CN107342428A - A kind of method of the extracellular electron transmission of enhancement microbiological in microorganism electrochemical system - Google Patents
A kind of method of the extracellular electron transmission of enhancement microbiological in microorganism electrochemical system Download PDFInfo
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- CN107342428A CN107342428A CN201710429781.XA CN201710429781A CN107342428A CN 107342428 A CN107342428 A CN 107342428A CN 201710429781 A CN201710429781 A CN 201710429781A CN 107342428 A CN107342428 A CN 107342428A
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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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- H—ELECTRICITY
- H01—ELECTRIC ELEMENTS
- H01M—PROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
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Abstract
The method that the present invention provides the extracellular electron transmission of enhancement microbiological in a kind of microorganism electrochemical system, graphene or the graphene-supported carbon electrode that arrives of azepine are wherein used as anode, wherein the graphene or azepine graphene are directly loaded to the carbon electrode by electrophoretic deposition.The carbon electrode of the present invention also modification of the offer as microorganism electrochemical system Anodic, the method for preparing the carbon electrode, and including the carbon electrode microorganism electrochemical system.System and method of the invention are simple to operate, operating cost is low, and electricity production effect is good, is easy to scale to use.
Description
Technical field
The present invention relates to microorganism electrochemical field, more particularly to a kind of method of the extracellular electron transmission of enhancement microbiological.
Background technology
Nowadays environmental pollution and energy shortage are the two large problems of facing mankind.Microorganism electrochemical system is to utilize micro- life
A kind of bioreactor that thing driving oxidation or reduction reaction are carried out, can produce electric energy, microorganism while degradation of contaminant
Electro-chemical systems as a kind of renewable energy technologies, can alleviating energy crisis, contribute to the sustainable development of the mankind.
At present, the practical application of this technology is primarily limited to its weaker electricity generation ability, be mainly due to microorganism and
Electron transmission ability is relatively low between anode.Traditional anode material need to possess in microorganism electrochemical system：It is high conductivity, good
Biocompatibility, big specific surface area, good chemical stability, high mechanical strength and these low features of expense.
In microorganism electrochemical system, current most widely used electrode material is carbon material, and they generally possess well
Biocompatibility, it is corrosion-resistant and inexpensive the advantages that.Common carbon material has in microorganism electrochemical system：Carbon paper, carbon
Felt, carbon cloth, carbon brush, carbon fiber etc., but the simple anode by the use of carbon material as microorganism electrochemical system, its electricity production property
Can be relatively low, the expected requirement of people can not be reached.
The content of the invention
In view of this, in some embodiments, a kind of method of the extracellular electron transmission of enhancement microbiological of the present invention, wherein
It is graphene-supported to carbon electrode as anode using graphene or azepine, wherein the graphene or azepine graphene pass through electrophoresis
Deposition is directly loaded to the carbon electrode.
In some embodiments, in some embodiments, the anode available for the present invention can have flat shape, circle
Cylindricality, spiral shape, shaped form, including but not limited to piece, multiple, woven wire, antipriming pipe and spongy.In some embodiment party
In case, anode of the invention has larger surface-to-volume ratio.In some embodiments, anode can be from Microbial fuel electricity
Pond removes.In some embodiments, anode material includes the conduction materials such as carbon, CNT, carbon nano-fiber, carbon cloth, carbon paper
Material.In some embodiments, anode preferably has high surface area, low resistance, high conductivity or its combination.In some realities
Apply in scheme, anode allows high bacterial growth density.In some embodiments, can be used for the carbon electrode of the present invention includes carbon
Paper, carbon cloth, carbon fiber, carbon brush, carbon felt.
In some embodiments, directly graphene or azepine graphene are born by electrophoretic deposition such as ability cathode electrophoresis deposition
Carbon electrode is downloaded to as plate-load to the carbon electrode.In some embodiments, it can be used for the electrophoretic deposition of the present invention
Method is not particularly limited.In some embodiments, can be used for the deposition dispersion liquid of the present invention includes acetone, isopropanol
Or ethanol.
