CN101635361A - Membrane electrode and biofuel cell adopting same - Google Patents
Membrane electrode and biofuel cell adopting same Download PDFInfo
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- CN101635361A CN101635361A CN200810142523A CN200810142523A CN101635361A CN 101635361 A CN101635361 A CN 101635361A CN 200810142523 A CN200810142523 A CN 200810142523A CN 200810142523 A CN200810142523 A CN 200810142523A CN 101635361 A CN101635361 A CN 101635361A
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Abstract
The invention relates to a membrane electrode, comprising a proton exchange membrane, an anode electrode and a cathode electrode, wherein, the anode electrode and the cathode electrode are respectively arranged on the two opposite surfaces of the proton exchange membrane; and the anode electrode comprises at least one carbon nano tube long-line composite structure, and the carbon nano tube long-line composite structure comprises a carbon nano tube long line and enzyme catalyst distributed in the carbon nano tube long line.
Description
Technical field
The present invention relates to a kind of membrane electrode and adopt the biological fuel cell of this membrane electrode, relate in particular to a kind of based on carbon nano-tube membrane electrode and adopt the biological fuel cell of this membrane electrode.
Background technology
Fuel cell is a kind of electrochemical generating unit that fuel and oxidant gas is converted into electric energy, the fields such as military and national defense and civilian electric power, automobile, communication that are widely used in (see also, Recentadvances in fuel cell technology and its application, Journal of Power Sources, V100, P60-66 (2001)).
Biological fuel cell is to be catalyst with the enzyme, the chemical energy in the organic substance is converted into the device of electric energy.Usually, the prior biological fuel cell comprises: a membrane electrode (Membrane ElectrodeAssembly, be called for short MEA), this membrane electrode comprises a proton exchange membrane (Proton ExchangeMembrane) and is separately positioned on the cathode electrode and the anode electrode of two facing surfaces of proton exchange membrane; One is equipped with the anode room of bio-fuel, and anode electrode is soaked in this bio-fuel; One baffler (Flow Field Plate is called for short FFP) is arranged at the surface of cathode electrode away from proton exchange membrane; One collector plate (Current Collector Plate is called for short CCP) is arranged at the surface of baffler away from proton exchange membrane; And relevant accessory, as: air blast, valve, pipeline etc.
Wherein, anode electrode comprises a carbon fiber paper and the enzyme catalyst that is distributed in this carbon fiber paper surface.Cathode electrode comprises that a gas diffusion layers and is arranged at the catalyst layer of this gaseous diffusion laminar surface, and catalyst layer is between proton exchange membrane and gas diffusion layers.This catalyst layer includes catalyst material (be generally noble metal granule, as: platinum, gold or ruthenium etc.) and carrier thereof (be generally carbon granule, as: graphite, carbon black, carbon fiber or carbon nano-tube).Described gas diffusion layers mainly is made of carbon fiber paper.Proton exchange membrane material is selected from perfluorinated sulfonic acid, polystyrolsulfon acid, polytrifluorostyrene sulfonic acid, phenolic resins sulfonic acid or hydrocarbon.
Yet, the membrane electrode of biological fuel cell of the prior art has the following disadvantages: first, since anode electrode comprise a carbon fiber paper and be distributed in this carbon fiber paper surface enzyme catalyst, on the one hand, contain a large amount of mixed and disorderly carbon fibers that distribute in this carbon fiber paper, cause carbon fiber paper mesopore structure distribution inhomogeneous, and specific area is little, thereby influenced the uniformity that enzyme catalyst distributes, made that the contact area of enzyme catalyst and bio-fuel is little, limited the utilance of catalyst; On the other hand, carbon fiber paper resistivity is big, has restricted the transmission of the electronics of reaction generation, thereby has directly influenced the reactivity of membrane electrode.Second, because cathode electrode comprises that a gas diffusion layers and is formed at the Catalytic Layer of gaseous diffusion laminar surface, on the one hand, this cathode electrode structure makes the membrane electrode of preparation have bigger thickness, and increased the contact resistance between the gas diffusion layers and Catalytic Layer in the membrane electrode, be unfavorable for reacting necessary electrical conductivity, thereby directly influenced the reactivity of membrane electrode; On the other hand, the catalyst in the Catalytic Layer in this cathode electrode structure divides distribution evenly, and is little with the contact area of reacting gas, limited the utilance of catalyst.
