PtPd carbon nanofiber membrane electrode and preparation method and application thereof

By loading PtPd alloy onto graphene nanofibers and preparing PtPd carbon nanofiber membrane electrodes using the NaBH4 low-temperature reduction method, the catalyst coating problem was solved, resulting in a low-cost and high-efficiency fuel cell catalyst with improved catalytic activity and durability.

CN120933408APending Publication Date: 2025-11-11山东国创燃料电池技术创新中心有限公司
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Patent Information

Application Number
CN202510882037.X
Authority / Receiving Office
CN · China
Patent Type
Applications(China)
Current Assignee / Owner
Filing Date
2025-06-27
Publication Date
2025-11-11

AI Technical Summary

Technical Problem

In existing technologies, the catalytically active components of nanofiber catalysts prepared by electrospinning are encapsulated inside the binder, resulting in low catalyst utilization and limited catalytic activity. This also leads to high usage of the precious metal platinum and higher costs.

Method used

Using graphene nanofibers as a carrier, PtPd carbon nanofiber membrane electrodes were prepared by electrospinning. Combined with the low-temperature reduction method of NaBH4, Pt and Pd were exposed on the graphene surface to form a PtPd alloy, which improved the utilization rate and durability of the catalyst.

Benefits of technology

This resulted in a highly efficient catalyst with low platinum loading, improving Pt utilization and mass transport efficiency, reducing fuel cell manufacturing costs, and enhancing the durability and catalytic activity of the membrane electrode assembly.

✦ Generated by Eureka AI based on patent content.

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Abstract

The invention belongs to the technical field of electrode material preparation, and discloses a PtPd carbon nanofiber membrane electrode and a preparation method and application thereof.The preparation method comprises the following steps that graphene, water, alcohol, Nafion, polyvinyl alcohol and polyacrylic acid are mixed in proportion, and an electrostatic spinning solution is obtained; preparing graphene nanofibers from the electrostatic spinning solution through an electrostatic spinning technology; performing heating esterification on the graphene nanofibers, and performing hot-pressing transfer printing on the graphene nanofibers to a proton exchange membrane; dipping the proton exchange membrane loaded with the graphene nanofibers in a mixed solution of chloroplatinic acid and chloropalladic acid, adjusting the pH value to be alkaline, and gradually adding a NaBH4 solution into the mixed solution; after the reaction is finished, adjusting the pH value of a reaction system to be acidic, and washing and drying to obtain a single-side PtPd graphene nanofiber membrane electrode; and finally, spraying an anode to obtain the PtPd graphene nanofiber membrane electrode. The PtPd alloy improves the durability of the membrane electrode, and finally, the NaBH4 low-temperature reduction yield is high, the energy consumption is low, and the low-cost large-scale preparation of the membrane electrode with low Pt loading capacity and high durability is realized.
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Description

Technical Field

[0001] This invention belongs to the field of electrode material preparation technology, specifically relating to a PtPd carbon nanofiber membrane electrode, its preparation method, and its application. Background Technology

[0002] The statements herein provide only background information in relation to this invention and do not necessarily constitute prior art.

[0003] Hydrogen fuel cells have attracted much attention due to their high energy density and zero emissions, and are considered an ideal energy source for achieving sustainable development. However, their application faces the challenge of high cost, mainly due to the expensive price of catalysts such as platinum. Therefore, reducing catalyst usage and developing high-performance membrane electrode assemblies with low platinum loading have become key breakthrough directions.

[0004] Constructing ordered membrane electrodes can effectively reduce the amount of Pt used and improve catalyst utilization. Electrospinning is an effective method for constructing ordered nanofiber membrane electrodes. The specific process involves mixing the catalyst with solvents, binders, etc., to prepare an electrospinning slurry, and then preparing nanofiber catalysts through electrospinning. However, in nanofiber catalysts prepared by this method, many catalytically active components are encapsulated inside the binder, reducing catalyst utilization and easily leading to limited catalytic activity of the prepared nanofiber catalysts. Summary of the Invention

[0005] To address the shortcomings of existing technologies, the purpose of this invention is to provide a PtPd carbon nanofiber membrane electrode, its preparation method, and its application.

