CN113410499A - Method for improving electricity generation performance of microbial fuel cell - Google Patents
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- H—ELECTRICITY
- H01—ELECTRIC ELEMENTS
- H01M—PROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
- H01M8/00—Fuel cells; Manufacture thereof
- H01M8/16—Biochemical fuel cells, i.e. cells in which microorganisms function as catalysts
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- C—CHEMISTRY; METALLURGY
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- C08G—MACROMOLECULAR COMPOUNDS OBTAINED OTHERWISE THAN BY REACTIONS ONLY INVOLVING UNSATURATED CARBON-TO-CARBON BONDS
- C08G73/00—Macromolecular compounds obtained by reactions forming a linkage containing nitrogen with or without oxygen or carbon in the main chain of the macromolecule, not provided for in groups C08G12/00 - C08G71/00
- C08G73/06—Polycondensates having nitrogen-containing heterocyclic rings in the main chain of the macromolecule
- C08G73/0605—Polycondensates containing five-membered rings, not condensed with other rings, with nitrogen atoms as the only ring hetero atoms
- C08G73/0611—Polycondensates containing five-membered rings, not condensed with other rings, with nitrogen atoms as the only ring hetero atoms with only one nitrogen atom in the ring, e.g. polypyrroles
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- C08G73/00—Macromolecular compounds obtained by reactions forming a linkage containing nitrogen with or without oxygen or carbon in the main chain of the macromolecule, not provided for in groups C08G12/00 - C08G71/00
- C08G73/06—Polycondensates having nitrogen-containing heterocyclic rings in the main chain of the macromolecule
- C08G73/0666—Polycondensates containing five-membered rings, condensed with other rings, with nitrogen atoms as the only ring hetero atoms
- C08G73/0672—Polycondensates containing five-membered rings, condensed with other rings, with nitrogen atoms as the only ring hetero atoms with only one nitrogen atom in the ring
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- 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
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Abstract
The invention belongs to the field of microbial electrochemistry and discloses a method for improving the electricity generation performance of a microbial fuel cell, which adopts a biocompatible means to sequentially and functionally modify a conductive polymer polypyrrole (PPy) and Polydopamine (PDA) on the surface of an electricity generation bacterium to form the PDA @ PPy @ electricity generation bacterium which sequentially comprises the electricity generation bacterium, the polypyrrole and the polydopamine from inside to outside; the modification of the polypyrrole greatly accelerates the electron transfer rate, the modification of the polydopamine promotes the adhesion biomass on the surface of the electrode, and the promotion effect of the polypyrrole on the extracellular electron transfer capability of the electrogenic bacteria is further exerted. Compared with the unmodified bacterial MFC, the output voltage of the MFC modified by polydopamine and polypyrrole is 4.6 times that of the unmodified bacterial MFC, and the maximum power density of the MFC modified by polydopamine and polypyrrole is 11.8 times that of the unmodified bacterial MFC. The method has the advantages of universality, stable effect and the like, and provides a method for effectively improving the power generation performance of the MFC.
Description
Technical Field
The invention belongs to the field of microbial electrochemistry, and particularly relates to a method for improving the electricity generation performance of a microbial fuel cell.
Background
Energy and environmental issues are two major issues facing the world today. The use of fossil energy is accompanied by the consumption of energy and the generation of environmental problems, and therefore, it is of great significance to develop and utilize cleanable energy while solving environmental problems. Microbial Fuel Cells (MFCs) are a technology that integrates application functions such as sewage treatment, power generation, sensing monitoring, green energy recovery, and the like. By attaching the electrogenic microorganisms on the surface of the anode, the electrogenic bacteria metabolize and degrade organic matters and generate electrons, and the electrons are collected by the electric circuit, so that the application of MFC in the field of electrogenesis is realized. The microbial fuel cell can generate electricity simultaneously in the process of sewage degradation, can solve the problem of too large power consumption of a sewage treatment plant, and has good engineering application prospect.
