CN111916762A - Diffusion layer of proton exchange membrane fuel cell and preparation method thereof - Google Patents
Diffusion layer of proton exchange membrane fuel cell and preparation method thereof Download PDFInfo
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- CN111916762A CN111916762A CN202010607715.9A CN202010607715A CN111916762A CN 111916762 A CN111916762 A CN 111916762A CN 202010607715 A CN202010607715 A CN 202010607715A CN 111916762 A CN111916762 A CN 111916762A
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- 239000000446 fuel Substances 0.000 title claims abstract description 37
- 238000009792 diffusion process Methods 0.000 title claims abstract description 34
- 239000012528 membrane Substances 0.000 title claims abstract description 32
- 238000002360 preparation method Methods 0.000 title claims abstract description 12
- OKTJSMMVPCPJKN-UHFFFAOYSA-N Carbon Chemical compound [C] OKTJSMMVPCPJKN-UHFFFAOYSA-N 0.000 claims abstract description 89
- 229910002804 graphite Inorganic materials 0.000 claims abstract description 37
- 239000010439 graphite Substances 0.000 claims abstract description 37
- 239000004810 polytetrafluoroethylene Substances 0.000 claims abstract description 21
- 229920001343 polytetrafluoroethylene Polymers 0.000 claims abstract description 21
- 239000003575 carbonaceous material Substances 0.000 claims abstract description 19
- 238000000034 method Methods 0.000 claims abstract description 19
- 229910021389 graphene Inorganic materials 0.000 claims abstract description 16
- 239000000463 material Substances 0.000 claims abstract description 8
- 238000005507 spraying Methods 0.000 claims abstract description 8
- 230000002209 hydrophobic effect Effects 0.000 claims abstract description 5
- 230000004913 activation Effects 0.000 claims abstract description 3
- 239000006255 coating slurry Substances 0.000 claims abstract description 3
- 229920004890 Triton X-100 Polymers 0.000 claims description 14
- 239000013504 Triton X-100 Substances 0.000 claims description 14
- 238000010438 heat treatment Methods 0.000 claims description 8
- 238000011068 loading method Methods 0.000 claims description 8
- 239000002002 slurry Substances 0.000 claims description 6
- 239000002270 dispersing agent Substances 0.000 claims description 4
- 230000008569 process Effects 0.000 claims description 4
- 229910052799 carbon Inorganic materials 0.000 claims description 3
- 239000002131 composite material Substances 0.000 claims description 3
- CREMABGTGYGIQB-UHFFFAOYSA-N carbon carbon Chemical compound C.C CREMABGTGYGIQB-UHFFFAOYSA-N 0.000 claims description 2
- 239000011203 carbon fibre reinforced carbon Substances 0.000 claims description 2
- 238000005260 corrosion Methods 0.000 abstract description 7
- 230000007797 corrosion Effects 0.000 abstract description 7
- 239000010410 layer Substances 0.000 description 34
- 238000007792 addition Methods 0.000 description 9
- 239000000839 emulsion Substances 0.000 description 5
- 238000002156 mixing Methods 0.000 description 5
- 238000003756 stirring Methods 0.000 description 5
- 238000005303 weighing Methods 0.000 description 5
- 230000009286 beneficial effect Effects 0.000 description 3
- 239000003054 catalyst Substances 0.000 description 3
- 241001089723 Metaphycus omega Species 0.000 description 2
- 230000008901 benefit Effects 0.000 description 2
- 230000008859 change Effects 0.000 description 2
- 238000005530 etching Methods 0.000 description 2
- 238000011031 large-scale manufacturing process Methods 0.000 description 2
- 239000002994 raw material Substances 0.000 description 2
- 230000005540 biological transmission Effects 0.000 description 1
- 239000006227 byproduct Substances 0.000 description 1
- 150000001721 carbon Chemical group 0.000 description 1
- 238000002485 combustion reaction Methods 0.000 description 1
- 230000000052 comparative effect Effects 0.000 description 1
- 150000001875 compounds Chemical class 0.000 description 1
- 230000000694 effects Effects 0.000 description 1
- 239000006260 foam Substances 0.000 description 1
- 230000006872 improvement Effects 0.000 description 1
- 238000004519 manufacturing process Methods 0.000 description 1
- 239000002086 nanomaterial Substances 0.000 description 1
- 230000010287 polarization Effects 0.000 description 1
- 239000011148 porous material Substances 0.000 description 1