In view of this, necessaryly provide a kind of high reaction activity and high that has, and can improve the membrane electrode of utilance of catalyst and the biological fuel cell that adopts this membrane electrode.
Summary of the invention
A kind of membrane electrode, it comprises: a proton exchange membrane, one anode electrode and a cathode electrode, described anode electrode and cathode electrode are arranged at two facing surfaces of this proton exchange membrane respectively, wherein, described anode electrode comprises at least one carbon nanotube long line composite construction, and this carbon nanotube long line composite construction comprises that carbon nanotube long line and enzyme catalyst are distributed in this carbon nanotube long line.
A kind of biological fuel cell, it comprises: a proton exchange membrane; One anode electrode and a cathode electrode, described anode electrode and cathode electrode are separately positioned on two facing surfaces of this proton exchange membrane; One is equipped with the anode room of bio-fuel, and anode electrode is soaked in this bio-fuel; One baffler is arranged at the surface of cathode electrode away from proton exchange membrane; And air feed and air extractor are connected with this baffler, wherein, described anode electrode comprises at least one carbon nanotube long line composite construction, and this carbon nanotube long line composite construction comprises that carbon nanotube long line and enzyme catalyst are distributed in this carbon nanotube long line.
Compared to prior art, described membrane electrode has the following advantages: first, described anode electrode adopts the carbon nanotube long line composite construction, so avoided the contact resistance between the diffusion layer and catalyst layer in the prior art, helps reacting the conduction of the electronics that necessary electronics and reaction generate.The second, carbon nanotube long line has great specific area, so, adopt this carbon nanotube long line can be effective and catalyst-loaded uniformly, make enzyme catalyst and bio-fuel have bigger contact area, improved the utilance of enzyme catalyst.The 3rd, because the resistivity of carbon nano-tube itself will be lower than the resistivity of carbon fiber, so adopt the resistivity of anode electrode of this carbon nanotube long line composite construction low, can effectively conduct the electronics that necessary electronics of reaction and reaction generate, help to improve the reactivity of membrane electrode.
Description of drawings
Fig. 1 is the structural representation of the membrane electrode of the technical program embodiment.
The surperficial evaporation that Fig. 2 provides for the technical program embodiment has the partial sweep electromicroscopic photograph of the carbon nano-tube film of platinum layer.
Fig. 3 is the structural representation of the biological fuel cell of the technical program embodiment.
Embodiment
Below with reference to accompanying drawing the technical program is described in further detail.
See also Fig. 1, the technical program embodiment provides a kind of membrane electrode 200, and it comprises: a proton exchange membrane 202, one anode electrodes 204 and a cathode electrode 206.Described anode electrode 204 and cathode electrode 206 are separately positioned on two facing surfaces of this proton exchange membrane 202.At least one electrode in described anode electrode 204 and the cathode electrode 206 comprises a carbon nanotube long line composite construction.Wherein, described anode electrode 204 is the composite construction of a carbon nanotube long line and enzyme catalyst.Described cathode electrode 206 is the composite construction of a carbon nanotube long line and noble metal catalyst.
Described carbon nanotube long line comprises a plurality of carbon nano-tube that join end to end and be arranged of preferred orient.Particularly, in this carbon nanotube long line carbon nano-tube along this carbon nanotube long line axially/length direction be arranged in parallel or in the shape of a spiral shape arrange.Length of carbon nanotube is basic identical in this carbon nanotube long line, and combines closely by Van der Waals force between the adjacent carbon nano-tube.Described carbon nano-tube comprises one or more in Single Walled Carbon Nanotube, double-walled carbon nano-tube and the multi-walled carbon nano-tubes.The diameter of described Single Walled Carbon Nanotube is 0.5 nanometer～10 nanometers, and the diameter of double-walled carbon nano-tube is 1.0 nanometers～15 nanometers, and the diameter of multi-walled carbon nano-tubes is 1.5 nanometers～50 nanometers.The length of this carbon nano-tube is greater than 100 microns.In the present embodiment, preferably, the length of carbon nano-tube is 200～900 microns.