In some embodiments, the electricity production bacterium bag that can be used for the present invention includes pseudomonad (Pseudomonas), the thin end of the scroll
Bacterium (Geobacter), Shewanella (Shewanella) and red educate bacterium (Rhodoferax).In some embodiments, can be with
For the present invention electricity production bacterium bag include for example pseudomonas aeruginosa (Pseudomonas aeruginosa), pseudomonas putida,
Shewanella such as Shewanella (Shewanella oneidensis) MR-1, Shewanella putrefaciens (Shewanell
Putrefaciens) IR-1, Shewanella DSP10, the thin end of the scroll Pseudomonas, sulphur reduction ground bacillus (Geobacter
Sulfurreducens), metal reduction ground bacillus (Geobacter metallireducens), the warm ground bacillus of happiness
(Peletomaculum thermopropionicum), hot autotrophy methane thermal bacillus (Methanothermobacter
Thermautotrophicus), human pallid bacillus (Ochrobactrum anthropi), clostridium butyricum (Clostridium
Butyricum) EG3, Desulfuromonas acetoxidans (Desulfuromonas acetoxidans), iron vat red educate bacterium
(Rhodoferax ferrireducens), Aeromonas hydrophila (Aeromonas hydrophila) A3, propionic acid take off sulfolobus
(Desulfobulbus ropionicus)、Geopsychrobacter electrodiphilus、Geothrix
Fermentans, Escherichia coli (Escherichia coli), Rhodopseudomonas palustris (Rhodopseudomonas
Palustris), human pallid bacillus YZ-1, desulfovibrio desulfurican (Desulfovibrio desulfuricans), acidophilus Pseudomonas
Species (Acidiphilium sp.), Friedlander's bacillus (Klebsiella pneumonia) L17.In some embodiments
In, it is used as electricity production bacterium using Shewanella such as MR--1.In some embodiments, in microorganism electrochemical system response room
Culture medium is configured to the nanobacteria innocuous to being in contact with it.In some embodiments, can adjust culture medium or solvent so that its with
The metabolism of bacterium matches.In some embodiments, can be by adjusting pH to about pH3-9 e.g., from about 5-8.5 models
In enclosing.In some embodiments, it has been found possible to do not implement the present invention under conditions of neutral ph, and to electricity generation ability without bright
Aobvious adverse effect.Therefore, in some embodiments, the medium pH of the present invention can be adjusted to e.g., from about 3-6.5,4-6,
4.5-5.5,7.5-8 etc..If desired, buffer can be added into culture medium or solvent, and oozed by diluting or adding
Activating substance is pressed to adjust the concentration of culture medium or solvent thoroughly.In some embodiments, a kind of salt can be added to adjust ion
Intensity.In addition, if it is desired, it is thin with what is kept fit to may also include nutrients, co-factor, vitamin and other similar additives
Strain group.In some embodiments, the fluid with low electric conductivity can be used in system and method for the invention, without
Want buffer solution.In some embodiments, system and method for the invention can be effectively from containing Biodegradable material
Fluid production energy, and Biodegradable material is effectively removed from fluid.The system and method for the present invention can avoid flowing
The notable acidifying of body.In some embodiments, system and method for the invention have high current density.In some embodiment party
In case, there is low or without buffering raw material to obtain high current density for use of the invention.In some embodiments,
The system and method for the present invention are reduced for example due to loss caused by ion transport.
In some embodiments, the present invention provides the carbon electrode of the modification as microorganism electrochemical system Anodic,
The carbon electrode of wherein described modification is the carbon electrode for being loaded with graphene or azepine graphene, wherein the graphene or azepine stone
Black alkene is directly loaded to the carbon electrode by electrophoretic deposition.
In some embodiments, the carbon electrode includes carbon paper, carbon cloth, carbon fiber, carbon brush, carbon felt.
In some embodiments, the present invention provides a kind of microorganism electrochemical system, and it includes the modification of the present invention
Carbon electrode is as anode.
In some embodiments, the microorganism electrochemical system includes microbiological fuel cell and microorganism is electrolysed
Pond.
In some embodiments, the microbiological fuel cell includes the carbon electrode of the modification of the present invention as anode,
Negative electrode, and connect the conductor of the anode and the negative electrode.
In some embodiments, as described above, the anode available for the present invention can have various suitable shapes.
