CN119481087A - A proton exchange membrane fuel cell cathode and a membrane electrode comprising the same - Google Patents
A proton exchange membrane fuel cell cathode and a membrane electrode comprising the same Download PDFInfo
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- CN119481087A CN119481087A CN202510059432.8A CN202510059432A CN119481087A CN 119481087 A CN119481087 A CN 119481087A CN 202510059432 A CN202510059432 A CN 202510059432A CN 119481087 A CN119481087 A CN 119481087A
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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
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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
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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
- H01M8/00—Fuel cells; Manufacture thereof
- H01M8/10—Fuel cells with solid electrolytes
- H01M8/1004—Fuel cells with solid electrolytes characterised by membrane-electrode assemblies [MEA]
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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
- H01M2004/8678—Inert electrodes with catalytic activity, e.g. for fuel cells characterised by the polarity
- H01M2004/8689—Positive electrodes
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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
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Abstract
The invention belongs to the technical field of fuel cells, and particularly relates to a proton exchange membrane fuel cell cathode and a membrane electrode comprising the same. The cathode comprises a cathode gas diffusion layer and a cathode catalytic layer which are sequentially arranged from the outside to the inside in the direction of the proton exchange membrane, and further comprises a sulfur dioxide mass transfer barrier layer positioned at the outer side of the cathode gas diffusion layer, wherein the sulfur dioxide mass transfer barrier layer comprises a sulfur dioxide electro-oxidation catalyst and a resin binder with alkalinity, and the mass ratio of the sulfur dioxide electro-oxidation catalyst to the resin binder is 1:1-4:1. According to the invention, on-line removal of sulfur dioxide in the barrier layer is realized in a mode of alkaline resin adsorption-electrocatalyst oxidation, and mass transfer from the sulfur dioxide to the cathode catalytic layer is inhibited, so that poisoning effect of the sulfur dioxide on the cathode catalyst is reduced, the output performance of the fuel cell under direct supply of sulfur dioxide-containing air is remarkably improved, and the adaptability of the cell system to the running environment is further improved.
Description
Technical Field
The invention belongs to the technical field of fuel cells, and particularly relates to a proton exchange membrane fuel cell cathode and a membrane electrode comprising the same.
Background
The proton exchange membrane fuel cell can convert chemical energy in fuel into electric energy, has the advantages of green pollution-free, low noise, high energy conversion efficiency, quick start and the like, is widely regarded as an energy conversion device with the most application prospect, and is widely applied to the fields of transportation, household electric power, distributed power stations and the like. In practical use, compressed air is most commonly used as the cathode feed gas in view of cost and convenience. However, since sulfur dioxide combines with platinum more strongly than oxygen, the fuel cell platinum-based catalyst is very sensitive to sulfur dioxide, and trace amounts of sulfur dioxide in the air can cause irreversible performance degradation of the cell. To avoid the negative effects of sulfur dioxide, fuel cell systems mostly use purified air or pure oxygen as the cathode feed gas, which greatly increases the complexity and cost of the cell system.
At present, two main technical approaches for reducing the poisoning effect of sulfur dioxide are to optimize the catalyst, including alloying the platinum-based catalyst, adding metal oxide into the platinum-based catalyst, developing non-noble metal catalyst and the like. This approach is only in the laboratory stage and no widely accepted commercial sulfur dioxide poisoning resistant catalysts have been developed. And secondly, before the sulfur dioxide-containing air enters the cathode of the fuel cell, the air is firstly subjected to desulfurization treatment by an external purification device in a physical adsorption, chemical adsorption or electrochemical oxidation mode. The introduction of new structures, however, can result in increased volume and weight of the battery system, which can increase not only the complexity and cost of the fuel cell system, but also the difficulty of integration with other electronic devices.
Disclosure of Invention
The invention aims to provide a proton exchange membrane fuel cell cathode and a membrane electrode comprising the same, which do not need an external purification device, realize the online removal of sulfur dioxide in a barrier layer in a sulfur dioxide mass transfer barrier layer by an alkaline resin adsorption-catalyst oxidation mode, inhibit the mass transfer of sulfur dioxide to a cathode catalytic layer, obviously improve the output performance under the supply of a cathode containing sulfur dioxide, and further improve the adaptability of a fuel cell system to the running environment.
