CN111082116A - Electricity generating device and electricity generating method of hollow fiber membrane assembly used as methane-driven microbial fuel cell anode - Google Patents
Electricity generating device and electricity generating method of hollow fiber membrane assembly used as methane-driven microbial fuel cell anode Download PDFInfo
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- VNWKTOKETHGBQD-UHFFFAOYSA-N methane Chemical compound C VNWKTOKETHGBQD-UHFFFAOYSA-N 0.000 title claims abstract description 121
- 239000012528 membrane Substances 0.000 title claims abstract description 73
- 239000012510 hollow fiber Substances 0.000 title claims abstract description 62
- 230000000813 microbial effect Effects 0.000 title claims abstract description 55
- 239000000446 fuel Substances 0.000 title claims abstract description 49
- 230000005611 electricity Effects 0.000 title claims abstract description 28
- 238000000034 method Methods 0.000 title claims abstract description 18
- 239000007789 gas Substances 0.000 claims abstract description 37
- 239000000758 substrate Substances 0.000 claims abstract description 15
- 229910000831 Steel Inorganic materials 0.000 claims abstract description 9
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- 229910052799 carbon Inorganic materials 0.000 claims abstract description 6
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- 239000007787 solid Substances 0.000 claims description 16
- HEMHJVSKTPXQMS-UHFFFAOYSA-M Sodium hydroxide Chemical compound [OH-].[Na+] HEMHJVSKTPXQMS-UHFFFAOYSA-M 0.000 claims description 15
- 229920000049 Carbon (fiber) Polymers 0.000 claims description 14
- 239000004917 carbon fiber Substances 0.000 claims description 14
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- 238000007254 oxidation reaction Methods 0.000 claims description 12
- 238000010248 power generation Methods 0.000 claims description 11
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- 239000003792 electrolyte Substances 0.000 claims description 5
- 230000002572 peristaltic effect Effects 0.000 claims description 5
- UXVMQQNJUSDDNG-UHFFFAOYSA-L Calcium chloride Chemical compound [Cl-].[Cl-].[Ca+2] UXVMQQNJUSDDNG-UHFFFAOYSA-L 0.000 claims description 4
- 229910021580 Cobalt(II) chloride Inorganic materials 0.000 claims description 4
- 229910021380 Manganese Chloride Inorganic materials 0.000 claims description 4
- GLFNIEUTAYBVOC-UHFFFAOYSA-L Manganese chloride Chemical compound Cl[Mn]Cl GLFNIEUTAYBVOC-UHFFFAOYSA-L 0.000 claims description 4
- 229910004619 Na2MoO4 Inorganic materials 0.000 claims description 4
- 239000001110 calcium chloride Substances 0.000 claims description 4
- 229910001628 calcium chloride Inorganic materials 0.000 claims description 4
- 229910052927 chalcanthite Inorganic materials 0.000 claims description 4
- XLYOFNOQVPJJNP-ZSJDYOACSA-N heavy water Substances [2H]O[2H] XLYOFNOQVPJJNP-ZSJDYOACSA-N 0.000 claims description 4
- 229910001629 magnesium chloride Inorganic materials 0.000 claims description 4
- 239000011565 manganese chloride Substances 0.000 claims description 4
- 229910052757 nitrogen Inorganic materials 0.000 claims description 4
- 239000011684 sodium molybdate Substances 0.000 claims description 4
- NWONKYPBYAMBJT-UHFFFAOYSA-L zinc sulfate Chemical compound [Zn+2].[O-]S([O-])(=O)=O NWONKYPBYAMBJT-UHFFFAOYSA-L 0.000 claims description 4
- 229910000368 zinc sulfate Inorganic materials 0.000 claims description 4
- 239000011686 zinc sulphate Substances 0.000 claims description 4
- 241000203069 Archaea Species 0.000 claims description 3
- 239000007836 KH2PO4 Substances 0.000 claims description 3
- 229910020350 Na2WO4 Inorganic materials 0.000 claims description 3
- 229910021586 Nickel(II) chloride Inorganic materials 0.000 claims description 3
- 239000002033 PVDF binder Substances 0.000 claims description 3
- 229910018143 SeO3 Inorganic materials 0.000 claims description 3
