CN111082067B - Fuel cell gas diffusion layer and preparation method thereof - Google Patents

Fuel cell gas diffusion layer and preparation method thereof Download PDF

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CN111082067B
CN111082067B CN201911101931.XA CN201911101931A CN111082067B CN 111082067 B CN111082067 B CN 111082067B CN 201911101931 A CN201911101931 A CN 201911101931A CN 111082067 B CN111082067 B CN 111082067B
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gas diffusion
diffusion layer
fuel cell
base layer
agent content
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CN111082067A (en
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倪蕾蕾
季文姣
杨敏
朱星烨
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Shanghai Electric Group Corp
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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
    • H01M4/8803—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
    • H01M8/00—Fuel cells; Manufacture thereof
    • H01M8/10—Fuel cells with solid electrolytes
    • H01M8/1004—Fuel cells with solid electrolytes characterised by membrane-electrode assemblies [MEA]
    • 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

Abstract

The invention discloses a fuel cell gas diffusion layer, which aims to solve the technical problem of limited water vapor transmission performance of a membrane electrode in the prior art. By carrying out hydrophobic treatment of different degrees on different areas of a substrate layer in the gas diffusion layer, correspondingly customized water-gas transmission management can be carried out on different areas of the membrane electrode, the running condition of the membrane electrode is improved, the discharge voltage of the membrane electrode is improved, and the discharge efficiency is improved.

