CN211530098U - Composite proton exchange membrane and fuel cell - Google Patents
Composite proton exchange membrane and fuel cell Download PDFInfo
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- CN211530098U CN211530098U CN202020357172.5U CN202020357172U CN211530098U CN 211530098 U CN211530098 U CN 211530098U CN 202020357172 U CN202020357172 U CN 202020357172U CN 211530098 U CN211530098 U CN 211530098U
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- Y02E—REDUCTION OF GREENHOUSE GAS [GHG] EMISSIONS, RELATED TO ENERGY GENERATION, TRANSMISSION OR DISTRIBUTION
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Abstract
The utility model belongs to the technical field of fuel cell material, concretely relates to compound proton exchange membrane and fuel cell. The utility model discloses a compound proton exchange membrane includes proton exchange membrane, sets up in the first porous enhancement layer of proton exchange membrane's positive pole side and sets up in the porous enhancement layer of second of proton exchange membrane's negative pole side, and the porosity of first porous enhancement layer is less than the porosity of the porous enhancement layer of second. The utility model provides a compound proton exchange membrane sets up porous enhancement layer through the both sides at proton exchange membrane, and the porosity of the porous enhancement layer of positive side is less than the porosity of the porous enhancement layer of negative side, makes the effective reaction area of positive side reduce, and the reaction rate of positive side matches with the reaction rate of negative side this moment to promote the mechanical properties and the chemical durability of membrane electrode, prolong its life-span.
Description
Technical Field
The utility model belongs to the technical field of fuel cell material, more specifically say, relate to a compound proton exchange membrane and fuel cell.
Background
The proton exchange membrane is a core material of a Proton Exchange Membrane Fuel Cell (PEMFC), plays a role in blocking fuel (hydrogen) and oxidant (oxygen) and conducting protons, and the stability directly determines the service life of the whole PEMFC. The degradation of the proton exchange membrane in the cell environment includes chemical/electrochemical degradation, thermal degradation and mechanical property degradation (mainly mechanical strength reduction, water loss-swelling deformation), wherein the chemical/electrochemical degradation is the main degradation process of the proton exchange membrane and directly causes the reduction of proton conductivity and the degradation of cell performance. Currently commercialized proton exchange membranes are Nafion series perfluorosulfonic acid membranes manufactured by dupont, usa. The Nafion series membrane has high proton conductivity under the condition of high humidification degree, but the Nafion series membrane has high hydrogen permeability, the service life of the Nafion series membrane does not meet the requirement, and the Nafion series membrane is expensive. In addition, when free radicals such as HO/HOO exist in the cell, the free radicals can attack carboxyl at the tail end of the polymer, so that the chemical structure of the proton exchange membrane is degraded, the thickness of the proton exchange membrane is reduced, even pinholes are formed by perforation, gas on two sides is subjected to cross permeation, and the performance of the membrane electrode is reduced.
SUMMERY OF THE UTILITY MODEL
The application aims to provide a composite proton exchange membrane and a fuel cell so as to solve the technical problems of short service life, poor performance and the like in the existing proton exchange membrane technology.
To achieve the above objects, in one aspect, the present invention provides a composite proton exchange membrane, comprising:
a proton exchange membrane;
a first porous reinforcement layer disposed on an anode side of the proton exchange membrane;
a second porous reinforcement layer disposed on a cathode side of the proton exchange membrane;
the first porous reinforcing layer has a porosity less than a porosity of the second porous reinforcing layer.
Further, the pore size of the first porous reinforcing layer is 0.1 to 0.9 μm.
Further, the porosity of the first porous reinforcing layer is 40% -70%.
Further, the pore size of the second porous reinforcing layer is 0.1 to 0.9 μm.
Further, the porosity of the second porous reinforcing layer is 71% -98%.
Further, the thickness of the first porous reinforcing layer and/or the second porous reinforcing layer is 1 μm to 15 μm.
Further, the first porous reinforcing layer is an e-PTFE reinforcing layer or a PVDF reinforcing layer.
