CN117013023A - Fuel cell membrane electrode with mass transfer array and preparation method thereof - Google Patents

Fuel cell membrane electrode with mass transfer array and preparation method thereof Download PDF

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Publication number
CN117013023A
CN117013023A CN202310916671.1A CN202310916671A CN117013023A CN 117013023 A CN117013023 A CN 117013023A CN 202310916671 A CN202310916671 A CN 202310916671A CN 117013023 A CN117013023 A CN 117013023A
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China
Prior art keywords
cathode
anode
layer
fuel cell
catalytic layer
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CN202310916671.1A
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Chinese (zh)
Inventor
朱凤鹃
王超
王一鑫
龚云海
沈逸东
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Zhejiang Tangfeng Energy Technology Co ltd
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Zhejiang Tangfeng Energy Technology Co ltd
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Priority to CN202310916671.1A priority Critical patent/CN117013023A/en
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    • H—ELECTRICITY
    • H01—ELECTRIC ELEMENTS
    • H01M—PROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
    • H01M8/00—Fuel cells; Manufacture thereof
    • H01M8/10—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
    • H01M4/00—Electrodes
    • H01M4/86—Inert electrodes with catalytic activity, e.g. for fuel cells
    • 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
    • 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
    • H01M4/90—Selection of catalytic material
    • H01M4/92—Metals of platinum group
    • 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
    • H01M8/1016—Fuel cells with solid electrolytes characterised by the electrolyte material
    • H01M8/1018—Polymeric electrolyte materials
    • 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)
  • Life Sciences & Earth Sciences (AREA)
  • Sustainable Development (AREA)
  • Sustainable Energy (AREA)
  • Materials Engineering (AREA)
  • Inert Electrodes (AREA)
  • Fuel Cell (AREA)

Abstract

The invention relates to the technical field of fuel cells, in particular to a fuel cell membrane electrode with a mass transfer array and a preparation method thereof, wherein the fuel cell membrane electrode comprises a cathode catalytic layer, the cathode catalytic layer is a cathode catalyst slurry solidifying layer coated on the front surface of a cathode substrate membrane, a plurality of through holes extending up and down and penetrating through the cathode catalyst slurry solidifying layer are formed on the cathode catalyst slurry solidifying layer, the aperture of each through hole is 1-2 mu m, each through hole is rectangular dot array, the hole distance between two adjacent through holes is 7-13 mu m, each through hole is a laser hole, and the mass transfer effect is good.

