CN112290069A - Air cathode microbial fuel cell and cathode preparation method thereof - Google Patents

Air cathode microbial fuel cell and cathode preparation method thereof Download PDF

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Publication number
CN112290069A
CN112290069A CN202011228080.8A CN202011228080A CN112290069A CN 112290069 A CN112290069 A CN 112290069A CN 202011228080 A CN202011228080 A CN 202011228080A CN 112290069 A CN112290069 A CN 112290069A
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cathode
carbon cloth
fuel cell
exchange membrane
proton exchange
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CN112290069B (en
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朱冬冬
尤晓慧
周莉
杭小帅
陈玉东
丁程成
崔益斌
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Nanjing Institute of Environmental Sciences MEE
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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
    • H01M4/00—Electrodes
    • H01M4/86—Inert electrodes with catalytic activity, e.g. for fuel cells
    • H01M4/88—Processes of manufacture
    • H01M4/8825—Methods for deposition of the catalytic active composition
    • H01M4/8828—Coating with slurry or ink
    • H—ELECTRICITY
    • H01—ELECTRIC ELEMENTS
    • H01M—PROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
    • H01M4/00—Electrodes
    • H01M4/86—Inert electrodes with catalytic activity, e.g. for fuel cells
    • H01M4/90—Selection of catalytic material
    • H01M4/9016—Oxides, hydroxides or oxygenated metallic salts
    • H—ELECTRICITY
    • H01—ELECTRIC ELEMENTS
    • H01M—PROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
    • H01M4/00—Electrodes
    • H01M4/86—Inert electrodes with catalytic activity, e.g. for fuel cells
    • H01M4/90—Selection of catalytic material
    • H01M4/9075—Catalytic material supported on carriers, e.g. powder carriers
    • H01M4/9083—Catalytic material supported on carriers, e.g. powder carriers on carbon or graphite
    • 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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  • Chemical & Material Sciences (AREA)
  • General Chemical & Material Sciences (AREA)
  • Engineering & Computer Science (AREA)
  • Chemical Kinetics & Catalysis (AREA)
  • Electrochemistry (AREA)
  • Manufacturing & Machinery (AREA)
  • Materials Engineering (AREA)
  • Life Sciences & Earth Sciences (AREA)
  • Biochemistry (AREA)
  • Microbiology (AREA)
  • Sustainable Development (AREA)
  • Sustainable Energy (AREA)
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Abstract

The invention relates to an air cathode microbial fuel cell and a cathode preparation method thereof, wherein a cell unit comprises a cathode and an anode coaxially sleeved on the cathode. The cathode comprises a PVC pipe, an activated proton exchange membrane and a carbon cloth modified by graphene and a catalyst. Carbon cloth and proton exchange membrane parcel in proper order are in PVC pipe lower part, and proton exchange membrane upper portion surpasss carbon cloth, and a plurality of air vents are evenly seted up to the cladding section of PVC pipe, alternate a copper conductor that is used for series connection in the carbon cloth, and the copper conductor passes the PVC pipe and upwards wears out. According to the invention, the cathode carbon cloth is modified by graphene, so that the resistance of the battery cathode is effectively reduced, and the internal resistance of the battery is reduced. The cathode carbon cloth is coated with manganese dioxide and activated carbon powder, so that the catalytic action on oxygen in the air is effectively improved, and the reaction process efficiency is accelerated. The invention can realize waste utilization of the sludge and reduce the pollution of the sludge to the environment.