After described carbon nanotube long line can obtain a carbon nano-tube film by the carbon nano pipe array that stretches, through mechanical external force shrink process (surface tension effects of organic solvent volatilization); Reversing spinning handles or curls and obtain.The diameter of described carbon nanotube long line is 1 micron～1 millimeter, and its length is not limit, and can make according to the actual requirements.By above-mentioned carbon nanotube long line is soaked, can obtain the composite construction of carbon nanotube long line and enzyme catalyst in the glucose oxidase enzyme aqueous solution.Before the composite construction of preparation carbon nanotube long line and enzyme catalyst, need carbon nanotube long line through functionalization, with on the tube wall of the carbon nano-tube in carbon nanotube long line or end cap place introduce hydrophilic carboxyl (COOH) or hydroxyl (OH), improve the adsorptivity of carbon nano-tube to enzyme catalyst.So in the composite construction of this carbon nanotube long line and enzyme catalyst, enzyme catalyst is uniformly distributed in the carbon nano tube surface of carbon nanotube long line.Before the carbon nano-tube film that will pull is prepared into carbon nanotube long line, earlier noble metal catalyst is deposited to the carbon nano-tube film surface by physics or chemical method, again through mechanical external force shrink process (surface tension effects of organic solvent volatilization); Reverse the spinning processing or curl and to obtain the composite construction of carbon nanotube long line and noble metal catalyst.See also Fig. 2, platinum catalyst is uniformly distributed in the carbon nano tube surface of carbon nano-tube film.So in the composite construction of this carbon nanotube long line and noble metal catalyst, noble metal catalyst is uniformly distributed in the carbon nano tube surface of carbon nanotube long line.
Described enzyme catalyst can be any enzyme catalyst that can carry out catalysis to bio-fuel, as: contain the oxidizing ferment of prothetic group FAD or contain prothetic group NAD (P)
+Dehydrogenase.This enzyme catalyst evenly is adsorbed in the carbon nano tube surface in the carbon nanotube long line, and combines with this carbon nano-tube by carboxyl or hydroxyl.Be appreciated that to different bio-fuels selected enzyme catalyst difference.In the present embodiment, bio-fuel is a glucose solution, and enzyme catalyst is a glucose oxidase.
Described noble metal catalyst is a noble metal granule, as: the mixture of a kind of or its combination in any in platinum, gold, the ruthenium.The diameter dimension of this metallic particles is 1～10 nanometer.The loading of described noble metal catalyst is lower than 0.5mg/cm
2, and be uniformly distributed in the carbon nano tube surface of carbon nanotube long line.In the present embodiment, noble metal catalyst is a platinum.
Described carbon nanotube long line composite construction is fixed in the surface of proton exchange membrane 202 by the method for self viscosity, binding agent or hot pressing.When described anode electrode 204 or cathode electrode 206 comprise a plurality of carbon nanotube long line composite construction, a plurality of carbon nanotube long line composite constructions can be arranged in parallel or be arranged in a crossed manner in the surface of proton exchange membrane 202, and can not have gap setting or setting at interval between the carbon nanotube long line composite construction.When a plurality of carbon nanotube long line composite constructions intersect and be provided with at interval, form between the described carbon nanotube long line composite construction a plurality of evenly and the micropore of regular distribution, and this micropore size is less than 1 micron.
