CN110676468A - Method for processing hydrophobic property of cathode gas diffusion layer material in proton exchange membrane fuel cell - Google Patents
Method for processing hydrophobic property of cathode gas diffusion layer material in proton exchange membrane fuel cell Download PDFInfo
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- CN110676468A CN110676468A CN201910811774.5A CN201910811774A CN110676468A CN 110676468 A CN110676468 A CN 110676468A CN 201910811774 A CN201910811774 A CN 201910811774A CN 110676468 A CN110676468 A CN 110676468A
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- H—ELECTRICITY
- H01—ELECTRIC ELEMENTS
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- H01M4/00—Electrodes
- H01M4/86—Inert electrodes with catalytic activity, e.g. for fuel cells
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- H—ELECTRICITY
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- H01M4/86—Inert electrodes with catalytic activity, e.g. for fuel cells
- H01M2004/8678—Inert electrodes with catalytic activity, e.g. for fuel cells characterised by the polarity
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Abstract
The invention discloses a method for processing the hydrophobic property of a cathode gas diffusion layer material in a proton exchange membrane fuel cell. The solid part of the polar plate connected with the gas diffusion layer is a ridge, the area between the two ridges is a flow channel, the material of the cathode gas diffusion layer adopts carbon paper, and the specific processing method mainly comprises the following steps: cleaning, removing dust, drying, soaking the carbon paper in a diluted polytetrafluoroethylene suspension, washing a specific area to remove a solution, drying again and the like. The treatment method only performs hydrophobic property treatment on the cathode gas diffusion layer under the flow channel and under the ridge. The invention can realize the macroscopic regulation and control of the water transmission behavior in the cathode gas diffusion layer, promote the water generated by the catalyst layer to be discharged in time and effectively slow down the flooding phenomenon; on the other hand, according to different drying requirements below the ridge and the flow channel, the capability of transmitting the reaction gas of the cathode gas diffusion layer below the ridge or the flow channel can be directionally improved, so that the performance of the battery is improved.
Description
Technical Field
The invention belongs to the field of electrochemical fuel cells, and particularly relates to a method for controlling hydrophobic property of a gas diffusion layer in a proton exchange membrane fuel cell.
Background
A Proton Exchange Membrane Fuel Cell (PEMFC) is an electrochemical reaction power device capable of directly converting chemical energy in fuel into electric energy, has advantages of high power density and only water discharge, and is considered as one of the devices most likely to replace automobile power in the future. There is still a great room for improving the performance and life of the current pem fuel cell, wherein the water management and the quality of the reactant gas transport are key factors affecting the performance.
Excessive liquid water transport through the porous media in the Catalytic Layer (CL) and the Gas Diffusion Layer (GDL) may hinder the transport of the reaction gas (resulting in flooding), which is considered as one of the major factors hindering the improvement of the limiting current performance of the cell. In order to improve the water drainage capability of the gas diffusion layer, the gas diffusion layer (typically a carbon paper or a carbon cloth) is usually required to be subjected to a hydrophobic treatment with Polytetrafluoroethylene (PTFE). Most of the existing treatment technologies are to directly immerse carbon paper or carbon cloth in a cathode gas diffusion layer into a PTFE solution for hydrophobic treatment, and the method has the defects that the PTFE on the surface of carbon fibers in the carbon paper is uniformly distributed, and the transmission path of product water of a cathode catalyst layer is random and unpredictable in the process of discharging the product water out of a battery through the carbon paper, so that liquid water can spread and block a main channel for reaction gas to enter the catalyst layer, the electrochemical reaction strength is weakened, and the battery performance is reduced.
According to the invention, the cathode gas diffusion layer is subjected to non-uniform PTFE treatment, and parts of the gas diffusion layer corresponding to the part under the ridge and the part under the flow channel are subjected to hydrophobic treatment in different degrees, so that the effective path control of the movement of the product water of the cathode catalyst layer in the carbon paper can be realized, the possibility of random spread of the product water is reduced, the problem that the main transmission channel of the reaction gas is blocked by liquid water is effectively relieved, and the efficient and stable operation of the battery is ensured.
