CN113381045A - Fuel cell membrane electrode and preparation method thereof - Google Patents
Fuel cell membrane electrode and preparation method thereof Download PDFInfo
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Images
Classifications
-
- 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]
-
- 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
- H01M2008/1095—Fuel cells with polymeric electrolytes
-
- 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
Abstract
The invention belongs to the field of fuel cells, and particularly relates to a preparation method of a fuel cell membrane electrode, which comprises the following steps: preparing a first transfer film compounded with a first catalyst layer, a second transfer film compounded with a second catalyst layer and a proton exchange membrane compounded with a protective film; compounding a first transfer film compounded with a first catalyst layer on a first support film, wherein the first transfer film is connected with the first support film; hot-pressing and transferring the proton exchange membrane compounded with the protective membrane to the surface of the first catalyst layer, and stripping the protective membrane; compounding the second transfer printing film compounded with the second catalyst layer on a second support film, and performing hot-pressing transfer printing on the surface of the proton exchange membrane, wherein the second catalyst layer is connected with the proton exchange membrane; and stripping the second transfer printing film and the second support film, pasting a second frame film on the edge of the second catalyst layer, stripping the first transfer printing film and the first support film, and pasting a first frame film on the edge of the first catalyst layer. Compared with the prior art, the invention solves the problem of wrinkling of the proton exchange membrane.
Description
Technical Field
The invention belongs to the technical field of fuel cells, and particularly relates to a fuel cell membrane electrode and a preparation method thereof.
Background
A fuel cell is a power generation device that directly converts chemical energy present in a fuel and an oxidant into electrical energy. The fuel cell has the advantages of zero emission, no vibration noise, good load responsiveness, high reliability and the like. Fuel cells can be generally classified into alkaline fuel cells, phosphoric acid type fuel cells, molten carbon carbonate fuel cells, solid oxide fuel cells, proton exchange membrane fuel cells, and the like; among them, the proton exchange membrane fuel cell has high energy conversion efficiency, can be started quickly at room temperature, has no loss of electrolytic water, has long service life, and is developed rapidly and more emphasized in recent years.
The membrane electrode is a core component of a proton exchange membrane fuel cell, and generally consists of a proton exchange membrane and electrodes respectively arranged on two surfaces of the proton exchange membrane. Typically, the electrode in turn comprises a catalyst layer and a gas diffusion layer, with the catalyst layer being disposed between the gas diffusion layer and the proton exchange membrane. The catalyst layer is prepared by two methods, one is a direct method in which the catalyst slurry is directly coated on the proton exchange membrane, and the other is an indirect method in which the catalyst slurry is coated on a transfer medium and then the catalyst layer is fixed on the proton exchange membrane by hot pressing. Although the direct method is simple to operate, the catalyst slurry contains a lower alcohol solvent, and the proton exchange membrane can generate swelling wrinkles after meeting the solvent, so that the direct coating of the catalyst slurry is difficult, particularly when the coating of the second surface of the proton exchange membrane is completed. Although the indirect method can solve the problem of swelling and wrinkling of the proton exchange membrane, the proton exchange membrane can lose water and shrink under the action of hot pressing (the temperature is more than 80 ℃ and the pressure is more than 1 MPa) in the transfer process, and the proton exchange membrane can also wrinkle.
Disclosure of Invention
One of the objects of the present invention is: aiming at the defects of the prior art, the preparation method of the fuel cell membrane electrode is provided, the problem of wrinkling of the proton exchange membrane is solved, and the flatness is improved.
In order to achieve the purpose, the invention adopts the following technical scheme:
a preparation method of a fuel cell membrane electrode comprises the following steps:
s1, preparing a first transfer film compounded with a first catalyst layer, a second transfer film compounded with a second catalyst layer and a proton exchange membrane compounded with a protective film respectively;
s2, laminating the first transfer film laminated with the first catalyst layer on a first support film, the first transfer film being connected to the first support film;
s3, transferring the proton exchange membrane compounded with the protective membrane to the surface of the first catalyst layer in a hot pressing manner, and stripping the protective membrane;
s4, compounding the second transfer printing film compounded with the second catalyst layer on a second support film, and performing hot-pressing transfer printing on the surface of the proton exchange membrane, wherein the second catalyst layer is connected with the proton exchange membrane to form a membrane electrode intermediate;
and S5, peeling the second transfer film and the second support film which are connected with the second catalyst layer, attaching a second frame film at the edge of the second catalyst layer, peeling the first transfer film and the first support film which are connected with the first catalyst layer, and attaching a first frame film at the edge of the first catalyst layer to obtain the membrane electrode.