Description

Air cathode microbial fuel cell and cathode preparation method thereof
Technical Field
The invention belongs to the technical field of sludge treatment, and particularly relates to an air cathode microbial fuel cell and a cathode preparation method thereof.
Background
The activated sludge process is the most widely used sewage treatment process at present, has the advantages of high efficiency, small occupied area and the like, but a large amount of activated sludge is remained in the treatment process to cause secondary pollution. The method is a common disposal method for domestic large-scale sewage treatment plants, and is used for dewatering after digesting the activated sludge and then performing landfill. The disposal method is economical, but inevitably needs to occupy a large amount of land, increases the danger of pollution to underground water, and wastes recyclable resources in activated sludge.
On the other hand, microbial fuel cells are a new energy and environmental technology developed in recent years, which directly convert chemical energy in organic substances into electric energy by the metabolism of microbes themselves, thereby realizing waste treatment and energy recovery. The activated sludge contains a large amount of organic matters, and is suitable for being treated by a microbiological method. However, the existing microbial fuel cell has the following problems: first, current microbial fuel cell output power is still low. Second, microbial fuel cells generally have a low capacity.
Disclosure of Invention
In view of the problems identified in the background art, the present invention provides an air cathode microbial fuel cell and a method for preparing the cathode thereof.
The technical scheme adopted by the invention is as follows:
an air cathode microbial fuel cell comprises an organic glass container filled with sludge and a plurality of battery units which are uniformly inserted into the sludge at intervals, wherein the battery units are sequentially connected in series through copper wires and externally connected with a resistor.
Further, the interval between the adjacent battery cells was 2 cm.
Further, the number of battery cells is three.
Further, the resistance value of the resistor is 1000 Ω.
Further, the battery unit comprises a cathode and an anode coaxially sleeved on the cathode;
the cathode comprises a PVC pipe, an activated proton exchange membrane and carbon cloth modified by graphene and a catalyst; the carbon cloth and the proton exchange membrane are sequentially wrapped at the lower part of the PVC pipe, the upper part of the proton exchange membrane exceeds the carbon cloth, a plurality of vent holes are uniformly formed in the wrapping section of the PVC pipe, a copper wire for series connection is inserted into the carbon cloth, and the copper wire penetrates through the PVC pipe and upwards penetrates out of the inner cavity of the PVC pipe;
the anode is made into a cylinder shape by rolling a stainless steel wire net, the joint is connected through a copper wire, and meanwhile, the stainless steel wire net is also connected with a copper wire used for series connection;
when the proton exchange membrane is inserted, the top of the proton exchange membrane is flush with the top of the sludge, and the top of the anode is flush with the top of the sludge.
Further, the radial distance between the cathode and the anode is 2 cm.
Further, the diameter of the PVC pipe is 1.5cm, and the length of the PVC pipe is 20 cm; the size of the carbon cloth is 6 multiplied by 13 cm; the size of the proton exchange membrane is 8 multiplied by 17 cm; the number of the stainless steel wire meshes is three, the size of a single stainless steel wire mesh is 16 multiplied by 11cm, and the three stainless steel wire meshes are connected in series after being rolled into a cylinder shape.
Further, the diameter of the vent hole is 1 cm.
A method for preparing a cathode of an air cathode microbial fuel cell comprises the following steps:
1) and graphene modification: dissolving aniline purified by reduced pressure distillation into 12mol/L HCl solution in a volume ratio of 110mL/L, and adding graphene powder in a mass ratio of 1: 9 to aniline monomer; after the ultrasonic dispersion is uniform, putting the carbon cloth, dropwise adding APS solution under the conditions of ice bath and magnetic stirring to ensure that the molar ratio of APS to aniline in the reaction solution is 1: 1, taking out the carbon cloth after reacting for 6 hours, soaking the carbon cloth in 1mol/L HCl solution until the color of the carbon cloth is not faded, washing the carbon cloth with deionized water, and drying the carbon cloth in a 60 ℃ oven;
