membrane electrode includes the sun contacted successively
Pole, barrier film and negative electrode；Reative cell is divided into anode chamber and cathode chamber by the girdle type membrane electrode；Anode is anode chamber's locular wall；It is cloudy
Extremely cathode chamber locular wall；
The cathode surface adheres to photosynthetic helotisn biomembrane；
The anode surface adheres to electroactive bacterial biof iotalm；
The annular fixed frame of fixed girdle type membrane electrode；
It is arranged at the anode posts of the anode compartment；
The cathode separator inside the cathode chamber is arranged at, one end of cathode separator is contacted with reative cell, and relative is another
End and cathode contacts；
The anode clapboard of the anode compartment is arranged at, one end of anode clapboard is contacted with anode posts, and relative is another
End and positive contact；
The anode chamber bottom is provided with the top of anode water inlet, the anode chamber and is provided with anode delivery port；
Provided with the negative electrode water inlet communicated with anode delivery port at the top of the cathode chamber, the cathode chamber bottom is provided with negative electrode
Delivery port；
The adjustable resistor and potentiostat being connected in a series arrangement with the negative electrode and anode.
Preferably, the negative electrode is carbon felt or foam metal net.
Preferably, the also negative electrode conductive metal ring with negative electrode equivalent diameter and with latch including being arranged at cathode internal；
Also include the anode conducting becket with anode equivalent diameter and with latch for being arranged at anode interior.
Preferably, the anode surface sets anodic coating, and the anodic coating includes conductive material, amboceptor and metallization
One or more in compound.
Preferably, the cathode surface sets cathode, and the cathode includes conductive material, amboceptor and metallization
One or more in compound.
Preferably, the anode clapboard is semicircle；The cathode separator is semicircle.
Preferably, the anode water inlet is located at anode clapboard both sides with anode delivery port；The negative electrode water inlet and the moon
Pole delivery port is located at cathode separator both sides.
Preferably, the cathode separator and anode clapboard be in the same plane.
The invention provides girdle type biological membrane electrode electrochemical appliance processing cultivation described in a kind of above-mentioned technical proposal is useless
The method of water, comprises the following steps：
Pending breeding wastewater is entered into anode chamber from anode water inlet, the anode surface adheres to electroactive bacterium life
Thing film, reaction, obtains anolyte；
The anolyte is delivered to negative electrode water inlet by anode delivery port and enters cathode chamber, the cathode surface attachment
Under the separately-driven bioelectrochemistry effect of photosynthetic helotisn biomembrane, in the daytime algae light reaction, and night potentiostat
Waste water after to processing.
Preferably, the voltage of the potentiostat is 0.1~1.2V.
The invention provides a kind of girdle type biological membrane electrode electrochemical appliance, include the reative cell of cylinder：It is arranged at
Girdle type membrane electrode inside the reative cell, the girdle type membrane electrode includes anode, barrier film and the negative electrode contacted successively；Institute
State girdle type membrane electrode and reative cell is divided into anode chamber and cathode chamber；Anode is anode chamber's locular wall；Negative electrode is cathode chamber locular wall；Institute
State cathode surface and adhere to photosynthetic helotisn biomembrane；The anode surface adheres to electroactive bacterial biof iotalm；Fixed girdle type
The annular fixed frame of membrane electrode；It is arranged at the anode posts of the anode compartment；It is arranged at the negative electrode inside the cathode chamber
Dividing plate, one end of cathode separator is contacted with reative cell, the relative other end and cathode contacts；It is arranged at the anode compartment
Anode clapboard, one end of anode clapboard is contacted with anode posts, the relative other end and positive contact；The anode chamber bottom is provided with
Anode delivery port is provided with the top of anode water inlet, the anode chamber；It is provided with what is communicated with anode delivery port at the top of the cathode chamber
Negative electrode water inlet, the cathode chamber bottom is provided with negative electrode delivery port；With the negative electrode and anode be connected in a series arrangement it is adjustable