[0006] To achieve the above objectives, the present invention is implemented through the following technical solution: In a first aspect, the present invention provides a method for preparing a PtPd carbon nanofiber membrane electrode, comprising the following steps: Graphene, water, alcohol, Nafion and binder are mixed in a certain proportion to obtain an electrospinning solution; Graphene nanofibers were prepared by electrospinning the electrospinning solution. Graphene nanofibers are heated, esterified, and then hot-pressed onto a proton exchange membrane. A proton exchange membrane loaded with graphene nanofibers was immersed in a mixed solution of chloroplatinic acid and chloropalladic acid, the pH was adjusted to alkaline, and NaBH4 solution was gradually added to it while stirring the reaction. After the reaction was complete, the pH of the reaction system was adjusted to acidic, and after washing and drying, a single-sided PtPd graphene nanofiber membrane electrode was obtained. Finally, the anode is sprayed to obtain a PtPd graphene nanofiber membrane electrode.

[0007] Secondly, the present invention provides a PtPd carbon nanofiber membrane electrode, which is prepared by the aforementioned preparation method.

[0008] Thirdly, the present invention provides the application of the PtPd carbon nanofiber membrane electrode in the preparation of fuel cells.

[0009] The beneficial effects achieved by one or more embodiments of the present invention described above are as follows: In this invention, PtPd graphene nanofiber membrane electrodes were successfully prepared by low-temperature reduction with NaBH4.

[0010] First, the electrospinning preparation of ordered nanofiber membrane electrodes can improve the utilization rate of Pt, reduce the Pt loading, and simultaneously improve the mass transport efficiency.

[0011] Secondly, the use of low-temperature reduction with NaBH4 exposes more Pt to the three-phase interface, further improving the utilization rate of Pt.

[0012] Then, the PtPd alloy improves the durability of the membrane electrode. Finally, the low-temperature reduction of NaBH4 yields high output and low energy consumption, enabling the low-cost, large-scale preparation of high-durability membrane electrodes with low Pt loading. Attached Figure Description

[0013] The accompanying drawings, which form part of this invention, are used to provide a further understanding of the invention. The illustrative embodiments of the invention and their descriptions are used to explain the invention and do not constitute an improper limitation of the invention.

[0014] Figure 1 SEM image of the graphene nanofibers prepared in Example 1 of this invention; Figure 2 This is a SEM image of the single-sided PtPd graphene nanofiber membrane electrode prepared in Example 1 of the present invention. Figure 3 Polarization curves of the graphene nanofiber membrane electrodes prepared in Examples 1-3; Figure 4 The polarization curves are for the graphene nanofiber membrane electrodes prepared in Example 1 and Comparative Examples 1-3. Figure 5 This is a comparison of the durability of the graphene nanofiber membrane electrodes prepared in Example 1 and Comparative Example 1. Figure 6 Polarization curves of the graphene nanofiber membrane electrodes prepared in Example 1 and Comparative Examples 4-5; Figure 7 This is a comparison of the durability of the graphene nanofiber membrane electrodes prepared in Example 1 and Comparative Example 4. Detailed Implementation

[0015] It should be noted that the following detailed description is illustrative and intended to provide further explanation of the invention. Unless otherwise specified, all technical and scientific terms used in this invention have the same meaning as commonly understood by one of ordinary skill in the art to which this invention pertains.

[0016] In a first aspect, the present invention provides a method for preparing a PtPd carbon nanofiber membrane electrode, comprising the following steps: Graphene, water, alcohol, Nafion, polyvinyl alcohol and polyacrylic acid are mixed in a certain proportion to obtain an electrospinning solution; Graphene nanofibers were prepared by electrospinning the electrospinning solution. Graphene nanofibers are heated, esterified, and then hot-pressed onto a proton exchange membrane. A proton exchange membrane loaded with graphene nanofibers was immersed in a mixed solution of chloroplatinic acid and chloropalladic acid, the pH was adjusted to alkaline, and NaBH4 solution was gradually added to it while stirring the reaction. After the reaction was complete, the pH of the reaction system was adjusted to acidic, and after washing and drying, a single-sided PtPd graphene nanofiber membrane electrode was obtained. Finally, the anode is sprayed to obtain a PtPd graphene nanofiber membrane electrode.