In order to achieve the above object, the technical scheme of the present invention is as follows:
The invention provides a cathode of a proton exchange membrane fuel cell, which comprises a cathode gas diffusion layer and a cathode catalytic layer which are sequentially arranged from outside to inside in the direction of a proton exchange membrane, and also comprises a sulfur dioxide mass transfer barrier layer positioned at the outer side of the cathode gas diffusion layer;
The sulfur dioxide mass transfer barrier layer comprises a sulfur dioxide electro-oxidation catalyst and a resin binder with alkalinity, wherein the mass ratio of the sulfur dioxide electro-oxidation catalyst to the resin binder is 1:1-4:1.
Further, the cathode gas diffusion layer comprises cathode carbon paper and a cathode microporous layer which are sequentially arranged from the outside to the direction of the internal proton exchange membrane.
Further, the sulfur dioxide mass transfer barrier layer is coated on the outer surface of the cathode support layer, and the coating comprises spraying, knife coating, brush coating or screen printing.
Further, the sulfur dioxide electrooxidation catalyst comprises one or a combination of more of a carbon-supported metal material, a carbon material and a doped carbon material, wherein the doped carbon material comprises one or a combination of more of a nitrogen-doped carbon material, an oxygen-doped carbon material, a nitrogen and oxygen co-doped carbon material, a metal-doped carbon material and a metal and nitrogen co-doped carbon material, the carbon-supported metal material comprises Pt/C or Au/C, and the carbon material comprises carbon nano tubes, carbon fibers or carbon powder.
Further, the resin binder with alkalinity comprises one or more of TP-85, TP-100, fumion FAA, sustainion, piperION.
Further, the loading capacity of the sulfur dioxide electrooxidation catalyst in the sulfur dioxide mass transfer barrier layer is 0.1-0.5 mg cm -2.
In another aspect, the invention provides a proton exchange membrane fuel cell membrane electrode comprising a cathode, a proton exchange membrane and an anode which are sequentially stacked, wherein the cathode is the cathode.
Further, the anode comprises an anode gas diffusion layer and an anode catalytic layer which are sequentially arranged from the outside to the inside in the direction of the proton exchange membrane.
Further, the anode gas diffusion layer comprises anode carbon paper and an anode microporous layer which are sequentially arranged from the outside to the direction of the internal proton exchange membrane.
The invention also provides a fuel cell comprising the membrane electrode.
Compared with the prior art, the invention has the beneficial effects that:
(1) The cathode and the membrane electrode comprising the cathode provided by the invention construct a sulfur dioxide mass transfer barrier layer integrally laminated with cathode gas diffusion by using the sulfur dioxide electrocatalyst with conductivity and the resin binder with alkalinity on the premise of not increasing the additional structure of the fuel cell and hardly increasing the volume and the mass of the cell, thereby fully ensuring the simplicity and portability of the cell structure.
(2) The resin component with alkalinity is used as a binder and is also used as a site for adsorbing acid sulfur dioxide gas, so that mass transfer of sulfur dioxide to a catalytic layer is inhibited. Meanwhile, the conductive sulfur dioxide electrooxidation catalyst can further oxidize the trapped sulfur dioxide, release sites for absorbing sulfur dioxide in the resin, and repeat a new round of capture-oxidation in the barrier layer. Therefore, the cooperative cooperation of the alkaline resin and the electro-oxidation catalyst realizes continuous and effective online oxidation removal of sulfur dioxide in the barrier layer.
(3) The adaptive range of the membrane electrode to the working environment improves the output power of the membrane electrode under the supply of the air containing sulfur dioxide, and the fuel cell adopting the membrane electrode structure is insensitive to the gas supplied by the cathode, and the direct supply of the air containing sulfur dioxide does not cause the obvious change of the output performance of the cell.