Be appreciated that, when described anode electrode 204 comprises the composite construction of at least one carbon nanotube long line and enzyme catalyst, described cathode electrode 206 structures are not limit, can comprise that a diffusion layer and a catalyst layer are arranged on this diffusion layer, and this catalyst layer is arranged between proton exchange membrane and the diffusion layer.Described diffusion layer can be a carbon fiber paper or carbon nanotube layer.This catalyst layer includes precious metal catalyst agent material and carrier thereof (be generally carbon granule, as: graphite, carbon black, carbon fiber or carbon nano-tube).When described cathode electrode 206 comprises the composite construction of at least one carbon nanotube long line and noble metal catalyst, described anode electrode 204 structures are not limit, can comprise that a diffusion layer and a catalyst layer are arranged on this diffusion layer, and this catalyst layer is arranged between proton exchange membrane and the diffusion layer.Described diffusion layer can be a carbon fiber paper or carbon nanotube layer.Described catalyst layer includes enzyme catalyst material and carrier thereof (be generally carbon granule, as: graphite, carbon black, carbon fiber or carbon nano-tube).In the present embodiment, preferably, described anode electrode 204 includes a plurality of carbon nanotube long line composite constructions with cathode electrode 206.That is, described anode electrode 204 comprises the composite construction of a plurality of carbon nanotube long line and enzyme catalyst.Described cathode electrode 206 comprises the composite construction of a plurality of carbon nanotube long line and noble metal catalyst.And the parallel no gap of a plurality of carbon nanotube long line composite constructions is arranged at the surface of proton exchange membrane 202.
The material of described proton exchange membrane 202 is perfluorinated sulfonic acid, polystyrolsulfon acid, polytrifluorostyrene sulfonic acid, phenolic resins sulfonic acid or hydrocarbon.In the present embodiment, proton exchange membrane 202 materials are perfluorinated sulfonic acid.
Described membrane electrode 200 has the following advantages: first, described anode electrode 204 all adopts the carbon nanotube long line composite construction with cathode electrode 206, so avoided the contact resistance between the diffusion layer and catalyst layer in the prior art, helped reacting the conduction of the electronics that necessary electronics and reaction generate.The second, carbon nanotube long line has great specific area, so, adopt this carbon nanotube long line can be effective and catalyst-loaded uniformly, make catalyst and bio-fuel or oxidant gas have bigger contact area, improved the utilance of catalyst.The 3rd, because the resistivity of carbon nano-tube itself will be lower than the resistivity of carbon fiber, so adopt the resistivity of electrode of this carbon nanotube long line composite construction low, can effectively conduct the electronics that necessary electronics of reaction and reaction generate, help to improve the reactivity of membrane electrode.The 4th, described anode electrode 204 all adopts the carbon nanotube long line composite construction with cathode electrode 206, and this carbon nanotube long line has collected current and effect catalyst-loaded and diffusion bio-fuel or oxidant gas simultaneously, and is simple in structure, easy to use.
See also Fig. 3, the technical program embodiment also further provides the biological fuel cell 20 of the above-mentioned membrane electrode 200 of an employing, and it comprises: 200, one anode rooms 214 of a membrane electrode, 208, one collector plate 210 of a baffler and an air feed and air extractor 212.
The structure of described membrane electrode 200 as previously mentioned.And described anode electrode 204 comprises that the parallel no gap with the composite construction of enzyme catalyst of a plurality of carbon nanotube long line is arranged at the surface of proton exchange membrane 202.Described cathode electrode 206 comprises that the parallel no gap with the composite construction of noble metal catalyst of a plurality of carbon nanotube long line is arranged at the surface of proton exchange membrane 202.
Described anode room 214 is arranged at anode electrode 204 1 sides of membrane electrode 200, is used for loading bio-fuel 216.In the present embodiment, bio-fuel 216 is a glucose solution.Described membrane electrode 200 separates bio-fuel 216 and oxidant gas, and anode electrode 204 is soaked in this bio-fuel 216, makes enzyme catalyst to contact with bio-fuel 216.
Described baffler 208 is arranged at the surface of cathode electrode 206 away from proton exchange membrane 202 respectively, and has one or more guiding gutter 218 on the surface of baffler 208 close cathode electrodes 206, is used to conduct oxidant gas and reaction product water.This baffler 208 adopts metal or conductive carbon material to make.
Described collector plate 210 adopts electric conducting material to make, and is arranged at the surface away from proton exchange membrane 202 of baffler 208, is used for collecting and the needed electronics of conduction reaction.Be appreciated that in the present embodiment, because the carbon nanotube long line structure has good electrical conductivity, can be used for collected current, so but this collector plate 210 is a choice structure.
