WO2022145771A1 - 연료전지용 촉매층, 이의 제조 방법, 이를 포함하는 막-전극 접합체 및 연료전지 - Google Patents
연료전지용 촉매층, 이의 제조 방법, 이를 포함하는 막-전극 접합체 및 연료전지 Download PDFInfo
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- WO2022145771A1 WO2022145771A1 PCT/KR2021/018237 KR2021018237W WO2022145771A1 WO 2022145771 A1 WO2022145771 A1 WO 2022145771A1 KR 2021018237 W KR2021018237 W KR 2021018237W WO 2022145771 A1 WO2022145771 A1 WO 2022145771A1
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- Prior art keywords
- catalyst layer
- fuel cell
- catalyst
- electrode
- heat dissipation
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Images
Classifications
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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
- H01M8/1016—Fuel cells with solid electrolytes characterised by the electrolyte material
- H01M8/1018—Polymeric electrolyte materials
-
- 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
-
- 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
-
- 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
- H01M4/8668—Binders
-
- 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
- H01M4/8673—Electrically conductive fillers
-
- 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
-
- 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
- H01M4/8828—Coating with slurry or ink
-
- 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
- H01M4/8878—Treatment steps after deposition of the catalytic active composition or after shaping of the electrode being free-standing body
- H01M4/8892—Impregnation or coating of the catalyst layer, e.g. by an ionomer
-
- 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
- H01M4/00—Electrodes
- H01M4/86—Inert electrodes with catalytic activity, e.g. for fuel cells
- H01M4/90—Selection of catalytic material
- H01M4/92—Metals of platinum group
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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
- H01M4/92—Metals of platinum group
- H01M4/925—Metals of platinum group supported on carriers, e.g. powder carriers
- H01M4/926—Metals of platinum group 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
-
- 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]
-
- 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
- H01M2008/1095—Fuel cells with polymeric electrolytes
-
- 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
Definitions
- the present invention relates to a catalyst layer for a fuel cell, a method for manufacturing the same, a membrane-electrode assembly including the same, and a fuel cell.
- a fuel cell is a power generation system that directly converts the chemical reaction energy of hydrogen and oxygen contained in hydrocarbon-based substances such as methanol, ethanol, and natural gas into electrical energy.
- a typical example of such a fuel cell is a polymer electrolyte fuel cell (PEMFC).
- PEMFC polymer electrolyte fuel cell
- the PEMFC is in the spotlight as a next-generation energy source, and research for commercialization is being actively conducted due to its advantages such as an eco-friendly image in automobile-related fields.
- a membrane-electrode assembly that substantially generates electricity is an anode electrode (also called an anode or oxidation electrode) with a polymer electrolyte membrane including a hydrogen ion conductive polymer interposed therebetween. and a cathode electrode (also called an air electrode or a cathode electrode) have a structure in which they are located.
- Each electrode is composed of a catalyst, an ionomer, a solvent, and an additive, and among these components, the catalyst is a major factor determining the activity and durability of a fuel cell.
- Another object of the present invention is to provide a membrane-electrode assembly including the catalyst layer.
- Another object of the present invention is to provide a fuel cell including the membrane-electrode assembly.
- Another object of the present invention is to provide a method for preparing the catalyst layer.
- a catalyst layer for a fuel cell includes a catalyst, a heat dissipation material, and an ionomer.
- the catalyst may include a support and metal particles supported on the support.
- the carrier may include at least one selected from the group consisting of carbon black, Ketjen black, porous carbon, carbon fiber, carbon nanotube, carbon nanohorn, and graphene.
- the metal particles may include platinum or a platinum-based alloy.
- the heat dissipation material may be adjacent to the catalyst and may be irregularly distributed in the catalyst layer.
- the heat dissipation material may include one or more selected from the group consisting of ceramic nanoparticles, ultrahigh molecular weight polyethylene (UHMWPE), and polyacetylene.
- UHMWPE ultrahigh molecular weight polyethylene
- polyacetylene polyacetylene
- the ceramic nanoparticles may include at least one selected from the group consisting of boron nitride, aluminum nitride, aluminum oxide, silicon carbide, and beryllium oxide.
- the ceramic nanoparticles may have an average diameter of 10 to 500 nm.
- the thickness of the catalyst layer may be 1 to 15 ⁇ m.
