CN106981668A - A kind of microorganism electrode and its preparation method and application - Google Patents
A kind of microorganism electrode and its preparation method and application Download PDFInfo
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- CN106981668A CN106981668A CN201710327792.7A CN201710327792A CN106981668A CN 106981668 A CN106981668 A CN 106981668A CN 201710327792 A CN201710327792 A CN 201710327792A CN 106981668 A CN106981668 A CN 106981668A
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- microorganism
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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
- H01M4/00—Electrodes
- H01M4/86—Inert electrodes with catalytic activity, e.g. for fuel cells
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- G—PHYSICS
- G01—MEASURING; TESTING
- G01N—INVESTIGATING OR ANALYSING MATERIALS BY DETERMINING THEIR CHEMICAL OR PHYSICAL PROPERTIES
- G01N27/00—Investigating or analysing materials by the use of electric, electrochemical, or magnetic means
- G01N27/26—Investigating or analysing materials by the use of electric, electrochemical, or magnetic means by investigating electrochemical variables; by using electrolysis or electrophoresis
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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
- H01M4/00—Electrodes
- H01M4/86—Inert electrodes with catalytic activity, e.g. for fuel cells
- H01M4/88—Processes of manufacture
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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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- 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 present invention discloses a kind of microorganism electrode and its preparation method and application, in electrode building process, it is suitable in the conductive hydrogel polycondensation monomer solution of microbe survival add appropriate electro-chemical activity microorganism to conditions such as pH, temperature, forms the dispersed bacteria suspension of microbial cell.Inactive, conductive material is immersed in bacteria suspension, then in a mild condition, conductive hydrogel monomer polymerizing curable is made, electro-chemical activity microorganism is fixed in conductive hydrogel after shaping, so as to form microorganism electrode.This method improves the quantity for the microorganism being enriched with microorganism electrode by embedded immobilization, while contact area between microorganism and electrode material is added, so as to reduce microorganism to the resistance of electrodes transfer electronics.The microorganism electrode can improve microbiological fuel cell output voltage and power density as anode of microbial fuel cell；Microorganism electrode then can improve the sensitivity of microbiological sensor as the microbiological sensor of electrochemistry type by improving electric current output.
Description
Technical field
The present invention relates to microbiological fuel cell and microbiological sensor technical field, more particularly to a kind of microorganism electricity
Pole and its preparation method and application.
Background technology
Microorganism electrode is that a kind of microorganism using with electro-chemical activity or intact cell are used as catalyst or sensitive member
Part is combined together and constituted with electrode, and it decomposes substrate by the metabolism of microorganism, by chemical energy therein
It is converted into the device of electric energy or electric signal.Microorganism electrode can be passed as anode of microbial fuel cell and electrochemistry microorganism
Sensor electrode is used.
The chemical energy contained in organic matter can be converted into electric energy by microbiological fuel cell, be a kind of preferable sewage disposal
And clean energy technology, wherein the critical component for realizing energy conversion is exactly the microorganism electrode as anode.
Microorganism electrode is the core component of electrochemistry type microbiological sensor.The telecommunications produced in microbial metabolism
Number relevant with the content of organics and composition in the environment residing for it, microbiological sensor can be by measuring microorganism electrode
The electric signals such as electric current, the voltage of generation obtain concentration of substrate and the related information of composition.
The building mode of traditional microbiological electrode is mainly by way of absorption is enriched with electricity in prefabricated electrode surface
Chemism microorganism.Such way is limited due to electrode surface area, the electro-chemical activity micro organism quantity that can be enriched with by
To considerable restraint.
Also it is commonly used in sensor electrode preparation process and uses polyvinyl alcohol, sodium alginate Polymer material by electrification
Learn active microorganism and adhere to electrode surface.But because general high polymer material does not possess conductive capability, it is used as electrode and electricity
Attachment between chemism microorganism can cause microorganism to electrode surface transmission electron drag increase, so as to reduce electric current
The harmful effect for causing sensitivity to decline.
Above-mentioned unfavorable factor causes existing microorganism electrode to be applied to anode of microbial fuel cell or as sensor
In use, the performance such as power output and sensitivity also has many problems, it still can not well meet and be actually needed.These all shadows
The development of microbiological fuel cell and electrochemistry microbiological sensor is rung.