Described air feed and air extractor 212 comprise air blast, pipeline, valve etc. (not indicating among the figure).Air blast links to each other with baffler 208 by pipeline, is used for providing oxidant gas to cathode electrode 206.In the present embodiment, oxidant gas is purity oxygen or oxygen containing air.
When above-mentioned biological fuel cell 20 was worked, at anode electrode 204 1 ends, following reaction took place in bio-fuel 216 (is example with glucose) under the catalytic action of enzyme catalyst: glucose → gluconic acid+2H
++ 2e.The proton that reaction generates passes proton exchange membrane 202 and arrives cathode electrode 206, and the electronics that reaction generates then enters external circuit.
At cathode electrode 206 1 ends, utilize its air feed and air extractor 212 to feed oxidant gas (is example with oxygen) to cathode electrode 206 by baffler 208.Oxygen diffusion is time the cathode electrode 206, and electronics then arrives cathode electrode 206 by external circuit.Under the noble metal catalyst effect, following reaction: 1/2O takes place in oxygen and proton and electronics
2+ 2H
++ 2e → H
2O.In this process, between anode electrode 204 and cathode electrode 206, can form certain electrical potential difference, when external circuit inserts a load 220, will form electric current.The water that reaction generates is then discharged biological fuel cell 20 by baffler 208.
In addition, those skilled in the art also can do other variations in spirit of the present invention, and certainly, the variation that these are done according to spirit of the present invention all should be included within the present invention's scope required for protection.
Claims (17)
1. membrane electrode, it comprises: a proton exchange membrane, one anode electrode and a cathode electrode, described anode electrode and cathode electrode are arranged at two facing surfaces of this proton exchange membrane respectively, it is characterized in that, described anode electrode comprises at least one carbon nanotube long line composite construction, and this carbon nanotube long line composite construction comprises that carbon nanotube long line and enzyme catalyst are distributed in this carbon nanotube long line.
2. membrane electrode as claimed in claim 1 is characterized in that, described anode electrode comprises that a plurality of carbon nanotube long line composite constructions are arranged in parallel or be arranged in a crossed manner in the surface of this proton exchange membrane.
3. membrane electrode as claimed in claim 1 is characterized in that, the diameter of described carbon nanotube long line composite construction is 1 micron～1 millimeter.
4. membrane electrode as claimed in claim 1 is characterized in that, described carbon nanotube long line composite construction comprises that a plurality of end to end carbon nano-tube are arranged of preferred orient.
5. membrane electrode as claimed in claim 4 is characterized in that, described carbon nano-tube is arranged along the axially parallel of carbon nanotube long line composite construction.
6. membrane electrode as claimed in claim 4 is characterized in that, described carbon nano-tube is arranged along the axial screw of carbon nanotube long line composite construction.
7. membrane electrode as claimed in claim 4 is characterized in that, combines closely by Van der Waals force between the adjacent carbon nano-tube in the described carbon nanotube long line composite construction.
8. membrane electrode as claimed in claim 4 is characterized in that, the length of described carbon nano-tube is 200～900 microns, and diameter is less than 50 nanometers.
9. membrane electrode as claimed in claim 4 is characterized in that described carbon nano tube surface comprises a plurality of carboxyls or hydroxyl, and described enzyme catalyst evenly is adsorbed in carbon nano tube surface by this carboxyl or hydroxyl.
10. membrane electrode as claimed in claim 1 is characterized in that described enzyme catalyst comprises oxidizing ferment or dehydrogenase.
11. membrane electrode as claimed in claim 1 is characterized in that, described cathode electrode comprises at least one carbon nanotube long line composite construction, and this carbon nanotube long line composite construction comprises that carbon nanotube long line and catalyst distribution are in this carbon nanotube long line.
12. membrane electrode as claimed in claim 11 is characterized in that, described catalyst is a noble metal granule, and its material is the mixture of a kind of or its combination in any in platinum, gold or the ruthenium, and this noble metal granule is uniformly distributed in this carbon nanotube long line.