Disclosure of Invention
The invention aims to provide a method for processing the hydrophobic property of a cathode gas diffusion layer material in a proton exchange membrane fuel cell.
The technical scheme of the invention is as follows: the proton exchange membrane fuel cell is divided into a cathode plate, a cathode gas diffusion layer, a cathode catalyst layer, an electrolyte layer, an anode catalyst layer, an anode diffusion layer and an anode plate from top to bottom. The cathode plate and the anode plate are both in a flow channel-ridge structure, wherein the area between the two ridges is a flow channel. The cathode gas diffusion layer is made of carbon paper or carbon cloth, and the specific method for processing the hydrophobic property of the cathode gas diffusion layer material is as follows:
(1) cutting the carbon paper into squares with the area of 5cm multiplied by 5cm, putting the squares into a beaker filled with acetone solution, and putting the beaker into an ultrasonic oscillator to clean and remove dust;
(2) and taking out the carbon paper, cleaning the carbon paper again by using clean acetone, putting the cleaned carbon paper into a drying box, adjusting the temperature to 80-100 ℃ for drying, and weighing the dried carbon paper.
(3) The PTFE suspension was diluted with distilled water to a target concentration of 2 wt%.
(4) And slowly putting the carbon paper into the diluted PTFE solution, and then putting the carbon paper into an ultrasonic vibrator to enable the PTFE solution to be fully immersed into the carbon paper.
(5) Taking out the carbon paper, and marking a region mark on the carbon paper, wherein the area of the mark is as follows: the length is 5cm, the width is 1mm, the marked area is washed by a water gun with the pressure of 0.5MPa, and the PTFE solution in the area is removed.
(6) The carbon paper was dried at 80 to 100 c, and the carbon paper containing PTFE after drying was weighed, thereby calculating the content of PTFE added.
(7) And repeating the steps 4-6 until the content of the PTFE in the carbon paper reaches the target value concentration.
(8) The carbon paper is put into an oven at 150 ℃, the temperature is gradually increased to 270 ℃, the temperature is maintained for 10 minutes, the organic components in the carbon paper and PTFE are removed, then the temperature of the oven is increased to 320-350 ℃, and the carbon paper is sintered for half an hour.
(9) And reducing the temperature of the oven to 150 ℃, maintaining for half an hour, taking out, finishing the hydrophobic property treatment of the carbon paper, and taking the carbon paper as a cathode gas diffusion layer.
The cathode catalyst layer generates electrochemical reaction to generate water, and the water generated from the catalyst layer needs to flow through the cathode gas diffusion layer to reach the flow channel so as to be discharged out of the cell along with the gas flow. The drainage performance of the carbon paper can be improved by performing a regionalized hydrophobic performance treatment on the cathode gas diffusion layer. The conventional treatment process is to perform uniform PTFE treatment on the cathode gas diffusion layer, so that there is no difference in surface hydrophobicity of the cathode gas diffusion layer and no directionality in water flow. The proposal provides that the cathode gas diffusion layer is subjected to non-uniform treatment, so that the function of regulating and controlling the water transmission in the cathode gas diffusion layer can be realized. The performance of the proton exchange membrane fuel cell is improved by controlling the transmission and the characteristic distribution of water.
The invention has the advantages and innovations that:
on one hand, the macroscopic regulation and control of the water transmission behavior in the cathode gas diffusion layer can be realized, so that the water generated by the cathode catalyst layer is promoted to be discharged out of the cell in time, and the cathode flooding phenomenon of the proton exchange membrane fuel cell is effectively relieved; on the other hand, according to different drying requirements below the ridge and the flow channel, the capability of transmitting the reaction gas of the cathode gas diffusion layer below the ridge or the flow channel can be directionally improved, so that the performance of the battery is improved.
Drawings
FIG. 1 is a schematic diagram of a proton exchange membrane fuel cell.
Wherein: 1-cathode plate, 2-cathode gas diffusion layer, 3-cathode catalyst layer, 4-proton exchange membrane, 5-anode catalyst layer, 6-anode gas diffusion layer and 7-anode plate.