2) and catalyst modification: weighing 2g of manganese dioxide and 2g of activated carbon powder, putting the manganese dioxide and the activated carbon powder into a beaker, adding 20ml of distilled water, mixing, adding 60 wt% of PTFE, and ultrasonically cleaning for 1 h; then brushing and coating the dried carbon cloth on one side in contact with the PVC pipe, and naturally airing for 24 hours;
3) and heating the proton exchange membrane in a water bath at 50 ℃ for 3h for activation, covering the proton exchange membrane on carbon cloth, and adhering the periphery and the bottom of the proton exchange membrane by using glass cement to prevent water seepage.
Further, the APS solution is: 15.06g of ammonium persulfate was made up to 50mL with 1mol/L HCl solution.
The invention has the beneficial effects that:
according to the invention, the plurality of battery units are connected in series, so that the overall operation efficiency of the battery can be improved. The cathode carbon cloth is modified by graphene to effectively reduce the resistance of the cathode of the battery and the internal resistance of the battery. The cathode carbon cloth is coated with manganese dioxide and activated carbon powder, so that the catalytic action on oxygen in the air is effectively improved, and the reaction process efficiency is accelerated. The invention can realize waste utilization of the sludge and reduce the pollution of the sludge to the environment.
Drawings
FIG. 1 is a schematic view of the structure of a microbial fuel cell of the present invention;
FIG. 2 is a schematic view of a disassembled structure of a cathode;
reference numerals: 1-anode, 2-cathode, 201-PVC tube, 202-carbon cloth, 203-proton exchange membrane, 3-resistor, 4-organic glass container, 5-copper wire.
Detailed Description
The technical solution of this aspect is further illustrated by the following specific examples:
as shown in figure 1, the air cathode microbial fuel cell comprises an organic glass container 4 filled with sludge and a plurality of battery units which are uniformly inserted into the sludge at intervals, wherein the battery units are sequentially connected in series through copper wires 5 and are externally connected with a resistor 3. In this example, the interval between adjacent battery cells was 2 cm. The number of battery cells is three. The resistance of the resistor 3 is 1000 omega.
Specifically, referring to fig. 2, the battery cell includes a cathode 2 and an anode 1 coaxially fitted over the cathode 2. The cathode 2 comprises a PVC pipe 201 and an activated proton exchange membrane 203, and a carbon cloth 202 modified by graphene and a catalyst. Carbon cloth 202 and proton exchange membrane 203 wrap up in proper order in PVC pipe 201 lower part, and carbon cloth 202 is surpassed on proton exchange membrane 203 upper portion, and a plurality of air vents (in this embodiment, the air vent diameter is 1cm) are evenly seted up to the cladding section of PVC pipe 201, alternates a copper conductor 5 that is used for series connection in carbon cloth 202, and copper conductor 5 passes PVC pipe 201 and upwards wears out from PVC pipe 201 inner chamber. The anode 1 is made into a cylinder shape by rolling a stainless steel wire net, the joint is connected through a copper wire 5, and meanwhile, the stainless steel wire net is also connected with a copper wire 5 used for series connection. When the proton exchange membrane is inserted, the top of the proton exchange membrane 203 is flush with the top of the sludge, and the top of the anode 1 is flush with the top of the sludge.
In this embodiment, the radial distance between the cathode 2 and the anode 1 is 2 cm. The PVC pipe 201 has a diameter of 1.5cm and a length of 20 cm. The size of the carbon cloth 202 was 6 × 13 cm. The proton exchange membrane 203 has a size of 8 × 17 cm. The number of the stainless steel wire meshes is three, the size of a single stainless steel wire mesh is 16 multiplied by 11cm, and the three stainless steel wire meshes are all rolled into cylinders and then connected in series (the heads and the tails are sequentially connected through copper wires).