- a membrane-electrode assembly includes an anode electrode; cathode electrode; and an ion exchange membrane positioned between the anode electrode and the cathode electrode, wherein at least one of the anode electrode and the cathode electrode includes the catalyst layer.
- a fuel cell according to another embodiment of the present invention includes the membrane-electrode assembly.
- a method for manufacturing a catalyst layer for a fuel cell includes preparing an electrode slurry including a catalyst, a heat dissipation material, an ionomer, and a dispersion medium; forming a slurry layer by coating the electrode slurry on a substrate; and removing the dispersion medium from the slurry layer.
- the dispersion medium may be 80 wt% to 95 wt% based on the total weight of the electrode slurry.
- the heat dissipation material may be 0.1 to 15% by weight based on the total weight of the electrode slurry.
- the weight ratio of the catalyst and the heat radiation material may be 5:1 to 20:1, and the weight ratio of the catalyst and the ionomer may be 10:1 to 2:3.
- the preparing of the electrode slurry includes homogeneous mixing, and the homogeneous mixing may be performed using any one selected from the group consisting of a ball mill, a powder mixer, and a resonance acoustic mixer.
- the catalyst layer of the present invention includes a heat dissipation material, heat generated due to the exothermic reaction in the catalyst layer is efficiently discharged to the outside, thereby suppressing the deterioration of the membrane-electrode assembly due to the temperature rise of the catalyst layer.
- FIG. 1 is a TEM photograph of an electrode manufactured according to an embodiment of the present invention.
- FIG 2 is an SEM photograph of an electrode manufactured according to an embodiment of the present invention.
- FIG. 3 is a schematic cross-sectional view of a membrane-electrode assembly according to an embodiment of the present invention.
- FIG. 4 is a schematic diagram illustrating an overall configuration of a fuel cell according to an embodiment of the present invention.
- preferred refers to an embodiment of the invention that has certain advantages under certain conditions. However, other embodiments may also be preferred under the same or different conditions. Furthermore, one or more preferred embodiments do not mean that other embodiments are not useful, nor do they exclude other embodiments that are within the scope of the present invention.
- the term "comprises” is used to enumerate materials, compositions, devices, and methods useful in the present invention and is not limited to the enumerated examples.
- a catalyst layer for a fuel cell according to an embodiment of the present invention includes a catalyst, a heat dissipation material, and an ionomer.
- the catalyst may include any metal particles that can be used as a catalyst for a hydrogen oxidation reaction and an oxygen reduction reaction, and may preferably include a platinum-based metal.
- the platinum-based metal is platinum (Pt), palladium (Pd), ruthenium (Ru), iridium (Ir), osmium (Os), platinum-M alloy (wherein M is palladium (Pd), ruthenium (Ru), iridium ( Ir), osmium (Os), gallium (Ga), titanium (Ti), vanadium (V), chromium (Cr), manganese (Mn), iron (Fe), cobalt (Co), nickel (Ni), copper ( Cu), silver (Ag), gold (Au), zinc (Zn), tin (Sn), molybdenum (Mo), tungsten (W), any one selected from the group consisting of lanthanum (La) and rhodium (Rh) above) and combinations thereof, and more preferably, a combination
- the platinum-based alloy is (i) Pt-Co, Pt-Pd, Pt-Mn, Pt-Sn, Pt-Mo, Pt-Cr, Pt-W, Pt-Ir, Pt-Ru, Pt- Binary alloys such as Ni, Pt-Fe, (ii) Pt-Ru-W, Pt-Ru-Ni, Pt-Ru-Mo, Pt-Ru-Ir, Pt-Co-Mn, Pt- Co-Ni, Pt-Co-Fe, Pt-Co-Ir, Pt-Co-S, Pt-Co-P, Pt-Fe-Ir, Pt-Fe-S, Pt-Fe-P, Pt-Au- ternary alloys such as Co, Pt-Au-Fe, Pt-Au-Ni, Pt-Ni-Ir, Pt-Cr-Ir, or (iii) Pt-Ru-Rh-Ni, Pt
- the metal particles and the heat dissipation material of the catalyst may be used in an unsupported state, but the fact that the metal particles of the catalyst are supported on the carrier can prevent a decrease in surface area due to aggregation of the metal particles and the heat dissipation material. Therefore, in the catalyst layer, the catalyst may include a support and metal particles supported on the support, and it is preferable for the heat dissipation material to be irregularly distributed in the catalyst layer adjacent to the catalyst in terms of the catalytic efficiency of the catalyst layer and the heat dissipation efficiency of the heat dissipation material. .