Further, the second porous reinforced layer is an e-PTFE reinforced layer or a PVDF reinforced layer.
Further, the first porous reinforcing layer is a first porous reinforcing layer containing a radical quencher.
Further, the second porous reinforcing layer is a second porous reinforcing layer containing a radical quencher.
Still further, the radical quencher is at least one selected from a radical quencher containing manganese and a radical quencher containing cerium.
Further, the first porous reinforcing layer is a first porous reinforcing layer containing a perfluorosulfonic acid resin.
Further, the second porous reinforcing layer is a second porous reinforcing layer containing a perfluorosulfonic acid resin.
Further, the proton exchange membrane is a perfluorosulfonic acid proton exchange membrane.
Further, the thickness of the proton exchange membrane is 5-50 μm.
On the other hand, the utility model also provides a fuel cell, and this fuel cell includes foretell compound proton exchange membrane.
The utility model has the advantages that the first porous enhancement layer is arranged on the anode side of the proton exchange membrane, and the second porous enhancement layer is arranged on the cathode side of the proton exchange membrane, so that the mechanical strength of the proton exchange membrane is enhanced; meanwhile, the porosity of the first porous enhancement layer is smaller than that of the second porous enhancement layer, so that the effective reaction area of the anode side is smaller than that of the cathode side, the hydrogen oxidation reaction rate of the anode side is properly reduced, the reaction rates of the anode side and the cathode side are more balanced, and the chemical durability and the service life of the proton exchange membrane are improved.
Drawings
In order to more clearly illustrate the technical solutions in the embodiments of the present application, the drawings needed to be used in the embodiments or the prior art descriptions will be briefly described below, and it is obvious that the drawings in the following description are only some embodiments of the present application, and it is obvious for those skilled in the art to obtain other drawings based on these drawings without inventive exercise.
FIG. 1 is a schematic structural diagram of a composite proton exchange membrane provided in an embodiment of the present application;
wherein, in the figures, the respective reference numerals:
10-a proton exchange membrane; 20-a first porous reinforcing layer; 30-a second porous reinforcing layer.
Detailed Description
In order to make the technical problems, technical solutions and advantageous effects to be solved by the present application clearer, the present application is further described in detail below with reference to the accompanying drawings and embodiments. It should be understood that the specific embodiments described herein are merely illustrative of the present application and are not intended to limit the present application.
It will be understood that when an element is referred to as being "secured to" or "disposed on" another element, it can be directly on the other element or be indirectly on the other element. When an element is referred to as being "connected to" another element, it can be directly connected to the other element or be indirectly connected to the other element.
Furthermore, the terms "first", "second" and "first" are used for descriptive purposes only and are not to be construed as indicating or implying relative importance or implicitly indicating the number of technical features indicated. Thus, a feature defined as "first" or "second" may explicitly or implicitly include one or more of that feature.
The composite proton exchange membrane provided in the examples of the present application will now be described with reference to fig. 1. A composite proton exchange membrane comprising:
a proton exchange membrane 10;
a first porous reinforcement layer 20 disposed on the anode side of the proton exchange membrane 10;
a second porous reinforcement layer 30 disposed on the cathode side of the proton exchange membrane 20;
wherein the porosity of the first porous reinforcing layer 20 is smaller than the porosity of the second porous reinforcing layer 30.
In the hydrogen-oxygen fuel cell reaction, because the hydrogen oxidation reaction at the anode side is extremely rapid, and the oxygen reduction reaction at the cathode side is relatively slow, the problems that the reactions at the two poles are not balanced, the reaction rate of the hydrogen-oxygen fuel cell is determined by the oxygen reduction reaction at the cathode side, and the like exist. According to the composite proton exchange membrane provided by the application, the first porous reinforcing layer 20 is arranged on the anode side of the proton exchange membrane 10, and the second porous reinforcing layer 30 is arranged on the cathode side of the proton exchange membrane 10, so that the obtained composite proton exchange membrane is higher in mechanical strength; meanwhile, because the porosity of the first porous reinforcing layer 20 is smaller than that of the second porous reinforcing layer 30, the effective reaction area of the anode side is smaller than that of the cathode side, so that the hydrogen oxidation reaction rate of the anode side is properly reduced, the reaction rates of the anode side and the cathode side are more balanced, and the chemical durability and the service life of the composite proton exchange membrane are improved.