Resistor and potentiostat.The device that the present invention is provided is designed using disc, and just bioelectrochemistry principle has with A/O techniques
Highly integrated, configuration compact is imitated, is taken up space small；Dividing plate is set in cathode chamber, anode chamber respectively and in dividing plate both sides upper and lower side
Opening design makes sewage be flowed in a ring along reative cell, is fully contacted with girdle type biological membrane electrode surface, realizes in waste water
The gradient of pollutant and efficiently removal；Aerobic negative electrode aeration is eliminated by introducing photosynthetic algae in cathode chamber, and it is cloudy to combine annular
Pole room is designed to be coordinated with annular negative electrode, realizes that negative electrode algae 360 degrees omnidirection receives illumination, phycomycete is strengthened in high-efficiency photosynthetic oxygen supply
Cooperate with aerobic degradation pollutant；Meanwhile, apply voltage, reinforcing negative electrode, Anode using miniature low-power potentiostat at night
Thing electrochemical process, realizes that whole day continues and Effec-tive Function.The present invention is applied to processing breeding wastewater, can effectively remove simultaneously useless
Organic matter and nitrogen-containing compound in water, and antibiotic and heavy metal.Test result indicate that：Device COD clearances are up to
92.7%, NH3- N clearances are up to 85.4%, NO3- N clearances are up to 92.8%, and terramycin removal efficiency is up to 93.7%,
Cu2+Removal efficiency is up to 92.5%.
Brief description of the drawings
The positive structure diagram for the girdle type biological membrane electrode electrochemical appliance that Fig. 1 provides for the present invention；
The overlooking the structure diagram for the girdle type biological membrane electrode electrochemical appliance that Fig. 2 provides for the present invention.
Embodiment
The invention provides a kind of girdle type biological membrane electrode electrochemical appliance, include the reative cell of cylinder：
The girdle type membrane electrode inside the reative cell is arranged at, the girdle type membrane electrode includes the sun contacted successively
Pole, barrier film and negative electrode；Reative cell is divided into anode chamber and cathode chamber by the girdle type membrane electrode；Anode is anode chamber's locular wall；It is cloudy
Extremely cathode chamber locular wall；
The cathode surface adheres to photosynthetic helotisn biomembrane；
The anode surface adheres to electroactive bacterial biof iotalm；
The annular fixed frame of fixed girdle type membrane electrode；
It is arranged at the anode posts of the anode compartment；
The cathode separator inside the cathode chamber is arranged at, one end of cathode separator is contacted with reative cell, and relative is another
End and cathode contacts；
The anode clapboard of the anode compartment is arranged at, one end of anode clapboard is contacted with anode posts, and relative is another
End and positive contact；
The anode chamber bottom is provided with the top of anode water inlet, the anode chamber and is provided with anode delivery port；
Provided with the negative electrode water inlet communicated with anode delivery port at the top of the cathode chamber, the cathode chamber bottom is provided with negative electrode
Delivery port；
The adjustable resistor and potentiostat being connected in a series arrangement with the negative electrode and anode.
Referring to Fig. 1 and Fig. 2, the structure of facing for the girdle type biological membrane electrode electrochemical appliance that Fig. 1 provides for the present invention is shown
It is intended to；The overlooking the structure diagram for the girdle type biological membrane electrode electrochemical appliance that Fig. 2 provides for the present invention.Wherein, 1 is annulus
Formula membrane electrode, 2 be anode, and 3 be negative electrode, and 4 be barrier film, and 5 be ring-like fixed frame, 6 is conductive metal ring, 7 is anode posts, 8 be sun
Pole dividing plate, 9 be anode water inlet, and 10 be anode delivery port, and 11 be cathode separator, and 12 be negative electrode water inlet, and 13 be negative electrode water outlet
Mouthful, 14 be adjustable resistor, and 15 be potentiostat.
The electrochemical appliance that the present invention is provided includes the reative cell of cylinder, the outer wall of the reative cell for light transmittance it is strong,
Corrosion-resistant and easy to process pmma material is made.In a particular embodiment of the present invention, the reative cell is that printing opacity is good
And the annular outer shell that pmma material easy to process makes, volume is 3.14L.
