CN111342062A - Supported fuel cell catalyst and application thereof - Google Patents
Supported fuel cell catalyst and application thereof Download PDFInfo
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- CN111342062A CN111342062A CN202010128942.3A CN202010128942A CN111342062A CN 111342062 A CN111342062 A CN 111342062A CN 202010128942 A CN202010128942 A CN 202010128942A CN 111342062 A CN111342062 A CN 111342062A
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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
- H01M4/90—Selection of catalytic material
- H01M4/9075—Catalytic material supported on carriers, e.g. powder carriers
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- H—ELECTRICITY
- H01—ELECTRIC ELEMENTS
- H01M—PROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
- H01M4/00—Electrodes
- H01M4/86—Inert electrodes with catalytic activity, e.g. for fuel cells
- H01M4/88—Processes of manufacture
- H01M4/8825—Methods for deposition of the catalytic active composition
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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
- H01M4/90—Selection of catalytic material
- H01M4/9075—Catalytic material supported on carriers, e.g. powder carriers
- H01M4/9083—Catalytic material supported on carriers, e.g. powder carriers on carbon or graphite
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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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- Y—GENERAL TAGGING OF NEW TECHNOLOGICAL DEVELOPMENTS; GENERAL TAGGING OF CROSS-SECTIONAL TECHNOLOGIES SPANNING OVER SEVERAL SECTIONS OF THE IPC; TECHNICAL SUBJECTS COVERED BY FORMER USPC CROSS-REFERENCE ART COLLECTIONS [XRACs] AND DIGESTS
- Y02—TECHNOLOGIES OR APPLICATIONS FOR MITIGATION OR ADAPTATION AGAINST CLIMATE CHANGE
- Y02E—REDUCTION OF GREENHOUSE GAS [GHG] EMISSIONS, RELATED TO ENERGY GENERATION, TRANSMISSION OR DISTRIBUTION
- Y02E60/00—Enabling technologies; Technologies with a potential or indirect contribution to GHG emissions mitigation
- Y02E60/30—Hydrogen technology
- Y02E60/50—Fuel cells
Abstract
The invention discloses a supported fuel cell catalyst and application thereof, wherein the catalyst for a fuel cell comprises a carrier, noble metal nano-particles are loaded on the carrier, and the catalyst has better performance under different current densities through the special design of the carrier.
Description
Technical Field
The invention relates to a catalyst for a fuel cell and application thereof, in particular to a supported fuel cell catalyst and application thereof.
Background
A fuel cell is a chemical device that directly converts chemical energy of fuel into electrical energy, and is also called an electrochemical generator. It is a fourth power generation technology following hydroelectric power generation, thermal power generation and atomic power generation. The fuel cell has the advantages of high efficiency, environmental protection and the like, and is the most promising power generation technology from the viewpoint of energy conservation and ecological environment protection.
The main components of the fuel cell are: electrodes (electrodes), electrolyte membranes (electrolemmers), Current collectors (Current collectors), and the like. The electrode is an electrochemical reaction site where the fuel undergoes an oxidation reaction and the oxidant undergoes a reduction reaction, and the key to the performance of the electrode is the performance of the catalyst (catalyst), the material of the electrode, the manufacturing process of the electrode, and the like. As one of the fuel cells, a Proton Exchange Membrane Fuel Cell (PEMFC) has advantages of high efficiency and cleanliness, is a promising cell, and can be widely used for mobile power sources and portable power sources.
The catalysts used in PEMFCs are typically nanoscale Pt and its alloy particles supported on carbon materials, their support materials such as carbon nanotubes, carbon particles, etc. In certain cases of catalysts, the performance and durability are directly related to the loading of the catalyst. However, catalyst particles are expensive metals and are not an economical option to increase the amount of catalyst used to provide fuel cell performance. Efficient use of expensive catalytic particles is a necessary option in order to reduce costs without affecting the performance of the fuel cell.
