WO2019181281A1 - 微生物発電装置及びその運転方法 - Google Patents

微生物発電装置及びその運転方法 Download PDF

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Publication number
WO2019181281A1
WO2019181281A1 PCT/JP2019/004988 JP2019004988W WO2019181281A1 WO 2019181281 A1 WO2019181281 A1 WO 2019181281A1 JP 2019004988 W JP2019004988 W JP 2019004988W WO 2019181281 A1 WO2019181281 A1 WO 2019181281A1
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Prior art keywords
anode
power generation
anode chamber
chamber
oxygen
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PCT/JP2019/004988
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English (en)
French (fr)
Japanese (ja)
Inventor
和也 小松
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栗田工業株式会社
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Priority to KR1020207014300A priority Critical patent/KR20200138147A/ko
Priority to CN201980006296.9A priority patent/CN111448698A/zh
Publication of WO2019181281A1 publication Critical patent/WO2019181281A1/ja

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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
    • H01M8/04—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
    • H01M8/04186—Arrangements for control of reactant parameters, e.g. pressure or concentration of liquid-charged or electrolyte-charged reactants
    • 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
    • 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

Definitions

  • the present invention relates to a power generation device that utilizes a metabolic reaction of a microorganism and an operation method thereof.
  • the present invention relates to a microbial power generation apparatus that extracts, as electric energy, a reducing power obtained when an organic substance is oxidatively decomposed into microorganisms, and an operation method thereof.
  • Patent Documents 1 and 2 describe a device in which a cathode chamber and an anode chamber are partitioned by an electrolyte membrane.
  • Patent Document 1 describes that by adjusting the pH in the anode chamber to 7 to 9, it is possible to prevent the pH from being lowered due to the generation of carbon dioxide gas accompanying the microbial reaction in the anode chamber and to increase the power generation efficiency. ing.
  • methanogens grow in the anode chamber under anaerobic conditions using organic substances as a substrate.
  • the internal resistance increases, and the organic matter to be used for the power generation reaction is consumed by the methanogen, resulting in a decrease in power generation efficiency.
  • An object of the present invention is to provide a microbial power generation apparatus that suppresses the growth of methanogenic bacteria in the anode chamber in a microbial power generation apparatus and can stably obtain a high power generation amount for a long period of time, and an operating method thereof.
  • the microbial power generation device of the present invention has an anode chamber having an anode and holding a liquid containing a microorganism and an electron donor, and a cathode chamber separated from the anode chamber by a porous non-conductive film.
  • oxygen supply means for intermittently supplying oxygen into the anode chamber is provided. It is characterized by that.
  • the oxygen supply means is an aeration means for an oxygen-containing gas.
  • the oxygen supply means is oxygen dissolved water supply means.
  • An operation method of a microbial power generation device of the present invention includes an anode chamber having an anode and holding a liquid containing a microorganism and an electron donor, and a cathode chamber separated from the anode chamber via a porous non-conductive film. And supplying the organic material-containing raw water to the anode chamber, supplying a fluid containing an electron acceptor to the cathode chamber, and supplying oxygen intermittently into the anode chamber. It is characterized by doing.
  • the oxygen-containing gas is supplied to the anode chamber at a frequency of once every 2 hours to 30 days for 30 seconds to 12 hours.
  • oxygen is supplied so that the dissolved oxygen concentration in the anode chamber is 2 to 8 mg / L.
  • oxygen is intermittently supplied to the anode chamber.
  • the growth of the methanogen which is an absolute anaerobic bacterium can be suppressed.
  • facultative anaerobic bacteria that can survive even under aerobic conditions, so that the power generation reaction in the anode chamber is stably maintained.
  • FIG. 1 is a schematic cross-sectional view of a microbial power generation apparatus according to an embodiment of the present invention.
  • FIG. 2 is a schematic cross-sectional view of a microbial power generation device according to an embodiment of the present invention.