- 238000007599 discharging Methods 0.000 claims description 3
- 229910052603 melanterite Inorganic materials 0.000 claims description 3
- 229910000402 monopotassium phosphate Inorganic materials 0.000 claims description 3
- QMMRZOWCJAIUJA-UHFFFAOYSA-L nickel dichloride Chemical compound Cl[Ni]Cl QMMRZOWCJAIUJA-UHFFFAOYSA-L 0.000 claims description 3
- 229920002981 polyvinylidene fluoride Polymers 0.000 claims description 3
- 239000011736 potassium bicarbonate Substances 0.000 claims description 3
- 229910000028 potassium bicarbonate Inorganic materials 0.000 claims description 3
- GNSKLFRGEWLPPA-UHFFFAOYSA-M potassium dihydrogen phosphate Chemical compound [K+].OP(O)([O-])=O GNSKLFRGEWLPPA-UHFFFAOYSA-M 0.000 claims description 3
- -1 potassium ferricyanide Chemical compound 0.000 claims description 3
- TYJJADVDDVDEDZ-UHFFFAOYSA-M potassium hydrogencarbonate Chemical compound [K+].OC([O-])=O TYJJADVDDVDEDZ-UHFFFAOYSA-M 0.000 claims description 3
- XMVONEAAOPAGAO-UHFFFAOYSA-N sodium tungstate Chemical compound [Na+].[Na+].[O-][W]([O-])(=O)=O XMVONEAAOPAGAO-UHFFFAOYSA-N 0.000 claims description 3
- 230000000087 stabilizing effect Effects 0.000 claims description 3
- 239000002609 medium Substances 0.000 claims description 2
- 238000012546 transfer Methods 0.000 abstract description 4
- 238000005516 engineering process Methods 0.000 abstract description 3
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- 239000000835 fiber Substances 0.000 abstract 1
- 230000027756 respiratory electron transport chain Effects 0.000 description 6
- LFQSCWFLJHTTHZ-UHFFFAOYSA-N Ethanol Chemical compound CCO LFQSCWFLJHTTHZ-UHFFFAOYSA-N 0.000 description 3
- 238000010586 diagram Methods 0.000 description 3
- 238000009826 distribution Methods 0.000 description 3
- 238000011065 in-situ storage Methods 0.000 description 3
- 238000003860 storage Methods 0.000 description 3
- XLYOFNOQVPJJNP-UHFFFAOYSA-N water Substances O XLYOFNOQVPJJNP-UHFFFAOYSA-N 0.000 description 3
- SRBFZHDQGSBBOR-IOVATXLUSA-N D-xylopyranose Chemical compound O[C@@H]1COC(O)[C@H](O)[C@H]1O SRBFZHDQGSBBOR-IOVATXLUSA-N 0.000 description 2
- 230000000694 effects Effects 0.000 description 2
- 230000001404 mediated effect Effects 0.000 description 2
- QTBSBXVTEAMEQO-UHFFFAOYSA-M Acetate Chemical compound CC([O-])=O QTBSBXVTEAMEQO-UHFFFAOYSA-M 0.000 description 1
- FERIUCNNQQJTOY-UHFFFAOYSA-M Butyrate Chemical compound CCCC([O-])=O FERIUCNNQQJTOY-UHFFFAOYSA-M 0.000 description 1
- FERIUCNNQQJTOY-UHFFFAOYSA-N Butyric acid Natural products CCCC(O)=O FERIUCNNQQJTOY-UHFFFAOYSA-N 0.000 description 1
- 102000018832 Cytochromes Human genes 0.000 description 1
- 108010052832 Cytochromes Proteins 0.000 description 1
- 102000004190 Enzymes Human genes 0.000 description 1
- 108090000790 Enzymes Proteins 0.000 description 1
- WQZGKKKJIJFFOK-GASJEMHNSA-N Glucose Natural products OC[C@H]1OC(O)[C@H](O)[C@@H](O)[C@@H]1O WQZGKKKJIJFFOK-GASJEMHNSA-N 0.000 description 1
- XBDQKXXYIPTUBI-UHFFFAOYSA-M Propionate Chemical compound CCC([O-])=O XBDQKXXYIPTUBI-UHFFFAOYSA-M 0.000 description 1
- 238000005273 aeration Methods 0.000 description 1
- 239000010405 anode material Substances 0.000 description 1
- PYMYPHUHKUWMLA-UHFFFAOYSA-N arabinose Natural products OCC(O)C(O)C(O)C=O PYMYPHUHKUWMLA-UHFFFAOYSA-N 0.000 description 1
- QVGXLLKOCUKJST-UHFFFAOYSA-N atomic oxygen Chemical compound [O] QVGXLLKOCUKJST-UHFFFAOYSA-N 0.000 description 1
- SRBFZHDQGSBBOR-UHFFFAOYSA-N beta-D-Pyranose-Lyxose Natural products OC1COC(O)C(O)C1O SRBFZHDQGSBBOR-UHFFFAOYSA-N 0.000 description 1
- WQZGKKKJIJFFOK-VFUOTHLCSA-N beta-D-glucose Chemical compound OC[C@H]1O[C@@H](O)[C@H](O)[C@@H](O)[C@@H]1O WQZGKKKJIJFFOK-VFUOTHLCSA-N 0.000 description 1
- 239000011942 biocatalyst Substances 0.000 description 1
- 238000006243 chemical reaction Methods 0.000 description 1
- 150000001875 compounds Chemical class 0.000 description 1