In some embodiments, anode can be connected by wire such as copper with negative electrode.In some embodiments, microorganism of the invention combustion
The negative electrode of material battery includes following conductive material：Metal, carbon, CNT, carbon nano-fiber, carbon cloth, carbon paper, platinum, graphite,
Graphite rod, graphite felt, granular graphite or other conductive materials.In some embodiments, can be incited somebody to action by sept such as dividing plate or film
Anode chamber and cathode chamber separate.In some embodiments, the sept that anode chamber and cathode chamber separate is slowed down, reduced or hindered
Only electronics moves directly to negative electrode from anode, and electronics is flowed by the wire of circuit.In some embodiments, the interval
Thing can be such as biomembrane, fabric, screen, amberplex.
In some embodiments, system provided by the invention such as microbiological fuel cell includes：Sheet as anode
The carbon electrode of the modification of invention, the electricity-producing microorganism with the positive contact, the negative electrode containing one or more conductive materials, institute
State the amberplex between anode and the negative electrode, electric conductor, itself and the anode and the negative electrode.In some embodiments
In, method and system of the invention can include the device that flowing material is directed to anode.In some embodiments, it is described
Anode and/or the negative electrode are in the room of sealing.In some embodiments, have in anode chamber and be adapted for introduction into containing life
The entrance of the fluid of thing degradable material and the outlet for removing fluid from the chamber.In some embodiments, in negative electrode
Room has the entrance for being suitable for introducing oxygen-containing gas.In some embodiments, cathode chamber is that air is opened wide.At some
In embodiment, the anode chamber and/or cathode chamber are dismountable.
In some embodiments, the present invention provides the device for including microbiological fuel cell and microorganism electrolysis cell, its
Middle microbiological fuel cell can be battery as described above, and wherein microorganism electrolysis cell can include the carbon of the modification of the present invention
Electrode is anode and negative electrode such as platinum electrode.In some embodiments, cathode of electrolytic tank room has gas vent.In some realities
Apply in scheme, described electrolytic cell anode room can be connected by conduit with cathode of electrolytic tank room.In some embodiments,
Fuel cell anode electrodes are connected with cathode of electrolytic tank electrode, and fuel battery negative pole electrode is connected with electrolytic cell anode electrode.
In some embodiments, electrolytic cell anode room has carbon source entrance.In said device, the microbiological fuel cell can be
Microorganism electrolysis cell provides power supply.In some embodiments, described device can be used for the purposes such as wastewater treatment.
In some embodiments, the present invention provides a kind of method for the carbon electrode for preparing described modification, and it includes will
Graphene or azepine it is graphene-supported to carbon electrode as anode the step of, wherein the graphene or azepine graphene pass through electricity
Swimming deposition is directly loaded to the carbon electrode.
The method that the present invention deposits first with ability cathode electrophoresis, graphene and azepine is graphene-supported to carbon paper electrode table
Face, then the anode of microorganism electrochemical system is used as to promote to produce electricity.In the present invention, microorganism is as oxidation/reduction
The catalyst of reaction, while microbial consumption substrate lactic acid, electronics is produced, is transferred to by way of extracellular electron transmission
Anode, produce electric energy.
The method that the present invention is deposited using ability cathode electrophoresis, graphene and azepine is graphene-supported to carbon paper electrode surface use
Make biological anode to promote BESs electricity production.The present invention can make BESs using the anode after graphene and azepine graphene modified
Electricity generation ability improve 6~8 times.It has also been found that BESs electricity generation ability is about azepine when graphene is as anode modification thing
1.3 times or so of BESs electricity generation abilities after graphene modified anode, this will be attributed to the more preferable biocompatibility of graphene, more
High electrical conductivity and to the more preferable response of riboflavin.This method is simple to operate and operating cost is low, promotes BESs electricity productions effect good,
Experimental facilities requirement is simple, is easy to scale to use.