It is arranged at the girdle type membrane electrode 1 inside the reative cell.In the present invention, the girdle type membrane electrode include according to
Anode 2, barrier film 4 and the negative electrode 3 of secondary contact；Negative electrode is cathode chamber locular wall.By the integrated girdle type membrane electrode by reative cell
It is divided into anode chamber and the cathode chamber of donut.It is respectively anode and negative electrode, the sun inside and outside the girdle type membrane electrode
Pole 2 is flexible, porous and corrosion resistant conductive material；Anode is anode chamber's locular wall；Specifically, the anode 2 is preferably carbon felt
Or foam metal net.It is electroactive in the electroactive bacterial biof iotalm of the surface attachment of anode 2, the electroactive bacterial biof iotalm
Bacterium includes the anaerobism heterotroph of complicated organic matter and anaerobic oxidation organic matter in degradable breeding wastewater and produces electronics and transmit
Electro-chemical activity bacterium to electrode；In order to strengthen electroactive bacterial biof iotalm and electron transmission, the preferred modified anode of anode surface
Coating, the anodic coating includes the one or more in conductive material, amboceptor and metallic compound；The anodic coating can
Increase the surface area of anode and the electric conductivity of increase anode；The conductive material is preferably graphene film, polypyrrole film or polyphenyl
Amine film；The amboceptor coating is preferably selected from anthraquinone analog compound and/or transition metal.The anodic coating can be single conduction
Material coating, or single amboceptor coating, or single metal compound coatings, or three are layering coating, or three's mixing is even
Matter coating.The present invention adheres to electroactive bacterial biof iotalm again after anode is modified.The electrochemical appliance that the present invention is provided is excellent
Choosing includes conductive metal ring 6, and the conductive metal ring is divided into anode conducting becket and negative electrode conductive metal ring.In order to strengthen receipts
Collect anode current release, reduce dispersing electrode area and reduction contact resistance, preferably set straight on an equal basis with anode in anode interior
Footpath and the anode conducting becket with latch；Latch on the anode conducting becket is preferably set in equally spaced manner；
The anode conducting becket has excellent corrosion resistance.The anode conducting becket by corrosion resistant metal wire with can
Adjust resistor to be connected and constitute loop.
The negative electrode 3 is flexible, porous and corrosion resistant conductive material, is shaped as annular；Negative electrode is cathode chamber locular wall；Institute
It is preferably carbon felt or or foam metal net to state negative electrode 3.The cathode surface adheres to photosynthetic helotisn biomembrane, the photosynthetic algae
Bacterium in bacterium symbiont film preferably includes hydrogen reduction bacterium, heavy metal reducing bacteria, nitrifier, denitrifying bacterium and Degradation of Antibiotics
Bacterium.In order to strengthen helotisn biomembrane overlay film and catalysis oxygen and nitrate reduction, the surface of negative electrode 3 is preferably provided with cathode,
The cathode includes the one or more in conductive material, amboceptor and metallic compound；The cathode can increase
Cathodic surface area.The cathode can be single conductive material coating, or single amboceptor coating, or single metallic compound
Coating, or three are layering coating, or three mixes homogeneous coating.The present invention adheres to photosynthetic algae again after negative electrode is modified
Bacterium symbiont film.Cathode electronics release is collected in order to strengthen, dispersing electrode area and reduction contact resistance are reduced, preferably in the moon
It is extremely internal to set and anode equivalent diameter and the negative electrode conductive metal ring with latch；Latch on the negative electrode conductive metal ring is excellent
Choosing is set in equally spaced manner；The negative electrode conductive metal ring has excellent corrosion resistance.The negative electrode conductive metal ring
It is connected by corrosion resistant metal wire with adjustable resistor and constitutes loop.In a particular embodiment of the present invention, the reative cell
Shell be made by transparent organic glass, add annular negative electrode so that cathode electrode surface can 360 degree fully receive illumination, have
Effect promotes the photoreactivity energy of negative electrode, so that the bioelectrochemistry reinforcing of integral lifting apparatus removes the effect of Pollutants in Wastewater
Energy.
