CN105375049A - Carbon tubular oxygen reduction cathode microbial fuel cell and preparation method thereof - Google Patents
Carbon tubular oxygen reduction cathode microbial fuel cell and preparation method thereof Download PDFInfo
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- CN105375049A CN105375049A CN201510925280.1A CN201510925280A CN105375049A CN 105375049 A CN105375049 A CN 105375049A CN 201510925280 A CN201510925280 A CN 201510925280A CN 105375049 A CN105375049 A CN 105375049A
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- H—ELECTRICITY
- H01—ELECTRIC ELEMENTS
- H01M—PROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
- H01M8/00—Fuel cells; Manufacture thereof
- H01M8/16—Biochemical fuel cells, i.e. cells in which microorganisms function as catalysts
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- 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
- H01M4/8605—Porous electrodes
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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
- H01M4/88—Processes of manufacture
- H01M4/8817—Treatment of supports before application of the catalytic active composition
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- Y02—TECHNOLOGIES OR APPLICATIONS FOR MITIGATION OR ADAPTATION AGAINST CLIMATE CHANGE
- Y02E—REDUCTION OF GREENHOUSE GAS [GHG] EMISSIONS, RELATED TO ENERGY GENERATION, TRANSMISSION OR DISTRIBUTION
- Y02E60/00—Enabling technologies; Technologies with a potential or indirect contribution to GHG emissions mitigation
- Y02E60/30—Hydrogen technology
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Abstract
The invention discloses a carbon tubular oxygen reduction cathode microbial fuel cell and a preparation method thereof. The carbon tubular oxygen reduction cathode microbial fuel cell comprises an anode and a cathode and is characterized in that the cathode adopts a bamboo charcoal tube, wherein the outer surface of the bamboo charcoal tube is coated with polytetrafluoroethylene emulsion with the concentration of 5-10% and a partition membrane with pore size less than 1 m um is mounted on the inner surface of the bamboo charcoal tube; the outer side of the cathode is wound with a titanium wire, the anode is inserted in the bamboo charcoal tube along the axial direction of the bamboo charcoal tube, and the anode adopts carbon cloth, a carbon brush, carbon paper, carbon felt, a carbon rod or graphite flake; an end plate is arranged at each of the two ends of the cathode and the end plates are fixed with bolts; an electrolyte inlet is formed in one of the end plates and an electrolyte outlet is formed in the other end plate. Since a natural and cheap porous material is used as a precursor and a structural material, the fuel cell is low in cost and has good application prospect.
Description
Technical field
The present invention relates to microbiological fuel cell, be specifically related to carbonaceous tubular type oxygen reduction cathode microbiological fuel cell and preparation method.
Background technology
Microbiological fuel cell (MicrobialFuelCells, MFCs) be a kind ofly utilize microbe that the chemical energy in organic substance is directly changed into the device of electric energy, have that fuel source is extensive, reaction condition is gentle, good biocompatibility, while generation electric energy, carry out waste water treatment unique advantage, become the focus that global regenerative resource researcher pays close attention to.But although in the past few decades, the performance of microbiological fuel cell obtains great lifting, low power density and high cost are still two large bottlenecks of restriction micro-organisms fuel cell practice.Negative electrode is as the important component part of microbiological fuel cell, and the rate of reduction of its performance characteristics and electron acceptor is closely related; Therefore, negative electrode just becomes a kind of very important limiting factor.Meanwhile, research finds, adopts carbonaceous cathodes material under low cost condition, largely can promote the performance of battery, so, find a kind of low cost, high performance cathode material is of great significance with regard to tool.
The negative electrode that microbiological fuel cell is conventional is mainly divided into chemical cathode and air cathode.Chemical cathode mainly uses a series of chemicals such as the potassium ferricyanide, potassium peroxydisulfate and postassium hypochlorite as cathode electronics acceptor.Air cathode is by the oxygen in use air as final electron acceptor, and its wide material sources, product is pollution-free, advantages of simple structure and simple.Air cathode is generally made up of cathode construction material and catalyst.Conventional catalyst mainly contains following several method: 1.. platinum metal catalyst.2.. transition-metal catalyst.Such as: manganese, ferric iron, cobalt, silver, titanium etc.3.. carbonaceous catalyst.Such as: active carbon, the carbonaceous material such as cellulose modified of the element such as nitrogen and phosphorus.And conventional cathode material has: 1.. carbon cloth/active carbon cloth.2.. carbon felt.3.. carbon paper.4.. carbon fiber, 5.. carbon yarn etc.