Description

Fuel cell membrane electrode with mass transfer array and preparation method thereof
Technical Field
The invention relates to the technical field of fuel cells, in particular to a fuel cell membrane electrode with a mass transfer array and a preparation method thereof.
Background
The performance of the existing fuel cell faces three losses, namely electrochemical polarization, ohmic polarization and mass transfer polarization, wherein the catalytic layer has low porosity and few through holes, and is a main component for occurrence of mass transfer polarization of the membrane electrode. Therefore, the improvement of the mass transfer efficiency of the catalytic layer is of great significance for improving the battery performance. At present, the mass transfer efficiency of the catalytic layer is improved by the following steps, firstly, a large number of secondary holes are promoted in the preparation and forming process of the catalytic layer by adjusting a solvent and an additive, so that a convenient channel of oxygen is formed, and the method has low flexibility of material use and is not beneficial to quickly manufacturing membrane electrodes applicable to different requirements; secondly, platinum is loaded on an ordered nano array to be used as a catalytic layer, and a large number of through holes are formed in the catalytic layer, so that the catalytic layer is the most ideal oxygen mass transfer path, but the preparation process has higher cost and is not beneficial to large-scale production; thirdly, the fibrous material is used for preparing the catalytic layer, and the fibrous platinum-carbon catalyst or the ionic resin can be used for lap joint into a loose structure by utilizing the length of the fibrous material to form large-size secondary holes, but the fibrous material has a lower fiber ratio on the surface, platinum is difficult to load, and the excessive addition of the fibrous material adversely affects the performance of the battery.
A method of manufacturing a membrane electrode assembly, a membrane electrode assembly manufactured thereby, and a fuel cell including the membrane electrode assembly are disclosed in chinese patent application No. 201780021158.9. The method for manufacturing the membrane electrode assembly further comprises the following steps: after drying the catalyst slurry composition and then adding the solvent B thereto, the catalyst slurry composition is re-homogenized by ultrasonic waves, and this manufacturing method is first carried out during the preparation of the catalyst layer by ultrasonic means, but the manufacturing time is long, the solvent is required to be used several times, and the production efficiency and cost are not optimized.
Disclosure of Invention
The invention aims to provide a fuel cell membrane electrode with a mass transfer array and a preparation method thereof, wherein the fuel cell membrane electrode has good mass transfer effect.
The above object of the present invention is achieved by the following technical solutions:
the cathode catalyst layer of the fuel cell is a cathode catalyst slurry curing layer coated on the front surface of a cathode substrate film, a plurality of through holes extending up and down and penetrating through the cathode catalyst slurry curing layer are formed on the cathode catalyst slurry curing layer, the aperture of each through hole is 1-2 mu m, each through hole is in a rectangular point array shape, the hole distance between two adjacent through holes is 7-13 mu m, and each through hole is a laser hole.
As a preferred mode of the present invention, the cathode catalyst slurry cured layer has a thickness of 6 to 7 μm and a platinum loading of 0.2 to 0.4mg/cm 2 。
The fuel cell membrane electrode comprises the fuel cell cathode catalytic layer, an anode catalytic layer and a proton membrane, wherein the anode catalytic layer is an anode catalyst slurry curing layer coated on the front surface of an anode substrate membrane, and the proton membrane is bonded between the cathode catalytic layer and the anode catalytic layer in a hot-pressing mode.
As a preferred embodiment of the present invention, the cathode base film and the anode base film are both PTFE films.
As a preferable mode of the invention, the platinum loading of the anode catalytic layer is 0.02-0.1mg/cm 2 。
A method for preparing a cathode catalytic layer of a fuel cell, comprising the steps of: step 1, adding a platinum carbon catalyst and an ionic resin into a mixed solvent of water and isopropanol to form cathode initial slurry, and ball-milling the cathode initial slurry for 24 hours to obtain cathode catalyst slurry; step 2, spraying cathode catalyst slurry on the front surface of the cathode substrate film, and then drying to obtain a cathode catalyst layer to be treated, which is attached to the cathode substrate film; and 3, punching a plurality of through holes in a rectangular point array shape on the cathode catalytic layer to be treated by using a laser beam to obtain the cathode catalytic layer attached to the cathode substrate film.
As a preferable mode of the present invention, the diameter of the through hole is 1-2 μm, and the hole spacing between two adjacent through holes is 7-13 μm.
