CN113948715A - Fuel cell gas diffusion layer and preparation method and application thereof - Google Patents

Fuel cell gas diffusion layer and preparation method and application thereof Download PDF

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CN113948715A
CN113948715A CN202111196304.6A CN202111196304A CN113948715A CN 113948715 A CN113948715 A CN 113948715A CN 202111196304 A CN202111196304 A CN 202111196304A CN 113948715 A CN113948715 A CN 113948715A
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layer
gas diffusion
diffusion layer
fuel cell
graphene
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马千里
曹婷婷
米新艳
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FAW Jiefang Automotive Co Ltd
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FAW Jiefang Automotive Co Ltd
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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
    • H01M4/8605—Porous electrodes
    • B—PERFORMING OPERATIONS; TRANSPORTING
    • B60—VEHICLES IN GENERAL
    • B60L—PROPULSION OF ELECTRICALLY-PROPELLED VEHICLES; SUPPLYING ELECTRIC POWER FOR AUXILIARY EQUIPMENT OF ELECTRICALLY-PROPELLED VEHICLES; ELECTRODYNAMIC BRAKE SYSTEMS FOR VEHICLES IN GENERAL; MAGNETIC SUSPENSION OR LEVITATION FOR VEHICLES; MONITORING OPERATING VARIABLES OF ELECTRICALLY-PROPELLED VEHICLES; ELECTRIC SAFETY DEVICES FOR ELECTRICALLY-PROPELLED VEHICLES
    • B60L50/00—Electric propulsion with power supplied within the vehicle
    • B60L50/50—Electric propulsion with power supplied within the vehicle using propulsion power supplied by batteries or fuel cells
    • B60L50/70—Electric propulsion with power supplied within the vehicle using propulsion power supplied by batteries or fuel cells using power supplied by 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
    • H01M4/8647—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]
    • H—ELECTRICITY
    • H01—ELECTRIC ELEMENTS
    • H01M—PROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
    • H01M2250/00—Fuel cells for particular applications; Specific features of fuel cell system
    • H01M2250/20—Fuel cells in motive systems, e.g. vehicle, ship, plane
    • 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
    • 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
    • Y02T—CLIMATE CHANGE MITIGATION TECHNOLOGIES RELATED TO TRANSPORTATION
    • Y02T90/00—Enabling technologies or technologies with a potential or indirect contribution to GHG emissions mitigation
    • Y02T90/40—Application of hydrogen technology to transportation, e.g. using fuel cells

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  • Engineering & Computer Science (AREA)
  • Chemical & Material Sciences (AREA)
  • General Chemical & Material Sciences (AREA)
  • Electrochemistry (AREA)
  • Chemical Kinetics & Catalysis (AREA)
  • Sustainable Energy (AREA)
  • Life Sciences & Earth Sciences (AREA)
  • Sustainable Development (AREA)
  • Manufacturing & Machinery (AREA)
  • Mechanical Engineering (AREA)
  • Transportation (AREA)
  • Power Engineering (AREA)
  • Composite Materials (AREA)
  • Fuel Cell (AREA)

Abstract

The invention provides a gas diffusion layer of a fuel cell, which comprises a substrate layer and a microporous layer positioned on the surface of the substrate layer; the raw materials of the microporous layer include an organosiloxane and graphene. The use of the microporous layer in a gas diffusion layer of the present invention can improve the roughness and contact angle of the gas diffusion layer, thereby improving the hydrophobic property of the gas diffusion layer, and the use of the gas diffusion layer in a proton exchange membrane fuel cell can also improve the electrochemical performance of the fuel cell.

