CN111082072B - Gas diffusion layer for fuel cell and preparation method thereof - Google Patents
Gas diffusion layer for fuel cell and preparation method thereof Download PDFInfo
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- CN111082072B CN111082072B CN201911416425.XA CN201911416425A CN111082072B CN 111082072 B CN111082072 B CN 111082072B CN 201911416425 A CN201911416425 A CN 201911416425A CN 111082072 B CN111082072 B CN 111082072B
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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
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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
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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
- H01M4/8663—Selection of inactive substances as ingredients for catalytic active masses, e.g. binders, fillers
- H01M4/8673—Electrically conductive fillers
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- H—ELECTRICITY
- H01—ELECTRIC ELEMENTS
- H01M—PROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
- H01M4/00—Electrodes
- H01M4/86—Inert electrodes with catalytic activity, e.g. for fuel cells
- H01M4/88—Processes of manufacture
- H01M4/8803—Supports for the deposition of the catalytic active composition
- H01M4/8807—Gas diffusion layers
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- 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 relates to a gas diffusion layer for a fuel cell, which comprises a microporous layer taking a conductive material as a main component and a mixed substrate layer formed by sintering the conductive material and a porous carbon material, wherein the mixed substrate layer and the microporous layer respectively contain a pore structure with the pore diameter of 300-500 mu m, and the preparation method comprises the following steps: uniformly mixing a conductive material, an adhesive, carbon fibers and a pore-forming agent to obtain the conductive slurry; fixing the lower surface of the porous carbon material on a base platform through adsorption, and uniformly coating the upper surface of the porous carbon material with conductive slurry; and sintering the porous carbon material coated with the conductive paste to form the microporous layer and the mixed substrate layer. Compared with the prior art, the invention has the advantages of high material consistency, stable structure, good water transmission performance, simple preparation process and the like.
Description
Technical Field
The invention relates to the technical field of fuel cells, in particular to a gas diffusion layer for a fuel cell and a preparation method thereof.
Background
The fuel cell can convert chemical energy of fuel and oxidant into electric energy, the energy conversion efficiency is not limited by the cycle theoretical efficiency of the Carnot heat engine, and the fuel cell has the advantages of high efficiency, environmental friendliness, quietness, high reliability and the like, and has wide development prospect in various fields. The proton exchange membrane fuel cell has high power density, quick start and quick response to load change, and becomes an important development direction of energy in the field of transportation. The core component of the fuel cell is a membrane electrode material, and is formed by compounding a proton exchange membrane, a catalyst and a gas diffusion layer through a hot pressing process. The reaction gas (the anode is usually hydrogen, the cathode is air or oxygen) is guided by the guide polar plate, and then diffused to the surface of the catalyst by the gas diffusion layer to react, and the water of the reaction product passes out of the diffusion layer from the surface of the membrane electrode and is converged into the gas flow to be discharged. In the reaction process of the fuel cell, water management is an important process, which not only ensures that the proton exchange membrane contains enough water to achieve the optimal conductivity, but also requires that the water generated by the reaction can be sufficiently discharged to prevent the membrane electrode surface from flooding, so that the reaction can not be carried out, and strict requirements are designed on the structure design of gas diffusion.
The current commercial gas diffusion layer generally comprises a substrate layer and a microporous layer, and the main production processing method is to coat a microporous structure on the treated substrate layer. Considering that the microporous layer has certain fluidity during processing, the gas diffusion layer actually processed and produced has three structures: a microporous layer, a mixed layer of the microporous layer and the base layer, and a base layer. To ensure the stability of the three-layer structure, the preparation process of the microporous layer must be strictly controlled, the process is harsh, and the cost is high. Therefore, some new materials, new processes and structural designs are applied to the preparation of the gas diffusion layer.
Chinese patent CN107681164 discloses a gas diffusion layer with 1-2 layers of microporous structure, which is prepared by using porous graphite paper as a substrate layer material and coating with conductive paint. The porous graphite is obtained by adopting a laser drilling method, and the size and the spacing of the aperture are controllable. The air permeability of the graphite paper adopted by the method is far lower than that of the carbon fiber substrate. Furthermore, the microporous conductive layer is directly coated on the substrate after laser drilling, and the uniformity of the structure of the gas diffusion layer after coating is difficult to control due to the difference of the drilled areas.
