CN106734158A - A kind of electric microfield stimulates the aerobic method and apparatus for realizing Polychlorinated biphenyls removal in bed mud of coupling negative electrode anaerobism/anode - Google Patents
A kind of electric microfield stimulates the aerobic method and apparatus for realizing Polychlorinated biphenyls removal in bed mud of coupling negative electrode anaerobism/anode Download PDFInfo
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- B09C1/00—Reclamation of contaminated soil
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- B09C1/085—Reclamation of contaminated soil chemically electrochemically, e.g. by electrokinetics
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Abstract
Stimulate the aerobic method and apparatus for realizing Polychlorinated biphenyls removal in bed mud of coupling negative electrode anaerobism/anode the invention discloses a kind of electric microfield.The device is made up of anode chamber and cathode chamber, and anode chamber and cathode chamber are separated by cation-exchange membrane；Granular graphite is evenly distributed with anode chamber and cathode chamber；The anode electrode produces oxygen material and modifies by high-performance catalysis, and the cathode electrode produces hydrogen material and modifies by high-performance catalysis.The method for realizing Polychlorinated biphenyls removal in bed mud using said apparatus includes step：（1）In bed mud of anode chamber's inoculation containing aerobic dehalogenation bacterium, low Polychlorinated biphenyls, electron donor and nutrient solution are added；（2）Mixing sludge of the inoculation containing anaerobic dechlorination bacterium in cathode chamber, adds Polychlorinated biphenyls high；（3）External circuit is connected, startup optimization device realizes anaerobic-aerobic coupled synchronous degradation PCBs.The inventive method is simple to operate, economic and practical, does not produce secondary pollution.
Description
Technical field
The present invention relates to microbial degradation of polychlorinated biphenyls technical field, and in particular to a kind of electric microfield stimulates coupling negative electrode to detest
The aerobic method and apparatus for realizing Polychlorinated biphenyls removal in bed mud of oxygen/anode.
Background technology
Polychlorinated biphenyls（Polychlorinated Biphenyls, abbreviation PCBs）It is that a class is reacted by chemical catalysis,
The chlorinated aromatic hydrocarbons compound that hydrogen atom chlorination substitution on biphenyl is generated, has 209 kinds of homologues（PCB1~PCB
209）, its chemical expression is C12H10-nCln, PCBs has the excellent physics and chemistry such as thermodynamic stability, incombustibility, chemical inertness
Property, was once widely used in the fields such as electric power processing, plastic processing, chemical industry and printing, and main commercial type includes
Aroclor, Fenclor, Kanechlor, Phenclor etc..After be found to have immunotoxicity, neurotoxicity, development toxicity and
" three cause " characteristic, PCBs is disabled and lists in《Convention of Stockholm》First batch of persistence organic pollutant（Persistent
Organic Pollutants, abbreviation POPs）List.
The removal of PCBs relies primarily on the photodegradation of ultraviolet irradiation and the enzymatic of indigenous microorganism in nature
Effect, efficiency is often very low, for example：In water the half-life period of PCBs more than two months, Soil sediment be more than six months, animal body
Inside then it is up to 1~20 year.Therefore, with PCBs as target contaminant, a kind of efficient, economic, controllable microorganism is sought strong
Change method, realizes that pollutant removal, toxicity reduction seem very necessary, also has important ginseng to the actual repair of IA soil
Examine meaning.
The process of microorganism removal PCBs include reduction dechlorination under anaerobic condition and it is aerobic under the conditions of oxidative degradation, it is high
Askarel carries out reduction dechlorination and converts to low chlorine state biphenyl under anaerobic, is then decomposed by aerobic bacteria open loop until completely
Mineralising.The biodegradation of PCBs most starts to be also that most important step is anaerobic reductive dechlorination process, therefore to soil and sinks
Product substance environment in microorganism drive anaerobic reduction process spread research it is most important, this in-situ immobilization to contaminated area soil and
Toxicity reduction has theoretical reference value and practical application potentiality.