Because chemical cathode can cause secondary pollution and cost intensive, be unsuitable for extensive practice.Extensively study mainly for air cathode at present, but these conventional cathode materials above-mentioned generally have the shortcoming that mechanical performance is poor, make processing technology complexity, and the cost of metallic cathode catalyst is higher, also may cause heavy metal pollution.Therefore, carbonaceous catalyst that is cheap, better performances has better practice prospect, but carbonaceous cathodes catalyst and cathode construction still need research further and improve at present.
Summary of the invention
Technical problem to be solved by this invention is to provide carbonaceous tubular type oxygen reduction cathode microbiological fuel cell and preparation method.
In order to solve the problems of the technologies described above, first technical scheme of the present invention is: carbonaceous tubular type oxygen reduction cathode microbiological fuel cell preparation method, is characterized in that: comprise the following steps:
A. cathode material carbonization: fresh bamboo trunk is positioned among baking oven, toast 3 ~ 7 days in the baking oven of temperature 80 ~ 105 DEG C, again dry bamboo trunk is positioned over high-temperature atmosphere furnace, after high-temperature atmosphere stove evacuation, filling nitrogen, with the heating rate of 1 ~ 3 DEG C/min heating 900 ~ 1000 DEG C, under nitrogen atmosphere, nitrogen flow 100 ~ 300cm
3/ min, carbonization 2 ~ 3 hours, is down to less than 100 DEG C taking-ups by furnace temperature; Under again bamboo trunk being positioned over air ambient, 330 ~ 350 DEG C of temperature carry out heat treatment in 2 ~ 3 hours, then the inner surface of heat treated bamboo trunk and outer surface are polished, obtain wall thickness and be about 2 ~ 3mm, the bamboo charcoal tube that length is certain;
B. negative electrode preparation: bamboo charcoal tube deionized water is cleaned, then dries; By the concentration prepared be 5 ~ 10% polytetrafluoroethylene (PTFE) emulsion evenly brush outer wall at bamboo charcoal tube, and to heat 20 ~ 30 minutes under 330 ~ 370 DEG C of conditions; And then mount at bamboo charcoal tube inwall the separation membrane that one deck hole is less than 1 μm;
C. battery assembling: the cathode outer side prepared in stepb is wound around titanium silk, anode inserts in bamboo charcoal tube along bamboo charcoal tube axial direction; Load onto end plate respectively at bamboo charcoal tube two ends, and fix with bolt; An end plate leaves electrolyte inlet wherein, another end plate leaves electrolyte outlet, form carbonaceous tubular type oxygen reduction cathode microbiological fuel cell.
For carbonaceous oxygen reduction catalyst and the cathode construction of preparation high efficiency, low cost, the present invention will adopt bamboo trunk as presoma.
Concrete principle of the present invention is: first using the bamboo with nitrogen phosphorus enrichment material as the presoma of negative electrode and architecture basics, carry out drying under cryogenic, under preventing higher baking temperature, bamboo trunk bursts, and treats that its dehydration is to the drying that to a certain degree heats up afterwards, guarantees bamboo trunk drying and dehydrating.The bamboo of drying is carried out carbonization under nitrogen atmosphere, and this not only ensure that natural tubular structure and the microcellular structure of bamboo, obtains simultaneously and is rich in nitrogen P elements carbonaceous material, and high temperature cabonization ensure that char-forming material has lower ohmic internal resistance.This nitrogen phosphorus enrichment carbonaceous material has a large amount of C-N and C-P chemical bonds, has better oxygen desorption and catalytic action for oxygen reduction reaction, makes carbonaceous cathodes have good hydrogen reduction performance.The bamboo charcoal tube that carbonization completes heat treatment at about 350 DEG C temperature can be good at being oxidized a part of carbon, makes bamboo charcoal tube have more flourishing microcellular structure, to reach good oxygen transmission characteristic.Outside external coating 5 ~ 10% ptfe emulsion can effective anti-sealing infiltration and saltout, avoid the oxygen transmission caused thus simultaneously and be obstructed.The barrier material that one deck hole that inside pipe wall mounts is less than 1 μm, can effectively prevent from directly contacting the short circuit caused between anode and cathode, bacterium can be stoped to grow at negative electrode through separation membrane simultaneously, thus avoid the adverse effect of biomembrane target performance.