In some embodiments, the first porous reinforcement layer 20 has a porosity of 40% to 70%. Since the first porous reinforcing layer 20 is disposed on the anode side of the proton exchange membrane 10, the rate of the hydrogen oxidation reaction on the anode side is relatively high, and the porosity of the first porous reinforcing layer 20 is limited to the above range, so that the chemical resistance of the anode side of the membrane can be maintained, the effective reaction area is reduced, and the oxidation reaction on the anode side can be controlled more appropriately. Specifically, the first porous reinforcing layer 20 typically, but not by way of limitation, has a porosity of 40%, 45%, 50%, 55%, 60%, 65%, 70%.
In some embodiments, the porosity of the second porous reinforcing layer 30 is 71% -98%. Since the second porous reinforcing layer 30 is disposed on the cathode side of the proton exchange membrane 10, the rate of the oxygen reduction reaction on the cathode side is relatively slow, and the porosity of the second porous reinforcing layer 30 is increased, which is helpful for improving the gas permeability, and the chemical resistance of the membrane is enhanced while the decrease of the reaction rate on the cathode side is properly reduced, so that the reaction rate on the cathode side is more balanced with the reaction rate on the anode side. Specifically, the second porous reinforcing layer 30 typically, but not by way of limitation, has a porosity of 71%, 75%, 80%, 85%, 90%, 95%, 98%.
In some embodiments, the pore size of the first porous reinforcing layer and/or the second porous reinforcing layer is set to 0.1 μm to 0.9 μm. If the pore diameter is too small, the proton exchange capacity is reduced when the porous enhancement layer is soaked in the proton exchange membrane solution, which is not beneficial to the optimization of the proton exchange function of the composite proton exchange membrane; too large a pore size affects the overall mechanical properties of the composite proton exchange membrane. Specifically, the typical, but not limiting, pore sizes of the first and/or second porous-reinforced layers are 0.1 μm, 0.2 μm, 0.3 μm, 0.4 μm, 0.5 μm, 0.6 μm, 0.7 μm, 0.8 μm, 0.9 μm.
The thickness of the porous reinforcing layer is positively related to the dimensional stability and mechanical strength thereof, but negatively related to the electrical conductivity and gas permeability, and thus, in some embodiments, the thickness of the first and second porous reinforcing layers 20 and 30 is set to be 1 μm to 15 μm in order to balance the mechanical strength and properties of the resulting composite proton exchange membrane, such as electrical conductivity and gas permeability. Specifically, typical, but not limiting, thicknesses of the first/second porous reinforcing layer are 1 μm, 2 μm, 3 μm, 4 μm, 5 μm, 6 μm, 7 μm, 8 μm, 9 μm, 10 μm, 11 μm, 12 μm, 13 μm, 14 μm, 15 μm.
Preferably, the thickness of the first porous reinforcing layer 20 is set to be 5 μm to 10 μm, which is beneficial to further improving the mechanical strength and the service life of the composite proton exchange membrane; setting the thickness of the second porous reinforcing layer 30 to 1 μm to 6 μm is advantageous for further accelerating the reaction rate on the cathode side.
The expanded polytetrafluoroethylene (e-PTFE) material has the performances of high uniformity, high strength and low shrinkage, and micropores on the expanded polytetrafluoroethylene (e-PTFE) material can prevent electrolyte from passing through and allow air and oxygen to pass through at the same time, and can be filled with resin, so that the expanded polytetrafluoroethylene (e-PTFE) material is favorable for further fusion with the proton exchange membrane 10 and avoids interface separation; polyvinylidene fluoride (PVDF) materials have good chemical resistance, high temperature resistance, and oxidation resistance. In some embodiments, e-PTFE or PVDF is used as the material of the first porous reinforcing layer 20 and/or the second porous reinforcing layer 30, which is beneficial to improve the mechanical strength and service life of the resulting composite proton exchange membrane.