In steps S3 and S4, the temperature of the hot-press transfer printing is 80-160 ℃, and the pressure is 1-6 MPa. In the hot press transfer process, temperature is an important factor. Only when the temperature during hot pressing exceeds a certain temperature (more than 80 ℃), the hydrogen-conducting proton resin in the catalyst layer is fused and bonded with the proton exchange membrane under a certain pressure, and the first catalyst layer, the second catalyst layer and the proton exchange membrane can be firmly combined, so that the aim of reducing the contact resistance is fulfilled, and the transfer medium can be peeled off from the release membrane.
In the preparation method, on one hand, the first catalyst layer and the second catalyst layer are respectively compounded with the proton exchange membrane by adopting a hot-pressing transfer printing method, so that swelling and wrinkling caused by directly spraying the catalyst slurry on the proton exchange membrane can be avoided; on the other hand, a layer of protective film is compounded on the proton exchange membrane, and a support film is compounded outside the transfer release film, so that in the transfer process, the protective film plays a role in supporting and reinforcing the proton exchange membrane, the support film and the proton exchange membrane form good bonding support, and the proton exchange membrane can be prevented from wrinkling due to water loss shrinkage under the hot pressing effect.
In step S1, a first catalyst is mixed with a hydrogen-conductive proton resin solution, and a mixture of deionized water and one or more organic solvents is added to the mixture to prepare a first catalyst slurry through ultrasonic or shear emulsification, the first catalyst slurry is coated on the surface of a first transfer membrane, and the first transfer membrane compounded with a first catalyst layer is obtained through drying. The hydrogen-conducting proton resin solution can be a perfluorinated sulfonic acid resin solution, a partially fluorinated resin solution, a non-fluorinated resin solution or a hydrocarbon resin solution.
As an improvement of the preparation method of the fuel cell membrane electrode, the first catalyst is a noble metal catalyst or a carbon-supported noble metal catalyst, wherein the content of noble metal is 0.01-1 mg/cm2The noble metal is at least one of Pt, Ru, Ir, Au, Ag and Pd, or the noble metal is binary or above alloy formed by at least one of Pt, Ru, Ir, Au, Ag and Pd and Co, Ni or Mn.
In step S1, a second catalyst is mixed with a hydrogen-conductive proton resin solution, and a mixture of deionized water and one or more organic solvents is added, and a second catalyst slurry is prepared by ultrasonic or shear emulsification, and is coated on the surface of a second transfer film, and dried to obtain the second transfer film with a second catalyst layer. The hydrogen-conducting proton resin solution can be a perfluorinated sulfonic acid resin solution, a partially fluorinated resin solution, a non-fluorinated resin solution or a hydrocarbon resin solution.
As an improvement of the method for preparing a fuel cell membrane electrode according to the present invention,the second catalyst is a noble metal catalyst or a carbon-supported noble metal catalyst, wherein the content of noble metal is 0.01-1 mg/cm2The noble metal is at least one of Pt, Ru, Ir, Au, Ag and Pd, or the noble metal is binary or above alloy formed by at least one of Pt, Ru, Ir, Au, Ag and Pd and Co, Ni or Mn.
As an improvement of the method for manufacturing a fuel cell membrane electrode according to the present invention, in step S5, the first frame film and the second frame film are provided with a reinforcing layer, and the reinforcing layer is peeled off after the attachment. The reinforcing layer is used for reinforcing the strength of the first frame film and the second frame film and preventing the first frame film and the second frame film from wrinkling, warping and even being damaged in the pasting process.
The proton exchange membrane comprises but is not limited to a perfluorinated sulfonic acid resin proton exchange membrane, a sulfonated polyphenylquinoxaline proton exchange membrane, a sulfonated poly-diphenol proton exchange membrane, a polybenzimidazole proton exchange membrane, a polyether ether ketone proton exchange membrane, a sulfonated polysulfone proton exchange membrane, a sulfonated polyether sulfone proton exchange membrane or a porous PTFE composite proton exchange membrane deposited with perfluorinated sulfonic acid resin. The proton exchange membrane only needs to be capable of conducting hydrogen protons, and is a perfluorinated, partially fluorinated or non-fluorinated proton exchange membrane.
As an improvement of the preparation method of the fuel cell membrane electrode of the present invention, the first transfer film and the second transfer film are both release films, and the protective film, the first support film and the second support film are thin films on which bonding layers are coated. The release film includes but is not limited to any one of a PET release film, a BOPP release film, a PTFE release film, an ETFE release film, an FEP release film, a PMP release film, a PE release film, a PVC release film, an EVA release film, a PC release film, an ABS release film, a PS release film and a PMMA release film or a composite film formed by at least two of the above.