Description

Fuel cell gas diffusion layer and preparation method thereof
Technical Field
The present invention relates to a gas diffusion layer for a fuel cell and a method for preparing the same.
Background
A proton exchange membrane fuel cell is a primary cell that converts the chemical energy of hydrogen and oxygen in the air into electrical energy and heat energy through an electrochemical reaction. The monolithic cell mainly comprises an anode gas diffusion layer, a cathode gas diffusion layer, an anode catalyst layer, a cathode catalyst layer and a proton exchange membrane. Respectively preparing an anode catalyst layer and a cathode catalyst layer on the surfaces of two sides of a proton exchange membrane to form a three-in-one membrane electrode, namely CCM (catalyst coated membrane); then, the anode gas diffusion layer covers the outer side of the anode catalyst layer, and the cathode gas diffusion layer covers the outer side of the cathode catalyst layer, so that a five-in-one membrane electrode is formed. Wherein the gas diffusion layer has the functions of providing certain mechanical support for single cells, conducting electrons, conducting heat, uniformly dispersing and effectively transmitting reaction gas and discharging water which is the final product of electrochemical reaction.
The mainstream gas diffusion layer is mainly composed of two parts, i.e., a substrate layer and a microporous layer, and the microporous layer is usually prepared on one side of the substrate layer to form the gas diffusion layer. And covering the surface of the cathode/anode gas diffusion layer with the microporous layer on the corresponding surface of the cathode/anode catalytic layer respectively to form the membrane electrode.
In general, the substrate layer and the microporous layer are subjected to hydrophobic treatment to improve the water vapor transmission performance of the gas diffusion layer, so as to realize a high-efficiency and reasonable water vapor transmission state, thereby realizing high-power and high-efficiency discharge and applicable service life of the proton exchange membrane fuel cell.
In a proton exchange membrane fuel cell, the working environment of a membrane electrode of the fuel cell is relatively complex, and particularly for a membrane electrode with a large active area in a galvanic pile, the external gas flow states of different regions of the same cell may be different, and different gas diffusion layer properties are required to optimize the water-gas mass transfer of the region so as to strive to achieve the optimal discharge state. Generally, the gas flow rate in the area close to the gas inlet in the stack is high, the gas supply stoichiometry in the area is high, and the high gas flow rate can cause dehydration of the perfluorinated sulfonic acid resin in the proton exchange membrane and the catalytic layer in the area, so that the internal resistance of the cell in the area is increased, the discharge current density is reduced, and the service life of the cell is influenced; in general, in the stack, near the gas outlet region, the flow rate of the consumed gas is reduced, and liquid water is accumulated particularly at the cathode, so that the cathode catalytic layer is flooded, the permeability of the air of the reactant gas is reduced, and the discharge current density in the region is reduced; or water accumulation occurs at the anode of the area, the permeability of the reaction gas hydrogen is reduced, the discharge current density of the area is reduced, and in severe cases, abnormal high potential is caused to cause the burning of relevant parts of the galvanic pile.
In the existing gas diffusion layer of the commercial traditional fuel cell, different hydrophobic treatments are carried out on different areas of the diffusion layer used by the membrane electrode on the substrate layer and the microporous layer in the plane direction, and reasonable water and gas transmission of the membrane electrode is difficult to realize in a galvanic pile, so that the performance and the service life of the membrane electrode are improved.
In view of the above, it is an urgent problem in the art to overcome the above-mentioned drawbacks of the prior art.
Disclosure of Invention
The invention provides a fuel cell gas diffusion layer with base layers with different hydrophobicity degrees and a preparation method thereof, aiming at overcoming the technical problem that the water-gas transmission performance of a membrane electrode is limited in the prior art.
In order to achieve the above object, the present invention discloses a fuel cell gas diffusion layer comprising a substrate layer having a gas diffusion layer surface on one side, and a microporous layer adjacent to the other side of the substrate layer, the substrate layer comprising a first portion having a first hydrophobic agent content and a second portion having a second hydrophobic agent content.
Further, the first portion and the second portion are symmetrically disposed.
Further, the first portion occupies half of the area of the base layer, and the second portion occupies the other half of the area of the base layer.
Further, the first portion comprises a plurality of first sections; the second portion comprises a plurality of second sections; the at least one second section is sandwiched between the two first sections.
Further, the hydrophobic agent is polytetrafluoroethylene.
Further, the first hydrophobizing agent content Δ a and the second hydrophobizing agent content Δ b range in value from 0.5% to 20%, and Δ a > Δ b.
Further, the first portion is located in the gas diffusion layer near a gas inlet through which gas moves toward the gas diffusion layer; the second portion is in the gas diffusion layer at a location proximate to a gas outlet through which gas moves away from the gas diffusion layer.
The invention also provides a method of preparing a fuel cell gas diffusion layer as described in any one of the above, comprising the steps of:
step 1: taking a piece of dry base layer material which is not subjected to hydrophobic treatment, and dividing the dry base layer material into a part A and a part B in the plane direction;
step 2: placing the base layer material at an inlet of a vacuum box, and opening the vacuum box;
and step 3: covering the upper surface of the part B with a film, and coating an aqueous solution with the hydrophobic agent content of m1 on the upper surface of the part A;