In the present invention, the anode and negative electrode are discoid, the highly integrated integration of concentric circles, are taken up space small.
In the present invention, the barrier film 4 can be by ion, and the barrier film is preferably selected from cation-exchange membrane, milipore filter
Or microfiltration membranes.Barrier film 4 is used to separate cathode chamber and anode chamber, it is to avoid catholyte, anolyte mixing.
The electrochemical appliance that the present invention is provided includes the annular fixed frame 5 of fixed girdle type membrane electrode；The annular is solid
Determining the material of framework has corrosion resistance.The annular fixed frame 5 of the girdle type membrane electrode is made using lucite, is made
Clip type, sandwich barrier film.
The electrochemical appliance that the present invention is provided includes being arranged at the anode posts 7 of the anode compartment；The anode posts are
Annular, for fixed anode dividing plate 8 and make anode water inlet flow in a ring.
The electrochemical appliance that the present invention is provided includes being arranged at the cathode separator 11 inside the cathode chamber, cathode separator
One end is contacted with reative cell, the relative other end and cathode contacts；It is arranged at the anode clapboard 8 of the anode compartment, anode
One end of dividing plate is contacted with anode posts, the relative other end and positive contact.The material of the anode clapboard 8 and cathode separator 11
For corrosion-resistant material；The anode clapboard 8 and cathode separator 11 are preferably in the same plane.Cathode separator is set in cathode chamber
It is waste water is flowed in a ring in each reative cell with setting anode clapboard purpose in anode chamber, so that Pollutants in Wastewater
Effectively in gradient, fully it can contact and act on electrode surface microorganism, and be able to efficiently remove
In the present invention, the anode chamber bottom is provided with the top of anode water inlet 9, the anode chamber and is provided with anode delivery port
10.Anode chamber's water inlet is preferably set by anode clapboard, is opened in order that obtaining pending waste water from the anode chamber of cylinder
Head flowing, increases circulation distance, increase waste water and electrode surface biofilm contact time, strengthens Pollutants in Wastewater to greatest extent
Removal effect.
In the present invention, provided with the negative electrode water inlet 12 communicated with anode delivery port, the negative electrode at the top of the cathode chamber
Room bottom is provided with negative electrode delivery port 13；
In the present invention, the electrochemical appliance includes the adjustable resistance being connected in a series arrangement with the negative electrode and anode
Device 14 and potentiostat 15.In the present invention, the potentiostat 15 accesses circuit at night in a series arrangement, and voltage control exists
0.1~1.2V.
Pending breeding wastewater enters anode chamber by the water inlet 9 through cathode chamber, and current are under the barrier of anode clapboard 8
Flowed in anti-clockwise loops for example, the top-end water-outlet mouthful 10 on the right side of the anode clapboard of the water outlet after processing flows out, via positioned at negative electrode every
The water inlet 12 of the right hand top of plate 11 enters cathode chamber, and annularly flow, and the anolyte after processing is from positioned at the right side of cathode separator 11
The delivery port 13 of side roof part flows out；In running, circuital current, control negative electrode, sun can be adjusted by adjusting outer meeting resistance 14
Pole bioelectrochemistry reaction rate.At night, voltage, reinforcing negative electrode, anode bioelectrochemistry can be applied by potentiostat 15
Process.
In the present invention, the cathode surface adheres to photosynthetic helotisn biomembrane and anode surface attachment is electroactive
Bacterial biof iotalm tames what is obtained by the following method：
Using the microorganism in breeding wastewater as the microbionation source of anode and negative electrode, while being added in cathode chamber photosynthetic
Green alga, anode chamber's sealing, cathode chamber applies continuous artificial light source (5000lux), in continuous stream and hydraulic detention time 24 hours
Under the conditions of starter.Observe the growth conditions of negative electrode algae, test dissolved oxygen concentration, at the same using data acquisition unit monitor it is cloudy,
Voltage between positive the two poles of the earth, when voltage is stepped up to stable voltage, shows the electroactive bacterial biof iotalm of anode and negative electrode light
Helotisn biofilms domestication is closed to complete.
