CN109962248B - Preparation method of fuel cell catalyst with moisture retention function - Google Patents

Preparation method of fuel cell catalyst with moisture retention function Download PDF

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CN109962248B
CN109962248B CN201711427253.7A CN201711427253A CN109962248B CN 109962248 B CN109962248 B CN 109962248B CN 201711427253 A CN201711427253 A CN 201711427253A CN 109962248 B CN109962248 B CN 109962248B
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fuel cell
product
transition metal
water
stirring
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CN109962248A (en
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曾蓉
刘晓鹏
蒋利军
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GRIMN Engineering Technology Research Institute Co Ltd
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    • B—PERFORMING OPERATIONS; TRANSPORTING
    • B82—NANOTECHNOLOGY
    • B82Y—SPECIFIC USES OR APPLICATIONS OF NANOSTRUCTURES; MEASUREMENT OR ANALYSIS OF NANOSTRUCTURES; MANUFACTURE OR TREATMENT OF NANOSTRUCTURES
    • B82Y30/00—Nanotechnology for materials or surface science, e.g. nanocomposites
    • 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
    • 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
    • H01M4/9041—Metals or alloys
    • 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
    • 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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  • Crystallography & Structural Chemistry (AREA)
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Abstract

The invention discloses a preparation method of a fuel cell catalyst with a moisturizing function, which comprises the following steps: (1) dispersing a nano inorganic oxide in water, adding a surfactant, adjusting the pH value of the solution to 1-6, adding a transition metal salt after uniformly stirring, adding a reducing agent sodium borohydride or hydrazine hydrate after uniformly stirring, and reacting to obtain a transition metal-loaded inorganic oxide; (2) dispersing inorganic oxide loaded with transition metal in water or ethanol, adding nitrogen-containing organic matter, stirring and mixing uniformly, transferring into a high-pressure kettle, and heating at 100-200 ℃ for 1-72 hours; taking out and drying, heating to 500-1100 ℃ in an inert atmosphere, heating for 0.5-3 hours, and cooling to obtain a product; (3) dispersing the product of the step (2) in water or absolute ethyl alcohol, adding noble metal acid or salt, stirring and reacting for 0.5-5 hours, and cleaning and drying the product to obtain the final product.

Description

Preparation method of fuel cell catalyst with moisture retention function
Technical Field
The invention relates to a preparation method of a fuel cell catalyst with a moisturizing function, and belongs to the technical field of catalyst preparation.
Background
The fuel cell is a device for directly converting chemical energy into electric energy, and the core of the fuel cell is to adopt a catalyst to catalyze oxygen reduction and hydrogen oxidation or alcohol oxidation, formic acid oxidation and the like.
The fuel cell is facing the beginning of commercialization, and an important problem affecting the commercialization of the fuel cell is the cost of the fuel cell, the cost of the fuel cell control system is equivalent to the cost of the fuel cell stack, and any means for simplifying the fuel cell system can reduce the cost of the fuel cell system. Stable operation and fast response of the fuel cell are related to fast water-heat balance in the fuel cell, and the high performance advantage of the fuel cell is difficult to be exerted when the membrane electrode of the fuel cell is in a water-flooded or dry environment. Therefore, the improvement of the moisture retention capability of the membrane electrode per se and the reduction of the dependence of the fuel cell on water can improve the operation stability of the fuel cell on one hand and greatly simplify the control system of the fuel cell on the other hand, and the improvement is an important direction for the development of the fuel cell.
A hydrophilic carbon microporous layer (s.hirakata et al, Electrochimica Acta 120, 240-247, 2014) is added between the catalytic layer and the carbon microporous layer of the fuel cell membrane electrode, which is more favorable for water removal due to smaller micropore size, and can keep water in the membrane electrode under the condition of low humidity due to the hydrophilic characteristic of the microporous layer, so that the method for obtaining the self-humidifying membrane electrode is provided.