It is more for the existing method species of PCBs pollution controls, have some limitations：Physics is burned to equipment
It is required that it is high, secondary pollution can be brought（Produce the materials such as bioxin）；Chemical catalysis need expensive catalyst, complex operation；It is micro-
It is slow and not thorough enough that biological prosthetic limitation shows as, degradation speed strong to environmental condition dependence.Even so, microorganism is repaiied
Complex phase has the advantages that environment-friendly, simple to operate, economic and practical to first two method and can carry out massive pollution treatment
And obtain extensive concern.
The content of the invention
In order to solve the shortcoming and defect part of prior art, primary and foremost purpose of the invention is to provide a kind of using micro- electricity
Field stimulates the aerobic device for realizing Polychlorinated biphenyls removal in bed mud of coupling negative electrode anaerobism/anode.
A kind of electric microfield another object of the present invention is to provide utilization said apparatus stimulates coupling negative electrode anaerobism/anode
The aerobic method for realizing Polychlorinated biphenyls removal in bed mud.
The object of the invention is achieved through the following technical solutions.
A kind of electric microfield stimulates the aerobic device for realizing Polychlorinated biphenyls removal in bed mud of coupling negative electrode anaerobism/anode, by sun
Pole room and cathode chamber are constituted, and anode chamber and cathode chamber are separated by cation-exchange membrane；The anode chamber sets galvanic anode
Filling opening and anode electrode, the cathode chamber set negative electrode filling opening and cathode electrode, and anode electrode and cathode electrode are by outer
Circuit connects external power and contactor；Granular graphite is evenly distributed with the anode chamber and the cathode chamber；The anode electricity
Pole is produced oxygen material and is modified by high-performance catalysis, and the cathode electrode produces hydrogen material and modifies by high-performance catalysis.
Further, the high-performance produces oxygen material includes transition metal oxide, multi-element metal oxide or nonmetallic
Compound.
Further, hydrogen material is produced in the high-performance catalysis includes transition metal phosphide, transition metal nitride or mistake
Cross metal carbides.
Further, the anode electrode is modified with nickel acetate.
Further, the cathode electrode is modified with ferric nitrate.
Further, the material of the anode electrode and cathode electrode is carbon paper, carbon cloth, graphite felt, stainless (steel) wire or bubble
Foam nickel.
Further, the material of the anode electrode and cathode electrode is the graphite felt by pre-processing；Graphite felt has
There are specific surface area higher, good biocompatibility and reasonable prices, be conducive to the formation of biomembrane, graphite felt is carried out
Pretreatment is conducive to improving its stability and electric conductivity.
Anode electrode is modified with nickel acetate and cathode electrode ferric nitrate is modified, and metallic nickel can be catalyzed analysis oxygen, metallic iron
Product hydrogen can be catalyzed.
Further, described pretreatment is：Graphite felt is placed in the hydrogen peroxide solution that mass fraction is 10%, in temperature
Spend for water-bath is boiled 2 hours under the conditions of 90 DEG C, then with deionized water, water-bath is boiled 2 hours at the same temperature, then uses oven for drying.
Further, by HCl treatment, granular graphite is anode in the abundance of anode chamber or cathode chamber to the granular graphite
Room or the 10% of negative electrode building volume.
A kind of electric microfield of utilization said apparatus stimulate coupling negative electrode anaerobism/anode be aerobic realize bed mud in Polychlorinated biphenyls go
The method removed, comprises the following steps：
（1）To anode chamber's inoculation by PCB9 bed muds of the domestication containing aerobic dehalogenation bacterium, add and contain PCB9（2,5-CB）Bed mud,
Add sodium acetate as electron donor, add the mixed liquor of phosphate buffer solution and nutrient solution as nutriment；
（2）Added in cathode chamber and contain PCB61（2,3,4,5-CB）Bed mud and by PCB61 domestications containing being with the PCB61 that degrades
The mixing sludge of main anaerobic dechlorination bacterium, adds the mixed liquor of phosphate buffer solution and nutrient solution as nutriment；
（3）Closed circuit is switched, and connects external circuit, startup optimization device；In running, anode electrode analysis oxygen, and it is aerobic
Dehalogenation bacterium is utilized, and PCB9 is oxidized into dichlorobenzoic acid, and the further oxide ore of dichlorobenzoic acid turns to carbon dioxide and water；Oxidation
The H of generation+Cathode chamber is entered by cation-exchange membrane, hydrogen is reduced in cathode electrode, for anaerobic dechlorination bacterium provides electricity
PCB61 is finally reduced to PCB9 by son, and PCB9 carries out mineralising into anode chamber；So realize that anaerobic-aerobic couples synchronous degradation
PCB9 and PCB61.