and 4, step 4: covering the upper surface of the area A with a film, and coating the upper surface of the part B with an aqueous solution with the content of a hydrophobic agent m 2;
and 5: coating microporous layer slurry on one side of the base layer material subjected to the hydrophobic treatment;
step 6: and (5) sintering the substrate material coated in the step 5 at a high temperature to form the fuel cell gas diffusion layer.
Further, the step 3 further comprises:
step 31: covering the upper surface of the part B with a film, coating an aqueous solution with the content of a hydrophobic agent of m1 on the upper surface of the part A, taking off the film on the upper surface of the part B after 3-8 seconds, and turning over the upper surface and the lower surface of the base layer material;
step 32: repeating the step 31 until the water solution with the water repellent agent content of m1 is sprayed in a proper dosage;
step 33: the upper and lower surfaces of the base layer material were inverted every 3-8 seconds until the base layer material was at the inlet of the vacuum box for 13-20 minutes.
Further, the step 4 further includes:
step 41: covering the upper surface of the area A with a film, coating the upper surface of the part B with an aqueous solution with the content of a hydrophobic agent of m2, taking off the film on the upper surface of the part A after 3-8 seconds, and turning over the upper surface and the lower surface of the base layer material;
step 42: repeating the step 41 until the water solution with the water repellent agent content of m2 is sprayed by proper dosage;
step 43: the upper and lower surfaces of the base layer material were inverted every 3-8 seconds until the base layer material was at the inlet of the vacuum box for 13-20 minutes.
Further, the base layer material may be any one of carbon paper, carbon cloth, and carbon felt.
The technical scheme provided by the invention has the advantages that: by utilizing the effect of the internal and external pressure difference at the inlet of the vacuum box, the hydrophobic agent rapidly permeates into the substrate layer from one side of the substrate layer to the other side, and carries out hydrophobic treatment with different degrees on different areas of the substrate layer in the gas diffusion layer, so that corresponding customized water-gas transmission management can be carried out on different areas of the membrane electrode, the running condition of the membrane electrode is improved, the discharge voltage of the membrane electrode is improved, and the discharge efficiency is improved. The technical scheme provided by the invention can be realized only by changing the content of the hydrophobing agent, and has the advantages of low cost and relatively simple process.
Drawings
The accompanying drawings, which are incorporated in and constitute a part of this specification, illustrate embodiments of the apparatus and method consistent with the present invention and, together with the detailed description, serve to explain the advantages and principles consistent with the invention. In the drawings:
figure 1 is a schematic cross-sectional view of a fuel cell gas diffusion layer designed according to one embodiment of this invention;
figure 2 is a schematic cross-sectional view of a fuel cell gas diffusion layer designed according to another embodiment of this invention;
fig. 3 is a graph comparing the membrane electrode polarization curves I-V of a fuel cell using gas diffusion layers prepared according to an embodiment of the present invention and a conventional fuel cell.
Description of the reference numerals: 1. a base layer; 2. a first portion; 3. a second portion; 4. a microporous layer; 5. a first section; 6. a second section.
Detailed Description
Specific embodiments of the present invention are described in detail below with reference to the accompanying drawings. However, the present invention is not limited to the embodiments described below. In addition, the technical features involved in the respective embodiments of the present invention described below may be combined with each other as long as they do not conflict with each other, and the technical idea of the present invention may be implemented in combination with other known techniques or other techniques identical to those known techniques.
Implementation mode one
Fig. 1 discloses a schematic cross-sectional view of a fuel cell gas diffusion layer of a design of this embodiment, comprising a substrate layer 1 having a gas diffusion layer surface on one side, and a microporous layer 4 adjacent to the other side of the substrate layer 1, the substrate layer 1 comprising a first portion 2 having a first hydrophobizing agent content and a second portion 3 having a second hydrophobizing agent content. In the embodiment shown in fig. 1, the first portion 2 and the second portion 3 are symmetrically arranged, each occupying half the area of the substrate layer 1. In practical implementation, the area ratio of the first part 2 and the second part 3 can be adjusted according to the specific situation of different fuel cells.
Second embodiment
Figure 2 discloses a schematic cross-sectional view of a fuel cell gas diffusion layer of a second design of this embodiment, in which the first part 2 and the second part 3 are not separate one integral area, the first part 2 comprising a plurality of first segments 5, the second part 3 comprising a plurality of second segments 6, at least one second segment 6 being sandwiched between two first segments 5.
In an embodiment, the hydrophobizing agent is Polytetrafluoroethylene (PTFE), the first hydrophobizing agent content Δ a and the second hydrophobizing agent content Δ b have a value in the range of 0.5% to 20%, and Δ a > Δ b.
The first part 2 is in the gas diffusion layer at a position close to a gas inlet through which gas moves towards the gas diffusion layer; the second part 3 is in the gas diffusion layer at a position close to the gas outlet through which the gas moves away from the gas diffusion layer. However, due to the complexity of the fuel cell membrane electrode itself, the first part 2 can also be located close to the gas outlet in the membrane electrode and the second part 3 close to the gas inlet in the membrane electrode.
Third embodiment