As a preferred mode of the present invention, the laser beam is a lattice laser beam.
The preparation method of the fuel cell membrane electrode comprises the preparation method of the fuel cell cathode catalytic layer, and further comprises the following steps: step 4, adding a platinum carbon catalyst and an ion resin into the mixed solvent of water and isopropanol to form anode initial slurry, and ball-milling the anode initial slurry for 24 hours to obtain anode catalyst slurry; step 5, spraying anode catalyst slurry on the front surface of the anode substrate film, and drying to obtain an anode catalyst layer attached to the anode substrate film; and 6, respectively placing the cathode catalytic layer and the anode catalytic layer on two sides of the proton membrane, enabling the proton membrane to be clamped between the surface of the anode catalytic layer and the surface of the anode catalytic layer, carrying out hot pressing and compounding on the cathode catalytic layer and the anode catalytic layer through a hot press, and removing the substrate membranes on the two sides to obtain the membrane electrode.
As a preferable mode of the invention, the platinum loading of the anode catalytic layer is 0.02-0.1mg/cm 2 。
The invention has the beneficial effects that: the cathode catalytic layer is provided with a large number of straight through holes in the shape of a dot array, so that the mass transfer efficiency is excellent;
the novel preparation method adopts the laser technology to prepare the straight-through hole lattice on the surface of the cathode catalytic layer, has high preparation efficiency and is suitable for rapid production.
Drawings
FIG. 1 is a schematic view showing the structure of example 1, which is a 1 st laser treatment mode of a cathode catalytic layer in the example;
FIG. 2 is a schematic diagram of a cathode catalytic layer of a laser processing mode according to example 2;
FIG. 3 is a schematic view showing the structure of example 3, which is a 3 rd laser treatment mode of the cathode catalytic layer in the example;
FIG. 4 is a schematic diagram showing the structure of a fourth comparative example of the No. 4 laser treatment mode of the cathode catalyst layer in the example;
FIG. 5 is a schematic illustration of electrical properties of 4 cathode catalytic layers of the membrane electrode in the example under different laser treatments;
fig. 6 is a schematic diagram of mass transfer performance of 4 cathode catalytic layers of the membrane electrode in the example under different laser treatments.
Detailed Description
The present invention will be described in further detail with reference to the accompanying drawings.
The present embodiment is only for explanation of the present invention and is not to be construed as limiting the present invention, and modifications to the present embodiment, which may not creatively contribute to the present invention, may be made by those skilled in the art after reading the present specification, are only protected by patent laws within the scope of the claims of the present invention.
Examples: as shown in fig. 1-6, a cathode catalyst layer of a fuel cell is a cathode catalyst slurry solidified layer 12 coated on the front surface of a cathode substrate film 11, a plurality of through holes 120 extending up and down and penetrating through the cathode catalyst slurry solidified layer 12 are formed on the cathode catalyst slurry solidified layer 12, the aperture of each through hole 120 is 1-2 μm, each through hole 120 is in a rectangular point array shape, the hole spacing between two adjacent through holes 120 is 7-13 μm, each through hole 120 is a laser hole, the through holes 120 in the embodiment are characterized by being laser holes, namely, holes punched by laser and are arranged in a rectangular lattice structure, preferably, the hole spacing between two adjacent through holes 120 is a spacing in the left-right direction or the front-back direction, namely, the center spacing between two adjacent holes in the orthogonal direction, the structure can be processed, the cathode catalyst layer of the structure is better in efficiency, namely, the cell is well designed in the design, the mass transfer process is better in the mass transfer process, and the mass transfer condition is better in the mass transfer process is planned, and the mass transfer process is better in the mass transfer process.
Preferably, the cathode catalyst slurry cured layer 12 has a thickness of 6 to 7 μm and a platinum loading of 0.2 to 0.4mg/cm 2 . The platinum loading is relatively large due to the need to provide through-holes 120.
The present embodiment also provides a fuel cell membrane electrode, which comprises the foregoing fuel cell cathode catalytic layer, and further comprises an anode catalytic layer and a proton membrane 3, wherein the anode catalytic layer is an anode catalyst slurry curing layer 22 coated on the front surface of the anode substrate membrane 21, and the proton membrane 3 is bonded between the cathode catalytic layer and the anode catalytic layer by hot pressing, so that the membrane electrode uses the new cathode catalytic layer, and the anode catalytic layer is not provided with a through hole 120, and the anode catalytic layer is only coated, dried and cured.