Further, step（1）In, in the bed mud containing PCB9, the concentration of PCB9 is 0.6 μm of ol/g.
Further, step（1）In, the bed mud containing PCB9 is added, it is necessary to add consumption water-soluble for what is formed in anode chamber
The TW80 surfactants of liquid 1g/L increase the water solubility of PCB9.
Further, step（1）In, the amount of the bed mud containing aerobic dehalogenation bacterium is the 40~50% of anode building volume.
Further, step（1）In, the addition of the sodium acetate is 10 ~ 20 of the aqueous solution of formation in anode chamber
mmol/L。
Further, step（1）、（2）In, the concentration of the phosphate buffer is 0.1 mol/L, the pH of phosphate buffer
=7.0。
Further, step（1）、（2）In, the phosphate buffer is that every liter of phosphoric acid delays with the mixed liquor proportioning of nutrient solution
Fliud flushing adds 10 mL nutrient solutions.
Further, step（1）、（2）In, the phosphate buffer is anode chamber with the addition of the mixed liquor of nutrient solution
Or the 40-52% of negative electrode building volume, preferably 50%.
Further, step（1）、（2）In, 0.1 mol of pH of the mixed liquor of the phosphate buffer and nutrient solution.L-1 H3PO4It is adjusted to 7.
Further, step（1）、（2）In, the nutrient solution composition includes：2.7 g.L-1 NaHCO3、0.5 g.L-1
K2HPO4、0.10 g.L-1 KCl、0.015 g.L-1 CaCl2、0.25 g.L-1 NH4Cl、10 mL.L-1Mineral solution and 10
mL.L-1Vitamin.
Further, the mineral solution composition includes 1.5 g.L-1 C6H6NO6·3Na·12H2O、0.13 g.L-1 ZnCl2、3.0 g.L-1 MgSO4、0.01 g.L-1 CuSO4·5H2O、0.5 g.L-1 MnSO4·H2O、0.01 g.L-1 AlK
(SO4)2·12H2O、1.0 g.L-1 NaCl、0.01 g.L-1 H3BO3、0.1 g.L-1 FeSO4·7H2O、0.025 g.L-1
Na2MoO4、0.1 g.L-1 CaCl2·2H2O、0.024 g.L-1 NiCl2·6H2O、0.1 g.L-1 CoCl2·6H2O and 0.025
g.L-1 Na2WO4·2H2O。
Further, step（2）In, in the bed mud containing PCB61, the concentration of PCB61 is 0.1 μm of ol/g.
Further, step（2）In, the bed mud containing PCB61 is added, it is necessary to it is the water formed in cathode chamber to add consumption
The TW80 surfactants of the g/L of solution 1 increase the water solubility of PCB61.
Further, step（2）In, the amount of the mixing sludge of the anaerobism dehalogenation bacterium containing based on the PCB61 that degrades
It is the 40% of negative electrode building volume.
Further, step（3）In, the voltage that external circuit applies is 1.0 ~ 2.5 V.
Principle of the invention is：By building the microorganism electrolysis cell with anode chamber and cathode chamber（MEC）, be powered operation
During, anode electrode analysis oxygen, the aerobic dehalogenation bacterium in anode chamber utilizes dioxygen oxidation 2, and 5-CB is dichlorobenzoic acid, dichloro-benzenes
The further oxide ore of formic acid turns to carbon dioxide and water；The H that anode effect is produced+By cation in the presence of concentration gradient
Exchange membrane enters negative electrode, the H in the presence of cathodic electrolytic water+Obtain electronics and produce H2, so as to be supplied as the electronics of anaerobic dechlorination bacterium
It is 2,5-CB by 2,3,4,5-CB reduction dechlorinations that body promotes anaerobic dechlorination bacterium；In this way, reach 2,3,4,5 ,-CB reduction dechlorinations and 2,
5-CB aoxidizes mineralising collective effect, makes Oxygen anodic evolution to aoxidize PCB9 and negative electrode product hydrogen reduction PCB61, forms askarel high
Carry out reduction dechlorination under anaerobic to convert to low chlordiphenyl, then low chlordiphenyl is decomposed until complete ore deposit by aerobic bacteria open loop
Change, be finally reached anaerobic-aerobic coupling synchronous degradation 2,3,4,5-CB and 2,5-CB, realize the removal of Polychlorinated biphenyls.