Brief description of the drawings
Fig. 1：Fig. 1 a, Fig. 1 b, Fig. 1 c are carbon paper electrode, graphene-carbon paper electrode and the azepine that the embodiment of the present invention 1 uses
The scanning electron microscope (SEM) photograph of graphene-carbon paper electrode；
Fig. 2：Fig. 2 a, Fig. 2 b are the transmission electron microscope picture of the graphene that the embodiment of the present invention 1 uses and azepine graphene；
Fig. 3 is the XPS sign collection of illustrative plates of the graphene that the embodiment of the present invention 1 uses and azepine graphene；
Fig. 4 be the embodiment of the present invention 1 use graphene, azepine graphene, carbon paper electrode, graphene-carbon paper electrode and
The specific surface area block diagram of azepine graphene-carbon paper electrode；
Fig. 5：Fig. 5 a, Fig. 5 b, Fig. 5 c are carbon paper electrode, graphene-carbon paper electrode and the azepine that the embodiment of the present invention 1 uses
The water contact angle of graphene-carbon paper electrode characterizes picture；
Fig. 6 is carbon paper electrode, graphene-carbon paper electrode and the azepine graphene-carbon paper electrode that the embodiment of the present invention 1 uses
EIS impedance spectras；
Fig. 7 is that the embodiment of the present invention 2 has used carbon paper electrode, graphene-carbon paper electrode and azepine graphene-carbon paper electrode
The electricity production figure of the microorganism electrochemical system of installation；
Fig. 8：After Fig. 8 a, Fig. 8 b, the reactor end of run that Fig. 8 c are the installation of the embodiment of the present invention 2, anode surface is micro-
The scanning electron microscope (SEM) photograph of biology；
Fig. 9 is the BCA method albumen of anode surface microorganism after the reactor end of run that the embodiment of the present invention 2 is installed
Determine block diagram.
Figure 10 is the cyclic voltammetry scan at electricity production peak value in the reactor running that the embodiment of the present invention 2 is installed
Figure；
Figure 11 is carbon paper electrode, graphene-carbon paper electrode and azepine graphene-carbon paper electricity that the embodiment of the present invention 3 uses
Cyclic voltammetry scan figure of the pole in riboflavin system.
Embodiment
Below in conjunction with the accompanying drawing of the embodiment of the present invention, the technical scheme in the embodiment of the present invention is carried out clear, complete
Ground describes, it is clear that described embodiment is only part of the embodiment of the present invention, rather than whole embodiments.Based on this
Embodiment in invention, the every other reality that those of ordinary skill in the art are obtained under the premise of creative work is not made
Example is applied, belongs to the scope of protection of the invention.
Experiment material：
Following experiment materials are used herein：
Graphene and azepine graphene：Chengdu Organical Chemical Co., Ltd., Chinese Academy of Sciences
Xi Washi MR-1 bacteriums：There is provided by professor K.H.Nealson of University of Southern California
LB culture mediums：10g/L peptones；5g/L NaCl；5g/L yeast extracts.Wherein, peptone and yeast extract are purchased from：
Oxoid Ltd.Wade Road.Basingstoke.Hants.RG24 8PW.UK.Made in the United Kingdom,
NaCl is purchased from：Chemical Reagent Co., Ltd., Sinopharm Group.
Aerobic culture medium：10mL/L macroelements, 10mL/L trace elements, 10mL/LMgSO4·7H2O、2.788mL/LL-
The μ L of sodium lactate (60%), 11.91g/L HEPES, 1L culture mediums/2mL Casa mino Acid concentrates, 1L culture mediums/500
Vitamin
Anaerobic culture medium：10mL/L macroelements, 10mL/L trace elements, 10mL/LMgSO4·7H2O、2.788mL/L
Pfansteihl sodium (60%), 6.4g/L fumaric acid 11.91g/L HEPES, 1L culture mediums/2mL Casa mino Acid concentrations
The μ L Vitamin of liquid, 1L culture mediums/500
Macroelement forms and specific source：
NH4Cl Chemical Reagent Co., Ltd., Sinopharm Group
(NH4)2SO4Chemical Reagent Co., Ltd., Sinopharm Group
K2HPO4Chemical Reagent Co., Ltd., Sinopharm Group
KH2PO4Chemical Reagent Co., Ltd., Sinopharm Group