- 239000008367 deionised water Substances 0.000 description 1
- 229910021641 deionized water Inorganic materials 0.000 description 1
- 239000012153 distilled water Substances 0.000 description 1
- 239000008103 glucose Substances 0.000 description 1
- 238000010438 heat treatment Methods 0.000 description 1
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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
-
- 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
- H01M8/04—Auxiliary arrangements, e.g. for control of pressure or for circulation of fluids
- H01M8/04082—Arrangements for control of reactant parameters, e.g. pressure or concentration
- H01M8/04089—Arrangements for control of reactant parameters, e.g. pressure or concentration of gaseous reactants
-
- 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
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- Life Sciences & Earth Sciences (AREA)
- Chemical & Material Sciences (AREA)
- Engineering & Computer Science (AREA)
- Manufacturing & Machinery (AREA)
- Sustainable Development (AREA)
- Sustainable Energy (AREA)
- Chemical Kinetics & Catalysis (AREA)
- Electrochemistry (AREA)
- General Chemical & Material Sciences (AREA)
- Biochemistry (AREA)
- Microbiology (AREA)
- Apparatus Associated With Microorganisms And Enzymes (AREA)
Abstract
The invention relates to the field of microbial electrochemistry, in particular to an electricity generating device and an electricity generating method of a microbial fuel cell anode driven by a hollow fiber membrane component, wherein the electricity generating device comprises an anode chamber and a cathode chamber, the anode chamber takes a conductive hollow fiber membrane component as an electrode material, the hollow fiber membrane component continuously provides a gas substrate methane as an electron donor for the microbial fuel cell by connecting a gas steel cylinder, and the cathode chamber takes carbon adhesion as the electrode material; the improved hollow fiber membrane component is suitable for all microbial fuel cell systems which take gas as a substrate, can conduct electricity and simultaneously improve the mass transfer efficiency of the gas substrate, thereby improving the electricity generation efficiency of the microbial fuel cell; the invention integrates the fiber membrane reactor and the microbial electrochemical system, promotes the development of microbial fuel cell technology using gas methane as a substrate and the recycling of energy, and simultaneously reduces the emission of greenhouse gas methane.
Description
Technical Field
The invention relates to the field of microbial electrochemistry, in particular to a power generation device and a power generation method of a hollow fiber membrane component used as a methane-driven microbial fuel cell anode.
Background
Microbial fuel cells are an emerging electrochemical device that can convert chemical energy in organic matter into electrical energy using electroactive bacteria as a biocatalyst. The electron transfer process from the electroactive bacteria to the electrodes is critical to the power generation performance of the microbial fuel cell. It is reported that electron transfer involves indirect electron transfer process mediated by an intermediate mediator or electron shuttle, and direct electron transfer process mediated by membrane-associated cytochrome or nanowire. Microbial fuel cells can utilize simple compounds (e.g., acetate, propionate, butyrate, glucose, ethanol, and xylose), and can also utilize complex organic waste waters and sediments for the production of electricity. Methane is an abundant energy gas and is considered as a potential substrate for microbial fuel cells. However, methane-driven microbial fuel cells have only recently been investigated and there are still many unsolved problems and challenges.