Drawings
FIG. 1 is a schematic view of a membrane electrode according to the present invention;
In the figure, 1, a cathode, 2, a proton exchange membrane, 3, an anode, 4 and a sulfur dioxide mass transfer barrier layer;
101. Cathode carbon paper 102, cathode microporous layer 103, cathode catalytic layer 301, anode carbon paper 302, anode microporous layer 303, anode catalytic layer;
Fig. 2 shows the performance comparison of the PEMFC assembled by the membrane electrodes of example 1, example 3, and example 4 and the membrane electrode of comparative example 1 under different cathode supplies, a being comparative example 1, b being example 1, c being example 3, and d being example 4.
Detailed Description
The technical solutions of the present invention will be clearly and completely described below with reference to the accompanying drawings and examples, and it is apparent that the described examples are only some, but not all, of the examples of the invention, and all other examples obtained by those skilled in the art without making any inventive effort are within the scope of the present invention.
Unless otherwise indicated, all materials used in the examples of the present invention were commercially available or prepared according to conventional methods well known to those skilled in the art.
The invention provides a proton exchange membrane fuel cell membrane electrode, the structure of which is shown in figure 1, comprising an anode 3, a proton exchange membrane 2 and a cathode 1 which are sequentially stacked, wherein the cathode 1 comprises a cathode gas diffusion layer and a cathode catalytic layer 103 which are sequentially arranged from the outside to the inside in the direction of the proton exchange membrane 2, the cathode 2 also comprises a sulfur dioxide mass transfer barrier layer 4 positioned at the outer side of the cathode gas diffusion layer, and the anode 3 comprises an anode gas diffusion layer and an anode catalytic layer 303 which are sequentially arranged from the outside to the inside in the direction of the proton exchange membrane.
In one embodiment of the invention, the cathode 1 comprises cathode carbon paper 101, a cathode microporous layer 102 and a cathode catalytic layer 103 which are sequentially arranged from outside to inside in the direction of the proton exchange membrane 2, the sulfur dioxide mass transfer barrier layer 4 is positioned on the outer side of the cathode carbon paper 101, and the anode 3 comprises anode carbon paper 301, an anode microporous layer 302 and an anode catalytic layer 303 which are sequentially arranged from outside to inside in the direction of the proton exchange membrane.
Example 1
As shown in figure 1, a membrane electrode of a proton exchange membrane fuel cell is constructed by adopting nickel-nitrogen co-doped carbon (Ni-N-C), and the preparation method of the membrane electrode comprises the following steps:
dissolving 5mg Ni-N-C in 5ml of absolute ethyl alcohol solution, then adding 25 mg of 5wt.% TP-100 solution as a binder and interception sites of a sulfur dioxide mass transfer barrier layer to obtain barrier layer ink, wherein a cathode gas diffusion layer consists of 5wt.% of hydrophobic carbon paper (Toray TGP-H-060) with PTFE content of 40wt.% and a microporous layer with PTFE content of 1 mg cm -2 supported by carbon powder Vulcan XC-72, the barrier layer ink is sprayed on one side of the outer surface of carbon paper with an area of 5 cm by 5 cm, the loading amount of Ni-N-C in the sulfur dioxide mass transfer barrier layer 4 is 0.1 mg cm -2, the mass fraction of TP-100 in the barrier layer ink solid is 20%, an anode gas diffusion layer consists of 5wt.% of hydrophobic carbon paper (Toray TGP-H-060) with PTFE content of 40wt.%, the microporous layer with the loading amount of 1 mg cm -2 supported by the Vulcan XC-72, a cathode gas diffusion layer, a catalyst coated Nafion 211 membrane (anode and a cathode catalyst are 1/2.37.24℃), and a membrane is formed by stacking membrane forming after the anode gas diffusion layer and the anode gas diffusion layer are carried by 4 for 2.4 minutes, and the anode gas diffusion layer is carried by MPa, and the anode gas diffusion layer is carried by 4 minutes, and the anode gas diffusion layer is carried by 4, and the anode gas diffusion layer is carried by 4, and the anode gas is carried by 4 is 4 and the anode gas is coated by 4 and has 2 and has 2.is coated.