Chinese patent CN109167070 discloses a fuel cell gas diffusion layer with a gradient structure and a preparation method thereof. A gradient pore structure from small to large is formed on the microporous layer, the carbon black and the carbon fiber layer in sequence on the gas diffusion layer through the doped diamond layer. Because only small pore size structures are available near the membrane electrode, the method cannot improve flooding due to the generation of large amounts of water at high current densities. In addition, to achieve the gradient structure, a chemical vapor deposition method is needed, and the cost of large-scale preparation is high.
Disclosure of Invention
The invention aims to overcome the defect that the gas diffusion layer is easy to be flooded by water in the prior art, and provides the gas diffusion layer for the fuel cell and the preparation method thereof.
The purpose of the invention can be realized by the following technical scheme:
a gas diffusion layer for a fuel cell comprises a microporous layer with a conductive material as a main component and a mixed substrate layer formed by sintering the conductive material and a porous carbon material, wherein the mixed substrate layer and the microporous layer both contain pore structures with the pore diameter of 300-500 mu m.
Based on the fundamental effect on the gas diffusion layer of the fuel cell, the newly designed structure contains a macroporous double-layer structure, so that the macroporous structure is fully distributed in the microporous layer and the mixed substrate layer, and the generated liquid water can be quickly discharged; the double-layer structure design overcomes the problem of poor consistency generated after the traditional microporous layer is coated, and simplifies the processing technology; in addition, the mixed substrate layer is composed of the microporous layer and the porous carbon material, so that the surface roughness is reduced, and the service life of the proton exchange membrane is prolonged. The invention reduces the cost of the processing technology on one hand, and can meet the requirement of water vapor transmission under high current density on the other hand.
The pore size of the mixed substrate layer and microporous layer is very important, and the gas diffusion layer provides a channel for the reaction gas and needs to be able to smoothly discharge the water from the catalyst layer to allow the gas to enter the surface of the catalyst layer for continuous reaction. 300-500um can satisfy the transmission of liquid water, which is beneficial to establish the channel of the whole process of the liquid water transmission from the catalyst layer interface to the gas diffusion layer, if the pore size of the gas diffusion layer is less than 300um, the water transmission is not beneficial, however, if the pore size is too large, the diffusion stability of the gas diffusion layer is not beneficial.
The thickness of the mixed substrate layer is 100-300 mu m; the thickness of the microporous layer is 30-110 μm, and preferably 30-80 μm.
The mixed base layer and the microporous layer have a pore structure of 300-500 mu m, and the porosity of the gas diffusion layer for the fuel cell is 50-85%.
By controlling the thickness of the microporous layer, lower contact resistance and good water vapor transmission can be ensured.
The raw material components of the conductive material are selected from one or more of acetylene black, crystalline flake graphite, flexible graphite and carbon nano tubes.
The porous carbon material is selected from carbon fiber paper or fabric.
A method for producing a gas diffusion layer for a fuel cell according to claim 1, comprising the steps of:
(1) uniformly mixing a conductive material, an adhesive and a pore-forming agent to obtain the conductive slurry;
(2) fixing the lower surface of the porous carbon material on a base platform through adsorption, and uniformly coating the conductive slurry on the upper surface of the porous carbon material;
(3) and sintering the porous carbon material coated with the conductive paste to form the microporous layer and the mixed substrate layer.
In the coating process, the adsorption strength of the conductive slurry on the porous carbon material is 10-50N/cm2。
The conductive paste comprises the following raw material components in parts by weight: 60-90 parts of conductive material, 10-40 parts of adhesive and 1-5 parts of pore-forming agent; the average particle size of the pore-forming agent is 200-600 mu m.
The pore-forming agent is one or more of ammonium chloride, ammonium bicarbonate or ammonium oxalate.
The adhesive is one or a mixture of carboxymethyl cellulose sodium or polyethylene glycol.
By optimizing the specific conductive paste composition, particularly without carbon fibers, the surface of the formed microporous layer has low roughness, which is beneficial for protecting the catalyst layer and the proton exchange membrane (CCM), and if the surface of the microporous layer is made of polymer resin, carbon fibers and conductive particles, and the microporous layer is in direct contact with the catalyst layer, the uneven carbon fibers can cause CCM perforation.
The sintering temperature is 300-800 ℃, and the sintering time is 3-8 h.
The sintering treatment makes the material complete pore forming completely, ensures the stability of the chemical structure and influences the formation of micropores by the sintering condition.