- 238000001878 scanning electron micrograph Methods 0.000 description 1
- 239000002356 single layer Substances 0.000 description 1
- 238000009736 wetting Methods 0.000 description 1
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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
- H01M4/8803—Supports for the deposition of the catalytic active composition
- H01M4/8807—Gas diffusion layers
-
- 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
-
- 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
-
- 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)
- Chemical Kinetics & Catalysis (AREA)
- Electrochemistry (AREA)
- General Chemical & Material Sciences (AREA)
- Engineering & Computer Science (AREA)
- Manufacturing & Machinery (AREA)
- Composite Materials (AREA)
- Carbon And Carbon Compounds (AREA)
- Fuel Cell (AREA)
- Inert Electrodes (AREA)
Abstract
The invention discloses a diffusion layer of a proton exchange membrane fuel cell and a preparation method thereof. The preparation method of the proton exchange membrane fuel cell diffusion layer comprises the steps of spraying or blade coating slurry containing graphene sheet-based carbon materials, carbon powder and PTFE on the surface of a support material subjected to hydrophobic treatment, and carrying out activation treatment to obtain the proton exchange membrane fuel cell diffusion layer. According to the method, a proper amount of graphite sheet base carbon material is added into the microporous layer prepared by the traditional method, so that the conductivity and the corrosion resistance of the diffusion layer of the proton exchange membrane fuel cell are obviously improved.
Description
Technical Field
The invention relates to a proton exchange membrane fuel cell diffusion layer, in particular to a graphene sheet-based carbon material modified proton exchange membrane fuel cell diffusion layer (GDL) and a preparation method thereof, and belongs to the technical field of preparation of Proton Exchange Membranes of Fuel Cells (PEMFC) electrodes.
Background
Proton exchange membrane fuel cells have entered the early stages of commercial application, but still have short service life and low practical output efficiency compared to internal combustion engines. Therefore, it becomes key to improve the comprehensive performance of each material in the battery. The microporous layer prepared by the traditional method has relatively low conductivity, durability and reliability, which restricts the large-scale commercial application of the fuel cell to a certain extent. Therefore, a great deal of improvement in the microporous layer is required to meet practical applications under various conditions. As a substitute for the traditional nano material, graphene is a two-dimensional honeycomb-shaped arranged carbon atom single-layer lattice and has good conductivityElectrical and thermal conductivity. Leeuwner et al reported a geometric area of 5cm at the electrode2The addition of commercial graphene foam to the small stack of (a) is beneficial to reducing contact resistance, improving mechanical integrity between the gas diffusion layer and the catalyst layer, and performance especially at low current densities. However, the byproduct graphite flakes remaining during the preparation of graphene are of little concern.
Disclosure of Invention
Aiming at the problems that the diffusion layer (microporous layer) prepared by the traditional method has relatively low conductivity, durability and reliability, thereby restricting the large-scale commercial application of the fuel cell to a certain extent and the like, the invention aims to provide the gas diffusion layer of the proton exchange membrane fuel cell, which has excellent conductivity and durability and can improve the performance of the fuel cell.
The second purpose of the present invention is to provide a method for improving the conductivity and durability of the gas diffusion layer of the existing proton exchange membrane fuel cell by using a graphite sheet-based carbon material, wherein the graphite sheet-based carbon material is added in the traditional process for preparing the gas diffusion layer of the proton exchange membrane fuel cell, and the method has the advantages of simple operation, low raw material cost and benefit for large-scale production.