Description

Fuel cell gas diffusion layer and preparation method and application thereof
Technical Field
The invention relates to the field of fuel cells, in particular to a gas diffusion layer of a fuel cell and a preparation method and application thereof.
Background
A Proton Exchange Membrane Fuel Cell (PEMFC) is a low temperature fuel cell that uses a proton exchange membrane as an electrolyte, Pt/C as a catalyst, hydrogen as a fuel, and air or pure oxygen as an oxidant. Considering that environmental pollution and energy problems are now serious, PEMFC has the advantages of higher power density and environmental friendliness, making it promising to replace fossil fuels as an energy resource applied to automatic, stationary and portable devices. A Membrane Electrode Assembly (MEA) is a vital part of a proton exchange membrane fuel cell system and includes a proton exchange membrane, a catalytic layer, and a Gas Diffusion Layer (GDL).
CN108878922A discloses a fuel cell thin-layer graphene gas diffusion layer and a preparation method thereof. Graphene is dispersed in the ultra-high molecular weight polyethylene formed by the ethylene monomer, so that the graphene can be preferably dispersed in the ultra-high molecular weight polyethylene. The obtained base material has high strength, and can realize ultra-thinness so as to reduce the thickness of the base material of the gas diffusion layer. Ensures good strength and durability of the base material after thinning.
CN112724724A discloses a fuel cell membrane electrode gas diffusion layer, a preparation method and application of a microporous layer thereof. Active monomers are used as curing agents, the active monomers form organic polymers under the action of photoinitiators, organic siloxane and carbon materials are uniformly cured on the outer surface of the supporting layer, an ultraviolet light curing process is adopted, the whole reaction process is complex, the requirement of initiation reaction on the environment is high, and the process cost is high.
CN113113617A discloses a membrane electrode, a fuel cell gas diffusion layer and a preparation method thereof, wherein hydrophobic carbon paper is subjected to vacuum pre-permeation microporous layer slurry treatment before the coating of a micro-pricked layer polymer material, the microporous layer slurry is permeated into the hydrophobic carbon paper layer by overcoming capillary pressure through vacuum adsorption force, then part of carbon powder is filled in macropores on the surface of the hydrophobic carbon paper, and the change caused by the pre-permeation treatment is beneficial to forming a good contact interface between the subsequent coating microporous layer slurry and the carbon paper layer, so that the contact area between the subsequent coating microporous layer slurry and the carbon paper layer is increased. The increase of the contact area can also ensure that the microporous layer and the hydrophobic carbon paper layer are more firmly attached, thereby being beneficial to improving the water-vapor scouring resistance of the microporous layer and the durability of the gas diffusion layer. But does not improve the hydrophobicity of the gas diffusion layer of the fuel cell.
How to prepare a hydrophobic fuel cell gas diffusion layer on a large scale at low cost is an important research direction for fuel cells.
Disclosure of Invention
In view of the defects in the prior art, the invention aims to provide a gas diffusion layer of a fuel cell, a preparation method and an application thereof, wherein the preparation method can improve the hydrophobic property of the gas diffusion layer, and the electrochemical property of the fuel cell can be improved by using the gas diffusion layer in a proton exchange membrane fuel cell.
In order to achieve the purpose, the invention adopts the following technical scheme:
one of the objects of the present invention is to provide a gas diffusion layer for a fuel cell, which comprises a substrate layer and a microporous layer on the surface of the substrate layer.
The raw materials of the microporous layer include an organosiloxane and graphene.
The organic siloxane in the invention is decomposed into substances with smaller molecular weight under the heat treatment condition, so that the surface tension of the microporous layer is reduced, and the organic siloxane and the graphene form a micro-nano structure, and the micro-nano structure has a layered structure, and can improve the roughness and the contact angle of a gas diffusion layer when being used in the gas diffusion layer, so that the hydrophobic property of the gas diffusion layer is improved; the gas diffusion layer used for the proton exchange membrane fuel cell can improve the electrochemical performance of the fuel cell, so that the gas diffusion layer can be applied to a fuel cell automobile.
In a preferred embodiment of the present invention, the substrate layer is a carbon paper layer.
Preferably, the organosiloxane comprises polymethylsiloxane.
Preferably, the raw material of the microporous layer further includes an organic solvent.
Preferably, the organic solvent comprises tetrahydrofuran.