- the carrier may be selected from a carbon-based carrier, a porous inorganic oxide such as zirconia, alumina, titania, silica, ceria, or zeolite.
- the carbon-based carrier is super P, carbon fiber (carbon fiber), carbon sheet (carbon sheet), carbon black (carbon black), Ketjen Black (Ketjen Black), acetylene black (acetylene black), carbon nanotubes (carbon nano tube, CNT), carbon sphere (carbon sphere), carbon ribbon (carbon ribbon), fullerene (fullerene), graphene, may be selected from activated carbon and one or more combinations thereof, but is not limited thereto, Carriers usable in the technical field of the present invention can be used without limitation.
- the carrier is a carbon-based material, and containing one of carbon black, ketjen black, carbon nanotubes, and graphene may help facilitate electron exchange with the catalyst.
- the carrier has a specific surface area of 50 m 2 /g or more or 50 to 1200 m 2 /g, and an average of 10 to 300 nm or 20 to 200 nm It is preferable to have a particle size.
- the catalyst metal particles and the heat dissipation material supported on the support may be positioned on the surface of the support, or may penetrate into the support while filling the internal pores of the support.
- the heat dissipation material helps to efficiently transfer thermal energy due to an exothermic reaction occurring on the catalyst surface to the outside of the catalyst layer.
- the heat dissipation material may specifically include one or more selected from the group consisting of ceramic nanoparticles, ultrahigh molecular weight polyethylene (UHMWPE), and polyacetylene.
- UHMWPE ultrahigh molecular weight polyethylene
- polyacetylene the heat dissipation function can be further improved by using it together with the ceramic nanoparticles.
- the ceramic nanoparticles may be one or more selected from the group consisting of boron nitride, aluminum nitride, aluminum oxide, silicon carbide, and beryllium oxide. have.
- the ceramic nanoparticles are supported on the carrier to increase the surface area of the catalyst layer and have excellent thermal conductivity, thereby having an effect of easily transferring heat to the outside of the catalyst layer and an effect of inhibiting evaporation of moisture in the catalyst layer. Therefore, it is preferable that the ceramic nanoparticles have an average diameter of 10 to 500 nm, and when it is larger than the above range, the increase in surface area due to the large particles is insignificant, so it may be difficult to properly impart a heat dissipation effect. Alternatively, agglomeration may occur around the catalyst, thereby deteriorating the function of the catalyst.
- the heat dissipation material may be used including ultrahigh molecular weight polyethylene (UHMWPE) having a weight average molecular weight (Mw) of 3,500,000 to 10,500,000.
- UHMWPE ultrahigh molecular weight polyethylene
- Mw weight average molecular weight
- the UHMWPE is included in the catalyst layer to increase the tensile strength of the catalyst layer, has water repellency to easily discharge moisture generated from the catalyst layer to the outside, and quickly transfers heat generated in the catalyst layer to the outside through a long chain can play a role in making
- the heat dissipation material When polyacetylene is included as the heat dissipation material, an excellent electrical conduction effect and a heat dissipation effect can be realized at the same time.
- the polyacetylene having a long chain with a weight average molecular weight (Mw) of 20,000 to 1,000,000 is advantageous for efficiently discharging heat inside the catalyst layer, but is not limited to the molecular weight.
- the ionomer may be a cation conductor having a cation exchange group such as a proton, or an anion conductor having an anion exchange group such as a hydroxy ion, carbonate or bicarbonate.
- a cation conductor having a cation exchange group such as a proton
- an anion conductor having an anion exchange group such as a hydroxy ion, carbonate or bicarbonate.
- an ionomer generally used in a fuel cell may be used.
- the cation exchange group may be any one selected from the group consisting of a sulfonic acid group, a carboxyl group, a boronic acid group, a phosphoric acid group, an imide group, a sulfonimide group, a sulfonamide group, and combinations thereof, and generally a sulfonic acid group or a carboxyl group have.