The mass ratio of the conductive slurry to the porous carbon material is 1/5-1/3, so that the diffusion layer is guaranteed to have excellent conductivity and structural strength.
The preparation process of the invention is simple, the gas diffusion layer obtained by the invention only has two-layer structure of the mixed substrate layer and the conductive microporous layer, and three structures of the microporous layer, the mixed layer of the microporous layer and the substrate layer in the prior art can not exist, because the conductive slurry can form a smooth microporous layer by controlling the viscosity of the conductive slurry and the adsorption force of the porous carbon fiber, and can ensure that the conductive slurry is uniformly distributed in the whole porous carbon material.
Through the optimization selection of the size of the pore-forming agent, after high-temperature carbonization treatment, a pore-size structure with a specific size, such as a macroporous structure of 300-.
Compared with the prior art, the invention has the following advantages:
(1) the gas diffusion layer is designed into a double-layer structure, so that the consistency of materials is improved, the preparation process is simplified, and the cost of the processing process is reduced;
(2) the result of large aperture is introduced into the microporous layer and the mixed substrate layer, so that the water vapor transmission requirement under the high-power density operation is met, and the high-power development requirement of the fuel cell is met.
Drawings
FIG. 1 is a schematic structural view of the present invention;
in the figure, 1 is a microporous layer, 2 is a mixed base layer, and 3 is a pore structure.
Detailed Description
The present invention will be described in detail with reference to specific examples. The following examples will assist those skilled in the art in further understanding the invention, but are not intended to limit the invention in any way. It should be noted that variations and modifications can be made by persons skilled in the art without departing from the spirit of the invention. All falling within the scope of the present invention.
Examples 1 to 4
A method for preparing a gas diffusion layer is provided,
1) the conductive coating is prepared by taking acetylene black as a conductive material, wherein the conductive coating comprises the following raw materials in parts by weight, wherein the total weight of solid matters in the conductive coating is 100 percent: 80 parts of conductive material, 30 parts of adhesive and 4 parts of pore-forming agent by weight, wherein the pore-forming agent is a mixture of ammonium chloride, ammonium bicarbonate and ammonium oxalate, and the average particle size of the pore-forming agent is 500 mu m; the binder is a mixture of sodium carboxymethylcellulose and polyethylene glycol.
2) Placing a porous carbon material on a base platform which has adsorption effect and can be continuously conveyed;
3) coating the conductive slurry on the non-adsorption surface of the porous carbon material, wherein the adsorption strength in the coating process is shown in table 1, the base platform rotates at a constant speed to continuously convey the coated material, and the mass ratio of the conductive slurry to the porous carbon material is 1/4;
4) the coated material was subjected to a sintering treatment for 5 hours to obtain a unified gas diffusion layer having only the mixed layer and the conductive microporous layer combined.
Specification parameters, adsorption strength and pore size distribution of the porous carbon material prepared in the preparation process of the embodiment are shown in table 1, and the prepared gas diffusion layer is shown in fig. 1 and comprises a microporous layer 1 and a mixed substrate layer 2, wherein the microporous layer 1 and the mixed substrate layer 2 both have a pore structure of 300-500 μm.
TABLE 1 Process parameters for the preparation of examples 1-4
Example 5
A method for preparing a gas diffusion layer is provided,
1) the conductive coating is prepared by taking acetylene black as a conductive material, wherein the conductive coating comprises the following raw materials in parts by weight, wherein the total weight of solid matters in the conductive coating is 100 percent: 60 percent of conductive material, 10 percent of adhesive and 1 percent of pore-forming agent by weight; the pore-forming agent is ammonium chloride, the average particle size of the pore-forming agent is 200 mu m, and the binder is sodium hydroxymethyl cellulose.
2) Placing a porous carbon material with the thickness of 100 mu m on a base station which has adsorption effect and can continuously convey;
3) the conductive slurry is coated on the non-adsorption surface of the porous carbon material, and the adsorption strength in the coating process is 30N/cm2The base station rotates at a constant speed to continuously convey the coated material, and the mass ratio of the conductive paste to the porous carbon material is 1/3;
4) the coated material was subjected to a sintering treatment at 300 ℃ for 8 hours to obtain a unified gas diffusion layer having only the mixed layer and the conductive microporous layer combined.