Methane-driven microbial fuel cells are currently not commercially viable due to the lower solubility of methane and the longer doubling time of anaerobic microorganisms. Aerating methane directly into the reactor consumes a large amount of energy and is likely to result in methane leaks. To avoid this problem, hollow fiber membranes can be used to transport the gaseous substrate. In the hollow fiber membrane system, methane is supplied through a non-porous aeration membrane, and the gas flow rate can be controlled through a pressure reducing valve, which not only ensures the safety of methane supply, but also improves the mass transfer efficiency of methane. However, conventional fibrous membranes are not electrically conductive and cannot be used as anode materials for microbial fuel cells.
Disclosure of Invention
In order to solve the problems, the invention uses carbon fibers to wind the surface of the hollow fiber membrane yarn, constructs a conductive hollow fiber membrane component as the anode of the methane-driven microbial fuel cell to generate electricity, promotes the in-situ utilization of methane, can reduce the possibility of leakage in the methane storage and distribution process to the maximum extent, and slows down the global greenhouse effect.
In order to achieve the purpose, the invention is realized by the following technical scheme:
an electricity generating device using a hollow fiber membrane module as an anode of a methane-driven microbial fuel cell, comprising an anode chamber and a cathode chamber, wherein the anode chamber and the cathode chamber are separated by an upper proton exchange membrane and a lower proton exchange membrane, and the electricity generating device further comprises:
the conductive hollow fiber membrane component is arranged in the anode chamber and used as an electrode material;
the gas steel cylinder is connected with the hollow fiber membrane component through a gas guide pipe and is used for continuously providing gas substrate methane for the microbial fuel cell;
carbon paste arranged in the cathode chamber as an electrode material;
a reference electrode mounted on the anode chamber with its end extending into the anode chamber;
the gas outlet is arranged at the top of the anode chamber and used for discharging redundant gas;
the pH meter is arranged on the side wall of the anode chamber, and the monitoring end of the pH meter extends into the anode chamber and is used for monitoring the pH value in the anode chamber;
the input end and the output end of the peristaltic pump are respectively communicated with the anode chamber and are used for driving liquid in the anode chamber to perform internal circulation;
the thermometer is arranged on the cathode chamber, and the temperature measuring end of the thermometer extends into the cathode chamber and is used for monitoring the temperature in the cathode chamber;
the pressure stabilizing valve is arranged on the gas guide pipe connected with the gas steel cylinder;
the anode chamber and the cathode chamber are connected with an external resistor through a conducting wire to form a passage.
Further, the hollow fiber membrane module comprises hollow fiber membrane wires, carbon fibers, a hollow fixing block and a solid fixing block, the hollow fiber membrane wires are uniformly arranged between the hollow fixing block and the solid fixing block, the upper ends of the hollow fiber membrane wires are communicated with the cavity inside the hollow fixing block, the lower ends of the hollow fiber membrane wires are fixed on the solid fixing block, the hollow fixing block is connected with an external gas steel cylinder through an air duct, the carbon fibers are wound on each hollow fiber, and the upper ends of the carbon fibers are wound into a bundle of conducting wires to be connected with the conducting wires.
Preferably, the hollow fiber membrane filaments are 48 in total and made of polyvinylidene fluoride, and the total external surface area of the hollow fiber membrane filaments is 0.01m2。
Preferably, the hollow fiber membrane filaments are wrapped with carbon fibers for electrical conduction in 50% of the total outer surface area.
Furthermore, two groups of fixing screws are arranged between the hollow fixing block and the solid fixing block and used for limiting the distance between the hollow fixing block and the solid fixing block.
The invention further provides an electricity generating method of an electricity generating device based on the hollow fiber membrane module as the methane-driven microbial dye battery anode, which comprises the following steps:
1): injecting electrolyte into a cathode chamber of the microbial fuel cell;
2): injecting denitrifying anaerobic methane oxidation enrichment flora, an anaerobic mineral salt culture medium and a nitrogen source into an anode chamber of the microbial fuel cell;
3): methane is continuously supplied to the microbial fuel cell from the inner cavity of the hollow fiber membrane component as a substrate to generate electricity.