According to the preferred version of carbonaceous tubular type oxygen reduction cathode microbiological fuel cell preparation method of the present invention, described separation membrane adopts poly (ether sulfone) film, poly tetrafluoroethylene, polyvinylidene fluoride film or glass fibre membrane etc.
According to a kind of preferred version of carbonaceous tubular type oxygen reduction cathode microbiological fuel cell preparation method of the present invention, the anode substrate of described microbiological fuel cell adopts carbon cloth, carbon brush, carbon paper, carbon felt, carbon-point or graphite flake.
Second technical scheme of the present invention is: carbonaceous tubular type oxygen reduction cathode microbiological fuel cell, comprises anode and negative electrode, it is characterized in that: described negative electrode adopts bamboo carbon pipe; The outer surface of this bamboo carbon pipe is coated with the ptfe emulsion that concentration is 5 ~ 10%, and the inner surface of this bamboo carbon pipe is pasted with the separation membrane that hole is less than 1 μm; Cathode outer side is wound around titanium silk, and anode inserts in bamboo charcoal tube along bamboo charcoal tube axial direction, and anode adopts carbon cloth, carbon brush, carbon paper, carbon felt, carbon-point or graphite flake; Be respectively arranged with end plate at negative electrode two ends, end plate is bolted; An end plate is provided with electrolyte inlet wherein, another end plate is provided with electrolyte outlet.
According to a kind of preferred version of carbonaceous tubular type oxygen reduction cathode microbiological fuel cell of the present invention, described separation membrane adopts poly (ether sulfone) film, poly tetrafluoroethylene, polyvinylidene fluoride film or glass fibre membrane.
The beneficial effect of carbonaceous tubular type oxygen reduction cathode microbiological fuel cell of the present invention and preparation method is: the present invention adopts the porous material of natural cheapness as presoma and structural material, greatly reduce on the one hand making and the processing cost of microbiological fuel cell, tubular structure is that the amplification of battery and scale provide good architecture basics simultaneously; Due to the enrichment of this material nitrogen phosphorus, make it have a large amount of C-N and C-P chemical bonds, for oxygen reduction reaction, there is better oxygen desorption and catalytic action, make carbonaceous cathodes have good hydrogen reduction performance, thus improve the performance of microbiological fuel cell; Energy consumption of the present invention is low, and method is simple, and easy to operate, cost is low, has a good application prospect.
Accompanying drawing explanation
Fig. 1 is carbonaceous tubular type oxygen reduction cathode principle of microbial fuel cells figure and pictorial diagram.
Fig. 2 is the photo under carbonaceous bamboo trunk carbon cloth is placed in scanning electron microscopy.
Fig. 3 is the microbiological fuel cell performance map adopting the present invention to obtain.
Fig. 4 is COD clearance and coulombic efficiency under different COD condition.
Fig. 5 is COD clearance and coulombic efficiency under different extrernal resistance condition.
Embodiment
Below in conjunction with embodiment, the present invention is further described specifically, but embodiments of the present invention are not limited thereto.
With reference to figure 1, carbonaceous tubular type oxygen reduction cathode microbiological fuel cell, comprises anode 4 and negative electrode 3; Described negative electrode 3 adopts bamboo carbon pipe; The outer surface of this bamboo carbon pipe is coated with the ptfe emulsion that concentration is 5 ~ 10%, the inner surface of this bamboo carbon pipe is pasted with the separation membrane 5 that hole is less than 1 μm, and described separation membrane adopts poly (ether sulfone) film, poly tetrafluoroethylene, polyvinylidene fluoride film or glass fibre membrane; The outer wall of bamboo carbon pipe is wound around titanium silk 1, and anode 4 inserts in bamboo charcoal tube along bamboo charcoal tube axial direction, and anode 4 can adopt carbon cloth, carbon brush, carbon paper, carbon felt, carbon-point or graphite flake; Be respectively arranged with end plate 6 at negative electrode 3 two ends, end plate 6 adopts poly (methyl methacrylate) plate; An end plate arranges electrolyte inlet 7 wherein, another end plate is arranged electrolyte outlet 8; End plate 6 is fixed by bolt 2.