This example provides a method for preparing a gas diffusion layer of a fuel cell according to the first embodiment, taking a carbon paper 20cm x 20cm without hydrophobic treatment of dongli TGP-H-060, equally dividing the carbon paper into two regions along a plane direction, which are respectively marked as part a and part B, covering the upper side of the part B with a PI film, contacting the lower surface of the carbon paper with a vacuum microporous aluminum plate to maintain a pressure of-20 Pa, taking 1.5mL of a water repellent aqueous solution with a PTFE content of 10% with a spray gun, uniformly spraying the upper surface of the part a, turning over the upper surface and the lower surface of the carbon paper every 5 seconds, and still spraying the part a until the spraying of the water repellent is finished, and then circulating the turning process for 15 minutes, wherein the surface on the upper side of the part B is covered with the PI film; after 15 minutes of overturning spraying is finished, drying and placing for 6 hours at room temperature, and weighing to obtain a part A with a PTFE content value of 8%; then, the upper surface of part A was covered with a PI film, and part B was subjected to the same procedure as that carried out for part A above by taking 1.5mL of an aqueous solution of a hydrophobizing agent having a PTFE content of 5% by means of a spray gun, and weighed to obtain a PTFE content value of part B of 4.3%. And (3) coating the microporous layer slurry on one side surface of the carbon paper, and heating the carbon paper in the air at 350 ℃ for 80 seconds in a hot stage to finish the preparation of the fuel cell gas diffusion layer.
The carbon paper in the scheme can also be carbon cloth or carbon felt, which are both base layer materials of gas diffusion layers commonly used in proton exchange membrane fuel cells.
The PI film, namely the polyimide film, used in the scheme has the purpose of performing partial shielding effect when hydrophobic treatment is performed and hydrophobic slurry is sprayed, and other films with similar effect, such as preservative films, PET films, PEN films and the like, can be used in the scheme.
Comparative example
Experimental data now verify the difference between the performance of the fuel cell of the gas diffusion layer prepared according to the embodiment of the present invention and the performance of the membrane electrode of the existing conventional fuel cell.
Preparing MEA-1: the gas diffusion layer prepared in example 3 above was used as a membrane electrode cathode gas diffusion layer, in which the part a with a base layer PTFE content of 8% was close to the cathode air inlet and the part B with a base layer PTFE content of 4.3% was close to the cathode air outlet. A gas diffusion layer having a single PTFE content of 8% in the substrate layer prepared in a similar manner as in example 3 was used as the membrane electrode anode gas diffusion layer, and the cathode gas diffusion layer and the anode gas diffusion layer were hot-pressed in CCM (catalyst coated membrane, anode and cathode platinum loadings, respectively, of 0.2mg/cm 2 And 0.4mg/cm 2 The proton exchange membrane used is Nafion212,) two sides, the hot pressing condition is 120s, 1MPa, 140 ℃; preparing and forming a five-in-one membrane electrode MEA-1.
Preparing MEA-2: the gas diffusion layer with single PTFE content of 8% in the substrate layer is prepared as the cathode gas diffusion layer and the anode gas diffusion layer by the same preparation method as the anode gas diffusion layer of the MEA-1, and the two sides of the same CCM in the MEA-1 are hot-pressed by the same process to form the five-in-one membrane electrode MEA-1.
And (3) respectively and completely activating the MEA-1 membrane electrode and the MEA-2 membrane electrode, and then performing membrane electrode polarization curve I-V characterization.
The battery test conditions are as follows: the cell temperature was 70 ℃, the humidification temperature was 60 ℃, the cell outlet back pressure (cathode air side, anode hydrogen side) was 0kPa, the anode hydrogen stoichiometric ratio was 1.5, and the cathode air stoichiometric ratio was 2.5; the active area of the battery is 150cm 2 。
As shown in FIG. 3, it can be seen that the voltage of MEA-1 is higher than that of MEA at the same current density, and MEA-1 has better discharge performance and discharge efficiency.
Compared with the prior art, the gas diffusion layer of the fuel cell provided by the invention has the advantages that the different areas of the substrate layer in the gas diffusion layer are subjected to hydrophobic treatment in different degrees, so that correspondingly customized water-gas transmission management can be performed on the different areas of the membrane electrode, the running condition of the membrane electrode is improved, the discharge voltage of the membrane electrode is increased, and the discharge efficiency is improved. The technical scheme provided by the invention can be realized only by changing the content of the hydrophobing agent, and has the advantages of low cost and relatively simple process.
The terms "first" and "second" as used herein do not denote any order, quantity, or importance, but rather are used to distinguish one element from another, unless otherwise specified. Similarly, modifiers similar to "about", "approximately" or "approximately" that occur before a numerical term herein typically include the same number, and their specific meaning should be read in conjunction with the context. Similarly, unless a specific number of a claim recitation is intended to cover both the singular and the plural, and also that claim may include both the singular and the plural.
In the description of the specific embodiments above, the use of the directional terms "upper", "lower", "left", "right", "top", "bottom", "vertical", "transverse", and "lateral", etc., are for convenience of description only and should not be considered limiting.
While specific embodiments of the invention have been described above, it will be appreciated by those skilled in the art that these are by way of example only, and that the scope of the invention is defined by the appended claims. Various changes and modifications to these embodiments may be made by those skilled in the art without departing from the spirit and scope of the invention, and these changes and modifications are within the scope of the invention.

