CN105810954A - Active carbon air negative electrode and preparation method thereof - Google Patents

Active carbon air negative electrode and preparation method thereof Download PDF

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Publication number
CN105810954A
CN105810954A CN201610207901.7A CN201610207901A CN105810954A CN 105810954 A CN105810954 A CN 105810954A CN 201610207901 A CN201610207901 A CN 201610207901A CN 105810954 A CN105810954 A CN 105810954A
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negative electrode
active carbon
activated carbon
air negative
preparation
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张恩仁
罗月
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Yangzhou University
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Yangzhou University
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    • H—ELECTRICITY
    • H01—ELECTRIC ELEMENTS
    • H01M—PROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
    • H01M4/00—Electrodes
    • H01M4/86—Inert electrodes with catalytic activity, e.g. for fuel cells
    • H01M4/8647—Inert electrodes with catalytic activity, e.g. for fuel cells consisting of more than one material, e.g. consisting of composites
    • H01M4/8657—Inert electrodes with catalytic activity, e.g. for fuel cells consisting of more than one material, e.g. consisting of composites layered
    • 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
    • H01M4/8878—Treatment steps after deposition of the catalytic active composition or after shaping of the electrode being free-standing body
    • H01M4/8896—Pressing, rolling, calendering
    • 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
    • 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
    • Y02P—CLIMATE CHANGE MITIGATION TECHNOLOGIES IN THE PRODUCTION OR PROCESSING OF GOODS
    • Y02P70/00—Climate change mitigation technologies in the production process for final industrial or consumer products
    • Y02P70/50—Manufacturing or production processes characterised by the final manufactured product

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  • Chemical & Material Sciences (AREA)
  • General Chemical & Material Sciences (AREA)
  • Chemical Kinetics & Catalysis (AREA)
  • Electrochemistry (AREA)
  • Manufacturing & Machinery (AREA)
  • Engineering & Computer Science (AREA)
  • Life Sciences & Earth Sciences (AREA)
  • Composite Materials (AREA)
  • Biochemistry (AREA)
  • Microbiology (AREA)
  • Sustainable Development (AREA)
  • Sustainable Energy (AREA)
  • Inert Electrodes (AREA)

Abstract

The invention discloses an active carbon air negative electrode and a preparation method thereof. The air negative electrode comprises an active carbon catalytic layer, a stainless steel mesh substrate and a polytetrafluoroethylene micropore filter membrane, wherein the active carbon catalytic layer is prepared by uniformly stirring active carbon, absolute ethyl alcohol and a polytetrafluoroethylene (PTFE) emulsion. The preparation method comprises the following steps of (1) stirring the active carbon, the absolute ethyl alcohol and the PTFE emulsion to be in a bulk shape, rolling the mixture to a thin sheet, and naturally volatilizing and drying the thin sheet to obtain the active carbon catalytic layer; and (2) placing the active carbon, the stainless steel mesh and the polytetrafluoroethylene micropore filter membrane in a die, and pressing and combining the obtained mixture by a vulcanizing machine under 17MPa. The air negative electrode prepared according to the method is low in cost, and the preparation process is rapid, simple and convenient; moreover, the air negative electrode represents relatively stable catalytic activity and electrochemical performance in a microbial fuel cell; and the problems of high cost and difficulty in expanded production of the microbial fuel cell are solved.