In the present invention, after described device is successfully started up, negative electrode starts to carry out alternately dark/light reaction according to day and night change.
In daytime, according to useless Organic substance in water and ammonia nitrogen concentration, regulation external resistance and water conservancy residence time, remove the two synchronous high-efficiency.
Night, when cathode dissolution oxygen is less than 0.5mg/L, when magnitude of voltage is reduced to the 30% of daytime burning voltage, between negative electrode, anode
Start to connect potentiostat, apply low-voltage, regulation applies voltage levels and adjustable resistor, control in the range of 0.1~1.2V
Heavy metal speed speed is reclaimed in night anode organic matter removal processed, negative electrode denitrogenation and reduction.
In the present invention, the process of said apparatus processing breeding wastewater is：
Pending breeding wastewater is entered into sun from bottom of device through cathode chamber by the anode water inlet on the right side of anode clapboard
Pole room, removes most of easily biodegradable organicses in waste water using the electroactive bacterial biof iotalm of anode surface under anaerobic,
Preliminary exposition is carried out to antibiotic type organic simultaneously；The anolyte obtained after processing is by being arranged on anode chamber top, a dividing plate left side
The anode delivery port discharge of side, then enters in cathode chamber from the negative electrode water inlet connected by pipeline, continues on through by negative electrode table
The biological film process of the helotisn in face；Based on algae caused by day and night change it is dark/light reaction makes cathode environment in replacing/anaerobism bar
Part：Daytime, the photosynthetic production oxygen of negative electrode algae provides organic in electron acceptor, the biological electrochemical degradation waste water of driving anode for negative electrode
Thing, while providing dissolved oxygen for negative electrode aerobic bacteria, promotes residual organic matter degraded, antibiotic anodic decomposition product in anode water outlet
Aerobic mineralising and ammonia nitrogen removal (Ammonia Nitrification is that nitrate+algae absorbs)；Night, negative electrode algae dark reaction, oxygen feeding stop, this
When, existing nitrate substitutes oxygen as cathode electronics acceptor using in ammoxidation generation on daytime and waste water, continues to drive anode
Organic matter in bioelectrochemistry degrading waste water, meanwhile, it is de- that nitrate receives the direct bioelectrochemistry reduction of electronics from anode
Denitrifying bacteria in nitrogen, and alga-bacteria biofilm also can anaerobic reduction nitrate denitrogenation, multipath removal nitrate.Meanwhile, give up
Heavy metal ion is also subjected to cathode electronics reduction and adsorbed in cathode surface in water, realizes the recovery of heavy metal.Due to nitric acid
Salt reduction potential is low compared with oxygen, causes the bioelectrochemistry course of reaction of night system cathode and anode to ease up, by using constant potential
Instrument applies a small voltage (0.1-1.0V) in cathode and anode can be obviously improved the biological electrochemical degradation organic matter of night anode
With cathodic reduction denitrogenation and go the efficiency of removing heavy metals.
The invention provides girdle type biological membrane electrode electrochemical appliance processing cultivation described in a kind of above-mentioned technical proposal is useless
The method of water, comprises the following steps：
Pending breeding wastewater is entered into anode chamber from anode water inlet, the anode surface adheres to electroactive bacterium life
Thing film, reaction, obtains anolyte；
The anolyte is delivered to negative electrode water inlet by anode delivery port and enters cathode chamber, the cathode surface attachment
Under the separately-driven bioelectrochemistry effect of photosynthetic helotisn biomembrane, in the daytime algae light reaction, and night potentiostat
Waste water after to processing.