The content of the invention
In order to overcome the above-mentioned deficiencies of the prior art, the invention provides the new paragon that a kind of microorganism electrode is built, use
To improve enriched amount of the electro-chemical activity microorganism on electrode on microorganism electrode, while reducing what microbial metabolism was produced
Resistance from electronics to electrodes transfer.
The technical solution adopted in the present invention is：Good, the gentle conductive hydrogel material of polymerizing condition using electric conductivity
Electro-chemical activity microorganism is fixed within conductive hydrogel as electrode material and constitutes micro- life by material by way of embedding
Thing electrode.
The microorganism electrode being prepared from it is a further object to provide a kind of above-mentioned preparation method is as micro- life
The application of thing anode of fuel cell.
Third object of the present invention is that a kind of above-mentioned preparation method of offer prepares microorganism electrode and passed as microorganism
Sensor, for the application in terms of target substance composition and Concentration Testing.
Microorganism electrode preparation method of the present invention is as follows：
(1) monomer solution before the polymerization of regulation conductive hydrogel, makes the conditions such as its pH, temperature be suitable to microbe survival.Tool
There is the eigenstate conductive hydrogel material for gripping pi bond structure altogether to usually require through overdoping to improve the conductive capability of hydrogel, such as
Layer/polyaniline conductive hydrogel can improve electrical conductivity by acid doping.In this case also need to add suitably in polymerized monomer
Dopant.
(2) appropriate electro-chemical activity microorganism is added into conductive hydrogel polycondensation monomer solution, microbial cell is formed equal
Even scattered bacteria suspension.
(3) inactive, conductive material is immersed in bacteria suspension, such as graphite fibre is used as being connected after shaping with external circuit.
Then conductive hydrogel monomer polymerizing curable is made in a mild condition, by the conduction of electro-chemical activity microorganism fixation after shaping
In hydrogel, microorganism electrode is formed.
There are following characteristics by microorganism electrode made from conductive hydrogel embedding electro-chemical activity Institute of Micro-biology：
(1) electro-chemical activity load of microorganisms amount is big on electrode, and there is microbial profile electrode material surface and inside.
(2) electro-chemical activity microorganism and electrode material contacts area are big, electro-chemical activity microorganism inside distribution electrode
Cell is wrapped up by electrode material completely, and the resistance that electronics is delivered to electrode from microbial cell is smaller.
(3) the electro-chemical activity microorganism being wrapped in inside electrode material enhances because being protected by electrode material
The stability of microbial cell structure, is allowed to accommodative ability of environment stronger.
The advantage of technical solution of the present invention is：
Compared with prior art, the mode that the present invention is enriched with electro-chemical activity microorganism on electrode is no longer traditional suction
Subsidiary formula formula, but investment fashion.The microorganism being enriched with this way is not distributed only over electrode material surface, and can deposit
It is inside electrode material, thus substantially increases the quantity of microorganism on electrode, see Fig. 1.
On the other hand, electro-chemical activity microorganism is enriched with by investment fashion, a large amount of microbial cells are wrapped in electrode
Material internal, this causes contact area increase of the microorganism between electrode material, advantageously reduces electronics and transmitted to electrode surface
The resistance being subject to.
In addition, there is big conjugatedπbond body in the eigenstate conductive hydrogel material that imbedded microbe is used, most structure
System, can form a large amount of electron holes after acid doping, with the effect for promoting electron transmission, see Fig. 2.
Brief description of the drawings
Fig. 1 is that conductive hydrogel embeds the microorganism electrode schematic diagram that electro-chemical activity Institute of Micro-biology builds.
Fig. 2 is electronics from electro-chemical activity microbial cell to electrodes transfer process schematic.
Fig. 3 is that Escherichia coli are electric in conductive hydrogel electrode surface and internal distribution scanning as electro-chemical activity microorganism
Mirror figure.
Fig. 4 microorganism electrodes are used for polarization curve and power density curve map obtained by double-chamber microbiological fuel cell anode.