In order to achieve the technical purpose, the invention provides a preparation method of a diffusion layer of a proton exchange membrane fuel cell, which comprises the steps of spraying or blade coating slurry containing graphene sheet-based carbon materials, carbon powder and PTFE on the surface of a support material subjected to hydrophobic treatment, and carrying out activation treatment to obtain the proton exchange membrane fuel cell diffusion layer.
Preferably, the content of the graphene sheet-based carbon material in the slurry is greater than 0% and less than or equal to 20% by mass. The content of the graphene sheet-based carbon material in the slurry is preferably 5 to 10 percent by mass.
The invention introduces the graphite sheet base carbon material into the micro-pore layer of the proton exchange membrane fuel cell, and the electric conductivity and the corrosion resistance of the proton exchange membrane fuel cell are obviously improved. The graphene sheets are added into the diffusion layer, so that the graphene sheets are easily horizontally stacked to form a smooth layer, and the dense smooth layer exists in the catalyst layer and the gas micro-layerCan improve catalyst utilization ratio between the porose layer, reduce interfacial resistance, promote the heat transfer, and along with graphite flake base carbon material addition increases, the inside conductive network of micropore layer increases, and the conductivity increases. However, if the amount of graphite flake-based carbon material added is further increased, the surface becomes rougher and rougher, resulting in poor contact with the plate interface. So that when the amount of the graphite-flake-based carbon material added was 10 wt%, the sheet resistivity was 3.5 m.OMEGA.cm and the bulk resistance was 6.4 m.OMEGA.cm2Lowest in all samples, and lower in sheet resistivity and bulk resistance than the SIGRACET 28BC series gas diffusion layers. After the corrosion of the 1.4V accelerated voltage, the corrosion of the traditional microporous layer is mainly concentrated at the crack, and the surface has no obvious change. And the crack of the microporous layer of the graphite sheet base is protected by the graphite sheet, the corrosion is mainly concentrated on the rough surface, and the corrosion resistance is the best when the addition amount of the graphite sheet is 5 wt%. The self-etching potential is 0.2V, and the self-etching current density is 0.0574 muA cm-2The corrosion current density after the potentiostatic test tends to be stable is 4.32 muA cm-2。
In a preferable scheme, the mass ratio of the carbon powder to the PTFE is 1-10: 1, and a more preferable mass ratio is 3-5: 1.
Preferably, the slurry contains a Triton X-100 dispersing agent, and the mass ratio of the Triton X-100 dispersing agent to carbon powder is 0.01-10000: 1. The preferable mass ratio is 0.1 to 100: 1.
Preferably, the supporting material is carbon paper.
Preferably, the graphite sheet-based carbon material comprises at least one of graphite sheets, industrial graphene, functionalized graphite sheets and carbon-carbon composite materials.
Preferably, the loading amount of the carbon powder on the surface of the support material subjected to hydrophobic treatment is 0.1-5 mg/cm2. The preferable load is 0.1-5 mg/cm2，1～3mg/cm2。
Preferably, the heat treatment process is as follows: and preserving the heat for 1-8 h at 100-600 ℃ in an inert atmosphere. The preferred heat treatment process is: and preserving the heat for 2-3 hours at the temperature of 300-400 ℃ in an inert atmosphere.
The invention provides a proton exchange membrane fuel cell diffusion layer, which is obtained by the preparation method.
Compared with the prior art, the technical scheme of the invention has the following beneficial technical effects:
according to the technical scheme, the graphite sheet carbon-based material is introduced into the diffusion layer of the proton exchange membrane fuel cell, so that the conductivity and durability of the gas diffusion layer of the proton exchange membrane fuel cell can be improved simultaneously, and the performance of the fuel cell is improved.
The diffusion layer of the proton exchange membrane fuel cell is added with the graphite flake-based carbon material in the traditional process of preparing the gas diffusion layer of the proton exchange membrane fuel cell, has simple operation and low cost of raw materials, and is beneficial to large-scale production.