Trace element composition and specific source：
NTA Chemical Reagent Co., Ltd., Sinopharm Group
MnCl2·4H2O Chemical Reagent Co., Ltd., Sinopharm Group
FeSO4·7H2O Chemical Reagent Co., Ltd., Sinopharm Group
CoCl2·6H2O Chemical Reagent Co., Ltd., Sinopharm Group
ZnCl2Chemical Reagent Co., Ltd., Sinopharm Group
CuSO4·4H2O Chemical Reagent Co., Ltd., Sinopharm Group
AlK(SO4)2·12H2O Chemical Reagent Co., Ltd., Sinopharm Group
H3BO3Chemical Reagent Co., Ltd., Sinopharm Group
NaMoO4·2H2O Chemical Reagent Co., Ltd., Sinopharm Group
NiCl2·6H2O Chemical Reagent Co., Ltd., Sinopharm Group
NaWO4·2H2O Chemical Reagent Co., Ltd., Sinopharm Group
NaSeO4Chemical Reagent Co., Ltd., Sinopharm Group
Casa mino Acid concentrates：20g Casa mino Acid powder is dissolved in 100mL distilled water raw work
Bioengineering (Shanghai) limited company
Vitamin and various medicines specific source：
10mg/L puridoxine hydrochlorides Chemical Reagent Co., Ltd., Sinopharm Group
5mg/L riboflavin Chemical Reagent Co., Ltd., Sinopharm Group
5mg/L vitamin B1s Chemical Reagent Co., Ltd., Sinopharm Group
5mg/L nicotinic acid Chemical Reagent Co., Ltd., Sinopharm Group
5mg/L calcium D-VB5 salt Chemical Reagent Co., Ltd., Sinopharm Group
5mg/L p-aminobenzoic acid Chemical Reagent Co., Ltd., Sinopharm Group
5mg/L lipoic acids Chemical Reagent Co., Ltd., Sinopharm Group
2mg/L biotins Chemical Reagent Co., Ltd., Sinopharm Group
2mg/L folic acid Chemical Reagent Co., Ltd., Sinopharm Group
0.1mg/L vitamin B12s Chemical Reagent Co., Ltd., Sinopharm Group
MgSO4·7H2O Chemical Reagent Co., Ltd., Sinopharm Group
Pfansteihl sodium (60%) Sangon Biotech (Shanghai) Co., Ltd.
HEPES Sangon Biotech (Shanghai) Co., Ltd.
Fumaric acid Aladdin reagent
Acetone soln Chemical Reagent Co., Ltd., Sinopharm Group
Elemental iodine Chemical Reagent Co., Ltd., Sinopharm Group
Carbon paper：The upper gloomy Electrical Appliances Co., Ltd's model in Haihe River：East beautiful 090.
Experimental program：
In a specific embodiment, the present invention may comprise steps of：
Carbon paper electrode surface is arrived by graphene and azepine are graphene-supported；
Xi Washi MR-1 bacteriums are cultivated in LB culture mediums, aerobic culture medium, anaerobic culture medium successively；
The installation of microorganism electrochemical system (BESs) in super-clean bench；
BESs is run under Shanghai Chen Hua electrochemical workstation (CHI1030C) control, Monitoring Data.
In the present invention, the method for the electrode modification can be electrophoretic deposition, the method deposited such as ability cathode electrophoresis.
In the present invention, the DC voltage value of the ability cathode electrophoresis deposition can be 10V~20V, such as 15V.
In the present invention, the time of the ability cathode electrophoresis deposition can be 5min~15min, such as 10min.
In the present invention, when high-temperature sterilization pot sterilizes, can be by its parameter setting：Temperature：121 DEG C, sterilization time：
20min。
In the present invention, microorganism electrochemical system can be run under conditions of 30 DEG C of room temperature.
In the present invention, occasion China electrochemical workstation such as Amperometric i-t curve can be used.
In the present invention, operationally, the control of its anode potential can be+0.1V v.s.Ag/ to microorganism electrochemical system
AgCl reference electrodes.
In the present invention, the microorganism can be pure bacterium S.Oneidensis MR-1, and the bacterium solution of the BESs systems can
To be made by following methods：
The method for first passing through monoclonal, S.Oneidensis MR-112h are cultivated in LB culture mediums；Then in aerobic ore deposit
S.Oneidensis MR-1 24h are cultivated in thing salt culture medium；Finally cultivated in anaerobism mineral salts medium
6~8h of S.Oneidensis MR-1 or so, such as 7h.
The present invention has no to the source of the acetone soln, carbon paper, graphene, azepine graphene, electricity production bacterium and elemental iodine
Special limitation, the present invention used in raw material be commercially available unless otherwise noted.