Pending breeding wastewater is entered anode chamber by the present invention from anode water inlet, and the anode surface attachment is electroactive
Bacterial biof iotalm, reaction, obtains anolyte.In the present invention, in the pending breeding wastewater ammonia nitrogen concentration be preferably 50~
1000mg/L；Nitrate nitrogen concentration is preferably 50~500mg/L；Organic pollution concentration is preferred in the pending breeding wastewater
For 500~3000mg COD/L；Antibiotic mass concentration is preferably 0.01~20mg/L；Heavy metal mass concentration is preferably 1~
50mg/L。
Obtain after anolyte, the anolyte is delivered to negative electrode water inlet by anode delivery port and enters the moon by the present invention
Pole room, the cathode surface adheres to photosynthetic helotisn biomembrane, and algae light reaction in the daytime, and night potentiostat drive respectively
Bioelectrochemistry effect under handled after waste water.Daytime, the photosynthetic production oxygen of negative electrode algae provides electron acceptor for negative electrode, drives
The useless Organic substance in water of the dynamic biological electrochemical degradation of anode, while providing dissolved oxygen for negative electrode aerobic bacteria, promotes residual in anode water outlet
Staying the removal of organic matter degradation, the aerobic mineralising of antibiotic anodic decomposition product and ammonia nitrogen, (Ammonia Nitrification is that nitrate+algae is inhaled
Receive).Night, negative electrode algae dark reaction, oxygen feeding stop now, is substituted with existing nitrate in ammoxidation generation on daytime and waste water
Oxygen continues to drive the useless Organic substance in water of the biological electrochemical degradation of anode as cathode electronics acceptor, meanwhile, nitrate, which is received, to be come
Also can anaerobic reduction nitric acid from the denitrifying bacteria in electronics direct bioelectrochemistry the reduction denitrogenation, and alga-bacteria biofilm of anode
Salt denitrogenation, multipath removes nitrate.Meanwhile, heavy metal ions in wastewater is also subjected to cathode electronics reduction and adsorbed in negative electrode
Surface, realizes the recovery of heavy metal.Because nitrate reduction current potential is low compared with oxygen, cause the biological electricity of night system cathode and anode
Chemical reaction process eases up, and applying a small voltage (0.1~1.2V) in cathode and anode by using potentiostat can be notable
Lift the biological electrochemical degradation organic matter of night anode and cathodic reduction denitrogenation and the efficiency for removing removing heavy metals.
In order to further illustrate the present invention, a kind of girdle type biological membrane electrode provided with reference to embodiment the present invention
Electrochemical appliance and its application are described in detail, but they can not be interpreted as into limiting the scope of the present invention.
Embodiment 1
Using the annular outer shell (volume 3.14L) of the good and easy to process pmma material producing device of printing opacity.Ring
The annular fixed frame of belt membrane electrode is also made using lucite, makes clip type, sandwich milipore filter (10K).Adopt
With conduction active-carbon felt as yin, yang electrode, annular fixed frame both sides are fixed on.
(1) startup of device：The breeding wastewater for being derived from certain pig farm is filtered by precipitation and suitably after dilution, as
The inoculum and growth medium of cathode and anode bacterium, while adding chlorella (20% of the culture in logarithmic phase in advance in cathode chamber
Inoculation) as photosynthetic algae source, by anode top seal, negative electrode uses continuous artificial lighting (intensity 5000lux), at the same by it is cloudy,
Anode connects 1000 Europe resistance, and continues feed flow by peristaltic pump, is opened under the continuous stream operation of 12 hours water conservancy residence times
Dynamic device, the domestication electroactive biomembrane of anode and negative electrode alga-bacteria biofilm.Utilize data acquisition unit continuous acquisition cathode and anode two ends
Voltage, observes generate the continual and steady voltages of 0.48V or so after 22 days, show that device is successfully started up.
(2) operation of device：Above-mentioned piggery wastewater is replaced with into analog culture waste water (COD：1000mg/L、NH3-N：
290mg/L、NO3-N：245mg/L, terramycin：15mg/L、Cu2+：30mg/L and extra nutritional element), negative electrode is changed between using
Occult light is according to (dark/light：12:12), night applies 0.2V voltages, and other conditions are equal and startup stage.After after system run all right,
Monitor each index concentration of water-in and water-out.