It is believed that the catalytic efficiency of Pt and its alloy particles is related to the degree of uniformity of their dispersion and also to their location in the MEA. In the prior art, the utilization efficiency of alloy particles is improved mainly by improving the dispersion uniformity degree of the alloy particles and the like. Further research, such as the research progress of applying the core-shell structure catalyst to the oxygen reduction of the proton exchange membrane fuel cell [ J ] in physical chemistry report, 2016,32(10): 2462-. These techniques are complex and, although the amount of precious metal can be reduced to some extent, they impose more stringent requirements on the manufacturing process, resulting in the same high manufacturing costs, which cannot be effectively reduced. The specific use effect of the composition is yet to be further verified.
Weiziwan, the research progress of proton exchange membrane fuel cell catalyst performance enhancement methods [ J ]. chemical progress, 2016,35(09) ]. Another improved design and preparation of novel catalyst materials and methods for improving catalyst activity or stability are introduced, including surface modification, coating, alloying, modulation of geometric and electronic structures and crystal structures, catalyst/carrier interaction, and other means.
There is no known theory of the interaction between the various materials or components of a fuel cell, particularly the effect on catalytic activity. The existing research shows that when the amount of Pt loaded on the cathode of the MEA is lower than 0.1mg/cm2When the current density is more than 1.5A/cm2In the case of (2), there can be a significant loss of performance due to oxygen conduction problems attributed to the Pt nanoparticles locally. Although studies have shown that this problem can be largely overcome by removing the ionomer from the surface of the Pt nanoparticles in 3M nanostructured thin films (NSTF), it is not clear whether this should be attributed to the film itself (structural reorganization of the polymer) or to the adsorption of anions on the surface of the Pt nanoparticles. It is also well known that sulfonate anions bind to the surface of Pt nanoparticles, and that binding can have a significant impact on Pt-based oxidation activity and performance at low current densities. It is clear that avoiding direct contact of Pt with the ionomer is important to improve the activity of the catalyst, but the ionomer is necessary for proton conduction to the reaction site and contact with Pt nanoparticles is unavoidable.
Disclosure of Invention
The invention aims to overcome the defects of the prior art and provides a supported fuel cell catalyst and application thereof.
The technical scheme adopted by the invention is as follows:
in a first aspect of the present invention, there is provided:
a catalyst for fuel cell comprises a carrier on which noble metal nanoparticles are supported,
the particle size or diameter of the carrier is not more than 250nm, and a plurality of pores with the pore diameter of not more than 25nm are formed on the outer wall; and
the diameter of the noble metal nano-particles is not more than 200nm, the shortest distance between the noble metal nano-particles and the outer wall of the carrier is not more than 125nm, and interpenetrating networks are arranged among the noble metal nano-particles.
In some examples of the catalyst, the noble metal nanoparticles have a diameter of 2 to 6 nm.
In some catalyst examples, the noble metal is Pt and/or alloys thereof.
In some examples of the catalyst, the carrier has a particle size or diameter of 20 to 200nm, or 25 to 180nm, 30 to 150nm, 30 to 100 nm.
In some examples of the catalyst, the pores on the outer wall of the carrier have a pore diameter of 5 to 20nm, or 5 to 18nm, 5 to 15nm, or 5 to 10 nm.
In some examples of catalysts, the support is mesoporous carbon nanoparticles or carbon nanotubes; preferably, the length of the carbon nanotube is 20 to 200nm, or 25 to 180nm, 30 to 150nm, 30 to 100 nm.
In a second aspect of the present invention, there is provided:
an MEA for a proton exchange membrane fuel cell having a catalyst of the first aspect of the invention in a catalytic layer.
In some examples of MEA, the catalyst is added in an amount of 0.05 to 0.4mg/cm2。
In a third aspect of the present invention, there is provided:
a fuel cell having a catalyst according to the first aspect of the invention, or an MEA according to the second aspect of the invention.