As an improvement of the preparation method of the fuel cell membrane electrode, the thickness of the first catalyst layer and the second catalyst layer is 0.5-100 μm, and the thickness of the first frame membrane and the second frame membrane is 10-500 μm.
The second purpose of the invention is: the fuel cell membrane electrode prepared by the preparation method described in any section of the specification comprises a proton exchange membrane, a first catalyst layer compounded on one surface of the proton exchange membrane, a second catalyst layer compounded on the other surface of the proton exchange membrane, a first frame membrane attached to the edge of the first catalyst layer, and a second frame membrane attached to the edge of the second catalyst layer.
Compared with the prior art, the invention at least has the following beneficial effects:
1) in the preparation method, the first catalyst layer and the second catalyst layer are respectively compounded with the proton exchange membrane by adopting a hot-pressing transfer printing method, so that swelling and wrinkling caused by directly spraying the catalyst slurry on the proton exchange membrane can be avoided.
2) In the preparation method, the protective film is compounded on the proton exchange membrane, the protective film plays a role in supporting and reinforcing, and the proton exchange membrane can be prevented from wrinkling caused by water loss under the action of hot pressing in the process of hot pressing and transfer printing of the proton exchange membrane.
3) In the preparation method, the support film is compounded outside the transfer-printing release film, and in the transfer-printing process, the support film and the proton exchange membrane form good bonding support, so that the proton exchange membrane can be prevented from wrinkling due to water loss under the action of hot pressing.
4) The membrane electrode prepared by the preparation method has high yield, and when the membrane electrode is used for a fuel cell, the membrane electrode has good durability and long service life.
Drawings
FIG. 1 is a schematic flow chart of the production process of the present invention.
Wherein: the catalyst comprises a proton exchange membrane 1, a first catalyst layer 2, a second catalyst layer 3, a first frame membrane 4, a second frame membrane 5, a first support membrane 6, a first transfer membrane 7, a first protection membrane 8, a second transfer membrane 9, a second support membrane 10, a membrane electrode intermediate 100 and a membrane electrode 200.
Detailed Description
The present invention will be described in further detail with reference to the following detailed description and the accompanying drawings, but the embodiments of the invention are not limited thereto.
Example 1
As shown in fig. 1, a method for preparing a membrane electrode of a fuel cell includes the following steps:
s1, preparing a first transfer film 7 compounded with the first catalyst layer 2, a second transfer film 9 compounded with the second catalyst layer 3, and a proton exchange membrane 1 compounded with the protective film 8, respectively;
s2, laminating the first transfer sheet 7 laminated with the first catalyst layer 2 on the first support sheet 6, the first transfer sheet 7 being connected to the first support sheet 6;
s3, transferring the proton exchange membrane 1 compounded with the protective membrane 8 to the surface of the first catalyst layer 2 in a hot pressing way, and stripping the protective membrane 8;
s4, compounding the second transfer film 9 compounded with the second catalyst layer 3 on the second support film 10, and performing hot-pressing transfer on the surface of the proton exchange membrane 1, wherein the second catalyst layer 3 is connected with the proton exchange membrane 1 to form a membrane electrode intermediate 100;
s5, the first transfer film 9 and the second support film 10 connected to the second catalyst layer 3 are peeled off, the second frame film 5 is attached to the edge of the second catalyst layer 3, the first transfer film 7 and the first support film 6 connected to the first catalyst layer 2 are peeled off, and the first frame film 4 is attached to the edge of the first catalyst layer 2, thereby obtaining the membrane electrode 200.
Preferably, in step S1, the first catalyst is mixed with the hydrogen-conductive proton resin solution, and a mixture of deionized water and one or more organic solvents is added, and the mixture is emulsified by ultrasound or shearing to prepare a first catalyst slurry, which is coated on the surface of the first transfer membrane 7 and dried to obtain the first transfer membrane 7 combined with the first catalyst layer 2. Wherein the first catalyst is a noble metal catalyst or a carbon-supported noble metal catalyst, and the content of noble metal is 0.01-1 mg/cm2The noble metal is at least one of Pt, Ru, Ir, Au, Ag and Pd, or the noble metal is Pt, Ru, Ir, Au, Ag and PdAnd at least one of Co, Ni and Mn. Similarly, the second catalyst is mixed with the hydrogen-conductive proton resin solution, and a mixed solution of deionized water and one or more organic solvents is added, and the mixture is prepared into a second catalyst slurry by ultrasonic or shear emulsification, and the second catalyst slurry is coated on the surface of the second transfer film 9 and dried to obtain the second transfer film 9 compounded with the second catalyst layer 3. The second catalyst is a noble metal catalyst or a carbon-supported noble metal catalyst, wherein the content of noble metal is 0.01-1 mg/cm2The noble metal is at least one of Pt, Ru, Ir, Au, Ag and Pd, or the noble metal is binary or above alloy formed by at least one of Pt, Ru, Ir, Au, Ag and Pd and Co, Ni or Mn.