Embodiment 1: carbonaceous tubular type oxygen reduction cathode microbiological fuel cell preparation method, comprises the following steps:
A. cathode material carbonization: be positioned among baking oven by ready fresh bamboo trunk, toasts 7 days, guarantees that bamboo trunk dewaters completely at the temperature of 80 DEG C; Again the bamboo charcoal of drying is positioned over high-temperature atmosphere furnace, vacuumizes, fill nitrogen after be heated to 900 DEG C with the heating rate of 1 ~ 3 DEG C/min, under nitrogen atmosphere, with nitrogen flow 300cm
3/ min carbonization 2 hours, is down to less than 100 DEG C and takes out bamboo trunk by furnace temperature; Under again bamboo trunk being positioned over air ambient, among 350 DEG C of temperature baking ovens, carrying out heat treatment in 2 hours, then the inner surface of heat treated bamboo trunk and outer surface are polished, obtain wall thickness and be about 2 ~ 3mm, the bamboo charcoal tube that length is certain.
B. negative electrode preparation: bamboo charcoal tube deionized water is carried out cleaning and after drying, be that the ptfe emulsion of 8% is evenly brushed at bamboo charcoal tube outer wall by the concentration prepared, and under 330 DEG C of conditions, heat oven dry in 30 minutes; Carry out four brushings altogether; After polytetrafluoroethylene brushing completes, mount at inside pipe wall the separation membrane that one deck hole is less than 1 μm, separation membrane adopts polyether sulfone PES film.
C. battery assembling: be wrapped with titanium silk 1 at negative electrode outer wall, the carbon brush anode 3 diameter being less than bamboo charcoal tube internal diameter inserts in bamboo charcoal tube along bamboo charcoal tube y direction; Load onto end plate 6 respectively at bamboo charcoal tube two ends, and fix with bolt 2; End plate 6 adopts poly (methyl methacrylate) plate; An end plate arranges electrolyte inlet 7 wherein, another end plate is arranged electrolyte outlet 8; Form carbonaceous tubular type oxygen reduction cathode microbiological fuel cell.
Embodiment 2
Carbonaceous tubular type oxygen reduction cathode microbiological fuel cell preparation method, comprises the following steps:
A. cathode material carbonization: adopt fresh bamboo trunk as presoma.Ready fresh bamboo trunk is positioned among baking oven, bamboo trunk internal diameter 5cm, length 12cm, toasts 2 days under 40 DEG C of conditions, toast 3 days under 80 DEG C of conditions, guarantee that bamboo trunk dewaters completely.The bamboo charcoal of drying is positioned over high-temperature atmosphere furnace, vacuumizes, fill nitrogen after be heated to 1000 DEG C with the heating rate of 1.5 DEG C/min, under nitrogen atmosphere, nitrogen flow 250cm
3/ min carbonization 2.5 hours, treats that furnace temperature is down to less than 100 DEG C and is taken out bamboo trunk; Observe its microscopic characteristics under bamboo trunk after carbonization is arranged in scanning electron microscopy, find that the bamboo charcoal after carbonization can keep abundant porousness, for mass transfer provides good passage, Fig. 2 is shown in by the photo under scanning electron microscopy.
B. negative electrode preparation: under the bamboo charcoal tube that step A carbonization is good is positioned over air conditions, 330 DEG C of temperature carry out heat treatment in 2.5 hours; Then by heat treated bamboo charcoal tube respectively inner surface and outer surface polish, formed wall thickness be about 3mm, length is the bamboo charcoal tube of 6cm, and cleans with deionized water.Complete and clean and after drying, be that the ptfe emulsion of 5% is evenly brushed at pipe outer wall by the concentration prepared, and heat 25 minutes under 360 DEG C of conditions; Carry out three brushings altogether; Mount at inside pipe wall the separation membrane that one deck hole is less than 1 μm after polytetrafluoroethylene brushing completes, separation membrane is glass fibre membrane.