Preferably, the electrolyte is a 20mM potassium ferricyanide solution.
Preferably, the anaerobic mineral salts medium comprises: macroelements, acidic trace elements and basic trace elements;
the constant elements include: KHCO3、KH2PO4、MgCl2·6H2O and CaCl2；
The acidic trace elements include: FeSO4·7H2O、ZnSO4·7H2O、CoCl2·6H2O、MnCl2·4H2O、CuSO4·5H2O、NiCl2·6H2O、H3BO3And HCl;
the basic trace elements include: na (Na)2SeO3、Na2WO4·2H2O、Na2MoO4And NaOH.
Preferably, the denitrification anaerobic methane oxidation enrichment flora comprises denitrification anaerobic methane oxidation archaea and denitrification anaerobic methane oxidation bacteria.
Preferably, the operating pH of the microbial fuel cell is 7.3-7.6, and the operating temperature is 35 ℃.
Has the advantages that:
(1) the methane mass transfer efficiency and the microbial electron transfer efficiency of the methane-driven microbial fuel cell are improved, and a stable voltage output of 600-700 mV is obtained.
(2) Methane utilization is performed in situ, and the possibility of leakage in the methane storage and distribution process can be reduced to the maximum extent.
(3) The invention integrates the membrane bioreactor with the electrochemical system, promotes the development of the microbial fuel cell technology which takes methane as a substrate and the recycling of energy, and simultaneously reduces the emission of greenhouse gases. Based on the advantages, the method can realize the high-efficiency conversion and utilization of methane, and promote the industrial application of the microbial fuel cell taking methane as the substrate.
Drawings
FIG. 1 is a schematic structural diagram of an electric power generating apparatus provided in the present invention;
FIG. 2 is a schematic structural view of a hollow fiber membrane module provided by the present invention;
fig. 3 is a diagram of a hollow fiber membrane module according to the present invention.
Fig. 4 is a diagram of the power generation effect of the power generation device provided by the invention.
The reference numerals in the drawings denote:
1. a hollow fiber membrane module; 2. an anode chamber; 3. a proton exchange membrane; 4. a cathode chamber; 5. carbon bonding; 6. a thermometer; 7. an external resistor; 8. a reference electrode; 9. an air outlet; 10, a pH meter; 11. a pressure maintaining valve; 12. a peristaltic pump; 13. a gas cylinder; 14. a conductive wire; 1-1, hollow fiber membrane filaments; 1-2. carbon fibers; 1-3, hollow fixing blocks; 1-4, solid fixed block; 1-5, fixing the screw.
Detailed Description
In order to make the objects, technical solutions and advantages of the embodiments of the present invention clearer, the technical solutions in the embodiments of the present invention will be clearly and completely described below with reference to the embodiments of the present invention, and it is obvious that the described embodiments are some embodiments of the present invention, but not all embodiments. All other embodiments, which can be derived by a person skilled in the art from the embodiments given herein without making any creative effort, shall fall within the protection scope of the present invention.
Referring to fig. 1 to 3, an electricity generating device using a hollow fiber membrane module as an anode of a methane-driven microbial fuel cell comprises an anode chamber 2 and a cathode chamber 4 (the working volume of each chamber is 1L), wherein the anode chamber 2 is separated from the cathode chamber 4 by an upper proton exchange membrane 3 and a lower proton exchange membrane 3 (the proton exchange membranes are circular and have an area of 28.26 cm)2) The power generation device further comprises:
the conductive hollow fiber membrane component 1 is arranged in the anode chamber 2 and is used as an electrode material;
a gas steel cylinder 13 connected with the hollow fiber membrane component 1 through a gas guide pipe and used for continuously providing gas substrate methane for the microbial fuel cell; wherein CH is stored in the gas cylinder 134:CO295: 5(v/v) of a mixed gas;
carbon 5(6 cm. times.12 cm. times.0.3 cm) disposed in the cathode chamber 4 as an electrode material;
a reference electrode 8 installed on the anode chamber 2 with its end extending into the anode chamber 2;
the gas outlet 9 is arranged at the top of the anode chamber 2 and used for discharging redundant gas;
a pH meter 10 which is arranged on the side wall of the anode chamber 2, and the monitoring end of which extends into the anode chamber 2 and is used for monitoring the pH value in the anode chamber 2;
the input end and the output end of the peristaltic pump 12 are respectively communicated with the anode chamber 2 and are used for driving liquid in the anode chamber 2 to carry out internal circulation;
the thermometer 6 is arranged on the cathode chamber 4, and the temperature measuring end of the thermometer extends into the cathode chamber 4 and is used for monitoring the temperature in the cathode chamber 4;
a pressure stabilizing valve 11 which is arranged on an air duct connected with a gas steel cylinder 13;
the anode chamber 2 and the cathode chamber 4 are connected to an external resistor 7(1000 Ω) via a conductive wire 14 to form a passage.