Compared with prior art, the invention has the advantages that and beneficial effect：（1）The present invention produces hydrogen using biological-cathode
Promote the degraded of pollutant with Oxygen anodic evolution, by microorganism electrolysis cell（MEC）With traditional microbiological degradation of polychlorinated biphenyl technology
It is combined, the purpose of the anaerobic-aerobic synchronous degradation that realization is difficult in traditional microbiological biodegrading process；Meanwhile, micro- life
Thing electrolytic cell is a kind of efficient, economic, controllable microbial augmentation method, realizes pollutant removal, toxicity reduction, there is environment
Friendly, simple to operate, economic and practical advantage；（2）In the present invention negative electrode using be electrolysed aquatic products hydrogen by the way of, on the one hand for carrying
For the electron donor needed for microbial degradation of polychlorinated biphenyls pollutant, the remaining H of another aspect2Can come real as inert gas
The cathode chamber of existing microorganism electrolysis cell keeps anaerobic state, improves the degradation rate of Polychlorinated biphenyls；
（3）The present invention strengthens microbial degradation of polychlorinated biphenyls compared to conventional physical and chemistry, can not only improve Polychlorinated biphenyls
Degradation rate, and do not produce secondary pollution, it is not necessary to expensive catalyst, overcome traditional microbiological reparation to environmental condition
Dependence is strong, degradation speed is slow and inadequate thoroughly limitation, for microorganism provides a stabilizing active condition.
Brief description of the drawings
Fig. 1 be inoculated with embodiment 1 electric microfield after bed mud stimulate coupling negative electrode anaerobism/anode it is aerobic realize it is many in bed mud
The schematic device of chlordiphenyl removal；
Fig. 2 is specific PCB9 oxidative degradation figures in the plant running process anode chamber of embodiment 1；
Fig. 3 is the change in concentration figure of 2,5- dichlorobenzoic acids in the plant running process anode chamber of embodiment 1；
Fig. 4 is the degraded figure of reduction PCB61 in the plant running process cathode chamber of embodiment 1；
Fig. 5 a are the change in concentration figure of the reduzate PCB23 of PCB61 in the plant running process cathode chamber of embodiment 1；
Fig. 5 b are the change in concentration figure of the reduzate PCB29 of PCB61 in the plant running process cathode chamber of embodiment 1；
Fig. 5 c are the change in concentration figure of the reduzate PCB9 of PCB61 in the plant running process cathode chamber of embodiment 1.
Specific embodiment
With reference to embodiment, the present invention is described in further detail, but embodiments of the present invention not limited to this.
The present embodiment of embodiment 1 use a kind of electric microfield stimulate coupling negative electrode anaerobism/anode is aerobic realize bed mud in Polychlorinated biphenyls go
Schematic diagram after the device inoculation bed mud 2 for removing as shown in figure 1, be made up of anode chamber 3 and cathode chamber 9, anode chamber 3 and cathode chamber 9
Separated by cation-exchange membrane 12, anode chamber 3 sets galvanic anode filling opening 4 and anode electrode 1, cathode chamber 9 sets the moon
Pole filling opening 8 and cathode electrode 11, anode electrode 1 and cathode electrode 11 connect external circuit power supply 7 and contactor by wire 5
6, granular graphite 10 is filled with anode chamber 3 and cathode chamber 9；
The material of anode electrode 1 and cathode electrode 11 is the graphite felt electrode by pre-processing, and preprocessing process is：By graphite
Felt is placed in the hydrogen peroxide solution that mass fraction is 10%, and water-bath is boiled 2 hours at 90 DEG C, then with deionized water in same temperature
The lower water-bath of degree is boiled 2 hours, then uses oven for drying；
Pretreated graphite felt is cut into 6.5 cm × 5 cm sizes wide long, is put on titanium silk, obtain pretreating graphite felt electricity
Pole；
The surface of pretreating graphite felt electrode is modified with nickel acetate, anode electrode is obtained；By the table of pretreating graphite felt electrode
Face is modified with ferric nitrate, obtains cathode electrode；
Assembling said apparatus：The titanium silk that pretreating graphite felt anode electrode will be connected is passed outward from anode casing aperture by interior,
The plane of graphite felt anode electrode is parallel with the plane of anode casing plate, and titanium silk is glued with anode casing aperture with AB glue, puts
Put and solidify；Cathode shell will in the same way be loaded by the graphite felt cathode electrode of pretreatment, then by cation exchange
Mould is pressed on cathode shell and cation-exchange membrane with anode casing in negative electrode room housing, then and fixed, and is finally screwed on
Screw nut；Granular graphite is filled in anode chamber and cathode chamber, loading is the 10% of anode chamber or negative electrode building volume.