[0017] During heating and esterification, PAA and PVA are esterified to obtain stable nanofibers, thereby improving the stability of the nanofibers.

[0018] A proton exchange membrane loaded with graphene nanofibers was immersed in a mixed solution of chloroplatinic acid and chloropalladic acid. By adding NaBH4 solution stepwise and using a low-temperature reduction method, chloroplatinic acid and chloropalladic acid were reduced to obtain platinum and palladium, which were adsorbed on the surface of the graphene nanofibers. This effectively prevented the platinum and palladium from being coated by the binder, thereby effectively improving the utilization rate of platinum and palladium.

[0019] Adding graphene to the electrospinning solution can effectively improve the mechanical strength and conductivity of graphene nanofibers. Furthermore, the synergistic effect of the graphene sheet wrinkles and the porous structure of the fibers can effectively increase the specific surface area of ​​the graphene nanofibers, thereby effectively increasing the adsorption capacity of the catalyst particles and enhancing the catalytic activity of the PtPd carbon nanofiber electrode.

[0020] During the reduction process, platinum and palladium form a PtPd alloy, which can effectively solve the three major failure problems of pure Pt catalysts in fuel cell operation: platinum dissolution / agglomeration, carbon support corrosion, and poisoning deactivation, thereby effectively improving electrode durability. Specifically: In PtPd alloys, Pd is more easily oxidized and dissolved, while a stable PdO passivation layer forms on the Pt surface, effectively preventing Pt dissolution. Pd atoms can effectively anchor the Pt lattice, increasing the metal bonding energy and inhibiting the migration of surface Pt atoms, thereby suppressing Pt aggregation.

[0021] Pd can optimize the oxygen reduction pathway, reduce H2O2 yield, and thus decrease the frequency of hydroxyl radical attack on the carbon support, effectively preventing carbon support corrosion. Pd can also effectively improve the bonding strength between Pt and the carbon support, reducing catalyst particle detachment.

[0022] In addition, the presence of Pd can reduce SO4 levels. 2- / HSO4 - The adsorption of anions, and the effective blocking of Cu²⁺ by the stable oxide of Pd. + / Fe² + Impurity ions are deposited on Pt active sites, which can effectively improve the electrode's resistance to poisoning.

[0023] In some embodiments, the mass ratio of graphene, water, alcohol, Nafion, and binder in the electrospinning solution is 1:12-25:9-14:0.5-1:0.15-0.3. The mass ratio of PAA to PVA is 1:0.2-0.7.

[0024] Preferably, the graphene is XC-72R, BP2000, EC300J, EC600JD or FCX80.

[0025] Preferably, the alcohol is methanol, ethanol, isopropanol or n-propanol.

[0026] In some embodiments, graphene nanofibers prepared by electrospinning are directly spun onto aluminum foil. This facilitates subsequent esterification and hot-press transfer steps, and esterification can improve the stability of the nanofibers.

[0027] In some embodiments, the heating esterification temperature is 130-150°C, and the heating esterification time is 1-3 h.

[0028] In some embodiments, the hot pressing temperature is 140-160°C and the hot pressing time is 1-5 min.

[0029] In some embodiments, a proton exchange membrane loaded with graphene nanofibers is immersed in a mixed solution of chloroplatinic acid and chloropalladic acid, and the pH value is adjusted to 10-12.

[0030] In some embodiments, after the reaction is complete, the pH of the reaction system is adjusted to ≤2 to allow the Pt particles to settle more uniformly.

[0031] Secondly, the present invention provides a PtPd carbon nanofiber membrane electrode, which is prepared by the aforementioned preparation method.

[0032] Thirdly, the present invention provides the application of the PtPd carbon nanofiber membrane electrode in the preparation of fuel cells.

[0033] The present invention will be further described below with reference to embodiments and comparative examples.