Drawings
FIG. 1 is a graph of wetting angle changes for different graphite flake loadings of a microporous layer;
FIG. 2 is a graph of the change in porosity and gas transmission of microporous layers for different graphite sheet additions;
FIG. 3 is a plan scanning electron micrograph: (a) graphite flake, (b) MPL-G0, (c) MPL-G5, (d) MPL-G10, (e) MPL-G15, and (f) MPL-G20.
Detailed Description
The following examples illustrate the preparation of a graphite sheet-based microporous layer for a gas diffusion layer of a fuel cell. The compounds in the following examples can be prepared directly according to the existing methods, but of course, in other examples, they can be directly commercially available, and are not limited thereto.
Example 1
Weighing a certain amount of carbon powder, PTFE and graphite flakes, adding the carbon powder, the PTFE and the graphite flakes into 20 wt% of Triton X-100 aqueous emulsion, dispersing, ultrasonically stirring for 2 hours, and uniformly mixing, wherein the mass ratio of the carbon powder to the PTFE is 4:1, the mass ratio of the carbon powder to the Triton X-100 is 1:2, the addition amount of the graphite flakes is 0 wt%, and the label is MPL-G0. The loading amount of the carbon powder is strictly controlled to be 1.5mg/cm by a spraying method2Nearby. And (3) placing the prepared sample in a tube furnace for heat treatment, and keeping the temperature for 2h at 350 ℃ in an Ar atmosphere.
Example 2
Weighing a certain amount of carbon powder, PTFE and graphite flakes, adding the carbon powder, the PTFE and the graphite flakes into 20 wt% of Triton X-100 aqueous emulsion, dispersing, ultrasonically stirring for 2 hours, and uniformly mixing, wherein the mass ratio of the carbon powder to the PTFE is 4:1, the mass ratio of the carbon powder to the Triton X-100 is 1:2, the addition amount of the graphite flakes is 5 wt%, and the label is MPL-G5. The loading amount of the carbon powder is strictly controlled to be 1.5mg/cm by a spraying method2Nearby. And (3) placing the prepared sample in a tube furnace for heat treatment, and keeping the temperature for 2h at 350 ℃ in an Ar atmosphere.
Example 3
Weighing a certain amount of carbon powder, PTFE and graphite flakes, adding the carbon powder, the PTFE and the graphite flakes into 20 wt% of Triton X-100 aqueous emulsion, dispersing, ultrasonically stirring for 2 hours, and uniformly mixing, wherein the mass ratio of the carbon powder to the PTFE is 4:1, the mass ratio of the carbon powder to the Triton X-100 is 1:2, the addition amount of the graphite flakes is 10 wt%, and the label is MPL-G10. The loading amount of the carbon powder is strictly controlled to be 1.5mg/cm by a spraying method2Nearby. And (3) placing the prepared sample in a tube furnace for heat treatment, and keeping the temperature for 2h at 350 ℃ in an Ar atmosphere.
Example 4
Weighing a certain amount of carbon powder, PTFE and graphite flakes, adding the carbon powder, the PTFE and the graphite flakes into 20 wt% of Triton X-100 aqueous emulsion, dispersing, ultrasonically stirring for 2 hours, and uniformly mixing, wherein the mass ratio of the carbon powder to the PTFE is 4:1, the mass ratio of the carbon powder to the Triton X-100 is 1:2, the addition amount of the graphite flakes is 15 wt%, and the label is MPL-G15. The loading amount of the carbon powder is strictly controlled to be 1.5mg/cm by a spraying method2Nearby. And (3) placing the prepared sample in a tube furnace for heat treatment, and keeping the temperature for 2h at 350 ℃ in an Ar atmosphere.
Example 5
Weighing a certain amount of carbon powder, PTFE and graphite flakes, adding the carbon powder, the PTFE and the graphite flakes into 20 wt% of Triton X-100 aqueous emulsion, dispersing, ultrasonically stirring for 2 hours, and uniformly mixing, wherein the mass ratio of the carbon powder to the PTFE is 4:1, the mass ratio of the carbon powder to the Triton X-100 is 1:2, the addition amount of the graphite flakes is 20 wt%, and the label is MPL-G20. The loading amount of the carbon powder is strictly controlled to be 1.5mg/cm by a spraying method2Nearby. And (3) placing the prepared sample in a tube furnace for heat treatment, and keeping the temperature for 2h at 350 ℃ in an Ar atmosphere.