The MFC electricity generation efficiency is mainly influenced by the electron transfer rate between the electricity generating bacteria and the anode, and the electron transfer process is divided into two steps of intracellular electron transfer and extracellular electron transfer. Intracellular electron transfer refers primarily to the transfer from an electron donor to an intracellular terminal electron acceptor (such as the extracellular membrane chromoprotein). The transfer process of the intracellular electrons conforms to the Moruo equation, and the transfer rate of the intracellular electrons must be increased from the aspect of increasing the content of active electrogenic bacteria in the anode biomembrane. Extracellular electron transfer refers to the transfer of electrons from the outer membrane of a microorganism to the anode, and there are three main ways of electron transfer. The first is direct electron transfer by protein-cytochrome (such as C-type cytochrome) with redox property on the cell membrane of the electrogenic bacteria by directly contacting the electrogenic bacteria with the anode; the second mode is indirect electron transfer through the secretion of soluble electron mediators (flavin, phenazine, etc.) by the electrogenic bacteria; the third way is to carry out remote electronic transmission through some outer membrane nanowires of the electrogenic bacteria. The high current density of the microbial electrochemical system is the basis of application, so that the improvement of the electricity generation efficiency of the MFC from the aspect of improving the electron rate transfer is of great significance to the application of the MFC.
The anode electrogenesis biomembrane is a biocatalyst for oxidizing organic matters by the MFCs, is a root for realizing electric energy recovery by the MFCs and carrying out sensing by using an electric signal. The electrogenic biofilms in MFCs are usually acclimatized and enriched from the environment, and the number, density and microbial species of the anode biofilms are significantly influenced by external conditions such as fluid morphology, pH, temperature, substance diffusion and the like. Therefore, most of the existing researches improve the electricity generation performance of the MFC by researching and developing a novel carrier material and optimizing the configuration and the operating conditions of the reactor. However, the above methods cannot fundamentally solve the problem of limiting the transfer rate of electrons from the outside of the cell, and the electron transfer capability of the anode microorganism is the main factor limiting the performance of MFCs. Therefore, a method for fundamentally regulating and controlling the electric activity of the electrogenic biomembrane and improving the electrogenic performance of the MFC needs to be found.
The cell surface modification technology is a technology for modifying a biocompatible material on the cell surface by adopting methods such as electrostatic adsorption, covalent crosslinking and the like and realizing the functional modification of the cell surface through artificial shell making. The cell surface modification technology is mainly applied to the fields of biomedicine, biotechnology and bioelectronics at present, and the catalytic metabolism capability or the environmental stress resistance capability of cells is improved through the modification technology. The modification materials studied at present mainly include materials such as minerals (silica, titanium dioxide, calcium carbonate, hydrogel, polymers, graphene, metal-organic complexes) and the like.
Disclosure of Invention
In view of the above defects or needs for improvement in the prior art, the present invention aims to provide a method for improving the electricity generation performance of a microbial fuel cell, wherein by modifying conductive polymers polypyrrole and polydopamine on the surface of shewanella bacterium, the extracellular direct electron transfer capability of the electricity generating bacterium is improved, the electron transfer distance of an electron mediator is shortened, meanwhile, the adhesion biomass on the surface of an anode is improved, and the electricity generation efficiency of the microbial fuel cell MFC is improved; compared with the unmodified bacterial MFC, the output voltage of the MFC modified by polydopamine and polypyrrole is 4.6 times that of the unmodified bacterial MFC, and the maximum power density of the MFC is 11.8 times that of the unmodified bacterial MFC. The method has the advantages of universality, stable effect and the like, and provides a method for effectively improving the power generation performance of the MFC.
In order to achieve the purpose, the invention provides a method for improving the electricity generation performance of a microbial fuel cell, which is characterized in that a biocompatible means is adopted to sequentially modify conductive polymers polypyrrole (PPy) and Polydopamine (PDA) on the surface of an electricity generation bacterium to form the PDA @ PPy @ electricity generation bacterium which sequentially comprises the electricity generation bacterium, the polypyrrole and the polydopamine from inside to outside; the modification of the polypyrrole greatly accelerates the electron transfer rate, the modification of the polydopamine promotes the adhesion biomass on the surface of the electrode, and the promotion effect of the polypyrrole on the extracellular electron transfer capability of the electrogenic bacteria is further exerted; the polypyrrole and polydopamine modification are used for optimizing the characteristics of the biological membrane, so that the electricity generation efficiency of the microbial fuel cell MFC is improved.
As a further optimization of the invention, the conductive polymers polypyrrole PPy and polydopamine PDA are sequentially and functionally modified on the surface of the electrogenesis bacteria by adopting a biocompatible means, and specifically, Fe is firstly added into the suspension of the electrogenesis bacteria3+Ionic followed by addition of pyrrole to bring the pyrrole to Fe3+Polymerizing under the catalysis of ions to obtain the electricity-generating bacteria with polypyrrole modified on the surface; then, generating electricity to the generatorAnd continuously adding dopamine into the bacteria suspension to ensure that the dopamine is subjected to self-polymerization on the electricity-generating bacteria of which the surfaces are modified with polypyrrole to form polydopamine.