[0034] Example 1 (1) Accurately weigh 0.6 g of EC600JD graphene carrier, add 4.2 g of 10 wt% Nafion, 7.4 g of isopropanol and 11.8 g of deionized water, cell disruption for 10 min, shearing for 20 min, and sonication for 40 min to mix evenly. Take 8.3 g of the evenly mixed solution and add 0.1 g of PAA and 0.3 g of 10% PVA solution, and stir for 24 h. (2) Control the temperature below 30℃, humidity below 50%, positive high voltage of 14 kV, negative high voltage of -2 kV, liquid flow rate of 0.2 mm / min, and electrospin on aluminum foil for 5 h to obtain graphene nanofibers. (3) The nanofibers were esterified in a muffle furnace at 140°C for 2 hours to obtain stable graphene nanofibers. (4) Graphene nanofibers were hot-pressed at 150°C for 3 min and transferred onto a proton exchange membrane to obtain a single-sided graphene nanofiber membrane electrode. (5) Take 1000 ml of water in a 3000 mL beaker, add 20 ml of 37.25 mg / mL H2PtCl6 aqueous solution, 20 ml of 37.25 mg / mL H2PdCl4 aqueous solution and 8 g NaOH, stir for 20 min until the solution is uniform, and then immerse the single-sided graphene nanofiber membrane electrode in the solution. (6) Dissolve 1 g NaBH4 in 500 ml of water and stir for 10 min until NaBH4 is completely dissolved; (7) Add the prepared NaBH4 solution dropwise to the graphene nanofiber membrane electrode solution and stir for 2 hours; (8) After the reaction is complete, the pH of the solution is adjusted to ≤2 with nitric acid, then washed with deionized water multiple times and dried under vacuum to obtain a single-sided PtPd graphene nanofiber membrane electrode. (9) Preparation of anode slurry: Take 0.23 g of PtC powder (the mass percentage of Pt in the PtC powder is 60%), add 1.6 g of deionized water, 0.645 g of 10% Nafion and 30.2 g of ethanol in sequence, crush the cells for 45 min, and sonicate for 30 min to obtain the spraying slurry. Then, spray the anode on the other side of the single-sided PtPd graphene nanofiber membrane electrode to obtain the PtPd graphene nanofiber membrane electrode.

[0035] Figure 1 These are SEM images of the graphene nanofibers prepared in Example 1. Figure 1 It can be seen that graphene nanofibers exhibit a uniform fibrous structure.

[0036] Figure 2 This is a SEM image of the PtPd graphene nanofiber membrane electrode prepared in Example 1. Figure 2 It can be seen that the nanofibers thickened after Pt and Pd were loaded, indicating that Pt and Pd were successfully loaded.

[0037] Example 2 (1) Accurately weigh 0.6 g of EC600JD graphene carrier, add 4.5 g of 10 wt% Nafion, 8 g of isopropanol, and 12.8 g of deionized water, cell pulverize for 10 min, shear for 20 min, and sonicate for 40 min to mix evenly. Take 8.3 g of the evenly mixed solution and add 0.1 g of PAA and 0.3 g of 10% PVA solution, and stir for 24 h. (2) Control the temperature below 30℃, humidity below 50%, positive high voltage of 14 kV, negative high voltage of -2 kV, liquid flow rate of 0.2 mm / min, electrospin on aluminum foil paper, and obtain graphene nanofibers after 6 h of electrospinning. (3) The nanofibers were esterified in a muffle furnace at 140°C for 2 h to obtain stable graphene nanofibers. (4) Graphene nanofibers were hot-pressed at 145°C for 3 min and transferred onto a proton exchange membrane to obtain a single-sided graphene nanofiber membrane electrode. (5) Take 1000 ml of water in a 3000 mL beaker, add 20 ml of 39.41 mg / mL H2PtCl6 aqueous solution, 20 ml of 36.64 mg / mL H2PdCl4 aqueous solution and 8 g of NaOH, stir for 20 min until the solution is uniform, and then immerse the single-sided graphene nanofiber membrane electrode in the solution. (6) Dissolve 1.5 g NaBH4 in 500 ml of water and stir for 20 min until NaBH4 is completely dissolved; (7) Add the prepared NaBH4 solution dropwise to the graphene nanofiber membrane electrode solution and stir for 2 hours; (8) After the reaction is complete, the pH of the solution is adjusted to ≤2 with nitric acid, then washed with deionized water multiple times and dried under vacuum to obtain a single-sided PtPd graphene nanofiber membrane electrode. (9) Preparation of anode slurry: Take 0.23 g of PtC powder (the mass percentage of Pt in the PtC powder is 60%), add 1.6 g of deionized water, 0.645 g of 10% Nafion and 30.2 g of ethanol in sequence, crush the cells for 45 min, and sonicate for 30 min to obtain the spraying slurry. Then, spray the anode on the other side of the single-sided PtPd graphene nanofiber membrane electrode to obtain the PtPd graphene nanofiber membrane electrode.