SiO2、TiO2、ZnO、ZrO2、WO3、ZrO2-SiO2Inorganic oxide of importance such as (Zr/Si ═ 0.5), and nano-compound α -ZrP and Cs having proton conducting function2.5H0.5PWO40Heteropolyacids, and functionalized multiwall carbon nanotubes (MWCNTs), montmorillonite (MMT), zeolites, SiO2And the like are commonly used as humectants to be added into proton exchange membrane catalytic layers (R.Zeng et al, electrochemical Acta, 52, 3895-. Thohalin et al (L.Chen et al, int.J.hydrogen Energy, 37, 4694-2Interaction with Nafion solution forms ordered SiO2With the Nafion composite membrane, the proton conductivity of the composite membrane is improved, particularly under the condition of low humidity, the composite membrane still shows good proton conductivity, the moisture retention of the proton exchange membrane is improved, and the proton conductivity at high temperature (higher than 100 ℃) is improved.
Lorveya (Lorveya et al. cell, 40(3), 127-3985, 2010), Hagihara (H. Hagihara et al, Electrochimica Acta 51, 3979-3985, 2006) and the like, a small amount of nano platinum particles are added into a proton exchange membrane, and hydrogen and oxygen which pass through the membrane are catalyzed by platinum to react to generate water in the membrane, so that the water content and proton conductivity of the proton exchange membrane are maintained under a dry environment, and the stable operation of a fuel cell is ensured.
The inorganic oxide and other nano compounds adopted in the prior art have poor conductivity, and if the inorganic oxide and other nano compounds are used in a catalytic layer or a carbon microporous layer, the resistance of a prepared membrane electrode is increased, and the performance of a fuel cell is reduced.
Disclosure of Invention
In view of the problems in the prior art, the invention aims to provide a preparation method of a fuel cell catalyst with a moisture retention function.
In order to achieve the purpose, the invention adopts the following technical scheme:
a preparation method of a fuel cell catalyst with a moisture retention function comprises the following steps:
(1) dispersing nano inorganic oxide in water, adding a surfactant, adjusting the pH value of the solution to 1-6, uniformly stirring, adding one or more transition metal salts, uniformly stirring, adding a reducing agent sodium borohydride or hydrazine hydrate, and reducing and depositing metal on the surface of the inorganic oxide; washing the product with absolute ethyl alcohol or water for several times, and drying to obtain the transition metal-loaded inorganic oxide;
(2) dispersing inorganic oxide loaded with transition metal in water or ethanol, adding nitrogen-containing organic matter, stirring and mixing uniformly, transferring into a high-pressure kettle, and heating at 100-200 ℃ for 1-72 hours; taking out and drying, heating to 500-1100 ℃ in an inert atmosphere for 0.5-3 hours; then, cooling to below 50 ℃, and taking out a product;
(3) dispersing the product in the step (2) in water or absolute ethyl alcohol, stirring uniformly, adding noble metal acid or salt, stirring for reaction for 0.5-5 hours, filtering and washing the product, and washing the product for 0.5-2 hours at room temperature-100 ℃ by using dilute acid; and washing with water, and drying to obtain the final product.
Preferably, after the noble metal acid or salt is added in the step (3), sodium borohydride or hydrazine hydrate reducing agent is added, and the reaction is stirred for 0.5 to 2 hours.
In the present invention, the transition metal salt is a nitrate, chloride or sulfate of a transition metal; the transition metal is iron, cobalt, nickel or copper, and the noble metal is platinum, gold, silver or palladium.
In the present invention, the surfactant is an anionic surfactant containing a sulfonic acid group or a carboxylic acid group, or an amphoteric surfactant including sodium dodecylbenzenesulfonate, sodium dodecylsulfonate, sodium octane sulfonate, sodium vinyl sulfonate, sodium citrate or acacia.
The nitrogen-containing organic matter is glucose, urea, melamine, dicyandiamide, hexamethylenediamine, polyvinylpyrrolidone, polyaniline or polypyrrole and other nitrogen-containing organic micromolecules or macromolecules.
Preferably, in the step (1), the concentration of the transition metal salt is 0.001-1.0 mol/L, and the mass fraction of the surfactant in the solution is 0.001-5%.