C. battery assembling: the negative electrode outer wall prepared in stepb is wrapped with titanium silk, and diameter is less than bamboo charcoal tube internal diameter, length is that the carbon-point anode of 4cm inserts in bamboo charcoal tube along bamboo charcoal tube y direction.Load onto end plate 6 respectively at bamboo charcoal tube two ends, and fix with bolt 2, an end plate arranges electrolyte inlet 7 wherein, another end plate is arranged electrolyte outlet 8; Form carbonaceous tubular type oxygen reduction cathode microbiological fuel cell.
D. the battery assembled Continuous Flow under 1000 Ω extrernal resistance conditions started, measure its performance curve after carrying out the cultivation of 10 days, as shown in Figure 3, experiment shows that this battery has good power output.Wherein nutrient media components is: 3.38 ~ 10.14g/LCH
3cOONa, 6g/LNa
2hPO
4, 1.5g/LKH
2pO
4, 0.05g/LNH
4cl, 0.5g/LNaCl, 0.1g/LMgSO
47H
2o, 15mg/LCaCl
22H
2o and 1.6mg/L trace element; Its medium trace element can adopt FeSO
47H
2o, ZnCl
2, MnCl4H
2o, H
3bO
3, CaCl
26H
2o, CuCl
22H
2o, NiCl
26H
2o or NaMoO
42H
2o, CoCl
26H
2o etc.
Embodiment 3: carbonaceous tubular type oxygen reduction cathode microbiological fuel cell preparation method, the method as different from Example 2 separation membrane is poly tetrafluoroethylene.By which preparation with after assembling battery, process the waste water of 200COD, 500COD, 1000COD, 1500COD respectively, its COD removal efficiency and coulombic efficiency are as shown in Figure 4.In COD situation, this carbonaceous tubular type oxygen reduction cathode microbiological fuel cell can realize higher COD clearance, has good waste treatment capacity.
Embodiment 4: carbonaceous tubular type oxygen reduction cathode microbiological fuel cell preparation method, the method as different from Example 2 separation membrane is polyvinylidene fluoride film, and under outer meeting resistance adopts 600 ohm, 200 ohm, 100 ohm, 50 ohm situations respectively, test this carbonaceous tubular type oxygen reduction cathode microbiological fuel cell COD removal efficiency and coulombic efficiency.As shown in Figure 5, illustrate when different extrernal resistance, this carbonaceous tubular type oxygen reduction cathode microbiological fuel cell can realize higher COD clearance, has good waste treatment capacity.And under certain loading condition, this single chamber MFC also has comparatively considerable coulombic efficiency, show that this battery can realize good energy regenerating.
Claims (4)
1. carbonaceous tubular type oxygen reduction cathode microbiological fuel cell preparation method, is characterized in that: comprise the following steps:
A. cathode material carbonization: fresh bamboo trunk is positioned among baking oven, toast 3 ~ 7 days in the baking oven of temperature 80 ~ 105 DEG C, again dry bamboo trunk is positioned over high-temperature atmosphere furnace, after high-temperature atmosphere stove evacuation, filling nitrogen, 900 ~ 1000 DEG C are heated to the heating rate of 1 ~ 3 DEG C/min, under nitrogen atmosphere, nitrogen flow 100 ~ 300cm
3/ min, carbonization 2 ~ 3 hours, is down to less than 100 DEG C and takes out bamboo trunk by furnace temperature; Under again bamboo trunk being positioned over air ambient, carrying out heat treatment in 2 ~ 3 hours 330 ~ 350 DEG C of temperature, obtain bamboo charcoal tube;
B. negative electrode preparation: bamboo charcoal tube deionized water is cleaned, then dries; By the concentration prepared be 5 ~ 10% ptfe emulsion evenly brush outer wall at bamboo charcoal tube, and to heat 20 ~ 30 minutes under 330 ~ 370 DEG C of conditions; And then mount at bamboo charcoal tube inwall the separation membrane (5) that one deck hole is less than 1 μm;
C. battery assembling: anode (4) is inserted in bamboo charcoal tube along bamboo charcoal tube axial direction; Load onto end plate (6) at bamboo charcoal tube two ends respectively, and fix with bolt (2); An end plate leaves electrolyte inlet wherein, another end plate leaves electrolyte outlet, form carbonaceous tubular type oxygen reduction cathode microbiological fuel cell.