Fig. 2 is a schematic view of a conventional cathode gas diffusion layer with a uniform surface hydrophobicity.
Figure 3 is a schematic view of a cathode gas diffusion layer treated to have a specific area of non-uniform surface hydrophobicity.
Fig. 4 shows the drainage capacity and water distribution of the cathode gas diffusion layer after the conventional PTFE treatment of the cell of example 1.
Fig. 5 is a comparison of water drainage capacity and water distribution after hydrophobic property treatment of the cathode gas diffusion layer under the flow channel in example 2.
Fig. 6 is a comparison of water drainage and water distribution after hydrophobic property treatment of the under-ridge cathode gas diffusion layer of example 3.
Detailed Description
The technical solution of the present invention is described in detail below with reference to the accompanying drawings and specific embodiments. It should be noted that the present embodiments are illustrative rather than limiting and do not limit the scope of the invention.
The specific method for processing the hydrophobic property of the cathode gas diffusion layer material is as follows:
(1) cutting the carbon paper into squares with the area of 5cm multiplied by 5cm, putting the squares into a beaker filled with acetone solution, and putting the beaker into an ultrasonic oscillator to clean and remove dust;
the method aims to remove dust accumulated on the surface of carbon fibers in the carbon paper after being exposed in the air for a long time, and the ultrasonic oscillation is favorable for enhancing the dust removal capacity of the solution, and particularly has stronger dust adhesion capacity for porous materials.
(2) And taking out the carbon paper, cleaning the carbon paper again by using clean acetone, putting the cleaned carbon paper into a drying box, adjusting the temperature to 80-100 ℃ for drying, and weighing the dried carbon paper.
(3) The PTFE suspension was diluted with distilled water to a target concentration of 2 wt%.
(4) And slowly putting the carbon paper into the diluted PTFE solution, and then putting the carbon paper into an ultrasonic vibrator to enable the PTFE solution to be fully immersed into the carbon paper.
(5) Taking out the carbon paper, and marking a region mark on the carbon paper, wherein the area of the mark is as follows: the length is 5cm, the width is 1mm, the marked area is washed by a water gun with the pressure of 0.5MPa, and the PTFE solution in the area is removed.
(6) The carbon paper was dried at 80 to 100 c, and the carbon paper containing PTFE after drying was weighed, thereby calculating the content of PTFE added.
(7) And repeating the steps 4-6 until the content of the PTFE in the carbon paper reaches the target value concentration.
(8) The carbon paper is put into an oven at 150 ℃, the temperature is gradually increased to 270 ℃, the temperature is maintained for 10 minutes, the organic components in the carbon paper and PTFE are removed, then the temperature of the oven is increased to 320-350 ℃, and the carbon paper is sintered for half an hour.
(9) And reducing the temperature of the oven to 150 ℃, maintaining for half an hour, taking out, finishing the hydrophobic property treatment of the carbon paper, and taking the carbon paper as a cathode gas diffusion layer.
The method for processing the hydrophobic property of the cathode gas diffusion layer material comprises two processing schemes of: firstly, only the cathode gas diffusion layer below the flow channel is subjected to hydrophobic property treatment, and the corresponding cathode gas diffusion layer below the ridge still keeps weak hydrophobicity; and secondly, only the cathode gas diffusion layer under the ridge is subjected to hydrophobic property treatment, and the cathode gas diffusion layer under the flow channel still keeps weak hydrophobicity.
The carbon paper is a porous material, and the carbon paper can also be carbon cloth. The imprinted area marked on the carbon paper, as a special area for treating the hydrophobicity of the cathode gas diffusion layer, causes the distribution of the hydrophobic properties inside the cathode gas diffusion layer to exhibit differences.
After the special area of the cathode gas diffusion layer is subjected to hydrophobic treatment, the drainage capacity of the special area inside the cathode gas diffusion layer is enhanced, and the water inside the cathode gas diffusion layer can be directionally transported.