Example 6
A method for preparing a gas diffusion layer is provided,
1) the conductive coating is prepared by taking acetylene black as a conductive material, wherein the conductive coating comprises the following raw materials in parts by weight, wherein the total weight of solid matters in the conductive coating is 100 percent: the conductive material 90, the adhesive 40, the carbon fiber 20 and the pore-forming agent 5 wt%, wherein the pore-forming agent is ammonium bicarbonate, and the average particle size of the pore-forming agent is 600 mu m; the binder is polyethylene glycol.
2) Placing a porous carbon material with the thickness of 300 mu m on a base station which has adsorption effect and can continuously convey;
3) the conductive slurry is coated on the non-adsorption surface of the porous carbon material, and the adsorption strength in the coating process is 30N/cm2The base station rotates at a constant speed to continuously convey the coated material, and the mass ratio of the conductive paste to the porous carbon material is 1/5;
4) the coated material was subjected to a sintering treatment at 800 ℃ for 3 hours to obtain a unified gas diffusion layer having only the mixed layer and the conductive microporous layer combined.
The foregoing description of specific embodiments of the present invention has been presented. It is to be understood that the present invention is not limited to the specific embodiments described above, and that various changes and modifications may be made by one skilled in the art within the scope of the appended claims without departing from the spirit of the invention.
Claims (9)
1. A gas diffusion layer for a fuel cell is characterized by comprising a microporous layer taking a conductive material as a main component and a mixed substrate layer formed by sintering the conductive material and a porous carbon material, wherein the mixed substrate layer and the microporous layer both internally contain a pore structure with the pore diameter of 300-500 mu m;
the gas diffusion layer is prepared by the following method:
(1) uniformly mixing a conductive material, an adhesive and a pore-forming agent to obtain conductive slurry; the adsorption strength of the conductive slurry on the upper surface of the porous carbon material is 10-50N/cm2；
The conductive paste comprises the following raw material components in parts by weight: 60-90 parts of conductive material, 10-40 parts of adhesive and 1-5 parts of pore-forming agent; the raw material components of the conductive material are selected from one or more of acetylene black, crystalline flake graphite, flexible graphite or carbon nano tubes; the pore-forming agent is one or more of ammonium chloride, ammonium bicarbonate or ammonium oxalate;
the adhesive is one or a mixture of carboxymethyl cellulose sodium or polyethylene glycol;
(2) fixing the lower surface of the porous carbon material on a base platform through adsorption, and uniformly coating the upper surface of the porous carbon material with conductive slurry;
(3) and sintering the porous carbon material coated with the conductive paste to form the microporous layer and the mixed substrate layer.
2. The gas diffusion layer for a fuel cell according to claim 1, wherein the thickness of the mixture base layer is 100 to 300 μm; the thickness of the microporous layer is 30-110 μm.
3. The gas diffusion layer for a fuel cell according to claim 1, wherein the mixture base layer and the microporous layer have a structure having a pore size of 300 to 500 μm, and the gas diffusion layer for a fuel cell has a porosity of 50 to 85%.
4. The gas diffusion layer for a fuel cell according to claim 1, wherein the porous carbon material is selected from carbon fiber paper or fabric.
5. A method for producing a gas diffusion layer for a fuel cell according to claim 1, comprising the steps of:
(1) uniformly mixing a conductive material, an adhesive and a pore-forming agent to obtain the conductive slurry;
(2) fixing the lower surface of the porous carbon material on a base platform through adsorption, and uniformly coating the upper surface of the porous carbon material with conductive slurry;
(3) and sintering the porous carbon material coated with the conductive paste to form the microporous layer and the mixed substrate layer.
6. The gas diffusion layer for a fuel cell according to claim 5, wherein the adsorption strength of the conductive paste on the upper surface of the porous carbon material in the coating process is 10 to 50N/cm2。
7. The gas diffusion layer for a fuel cell according to claim 5, wherein the pore-forming agent has an average particle diameter of 200 to 600 μm.
8. The gas diffusion layer for a fuel cell according to claim 5, wherein the sintering temperature is 300 to 800 ℃ and the sintering time is 3 to 8 hours.
9. The gas diffusion layer for a fuel cell according to claim 5, wherein a mass ratio of the conductive paste to the porous carbon material is 1/5 to 1/3.
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| CN112072119B (en) * | 2020-08-06 | 2022-06-21 | 江苏大学 | Fuel cell gas diffusion layer structure and processing method thereof |
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