The invention has the beneficial effects that:
in the catalyst of some examples of the invention, the distance between the noble metal nanoparticles and the ionomer is proper, the ionomer is difficult to directly contact with the noble metal nanoparticles in the using process, and simultaneously protons are easy to conduct to the catalytic core mainly comprising the noble metal nanoparticles, so that the utilization efficiency of the catalytic active particles can be well improved, and the catalyst of some examples of the invention is less in use amount under the condition of obtaining the same catalytic performance.
Meanwhile, the catalyst of some embodiments of the invention has better catalytic performance under different current densities, and the catalytic activity of the catalyst is not easy to lose.
Drawings
FIG. 1 is a TEM image of a typical mesoporous carbon nano-meter;
FIG. 2 is a schematic illustration of catalysts of different support structures;
FIG. 3 is a polarization curve for catalyst (a) and catalyst (b);
FIG. 4 is a kinetic voltage loss decay analysis of catalyst (a) and catalyst (b);
FIG. 5 is a resistance voltage loss decay analysis of catalyst (a) and catalyst (b);
FIG. 6 is a mass transfer voltage loss attenuation analysis of catalyst (a) and catalyst (b);
FIG. 7 is a polarization curve for catalyst (a) and catalyst (c);
FIG. 8 is a kinetic voltage loss decay analysis of catalyst (a) and catalyst (c);
FIG. 9 is a resistance voltage loss decay analysis of catalyst (a) and catalyst (c);
FIG. 10 is a mass transfer voltage loss attenuation analysis of catalyst (a) and catalyst (c);
fig. 11 is a polarization curve of catalyst (a), catalyst (b) and catalyst (c).
Detailed Description
In a first aspect of the present invention, there is provided:
a catalyst for fuel cell comprises a carrier on which noble metal nanoparticles are supported,
the particle size or diameter of the carrier is not more than 250nm, and a plurality of pores with the pore diameter of not more than 25nm are formed on the outer wall; and
the diameter of the noble metal nano-particles is not more than 200nm, the shortest distance between the noble metal nano-particles and the outer wall of the carrier is not more than 125nm, and interpenetrating networks are arranged among the noble metal nano-particles.
Therefore, the ionomer is away from the noble metal nanoparticles in the catalyst to a certain distance, so that the ionomer can be prevented from poisoning the noble metal nanoparticles in the using process, and can be easily contacted with protons. Not only ensures the stability of the catalytic performance of the catalyst, but also ensures the catalyst to have higher catalytic activity.
In some examples of the catalyst, the noble metal nanoparticles have a diameter of 2 to 6 nm.
The noble metal is a noble metal commonly used in fuel cells, and has no particular requirement per se. In some catalyst examples, the noble metal is Pt and/or alloys thereof.
In some examples of the catalyst, the carrier has a particle size or diameter of 20 to 200nm, or 25 to 180nm, 30 to 150nm, 30 to 100 nm.
In some examples of the catalyst, the pores on the outer wall of the carrier have a pore diameter of 5 to 20nm, or 5 to 18nm, 5 to 15nm, or 5 to 10 nm.
In some examples of catalysts, the support is mesoporous carbon nanoparticles or carbon nanotubes; preferably, the length of the carbon nanotube is 20 to 200nm, or 25 to 180nm, 30 to 150nm, 30 to 100 nm.
In a second aspect of the present invention, there is provided:
an MEA for a proton exchange membrane fuel cell having a catalyst of the first aspect of the invention in a catalytic layer.
In some examples of MEA, the catalyst is added in an amount of 0.05 to 0.4mg/cm2。
In a third aspect of the present invention, there is provided:
a fuel cell having a catalyst according to the first aspect of the invention, or an MEA according to the second aspect of the invention.
The technical scheme of the invention is further explained by combining the examples.
The carrier used in the present invention, such as mesoporous carbon nanoparticles or carbon nanotubes, may be prepared according to conventional methods or may be commercially available. The mesoporous carbon nanoparticles can be prepared according to the method described in CN105129765A or other known methods.