The present invention dc source used in ability cathode electrophoresis deposition is had no it is specifically limited, as long as its dependable performance and can reach
To the requirement of experiment of correlation.
The method that the present invention is deposited using ability cathode electrophoresis, graphene and azepine is graphene-supported to carbon paper electrode surface use
Make biological anode to promote BESs electricity production.The present invention can make BESs using the anode after graphene and azepine graphene modified
Electricity generation ability improve 6~8 times.It has also been found that BESs electricity generation ability is about azepine when graphene is as anode modification thing
1.3 times or so of BESs electricity generation abilities after graphene modified anode, this will be attributed to the more preferable biocompatibility of graphene, more
High electrical conductivity and to the more preferable response of riboflavin.This method is simple to operate and operating cost is low, promotes BESs electricity productions effect good,
Experimental facilities requirement is simple, is easy to scale to use.
In order to further illustrate the present invention, with reference to embodiments to a kind of extracellular electricity of enhancement microbiological provided by the invention
The method that son transmits is described in detail, but they can not be interpreted as into limiting the scope of the present invention.
Embodiment 1
First by 20mg graphenes or azepine graphene in 50ml acetone solns ultrasonic disperse 30min, then add 1 iodine
Simple substance, then ultrasonic 15min, obtain ability cathode electrophoresis deposition dispersion liquid, and the method then deposited using ability cathode electrophoresis controls its direct current
Voltage is：15V, sedimentation time：10min, graphene and azepine graphene are wrapped in carbon paper fibre by way of electrostatical binding
Dimension table face, the anode material after being modified.
The present invention is scanned electronic microscope photos to the anode material after modification, and it is that the embodiment of the present invention 1 uses to see Fig. 1, Fig. 1
Graphene and azepine graphene scanning electron microscope (SEM) photograph.The configuration of surface of electrode after modifying as seen from Figure 1.
The graphene and azepine graphene that the present invention is used embodiment 1 carry out transmission electron microscope analysis, see Fig. 2, Fig. 2 positions sheet
The graphene and the transmission electron microscope picture of azepine graphene that invention example 1 uses.Graphene and azepine graphene as seen from Figure 2
The configuration of surface of material itself.
The graphene and azepine graphene that the present invention is used embodiment 1 carry out XPS analysis, as a result see Fig. 3, can by Fig. 3
To find out chemical element species that commercially available graphene and the azepine graphene that uses of the present invention is included.
The present invention embodiment 1 is used graphene, azepine graphene, graphene-carbon paper, azepine graphene-carbon paper and
Carbon paper has carried out BET specific surface area measure respectively, as a result sees Fig. 4, and as seen from Figure 4, the specific surface area of graphene is about nitrogen
The similar specific surface of 7 times or so of miscellaneous graphene, graphene-carbon paper and azepine graphene-carbon paper, and the specific surface area of the two
Be each about 4 times of carbon paper or so, illustrate by graphene and azepine it is graphene-supported after, the increase of the specific surface area of carbon paper, more
Be advantageous to the attachment of microorganism.
Carbon paper electrode, graphene-carbon paper electrode and the azepine graphene-carbon paper electrode that the present invention is used embodiment 1 are entered
Go the sign of water contact angle, as a result see Fig. 5, the water that can be seen that azepine graphene-carbon paper electrode by Fig. 5 experimental result connects
Feeler is maximum, and its contact angle is more than 150 °, belongs to super hydrophobic material, and graphene-carbon paper electrode is taken second place, minimum for carbon paper electricity
Pole, illustrate after graphene or azepine graphene modified, anode material hydrophobicity improves.
Carbon paper electrode, graphene-carbon paper electrode and the azepine graphene-carbon paper electrode that the present invention is used embodiment 1 are entered
The sign of impedance spectrum is gone, has as a result seen Fig. 6, can be seen that by Fig. 6 experimental result and repaiied by graphene or azepine graphene
After decorations, the load transfer impedance of carbon paper electrode is greatly reduced, is advantageous to the extracellular electron transmission of microorganism.