- the cationic conductor may include a fluorine-based polymer including the cation exchange group and including fluorine in a main chain; Benzimidazole, polyamide, polyamideimide, polyimide, polyacetal, polyethylene, polypropylene, acrylic resin, polyester, polysulfone, polyether, polyetherimide, polyester, polyethersulfone, polyetherimide, poly hydrocarbon polymers such as carbonate, polystyrene, polyphenylene sulfide, polyetheretherketone, polyetherketone, polyarylethersulfone, polyphosphazene or polyphenylquinoxaline; partially fluorinated polymers such as polystyrene-graft-ethylenetetrafluoroethylene copolymer or polystyrene-graft-polytetrafluoroethylene copolymer; sulfone imides and the like.
- the polymers may include a cation exchange group selected from the group consisting of a sulfonic acid group, a carboxylic acid group, a phosphoric acid group, a phosphonic acid group, and derivatives thereof in a side chain, Specific examples include poly(perfluorosulfonic acid), poly(perfluorocarboxylic acid), a copolymer of tetrafluoroethylene and fluorovinyl ether containing a sulfonic acid group, defluorinated sulfurized polyether ketone, or mixtures thereof.
- a cation exchange group selected from the group consisting of a sulfonic acid group, a carboxylic acid group, a phosphoric acid group, a phosphonic acid group, and derivatives thereof in a side chain
- Specific examples include poly(perfluorosulfonic acid), poly(perfluorocarboxylic acid), a copolymer of tetrafluoroethylene and fluorovinyl ether
- a fluorine-based polymer comprising; Sulfonated polyimide (S-PI), sulfonated polyarylethersulfone (S-PAES), sulfonated polyetheretherketone (SPEEK), sulfonated polybenzimi Sulfonated polybenzimidazole (SPBI), sulfonated polysulfone (S-PSU), sulfonated polystyrene (S-PS), sulfonated polyphosphazene, sulfonated poly Sulfonated polyquinoxaline, sulfonated polyketone, sulfonated polyphenylene oxide, sulfonated polyether sulfone, sulfonated polyether ketone polyether ketone), sulfonated polyphenylene sulfone, sulfonated polyphenylene sulfide, sulfonated polyphenylene sulfide sulf
- the cation conductor may substitute Na, K, Li, Cs or tetrabutylammonium for H in the cation exchange group at the end of the side chain.
- NaOH is substituted during the preparation of the carbon structure composition, and when tetrabutylammonium is substituted with tetrabutylammonium hydroxide, K, Li or Cs is also used.
- Substitution may be made using an appropriate compound. Since the substitution method is widely known in the art, a detailed description thereof will be omitted herein.
- the cationic conductor may be used in the form of a single substance or a mixture, and may optionally be used together with a non-conductive compound for the purpose of further improving adhesion to the ion exchange membrane. It is preferable to use the amount adjusted to suit the purpose of use.
- non-conductive compound examples include polytetrafluoroethylene (PTFE), tetrafluoroethylene-hexafluoropropylene copolymer (FEP), tetrafluoroethylene-perfluoroalkylvinyl ether copolymer (PFA), ethylene/tetrafluoro ethylene/tetrafluoroethylene (ETFE), ethylene chlorotrifluoro-ethylene copolymer (ECTFE), polyvinylidene fluoride, polyvinylidene fluoride-hexafluoropropylene copolymer (PVdF-HFP), dode At least one selected from the group consisting of silbenzenesulfonic acid and sorbitol may be used.
- PTFE polytetrafluoroethylene
- FEP tetrafluoroethylene-hexafluoropropylene copolymer
- PFA tetrafluoroethylene-perfluoroalkylvinyl ether copo
- the anion conductor is a polymer capable of transporting anions such as hydroxy ions, carbonate or bicarbonate, and the anion conductor is commercially available in the form of a hydroxide or halide (usually chloride), and the anion conductor is an industrial essence (water purification), metal separation or carbon structure process, etc. can be used.
- a polymer doped with a metal hydroxide may be used in general, and specifically, poly(ethersulfone) doped with a metal hydroxide, polystyrene, vinyl-based polymer, poly(vinyl chloride), poly(vinylidene fluoride) , poly(tetrafluoroethylene), poly(benzimidazole), or poly(ethylene glycol) may be used.
- the fluorine-based polymer may be, for example, a perfluorosulfonic acid (PFSA)-based polymer or a perfluorocarboxylic acid (PFCA)-based polymer, but is not limited thereto.