[0038] Example 3 (1) Accurately weigh 0.8 g of EC600JD graphene carrier, add 3.6 g of 10 wt% Nafion, 7 g of isopropanol, and 10.8 g of deionized water, cell disruption for 10 min, shearing for 20 min, and sonication for 40 min to make it evenly mixed. Take 8.5 g of the evenly mixed solution, add 0.1 g of PAA and 0.5 g of 10% PVA solution, and stir for 24 h. (2) Control the temperature below 30℃, humidity below 50%, positive high voltage of 14 kV, negative high voltage of -2 kV, liquid flow rate of 0.2 mm / min, electrospin on aluminum foil paper, and obtain graphene nanofibers after 6 h of electrospinning. (3) The nanofibers were esterified in a muffle furnace at 150°C for 2 hours to obtain stable graphene nanofibers. (4) Graphene nanofibers were hot-pressed at 155°C for 3 min and transferred onto a proton exchange membrane to obtain a single-sided graphene nanofiber membrane electrode. (5) Take 1000 ml of water in a 3000 mL beaker, add 20 ml of 36.67 mg / mL H2PtCl6 aqueous solution, 20 ml of 36.95 mg / mL H2PdCl4 aqueous solution and 8 g NaOH, stir for 20 min until the solution is uniform, and then immerse the single-sided graphene nanofiber membrane electrode in the solution. (6) Dissolve 1.2 g NaBH4 in 500 ml of water and stir for 15 min until NaBH4 is completely dissolved; (7) Add the prepared NaBH4 solution dropwise to the graphene nanofiber membrane electrode solution and stir for 2 hours; (8) After the reaction is complete, the pH of the solution is adjusted to ≤2 with nitric acid, then washed with deionized water multiple times and dried under vacuum to obtain a single-sided PtPd graphene nanofiber membrane electrode. (9) Preparation of anode slurry: Take 0.23 g of PtC powder (the mass percentage of Pt in the PtC powder is 60%), add 1.6 g of deionized water, 0.645 g of 10% Nafion and 30.2 g of ethanol in sequence, crush the cells for 45 min, and sonicate for 30 min to obtain the spraying slurry. Then, spray the anode on the other side of the single-sided PtPd graphene nanofiber membrane electrode to obtain the PtPd graphene nanofiber membrane electrode.

[0039] Figure 3 These are polarization curves of the membrane electrodes prepared in Examples 1, 2, and 3. The performance of the membrane electrode prepared in Example 1 is not much different from that of the membrane electrodes prepared in Examples 2 and 3, indicating that PtPd carbon nanofibers have advantages in performance within the scope of patent protection.