Example 2
The sulfur dioxide mass transfer barrier layer was constructed using nickel-nitrogen co-doped carbon (Ni-N-C), and the membrane electrode was prepared in the same manner as in example 1, except that 100 mg of a 5 wt.% TP-100 solution was used as the resin binder having basicity, and the mass ratio of the sulfur dioxide electro-oxidation catalyst to the resin binder was 1:1.
Example 3
The sulfur dioxide mass transfer barrier layer was constructed using nickel-nitrogen co-doped carbon (Ni-N-C), and the membrane electrode was prepared in the same manner as in example 1, except that 12.5 mg of Ni-N-C, 125 mg wt.% TP-100 solution was used, the loading of Ni-N-C in the sulfur dioxide mass transfer barrier layer 4 was 0.25: 0.25 mg cm -2, and the mass ratio of the electro-oxidation catalyst to the resin binder was 2:1.
Example 4
The sulfur dioxide mass transfer barrier layer is constructed by adopting carbon powder Vulcan XC-72, and the preparation method of the membrane electrode comprises the following steps:
Dissolving 25 mg Vulcan XC-72 in 5ml of absolute ethanol solution, then adding 500 mg of 5wt.% TP-100 solution as a binder and a trapping site of a sulfur dioxide mass transfer barrier layer to obtain barrier layer ink, wherein a cathode gas diffusion layer is formed by 5wt.% of hydrophobic-treated carbon paper (Toray TGP-H-060) with PTFE content of 40wt.% and a microporous layer with PTFE content of 1 mg cm -2 of carbon powder Vulcan XC-72, the barrier layer ink is sprayed on one side of the outer surface of the carbon paper with an area of 5cm by 5cm, the loading amount of the Vulcan XC-72 in the sulfur dioxide mass transfer barrier layer 4 is 0.5 mg cm -2, the mass fraction of TP-100 in the barrier layer ink solid is 50%, an anode gas diffusion layer is formed by 5wt PTFE hydrophobically treated ay TGP-H-060 and a microporous layer with PTFE content of 40wt.%, the loading amount of 1 mg cm -2 of the carbon powder Vulcan XC-72, a cathode gas diffusion layer, a catalyst-coated Nafion film (anode and cathode catalyst are 5 cm/5 cm) and a anode gas diffusion layer (anode and cathode catalyst are 5.5.5.5.5229), and a film forming film is carried by hot pressing and a film is carried under the conditions of mg cm -2.0.2 ℃ for 0.2 minutes, respectively.
Example 5
The preparation method of the membrane electrode comprises the following steps of:
Dissolving 5 mg Pt/C in 5ml of absolute ethanol solution, adding 100mg of 5wt.% TP-100 as a binder and a trapping site of a sulfur dioxide mass transfer barrier layer to obtain barrier layer ink, forming a cathode gas diffusion layer by 5wt.% of carbon paper subjected to PTFE hydrophobic treatment (Toray TGP-H-060) and a microporous layer with PTFE content of 40wt.% and carbon powder Vulcan XC-72 carrying capacity of 1 mg cm -2, spraying the barrier layer ink on one side of the outer surface of the carbon paper with 5 cm by 5 cm, carrying capacity of Pt/C in the sulfur dioxide mass transfer barrier layer 4 of 0.1 mg cm -2, and forming a film by using TP-100 in the barrier layer ink solid at a mass fraction of 50%, forming an anode gas diffusion layer by 5wt.% of PTFE hydrophobically treated Toray TGP-H-060 and a microporous layer with PTFE content of 40wt.%, carrying capacity of 1 mg cm -2 by Vulcan XC-72, coating a Nafion 211 film (anode and cathode catalyst carrying capacity of Pt/C of 0.54 and mg cm -2 respectively), and carrying capacity of anode gas of MPa at a film forming temperature of 0.2.140 DEG after film forming and MPa in turn, and stacking the film in sequence.
Example 6
The sulfur dioxide mass transfer barrier layer was constructed using carbon-supported platinum (Pt/C), and the membrane electrode was prepared in the same manner as in example 5, except that TP-85 was used as the basic resin.