Further, the hollow fiber membrane component comprises hollow fiber membrane wires 1-1, carbon fibers 1-2, hollow fixed blocks 1-3 and solid fixed blocks 1-4, the hollow fiber membrane wires 1-1 are uniformly arranged between the hollow fixed blocks 1-3 and the solid fixed blocks 1-4, the upper ends of the hollow fiber membrane wires 1-1 are communicated with the inner cavities of the hollow fixed blocks 1-3, the lower ends of the hollow fiber membrane wires are fixed on the solid fixed blocks 1-4, the hollow fixed blocks 1-3 are connected with an external gas steel cylinder 13 through gas guide pipes, carbon fibers 1-2 are wound on each hollow fiber, and the upper ends of the carbon fibers 1-2 are wrapped into one bundle and connected with a conducting wire 14.
Preferably, the hollow fiber membrane filaments 1-1 have a total of 48 filaments made of polyvinylidene fluoride, a total volume of 230ml, inner and outer diameters of 0.70mm and 1.03mm, respectively, and a total outer surface area of the hollow fiber membrane filaments 1-1 of 0.01m2。
Preferably, the hollow fiber membrane filaments 1-1 are wrapped with carbon fibers 1-2 for 50% of the total outer surface area to form a conductive hollow fiber membrane module for electrical conduction.
Further, two groups of fixing screws 1-5 are arranged between the hollow fixing blocks 1-3 and the solid fixing blocks 1-4 and used for limiting the distance between the hollow fixing blocks 1-3 and the solid fixing blocks 1-4.
The embodiment of the invention further provides an electricity generating method of an electricity generating device based on the hollow fiber membrane module as the methane-driven microbial fuel cell anode, which comprises the following steps:
1): injecting a 20mM potassium ferricyanide solution as an electrolyte into a cathode chamber of the microbial fuel cell;
2): injecting denitrifying anaerobic methane oxidation enrichment flora, an anaerobic mineral salt culture medium and a nitrogen source into an anode chamber of the microbial fuel cell;
the denitrifying anaerobic methane oxidation enrichment flora comprises denitrifying anaerobic methane oxidation archaea and denitrifying anaerobic methane oxidation bacteria.
Further, the inoculation liquid of the denitrification anaerobic methane oxidation enrichment flora in the anode chamber comes from a denitrification anaerobic methane oxidation reactor which runs for more than 2 years. 160mL of the inoculum was centrifuged at 5000rpm for 10 minutes, collected, washed 3 times with fresh mineral media to remove residual electron acceptor, and then injected into the anode chamber of the microbial fuel cell.
The anaerobic mineral salt culture medium comprises: macroelements, acidic trace elements and basic trace elements;
the constant elements include: KHCO3、KH2PO4、MgCl2·6H2O and CaCl2；
The acidic trace elements include: FeSO4·7H2O、ZnSO4·7H2O、CoCl2·6H2O、MnCl2·4H2O、CuSO4·5H2O、NiCl2·6H2O、H3BO3And HCl;
the basic trace elements include: na (Na)2SeO3、Na2WO4·2H2O、Na2MoO4And NaOH.