Claims (5)

1. A fuel cell gas diffusion layer comprising a substrate layer having a gas diffusion layer surface on one side, and a microporous layer adjacent the other side of the substrate layer, wherein the substrate layer comprises a first portion having a first hydrophobic agent content and a second portion having a second hydrophobic agent content;
the first portion comprises a plurality of first sections; the second portion comprises a plurality of second sections; at least one second section sandwiched between two first sections;
the first part occupies half of the area of the substrate layer, and the second part occupies the other half of the area of the substrate layer;
the numerical ranges of the first hydrophobizing agent content Δ a and the second hydrophobizing agent content Δ b are from 0.5% to 20%, and Δ a > Δ b;
the first portion is in the gas diffusion layer at a position near a gas inlet through which gas moves toward the gas diffusion layer; the second portion is in the gas diffusion layer at a location proximate to a gas outlet through which gas moves away from the gas diffusion layer.
2. The fuel cell gas diffusion layer according to claim 1 wherein the hydrophobic agent is polytetrafluoroethylene.
3. A method of preparing a fuel cell gas diffusion layer according to claim 1 or 2, comprising the steps of:
step 1: taking a piece of dry base layer material which is not subjected to hydrophobic treatment, and dividing the dry base layer material into a part A and a part B in the plane direction;
and 2, step: placing the base layer material at an inlet of a vacuum box, and opening the vacuum box;
and 3, step 3: covering the upper surface of the part B with a film, and coating an aqueous solution with the hydrophobic agent content of m1 on the upper surface of the part A;
and 4, step 4: covering the upper surface of the part A with a film, and coating an aqueous solution with the hydrophobic agent content of m2 on the upper surface of the part B;
and 5: coating microporous layer slurry on one side of the base layer material subjected to the hydrophobic treatment;
step 6: sintering the base layer material coated in the step 5 at a high temperature to form the gas diffusion layer of the fuel cell;
the hydrophobic agent content of the part a of the base layer material produced in the step 6 is larger than the hydrophobic agent content of the part B.
4. The method of preparing a fuel cell gas diffusion layer according to claim 3, wherein step 3 further comprises:
step 31: covering the upper surface of the part B with a film, coating an aqueous solution with the hydrophobing agent content of m1 on the upper surface of the part A, taking off the film on the upper surface of the part B after 3-8 seconds, and turning over the upper surface and the lower surface of the base layer material;
step 32: repeating the step 31 until the water solution with the water repellent agent content of m1 is sprayed in a proper dosage;
step 33: turning over the upper and lower surfaces of the base layer material every 3-8 seconds until the base layer material continues at the inlet of the vacuum box for 13-20 minutes;
the step 4 further comprises:
step 41: covering the upper surface of the part A with a film, coating the upper surface of the part B with an aqueous solution with the content of a hydrophobic agent of m2, taking off the film on the upper surface of the part A after 3-8 seconds, and turning over the upper surface and the lower surface of the base layer material;
step 42: repeating the step 41 until the water solution with the water repellent agent content of m2 is sprayed by proper dosage;
step 43: the upper and lower surfaces of the base layer material were inverted every 3-8 seconds until the base layer material was at the inlet of the vacuum box for 13-20 minutes.
5. The method for preparing a gas diffusion layer for a fuel cell according to claim 3, wherein the base material is any one of carbon paper, carbon cloth, and carbon felt.
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CN113140737B (en) * 2021-01-08 2023-09-22 上海嘉资新材料科技有限公司 Gas diffusion layer, preparation method thereof, corresponding membrane electrode assembly and fuel cell
CN113140738B (en) * 2021-01-08 2023-09-22 上海嘉资新材料科技有限公司 Gas diffusion layer, preparation method thereof, corresponding membrane electrode assembly and fuel cell
CN113140768B (en) * 2021-04-12 2022-03-18 上海交通大学 Cathode side structure of integrated reversible fuel cell membrane electrode
CN115036519A (en) * 2022-07-04 2022-09-09 上海电气集团股份有限公司 Fluorine-doped porous carbon, microporous layer, gas diffusion layer, preparation method and application

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