Using said apparatus be used for electric microfield stimulate coupling negative electrode anaerobism/anode is aerobic realize bed mud in Polychlorinated biphenyls go
Remove, step is：
（1）To anode chamber's inoculation by bed mud of the domestication containing aerobic dehalogenation bacterium, add bed mud containing 0.6 μm of ol/g PCB9 and
Consumption is the TW80 surfactants of aqueous solution 1g/L, and the amount of the bed mud containing aerobic dehalogenation bacterium is the 40% of anode building volume；Plus
Enter the sodium acetate electron donor that consumption is the mmol/L of the aqueous solution 20；Add 0.1molL-1The phosphate buffer solution of pH 7.0 and training
The mixed liquor of nutrient solution is used as nutriment；Every liter of phosphate buffer adds 10 mL nutrient solutions, and phosphate buffer is mixed with nutrient solution
It is the 50% of anode building volume to close the addition of liquid；
The sludge that Qingyuan City dragon's pool town electronic waste disassembles place is taken from by PCB9 bed muds of the domestication containing aerobic dehalogenation bacterium,
The blue lid bottle aeration culture of 1000 mL, and be persistently aerated with oxygen pump, sludge uses the aerobic dehalogenation bacterium of PCB9 enrichment cultures；Training
The nutrient solution of foster aerobic dehalogenation bacterium and the composition of the nutrient solution for adding anode chamber are：0.1 mol L-1PBS
（PBS）, 12.7g L-1 NaHCO3、0.5g L-1 K2HPO4、0.10 g L-1 KCl、0.015 g L-1 CaCl2、0.25g L-1
NH4Cl、10 mL L-1Mineral solution and 10 mL L-1Vitamin, then with 0.1 mol L-1 H3PO4The pH of nutrient solution is adjusted
Try to be 7, wherein every liter of mineral solution composition is by 1.5 g C6H6NO6·3Na·12H2O, 0.13 g ZnCl2, 3.0 g
MgSO4, 0.01 g CuSO4·5H2O, 0.5 g MnSO4·H2O, 0.01 g AlK (SO4)2·12H2O, 1.0 g NaCl,
0.01 g H3BO3, 0.1 g FeSO4·7H2O, 0.025 g Na2MoO4, 0.1 g CaCl2·2H2O, 0.024 g NiCl2·
6H2O, 0.1 g CoCl2·6H2O and 0.025 g Na2WO4·2H2O is constituted.