Under conditions of examples detailed above setting, COD clearances are 78.6%, NH3- N clearances are 68.4%, NO3- N is removed
Rate is 71.2%, and terramycin removal efficiency is 66.9%, Cu2+Removal efficiency is 72.3%.
Example 2
On the basis of example 1, increase hydraulic detention time is 24 hours, and external resistance is reduced to 100 ohm, and night applies
Voltage increases to 0.8V, and intensity of illumination increases to 6000lux, and other conditions are equivalent.
Under conditions of examples detailed above setting, COD clearances are 83.5%, NH3- N clearances are 71.4%, NO3- N is removed
Rate is 81.8%, and terramycin removal efficiency is 75.7%, Cu2+Removal efficiency is 80.5%.
Example 3
On the basis of example 2, reduction influent load to COD：500mg/L、NH3-N：60mg/L、NO3-N：55mg/L, soil
Mycin：5mg/L、Cu2+：10mg/L, other conditions are equivalent.
Under conditions of examples detailed above setting, COD clearances are 92.7%, NH3- N clearances are 85.4%, NO3- N is removed
Rate is 92.8%, and terramycin removal efficiency is 93.7%, Cu2+Removal efficiency is 92.5%.
As seen from the above embodiment, the invention provides a kind of girdle type biological membrane electrode electrochemical appliance, including cylinder
The reative cell of shape：The girdle type membrane electrode inside the reative cell is arranged at, the girdle type membrane electrode includes what is contacted successively
Anode, barrier film and negative electrode；Reative cell is divided into anode chamber and cathode chamber by the girdle type membrane electrode；Anode is anode chamber's locular wall；
Negative electrode is cathode chamber locular wall；The cathode surface adheres to photosynthetic helotisn biomembrane；The anode surface attachment is electroactive thin
Bacterium biomembrane；The annular fixed frame of fixed girdle type membrane electrode；It is arranged at the anode posts of the anode compartment；It is arranged at institute
The cathode separator inside cathode chamber is stated, one end of cathode separator is contacted with reative cell, the relative other end and cathode contacts；Set
In the anode clapboard of the anode compartment, one end of anode clapboard is contacted with anode posts, the relative other end and positive contact；
The anode chamber bottom is provided with the top of anode water inlet, the anode chamber and is provided with anode delivery port；It is provided with the top of the cathode chamber
The negative electrode water inlet communicated with anode delivery port, the cathode chamber bottom is provided with negative electrode delivery port；With the negative electrode and anode with
The adjustable resistor and potentiostat of series system connection.The device that the present invention is provided is designed using disc, just biological electricity
The principles of chemistry and A/O technique effective depths are integrated, and configuration compact takes up space small；Dividing plate is set in cathode chamber, anode chamber respectively
It is abundant with girdle type biological membrane electrode surface and end opening design makes sewage be flowed in a ring along reative cell above and below dividing plate both sides
Contact, realizes the gradient to Pollutants in Wastewater and efficiently removal；Aerobic negative electrode is eliminated by introducing photosynthetic algae in cathode chamber
Aeration, and the annular cathode chamber design of combination and annular negative electrode cooperation, realize that negative electrode algae 360 degrees omnidirection receives illumination, efficiently
Photosynthetic oxygen supply, reinforcing phycomycete collaboration aerobic degradation pollutant；Meanwhile, apply electricity using miniature low-power potentiostat at night
Pressure, reinforcing negative electrode, anode bio-electrochemical process realize that whole day continues and Effec-tive Function.It is useless that the present invention is applied to processing cultivation
Water, can effectively remove organic matter in waste water, ammonia nitrogen, nitrate nitrogen, and antibiotic and heavy metal simultaneously.Test result indicate that：
Device COD clearances are up to 92.7%, NH3- N clearances are up to 85.4%, NO3- N clearances are up to 92.8%, and terramycin is gone
Except efficiency high is up to 93.7%, Cu2+Removal efficiency is up to 92.5%.