Preferably, in the step (1) or the step (3), the molar ratio of the amount of the sodium borohydride or the hydrazine hydrate added in the reaction to the amount of the transition metal salt or the noble metal salt is (1-10) to 1.
Preferably, in the step (2), the mass ratio of the transition metal-loaded inorganic oxide to the nitrogen-containing organic compound is (50-0.001): 1.
In the invention, the mass of the noble metal in the obtained catalyst is 0-70% of the mass of the catalyst.
The invention has the beneficial effects that:
the invention adjusts Zeta potential on the surface of inorganic oxide by adjusting pH value of solution and the kind and concentration of surfactant, improves dispersibility of inorganic oxide nano-particles, meanwhile, inorganic transition metal ions are enriched on the surface of nano inorganic oxide due to electrostatic interaction, and the transition metal is deposited on the surface of nano inorganic oxide under the action of reducing agent to form a shell layer. On the basis, a nitrogen-doped graphene layer is coated on a nano inorganic oxide transition metal shell layer through hydrothermal reaction and high-temperature treatment, and the nano catalyst loaded with noble metal or the catalyst coated with a noble metal shell layer to form a multi-layer core-shell structure is prepared by taking the nitrogen-doped graphene layer as a carrier.
The invention takes the nano inorganic oxide as the catalyst carrier, so that the water generated by the reaction of the fuel cell can quickly leave the surface of the catalyst, and the water is locked in the nano inorganic oxide, so that the water is stored in the catalyst layer, and the ionic conductivity of the catalyst layer and the proton exchange membrane under the low humidity condition is improved, thereby improving the performance of the membrane electrode. Meanwhile, the surface of the nano inorganic oxide is coated with the nitrogen-doped graphene, so that the conductivity of the nano inorganic oxide, the stability of the loaded nano noble metal particles or shell layers in an electrochemical environment are improved, and the catalytic activity of the catalyst is improved.
Drawings
FIG. 1 is a diagram showing the change in the structure of a catalyst in the production process of the present invention.
Detailed Description
The invention is further illustrated with reference to the following figures and examples. It should be emphasized that the following examples are merely illustrative and are not intended to limit the scope of the invention and its application.
Example 1
Preparing 200mL of 0.025mol/L silicon dioxide solution, then adding 0.05% sodium dodecyl sulfate by mass fraction, adding hydrochloric acid to adjust the pH value of the solution to 3, stirring uniformly, adding 0.025mol/L CoCl2And (3) uniformly stirring 200mL of the solution, adding 0.05mol/L of sodium borohydride, reacting for 2 hours under stirring, enabling the solution to turn black, enabling a reaction product to be a black precipitate, filtering or centrifugally separating the precipitate, washing the reaction product with water for multiple times, and drying at 50 ℃.
Taking 1g of the product and 1g of melamine, dispersing the product in absolute ethyl alcohol, reacting for 72 hours at 200 ℃ in a high-pressure kettle, taking out and drying the product, heating to 900 ℃ under an inert atmosphere, keeping the temperature for 2 hours, then cooling to below 50 ℃, and taking out the product.
Taking 0.5g of the product, dispersing in 200mL of absolute ethyl alcohol, adding 1.25g of chloroplatinic acid, adding 0.386g of sodium borohydride, stirring for reaction for 1 hour, washing the reaction product with water for multiple times, washing with diluted acid at 80 ℃, then washing with water for multiple times, and drying at 50 ℃. The catalyst of structure "2" in FIG. 1 was obtained.
Example 2
Preparing 200mL of 0.05mol/L silicon dioxide solution, then adding sodium dodecyl sulfate with the mass fraction of 0.1%, and adding hydrochloric acid to adjust the pH value of the solution to be3, adding FeCl of 0.025mol/L after stirring evenly3And NiCl2And (3) uniformly stirring 100mL of solution, wherein the ratio of Fe to Ni is 1: 1, adding 0.05mol/L of sodium borohydride, reacting for 2 hours under stirring, enabling the solution to turn black, separating precipitates, washing the precipitates with water for multiple times, and drying at 50 ℃.