The following table is a comparative result tested according to the diffusion layer prepared:
TABLE 1 sheet resistivity and bulk resistance
TABLE 2 polarization curves and potentiostatic curves electrochemical parameters
Claims (10)
1. A preparation method of a diffusion layer of a proton exchange membrane fuel cell is characterized in that: and spraying or blade-coating slurry containing the graphene sheet-based carbon material, carbon powder and PTFE on the surface of the support material subjected to hydrophobic treatment, and performing activation treatment to obtain the graphene/PTFE composite material.
2. The method of claim 1, wherein the diffusion layer of the proton exchange membrane fuel cell comprises: the graphene sheet-based carbon material accounts for more than 0% and less than or equal to 20% of the slurry by mass.
3. The method of claim 2, wherein the diffusion layer of the proton exchange membrane fuel cell comprises: the graphene sheet-based carbon material accounts for 5-10% of the slurry by mass percent.
4. The method of claim 1, wherein the diffusion layer of the proton exchange membrane fuel cell comprises: the mass ratio of the carbon powder to the PTFE is 10-1: 1.
5. The method of claim 1, wherein the diffusion layer of the proton exchange membrane fuel cell comprises: the slurry contains a Triton X-100 dispersing agent, and the mass ratio of the Triton X-100 dispersing agent to carbon powder is 0.01-10000: 1.
6. The method of claim 1, wherein the diffusion layer of the proton exchange membrane fuel cell comprises: the supporting material is carbon paper.
7. The method of claim 1, wherein the diffusion layer of the proton exchange membrane fuel cell comprises: the graphite sheet-based carbon material comprises at least one of graphite sheets, industrial graphene, functionalized graphite sheets and carbon-carbon composite materials.
8. The method of claim 1, wherein the diffusion layer of the proton exchange membrane fuel cell comprises: the loading capacity of the carbon powder on the surface of the support material subjected to hydrophobic treatment is 0.1-5 mg/cm2。
9. The method of claim 1, wherein the diffusion layer of the proton exchange membrane fuel cell comprises: the heat treatment process comprises the following steps: and preserving the heat for 1-8 h at 100-600 ℃ in an inert atmosphere.
10. A diffusion layer of a proton exchange membrane fuel cell, comprising: the preparation method of any one of claims 1 to 9.
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| CN202010607715.9A CN111916762A (en) | 2020-06-30 | 2020-06-30 | Diffusion layer of proton exchange membrane fuel cell and preparation method thereof |
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Cited By (2)
| Publication number | Priority date | Publication date | Assignee | Title |
|---|---|---|---|---|
| CN112928285A (en) * | 2021-03-10 | 2021-06-08 | 上海电气集团股份有限公司 | Gas diffusion layer, preparation method thereof, fuel cell anode and fuel cell |
| CN113948715A (en) * | 2021-10-14 | 2022-01-18 | 一汽解放汽车有限公司 | Fuel cell gas diffusion layer and preparation method and application thereof |
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2020
- 2020-06-30 CN CN202010607715.9A patent/CN111916762A/en active Pending
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Non-Patent Citations (1)
| Title |
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Cited By (2)
| Publication number | Priority date | Publication date | Assignee | Title |
|---|---|---|---|---|
| CN112928285A (en) * | 2021-03-10 | 2021-06-08 | 上海电气集团股份有限公司 | Gas diffusion layer, preparation method thereof, fuel cell anode and fuel cell |
| CN113948715A (en) * | 2021-10-14 | 2022-01-18 | 一汽解放汽车有限公司 | Fuel cell gas diffusion layer and preparation method and application thereof |
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Application publication date: 20201110 |