Fig. 5 microorganism electrodes do cyclic voltammetry scan figure for microbiological sensor to different substrates.
Fig. 6 microorganism electrodes do cyclic voltammetry scan figure and peak for microbiological sensor to different glucose solution
It is worth electric current to glucose concentration linear regression analysis figure.
Specific embodiment
The embodiment to technical solution of the present invention is described in detail below, but the present invention is not limited in following description
Hold：
Embodiment one
It is prepared by microorganism electrode
By taking polyaniline/polyvinyl alcohol composite conducting hydrogel embedding electro-chemical activity microorganism Escherichia coli as an example, explanation
The construction method of microorganism electrode：
(1) preformed solution of composite conducting hydrogel is prepared, 0.46ml aniline is added in 2.0mL10% poly-vinyl alcohol solutions
With 0.92mL solution A is configured to as 50% phytic acid of dopant.Weigh 0.25g ammonium persulfates and be dissolved in 0.5mL deionized waters
Middle obtained solution B.By two kinds of solution be cooled to 4 DEG C it is standby.
(2) disperse in foregoing solution A after 20mg Escherichia coli, make A, B solution mixing, immerse a branch of in mixed solution
Electrically conductive graphite fiber, makes it solidify in -10 DEG C of freezings, then melts at 4 DEG C, repeatedly for three times, makes composite conducting hydrogel complete
All solidstate formation is embedded with Escherichia coli conductive hydrogel.
(3) the Escherichia coli conductive hydrogel that is embedded with after solidifying is soaked in deionized water 6 hours, is removed unpolymerized
The small-molecule substances such as phytic acid, that is, complete the structure of microorganism electrode.
Embodiment two
Microorganism electrode is used as MFC anodes
Microorganism electrode described in embodiment one builds double-chamber microbiological fuel cell reactor as anode, by Nafion
117 films are stuck in centre, separate cathode chamber and anode chamber, cathode chamber and anode chamber's electrolyte volume are 15mL, mentioned microorganism
Electrode is as anode, and carbon paper is individually fixed in two Room ends as negative electrode.On anode chamber's rubber plug cover, and it is passed through nitrogen and removes
Oxygen, battery is put in Water Tank with Temp.-controlled, 37 DEG C of temperature control.10g/LNaHCO is added in LB culture mediums3, 8.5g/LNaH2PO4·H2O,
2g/L glucose, 80 μm of ol/L dimethyl diaminophenazine chlorides are used as Anolyte solution (pH=7).The composition of catholyte solution is pH=
7 0.1mol/L potassium ferricyanide 0.1mol/L phosphate buffer solutions.
Under external 1000 Ω loads, battery passes through the operation culture of 3 days or so, and stable operating voltage is left in 0.410V
The right side, peak power output density is close to 400mWm-2, the Ω of apparent internal resistance internal resistance 151 is shown in Fig. 4.
Embodiment three
Microorganism electrode is used as sensor electrode
Microorganism electrode described in embodiment one is used as sensor and platinum electrode (to electrode) and saturated calomel electrode (ginseng
Than electrode) and three-electrode system is constituted, three kinds of substrate solutions such as 10mmol/L maltose, glucose and aniline are entered respectively respectively
Row cyclic voltammetry.The cyclic voltammetry curve of three kinds of obtained substrates, the position that reduction peak occurs is significantly different, such as Fig. 5 institutes
Show.
Three-electrode system is built using the biology sensor, cyclic voltammetric surface sweeping is carried out to the glucose solution of various concentrations
Detection, as Pu Tang inquires into concentration increase, the reduction peak of cyclic voltammetry curve is constantly raised, as shown in Figure 6.By -0.274V places
Corresponding reduction peak current value is mapped with glucose concentration, and does linear regression analysis, and coefficient R is deposited between the two is
0.98204。
Claims (10)
1. a kind of preparation method of microorganism electrode, it is characterised in that comprise the following steps：
(1) monomer solution before the polymerization of regulation conductive hydrogel, makes the conditions such as its pH, temperature be suitable to microbe survival.
(2) appropriate electro-chemical activity microorganism is added into conductive hydrogel polycondensation monomer solution, microbial cell is formed and uniformly divides
Scattered bacteria suspension.