- PFSA perfluorosulfonic acid
- PFCA perfluorocarboxylic acid
- the ionomer may have a weight average molecular weight of 240 g/mol to 200,000 g/mol, specifically 240 g/mol to 10,000 g/mol.
- the thickness of the catalyst layer according to an embodiment of the present invention is 1 to 15 ⁇ m.
- the durability of the catalyst layer may be greatly deteriorated.
- the thickness of the catalyst layer is thicker than the above range, The mass transfer of the catalyst layer is deteriorated, and thus performance may be deteriorated or the thickness of the fuel cell may be increased.
- a membrane-electrode assembly includes an anode electrode and a cathode electrode positioned opposite to each other, and an ion exchange membrane positioned between the anode electrode and the cathode electrode, the anode electrode, the cathode electrode, and the Any one selected from the group consisting of both is to include the fuel cell catalyst layer as an electrode catalyst layer.
- the membrane-electrode assembly 100 includes the ion exchange membrane 50 and the electrodes 20 and 20 ′ respectively disposed on both surfaces of the ion exchange membrane 50 .
- the electrodes 20 and 20' include electrode substrates 40 and 40' and catalyst layers 30 and 30' formed on the surface of the electrode substrates 40 and 40', and the electrode substrates 40 and 40'. and a microporous layer (not shown) including conductive fine particles such as carbon powder and carbon black to facilitate material diffusion in the electrode substrates 40 and 40' between the catalyst layers 30 and 30'. It may include more.
- an oxidation reaction for generating hydrogen ions and electrons from fuel that is disposed on one surface of the ion exchange membrane 50 and transferred to the catalyst layer 30 through the electrode substrate 40 is performed.
- the causing electrode 20 is called an anode electrode, and it is disposed on the other side of the ion exchange membrane 50 and passes the hydrogen ions supplied through the ion exchange membrane 50 and the electrode substrate 40' to the catalyst layer 30')
- the electrode 20' that causes a reduction reaction to generate water from the oxidizing agent delivered to the oxidizer is called a cathode electrode.
- the anode electrode 20, the cathode electrode 20', and the catalyst layers 30 and 30' of any one electrode 20, 20' selected from the group consisting of both are one embodiment of the present invention described above.
- An electrode according to an example is included.
- a porous conductive substrate may be used so that hydrogen or oxygen can be smoothly supplied.
- Representative examples thereof include carbon paper, carbon cloth, carbon felt, or metal cloth (a porous film composed of a fibrous metal cloth or a metal film formed on the surface of a cloth formed of polymer fibers) ) can be used, but is not limited thereto.
- the fluorine-based resin includes polytetrafluoroethylene, polyvinylidene fluoride, polyhexafluoropropylene, polyperfluoroalkyl vinyl ether, polyperfluorosulfonylfluoride alkoxyvinyl ether, fluorinated ethylene propylene ( Fluorinated ethylene propylene), polychlorotrifluoroethylene, or a copolymer thereof may be used.
- the fuel cell according to an embodiment of the present invention includes the membrane-electrode assembly and may be, for example, a fuel cell using hydrogen gas as a fuel.
- FIG. 4 is a schematic diagram showing the overall configuration of the fuel cell.
- the fuel cell 200 includes a fuel supply unit 210 for supplying a mixed fuel in which fuel and water are mixed, and a reformer for generating reformed gas including hydrogen gas by reforming the mixed fuel ( 220), a stack 230 in which a reformed gas including hydrogen gas supplied from the reformer 220 causes an electrochemical reaction with an oxidizing agent to generate electrical energy, and an oxidizing agent to the reformer 220 and the stack It includes an oxidizing agent supply unit 240 for supplying to (230).
- the stack 230 induces an oxidation/reduction reaction of a reformed gas containing hydrogen gas supplied from the reforming unit 220 and an oxidizing agent supplied from the oxidizing agent supply unit 240 to generate electrical energy.
- Each unit cell refers to a unit cell for generating electricity, and includes the membrane-electrode assembly for oxidizing/reducing oxygen in the reformed gas containing hydrogen gas and the oxidizing agent, and the reforming gas containing hydrogen gas and an oxidizing agent. and a separator (also referred to as a bipolar plate, hereinafter referred to as a 'separator plate') for supplying the membrane-electrode assembly.