2. carbonaceous tubular type oxygen reduction cathode microbiological fuel cell preparation method according to claim 1, is characterized in that: described separation membrane adopts poly (ether sulfone) film, poly tetrafluoroethylene, polyvinylidene fluoride film or glass fibre membrane.
3. carbonaceous tubular type oxygen reduction cathode microbiological fuel cell, comprises anode (4) and negative electrode (3), it is characterized in that: described negative electrode (3) adopts bamboo charcoal tube; The outer surface of this bamboo charcoal tube is coated with the ptfe emulsion that concentration is 5 ~ 10%, and the inner surface of this bamboo carbon pipe is pasted with the separation membrane (5) that hole is less than 1 μm; Negative electrode outer wall is wound around titanium silk (1), and anode (4) inserts in bamboo charcoal tube along bamboo charcoal tube y direction; Be respectively arranged with end plate (6) at bamboo charcoal tube two ends, end plate (6) is fixed by bolt (2); An end plate is provided with electrolyte inlet wherein, another end plate is provided with electrolyte outlet.
4. carbonaceous tubular type oxygen reduction cathode microbiological fuel cell according to claim 3, is characterized in that: described separation membrane adopts poly (ether sulfone) film, poly tetrafluoroethylene, polyvinylidene fluoride film or glass fibre membrane.
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Cited By (4)
| Publication number | Priority date | Publication date | Assignee | Title |
|---|---|---|---|---|
| CN106505233A (en) * | 2016-11-10 | 2017-03-15 | 重庆大学 | A kind of microbiological fuel cell of bamboo charcoal bundled tube bubbling air cathode construction |
| CN108574105A (en) * | 2018-05-21 | 2018-09-25 | 西交利物浦大学 | A kind of air cathode of microbiological fuel cell |
| CN108649251A (en) * | 2018-05-28 | 2018-10-12 | 重庆大学 | Based on monoblock type carbonaceous from breathing cathode without film aminic acid fuel battery preparation method |
| CN108767301A (en) * | 2018-05-28 | 2018-11-06 | 重庆大学 | The controllable carbonaceous tubular type oxygen reduction cathode microbiological fuel cell of size and preparation method |
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| CN101485029A (en) * | 2006-05-02 | 2009-07-15 | 宾夕法尼亚州研究基金会 | Materials and configurations for scalable microbial fuel cells |
| CN103296278A (en) * | 2013-06-24 | 2013-09-11 | 西南大学 | Preparation method of plant material based energy conversion catalyst |
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Cited By (7)
| Publication number | Priority date | Publication date | Assignee | Title |
|---|---|---|---|---|
| CN106505233A (en) * | 2016-11-10 | 2017-03-15 | 重庆大学 | A kind of microbiological fuel cell of bamboo charcoal bundled tube bubbling air cathode construction |
| CN106505233B (en) * | 2016-11-10 | 2019-03-19 | 重庆大学 | A kind of microbiological fuel cell of bamboo charcoal bundled tube bubbling air cathode construction |
| CN108574105A (en) * | 2018-05-21 | 2018-09-25 | 西交利物浦大学 | A kind of air cathode of microbiological fuel cell |
| CN108649251A (en) * | 2018-05-28 | 2018-10-12 | 重庆大学 | Based on monoblock type carbonaceous from breathing cathode without film aminic acid fuel battery preparation method |
| CN108767301A (en) * | 2018-05-28 | 2018-11-06 | 重庆大学 | The controllable carbonaceous tubular type oxygen reduction cathode microbiological fuel cell of size and preparation method |
| CN108767301B (en) * | 2018-05-28 | 2021-03-12 | 重庆大学 | Size-controllable carbonaceous tubular oxygen reduction cathode microbial fuel cell and preparation method thereof |
| CN108649251B (en) * | 2018-05-28 | 2021-07-06 | 重庆大学 | Preparation method of membrane-free formic acid fuel cell based on integral carbonaceous self-breathing cathode |
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