（2）It is the T W80 surfaces of aqueous solution 1g/L to be added in cathode chamber containing 0.1 μm of bed mud and consumption of ol/g PCB61
Activating agent；It is inoculated with by PCB61 mixing sludges of the domestication containing the anaerobic dechlorination bacterium based on the PCB61 that degrades, it is de- containing anaerobism
The amount of the bed mud of halogen bacterium is the 40% of negative electrode building volume；Mixing sludge takes from the water that Qingyuan City dragon's pool town electronic waste disassembles place
Ditch bed mud, the cultural method of anaerobic dechlorination bacterium is identical with the cultural method of aerobic dehalogenation bacterium, and difference is to access
PCB9 changes PCB61 into, it is not necessary to aerobic aeration, and by the sealing of blue lid bottle and in 250 rad/min shaking tables, enrichment culture anaerobism takes off
Chlorine bacterium；Add 0.1molL-1The phosphate buffer solution of pH 7.0 and the mixed liquor of nutrient solution are used as nutriment；Every liter of phosphoric acid delays
Fliud flushing adds 10 mL nutrient solutions, and phosphate buffer is the 50% of anode building volume with the addition of the mixed liquor of nutrient solution；
（3）Closed circuit switch, connect external circuit, voltage be 1.0,1.5,2.0,2.5V, startup optimization device；Running
In, anode electrode analysis oxygen, and utilized by aerobic dehalogenation bacterium, PCB9 is oxidized to dichlorobenzoic acid, the further oxygen of dichlorobenzoic acid
It is carbon dioxide and water to change mineralising；Aoxidize the H for producing+Cathode chamber is entered by cation-exchange membrane, is reduced in cathode electrode
It is hydrogen, reduces PCB61 for anaerobic dechlorination bacterium provides electronics, PCB61 is reduced to PCB29, PCB23 and PCB21, goes forward side by side one
Step is reduced to PCB9, and PCB9 carries out mineralising into anode chamber；So realize anaerobic-aerobic coupling synchronous degradation PCB61 and PCB9.
Anode chamber's sterilizing contrast：Add 0.6 umol/L's in the device anode chamber containing sludge and sterilization treatment
PCB9, remaining conditional synchronization is rapid（2）, culture in 30 DEG C of constant incubators is placed on, run under 2.0V voltages；
The setting sampling time is sampled in the anode compartment in running, extracting and purifying is carried out after sampling, and use efficient liquid
The concentration of phase chromatographic quantitative analysis PCB9 and dichlorobenzoic acid；
Specific PCB9 oxidative degradations situation such as Fig. 2 in anode chamber containing aerobic dehalogenation bacterium and sterilizing, as shown in Figure 2,20 days with
Afterwards, the PCB9 in reactor starts obvious reduction, and aerobic dehalogenation bacterium has been in the rise period in illustrating at this moment reactor,
Its bioactivity also constantly strengthens, and the aerobic dehalogenation enzyme gene expression of microorganism is relatively good；Until after 100 days, due to
PCB9 degradeds are limited by dynamics and thermodynamically, and the degradation rate of PCB9 is constantly reduced.
Change in concentration containing the dichlorobenzoic acid in aerobic dehalogenation bacterium anode chamber is as shown in Figure 3.As seen from Figure 3,
PCB9 oxidation products are mainly 2,5- dichlorobenzoic acids, when reaction proceeds to 20 days, can be observed using GC-MS detection soil
To the detection peak for obvious 2,5- dichlorobenzoic acids occur, the oxygen that aerobic dechlorination microorganism is separated out by the use of anode electrode is used as electricity
Sub- acceptor aoxidizes PCB9；After reaction is carried out 80 days, it can be seen that the concentration of 2,5- dichlorobenzoic acids starts to reduce in soil,
Aerobic microbiological starts to be further CO by 2,5- dichlorobenzoic acids mineralising2, H2O and HCl.
Cathode chamber sterilizing contrast：Add 0.1 umol/L's in the device cathode chamber containing sludge and sterilization treatment
PCB61, remaining conditional synchronization is rapid（1）, culture in 30 DEG C of constant incubators is placed on, run under 2.0V voltages；
The setting sampling time is sampled in running, and the concentration of PCB61 and catabolite is then determined with GC-MS；
The degraded figure of specific PCB61 is as shown in Figure 4 in the negative electrode pole room of the bacterium of dehalogenation containing anaerobism and sterilizing.As shown in Figure 4, reaction is worked as
When proceeding to 10 days, the concentration of PCB61 starts to reduce in soil, illustrates that the amounts of hydrogen that cathode electrode is produced has reached anaerobism dehalogenation
The dehalogenation protease gene for utilizing value, microorganism of microorganism can be good at expression；After reaction proceeds to 100 days, PCB61
Degradation rate start to reduce, illustrate anaerobism dehalogenation microbial degradation PCB61 by dynamics and thermodynamic (al) limitation, PCB61
It is difficult to further be degraded；
The change in concentration of catabolite can be seen that anaerobism in cathode chamber as shown in Fig. 5 a, Fig. 5 b and Fig. 5 c by Fig. 5 a and Fig. 5 b
PCB61 is first degraded to 2,3,5-CB by dechlorination microorganism by the use of the hydrogen that cathode electrode is produced as electron donor（PCB23）And
2,4,5-CB（PCB29）；Fig. 5 c show, after 40 days, after trichloro biphenyl runs up to finite concentration in the reactor, and anaerobism dehalogenation
Microorganism just further by PCB23 and PCB29 dechlorinations be PCB9；After reaction proceeds to 100 days, anaerobism dehalogenation microorganism
Degraded PCB61 is subject to dynamics and thermodynamic (al) limitation, the degradation rate reduction of PCB61.