- the separator is disposed on both sides of the membrane-electrode assembly at the center. In this case, the separation plates respectively positioned on the outermost side of the stack are specifically referred to as end plates.
- a supply pipe 232 is provided, and the other end plate includes a first discharge pipe 233 for discharging reformed gas including hydrogen gas remaining unreacted in the plurality of unit cells to the outside;
- a second discharge pipe 234 for discharging the unreacted and remaining oxidizing agent to the outside is provided.
- a catalyst layer manufacturing method comprises the steps of preparing an electrode slurry including a catalyst, a heat dissipation material, an ionomer and a dispersion medium: coating the electrode slurry on a substrate to form a slurry layer; and removing the dispersion medium from the slurry layer.
- the dispersion medium may be a solvent selected from the group consisting of water, a hydrophilic solvent, an organic solvent, and a mixture thereof.
- the hydrophilic solvent is one selected from the group consisting of alcohols, ketones, aldehydes, carbonates, carboxylates, carboxylic acids, ethers and amides containing a linear, branched, saturated or unsaturated hydrocarbon having 1 to 12 carbon atoms as a main chain. It may have more than one functional group, and these may include an alicyclic or aromatic cyclo compound as at least a part of the main chain.
- the alcohol examples include methanol, ethanol, isopropyl alcohol, ethoxy ethanol, n-propyl alcohol, butyl alcohol, 1,2-propanediol, 1-pentanol, 1.5-pentanediol, 1.9-nonanediol; Ketones include heptanone, octanone, and the like; Aldehydes include benzaldehyde, tolualdehyde and the like; Esters include methylpentanoate, ethyl-2-hydroxypropanoate, and the like; Examples of the carboxylic acid include pentanoic acid, heptanoic acid, and the like; Ethers include methoxybenzene, dimethoxypropane and the like; Amides include propanamide, butylamide, and dimethylacetamide.
- the organic solvent may be selected from N-methylpyrrolidone, dimethyl sulfoxide, tetrahydrofuran, and mixtures thereof.
- the dispersion medium may be contained in an amount of 80 wt% to 95 wt% based on the total weight of the electrode slurry, and when it is less than 80 wt%, the solid content is too high to cause cracking and high viscosity during electrode coating There may be a dispersion problem due to, and if it exceeds 95% by weight, it may be detrimental to electrode activity.
- the heat dissipation material is preferably 0.1 to 15% by weight based on the total weight of the electrode slurry. If the heat dissipation material is less than 0.1% by weight based on the total weight of the electrode slurry, it may be difficult for the heat dissipation material to effectively perform a heat dissipation function.
- the catalyst may be surrounded by the heat dissipation material having poor conductivity, or the ionomer may wrap the heat dissipation material instead of the catalyst, so that the chemical reaction does not occur smoothly on the catalyst surface and the electrical resistance of the catalyst layer increases.
- the heat dissipation material has less weight than the catalyst in relation to the catalyst, and more specifically, the weight ratio of the catalyst and the heat dissipation material is 5:1 to 20 It is preferably :1.
- the ratio of the heat-dissipating material is high compared to the weight range, the amount of the catalyst is reduced and the fuel cell performance may be deteriorated. There may be problems that cannot be done.
- the weight ratio of the catalyst and the ionomer is preferably 10:1 to 2:3, but is not limited thereto.
- the content of the ionomer (ionomer) is less than the above range compared to the catalyst.
- ions are not properly transferred to the electrolyte membrane, and when the content of the ionomer is greater than that of the catalyst, the gas permeation is blocked and the performance of the membrane-electrode assembly is deteriorated.
- the preparing of the electrode slurry includes homogeneous mixing, and the homogeneous mixing may be performed using any one selected from the group consisting of a ball mill, a powder mixer, and a resonance acoustic mixer.
- the homogeneous mixing of the catalyst slurry including the catalyst, the heat dissipation material, the ionomer and the dispersion medium may be mixed using any one selected from the group consisting of a ball mill, a powder mixer, and a resonance acoustic mixer, preferably a homogenizer and a resonance acoustic mixer It can be mixed by mixing.
- the resonant acoustic mixer applies low-frequency acoustic energy to the catalyst slurry composition to perform resonant vibratory mixing.