Preferably, in step S5, the first frame film 4 and the second frame film 5 are provided with reinforcing layers, and the reinforcing layers are peeled off after the attachment is completed.
Preferably, the proton exchange membrane 1 includes, but is not limited to, a perfluorosulfonic acid resin proton exchange membrane, a sulfonated polyphenylquinoxaline proton exchange membrane, a sulfonated poly-diphenol proton exchange membrane, a polybenzimidazole proton exchange membrane, a polyetheretherketone proton exchange membrane, a sulfonated polysulfone proton exchange membrane, a sulfonated polyethersulfone proton exchange membrane, or a porous PTFE composite proton exchange membrane deposited with a perfluorosulfonic acid resin. The proton exchange membrane 1 only needs to be capable of conducting hydrogen protons, and most of the proton exchange membrane 1 is a perfluorinated, partially fluorinated or non-fluorinated proton exchange membrane.
Preferably, the first transfer film 7 and the second transfer film 9 are both release films, and the protective film 8, the first support film 6, and the second support film 10 are films coated with adhesive layers. The release film includes but is not limited to any one of a PET release film, a BOPP release film, a PTFE release film, an ETFE release film, an FEP release film, a PMP release film, a PE release film, a PVC release film, an EVA release film, a PC release film, an ABS release film, a PS release film and a PMMA release film or a composite film formed by at least two of the above.
Preferably, the first catalyst layer 2 and the second catalyst layer 3 have a thickness of 0.5 to 100 μm, and the first frame film 4 and the second frame film 5 have a thickness of 10 to 500 μm.
Example 2
A fuel cell membrane electrode 200 prepared by the preparation method of embodiment 1 includes a proton exchange membrane 1, a first catalyst layer 2 compounded on one surface of the proton exchange membrane 1, a second catalyst layer 3 compounded on the other surface of the proton exchange membrane 1, a first frame membrane 4 attached to the edge of the first catalyst layer 2, and a second frame membrane 5 attached to the edge of the second catalyst layer 3.
Performance testing
1) 100 fuel cell membrane electrodes prepared by the preparation method of example 1, 100 fuel cell membrane electrodes prepared by the direct method described in the background art, and 100 fuel cell membrane electrodes prepared by the indirect method described in the background art were extracted, respectively, and the appearance of the membrane electrodes was observed, and the yield of the membrane electrodes was calculated. The results are shown in Table 1.
2) The fuel cell membrane electrode prepared by the preparation method of example 1, the membrane electrode prepared by the direct method and the membrane electrode prepared by the indirect method are respectively assembled into a galvanic pile for life test, the discharge temperature is 80 ℃, the anode hydrogen metering ratio is 1.5 times, the relative humidity is 80% RH, the cathode gas feeding ratio is 2 times, the relative humidity is 80% RH, and the discharge current density is 800mA/cm2The stack life is defined as the run time at which the stack output voltage decays by 10%.
TABLE 1 test results
It can be seen from the test results in table 1 that, compared with the membrane electrode prepared by the existing direct method and indirect method, the membrane electrode of the fuel cell prepared by the preparation method of the present invention has the advantages of good appearance, no wrinkling of the proton exchange membrane, intact catalyst layer, high yield and long service life. This is because, in the preparation method of the present invention, on one hand, the first catalyst layer and the second catalyst layer are respectively compounded with the proton exchange membrane by using a hot-pressing transfer method, which can avoid swelling and wrinkling caused by directly spraying the catalyst slurry on the proton exchange membrane; on the other hand, a layer of protective film is compounded on the proton exchange membrane, and a support film is compounded outside the transfer release film, so that in the transfer process, the protective film plays a role in supporting and reinforcing the proton exchange membrane, the support film and the proton exchange membrane form good bonding support, and the proton exchange membrane can be prevented from wrinkling due to water loss shrinkage under the hot pressing effect.
Variations and modifications to the above-described embodiments may also occur to those skilled in the art, which fall within the scope of the invention as disclosed and taught herein. Therefore, the present invention is not limited to the above-mentioned embodiments, and any obvious improvement, replacement or modification made by those skilled in the art based on the present invention is within the protection scope of the present invention. Furthermore, although specific terms are employed herein, they are used in a generic and descriptive sense only and not for purposes of limitation.