According to the preferable technical scheme of the invention, the microporous layer comprises the following raw materials in percentage by mass: 3-10% of organic siloxane, 3-15% of graphene and 75-94% of organic solvent.
The mass fraction of the organosiloxane may be 3%, 4%, 5%, 6%, 7%, 8%, 9%, 10%, etc., the mass fraction of the graphene may be 3%, 4%, 5%, 6%, 7%, 8%, 9%, 10%, 11%, 12%, 13%, 14%, 15%, etc., and the mass fraction of the organic solvent may be 75%, 76%, 77%, 78%, 79%, 80%, 81%, 82%, 83%, 84%, 85%, 86%, 87%, 88%, 89%, 90%, 91%, 92%, 93%, 94%, etc., but is not limited to the recited values, and other values not recited in the above numerical ranges are also applicable.
Preferably, the microporous layer is prepared from the following raw materials in percentage by mass: 5-8% of organic siloxane, 5-13% of graphene and 79-90% of organic solvent.
A second object of the present invention is to provide a method for preparing a gas diffusion layer according to the first object, the method comprising the steps of:
(1) mixing organic siloxane, graphene and an organic solvent to obtain a precursor of the microporous layer;
(2) and coating the precursor of the microporous layer on one side of the substrate layer, and curing to obtain the gas diffusion layer.
As a preferable technical scheme of the invention, the mixing mode in the step (1) is ultrasonic mixing.
Preferably, the ultrasonic mixing frequency is 80 to 120kHz, wherein the frequency can be 80kHz, 85kHz, 90kHz, 95kHz, 100kHz, 105kHz, 110kHz, 115kHz or 120kHz, and the like, but the ultrasonic mixing frequency is not limited to the enumerated values, and other non-enumerated values in the numerical range are also applicable, and the ultrasonic mixing frequency is more preferably 90 to 110 kHz.
Preferably, the power density of the ultrasonic mixing is 1.5-3.5W/cm2Wherein the power density may be 1.5W/cm2、2W/cm2、2.5W/cm2、3W/cm2Or 3.5W/cm2And the like, but not limited to the recited values, and other values not recited in the above numerical range are also applicable, and more preferably 2 to 3W/cm2；
Preferably, the ultrasonic mixing time is 20-75 min, wherein the time can be 20min, 25min, 30min, 35min, 40min, 45min, 50min, 55min, 60min, 65min, 70min or 75min, but is not limited to the recited values, and other non-recited values in the value range are also applicable, and more preferably 40-60 min.
As a preferred technical scheme of the invention, the coating mode of the step (2) is blade coating and/or spraying.
In a preferred embodiment of the present invention, the curing temperature in the step (2) is 130 to 220 ℃, and the temperature may be 130 ℃, 140 ℃, 150 ℃, 160 ℃, 170 ℃, 180 ℃, 190 ℃, 200 ℃, 210 ℃ or 220 ℃, but is not limited to the above-mentioned values, and other values not shown in the above-mentioned value range are also applicable, and more preferably 150 to 200 ℃.
Preferably, the curing time is 10 to 80min, and the curing time may be 10min, 15min, 20min, 25min, 30min, 35min, 40min, 45min, 50min, 55min, 60min, 65min, 70min, 75min, or 80min, but is not limited to the enumerated values, and other non-enumerated values within the numerical range are also applicable, and more preferably 30 to 60 min.
As a preferred technical scheme of the invention, the preparation method comprises the following steps:
(1) organic siloxane, graphene and an organic solvent are subjected to frequency of 80-120 kHz and power density of 1.5-3.5W/cm2Ultrasonic mixing for 20-75 min to obtain a precursor of the microporous layer;
(2) and coating the precursor of the microporous layer on one side of the support layer, and curing at the temperature of 130-220 ℃ for 10-80 min to obtain the gas diffusion layer.
It is a further object of the present invention to provide a proton exchange membrane fuel cell including the gas diffusion layer according to one of the objects.
Preferably, the fuel cell further comprises a proton membrane exchange layer and a catalytic layer.
The fourth purpose of the invention is to provide an application of the gas diffusion layer of the fuel cell of the third purpose, and the proton exchange membrane fuel cell is applied to the field of fuel cell automobiles.
The recitation of numerical ranges herein includes not only the above-recited numerical values, but also any numerical values between non-recited numerical ranges, and is not intended to be exhaustive or to limit the invention to the precise numerical values encompassed within the range for brevity and clarity.
Compared with the prior art, the invention has at least the following beneficial effects:
the microporous layer comprises organic siloxane and graphene, the organic siloxane is decomposed into substances with smaller molecular weight under the heat treatment condition, so that the surface tension of the microporous layer is reduced, and the microporous layer and the graphene form a micro-nano structure; the gas diffusion layer used for the proton exchange membrane fuel cell can improve the electrochemical performance of the fuel cell, so that the gas diffusion layer can be applied to a fuel cell automobile.
The microporous layer used for the gas diffusion layer can improve the roughness and the contact angle of the gas diffusion layer, wherein the contact angle can reach 170 ℃, so that the hydrophobic property of the gas diffusion layer is improved, and the electrochemical property of the fuel cell can be improved when the gas diffusion layer is used for a proton exchange membrane fuel cell.