When oxygen is reduced on the cathode, a small amount of hydrogen peroxide molecules are inevitably generated, and hydroxyl radicals generated by decomposition of the hydrogen peroxide molecules attack the proton exchange membrane 10 to destroy the skeleton structure of the proton exchange membrane 10, so that the stability/durability of the membrane electrode and the fuel cell is reduced. Therefore, by immersing the first porous reinforcing layer 20 and/or the second porous reinforcing layer 30 in the radical quencher to obtain the first porous reinforcing layer 20 containing the radical quencher and/or the second porous reinforcing layer 30 containing the radical quencher, the radical quencher can protect the proton exchange membrane 10 from being attacked by active radicals, thereby improving the durability of the membrane electrode and the fuel cell.
Preferably, the free radical quencher is at least one selected from a free radical quencher containing manganese and a free radical quencher containing cerium, so as to further improve the oxidation resistance of the proton exchange membrane. In particular, the radical quencher may be selected from CeO2And/or MnO2。
In some embodiments, in order to obtain a thin proton exchange membrane 10, the first porous reinforcement layer 20 and/or the second porous reinforcement layer 30 are impregnated with perfluorosulfonic acid resin to obtain a first porous reinforcement layer 20 containing perfluorosulfonic acid resin and/or a second porous reinforcement layer 30 containing perfluorosulfonic acid resin, the perfluorosulfonic acid resin is filled in the porous structure of the first porous reinforcement layer 20 and/or the second porous reinforcement layer 30, and then the first porous reinforcement layer 20 and the second porous reinforcement layer 30 are laminated or the like, so that the joint between the two parts can form the thin proton exchange membrane 10.
In some embodiments, a perfluorosulfonic acid material (Nafion) is selected as the material of the proton exchange membrane 10. The perfluorosulfonic acid membrane has the advantages of high mechanical strength, good chemical stability, large proton conductivity and the like, and is the most common membrane material in the current fuel cell. It is to be understood that, in addition to the perfluorosulfonic acid membrane, the proton exchange membrane 10 of the present application may be selected from any other membrane material suitable for a fuel cell.
The proton exchange membrane 10 in the composite proton exchange membrane of the present application can be prepared in two ways: the first method is as described above, the first porous reinforcement layer 20 and/or the second porous reinforcement layer 30 are/is impregnated with perfluorosulfonic acid resin to obtain the first porous reinforcement layer 20 containing perfluorosulfonic acid resin and/or the second porous reinforcement layer 30 containing perfluorosulfonic acid resin, the perfluorosulfonic acid resin is filled in the porous structure of the first porous reinforcement layer 20 and/or the second porous reinforcement layer 30, and then the first porous reinforcement layer 20 and the second porous reinforcement layer 30 are laminated and the like, so that the joint part of the two can form the proton exchange membrane 10 with a thin thickness; the second method is to take a perfluorosulfonic acid proton exchange membrane 10, and then attach the first porous reinforcing layer 20 and the second porous reinforcing layer 30 to the anode side and the cathode side of the perfluorosulfonic acid proton exchange membrane 10 respectively in a laminating manner, etc., at this time, the first porous reinforcing layer 20 and the second porous reinforcing layer 30 can selectively soak perfluorosulfonic acid resin. The composite proton exchange membrane prepared in the second way is relatively thicker than the composite proton exchange membrane prepared in the first way, and the thickness of the proton exchange membrane 10 has a significant correlation with the conductivity of the obtained composite proton exchange membrane, so that in order to obtain the composite proton exchange membrane with better conductivity, in some embodiments, the thickness of the proton exchange membrane 10 is controlled to be 5 μm to 50 μm. Specifically, typical but non-limiting proton exchange membranes 10 have a thickness of 5 μm, 6 μm, 7 μm, 8 μm, 9 μm, 10 μm, 11 μm, 12 μm, 13 μm, 14 μm, 15 μm, 16 μm, 17 μm, 18 μm, 19 μm, 20 μm, 21 μm, 22 μm, 23 μm, 24 μm, 25 μm, 26 μm, 27 μm, 28 μm, 29 μm, 30 μm, 31 μm, 32 μm, 33 μm, 34 μm, 35 μm, 36 μm, 37 μm, 38 μm, 39 μm, 40 μm, 41 μm, 42 μm, 43 μm, 44 μm, 45 μm, 46 μm, 47 μm, 48 μm, 49 μm, 50 μm.