A TEM image of a typical mesoporous carbon nanoparticle is shown in fig. 2. The nanoparticles have a diameter of less than 200nm and a pore size of about 8nm on the walls.
The noble metal nanoparticles may be obtained by mixing a noble metal salt with a carrier, followed by in-situ reduction. An exemplary mesoporous carbon nanoparticle supported catalyst was prepared as follows:
1) dispersing 0.1g of mesoporous carbon nanoparticles in 20mL of acetone, and performing ultrasonic dispersion;
2) adding 80mg of H under ultrasonic oscillation2PtCl6Ultrasonically dispersing for 1h, and then continuously stirring for 6 h;
3) after acetone is volatilized, the load H is carried2PtCl6The mesoporous carbon nano-particles are in Ar/H2And (95/5, v/v) heating to 450 ℃ under the protection of airflow, preserving heat for 2h, and cooling to obtain the catalyst.
Preparation of a noble metal nanoparticle catalyst supported by carbon nanotubes:
1) 1.85g (NH)4)6Mo7O24.4H2O and 0.732g Fe (NO)3)3.9H2Dissolving O in ultrapure water, adding 1.22g of MgO, and fully stirring;
2) adding 4g of citric acid after 1 hour, and carrying out moderate ultrasonic dispersion and stirring to obtain a mixture;
3) charging the mixture into a reaction furnace, N2Treating at 550 deg.C for 2h under atmosphere to obtain brown powder;
4) introduction of H2Reducing the powder in the reaction furnace at 900 ℃ for 1h, and cooling to room temperature under the protection of protective gas to obtain a carbon nano tube catalyst;
5) filling carbon nanotube catalyst into CVD chamber, blowing CH at 750-1000 deg.C at constant rate4And C2H4Preparing the carbon nano tube with the diameter of about 8-20 nm and the length of about 200 nm;
6) and (3) loading Pt nano particles in the carbon nano tube by referring to the preparation of the mesoporous carbon nano particle loaded catalyst to obtain the catalyst for the fuel cell.
And (3) performance testing:
catalysts with different carrier structures (as shown in figure 2) are respectively selected to be prepared into a standard fuel cell. Catalyst (a) (case (a)) is a conventional graphite-type catalyst; catalyst (b) (case (b)) is a high surface area type catalyst; catalyst (c) (case (c)) and catalyst (d) (case (d)) are two catalysts of the present invention.
The performance of the test piece was measured by using the standard voltage loss attenuation analysis (standard voltage loss analysis of MEAP), and the results are shown in FIGS. 3 to 6. FIG. 3 is a polarization curve for catalyst (a) and catalyst (b); FIGS. 4-6 are voltage loss attenuation analyses of catalyst (a) and catalyst (b), kinetic, resistance and mass transfer analyses, respectively.
The results show that catalyst (b) has a higher initial activity (A/cm) than catalyst (a)2) Since the Pt nanoparticles in the catalyst (b) are located in the pores of the carbon nanoparticles, it is not easy to contact with the ionomer and neutralize. However, at high current densities, the performance of catalyst (b) is poor because the distance of the Pt nanoparticles from the ionomer is too large, which results in limited proton conduction.
As shown in FIGS. 3 to 6, both the catalyst (a) and the catalyst (b) were insufficient. In contrast, the catalyst of the present invention can overcome the problems faced by it (ionomer poisoning and mass transfer limitations of Pt nanoparticles within the narrow pores) simultaneously. To further demonstrate the advantages of catalyst (c) of the present invention, it was compared in performance with catalyst (a) and catalyst (b). The results are shown in FIGS. 7 to 11. FIGS. 7 and 11 are polarization curves, and FIGS. 8-10 are kinetic, resistance and mass transfer analyses, respectively, of voltage loss attenuation.
The results show that the catalyst (c) of the invention has better performance at different current densities.