[0040] Comparative Example 1 The difference from Example 1 is that in step (5), the H2PdCl4 aqueous solution is omitted, while everything else is the same as in Example 1, as follows: (1) Accurately weigh 0.6 g of EC600JD graphene carrier, add 4.2 g of 10 wt% Nafion, 7.4 g of isopropanol and 11.8 g of deionized water, cell pulverize for 10 min, shear for 20 min, and sonicate for 40 min to mix evenly. Take 8.3 g of the evenly mixed solution and add 0.1 g of PAA and 0.3 g of 10% PVA solution, and stir for 24 h. (2) Control the temperature below 30℃, humidity below 50%, positive high voltage of 14 kV, negative high voltage of -2 kV, liquid flow rate of 0.2 mm / min, and electrospin on aluminum foil for 5 h to obtain graphene nanofibers. (3) The nanofibers were esterified in a muffle furnace at 140°C for 2 hours to obtain stable graphene nanofibers. (4) Graphene nanofibers were hot-pressed at 150°C for 3 min and transferred onto a proton exchange membrane to obtain a single-sided graphene nanofiber membrane electrode. (5) Take 1000 ml of water in a 3000 mL beaker, add 20 ml of 37.25 mg / mL H2PtCl6 aqueous solution and 8 g NaOH, stir for 20 min until the solution is uniform, and then immerse the single-sided graphene nanofiber membrane electrode in the solution; (6) Dissolve 1 g NaBH4 in 500 ml of water and stir for 10 min until NaBH4 is completely dissolved; (7) Add the prepared NaBH4 solution dropwise to the graphene nanofiber membrane electrode solution and stir for 2 hours; (8) Adjust the pH of the solution to ≤2 with nitric acid, then wash with deionized water multiple times, and vacuum dry to obtain a single-sided Pt graphene nanofiber membrane electrode. (9) Preparation of anode slurry: Take 0.23 g PtC powder, add 1.6 g deionized water, 0.645 g 10% Nafion and 30.2 g ethanol in sequence, crush the cells for 45 min, and sonicate for 30 min to obtain the spraying slurry. Then spray the anode on the other side of the single-sided Pt graphene nanofiber membrane electrode to obtain the Pt graphene nanofiber membrane electrode.

[0041] Comparative Example 2 (1) Weigh 0.5 g of 60% Pt / C catalyst, add 3.5 g of water, 2.8 g of Nafion and 65.9 g of ethanol, crush the cells for 40 min, and sonicate for 30 min to obtain catalyst slurry; (2) Spray the coating onto both sides of the proton exchange membrane to obtain the sprayed membrane electrode.

[0042] Comparative Example 3 (1) Weigh 1.5 g of 60% Pt / C catalyst, add 4.2 g of 10 wt% Nafion, 7.4 g of isopropanol, and 11.8 g of deionized water. Crush the cells for 10 min, shear for 20 min, and sonicate for 40 min to mix them evenly. Take 8.3 g of the evenly mixed solution, add 0.11 g of PAA, and stir for 24 h. (2) Control the temperature below 30℃, humidity below 50%, positive high voltage of 14 kV, negative high voltage of -2 kV, liquid flow rate of 0.15 mm / min, and electrospin for 5 h to obtain nanofiber catalyst layer; (3) At 150 °C and 0.3 MPa, nanofibers were transferred onto a proton exchange membrane to obtain a single-sided nanofiber membrane electrode. (4) Preparation of anode slurry: Take 0.23 g of PtC powder (the mass percentage of Pt in the PtC powder is 60%), add 1.6 g of deionized water, 0.645 g of 10% Nafion and 30.2 g of ethanol in sequence, crush the cells for 45 min, and sonicate for 30 min to obtain the spraying slurry. Then spray the anode on the other side of the single-sided nanofiber membrane electrode to obtain the Pt graphene nanofiber membrane electrode.

[0043] Figure 4The figures show the polarization curves of the membrane electrodes prepared in Examples 1, 1, 2, and 3. It can be seen from the figures that the membrane electrode prepared in Example 1 and the membrane electrode prepared in Comparative Example 1 have basically the same performance, indicating that the addition of Pd did not affect the performance of Pt carbon nanofibers. However, the performance of the membrane electrode prepared in Example 1 is much higher than that of the membrane electrodes prepared in Comparative Example 2 and 3, indicating that Pt particles wrapped around carbon nanofibers can improve the utilization rate of Pt and thus improve performance. In addition, the nanofiber structure can also improve the utilization rate of the catalyst.

[0044] Figure 5 This is a comparison chart of the durability tests of the graphene nanofiber membrane electrodes prepared in Example 1 and Comparative Example 1. Figure 5 It can be seen that the stability of Example 1 is higher than that of Comparative Example 1, and the Pd doping to form an alloy improves the stability of the nanofiber catalyst layer.