Preferably, the cathode base film 11 and the anode base film 21 are both PTFE films, i.e., polytetrafluoroethylene films. While the platinum loading of the anode catalytic layer is preferably 0.02-0.1mg/cm 2 The platinum loading can be set smaller without much.
The embodiment also provides a preparation method of the cathode catalytic layer of the fuel cell, which comprises the following steps: step 1, adding a platinum carbon catalyst and an ionic resin into a mixed solvent of water and isopropanol to form cathode initial slurry, and ball-milling the cathode initial slurry for 24 hours to obtain cathode catalyst slurry; step 2, spraying cathode catalyst slurry on the front surface of the cathode substrate film 11, and then drying to obtain a cathode catalyst layer to be treated, which is attached to the cathode substrate film; and 3, punching a plurality of through holes 120 in a rectangular point array shape on the cathode catalytic layer to be treated by using a laser beam to obtain the cathode catalytic layer attached to the cathode substrate film.
Preferably, the diameter of the through holes 120 is 1-2 μm, and the hole spacing between two adjacent through holes 120 is 7-13 μm. Further, the laser beam is a lattice laser beam.
The embodiment also provides a preparation method of the fuel cell membrane electrode, which comprises the preparation method of the fuel cell cathode catalytic layer and further comprises the following steps: step 4, adding a platinum carbon catalyst and an ion resin into the mixed solvent of water and isopropanol to form anode initial slurry, and ball-milling the anode initial slurry for 24 hours to obtain anode catalyst slurry; step 5, spraying anode catalyst slurry on the front surface of the anode substrate film, and drying to obtain an anode catalyst layer attached to the anode substrate film; step 6, respectively placing the cathode catalytic layer and the anode catalytic layer on two sides of the proton membrane 3 to enable the proton membrane 3 to be clamped on the surface of the anode catalytic layer and the surface of the anode catalytic layerAnd (3) hot-pressing and compounding the three materials by a hot press, and removing the substrate films on the two sides to obtain the membrane electrode. And the platinum loading of the anode catalytic layer is 0.02-0.1mg/cm 2 。
Through the design of the scheme, specific examples are:
and adding a mixed solvent of water and isopropanol into Pt/C (platinum carbon catalyst) and ion resin, and then ball-milling for 24 hours to obtain catalyst slurry. Pre-milling the slurry with an I/C value of between 0.4 and 0.6 (I/c=mass of ionic resin/mass of carbon in catalyst) and a solids content of between 4 and 5%;
spraying the slurry on a PTFE substrate, and drying to obtain a catalytic layer with a platinum loading of 0.3-0.4mg/cm 2 A thickness of about 6-7um;
punching a straight-through hole lattice on the dried catalytic layer by using a laser beam, wherein the aperture is 1-2um, and the hole spacing is 10um, so as to finally obtain a cathode catalytic layer;
the preparation method of the anode catalytic layer and the cathode catalytic layer is the same, but the platinum loading of the catalytic layer is 0.02-0.1mg/cm without laser treatment 2 ；
The anode catalytic layer and the cathode catalytic layer are thermally compounded on two sides of the proton membrane to obtain the membrane electrode.
Based on the specific preparation method, the following four different embodiment schemes are made for the laser treatment of the cathode catalytic layer:
example 1: the lattice aperture is 1um, and the hole spacing is 10um.
Example 2: the lattice aperture is 1um, and the hole spacing is 20um.
Example 3: the lattice is replaced by transverse grooves with the width of 1um, the groove spacing is 10um, and the direction of the transverse grooves is perpendicular to the flow field.
Comparative example 1: no treatment was performed.
After the experiment, the following conclusions can be drawn from fig. 5, 6:
example 1: the through holes enhance mass transfer efficiency and therefore perform better under high current conditions (fig. 5) and have lower mass transfer resistance (fig. 6).
Example 2: the number of through holes is reduced, and the mass transfer enhancement effect is weakened. Performance at high current is reduced compared to example 1 (FIG. 5) and mass transfer resistance is relatively high (FIG. 6)
Example 3: the transverse groove direction is perpendicular to the flow channel direction, so that the mass transfer effect under the ridge is enhanced, and the best mass transfer effect is achieved. Good performance can be achieved under high current conditions (FIG. 5) and mass transfer resistance is also significantly reduced (FIG. 6)
Comparative example 1: as a control group.
Thus, the mass transfer resistances of examples 1, 3 are lower.
While the invention has been described with reference to certain preferred embodiments, it will be understood by those skilled in the art that various changes and substitutions of equivalents may be made and equivalents will be apparent to those skilled in the art without departing from the scope of the invention. Therefore, the protection scope of the invention is subject to the protection scope of the claims.