Detailed Description
The technical solution of the present invention is further explained by the following embodiments.
Example 1
This example provides a method for preparing a gas diffusion layer:
6.5g of polymethylsiloxane and 9g of graphene are added to 84.5g of tetrahydrofuran, mechanically stirred at a frequency of 100kHz and a power density of 2.5W/cm2The ultrasonic mixing is carried out for 50min to form uniform suspension, then the suspension is coated on the surface of one side of the carbon paper subjected to hydrophobic treatment until the loading amount of the carbon material is 1mg/cm2, the suspension is naturally dried, and the suspension is placed in a drying box and sintered for 10min at 180 ℃ to obtain the gas diffusion layer.
Example 2
This example provides a method for preparing a gas diffusion layer:
adding 3g of polymethylsiloxane and 3g of graphene into 94g of tetrahydrofuran, and mechanically stirring at a frequency of 80kHz and a power density of 1.5W/cm2Ultrasonic mixing for 75min to form uniform suspension, and then coating the suspension on one side surface of the hydrophobic carbon paper until the loading amount of the carbon material is 1mg/cm2Naturally drying, placing in a drying oven at 150 deg.CAnd sintering for 30min to obtain the gas diffusion layer.
Example 3
This example provides a method for preparing a gas diffusion layer:
adding 10g of polymethylsiloxane and 15g of graphene into 75g of tetrahydrofuran, and mechanically stirring at a frequency of 120kHz and a power density of 3.5W/cm2Ultrasonic mixing for 40min to form uniform suspension, and then coating the suspension on one side surface of the hydrophobic carbon paper until the loading amount of the carbon material is 1mg/cm2And naturally drying, placing in a drying oven, and sintering at 130 ℃ for 80min to obtain the gas diffusion layer.
Example 4
This example provides a method for preparing a gas diffusion layer:
adding 8g of polymethylsiloxane and 13g of graphene into 79g of tetrahydrofuran, and mechanically stirring at a frequency of 110kHz and a power density of 3W/cm2The mixture is ultrasonically mixed for 20min to form uniform suspension, and then the suspension is blade-coated on one side surface of the hydrophobic carbon paper until the loading amount of the carbon material is 1mg/cm2And naturally drying, placing in a drying oven, and sintering at 200 ℃ for 60min to obtain the gas diffusion layer.
Example 5
This example provides a method for preparing a gas diffusion layer:
adding 5g of polymethylsiloxane and 5g of graphene into 90g of tetrahydrofuran, and mechanically stirring at a frequency of 90kHz and a power density of 2W/cm2The mixture is ultrasonically mixed for 60min to form uniform suspension, and then the suspension is blade-coated on one side surface of the carbon paper subjected to hydrophobic treatment until the loading amount of the carbon material is 1mg/cm2And naturally drying, placing in a drying oven, and sintering at 220 ℃ for 45min to obtain the gas diffusion layer.
Example 6
In this example, the polymethylsiloxane was replaced with polydimethylsiloxane under the same conditions as in example 1.
Example 7
This example replaces the polymethylsiloxane with a, w-dihydroxypolysiloxane, all other conditions being the same as in example 1.
Comparative example 1
This comparative example was carried out under the same conditions as in example 1 except that graphene was replaced with activated carbon black.
Comparative example 2
The comparative example replaced graphene with acetylene black, and the other conditions were the same as in example 1.
Comparative example 3
In the comparative example, graphene was replaced with graphite powder, and the other conditions were the same as in example 1.
Comparative example 4
In the comparative example, graphene was replaced with carbon nanotubes, and the other conditions were the same as in example 1.
Examples 1 to 7 and comparative examples 1 to 4 were subjected to contact angle tests using a DSA25 type contact angle tester. The test results are shown in table 1.
TABLE 1
Figure BDA0003303165140000071
Figure BDA0003303165140000081
From the above results, it can be seen that the organic siloxane used in the present invention can achieve the best contact angle when the polymethyl siloxane is replaced with other organic siloxane in examples 1 to 5 compared to examples 6 and 7, and the contact angle is measured. In example 1, compared to comparative examples 1 to 4, the effect achieved by graphene was the best when graphene was replaced with another carbon nanomaterial.
The above-mentioned embodiments are intended to illustrate the objects, technical solutions and advantages of the present invention in further detail, and it should be understood that the above-mentioned embodiments are only exemplary embodiments of the present invention, and are not intended to limit the present invention, and any modifications, equivalents, improvements and the like made within the spirit and principle of the present invention should be included in the protection scope of the present invention.