The above is only the preferred embodiment of the present invention, it is noted that for the ordinary skill people of the art
For member, under the premise without departing from the principles of the invention, some improvements and modifications can also be made, these improvements and modifications also should
It is considered as protection scope of the present invention.
Claims (10)
1. a kind of girdle type biological membrane electrode electrochemical appliance, includes the reative cell of cylinder：
Be arranged at the girdle type membrane electrode inside the reative cell, anode that the girdle type membrane electrode includes contacting successively, every
Film and negative electrode；Reative cell is divided into anode chamber and cathode chamber by the girdle type membrane electrode；Anode is anode chamber's locular wall；Negative electrode is the moon
Pole room locular wall；
The cathode surface adheres to photosynthetic helotisn biomembrane；
The anode surface adheres to electroactive bacterial biof iotalm；
The annular fixed frame of fixed girdle type membrane electrode；
It is arranged at the anode posts of the anode compartment；
Be arranged at the cathode separator inside the cathode chamber, one end of cathode separator is contacted with reative cell, the relative other end with
Cathode contacts；
Be arranged at the anode clapboard of the anode compartment, one end of anode clapboard is contacted with anode posts, the relative other end with
Positive contact；
The anode chamber bottom is provided with the top of anode water inlet, the anode chamber and is provided with anode delivery port；
Provided with the negative electrode water inlet communicated with anode delivery port at the top of the cathode chamber, the cathode chamber bottom is provided with negative electrode water outlet
Mouthful；
The adjustable resistor and potentiostat being connected in a series arrangement with the negative electrode and anode.
2. girdle type biological membrane electrode electrochemical appliance according to claim 1, it is characterised in that the negative electrode is carbon felt
Or foam metal net.
3. girdle type biological membrane electrode electrochemical appliance according to claim 2, it is characterised in that also including being arranged at the moon
The negative electrode conductive metal ring with negative electrode equivalent diameter and with latch inside extremely；
Also include the anode conducting becket with anode equivalent diameter and with latch for being arranged at anode interior.
4. girdle type biological membrane electrode electrochemical appliance according to claim 1, it is characterised in that the anode surface is set
Anodic coating is put, the anodic coating includes the one or more in conductive material, amboceptor and metallic compound.
5. girdle type biological membrane electrode electrochemical appliance according to claim 1, it is characterised in that the cathode surface is set
Cathode is put, the cathode includes the one or more in conductive material, amboceptor and metallic compound.
6. girdle type biological membrane electrode electrochemical appliance according to claim 1, it is characterised in that the anode clapboard is
It is semicircle；The cathode separator is semicircle.
7. girdle type biological membrane electrode electrochemical appliance according to claim 1, it is characterised in that the anode water inlet
It is located at anode clapboard both sides with anode delivery port；The negative electrode water inlet and negative electrode delivery port are located at cathode separator both sides.
8. girdle type biological membrane electrode electrochemical appliance according to claim 1, it is characterised in that the cathode separator and
Anode clapboard is in the same plane.
9. the method that girdle type biological membrane electrode electrochemical appliance described in a kind of claim 1 handles breeding wastewater, including it is following
Step：
Pending breeding wastewater is entered into anode chamber from anode water inlet, the anode surface adheres to electroactive bacterial biof iotalm
Organic pollution therefrom obtains electronics in degrading waste water, and by electron transmission to anode, while denitrification removes part in waste water
Nitrate nitrogen, anolyte after being handled；
Anolyte is delivered to negative electrode water inlet by anode delivery port and enters cathode chamber after the processing, and the cathode surface is attached
Photosynthetic helotisn biomembrane, algae light reaction in the daytime drives, and the bioelectrochemistry of night potentiostat reinforcing driving is made
With lower removal residual organic contaminants, ammonia nitrogen and nitrate nitrogen, the waste water after being handled.
10. method according to claim 9, it is characterised in that the voltage of the potentiostat is 0.1~1.2V.
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