As a further preferred aspect of the present invention, said Fe3+The ion is in particular Fe (NO)3)3·9H2Said Fe (NO) added to said suspension of said electrogenic bacteria in the form of O3)3·9H2The concentration of O in the electrogenic bacteria suspension is 5-15mmol/L, and the modification time is 20-40 min;
before polymerization reaction of pyrrole occurs, the concentration of the pyrrole in the electrogenesis bacteria suspension is 0.6-1.2 muL/mL, and the modification time is 2-8 h;
before the dopamine self-polymerization reaction occurs, the concentration of the dopamine in the electrogenesis bacteria suspension is 1-10mmol/L correspondingly, and the modification time is 10-30 min.
As a further preferred aspect of the present invention, said Fe3+The ion is in particular Fe (NO)3)3·9H2Said Fe (NO) added to said suspension of said electrogenic bacteria in the form of O3)3·9H2The concentration of O in the electrogenic bacteria suspension is 7.5mmol/L, and the modification time is 30 min;
before polymerization reaction of pyrrole occurs, the concentration of the pyrrole in the electrogenesis bacteria suspension is 0.88 mu L/mL correspondingly, and the modification time is 3 h;
before the dopamine self-polymerization reaction occurs, the concentration of the dopamine in the electrogenesis bacteria suspension is 2mmol/L correspondingly, and the modification time is 15 min.
As a further optimization of the invention, the polypyrrole and polydopamine modification are utilized to optimize the characteristics of the biomembrane, so that the electricity generation efficiency of the microbial fuel cell MFC is improved, and specifically, bacterial suspension of the electricity generation bacteria, the polypyrrole and polydopamine PDA @ PPy @ electricity generation bacteria in sequence from inside to outside is inoculated into the microbial fuel cell MFC reactor, and the electricity generation bacteria form a film on the surface of the anode after the MFC runs for one period.
As a further preferred aspect of the present invention, the microbial fuel cell MFC is configured such that the anolyte and the catholyte of the microbial fuel cell MFC are replaced with the anolyte and the catholyte each containing no electrogenic bacteria after the inoculation operation for one cycle.
In a further preferred embodiment of the present invention, the electrogenic bacterium is shewanella.
Compared with the prior art, the technical scheme of the invention has the advantages that the polymer is used for modifying the electrogenesis bacteria, the polymer is directly modified on the surfaces of the electrogenesis bacteria, the conductivity and the high adhesiveness of the modified polymer are used for enhancing the extracellular electronic capacity of the electrogenesis bacteria, and meanwhile, the electrogenesis performance of the MFC is optimized to the greatest extent by improving the amount of the anode surface biomembrane. By constructing the electricity generating biomembrane with high electron transfer efficiency, the electricity generating bacteria are directly started, the extracellular electron transfer rate of the electricity generating bacteria is fundamentally improved, and the problem that the electricity generating efficiency of the MFC is limited due to the extracellular electron transfer rate is solved. The invention has the advantages of universality, stable effect and the like, effectively improves the power generation performance of the MFC, and accelerates the practical application process of the MFC.
The first key for realizing functional application by using a cell surface modification technology is biological compatibility in the modification process, and at present, many researches adopt a bionic principle to modify, are inspired by organisms in the nature, and construct an artificial shell in a high-degree biological compatibility and functional mode to regulate cell behaviors. The functional modification material is selected, the extracellular electron transfer capability and the film forming property of the electrogenic bacteria are optimized, and the high-electric activity biomembrane is constructed to improve the electrogenic performance of the MFC. The invention utilizes the conductivity of the polypyrrole to improve the extracellular electron transfer rate of the electrogenic bacteria, but the modification of the polypyrrole reduces the adhesiveness of the electrogenic bacteria, and the Shewanella is difficult to form a film or the formed film is thinner, so the invention utilizes the high adhesiveness of the polydopamine to overcome the defect, which is beneficial to improving the microbial biomass on the surface of the anode, and can further play the modifying role of the polypyrrole on the electrogenic bacteria, thereby optimizing the electrical activity and the biomass of the electrogenic biomembrane and improving the electrogenic efficiency of the MFC. The invention adopts a biocompatible means to construct artificial conductive cell walls (polypyrrole and polydopamine) on the surfaces of the electrogenic bacteria, wherein the modification of the polypyrrole greatly shortens the extracellular electron transfer distance of the electrogenic bacteria, accelerates the electron transfer rate, improves the adhesion biomass on the electrode surface by the modification of the polydopamine, optimizes the problem that the electrogenic bacteria (such as Shewanella) are difficult to form films, and further plays a role in promoting the extracellular electron transfer capability of the electrogenic bacteria by the polypyrrole, thereby effectively improving the electrogenic performance of the MFC sensor. The method has universality, can be applied to various microbial systems, and accelerates the power generation application process of the MFC.