Correspondingly, the embodiment of the application also provides a fuel cell, which comprises the composite proton exchange membrane.
Because the composite proton exchange membrane has the advantages of better mechanical property and chemical durability and longer service life, correspondingly, the fuel cell has excellent mechanical property and chemical durability and longer service life by adopting the composite proton exchange membrane with the advantages.
Example 1
The proton exchange membrane is a Nafion film with the thickness of 5 microns, the first porous enhancement layer is e-PTFE soaked in Nafion solution, the porosity is 60 percent, the thickness is 5 microns, and the aperture is 0.2 microns; the second porous enhancement layer is e-PTFE soaked in Nafion solution, the porosity is 80%, the thickness is 3 mu m, and the pore diameter is 0.4 mu m. And respectively placing the first porous enhancement layer and the second porous enhancement layer on two sides of the proton exchange membrane, and performing hot press molding to obtain the composite proton exchange membrane. The swelling rate of the composite proton exchange membrane in water at 100 ℃ is tested to be 4.8%, the conductivity is 50mS/cm, and the mechanical tensile property of the composite proton exchange membrane is tested to be 50MPa through a universal drawing machine.
The conductivity is obtained by an alternating current impedance method by using an electrochemical impedance tester, and the testing method is referred to national standard GB/T20042.3-2009.
The tensile test was carried out according to the method described in GB/T1040.3-2006.
The swelling test method refers to the national standard GB/T20042.3-2009.
Examples 2 to 4
Examples 2-4 provide composite proton exchange membranes and processes substantially the same as example 1, except as shown in table 1.
Example 5
The first porous enhancement layer is e-PTFE soaked in Nafion solution, the porosity is 60%, the thickness is 15 microns, and the pore diameter is 0.4 microns; the second porous enhancement layer is PVDF soaked in Nafion solution, the porosity is 80%, the thickness is 10 mu m, and the pore diameter is 0.8 mu m. And (3) the first porous enhancement layer and the second porous enhancement layer are bonded and hot-pressed to form a proton exchange membrane with the thickness of 10 mu m at the joint of the first porous enhancement layer and the second porous enhancement layer, so as to obtain the composite proton exchange membrane. The swelling rate of the composite proton exchange membrane in water at 100 ℃ is tested to be 4.8%, the conductivity is 50mS/cm, and the mechanical tensile property of the composite proton exchange membrane is tested to be 50MPa through a universal drawing machine.
The conductivity is obtained by an alternating current impedance method by using an electrochemical impedance tester, and the testing method is referred to national standard GB/T20042.3-2009.
The tensile test was carried out according to the method described in GB/T1040.3-2006.
The swelling test method refers to the national standard GB/T20042.3-2009.
Examples 6 to 7
Examples 6-7 provide composite proton exchange membranes and processes substantially the same as example 5, except as shown in table 1.
TABLE 1 composite proton exchange membranes of examples 1-7 and performance test results
Comparative example 1
Testing the conductivity, tensile property and swelling ratio of a Nafion-HP composite membrane purchased from Heson electric appliances, wherein the conductivity is obtained by an alternating current impedance method through an electrochemical impedance tester, and the testing method refers to the national standard GB/T20042.3-2009; the tensile test is carried out according to the method in GB/T1040.3-2006; the swelling test method refers to the national standard GB/T20042.3-2009. The swelling ratio is 11%, the conductivity is 50mS/cm and the mechanical tensile property is 40 MPa.