  • FIG. 1 is a schematic cross-sectional view showing a schematic configuration of a microbial power generation apparatus according to an embodiment of the present invention.
  • the tank body 1 is partitioned into a cathode chamber 3 and an anode chamber 4 by a partition material 2 made of a porous non-conductive film.
  • a cathode 5 made of a conductive porous material is disposed so as to be in close contact with the partition material 2.
  • the cathode chamber 3 between the cathode 5 and the wall surface of the tank body 1 is filled with the cathode solution.
  • a diffuser tube 7 is provided in the lower part of the cathode chamber 3 so as to aerate the cathode solution. Oxygen-containing gas such as air is introduced into the aeration tube 7 and aeration exhaust gas flows out from the gas outlet 8 at the upper part of the cathode chamber. Since the catholyte solution evaporates or decreases due to aeration, the replenishment cathode solution is appropriately supplied from the replenishing port 16 having the valve 15.
  • An anode 6 made of a conductive porous material is disposed in the anode chamber 4.
  • the anode 6 is in close contact with the partition material 2, and protons (H + ) can be transferred from the anode 6 to the partition material 2.
  • Microorganisms are supported on the anode 6 made of this porous material.
  • the anode solution L is introduced into the anode chamber 4 from the inlet 4a, and the waste liquid is discharged from the outlet 4b.
  • the anode chamber 4 is anaerobic.
  • the anode solution L in the anode chamber 4 is circulated through a circulation outlet 9, a circulation pipe 10, a circulation pump 11, and a circulation return 12.
  • the circulation pipe 10 is provided with a pH meter 14 for measuring the pH of the liquid flowing out from the anode chamber 4 and connected with a pipe 13 for adding a pH adjusting agent such as alkali or acid.
  • a diffuser pipe 17 is installed in the anode chamber 4, and the inside of the anode chamber 4 is aerated with an oxygen-containing gas by opening the valve 17a.
  • a gas outlet 18 having a valve 18 a is provided in the upper part of the anode chamber 4.
  • alkali or acid is added to the anode solution L so that the pH detected by the pH meter 14 is preferably 7-9.
  • the alkali or acid may be added directly to the anode chamber 4, but by adding to the circulating water, the entire area in the anode chamber 4 can be maintained at a pH of 7 to 9 without partial deviation.
  • valves 17 a and 18 a are opened intermittently, the inside of the anode chamber 4 is aerated with the oxygen-containing gas from the diffuser tube 17, and the exhaust gas flows out from the gas outlet 18. Thereby, the growth of the methanogen in the anode chamber 4 is suppressed. While the anode chamber 4 is temporarily in an aerobic state due to this aeration, the power generation amount decreases, but when the DO is consumed after aeration is stopped, the power generation amount quickly recovers.
  • FIG. 2 is a schematic cross-sectional view of a microbial power generation apparatus according to another embodiment of the present invention.
  • Two plate-shaped partition members 31 are arranged in parallel with each other in a substantially rectangular parallelepiped tank body 30, thereby forming an anode chamber 32 between the partition members 31, 31.
  • Two cathode chambers 33 and 33 are formed by separating the partition member 31 from the partition member 32.
  • An anode 34 made of a porous material is disposed in the anode chamber 32 so as to be in close contact with each partition material 31.
  • the anode 34 is lightly pressed against the partition material (for example, at a pressure of 0.1 kg / cm 2 or less).
  • a cathode 35 made of a porous material is disposed in the cathode chamber 33 in contact with the partition material 31.
  • the cathode 35 is pressed by a spacer 36 made of rubber or the like and is pressed lightly (for example, at a pressure of 0.1 kg / cm 2 or less) against the partition material 31 to be in close contact therewith.
  • they may be welded or partially bonded with an adhesive.
  • the cathode 35 and the anode 34 are connected to an external resistor 38 via terminals 37 and 39.
  • the cathode chamber 33 between the cathode 35 and the side wall of the tank body 30 is filled with the cathode solution.
  • a diffuser tube 51 is installed in the lower part of each cathode chamber 33 so that the cathode solution can be aerated.
  • the aerated exhaust gas flows out from the gas outlet 52 at the top of the cathode chamber 33.
  • a replenishing port is provided for each cathode chamber 33 so as to replenish the cathode solution.
  • the anode solution L is introduced from the inlet 32a, and the waste liquid flows out from the outlet 32b.
  • the anode chamber 32 is anaerobic.