The cathode catalyst layer generates electrochemical reaction to generate water, and the water generated from the catalyst layer needs to flow through the cathode gas diffusion layer to reach the flow channel so as to be discharged out of the cell along with the gas flow. The conventional treatment process is a PTFE treatment that homogenizes the cathode gas diffusion layer (see fig. 2). The cathode gas diffusion layer material treated in this way will exhibit relatively uniform hydrophobic characteristics.
The porosity of the cathode gas diffusion layer material before PTFE treatment is typically above 0.7, and after hydrophobic property treatment, the porosity of the material decreases. Since only a specific region of the cathode gdl material is treated and the original porosity is maintained in the non-PTFE treated portion or region, the hydrophobicity and porosity distribution within the new cathode gdl will vary. This results in directional water transport within the cathode gas diffusion layer, which has superior drainage properties over cathode gas diffusion layers having a uniform distribution of hydrophobicity and porosity.
The experiment was carried out using three cells. The three batteries are different in the processing mode of cathode gas diffusion layer PTFE, and the adopted structures and materials are the same. The width of the flow channel was 500 μm, the width of the ridge was 250 μm, and the length of the flow channel was 200 μm. The cathode gas diffusion layer had a thickness of 200 μm, a porosity of 0.7 and a fiber diameter of 8 μm. The water inlet speed at the bottom of the cathode gas diffusion layer is 0.1 m/s. The gas diffusion contact angle (the hydrophobicity of the material surface is quantitatively defined by the contact angle) obtained by the traditional PTFE treatment mode is even to 120 degrees.
Example 1: the cell employs a cathode gas diffusion layer treated with conventional PTFE.
Example 2: the cell was treated with hydrophobic properties using only the cathode gas diffusion layer under the flow channels (scheme 1). After treatment, the contact angle of the part of the cathode gas diffusion layer below the flow channel is 120 degrees, and the contact angle of the part below the ridge is 90 degrees.
Example 3: the cell was treated with hydrophobic properties only for the cathode gas diffusion layer under the ridge (scheme 2). After treatment, the contact angle of the part of the cathode gas diffusion layer below the flow channel is 90 degrees, and the contact angle of the part below the ridge is 120 degrees.
Figure 4 shows: water drainage capacity and water distribution of the cathode gas diffusion layer. It can be seen that with the cathode gas diffusion layer of the conventional design, there is a significant accumulation of water in the flow channels and the portion under the ridge.
FIG. 5 shows: with the cathode gas diffusion layer of the embodiment 1 design, water substantially only builds up under the ridge and the main drainage path for water is at the location of the flow channel and ridge interface.
Figure 6 shows: with the cathode gas diffusion layer designed according to scheme 2, water is only accumulated below the flow channels, and the lower part of the ridge remains ideally dry.
As can be seen from fig. 5-6, both scheme 1 and scheme 2 can achieve the regulation of the water transport behavior inside the cathode gas diffusion layer, thereby optimizing the cell performance.
Because the PTFE on the surface of the carbon fibers in the carbon paper treated by the conventional process is distributed uniformly, the transmission path of the product water of the cathode catalyst layer is random and unpredictable (a large amount of liquid water is gathered under the ridges and the flow channels, see the attached drawing 4) in the process of discharging the product water out of the battery through the carbon paper, which can cause the liquid water to spread and block the main channel of the reaction gas entering the catalyst layer, weaken the electrochemical reaction strength and further reduce the battery performance.
The invention firstly provides a design for carrying out differential PTFE (polytetrafluoroethylene) hydrophobicity treatment on a gas diffusion layer, and effective path control of water as a cathode catalyst layer product in carbon paper is realized by carrying out hydrophobicity treatment on parts of the gas diffusion layer corresponding to the positions under ridges and under flow channels to different degrees (see figure 5 for transmission in the carbon paper under the ridges and figure 6 for transmission in the carbon paper under the flow channels), so that the possibility of random spread of the product water is reduced, the problem that the main transmission channel of reaction gas is blocked by liquid water is effectively solved, and the efficient and stable operation of a battery is ensured.