Claims (9)
1. A catalyst for a fuel cell, comprising a carrier on which noble metal nanoparticles are supported, characterized in that:
the particle size or diameter of the carrier is not more than 250nm, and a plurality of pores with the pore diameter of not more than 25nm are formed on the outer wall; and
the diameter of the noble metal nano-particles is not more than 200nm, the shortest distance between the noble metal nano-particles and the outer wall of the carrier is not more than 125nm, and interpenetrating networks are arranged among the noble metal nano-particles.
2. The catalyst for a fuel cell according to claim 1, characterized in that: the diameter of the noble metal nano-particles is 2-6 nm.
3. The catalyst for a fuel cell according to claim 1, characterized in that: the noble metal is Pt and/or an alloy thereof.
4. The catalyst for a fuel cell according to claim 1, characterized in that: the particle size or diameter of the carrier is 20-200 nm.
5. The catalyst for a fuel cell according to claim 1, characterized in that: the pore diameter of the pores on the outer wall of the carrier is 5-20 nm.
6. The catalyst for a fuel cell according to claim 1 or 4, characterized in that: the carrier is mesoporous carbon nano particles or carbon nano tubes; preferably, the length of the carbon nanotube is 20 to 200 nm.
7. An MEA for a proton exchange membrane fuel cell, comprising: a catalyst layer of the MEA has the catalyst for a fuel cell according to claim 1 therein.
8. The MEA of claim 7, wherein: in the catalyst layer, the addition amount of the catalyst is 0.05-0.4 mg/cm2。
9. A fuel cell, characterized by: having a catalyst according to claims 1 to 6, or an MEA according to claim 7 or 8.
Applications Claiming Priority (2)
| Application Number | Priority Date | Filing Date | Title |
|---|---|---|---|
| CN201911010644 | 2019-10-23 | ||
| CN2019110106448 | 2019-10-23 |
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| CN111342062A true CN111342062A (en) | 2020-06-26 |
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Citations (6)
| Publication number | Priority date | Publication date | Assignee | Title |
|---|---|---|---|---|
| CN1921195A (en) * | 2006-08-17 | 2007-02-28 | 武汉理工大学 | Proton superpolymer modified fuel cell catalyst using carbon as carrier and its preparation |
| CN105789648A (en) * | 2016-05-15 | 2016-07-20 | 河北工业大学 | Three-dimensional ordered bimodal mesoporous carbon supported Pt catalyst and preparation method thereof |
| KR20170088156A (en) * | 2016-01-22 | 2017-08-01 | 한국과학기술연구원 | Non-platinum catalyst for fuel cell and method of preparing the same |
| WO2018104775A2 (en) * | 2016-12-09 | 2018-06-14 | Toyota Jidosha Kabushiki Kaisha | Electrode catalyst for fuel cell, method of producing the same, and fuel cell |
| CN108232214A (en) * | 2016-12-09 | 2018-06-29 | 丰田自动车株式会社 | Electrode catalyst, preparation method and the fuel cell of fuel cell |
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-
2020
- 2020-02-28 CN CN202010128942.3A patent/CN111342062A/en active Pending
Patent Citations (6)
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| CN1921195A (en) * | 2006-08-17 | 2007-02-28 | 武汉理工大学 | Proton superpolymer modified fuel cell catalyst using carbon as carrier and its preparation |
| KR20170088156A (en) * | 2016-01-22 | 2017-08-01 | 한국과학기술연구원 | Non-platinum catalyst for fuel cell and method of preparing the same |
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| WO2018104775A2 (en) * | 2016-12-09 | 2018-06-14 | Toyota Jidosha Kabushiki Kaisha | Electrode catalyst for fuel cell, method of producing the same, and fuel cell |
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Address after: 528599 workshop, No. 25, Xingliang Road, Hecheng street, Gaoming District, Foshan City, Guangdong Province Applicant after: Guangdong Taiji Power Technology Co.,Ltd. Address before: 528599 No.4 factory building, No.1 HuiFu Road, Hecheng street, Gaoming District, Foshan City, Guangdong Province Applicant before: Guangdong Taiji Power Technology Co.,Ltd. |
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