Embodiment 2
First by reactor accessories such as reactor, magnetic agitation rotor, butyl rubber bungs by high-temperature sterilization, working electrode,
Platinum filament is sterilized to electrode and Ag/AgCl reference electrodes by uviol lamp, the then assembled battery in super-clean bench.The system uses
The MEC of single chamber, after wherein Xi Washi MR--1 bacteriums Anaerobic culturel process terminates, this anaerobic culture medium is directly dispensed into 6
In reactor, the volume of culture medium is 130mL in each reactor, and wherein H+ ion reductions production H occurs for platinum electrode2It is anti-
Should, anode occurs lactic acid and is oxidized the reaction of generation acetic acid, and discharges electronics in the process.After treating that battery installs, utilize
The electricity generation performance of occasion China electrochemical workstation monitoring BESs systems.Fig. 7 is seen, as seen from Figure 7, by different anode material groups
The reactor dressed up, the size of its electricity generation ability are：Graphene-carbon paper ＞ azepine graphene carbon paper ＞ carbon papers.
The present invention has carried out scanning electron microscope analysis to the anode surface microorganism after reactor end of run, sees Fig. 8, schemes
8 be the scanning electron microscope (SEM) photograph for the anode material surface microorganism that the embodiment of the present invention 2 uses.Reactor is run as seen from Figure 8
The form of the microorganism of electrode surface and decorative material after end.
The present invention is carried out using BCA methods albuminometry to the content of electrode surface microorganism after reactor end of run
Measure, is shown in Fig. 9, the content of the microorganism on different anode material surfaces is followed successively by from big to small as seen from Figure 9：Graphite
Alkene-carbon paper ＞ azepine graphene carbon paper ＞ carbon papers.
The present invention has carried out CV scannings in reactor running to its anode, sees Figure 10, goes out in electricity production peak value to each
Reactor has carried out CV scannings, and as seen from Figure 10, different anode materials, the size of its oxidation/reduction peak current is present
Difference, oxidation/reduction peak current be ranked up from big to small for：Graphene-carbon paper ＞ azepine graphene carbon paper ＞ carbon papers.
Embodiment 3
The electrolyte that the solution for being 5mM by the use of mineral salts medium configuration riboflavin concentration scans as CV, graphene-carbon
Paper electrode, azepine graphene-carbon paper electrode and carbon paper electrode are platinum electrode to electrode, reference is electric respectively as working electrode
Extremely Ag/AgCl reference electrodes, CV scannings then are done to different working electrodes using occasion China electrochemical workstation, it is as a result visible
Figure 11, it can be seen from Figure 11 result in riboflavin system, the oxidation of its CV scanning curve of different working electrodes/also
There is larger difference in parent peak electric current, oxidation/reduction peak current sorts from big to small to be followed successively by：Graphene-carbon paper electrode ＞ nitrogen
Miscellaneous graphene-carbon paper electrode ＞ carbon paper electrodes, illustrate that response of the graphene-carbon paper electrode to riboflavin is most strong, most beneficial for core
The progress of flavine receiving and losing electrons process, azepine graphene-carbon paper electrode are taken second place, and response of the carbon paper electrode to riboflavin is most weak.
Claims (10)
- A kind of 1. method of the extracellular electron transmission of enhancement microbiological, wherein arriving carbon electrode using graphene or azepine are graphene-supported As anode, wherein the graphene or azepine graphene are directly loaded to the carbon electrode by electrophoretic deposition.
- 2. the method described in claim 1, wherein carbon electrode include carbon paper, carbon cloth, carbon fiber, carbon brush, carbon felt.
- 3. the method described in claim 1 or 2, wherein the deposition dispersion liquid used includes acetone.
- 4. the method any one of claim 1-3, wherein the electricity production bacterium bag used includes pseudomonad (Pseudomonas), ground bacillus (Geobacter), Shewanella (Shewanella) and red bacterium (Rhodoferax) is educated.
- 5. the carbon electrode of the modification as microorganism electrochemical system Anodic, wherein the carbon electrode of the modification is to be loaded with stone The carbon electrode of black alkene or azepine graphene, wherein the graphene or azepine graphene be directly loaded to by electrophoretic deposition it is described Carbon electrode.
- 6. the carbon electrode of the modification described in claim 5, wherein the carbon electrode includes carbon paper, carbon cloth, carbon fiber, carbon brush, carbon Felt.
- 7. a kind of microorganism electrochemical system, it includes the carbon electrode of the modification described in claim 5 or 6 as anode.