Claims (10)

1. A gas diffusion layer of a fuel cell, comprising a substrate layer and a microporous layer on the surface of the substrate layer;
the raw materials of the microporous layer include an organosiloxane and graphene.
2. The gas diffusion layer of claim 1, wherein the substrate layer is a carbon paper layer;
preferably, the organosiloxane comprises polymethylsiloxane;
preferably, the raw material of the microporous layer further includes an organic solvent;
preferably, the organic solvent comprises tetrahydrofuran.
3. The gas diffusion layer according to claim 1 or 2, wherein the microporous layer is prepared from the following raw materials in mass fraction: 3-10% of organic siloxane, 3-15% of graphene and 75-94% of organic solvent;
preferably, the microporous layer is prepared from the following raw materials in percentage by mass: 5-8% of organic siloxane, 5-13% of graphene and 79-90% of organic solvent.
4. A method for preparing a gas diffusion layer according to any of claims 1 to 3, comprising the steps of:
(1) mixing organic siloxane, graphene and an organic solvent to obtain a precursor of the microporous layer;
(2) and coating the precursor of the microporous layer on one side of the substrate layer, and curing to obtain the gas diffusion layer.
5. The method according to claim 4, wherein the mixing in step (1) is carried out by ultrasonic mixing;
preferably, the frequency of the ultrasonic mixing is 80-120 kHz, and further preferably 90-110 kHz;
preferably, the power density of the ultrasonic mixing is 1.5-3.5W/cm2More preferably 2 to 3W/cm2；
Preferably, the ultrasonic mixing time is 20-75 min, and more preferably 40-60 min.
6. The method according to claim 4 or 5, wherein the coating in step (2) is knife coating and/or spray coating.
7. The method according to any one of claims 4 to 6, wherein the curing temperature in step (2) is 130 to 220 ℃, and more preferably 150 to 200 ℃;
preferably, the curing time is 10-80 min, and more preferably 30-60 min.
8. The method of any one of claims 4 to 7, comprising the steps of:
(1) organic siloxane, graphene and an organic solvent are subjected to frequency of 80-120 kHz and power density of 1.5-3.5W/cm2Ultrasonic mixing for 20-75 min to obtain a precursor of the microporous layer;
(2) and coating the precursor of the microporous layer on one side of the support layer, and curing at the temperature of 130-220 ℃ for 10-80 min to obtain the gas diffusion layer.
9. A proton exchange membrane fuel cell comprising a gas diffusion layer according to any one of claims 1 to 3;
preferably, the fuel cell further comprises a proton membrane exchange layer and a catalytic layer.
10. Use of a pem fuel cell according to claim 9 in the fuel cell automotive field.
CN202111196304.6A 2021-10-14 2021-10-14 Fuel cell gas diffusion layer and preparation method and application thereof Pending CN113948715A (en)

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CN117276576A (en) * 2023-10-20 2023-12-22 苏州大学 Microporous layer of proton exchange membrane fuel cell and preparation method and application thereof

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