  • the anode solution in the anode chamber 32 is circulated through a circulation outlet 41, a circulation pipe 42, a circulation pump 43, and a circulation return port 44.
  • the circulation pipe 42 is provided with a pH meter 47 and an alkali addition pipe 45 is connected thereto.
  • the pH of the anode solution flowing out from the anode chamber 32 is detected by a pH meter 47, and an alkali such as an aqueous sodium hydroxide solution is added so that this pH is preferably 7-9.
  • a diffuser tube 57 is installed in the anode chamber 32, and the anode chamber 32 is aerated with an oxygen-containing gas by opening the valve 57a.
  • a gas outlet 58 having a valve 58 a is provided in the upper part of the anode chamber 32.
  • an oxygen-containing gas is supplied to the aeration tube 51 to aerate the cathode solution in the cathode chamber 33, and the anode solution is circulated through the anode chamber 32, preferably the anode solution is circulated.
  • a potential difference is generated between the cathode 35 and the anode 34, and a current flows through the external resistor 38.
  • valves 57 a and 58 a are opened intermittently, the inside of the anode chamber 32 is aerated with the oxygen-containing gas from the diffuser tube 57, and the exhaust gas flows out from the gas outlet 58. Thereby, the growth of the methanogen in the anode chamber 32 is suppressed.
  • the aeration tube is disposed in the cathode chambers 3 and 33 and the cathode solution is aerated in the cathode chambers 3 and 33, but the cathode solution in the cathode chamber is introduced into another aeration chamber. It may be aerated.
  • the oxygen-containing gas may be any of air, oxygen, oxygen-enriched air, etc., but air is preferred.
  • the frequency of oxygen-containing gas supply to the anode chamber is preferably once every 2 hours to 30 days, and the oxygen-containing gas supply time per time is preferably 30 seconds to 12 hours, more preferably 6 hours to 3 days. 1 minute to 2 hours per time.
  • the dissolved oxygen concentration in the anode chamber is 2 to 8 mg / L, particularly 4 to 8 mg / L by supplying the oxygen-containing gas.
  • the oxygen-containing gas is supplied to the anode chamber by the diffuser pipes 17 and 57.
  • an aeration tank may be provided in the anode solution circulation pipes 10 and 42 to perform aeration with the oxygen-containing gas.
  • An oxygen-containing gas inflow pipe may be connected to the circulation pipes 10 and 42, and a line mixer may be provided in the circulation pipe downstream of the oxygen-containing gas inflow pipe. Further, oxygen-dissolved water may flow into the anode chamber or the circulation pipe.
  • the microorganism that produces electric energy by being contained in the anode solution L is not particularly limited as long as it has a function as an electron donor.
  • the chamber can be fed and microorganisms can be retained on the anode.
  • the amount of microorganisms retained in the anode chamber is preferably high, and for example, the microorganism concentration is preferably 1 to 50 g / L.
  • the anode solution L a solution that holds microorganisms or cells and has a composition necessary for power generation is used.
  • the anode solution may be an energy source necessary for metabolism of the respiratory system such as bouillon medium, M9 medium, L medium, Malt Extract, MY medium, or nitrifying bacteria selection medium.
  • a medium having a composition such as nutrients can be used.
  • organic waste such as sewage, organic industrial wastewater, and garbage can be used.
  • the anode solution L may contain an electron mediator in order to make it easier to extract electrons from microorganisms or cells.
  • the electron mediator include compounds having a thionin skeleton such as thionine, dimethyldisulfonated thionin, new methylene blue, and toluidine blue-O, and 2-hydroxy-1,4-naphthoquinone skeleton such as 2-hydroxy-1,4-naphthoquinone.
  • anode solution L a material that increases the power generation function of microorganisms, for example, an antioxidant such as vitamin C, or a function-enhancing material that works only a specific electron transfer system or substance transfer system in the microorganism is dissolved. It is preferable because electric power can be obtained more efficiently.
  • an antioxidant such as vitamin C
  • a function-enhancing material that works only a specific electron transfer system or substance transfer system in the microorganism
  • the anode solution L may contain a phosphate buffer as necessary.
  • the anode solution L contains an organic substance.
  • the organic substance is not particularly limited as long as it can be decomposed by microorganisms.
  • water-soluble organic substances, organic fine particles dispersed in water, and the like are used.