Claims (10)

1. The fuel cell membrane electrode with the mass transfer array is characterized by comprising a cathode catalytic layer, wherein the cathode catalytic layer is a cathode catalyst slurry solidified layer (12) coated on the front surface of a cathode substrate membrane (11), a plurality of through holes (120) which extend up and down and penetrate through the cathode catalyst slurry solidified layer (12) are formed on the cathode catalyst slurry solidified layer (12), the aperture of each through hole (120) is 1-2 mu m, each through hole (120) is in a rectangular point array shape, the hole distance between two adjacent through holes (120) is 7-13 mu m, and each through hole (120) is a laser hole.
2. The fuel cell membrane electrode with mass transfer array according to claim 1 wherein the cathode catalyst slurry solidified layer (12) has a thickness of 6-7 μm and a platinum loading of 0.2-0.4mg/cm 2 。
3. The fuel cell membrane electrode with mass transfer array according to claim 2 further comprising an anode catalyst layer, which is an anode catalyst slurry cured layer (22) coated at the front surface of the anode base membrane (21), and a proton membrane (3), which proton membrane (3) is thermocompression bonded between the cathode catalyst layer and the anode catalyst layer.
4. A fuel cell membrane electrode with a mass transfer array according to claim 1, characterized in that the cathode substrate membrane (11) and the anode substrate membrane (21) are both PTFE membranes.
5. A fuel cell membrane electrode with mass transfer array according to claim 3 wherein the anode catalytic layer has a platinum loading of 0.02-0.1mg/cm 2 。
6. The preparation method of the fuel cell membrane electrode is characterized by comprising the following steps of: step 1, adding a platinum carbon catalyst and an ionic resin into a mixed solvent of water and isopropanol to form cathode initial slurry, and ball-milling the cathode initial slurry for 24 hours to obtain cathode catalyst slurry; step 2, spraying cathode catalyst slurry on the front surface of a cathode substrate film (11), and then drying to obtain a cathode catalyst layer to be treated, which is attached to the cathode substrate film; and 3, punching a plurality of through holes (120) in a rectangular point array shape on the cathode catalytic layer to be treated by using a laser beam to obtain the cathode catalytic layer attached to the cathode substrate film.
7. The method for producing a fuel cell membrane electrode according to claim 6 wherein the through holes (120) have a pore diameter of 1 to 2 μm and a pore spacing between adjacent two of the through holes (120) is 7 to 13 μm.
8. The method for preparing a fuel cell membrane electrode according to claim 6 wherein said laser beam is a lattice laser beam.
9. The method for producing a fuel cell membrane electrode according to claim 6 further comprising the steps of: step 4, adding a platinum carbon catalyst and an ion resin into the mixed solvent of water and isopropanol to form anode initial slurry, and ball-milling the anode initial slurry for 24 hours to obtain anode catalyst slurry; step 5, spraying anode catalyst slurry on the front surface of the anode substrate film, and drying to obtain an anode catalyst layer attached to the anode substrate film; and 6, respectively placing the cathode catalytic layer and the anode catalytic layer on two sides of the proton membrane (3) to enable the proton membrane (3) to be clamped between the surface of the anode catalytic layer and the surface of the anode catalytic layer, carrying out hot pressing and compounding on the cathode catalytic layer and the anode catalytic layer by a hot press, and removing the substrate membranes on the two sides to obtain the membrane electrode.
10. The method for producing a fuel cell membrane electrode according to claim 6 wherein the anode catalyst layer has a platinum loading of 0.02 to 0.1mg/cm 2 。
CN202310916671.1A 2023-07-25 2023-07-25 Fuel cell membrane electrode with mass transfer array and preparation method thereof Pending CN117013023A (en)

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CN202310916671.1A CN117013023A (en) 2023-07-25 2023-07-25 Fuel cell membrane electrode with mass transfer array and preparation method thereof

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Application Number Priority Date Filing Date Title
CN202310916671.1A CN117013023A (en) 2023-07-25 2023-07-25 Fuel cell membrane electrode with mass transfer array and preparation method thereof

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CN117013023A true CN117013023A (en) 2023-11-07

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