The modification means and materials adopted by the invention are both biocompatible, and the modification process can not cause significant influence on the biological activity. The invention firstly modifies the conductive polymer polypyrrole PPy and then modifies the polydopamine PDA, for example, iron ions can be adsorbed through the electrostatic action of microorganisms, and polydopamine is modified after a layer of polypyrrole is coated on the surface of bacteria, so that negative effects on the activity of the electrogenic bacteria can not be caused. And the invention adopts a layer-by-layer modification method to obtain the polymer modified electrogenesis bacteria, firstly modifying the surface of the electrogenesis bacteria with conductive polymer polypyrrole, and then modifying a layer of polydopamine to improve the adhesion of the electrogenesis bacteria on the anode surface, and optimizing the influence of the conductive property of the polypyrrole on the electrogenesis biomembrane to the greatest extent. The invention further controls the time and concentration of the added polymer monomer, so that the polymer can be modified on the surface of the electrogenesis bacteria (such as Shewanella) on the premise of not influencing the activity of the electrogenesis bacteria.
Drawings
FIG. 1 is a SEM and TEM representation; in the figure, the top 3 sub-images from left to right and from top to bottom correspond to SEM images of unmodified bacteria, PPy @ Bacterial and PDA @ PPy @ Bacterial, respectively, and the last 3 sub-images are TEM images of unmodified bacteria, PPy @ Bacterial and PDA @ PPy @ Bacterial, respectively.
FIG. 2 is a graph showing the effect of polymer modification on the activity of electrogenic bacteria.
Fig. 3 is a graph of MFC power production.
FIG. 4 is a schematic diagram showing the structure of a biofilm obtained by the polymer modification treatment of the present invention compared with a conventional biofilm obtained without the modification treatment.
Detailed Description
In order to make the objects, technical solutions and advantages of the present invention more apparent, the present invention is described in further detail below with reference to the accompanying drawings and embodiments. It should be understood that the specific embodiments described herein are merely illustrative of the invention and are not intended to limit the invention. In addition, the technical features involved in the embodiments of the present invention described below may be combined with each other as long as they do not conflict with each other.
Generally, taking shewanella as an example of an electrogenic bacterium, the invention modifies polymer polypyrrole and polydopamine on the surface of the shewanella, inoculates an MFC reactor with the modified electrogenic bacterium, and applies the modified electrogenic bacterium to MFC electrogenesis. The difference in production efficiency can be analyzed and compared by inoculating the MFC reactor with unmodified bacteria (unmodified) and modified shewanella bacteria, respectively.
Examples
Modification of electrogenic bacteria: selecting pure Shewanella as an electrogenic bacterium object, adopting a layer-by-layer modification method, and firstly adsorbing Fe on the surface of the electrogenic bacterium through electrostatic adsorption3+Preferably, Fe (NO)3)3·9H2The O concentration is 7.5mmol/L, and the modification time is 30 min; centrifuging, resuspending, adding pyrrole monomer, preferably 0.88 μ L/mL, into the suspension of the electrogenic bacteria, modifying for 3h, and passing through Fe3+The polypyrrole is modified on the surface of the electrogenic bacteria to obtain PPy @ Bacterial. And further adding a dopamine monomer into the Bacterial suspension, preferably, the concentration of the dopamine monomer is 2mmol/L, the modification time is 15min, and modifying a polydopamine layer on the surface of the electrogenic bacteria through dopamine self-polymerization to obtain PDA @ PPy @ background.