  • the anodic solution may be an organic effluent such as sewage or food factory effluent.
  • the organic substance concentration in the anode solution L is preferably as high as about 100 to 10,000 mg / L in order to increase the power generation efficiency.
  • the temperature of the anode solution is preferably about 10 to 70 ° C.
  • the cathode solution is preferably neutral or alkaline, for example, pH 6.0 to 9.0, and may contain a buffer in order to keep the pH in such a range.
  • the cathode solution may contain a redox reagent such as potassium ferricyanide, manganese sulfate, manganese chloride, ferric chloride, and ferric sulfate as an electron acceptor.
  • a redox reagent such as potassium ferricyanide, manganese sulfate, manganese chloride, ferric chloride, and ferric sulfate as an electron acceptor.
  • concentration of the redox reagent in the cathode solution is preferably about 10 to 2,000 mM.
  • the cathode solution may contain a chelating agent.
  • a chelating agent By blending a chelating agent, tetravalent manganese can be present in a dissolved state, and the effect of increasing the speed of the reduction reaction can be obtained.
  • chelating agent can be used without limitation as long as it forms a chelate compound with manganese ions.
  • EDTA ethylenediaminetetraacetic acid
  • 1,2-dihydroxyanthraquinone-3-yl-methylamino-N N′-diacetic acid
  • 5,5′-dibromopyrogallolsulfophthalein 1- (1- Hydroxy-2-naphthylazo) -6-nitro-2-naphthol-4-sulfonic acid sodium salt
  • 4-Methylumbelliferone-8-methyleneiminodiacetic acid 3-sulfo-2,6-dichloro-3 ′, 3 ′′ -dimethyl-4′-fuxone-5 ′, 5 ′′ -dicarboxylic acid trisodium salt Salt, 3,3′-bis [N,
  • the oxygen-containing gas supplied to the cathode chamber air is suitable.
  • the exhaust gas from the cathode chamber may be deoxygenated as necessary, and then vented to the anode chamber to be used for purging dissolved oxygen from the anode solution L.
  • the supply amount of the oxygen-containing gas may be such that DO is detected (for example, 0.5 mg / L or less) when the dissolved oxygen (DO) concentration of the cathode solution is measured.
  • partition material paper made of a porous non-conductive material, woven fabric, non-woven fabric, so-called organic membrane (microfiltration membrane), honeycomb molded body, lattice-shaped molded body, and the like can be used.
  • a material made of a hydrophilic material is used because of easy proton movement, or a microfiltration membrane in which a hydrophobic membrane is made hydrophilic is preferable.
  • a hydrophobic material it is good to process it so that water can pass easily as shapes, such as a woven fabric, a nonwoven fabric, and a honeycomb.
  • the non-conductive material examples include polyethylene, polypropylene, polycarbonate, polyethersulfone (PES), polyvinylidene fluoride (PVDF), polytetrafluoroethylene (PTFE), polyvinyl alcohol (PVA), and cellulose. Cellulose acetate and the like are preferable.
  • the partition material is preferably a thin one having a thickness of 10 ⁇ m to 10 mm, particularly about 30 to 100 ⁇ m.
  • the partition material is excellent in water permeability with a thickness of about 1 to 10 mm, such as a honeycomb or lattice. Is preferred.
  • the partition material is optimally paper having a thickness of 1 mm or less in terms of thickness and price.
  • the microfiltration membrane which hydrophilized PES and PVDF is very thin, it is suitable as a partition material in the case of calculating
  • the anode is preferably a porous body having a large surface area, a large number of voids, and water permeability so that many microorganisms can be retained.
  • Specific examples include a conductive material sheet having a roughened surface and a porous conductor (for example, graphite felt, expanded titanium, expanded stainless steel, etc.) in which the conductive material is made into a felt-like porous sheet. .
  • the anode is preferably made of a fibrous body such as felt.
  • the anode When the anode has a thickness larger than the thickness of the anode chamber, the anode is compressed and inserted into the anode chamber, and comes into close contact with the partition material by its own restoring elasticity.
  • a plurality of sheet conductors may be laminated to form an anode.
  • the same kind of conductor sheets may be laminated, or different kinds of conductor sheets (for example, a graphite sheet having a rough surface and a graphite felt) may be laminated.
  • the total thickness of the anode is preferably 3 mm to 50 mm, particularly about 5 to 40 mm.
  • the laminated surface is preferably oriented in a direction connecting the liquid inlet and the outlet so that the liquid flows along a mating surface (laminated surface) between the sheets.