Description

A kind of active carbon air negative electrode and preparation method thereof
Technical field
The present invention relates to a kind of active carbon air negative electrode and preparation method thereof.
Background technology
Along with environmental pollution and energy starved are day by day serious, microbiological fuel cell is considered as one of following important technology processing sewage and energy regeneration.But for practical application, reduce the cost using cathode material in microbiological fuel cell and to select a kind of fast and convenient cathode preparation method be requisite.Research shows, CoTMPP, FePC, MnO2Can as the succedaneum of Pt catalyst, PTFE emulsion at a low price can substitute for Nafion solution as catalysis adhesive.Meanwhile, stainless (steel) wire or nickel foam can as microorganism fuel cell cathode collectors, carbon paper (the ＄ 1000/m that these materials are conventional compared to laboratory2) cheaply many on cost.Relative to metallic catalyst negative electrode, optimal succedaneum is the material with carbon element with significantly high surface area, such as graphite granule and activated carbon.Activated carbon is a kind of cheap, and porous material is applied in air cathode and shows, as catalyst, the chemical property that good catalysis is active and stable.Meanwhile, the extension application of cell reaction device and the feasibility of sewage disposal are implemented in being heavily dependent on the preparation of negative electrode, performance and cost.Therefore, it is required at present for selecting the cathode preparation method that a kind of extension being conducive to microbiological fuel cell produces.
Summary of the invention
In order to solve microbiological fuel cell high cost, extension produces difficult problem, selects a kind of low cost and method simple for production most important.The preparation method that the invention provides a kind of active carbon air negative electrode, solves the problems referred to above.
For achieving the above object, the present invention provides following technical scheme:
Air cathode of the present invention is to be made up of activated carbon catalysis layer, stainless (steel) wire matrix material and PTFE microporous filter membrane, compressed together with vulcanizer under a certain pressure, makes electrode；Wherein activated carbon catalysis layer is stirred according to a certain percentage by activated carbon, dehydrated alcohol and PTFE emulsion and to make.
The preferred SUS316 type of described stainless (steel) wire, order number 40-100 order.The preferred aperture 0.45um of described politef hydrophobic membrane, hydrophobic, air-permeability and corrosion-resistant.Described pressure is 17MPa, press time 5min.
The preparation method of active carbon air negative electrode of the present invention, comprises the steps:
(1) activated carbon, dehydrated alcohol and politef (PTFE) emulsion are stirred into bulk；, roll into the thin slice that thickness is 10mm, volatilization naturally, drying, obtain activated carbon catalysis layer；Activated carbon catalysis layer can be cut into required size；
(2) by compressed together under a certain pressure to activated carbon catalysis layer, stainless (steel) wire and politef microporous filter membrane, electrode is made.
In its step (1), activated carbon catalysis layer is stirred according to a certain percentage by activated carbon, dehydrated alcohol and PTFE emulsion and to make.Preferred activated carbon: the quality of PTFE emulsion is 3:7, dehydrated alcohol and activated carbon ratio are 2.85L:1g.
Drying temperature described in step (1) is 80 DEG C, time 2h.
In step (2), during compacting, described activated carbon catalysis layer, stainless (steel) wire and politef microporous filter membrane are to put according to position upper in lower.
Active carbon air negative electrode of the present invention be made as stainless (steel) wire matrix material, Catalytic Layer, the mutual consolidated structure of diffusion layer three layers.With the diffusion layer phase ratio smeared of self-control, diffusion layer in this invention is commercially available politef microporous filter membrane, there is good waterproof and breathable performance, the oxygen that ensure that in air enters cathode surface through diffusion layer, promote that catalyst reacts on negative electrode, substantially increase production efficiency simultaneously, reduce cost.Stainless (steel) wire is commercially available SUS316 type 40 order, string diameter 0.25mm, mesh 0.385mm, and its price is cheap, smooth surface, non-corrosive, corrosion-resistant, is a kind of conventional cathode base material.While considering that negative electrode prepares low cost problem and the making of succinct technique, stainless (steel) wire ensure that electrode has and stablizes firm internal structure, the concordance of holding electrode performance.