Above-described embodiment is the present invention preferably implementation method, but embodiments of the present invention are not by above-described embodiment
Limitation, it is other it is any without departing from Spirit Essence of the invention and the change, modification, replacement made under principle, combine, simplification,
Equivalent substitute mode is should be, is included within protection scope of the present invention.
Claims (10)
1. a kind of electric microfield stimulates the aerobic device for realizing Polychlorinated biphenyls removal in bed mud of coupling negative electrode anaerobism/anode, its feature
It is to be made up of anode chamber and cathode chamber, anode chamber and cathode chamber are separated by cation-exchange membrane；The anode chamber is set
Galvanic anode filling opening and anode electrode, the cathode chamber set negative electrode filling opening and cathode electrode, anode electrode and negative electrode electricity
Pole connects external power and contactor by external circuit；Granular graphite is evenly distributed with the anode chamber and cathode chamber；The sun
Pole electrode produces oxygen material and modifies by high-performance catalysis, and the cathode electrode produces hydrogen material and modifies by high-performance catalysis.
2. a kind of electric microfield stimulation coupling negative electrode anaerobism/anode according to claim 1 is aerobic realizes many chlorine connection in bed mud
The device of benzene removal, it is characterised in that the high-performance produce oxygen material include transition metal oxide, multi-element metal oxide or
Nonmetallic compound；Hydrogen material is produced in the high-performance catalysis includes transition metal phosphide, transition metal nitride or transition gold
Category carbide；The granular graphite is cathode chamber or anode in the abundance of anode chamber or cathode chamber by HCl treatment, granular graphite
The 8~10% of building volume.
3. a kind of electric microfield stimulation coupling negative electrode anaerobism/anode according to claim 1 is aerobic realizes many chlorine connection in bed mud
The device of benzene removal, it is characterised in that the anode electrode is the graphite felt modified with nickel acetate, and the cathode electrode is to use nitre
The graphite felt of sour iron modification；The graphite felt is the graphite felt by pre-processing, and the pretreatment is：Graphite felt is placed in quality
During fraction is 10% hydrogen peroxide solution, water-bath is boiled 2 hours under the conditions of being 90 DEG C in temperature, then with deionized water in same temperature
The lower water-bath of degree is boiled 2 hours, then uses oven for drying.
4. a kind of electric microfield based on claim 1 ~ 3 any one described device stimulates coupling negative electrode anaerobism/aerobic realization of anode
The method of Polychlorinated biphenyls removal in bed mud, it is characterised in that comprise the following steps：
（1）To anode chamber's inoculation by PCB9 bed muds of the domestication containing aerobic dehalogenation bacterium, the bed mud containing PCB9 is added, add acetic acid
Sodium adds the mixed liquor of phosphate buffer solution and nutrient solution as nutriment as electron donor；
（2）The bed mud containing PCB61 is added in cathode chamber and contains the anaerobic dechlorination based on the PCB61 that degrades by PCB61 domestications
The mixing sludge of bacterium, adds the mixed liquor of phosphate buffer solution and nutrient solution as nutriment；
（3）Closed circuit is switched, and connects external circuit, startup optimization device；In running, anode electrode analysis oxygen, and it is aerobic
Dehalogenation bacterium is utilized, and PCB9 is oxidized into dichlorobenzoic acid, and the further oxide ore of dichlorobenzoic acid turns to carbon dioxide and water；Oxidation
The H of generation+Cathode chamber is entered by cation-exchange membrane, hydrogen is reduced in cathode electrode, for anaerobic dechlorination bacterium provides electricity
PCB61 is finally reduced to PCB9 by son, and PCB9 carries out mineralising into anode chamber；So realize that anaerobic-aerobic couples synchronous degradation
PCB9 and PCB61.