[0045] Comparative Example 4 The difference from Example 1 is that step (3) esterification is omitted, while all other steps are the same as in Example 1.

[0046] Comparative Example 5 The difference from Example 1 is that the graphene carrier in step (1) is omitted, while everything else is the same as in Example 1.

[0047] Figure 6 The graphs are polarization curves of the graphene nanofiber membrane electrodes prepared in Example 1, Comparative Example 4 and Comparative Example 5. The performance of Example 1 and Comparative Example 4 is basically the same, indicating that the esterification of PAA and PVA has little effect on the performance. The performance of Comparative Example 5 is extremely poor, indicating that without carbon support, the performance of Pt is extremely poor.

[0048] Figure 7 This is a comparison chart of the durability tests of the graphene nanofiber membrane electrodes prepared in Example 1 and Comparative Example 4. The performance of the membrane electrode prepared in Example 1 remained basically unchanged before and after durability, while the performance of the membrane electrode prepared in Comparative Example 4 decreased significantly before and after durability, indicating that PAA and PVA esterification can improve the durability of the catalyst layer.

[0049] The above description is merely a preferred embodiment of the present invention and is not intended to limit the invention. Various modifications and variations can be made to the present invention by those skilled in the art. Any modifications, equivalent substitutions, improvements, etc., made within the spirit and principles of the present invention should be included within the scope of protection of the present invention.

Claims

1. A method for preparing a PtPd carbon nanofiber membrane electrode, characterized in that: Includes the following steps: Graphene, water, alcohol, Nafion, polyvinyl alcohol and polyacrylic acid are mixed in a certain proportion to obtain an electrospinning solution; Graphene nanofibers were prepared by electrospinning the electrospinning solution. Graphene nanofibers are heated, esterified, and then hot-pressed onto a proton exchange membrane. A proton exchange membrane loaded with graphene nanofibers was immersed in a mixed solution of chloroplatinic acid and chloropalladic acid, the pH was adjusted to alkaline, and NaBH4 solution was gradually added to it while stirring the reaction. After the reaction was complete, the pH of the reaction system was adjusted to acidic, and after washing and drying, a single-sided PtPd graphene nanofiber membrane electrode was obtained. Finally, the anode is sprayed to obtain a PtPd graphene nanofiber membrane electrode.

2. The method for preparing the PtPd carbon nanofiber membrane electrode according to claim 1, characterized in that: In the electrospinning solution, the mass ratio of graphene, water, alcohol, Nafion, and binder is 1:12-25:8-14:0.4-1:0.15-0.

3. Preferably, the graphene is XC-72R, BP2000, EC300J, EC600JD or FCX80.

3. The method for preparing the PtPd carbon nanofiber membrane electrode according to claim 1, characterized in that: The alcohol is methanol, ethanol, isopropanol, or n-propanol.

4. The method for preparing the PtPd carbon nanofiber membrane electrode according to claim 1, characterized in that: Graphene nanofibers, produced by electrospinning, are directly spun onto aluminum foil.

5. The method for preparing the PtPd carbon nanofiber membrane electrode according to claim 1, characterized in that: The heating esterification temperature is 130-150℃, and the heating esterification time is 1-3h.

6. The method for preparing the PtPd carbon nanofiber membrane electrode according to claim 1, characterized in that: The hot pressing temperature is 140-160℃, and the hot pressing time is 1-5 minutes.

7. The method for preparing the PtPd carbon nanofiber membrane electrode according to claim 1, characterized in that: The proton exchange membrane loaded with graphene nanofibers was immersed in a mixed solution of chloroplatinic acid and chloropalladic acid, and the pH was adjusted to 10-12.

8. The method for preparing the PtPd carbon nanofiber membrane electrode according to claim 1, characterized in that: After the reaction is complete, adjust the pH of the reaction system to ≤2.

9. A PtPd carbon nanofiber membrane electrode, characterized in that: It is prepared by any one of the preparation methods described in claims 1-8.

10. The application of the PtPd carbon nanofiber membrane electrode of claim 9 in the preparation of fuel cells.