(II) SEM/TEM characterization and activity characterization: unmodified bacteria (unmodified bacteria), PPy @ Bacterial and PDA @ PPy @ Bacterial samples were fixed with 2% formaldehyde overnight, washed three times with sterile 50mM Phosphate Buffer Saline (PBS), and then dehydrated with 25%, 50%, 75%, 95%, 100% (three times) gradients, each time for 15 min. Dropping the alcohol suspension of the bacteria on a conductive substrate, drying, spraying platinum, and performing SEM test on a machine. In the TEM test, the alcohol suspension of the bacteria is dropped on a copper net, and the bacteria are tested on a machine after being dried. The influence of polymer modification on the activity of Shewanella is quantitatively analyzed by a fluorescence spectrum method. The labeled substances were formulated with 100% live bacteria (using Shewanella without any polymer modification) and 100% dead bacteria (using a bacterial suspension of live bacteria after 20min of high temperature sterilization at 121 ℃). After the live and dead bacteria are washed three times by 0.9% NaCl solution, the bacteria are diluted to the density of OD600 about 0.3, and the live and dead bacteria are respectively proportioned to be 0%, 10%, 50%, 90% and 100%. Staining was performed using LIVE/DEAD back Bacterial staining Kits with staining solutions of 1: SYTO 9 of 1: and adding 9 mu L of mixed dye solution into each 3mL of bacterial solution of propidium iodide mixed dye solution. And dyeing for 30min in dark place, and testing on a machine. And selecting a fluorescence spectrum scanning mode, wherein the fixed excitation wavelength is 490nm, and the scanning emission wavelength range is 490nm-700 nm. The integral areas of the fluorescence spectrum curves under 510nm-540nm (green fluorescence) and 620nm-650nm (red fluorescence) are respectively calculated, and the ratio of the live bacteria and the dead bacteria in different known ratios and the ratio of the green fluorescence to the red fluorescence in the ratio are used for drawing, so that the standard curve can be obtained. The determination process of the unknown sample is consistent with the standard curve determination method, the unmodified bacteria, the polypyrrole modified bacteria, the polypyrrole and polydopamine double modified bacteria are respectively cleaned, diluted, dyed and scanned by fluorescence spectrum, the ratio of green fluorescence to red fluorescence is obtained, and the proportion of live bacteria and dead bacteria is obtained by standard curve calculation.
(III) establishment and activation of MFC sensors: the MFC reactor adopts an MFC double-chamber bottle type reactor, the volumes of an anode chamber and a cathode chamber of the bottle type reactor are respectively 100mL, the middle parts of the anode chamber and the cathode chamber are separated by a proton exchange membrane, and preferably, the middle parts of the anode chamber and the cathode chamber are separated by a Nafion 117 proton exchange membrane; the anode and cathode materials are carbon felts with the size of 2cm multiplied by 0.5 cm; the external circuit of the reactor adopts a resistance of 1000 omega to connect the anode and the cathode. After the reactor is assembled, the reactor is placed in a high-temperature sterilization pot for high-temperature sterilization at 121 ℃ for 20min for standby. The LB medium and PBS are aerated by nitrogen for 20min, and then sterilized at 121 ℃ for 20 min. Filtering the mineral solution and vitamin solution with 0.22 μm filter membrane, and irradiating with ultraviolet lamp for 30 min.
Respectively dispersing unmodified bacteria and modified bacteria suspension in culture solution for inoculation. The culture solution is prepared by using 5mL of LB culture medium, 1g/L of sodium acetate, 1.25mL of mineral solution and 0.5mL of vitamin solution, and 100mL of PBS is added to the volume of 100 mL. Respectively inoculating the unmodified bacteria and the modified bacteria suspension into an MFC reactor, inoculating for a period (more than 4-5 days) to form a film, and then replacing the MFC anolyte with a pure culture solution containing no electrogenic bacteria. Catholyte was prepared by dissolving 1.65g of potassium ferricyanide (50mM) and 0.75g of potassium chloride in 100mL of PBS. After the catholyte is injected into the cathode chamber, the cathode chamber is wrapped by tinfoil paper to avoid light. The voltage is acquired by adopting a keithley data acquisition instrument, and data is recorded every 10 min.