Claims (10)
1. A preparation method of a fuel cell membrane electrode is characterized by comprising the following steps:
s1, preparing a first transfer film compounded with a first catalyst layer, a second transfer film compounded with a second catalyst layer and a proton exchange membrane compounded with a protective film respectively;
s2, laminating the first transfer film laminated with the first catalyst layer on a first support film, the first transfer film being connected to the first support film;
s3, transferring the proton exchange membrane compounded with the protective membrane to the surface of the first catalyst layer in a hot pressing manner, and stripping the protective membrane;
s4, compounding the second transfer printing film compounded with the second catalyst layer on a second support film, and performing hot-pressing transfer printing on the surface of the proton exchange membrane, wherein the second catalyst layer is connected with the proton exchange membrane to form a membrane electrode intermediate;
and S5, peeling the second transfer film and the second support film which are connected with the second catalyst layer, attaching a second frame film at the edge of the second catalyst layer, peeling the first transfer film and the first support film which are connected with the first catalyst layer, and attaching a first frame film at the edge of the first catalyst layer to obtain the membrane electrode.
2. The method for preparing a fuel cell membrane electrode according to claim 1, wherein in step S1, the first catalyst is mixed with the hydrogen-conductive proton resin solution, and the mixture of deionized water and one or more organic solvents is added to the mixture to prepare a first catalyst slurry by ultrasonic or shear emulsification, and the first catalyst slurry is coated on the surface of the first transfer membrane and dried to obtain the first transfer membrane with the first catalyst layer.
3. The method for preparing a fuel cell membrane electrode according to claim 2, wherein the first catalyst is a noble metal catalyst or a carbon-supported noble metal catalyst, and the noble metal content is 0.01 to 1mg/cm2The noble metal is at least one of Pt, Ru, Ir, Au, Ag and Pd, or the noble metal is binary or above alloy formed by at least one of Pt, Ru, Ir, Au, Ag and Pd and Co, Ni or Mn.
4. The method for preparing a fuel cell membrane electrode according to claim 1, wherein in step S1, the second catalyst is mixed with the hydrogen-conductive proton resin solution, and a mixture of deionized water and one or more organic solvents is added to the mixture, and the mixture is ultrasonically or shear-emulsified to prepare a second catalyst slurry, which is coated on the surface of the second transfer film, and dried to obtain the second transfer film with the second catalyst layer.
5. The method for preparing a fuel cell membrane electrode according to claim 4, wherein the second catalyst is a noble metal catalyst or a carbon-supported noble metal catalyst, and the noble metal content is 0.01 to 1mg/cm2The noble metal is at least one of Pt, Ru, Ir, Au, Ag and Pd, or the noble metal is binary or above alloy formed by at least one of Pt, Ru, Ir, Au, Ag and Pd and Co, Ni or Mn.
6. The method for producing a fuel cell membrane electrode assembly according to claim 1, wherein in step S5, the first frame film and the second frame film are each provided with a reinforcing layer, and the reinforcing layers are peeled off after the attachment.
7. The method for preparing a fuel cell membrane electrode according to claim 1, wherein the proton exchange membrane comprises a perfluorosulfonic acid resin proton exchange membrane, a sulfonated polyphenylquinoxaline proton exchange membrane, a sulfonated poly-diphenol proton exchange membrane, a polybenzimidazole proton exchange membrane, a polyetheretherketone proton exchange membrane, a sulfonated polysulfone proton exchange membrane, a sulfonated polyethersulfone proton exchange membrane, or a porous PTFE composite proton exchange membrane deposited with a perfluorosulfonic acid resin.
8. The method for manufacturing a fuel cell membrane electrode according to claim 1, wherein the first transfer film and the second transfer film are both release films, and the protective film, the first support film, and the second support film are all thin films with adhesive layers applied thereto.
9. The method for producing a fuel cell membrane electrode according to claim 1, wherein the thickness of the first catalyst layer and the second catalyst layer is 0.5 to 100 μm, and the thickness of the first frame film and the second frame film is 10 to 500 μm.
10. A fuel cell membrane electrode comprises a proton exchange membrane, a first catalyst layer compounded on one surface of the proton exchange membrane, a second catalyst layer compounded on the other surface of the proton exchange membrane, a first frame membrane attached to the edge of the first catalyst layer and a second frame membrane attached to the edge of the second catalyst layer, and is characterized by being prepared by the preparation method of any one of claims 1 to 9.
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