- 8. the microorganism electrochemical system described in claim 7, it includes microbiological fuel cell and microorganism electrolysis cell.
- 9. the microorganism electrochemical system described in claim 8, wherein the microbiological fuel cell includes the carbon of the modification Electrode is as anode, negative electrode, and connects the conductor of the anode and the negative electrode.
- 10. a kind of method for the carbon electrode for preparing the modification described in claims requirement 5 or 6, it include graphene or Azepine is graphene-supported to arrive the step of carbon electrode is as anode, wherein the graphene or azepine graphene are straight by electrophoretic deposition Connect and be loaded to the carbon electrode.
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Cited By (10)
| Publication number | Priority date | Publication date | Assignee | Title |
|---|---|---|---|---|
| CN110343602A (en) * | 2019-06-28 | 2019-10-18 | 浙江大学 | The pure bacterium Geobacter microorganism belonging to genus electro-chemical systems that can simply start in aerobic environment |
| CN110364746A (en) * | 2019-07-18 | 2019-10-22 | 山西师范大学 | Anode of microbial fuel cell electrode material preparation method, anode of microbial fuel cell electrode slice and microbiological fuel cell |
| CN110528017A (en) * | 2019-07-25 | 2019-12-03 | 西安交通大学 | A kind of electrolysis hydrogen tympanites bubble column microorganism electro synthesis reactor and its application method |
| CN111029633A (en) * | 2019-11-15 | 2020-04-17 | 广东轻工职业技术学院 | Microbial fuel cell and preparation method and application thereof |
| CN112125409A (en) * | 2020-08-14 | 2020-12-25 | 同济大学 | Method for improving anaerobic denitrification efficiency by coupling oneidensisMR-1 and nano graphene sheet |
| CN110760469B (en) * | 2019-12-03 | 2021-06-08 | 中国科学院烟台海岸带研究所 | Desulfurization vibrio and application thereof |
| CN113270623A (en) * | 2021-06-10 | 2021-08-17 | 中国科学技术大学 | Microbial electrochemical system |
| CN113479994A (en) * | 2021-07-14 | 2021-10-08 | 南开大学 | Graphene-magnetite conductive skeleton electrode, preparation method and application thereof, and method for treating petrochemical wastewater |
| CN113736709A (en) * | 2021-09-24 | 2021-12-03 | 广东工业大学 | Manganese pollution repairing agent and preparation method and application thereof |
| CN114447349A (en) * | 2022-02-11 | 2022-05-06 | 天津大学 | Composite anode electrode for promoting electrogenesis and biofilm formation, and preparation method and application thereof |
Citations (3)
| Publication number | Priority date | Publication date | Assignee | Title |
|---|---|---|---|---|
| CN104201438A (en) * | 2014-09-23 | 2014-12-10 | 中国地质大学（武汉） | Lithium-air battery based on oxidized graphene-carbon paper gas catalytic electrode |
| CN105355936A (en) * | 2015-12-09 | 2016-02-24 | 中南大学 | Preparation method of catalytic carbon paper |
| CN105529473A (en) * | 2015-12-15 | 2016-04-27 | 中国科学院化学研究所 | Graphene oxide-modified electrode material for energy storage flow battery |
-
2017
- 2017-06-08 CN CN201710429781.XA patent/CN107342428B/en active Active
Patent Citations (3)
| Publication number | Priority date | Publication date | Assignee | Title |
|---|---|---|---|---|
| CN104201438A (en) * | 2014-09-23 | 2014-12-10 | 中国地质大学（武汉） | Lithium-air battery based on oxidized graphene-carbon paper gas catalytic electrode |
| CN105355936A (en) * | 2015-12-09 | 2016-02-24 | 中南大学 | Preparation method of catalytic carbon paper |
| CN105529473A (en) * | 2015-12-15 | 2016-04-27 | 中国科学院化学研究所 | Graphene oxide-modified electrode material for energy storage flow battery |
Non-Patent Citations (1)
| Title |
|---|
| 侯俊先等: "石墨烯修饰微生物燃料电池阳极的研究", 《工程热物理学报》 * |
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| CN111029633B (en) * | 2019-11-15 | 2023-03-28 | 广东轻工职业技术学院 | Microbial fuel cell and preparation method and application thereof |
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