  • the cathode is made of a felt-like or porous conductive material such as graphite felt, foamed stainless steel, or foamed titanium. In the case of a porous material, the diameter of the void is preferably about 0.01 to 1 mm.
  • a cathode it is preferable to use a cathode in which these conductive materials are formed in a shape (for example, a plate shape) that is easily adhered to the partition material.
  • an oxygen reduction catalyst is preferably used.
  • the catalyst may be supported using graphite felt as a base material. Examples of the catalyst include noble metals such as platinum, metal oxides such as manganese dioxide, and carbon-based materials such as activated carbon.
  • an inexpensive graphite electrode may be used as it is (without supporting platinum) as a cathode.
  • the thickness of the cathode is preferably 0.03 to 50 mm.
  • FIG. 1 and 2 each show a microbial power generation apparatus in which a cathode solution is held in a cathode chamber.
  • the present invention is not limited to such a microbial power generation apparatus, and the cathode chamber is an empty chamber.
  • the present invention can also be applied to an air cathode type microbial power generation apparatus that circulates.
  • an anode solution containing 1,000 mg / L of acetic acid, 50 mM phosphate buffer, and ammonium chloride with a pH maintained at 7.5 was passed. This raw water was heated to 35 ° C. in a separate water tank in advance and then passed through the anode chamber at 70 mL / min, thereby heating the anode chamber to 35 ° C. Prior to the passage of the anode solution, the effluent of another microbial power generation apparatus was passed through the anode chamber as an inoculum. A cathode solution containing 50 mM potassium ferricyanide and a phosphate buffer was supplied to the cathode chamber at a flow rate of 70 mL / min.
  • Power generation amount in one week after passing water starts 300 W / m 3 - reach the anode chamber volume, but remained in the subsequent 3 weeks 280 ⁇ 330W / m 3, was reduced by one week thereafter until 100W / m 3. While the concentration of acetic acid in treated water is almost unchanged, the current efficiency decreased from 60 to 80% while the power generation amount was 280 to 330 W / m 3 to 10 to 20% as the power generation amount decreased. It was thought that about one month after the start of water flow, methanogenic bacteria became dominant in the anode chamber.
  • Example 1 The same configuration as Comparative Example 1, passed through the water starts after 28 days, the power generation amount which has remained at 280 ⁇ 330W / m 3 is where drops below 250 W / m 3, the anode compartment and air aeration.
  • the power generation amount recovered to 300 W / m 3 and was maintained for 1 week thereafter.
  • the power generation amount decreased again, the anode chamber was recovered by air aeration in the same manner as the previous time, and then recovered and maintained at 300 W / m 3 for one week thereafter. During that time, the current efficiency remained at 50-70%.
  • Example 2 With the same configuration as Comparative Example 1, one week passed after the start of water flow, and when the power generation amount reached 300 W / m 3 , the anode chamber was aerated with air at a flow rate of 300 mL / min once a day for 10 minutes.
  • the amount of power generation was 300-320 W / m 3 over the next three months, and the current efficiency remained stable at around 70%.
  • the present invention suppresses the growth of methanogenic bacteria in the anode chamber of the microbial power generation apparatus, and can stably obtain a high power generation amount for a long period of time.

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  • Chemical & Material Sciences (AREA)
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  • Chemical Kinetics & Catalysis (AREA)
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  • Manufacturing & Machinery (AREA)
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PCT/JP2019/004988 2018-03-23 2019-02-13 微生物発電装置及びその運転方法 WO2019181281A1 (ja)

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CN112458487A (zh) * 2020-09-03 2021-03-09 南昌航空大学 一种中碱不对称微生物电解池及其在产氢中的应用
JP7478373B2 (ja) 2021-12-28 2024-05-07 福岡県 堆積物微生物燃料電池を用いた底質改善方法及び底質改善装置

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KR102608043B1 (ko) * 2020-12-31 2023-11-30 단국대학교 산학협력단 투명 미생물에너지 소자 및 그 제작 방법

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Publication number Priority date Publication date Assignee Title
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JP7478373B2 (ja) 2021-12-28 2024-05-07 福岡県 堆積物微生物燃料電池を用いた底質改善方法及び底質改善装置

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TWI823902B (zh) 2023-12-01
KR20200138147A (ko) 2020-12-09
JP2019169329A (ja) 2019-10-03

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