The air cathode present invention prepared is positioned in vaccinated single-chamber microbial fuel cell, is assembled into a single-chamber microbial fuel cell with the air cathode that carbon felt is biological anode with preparation, and recording its initial COD is 1380mg/L, regulates pH to 7.0.By constantly changing the culture fluid in battery chamber, the discharge curve of battery is cyclically-varying, and ceiling voltage reaches 517mV (under 100 Ω resistance condition), and periodically can maintain more than 500h.Compared with Pt-C air cathode prepared by same process, it is 27mA that activated carbon cathode can bear maximum current, and maximum power density can reach (2317 ± 12) mW/m2, its power density exceeds the 24% of Pt-C negative electrode.Meanwhile, compared to traditional electrode preparation section time, this kind of method removes dried outside the 2h time, and its whole processing technology required time is only 15min, is conducive to the mass production in practical application.
Accompanying drawing explanation
Fig. 1 is single-chamber microbial fuel cell structure of reactor figure；
Fig. 2 is the scanning electron microscope (SEM) photograph preparing activated carbon catalysis layer；
Fig. 3 is the scanning electron microscope (SEM) photograph of diffusion layer after compacting；
Fig. 4 is active carbon air cathodic discharge curve chart；
Fig. 5 is the polarization curve of active carbon air negative electrode.
Detailed description of the invention
Below according to drawings and Examples, the present invention is discussed further and explanation.
Embodiment one
The first step: the preparation of active carbon air negative electrode and sign
By activated carbon with dehydrated alcohol according to the ratio mixing and stirring that mass fraction is 0.35g/mL, add PTFE emulsion according to the ratio that activated carbon and PTFE mass ratio are 3:7 afterwards, be stirred continuously until in till soft solid-state bulk；With rotatingcylindrical drum, bulk activated carbon is rolled into the thin slice of 10mm thickness, naturally after volatilization 30min, puts into 80 DEG C of baking oven inner drying 2h, be cooled to room temperature.Select suitable irony mould, activated carbon thin slice, stainless (steel) wire and microporous teflon membran are put in mould according to order from bottom to up, under 17MPa, suppress 5min with vulcanizer, namely complete the preparation of negative electrode.
The activated carbon thin slice being pressed into by field emission microscopy observation and the surface texture of diffusion layer.Fig. 2 is activated carbon cathode, and closely, the material surface after compacting still has obvious hole, and has certain aperture in activated carbon granule distribution；Fig. 3 is politef microporous filter membrane, and activated carbon granule is irregular is distributed in filter membrane surface, is conducive to O2Enter cathode surface from diffusion layer, promote that catalyst reacts on negative electrode.Activated-carbon catalyst and the extruding of PTFE filter membrane, do not block the hole of PTFE filter membrane itself, be also mixed with by catalyst simultaneously, also show good catalytic performance when playing the performance of hydrophobic, air-permeability of filter membrane itself.
Second step: the checking of active carbon air electrochemical cathode performance
The air cathode of preparation is loaded in single chamber reactor shown in Fig. 1.1 is air cathode (working electrode), and 2 is biological anode (to electrode), and 3 is saturated calomel electrode (reference electrode), and 4 is lucite anode chamber.
Anolyte is simulation sewage, adds 1.64g/L sodium acetate Organic substance.With biological anode unit, the air cathode of preparation is dressed up single chamber is biological fuel cell, connects 100 Ω resistance, the cyclically-varying (Fig. 4) of observation period discharge curve.Initial start stage, reaction cell voltage when running to 1h rises very rapidly up to 517mV, after basically reach at about 450mV again stable, terminate at about 30h battery one periodic discharging, hereafter anode culture medium is changed through constantly, it will be seen that voltage rises rapidly again and reaches stable, thus generating period change.Therefore the cyclically-varying of voltage illustrates with the battery operation success that activated carbon cathode starts, it is possible to produce higher voltage, and its performance is still very stable when 400h, in order to life-time service.
When cell output voltage is stablized, NEWARE battery testing system is adopted to measure the polarization curve (Fig. 5) of negative electrode, by itself and the Pt-C air cathode contrast being prepared from said method, the output voltage of battery reduces with the increase of electric current, with the AC MFC the being negative electrode maximum current that can bear for 27mA, Pt-C air cathode can reach 24mA, and maximum power density reaches (2317 ± 12) mW/m2, than (1783 ± 7) mW/m being negative electrode with Pt-C air cathode2Exceed about 24%.Therefore, the air cathode for this invention preparation is cheap, and preparation technology is simple, and chemical property is more excellent, is conducive to the extension of microbiological fuel cell to produce.