A method for preparing a cathode of an air cathode microbial fuel cell comprises the following steps:
1) and graphene modification: dissolving aniline purified by reduced pressure distillation into 12mol/L HCl solution in a volume ratio of 110mL/L, and adding graphene powder with a mass ratio of 1: 9 to aniline monomer (0.545 g of graphene powder is added). After the ultrasonic dispersion is uniform, the carbon cloth 202 is placed, under the conditions of ice bath and magnetic stirring, APS solution (15.06g of ammonium persulfate is metered to 50mL by 1mol/L HCl solution) is added dropwise to enable the molar ratio of APS to aniline in the reaction solution to be 1: 1, after the reaction is carried out for 6 hours, the carbon cloth 202 is taken out, placed in 1mol/L HCl solution for soaking until the color is not faded, washed by deionized water and dried in an oven at 60 ℃.
2) And catalyst modification: 2g of manganese dioxide and 2g of activated carbon powder were weighed and placed in a beaker, 20mL of distilled water was added and mixed, and then 60 wt% PTFE (polytetrafluoroethylene) was added and ultrasonic cleaning was carried out for 1 hour. And then brushing the dried carbon cloth 202 on the side contacting the PVC pipe 201, and naturally airing for 24 h.
3) The proton exchange membrane 203 is used after being heated for 3 hours for activation in a water bath at 50 ℃, the proton exchange membrane 203 is covered on the carbon cloth 202, and the periphery and the bottom of the proton exchange membrane 203 are adhered by glass cement to prevent water seepage.
The working principle of the air cathode microbial fuel cell of the invention is as follows:
the anode microorganisms decompose organic matters in the sludge to generate protons and electrons, the protons reach the cathode 2 through the proton exchange membrane 203, and the electrons reach the cathode 2 through the external series circuit. The carbon cloth 202 in the cathode 2 is modified by graphene (the graphene has the characteristics of strong conductivity, high electron transfer efficiency and large specific surface area, and can improve the conductivity of the carbon cloth 202), so that the resistance of the cathode 2 can be effectively reduced, and the catalyst (manganese dioxide and activated carbon powder) can accelerate the reaction process efficiency, so that the electricity generation performance of the air cathode biofuel cell can be enhanced. In the embodiment, the mode that three battery units are connected in series is adopted, so that the voltage and the operation effect of the whole battery are improved.
The inventor researches and discovers that the maximum working voltage of the existing microbial fuel cell can be about hundreds of millivolts. This is mainly due to the slow oxidation rate of the substrate by the microorganisms, the low electron transfer rate, the low cathode activation potential, the large internal resistance of the cell, and so on. In order to enhance the output power of the microbial fuel cell, the inventors have made a lot of research, and made great efforts on the aspect of electrode materials, especially the material and structure of the cathode material can directly influence the electron acceptance rate and further influence the electricity generation power. In the experimental process, the output power, coulombic efficiency and energy efficiency are often adopted to evaluate the capacity condition of the battery, wherein the power is the most common evaluation index. And the maximum possible output power can be obtained only when the internal resistance and the external resistance of the battery are equal. Minimizing the internal resistance of the battery system is a method for improving productivity.
The air cathode biofuel cell of the invention has the maximum voltage of 1.2V. After sludge is treated by the air cathode microbial fuel cell for two weeks, COD of the sludge is degraded to 51.23mg/L from the initial 316mg/L, the removal rate of the COD reaches 83%, and simultaneously, the specific resistance of the sludge is reduced to 1.45 multiplied by 108s2The sludge reaches an easily dehydrated state.
The above description is only an embodiment of the present invention, but the scope of the present invention is not limited thereto, and any alternative or alternative method that can be easily conceived by those skilled in the art within the technical scope of the present invention should be covered by the scope of the present invention.