- the acoustic energy is supplied by periodic linear displacement of a vessel filled with the catalyst slurry composition, and for this purpose, a plurality of mechanical or electronic transducer arrangements are used, and more Specifically, it includes oscillator drives that transfer vibrations and accelerations to the vessel and a flexible elastic member such as a spring.
- the resonant mixing may be performed for 30 seconds to 30 minutes, and specifically, for a short time of 1 minute to 10 minutes. If the resonant mixing time is less than 30 seconds, less mixing or coating properties may not be confirmed, and if it exceeds 30 minutes, the sample or composition may be changed.
- a slurry layer is formed by coating the electrode slurry on a substrate.
- the electrode slurry composition is continuously or intermittently transferred to a coater and then uniformly applied to the substrate with a dry thickness of 1 to 15 ⁇ m.
- a coater such as a die, gravure, bar, comma coater, etc. continuously through a pump according to the viscosity of the electrode slurry composition
- slot die coating , bar coating, comma coating, screen printing, spray coating, doctor blade coating, brush, etc. are used to uniformly coat the catalyst layer with a dry thickness of 1 ⁇ m to 15 ⁇ m on the decal film and pass through a drying furnace maintained at a constant temperature. and evaporate the dispersion medium.
- the catalyst content is small and the activity may be decreased. can do.
- the drying process may be drying at 25 °C to 1200 °C for 12 hours or more. If the drying temperature is less than 25 °C and the drying time is less than 12 hours, there may be a problem that a sufficiently dried catalyst layer may not be formed. .
- the method of applying and drying the electrode slurry is not limited to the above.
- the method may further include cutting the dried catalyst layer and the substrate to a required size and bonding to the ion exchange membrane.
- a catalyst layer was prepared in the same manner as in Example, except that no heat dissipation material was added and 10 g of a platinum catalyst was dispersed in a mixed solution of water and N-propanol.
- FIG. 1 is a picture taken with a transmission electron microscope (TEM) of the catalyst layer of Example prepared through Preparation Example.
- TEM transmission electron microscope
- FIG. 2 is a SEM cross-sectional analysis of the membrane-electrode assembly prepared after coating the electrode including the catalyst layer of the embodiment including the heat dissipation material on the release film. Most of the heat dissipation materials exist in the form of random particles, but there is also agglomeration between particles. In FIG. 2, a portion of the heat dissipation material of the catalyst layer is indicated by a circle, and it can be confirmed that some heat dissipation material is present in the electrode layer.
- reaction heat and radical generation of the fuel cell increase, the size of the catalyst increases, and corrosion of the carrier occurs.
- the electrode (Example) to which the heat dissipation material is added according to the embodiment of the present invention effectively radiates heat within the cell, and thus has excellent durability performance after 10,000 cycles.
- stack 231 first supply pipe
- second discharge pipe 240 oxidizing agent supply unit
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Abstract
Description
Claims (17)
- 촉매, 방열 소재 및 이오노머를 포함하는 연료전지용 촉매층.
- 제1항에 있어서,상기 촉매는 담체 및 상기 담체에 담지된 금속 입자를 포함하는 것을 특징으로 하는 연료전지용 촉매층.
- 제2항에 있어서,상기 담체는 카본블랙, 케첸블랙, 다공성 탄소, 탄소섬유, 탄소나노튜브, 탄소나노혼 및 그래핀으로 이루어진 군으로부터 선택된 하나 이상을 포함하는 것을 특징으로 하는 연료전지용 촉매층.
- 제2항에 있어서,상기 금속 입자는 백금 또는 백금계 합금을 포함하는 것을 특징으로 하는 연료전지용 촉매층.
- 제1항에 있어서,상기 방열 소재는 상기 촉매와 인접하며 상기 촉매층 내에서 불규칙으로 분포되어 있는 것을 특징으로 하는 연료전지용 촉매층.
- 제1항에 있어서,상기 방열 소재는 세라믹 나노 입자, 초고분자량 폴리에틸렌(ultrahigh molecular weight polyethylene, UHMWPE) 및 폴리아세틸렌으로 이루어진 군으로부터 선택되는 하나 이상을 포함하는 것을 특징으로 하는 연료전지용 촉매층.