Claims (9)

1. an active carbon air negative electrode, it is characterised in that this air cathode is to be made up of activated carbon catalysis layer, stainless (steel) wire matrix and politef microporous filter membrane；Wherein activated carbon catalysis layer is stirred by activated carbon, dehydrated alcohol and PTFE emulsion and to make.
2. active carbon air negative electrode according to claim 1, it is characterised in that described stainless (steel) wire is SUS316 type, order number 40-100 order.
3. active carbon air negative electrode according to claim 1, it is characterised in that described politef hydrophobic membrane aperture 0.45um, hydrophobic, air-permeability and corrosion-resistant.
4. active carbon air negative electrode according to claim 1, it is characterised in that described pressure is 17MPa, press time 5min.
5. the preparation method of an active carbon air negative electrode, it is characterised in that: it is by compressed together to activated carbon catalysis layer, stainless (steel) wire matrix material and PTFE microporous filter membrane vulcanizer, makes electrode；Wherein activated carbon catalysis layer is stirred according to a certain percentage by activated carbon, dehydrated alcohol and PTFE emulsion and to make.
6. method according to claim 5, it is characterised in that comprise the steps:
(1) activated carbon, dehydrated alcohol and ptfe emulsion are stirred into bulk, roll into the thin slice that thickness is 10mm, volatilization naturally, drying, obtain activated carbon catalysis layer；
(2) activated carbon catalysis layer, stainless (steel) wire and politef microporous filter membrane are put in a mold, merge with vulcanizer compacting under 17MPa.
7. the preparation method of active carbon air negative electrode according to claim 6, it is characterised in that described drying temperature is 80 DEG C, time 2h.
8. the preparation method of active carbon air negative electrode according to claim 5, it is characterised in that described activated carbon catalysis layer, stainless (steel) wire and politef microporous filter membrane are to put according to position upper in lower.
9. the preparation method of active carbon air negative electrode according to claim 5, it is characterised in that activated carbon: the quality of PTFE emulsion is 3:7, dehydrated alcohol and activated carbon ratio are 2.85L:1g.
CN201610207901.7A 2016-04-05 2016-04-05 Active carbon air negative electrode and preparation method thereof Pending CN105810954A (en)

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Cited By (5)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
CN107623130A (en) * 2017-10-13 2018-01-23 吉林大学 A kind of air cathode of imitative fish gill filament structure
CN108063300A (en) * 2017-12-14 2018-05-22 合肥伏雷科技有限公司 A kind of air electrode surface hydrophobicity effect processing method
CN108213070A (en) * 2018-01-10 2018-06-29 清华大学 A kind of original position is electronic-device and method of electrochemistry collaboration repairing polluted soil and underground water
CN108767265A (en) * 2018-06-19 2018-11-06 哈尔滨工业大学 A kind of single-chamber microbial fuel cell activated carbon-film-air cathode and preparation method thereof
CN110707334A (en) * 2019-11-13 2020-01-17 刘伟春 Heat seal vulcanization pressing method for air electrode in metal-air battery

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Publication number Priority date Publication date Assignee Title
CN1450677A (en) * 2002-07-31 2003-10-22 吉林省华成新能源电控有限公司 Air electrode
CN2932637Y (en) * 2006-04-11 2007-08-08 北京长力联合能源技术有限公司 A zinc-air metal fuel battery oxygen electrode made by way of cold pressure technique
CN102655235A (en) * 2012-03-09 2012-09-05 南开大学 Microbial fuel cell air cathode and preparation method thereof
CN102709572A (en) * 2012-07-03 2012-10-03 北京中航长力能源科技有限公司 Novel air electrode and preparation method thereof

Patent Citations (4)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
CN1450677A (en) * 2002-07-31 2003-10-22 吉林省华成新能源电控有限公司 Air electrode
CN2932637Y (en) * 2006-04-11 2007-08-08 北京长力联合能源技术有限公司 A zinc-air metal fuel battery oxygen electrode made by way of cold pressure technique
CN102655235A (en) * 2012-03-09 2012-09-05 南开大学 Microbial fuel cell air cathode and preparation method thereof
CN102709572A (en) * 2012-07-03 2012-10-03 北京中航长力能源科技有限公司 Novel air electrode and preparation method thereof

Cited By (7)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
CN107623130A (en) * 2017-10-13 2018-01-23 吉林大学 A kind of air cathode of imitative fish gill filament structure
CN108063300A (en) * 2017-12-14 2018-05-22 合肥伏雷科技有限公司 A kind of air electrode surface hydrophobicity effect processing method
CN108063300B (en) * 2017-12-14 2021-11-05 合肥伏雷科技有限公司 Surface hydrophobic effect treatment method for air electrode and air contact
CN108213070A (en) * 2018-01-10 2018-06-29 清华大学 A kind of original position is electronic-device and method of electrochemistry collaboration repairing polluted soil and underground water
CN108767265A (en) * 2018-06-19 2018-11-06 哈尔滨工业大学 A kind of single-chamber microbial fuel cell activated carbon-film-air cathode and preparation method thereof
CN110707334A (en) * 2019-11-13 2020-01-17 刘伟春 Heat seal vulcanization pressing method for air electrode in metal-air battery
CN110707334B (en) * 2019-11-13 2021-01-12 刘伟春 Heat seal vulcanization pressing method for air electrode in metal-air battery

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