Further, an anaerobic mineral culture medium adopted by the anode chamber comprises the following components in each liter of anaerobic mineral culture medium:
constant elements: 0.5g KHCO3、0.05g KH2PO4、0.02g MgCl2·6H2O、0.02265g CaCl2；
0.2mL of an acidic trace element solution containing 2.085g of FeSO per liter of acidic trace element solution4·7H2O、0.068g ZnSO4·7H2O、0.12g CoCl2·6H2O、0.5g MnCl2·4H2O、0.5g CuSO4·5H2O、0.095gNiCl2·6H2O、0.014g H3BO3And 100ml HCl (1 mol/L);
0.5mL of an alkaline microelement solution containing 0.104g of Na per liter of alkaline microelement solution2SeO3、0.05gNa2WO4·2H2O、0.242g Na2MoO4And 10ml NaOH (1 mol/L);
before use, all solutions were treated with N2：CO295: 5(v/v) mixed gas purge for 30 minutes to remove oxygen.
Further, NH is selected as nitrogen source4Cl, concentration 0.12 g/L.
3): adding 1M HCl or 1M NaOH solution to keep the pH value in the reactor at 7.3-7.6; controlling the temperature of the reactor to be 35 ℃ by using a constant-temperature water bath kettle; methane as substrate, with CH4：CO295: 5(v/v) mixed gas is supplied from the inner cavity of the hollow fiber membrane. And the peristaltic pump is used for internal circulation of the liquid, so that the liquid is fully mixed.
Further, the carbon felt 5 electrode material in the cathode chamber is pretreated by heating in distilled water for 15 minutes before use, then is soaked in 1M HCl for 3 hours, and finally is thoroughly washed by deionized water to eliminate the influence of other impurities.
The microbial fuel cell constructed in this example was operated, connected to a personal computer using a voltage acquisition card, and voltage was acquired every 1 minute. The operation of the microbial fuel cell was divided into 6 electricity generation cycles, and at the end of each cycle, the culture medium in the anode and cathode chambers was completely replaced. As shown in fig. 4, the voltage output of the microbial fuel cell rose to 566mV on day 5 and increased to a maximum of 582mV on the last day of the 1 st cycle. In the 2 nd cycle, the voltage rise rate increases and the maximum voltage reaches 609 mV. And a repeatable and gradual increase in voltage output was observed during the power generation cycle thereafter (cycles 3-6), with the maximum voltage output of the microbial fuel cell reaching 701mV at the end of cycle 6. This indicates successful enrichment of electroactive bacteria on the anodic biofilm and exhibits stability for long term operation of the system.
From the above embodiments, it can be seen that the present invention utilizes the hollow fiber membrane module as the anode of the methane-driven microbial fuel cell, which improves the methane mass transfer efficiency and the microbial electron transfer efficiency of the methane-driven microbial fuel cell, and obtains a stable voltage output of 600 to 700 mV. The membrane bioreactor and the electrochemical system are integrated together, so that the in-situ utilization of methane is promoted, the possibility of leakage in the methane storage and distribution process can be reduced to the maximum extent, and the industrial application of the microbial fuel cell technology taking methane as a substrate is promoted.
The above examples are only intended to illustrate the technical solution of the present invention, but not to limit it; although the present invention has been described in detail with reference to the foregoing embodiments, it will be understood by those of ordinary skill in the art that: the technical solutions described in the foregoing embodiments may still be modified, or some technical features may be equivalently replaced; and such modifications or substitutions do not depart from the spirit and scope of the corresponding technical solutions of the embodiments of the present invention.
Claims (10)
1. An electricity generating device using a hollow fiber membrane module as an anode of a methane-driven microbial fuel cell, comprising an anode chamber (2) and a cathode chamber (4), wherein the anode chamber (2) and the cathode chamber (4) are separated by an upper proton exchange membrane (3) and a lower proton exchange membrane (3), and the electricity generating device is characterized by further comprising:
the conductive hollow fiber membrane component (1) is arranged in the anode chamber (2) and is used as an electrode material;
the gas steel cylinder (13) is connected with the hollow fiber membrane component (1) through a gas guide pipe and is used for continuously providing gas substrate methane for the microbial fuel cell;
a carbon paste (5) which is arranged in the cathode chamber (4) and is used as an electrode material;
a reference electrode (8) which is arranged on the anode chamber (2) and the tail end of which extends into the anode chamber (2);
the gas outlet (9) is arranged at the top of the anode chamber (2) and is used for discharging redundant gas;
the pH meter (10) is arranged on the side wall of the anode chamber (2), and the monitoring end of the pH meter extends into the anode chamber (2) and is used for monitoring the pH value in the anode chamber (2);
the input end and the output end of the peristaltic pump (12) are respectively communicated with the anode chamber (2) and are used for driving liquid in the anode chamber (2) to carry out internal circulation;
the thermometer (6) is arranged on the cathode chamber (4), the temperature measuring end of the thermometer extends into the cathode chamber (4), and the thermometer is used for monitoring the temperature in the cathode chamber (4);
the pressure stabilizing valve (11) is arranged on the gas guide pipe connected with the gas steel cylinder (13);
the anode chamber (2) and the cathode chamber (4) are connected with an external resistor (7) through a conducting wire (14) to form a passage.