5. a kind of electric microfield stimulation coupling negative electrode anaerobism/anode according to claim 4 is aerobic realizes many chlorine connection in bed mud
The method of benzene removal, it is characterised in that step（1）In, in the bed mud containing PCB9, the concentration of PCB9 is 0.6 μm of ol/g；
The bed mud containing PCB9 is added, it is necessary to add consumption for the TW80 surfactants of the aqueous solution 1g/L formed in anode chamber increase
The water solubility of PCB9；The amount of the bed mud containing aerobic dehalogenation bacterium is the 40~50% of anode building volume.
6. a kind of electric microfield stimulation coupling negative electrode anaerobism/anode according to claim 4 is aerobic realizes many chlorine connection in bed mud
The method of benzene removal, it is characterised in that step（1）In, the addition of the sodium acetate is the aqueous solution of formation in anode chamber
10~20 mmol/L.
7. a kind of electric microfield stimulation coupling negative electrode anaerobism/anode according to claim 4 is aerobic realizes many chlorine connection in bed mud
The method of benzene removal, it is characterised in that step（1）、（2）In, the concentration of the phosphate buffer is 0.1 mol/L, and phosphoric acid delays
PH=7.0 of fliud flushing；The phosphate buffer is that every liter of phosphate buffer adds 10 ml cultures with the mixed liquor proportioning of nutrient solution
Liquid；The phosphate buffer is cathode chamber or the 40-52% of anode building volume with the addition of the mixed liquor of nutrient solution.
8. a kind of electric microfield stimulation coupling negative electrode anaerobism/anode according to claim 4 is aerobic realizes many chlorine connection in bed mud
The method of benzene removal, it is characterised in that step（1）、（2）In, the nutrient solution composition includes：2.7 g.L-1 NaHCO3、0.5
g.L-1 K2HPO4、0.10 g.L-1 KCl、0.015 g.L-1 CaCl2、0.25 g.L-1 NH4Cl、10 mL.L-1Mineral solution and
10 mL.L-1Vitamin；The pH of the mixed liquor of the phosphate buffer and nutrient solution is with 0.1 mol L-1 H3PO4It is adjusted to 7.
9. a kind of electric microfield stimulation coupling negative electrode anaerobism/anode according to claim 8 is aerobic realizes many chlorine connection in bed mud
The method of benzene removal, it is characterised in that the mineral solution composition includes 1.5g.L-1 C6H6NO6·3Na·12H2O、0.13
g.L-1 ZnCl2、3.0 g.L-1 MgSO4、0.01 g.L-1 CuSO4·5H2O、0.5 g.L-1 MnSO4·H2O、0.01 g.L-1
AlK(SO4)2·12H2O、1.0 g.L-1 NaCl、0.01 g.L-1 H3BO3、0.1 g.L-1 FeSO4·7H2O、0.025 g.L-1
Na2MoO4、0.1 g.L-1 CaCl2·2H2O、0.024 g.L-1 NiCl2·6H2O、0.1 g.L-1 CoCl2·6H2O and 0.025
g.L-1 Na2WO4·2H2O。
10. a kind of electric microfield stimulation coupling negative electrode anaerobism/anode according to claim 4 is aerobic realizes many chlorine connection in bed mud
The method of benzene removal, it is characterised in that step（2）In, in the bed mud containing PCB61, the concentration of PCB61 is 0.1 μm of ol/g；
The bed mud containing PCB61 is added, it is necessary to add consumption for the TW80 surfactants of the aqueous solution 1g/L formed in cathode chamber increase
The water solubility of PCB61；The amount of the mixing sludge of the anaerobic dechlorination bacterium containing based on the PCB61 that degrades is negative electrode building volume
40~50%；Step（3）In, the voltage that external circuit applies is 1.0 ~ 2.5 V.
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