The test results of table 1 and comparative example 1 show that the composite proton exchange membranes obtained in examples 1 to 7 have reduced swelling ratio and enhanced tensile properties while ensuring a certain conductivity, and are beneficial to improving the service life of the composite proton exchange membranes in fuel cells.
The above description is only exemplary of the present application and should not be taken as limiting the present application, as any modification, equivalent replacement, or improvement made within the spirit and principle of the present application should be included in the protection scope of the present application.
Claims (10)
1. A composite proton exchange membrane comprising:
a proton exchange membrane;
a first porous reinforcement layer disposed on an anode side of the proton exchange membrane;
a second porous reinforcement layer disposed on a cathode side of the proton exchange membrane;
the first porous reinforcing layer has a porosity less than a porosity of the second porous reinforcing layer.
2. The composite proton exchange membrane according to claim 1 wherein the first porous reinforcement layer has a pore size of 0.1-0.9 μm; and/or
The porosity of the first porous reinforcing layer is 40% -70%; and/or
The pore diameter of the second porous enhancement layer is 0.1-0.9 μm; and/or
The porosity of the second porous reinforcing layer is 71% -98%.
3. The composite proton exchange membrane according to claim 1 wherein the thickness of the first porous reinforcement layer and/or the second porous reinforcement layer is 1 μ ι η to 15 μ ι η.
4. The composite proton exchange membrane according to claim 1 wherein said first porous reinforcement layer is an e-PTFE reinforcement layer or a PVDF reinforcement layer; and/or
The second porous reinforced layer is an e-PTFE reinforced layer or a PVDF reinforced layer.
5. The composite proton exchange membrane according to any one of claims 1 to 4 wherein said first porous reinforcing layer is a first porous reinforcing layer containing a radical quencher; and/or
The second porous reinforcing layer is a second porous reinforcing layer containing a radical quencher.
6. The composite proton exchange membrane according to claim 5, wherein the radical quencher is at least one of radical quencher containing manganese element and radical quencher containing cerium element.
7. The composite proton exchange membrane according to any one of claims 1 to 4, wherein the first porous reinforcing layer is a first porous reinforcing layer containing perfluorosulfonic acid resin; and/or
The second porous reinforcing layer is a second porous reinforcing layer containing perfluorosulfonic acid resin.
8. The composite proton exchange membrane according to any one of claims 1 to 4 wherein the proton exchange membrane is a perfluorosulfonic acid proton exchange membrane.
9. The composite proton exchange membrane according to any one of claims 1 to 4 wherein the thickness of the proton exchange membrane is 5 μm to 50 μm.
10. A fuel cell comprising the composite proton exchange membrane of any one of claims 1 to 9.
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Cited By (2)
| Publication number | Priority date | Publication date | Assignee | Title |
|---|---|---|---|---|
| CN114843568A (en) * | 2021-02-01 | 2022-08-02 | 恒大新能源技术(深圳)有限公司 | Composite proton exchange membrane, preparation method thereof and fuel cell |
| CN114914503A (en) * | 2022-06-10 | 2022-08-16 | 中国第一汽车股份有限公司 | Membrane electrode for fuel cell and preparation method and application thereof |
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Cited By (2)
| Publication number | Priority date | Publication date | Assignee | Title |
|---|---|---|---|---|
| CN114843568A (en) * | 2021-02-01 | 2022-08-02 | 恒大新能源技术(深圳)有限公司 | Composite proton exchange membrane, preparation method thereof and fuel cell |
| CN114914503A (en) * | 2022-06-10 | 2022-08-16 | 中国第一汽车股份有限公司 | Membrane electrode for fuel cell and preparation method and application thereof |
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