Example 7
The sulfur dioxide mass transfer barrier layer was constructed using carbon-supported platinum (Pt/C) and the membrane electrode was prepared in the same manner as in example 5, except that Fumion FAA was used as the resin binder having basicity.
Example 8
The sulfur dioxide mass transfer barrier layer is constructed by adopting carbon-supported platinum (Pt/C), and the membrane electrode adopts the same preparation method as in the example 5, wherein the difference is that the adopted resin binder with alkalinity is Sustainion.
Example 9
The sulfur dioxide mass transfer barrier layer is constructed by adopting carbon-supported platinum (Pt/C), and the membrane electrode adopts the same preparation method as in the example 5, wherein the difference is that the adopted resin binder with alkalinity is piperION.
Comparative example 1
A proton exchange membrane fuel cell membrane electrode comprises an anode, a proton exchange membrane and a cathode which are sequentially stacked, wherein the cathode comprises cathode carbon paper, a cathode micropore layer and a cathode catalytic layer which are sequentially arranged in the direction of the proton exchange membrane from outside to inside, and the anode comprises anode carbon paper, an anode micropore layer and an anode catalytic layer which are sequentially arranged in the direction of the proton exchange membrane from outside to inside.
The cathode gas diffusion layer consists of 5wt.% of carbon paper (Toray TGP-H-060) subjected to hydrophobic treatment with PTFE and a microporous layer with the PTFE content of 40wt.% and the carbon powder Vulcan XC-72 loading of 1mg cm -2, the anode gas diffusion layer consists of 5wt wt.% of microporous layer with the Toray TGP-H-060 subjected to hydrophobic treatment with PTFE and the PTFE content of 40wt.% and the carbon powder Vulcan XC-72 loading of 1mg cm -2, and the cathode gas diffusion layer, the catalyst-coated Nafion 211 film (anode and cathode catalysts are Pt/C catalysts with the loading of 0.2 mg cm -2 and 0.4 mg cm -2 respectively) and the anode gas diffusion layer are sequentially stacked and then hot pressed for 2 minutes at 140 ℃ and 0.1MPa to prepare the film electrode.
Test example 1
The membrane electrodes of examples 1, 3 and 4 and comparative example 1 were assembled into a fuel cell for performance evaluation under the conditions of a cell operating temperature of 80℃and a back pressure of 0.1MPa, anode and cathode gas flows of 0.2L/min and 0.8L/min, respectively, anode humidification of 100% and cathode humidification of 30% RH.
As shown in fig. 2, the conventional membrane electrode structure cell (fig. 2 a) of comparative example 1 was significantly degraded after the air containing sulfur dioxide was introduced, and could not withstand poisoning effect of ppm sulfur dioxide. The performance of example 1 and example 3 is superior to that of example 4, and the fuel cells of the membrane electrode structures of example 1 (fig. 2 b) and example 3 (fig. 2 c) of the present invention are insensitive to cathode supply gas, and direct supply of sulfur dioxide-containing air does not cause significant change in cell output performance, which proves that the membrane electrode structures of the present invention can improve the adaptability of the fuel cell system to the operating environment. The fuel cell of example 4 (fig. 2 d) with the membrane electrode structure had slightly reduced performance after passing through air containing 10ppm sulfur dioxide.
Furthermore, it should be understood that although the present disclosure describes embodiments, not every embodiment is provided with a separate embodiment, and that this description is provided for clarity only, and that the disclosure is not limited to the embodiments described in detail below, and that the embodiments described in the examples may be combined as appropriate to form other embodiments that will be apparent to those skilled in the art.
Claims (10)
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| US20060240295A1 (en) * | 2003-12-24 | 2006-10-26 | Bridgestone Corporation And Toshiba Fuel Cell Power Systems Corporation | Method and device for decontamination air for fuel cell, and fuel cell |
| CN102527187A (en) * | 2010-12-29 | 2012-07-04 | 中国科学院大连化学物理研究所 | A method of removing SO2 in the air by using an external voltage |
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