Claims (10)

1. An air cathode microbial fuel cell is characterized by comprising an organic glass container (4) filled with sludge and a plurality of cell units which are uniformly inserted into the sludge at intervals, wherein the cell units are sequentially connected in series through copper wires (5) and are externally connected with a resistor (3).
2. The air cathode microbial fuel cell according to claim 1, wherein the interval between adjacent cells is 2 cm.
3. The air cathode microbial fuel cell according to claim 1, wherein the number of the cell units is three.
4. An air cathode microbial fuel cell according to claim 3, characterized in that the resistance of the resistor (3) is 1000 Ω.
5. The air cathode microbial fuel cell according to any one of claims 1 to 4, wherein the cell unit comprises a cathode (2) and an anode (1) coaxially sleeved on the cathode (2);
the cathode (2) comprises a PVC pipe (201), an activated proton exchange membrane (203) and a carbon cloth (202) modified by graphene and a catalyst; the carbon cloth (202) and the proton exchange membrane (203) are sequentially wrapped at the lower part of the PVC pipe (201), the upper part of the proton exchange membrane (203) exceeds the carbon cloth (202), a plurality of vent holes are uniformly formed in the wrapping section of the PVC pipe (201), a copper wire (5) for series connection is inserted into the carbon cloth (202), and the copper wire (5) penetrates through the PVC pipe (201) and upwards penetrates out of the inner cavity of the PVC pipe (201);
the anode (1) is made into a cylinder shape by rolling a stainless steel wire net, the joint is connected through a copper wire (5), and meanwhile, the stainless steel wire net is also connected with a copper wire (5) used for series connection;
when the device is inserted, the top of the proton exchange membrane (203) is kept flush with the top of the sludge, and the top of the anode (1) is kept flush with the top of the sludge.
6. An air cathode microbial fuel cell according to claim 5, characterized in that the radial distance between the cathode (2) and the anode (1) is 2 cm.
7. The air cathode microbial fuel cell according to claim 5, wherein the PVC pipe (201) has a diameter of 1.5cm and a length of 20 cm; the size of the carbon cloth (202) is 6 multiplied by 13 cm; the size of the proton exchange membrane (203) is 8 multiplied by 17 cm; the number of the stainless steel wire meshes is three, the size of a single stainless steel wire mesh is 16 multiplied by 11cm, and the three stainless steel wire meshes are connected in series after being rolled into a cylinder shape.
8. The air cathode microbial fuel cell according to claim 5, wherein the vent hole has a diameter of 1 cm.
9. A method for preparing a cathode of an air cathode microbial fuel cell is characterized by comprising the following steps:
1) and graphene modification: dissolving aniline purified by reduced pressure distillation into 12mol/L HCl solution in a volume ratio of 110mL/L, and adding graphene powder in a mass ratio of 1: 9 to aniline monomer; after the ultrasonic dispersion is uniform, putting the carbon cloth (202), dropwise adding an APS solution under the conditions of ice bath and magnetic stirring to ensure that the molar ratio of APS to aniline in the reaction solution is 1: 1, after reacting for 6 hours, taking out the carbon cloth (202), soaking the carbon cloth in 1mol/L HCl solution until the color is not faded, washing the carbon cloth with deionized water, and drying the carbon cloth in a 60 ℃ oven;
2) and catalyst modification: weighing 2g of manganese dioxide and 2g of activated carbon powder, putting the manganese dioxide and the activated carbon powder into a beaker, adding 20ml of distilled water, mixing, adding 60 wt% of PTFE, and ultrasonically cleaning for 1 h; then brushing and coating the dried carbon cloth (202) on one side in contact with the PVC pipe (201), and naturally airing for 24 hours;
3) and the proton exchange membrane (203) is heated for 3 hours for activation in a water bath at 50 ℃ and then used, the proton exchange membrane (203) is covered on the carbon cloth (202), and the periphery and the bottom of the proton exchange membrane (203) are adhered by glass cement to prevent water seepage.
10. The method of preparing a cathode for an air cathode microbial fuel cell according to claim 9, wherein the APS solution is: 15.06g of ammonium persulfate was made up to 50mL with 1mol/L HCl solution.
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Cited By (1)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
CN113998773A (en) * 2021-11-01 2022-02-01 中国农业科学院都市农业研究所 Device and method for treating aquaculture sewage by using air cathode single-chamber microbial fuel cell

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CN105000667A (en) * 2015-06-05 2015-10-28 南开大学 Constructed wetland and microbial fuel cell combined sewage treatment system
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EP3012891A1 (en) * 2014-10-21 2016-04-27 Korea Advanced Institute of Science and Technology Current collector-catalyst monolithic three-dimensional nanofiber network for li-air batteries and manufacturing method thereof
CN106207208A (en) * 2016-07-04 2016-12-07 河海大学 A kind of microbiological fuel cell and the application in denitrogenation of waste water thereof
CN108172793A (en) * 2017-12-27 2018-06-15 辽宁工程技术大学 Centrifuge the method for preparing three-dimensional carbon foam/graphene oxide based composites

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Publication number Priority date Publication date Assignee Title
CN101431161A (en) * 2007-12-29 2009-05-13 哈尔滨工业大学 Pipe type lifting-flow air cathode microbiological fuel cell
CN102437348A (en) * 2011-12-08 2012-05-02 西安交通大学 Non-noble metal-catalyzed polymer fibrous membrane hydroborate fuel cell
CN103922487A (en) * 2014-04-25 2014-07-16 内蒙古科技大学 Method of preparing methanol by sewage treatment and carbon dioxide reduction
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CN105060630A (en) * 2015-08-01 2015-11-18 安徽工程大学 Control apparatus for acid mine drainage
CN106207208A (en) * 2016-07-04 2016-12-07 河海大学 A kind of microbiological fuel cell and the application in denitrogenation of waste water thereof
CN108172793A (en) * 2017-12-27 2018-06-15 辽宁工程技术大学 Centrifuge the method for preparing three-dimensional carbon foam/graphene oxide based composites

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* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
CN113998773A (en) * 2021-11-01 2022-02-01 中国农业科学院都市农业研究所 Device and method for treating aquaculture sewage by using air cathode single-chamber microbial fuel cell

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