13. membrane electrode as claimed in claim 1 is characterized in that, described cathode electrode comprises a diffusion layer and the catalyst layer that is formed at this diffusion layer surface, and this catalyst layer is arranged between proton exchange membrane and the diffusion layer.
14. membrane electrode as claimed in claim 13 is characterized in that, described diffusion layer is carbon nanotube layer or carbon fiber paper.
15. a biological fuel cell, it comprises: a proton exchange membrane; One anode electrode and a cathode electrode, described anode electrode and cathode electrode are separately positioned on two facing surfaces of this proton exchange membrane; One is equipped with the room of bio-fuel, and anode electrode is soaked in this bio-fuel; One baffler is arranged at the surface of cathode electrode away from proton exchange membrane; And air feed and air extractor are connected with this baffler, it is characterized in that, described anode electrode comprises at least one carbon nanotube long line composite construction, and this carbon nanotube long line composite construction comprises that carbon nanotube long line and enzyme catalyst are distributed in this carbon nanotube long line.
16. biological fuel cell as claimed in claim 15, it is characterized in that, described cathode electrode comprises at least one carbon nanotube long line composite construction, and this carbon nanotube long line composite construction comprises that carbon nanotube long line and catalyst distribution are in this carbon nanotube long line.
17. biological fuel cell as claimed in claim 16 is characterized in that, described catalyst is a noble metal granule, and its material is the mixture of a kind of or its combination in any in platinum, gold or the ruthenium, and this noble metal granule is uniformly distributed in this carbon nanotube long line.
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| Application Number | Priority Date | Filing Date | Title |
|---|---|---|---|
| CN2008101425234A CN101635361B (en) | 2008-07-25 | 2008-07-25 | Membrane electrode and biofuel cell adopting same |
| EP08253560A EP2056383A1 (en) | 2007-11-02 | 2008-10-30 | Membrane electrode assembly and method for making the same |
| US12/384,964 US9077042B2 (en) | 2008-07-25 | 2009-04-09 | Membrane electrode assembly and biofuel cell using the same |
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| CN2008101425234A CN101635361B (en) | 2008-07-25 | 2008-07-25 | Membrane electrode and biofuel cell adopting same |
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Cited By (4)
| Publication number | Priority date | Publication date | Assignee | Title |
|---|---|---|---|---|
| CN102724617A (en) * | 2011-03-29 | 2012-10-10 | 清华大学 | Thermoacoustic device and electronic device |
| CN102959784A (en) * | 2010-06-25 | 2013-03-06 | 索尼公司 | Biofuel cell |
| CN102956911A (en) * | 2011-08-30 | 2013-03-06 | 清华大学 | Biological fuel cell |
| CN113013415A (en) * | 2021-03-02 | 2021-06-22 | 西安工业大学 | High-power stable sodium ion battery cathode material and preparation method thereof |
Family Cites Families (1)
| Publication number | Priority date | Publication date | Assignee | Title |
|---|---|---|---|---|
| CN1912200A (en) * | 2006-08-15 | 2007-02-14 | 浙江大学 | Nano-fibre of carbon nanotube and its method of preparation and oxidation reduction fix |
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2008
- 2008-07-25 CN CN2008101425234A patent/CN101635361B/en active Active
Cited By (6)
| Publication number | Priority date | Publication date | Assignee | Title |
|---|---|---|---|---|
| CN102959784A (en) * | 2010-06-25 | 2013-03-06 | 索尼公司 | Biofuel cell |
| CN102724617A (en) * | 2011-03-29 | 2012-10-10 | 清华大学 | Thermoacoustic device and electronic device |
| CN102724617B (en) * | 2011-03-29 | 2015-06-03 | 清华大学 | Thermoacoustic device and electronic device |
| CN102956911A (en) * | 2011-08-30 | 2013-03-06 | 清华大学 | Biological fuel cell |
| CN102956911B (en) * | 2011-08-30 | 2016-03-30 | 清华大学 | Biological fuel cell |
| CN113013415A (en) * | 2021-03-02 | 2021-06-22 | 西安工业大学 | High-power stable sodium ion battery cathode material and preparation method thereof |
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