Analysis of Experimental results
The effect of polymer modification on the surface morphology of bacteria was characterized using SEM and TEM, and the results are shown in fig. 1. As can be seen from the SEM image, the surface of the unmodified bacteria is smooth, and the surface fluctuation is probably caused by the dehydration of gradient alcohol in the sample preparation process. Compared with unmodified bacteria, the PPy @ Bacterial has flaky substances on the surface, which shows that the modification process of polypyrrole can cause the morphological difference on the surface of the bacteria. After the poly-dopamine is re-modified, the substance coated on the surface of the bacteria becomes thicker, but the surface of the coating layer is smoother than that of the polypyrrole layer. Polydopamine is very easy to covalently cross-link with the surface of the material due to its abundant active groups. The re-modification of dopamine in the invention also aims to overcome the defect of conductive polypyrrole (difficult adhesion to the surface of a material) by utilizing the high adhesion of polydopamine, thereby fully exerting the conductive optimization characteristic of polypyrrole. According to TEM results, the surface of unmodified bacteria is very smooth, and the surface of Shewanella is coated with a layer of polymer after polypyrrole modification, so that the surface of Shewanella becomes uneven. And the modification of polydopamine enables the whole thallus to be wrapped in flocculent polymers, and each thallus is connected together through flocculent. SEM images and TEM images show that Shewanella thallus is wrapped by the polymer due to the modification of the polymer, and the surface morphology is obviously changed.
The modification method must not affect the activity of bacteria, and the living and dead cells are quantitatively analyzed by adopting a fluorescence staining marker of the bacteria and then a fluorescence spectrometer, and the result is shown in figure 2. The control was 100% unmodified strain, as can be seen from the figureOut of Fe3+The modification(s) does not affect the cellular activity at all. After 3h of pyrrole polymerization culture, only a few dead cells (1.89%) appear, which indicates that the pyrrole polymerization reaction does not cause significant influence on the cell activity. Then modifying dopamine on the surface of the polypyrrole-modified bacteria, and increasing the content of dead cells to 5.55%. In general, since pyrrole and dopamine are both biocompatible and the polymerization process is very mild, the bacterial activity is not significantly affected.
The pure bacteria MFC reactor is adopted to be inoculated for a cycle of operation and then operated in a mode of replacing sterile culture solution. As can be seen from FIG. 3, the maximum output voltage of the PDA @ PPy @ pure bacteria reactor is about 188mV, the maximum output voltage of the PPy @ pure bacteria reactor is about 107mV, and the maximum output voltage of the unmodified bacteria reactor is only about 58 mV. When the output voltage of the three groups of reactors is lower than 50mV, the sterile matrix solution is replaced. The maximum output voltage platform of the unmodified bacteria MFC reactor is about 57mV, which is not much different from the inoculation period. The highest output voltage of the PPy @ pure bacteria reactor is about 115mV, compared with about 2 times of that of an unmodified bacteria reactor, the polypyrrole can accelerate the direct electron transfer efficiency between the microorganism and the electrode and shorten the indirect electron transfer distance, so that the electricity generation efficiency of the MFC is improved. The maximum output voltage of the PDA @ PPy @ pure bacteria reactor reaches 265mV, the duration time of the high output voltage is prolonged, and the maximum output voltage is 4.6 times that of the unmodified bacteria MFC. Most probably, after one period of inoculation operation, a large number of bacteria modified by the high-adhesion PDA are attached to the surface of the electrode to form a film, so that the problem that Shewanella and a conductive polymer are difficult to adsorb to form a film due to modification is solved, the conductive effect of the conductive polymer polypyrrole can be exerted to a greater extent, and the electricity generation efficiency of the MFC is greatly improved.
The components of the microbial fuel cell MFC sensor in the present invention are commercially available or can be self-constructed according to the prior art. The source of the inoculated microorganisms is purchased from a strain preservation center, and the modification method has universality and can also be used for stably operating MFC anolyte or water inlet of a sewage treatment plant.
The above examples are only exemplified by Shewanella,the method has universality and can be applied to various electricigens. In addition to the concentrations and modification times used in the above examples, the concentrations and modification times can be flexibly varied according to the actual conditions, for example, Fe (NO)3)3·9H2The concentration of O can also be other values within the range of 5-15mmol/L, and the corresponding modification time can also be changed within the range of 20-40 min; the concentration of pyrrole monomer can also be other values within the range of 0.6-1.2 muL/mL, and the corresponding modification time can be changed within the range of 2-8 h; the concentration of dopamine may be other values in the range of 1-10mmol/L, and the corresponding modification time may vary in the range of 10-30 min.