(3) inactive, conductive material is immersed in bacteria suspension, conductive hydrogel monomer polymerizing curable is then made in a mild condition, will
Electro-chemical activity microorganism is fixed in conductive hydrogel after shaping, forms microorganism electrode.
2. according to the method described in claim 1, it is characterised in that the conductive hydrogel described in step (1) is polyaniline/poly- second
Enol composite conducting hydrogel.
3. method according to claim 2, it is characterised in that the preparation of the microorganism battery is concretely comprised the following steps：
(1) 0.46ml aniline is added in 2.0mL10% poly-vinyl alcohol solutions and is configured to solution A.Weigh 0.25g ammonium persulfates molten
Solution obtained solution B in 0.5mL deionized waters.By two kinds of solution be cooled to 4 DEG C it is standby.
(2) disperse in foregoing solution A after 20mg Escherichia coli, make A, B solution mixing, a branch of inertia is immersed in mixed solution
Conductive material, makes it solidify in -10 DEG C of freezings, then melts at 4 DEG C, repeatedly for three times, makes composite conducting hydrogel completely solid
Change and form the thick conductive hydrogel film layers of about 3mm.
(3) conductive hydrogel containing Escherichia coli after solidifying is soaked in deionized water 6 hours, removes unpolymerized phytic acid
Deng small-molecule substance, that is, complete the structure of microorganism electrode.
4. method according to claim 3, it is characterised in that during solution A in preparation steps (1), add
0.92mL50% phytic acid is used as dopant.
5. the method according to any one of Claims 1-4, it is characterised in that described inactive, conductive material is to lead
Electro-graphitic fiber.
6. a kind of microorganism electrode, it is characterised in that be prepared from according to the method described in 1 to 5 any one.
7. the application of the microorganism electrode described in a kind of claim 6, it is characterised in that the microorganism electrode is mainly used in micro-
The bioelectrode of biological fuel cell.
8. application according to claim 7, it is characterised in that described bioelectrode is anode of microbial fuel cell.
9. the application of the microorganism electrode described in a kind of claim 6, it is characterised in that the microorganism electrode is mainly used in micro-
Biology sensor.
10. application according to claim 9, it is characterised in that described microbiological sensor is electrochemistry type.
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Cited By (2)
| Publication number | Priority date | Publication date | Assignee | Title |
|---|---|---|---|---|
| CN107843624A (en) * | 2017-09-14 | 2018-03-27 | 中国肉类食品综合研究中心 | For detecting the detection means and its detection method of total plate count in food |
| CN113960141B (en) * | 2021-09-26 | 2023-10-20 | 武汉新烽光电股份有限公司 | Preparation method of immobilized microbial membrane for measuring BOD of seawater |
Citations (1)
| Publication number | Priority date | Publication date | Assignee | Title |
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| CN204809327U (en) * | 2015-06-20 | 2015-11-25 | 天津天狮学院 | Microbiological fuel cell positive pole |
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2017
- 2017-05-04 CN CN201710327792.7A patent/CN106981668A/en active Pending
Patent Citations (1)
| Publication number | Priority date | Publication date | Assignee | Title |
|---|---|---|---|---|
| CN204809327U (en) * | 2015-06-20 | 2015-11-25 | 天津天狮学院 | Microbiological fuel cell positive pole |
Non-Patent Citations (1)
| Title |
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| 邢达杰等: "导电水凝胶包埋大肠杆菌制备微生物传感器", 《电子技术与软件工程》 * |
Cited By (3)
| Publication number | Priority date | Publication date | Assignee | Title |
|---|---|---|---|---|
| CN107843624A (en) * | 2017-09-14 | 2018-03-27 | 中国肉类食品综合研究中心 | For detecting the detection means and its detection method of total plate count in food |
| CN107843624B (en) * | 2017-09-14 | 2020-06-02 | 中国肉类食品综合研究中心 | Detection device and detection method for detecting total number of bacterial colonies in food |
| CN113960141B (en) * | 2021-09-26 | 2023-10-20 | 武汉新烽光电股份有限公司 | Preparation method of immobilized microbial membrane for measuring BOD of seawater |
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