2. The power generation device of the methane-driven microbial fuel cell anode of claim 1, wherein the hollow fiber membrane module comprises hollow fiber membrane wires (1-1), carbon fibers (1-2), a hollow fixing block (1-3) and a solid fixing block (1-4), the hollow fiber membrane wires (1-1) are uniformly arranged between the hollow fixing block (1-3) and the solid fixing block (1-4), the upper end of each hollow fiber membrane wire (1-1) is communicated with the inner cavity of the hollow fixing block (1-3), the lower end of each hollow fiber membrane wire is fixed on the solid fixing block (1-4), the hollow fixing block (1-3) is connected with an external gas cylinder (13) through a gas guide tube, and each hollow fiber is wound with the carbon fibers (1-2), the upper end of the carbon fiber (1-2) is wrapped into a bundle and is connected with the conducting wire (14).
3. The apparatus for generating electricity as an anode of a methane-driven microbial fuel cell according to claim 1, wherein the hollow fiber membrane module comprises a total of 48 hollow fiber membrane filaments (1-1) made of polyvinylidene fluoride, and the total outer surface area of the hollow fiber membrane filaments (1-1) is 0.01m2。
4. A hollow fiber membrane module as a power generation device of an anode of a methane driven microbial fuel cell according to claim 2 or 3, wherein 50% of the total outer surface area of the hollow fiber membrane filaments (1-1) is wound with carbon fibers (1-2) for conduction.
5. The power generation device of the methane-driven microbial fuel cell anode with the hollow fiber membrane module as claimed in claim 4, wherein two sets of fixing screws (1-5) are arranged between the hollow fixing blocks (1-3) and the solid fixing blocks (1-4) for limiting the distance between the hollow fixing blocks (1-3) and the solid fixing blocks (1-4).
6. A method for generating electricity based on the hollow fiber membrane module as claimed in any one of claims 1 to 5 as an electricity generating means for an anode of a methane-driven microbial fuel cell, comprising the steps of:
1): injecting electrolyte into a cathode chamber of the microbial fuel cell;
2): injecting denitrifying anaerobic methane oxidation enrichment flora, an anaerobic mineral salt culture medium and a nitrogen source into an anode chamber of the microbial fuel cell;
3): methane is continuously supplied to the microbial fuel cell from the inner cavity of the hollow fiber membrane component as a substrate to generate electricity.
7. A method of generating electricity according to claim 6 wherein the electrolyte is a 20mM potassium ferricyanide solution.
8. The method of generating electricity according to claim 6, wherein the anaerobic mineral salts medium comprises: macroelements, acidic trace elements and basic trace elements;
the constant elements include: KHCO3、KH2PO4、MgCl2·6H2O and CaCl2；
The acidic trace elements include: FeSO4·7H2O、ZnSO4·7H2O、CoCl2·6H2O、MnCl2·4H2O、CuSO4·5H2O、NiCl2·6H2O、H3BO3And HCl;
the basic trace elements include: na (Na)2SeO3、Na2WO4·2H2O、Na2MoO4And NaOH.
9. The method of claim 6, wherein the denitrification anaerobic methane oxidation-enriched flora comprises denitrification anaerobic methane-oxidizing archaea and denitrification anaerobic methane-oxidizing bacteria.
10. The power generation method according to claim 6, wherein the operating pH of the microbial fuel cell is 7.3 to 7.6, and the operating temperature is 35 ℃.
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