The buffer solution used in the present invention is a phosphate buffer solution. The nitrogen gas in the present invention is nitrogen gas having a purity of not less than 99.99%. The anode used in the experiment was carbon felt, and electrodes such as carbon cloth, graphite plate, graphite rod, etc. were also used. The MFC sensor may adopt a bottle-type single-chamber structure or a cubic single-chamber structure in addition to the bottle-type double-chamber structure in the above-described embodiment. The buffer solution suitable for use in the present invention may be a 10-100mM phosphate buffer solution, in addition to the 50mM and 100mM phosphate buffer solutions used in the above experiments. In addition, in addition to sodium acetate as a carbon source used in the above embodiment, glucose, methanol or a carbohydrate may be used as a carbon source.
It will be understood by those skilled in the art that the foregoing is only a preferred embodiment of the present invention, and is not intended to limit the invention, and that any modification, equivalent replacement, or improvement made within the spirit and principle of the present invention should be included in the scope of the present invention.
Claims (7)
1. A method for improving the electricity generating performance of a microbial fuel cell is characterized in that a biocompatible means is adopted to sequentially modify conductive polymers polypyrrole (PPy) and Polydopamine (PDA) on the surface of an electricity generating bacterium to form the PDA @ PPy @ electricity generating bacterium which sequentially comprises the electricity generating bacterium, the polypyrrole and the polydopamine from inside to outside; the modification of the polypyrrole greatly accelerates the electron transfer rate, the modification of the polydopamine promotes the adhesion biomass on the surface of the electrode, and the promotion effect of the polypyrrole on the extracellular electron transfer capability of the electrogenic bacteria is further exerted; the polypyrrole and polydopamine modification are used for optimizing the characteristics of the biological membrane, so that the electricity generation efficiency of the microbial fuel cell MFC is improved.
2. The method of claim 1, wherein the electrically conductive polymers polypyrrole PPy and polydopamine PDA are functionally modified sequentially on the surface of the electrogenic bacteria by a biocompatible means, specifically by adding Fe to the suspension of the electrogenic bacteria3+Ionic followed by addition of pyrrole monomer to bring pyrrole to Fe3+Polymerizing under the catalysis of ions to obtain the electricity-generating bacteria with polypyrrole modified on the surface; and then, continuously adding a dopamine monomer into the electrogenesis bacteria suspension to enable dopamine to undergo self-polymerization on the electrogenesis bacteria of which the surfaces are modified with polypyrrole to form polydopamine.
3. The method of claim 2, wherein the Fe is3+The ion is in particular Fe (NO)3)3·9H2Said Fe (NO) added to said suspension of said electrogenic bacteria in the form of O3)3·9H2The concentration of O in the electrogenic bacteria suspension is 5-15mmol/L, and the modification time is 20-40 min;
before polymerization reaction of pyrrole occurs, the concentration of the pyrrole in the electrogenesis bacteria suspension is 0.6-1.2 muL/mL, and the modification time is 2-8 h;
before the dopamine self-polymerization reaction occurs, the concentration of the dopamine in the electrogenesis bacteria suspension is 1-10mmol/L correspondingly, and the modification time is 10-30 min.
4. The method of claim 2, wherein the Fe is3+The ion is in particular Fe (NO)3)3·9H2Said Fe (NO) added to said suspension of said electrogenic bacteria in the form of O3)3·9H2The concentration of O in the electrogenic bacteria suspension is 7.5mmol/L, and the modification time is 30 min;
before polymerization reaction of pyrrole occurs, the concentration of the pyrrole in the electrogenesis bacteria suspension is 0.88 mu L/mL correspondingly, and the modification time is 3 h;
before the dopamine self-polymerization reaction occurs, the concentration of the dopamine in the electrogenesis bacteria suspension is 2mmol/L correspondingly, and the modification time is 15 min.
5. The method according to claim 1, wherein the polypyrrole and polydopamine modification are used for optimizing the characteristics of the biological membrane to improve the electricity generation efficiency of the microbial fuel cell MFC, and specifically, bacterial suspensions of the electricity-generating bacteria, the PDA @ PPy @ electricity-generating bacteria of the polypyrrole and polydopamine are inoculated into the microbial fuel cell MFC reactor from inside to outside in sequence, and the electricity-generating bacteria form a membrane on the surface of an anode after one-cycle operation of the MFC.
6. The method according to any one of claims 1 to 5, wherein the microbial fuel cell MFC is one in which the anolyte and catholyte of the microbial fuel cell MFC are exchanged for anolyte and catholyte without electrogenic bacteria after one cycle of operation for inoculation.
7. The method according to any one of claims 1 to 6, wherein the electrogenic bacteria are Shewanella.
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