The invention is substantially different from the prior art in that the regional PTFE treatment in the carbon paper realizes that the transmission path of cathode product water is expected and can be macroscopically regulated and controlled as required in the process of discharging the cathode carbon paper, thereby effectively relieving the influence of the flooding phenomenon of the cathode on the performance of the battery.
Claims (5)
1. The method for processing the hydrophobic property of the cathode gas diffusion layer material in the proton exchange membrane fuel cell, the proton exchange membrane fuel cell is divided into a cathode plate, a cathode gas diffusion layer, a cathode catalyst layer, an electrolyte layer, an anode catalyst layer, an anode gas diffusion layer and an anode plate from top to bottom, wherein the solid part connected with the gas diffusion layer in the plate is a ridge, the area between the two ridges is a flow channel, the cathode gas diffusion layer adopts carbon paper or carbon cloth as the material, and the method is characterized in that: the specific method for processing the hydrophobic property of the cathode gas diffusion layer material is as follows:
(1) cutting the carbon paper into squares with the area of 5cm multiplied by 5cm, putting the squares into a beaker filled with acetone solution, and putting the beaker into an ultrasonic oscillator to clean and remove dust;
(2) taking out the carbon paper, cleaning the carbon paper again by using clean acetone, putting the cleaned carbon paper into a drying box, adjusting the temperature to 80-100 ℃ for drying, and weighing the dried carbon paper;
(3) diluting the polytetrafluoroethylene suspension with distilled water to a target concentration of 2 wt%;
(4) slowly placing the carbon paper into the diluted polytetrafluoroethylene solution, and then placing the carbon paper into an ultrasonic vibrator to enable the polytetrafluoroethylene solution to be fully immersed into the carbon paper;
(5) taking out the carbon paper, and marking a region mark on the carbon paper, wherein the area of the mark is as follows: the length is 5cm, the width is 1mm, a water gun with the pressure of 0.5MPa is used for washing the marked area, and polytetrafluoroethylene solution in the area is removed;
(6) drying the carbon paper at 80-100 ℃, and weighing the dried carbon paper containing the polytetrafluoroethylene, thereby calculating the content of the added polytetrafluoroethylene;
(7) repeating the steps 4-6 until the content of the polytetrafluoroethylene in the carbon paper reaches the target value concentration;
(8) placing the carbon paper into an oven at 150 ℃, gradually heating to 270 ℃, maintaining for 10 minutes, removing organic components in the carbon paper and polytetrafluoroethylene, then increasing the temperature of the oven to 320-350 ℃, and sintering the carbon paper for half an hour;
(9) and reducing the temperature of the oven to 150 ℃, maintaining for half an hour, taking out, finishing the hydrophobic property treatment of the carbon paper, and taking the carbon paper as a cathode gas diffusion layer.
2. The method of treating the hydrophobic property of a cathode gas diffusion layer material in a proton exchange membrane fuel cell according to claim 1, wherein: the processing method comprises two processing schemes for the battery flow channel: firstly, only the cathode gas diffusion layer below the flow channel is subjected to hydrophobic property treatment, and the corresponding cathode gas diffusion layer below the ridge still keeps weak hydrophobicity; and secondly, only the cathode gas diffusion layer under the ridge is subjected to hydrophobic treatment, and the cathode gas diffusion layer under the flow channel still keeps weak hydrophobicity.
3. The method of treating the hydrophobic property of a cathode gas diffusion layer material in a proton exchange membrane fuel cell according to claim 1, wherein: the marked area on the carbon paper is used as a special area for treating the hydrophobicity of the cathode gas diffusion layer, so that the distribution of the hydrophobic property inside the cathode gas diffusion layer shows difference.
4. The method of treating the hydrophobic property of a cathode gas diffusion layer material in a proton exchange membrane fuel cell according to claim 1 or 4, wherein: after the special area of the cathode gas diffusion layer is subjected to hydrophobic treatment, the porosity of the special area inside the cathode gas diffusion layer is reduced, and the water inside the cathode gas diffusion layer can be directionally transported.
5. The method of treating the hydrophobic property of a cathode gas diffusion layer material in a proton exchange membrane fuel cell according to claim 1, wherein: the carbon paper is a porous material.
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