- 제6항에 있어서,상기 세라믹 나노 입자는 질화 붕소(Boron nitride), 질화 알루미늄(Aluminum nitride), 산화 알루미늄(Aluminum oxide), 탄화 규소(Silicon carbide) 및 산화 베릴륨(Beryllium oxide)으로 이루어진 군으로부터 선택되는 하나 이상을 포함하는 것을 특징으로 하는 연료전지용 촉매층.
- 제6항에 있어서,상기 세라믹 나노 입자는 평균 직경이 10 내지 500 nm인 것을 특징으로 하는 연료전지용 촉매층.
- 제1항에 있어서,상기 촉매층의 두께는 1 내지 15 ㎛인 것을 특징으로 하는 연료전지용 촉매층.
- 애노드 전극;캐소드 전극; 및상기 애노드 전극과 상기 캐소드 전극 사이에 위치하는 이온 교환막을 포함하며,상기 애노드 전극 및 상기 캐소드 전극 중 하나 이상은 제1항 내지 제9항 중 어느 한 항에 따른 촉매층을 포함하는 막-전극 접합체.
- 제10항에 따른 막-전극 접합체를 포함하는 연료전지.
- 촉매, 방열 소재, 이오노머 및 분산매를 포함하는 전극 슬러리를 준비하는 단계;상기 전극 슬러리를 기재 상에 코팅하여 슬러리층(slurry layer)을 형성하는 단계; 및상기 슬러리층으로부터 상기 분산매를 제거하는 단계;를 포함하는,연료전지용 촉매층의 제조방법.
- 제12항에 있어서,상기 전극 슬러리를 준비하는 단계에서, 상기 분산매는 상기 전극 슬러리 전체 중량에 대하여 80 중량% 내지 95 중량%인 것을 특징으로 하는 연료전지용 촉매층의 제조방법.
- 제12항에 있어서,상기 전극 슬러리를 준비하는 단계에서, 상기 방열 소재는 상기 전극 슬러리 전체 중량에 대하여 0.1 내지 15 중량%인 것을 특징으로 하는 연료전지용 촉매층의 제조방법.
- 제12항에 있어서,상기 전극 슬러리를 준비하는 단계에서, 상기 촉매와 방열 소재의 중량비는 5:1 내지 20:1인 것을 특징으로 하는 연료전지용 촉매층의 제조방법.
- 제12항에 있어서,상기 전극 슬러리를 준비하는 단계에서, 상기 촉매와 이오노머의 중량비는 10:1 내지 2:3인 것을 특징으로 하는 연료전지용 촉매층의 제조방법.
- 제12항에 있어서,상기 전극 슬러리를 준비하는 단계는 균질 혼합하는 단계를 포함하며,상기 균질 혼합하는 단계는 볼밀, 파우더 믹서 및 공명 음향 혼합기로 이루어지는 군에서 선택되는 어느 하나를 이용하여 혼합하는 것을 특징으로 하는 연료전지용 촉매층의 제조방법.
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US18/250,841 US20230411633A1 (en) | 2020-12-31 | 2021-12-03 | Catalyst layer for fuel cell, manufacturing method therefor, and membrane-electrode assembly and fuel cell which comprise same |
JP2023528341A JP2023550327A (ja) | 2020-12-31 | 2021-12-03 | 燃料電池用触媒層、その製造方法、それを含む膜-電極接合体及び燃料電池 |
EP21915569.4A EP4235876A1 (en) | 2020-12-31 | 2021-12-03 | Catalyst layer for fuel cell, manufacturing method therefor, and membrane-electrode assembly and fuel cell which comprise same |
CN202180079021.5A CN116472624A (zh) | 2020-12-31 | 2021-12-03 | 用于燃料电池的催化剂层、其制备方法以及包括该催化剂层的膜-电极组件和燃料电池 |
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2021
- 2021-12-03 EP EP21915569.4A patent/EP4235876A1/en active Pending
- 2021-12-03 KR KR1020210171870A patent/KR20220097235A/ko unknown
- 2021-12-03 JP JP2023528341A patent/JP2023550327A/ja active Pending
- 2021-12-03 CN CN202180079021.5A patent/CN116472624A/zh active Pending
- 2021-12-03 WO PCT/KR2021/018237 patent/WO2022145771A1/ko active Application Filing
- 2021-12-03 US US18/250,841 patent/US20230411633A1/en active Pending
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