Taking 1g of the product and 1g of dicyandiamide, dispersing the product in absolute ethyl alcohol, reacting for 48 hours at 200 ℃ in an autoclave, taking out, drying, heating to 1000 ℃ under an inert atmosphere, keeping the temperature for 2 hours, then cooling to below 50 ℃, and taking out the product. Washing with diluted acid at 80 deg.C, washing with water for several times, and drying at 50 deg.C. The catalyst of structure "1" in figure 1 was obtained.
Example 3
Preparing 200mL of 0.025mol/L silicon dioxide solution, then adding sodium dodecyl sulfate with the mass fraction of 0.05 percent, adding hydrochloric acid to adjust the pH value of the solution to be 3, stirring uniformly, adding FeCl with the mass fraction of 0.025mol/L3And CoCl2And (3) uniformly stirring 100mL of solution, wherein the ratio of Fe to Co is 1: 1, adding 0.05mol/L of sodium borohydride, reacting for 2 hours under stirring, enabling the solution to turn black, separating precipitates, washing the precipitates with water for multiple times, and drying at 50 ℃.
1g of the product and 1g of hexamethylenediamine are taken and dispersed in water, the mixture reacts for 72 hours at 200 ℃ in an autoclave, the mixture is taken out and dried, and then the mixture is heated to 900 ℃ under inert atmosphere, the temperature is kept constant for 2 hours, and then the temperature is reduced to below 50 ℃, and the product is taken out.
Taking 0.5g of the product, dispersing in 200mL of absolute ethyl alcohol, adding 1.25g of chloroplatinic acid and 5mL of hydrazine hydrate, stirring for reacting for 1 hour, washing the reaction product with water for multiple times, washing with diluted acid at 80 ℃, then washing with water for multiple times, and drying at 50 ℃. The catalyst of structure "2" in FIG. 1 was obtained.
Example 4
Preparing 200mL of 0.025mol/L zinc oxide solution, then adding 0.01 mass percent of sodium dodecyl sulfate, adding hydrochloric acid to adjust the pH value of the solution to 3, stirring uniformly, adding 0.025mol/L NiCl2And CoCl2100mL of solution, wherein the ratio of Ni to Co is 1: 1, is evenly stirred, then 0.05mol/L of sodium borohydride is added, the reaction is carried out for 2 hours under the stirring condition, and the color of the solution changesBlack, separating the precipitate, washing the precipitate with water for several times, and drying at 50 ℃.
Taking 1g of the product and 1g of urea, dispersing the product and the urea in absolute ethyl alcohol, reacting for 72 hours at 200 ℃ in a high-pressure kettle, taking out and drying the product, heating to 900 ℃ under an inert atmosphere, keeping the temperature for 2 hours, then cooling to below 50 ℃, and taking out the product.
Taking 0.5g of the product, dispersing in 200mL of absolute ethyl alcohol, adding 1.25g of chloroplatinic acid and 5mL of hydrazine hydrate, stirring for reacting for 1 hour, washing the reaction product with water for multiple times, washing with dilute acid at 50 ℃, then washing with water for multiple times, and drying at 50 ℃. The catalyst of structure "2" in FIG. 1 was obtained.
Example 5
Preparing 200mL of 0.025mol/L zinc oxide solution, then adding sodium dodecyl benzene sulfonate with the mass fraction of 0.05%, adding hydrochloric acid to adjust the pH value of the solution to 3, stirring uniformly, adding FeCl with the mass fraction of 0.025mol/L3And NiCl2And (3) uniformly stirring 100mL of solution, wherein the ratio of Fe to Ni is 1: 1, adding 0.05mol/L of sodium borohydride, reacting for 2 hours under stirring, enabling the solution to turn black, separating precipitates, washing the precipitates with water for multiple times, and drying at 50 ℃.
Taking 1g of the product and 1g of urea, dispersing the product and the urea in absolute ethyl alcohol, reacting for 72 hours at 200 ℃ in a high-pressure kettle, taking out and drying the product, heating to 900 ℃ under an inert atmosphere, keeping the temperature for 2 hours, then cooling to below 50 ℃, and taking out the product.
Taking 0.5g of the product, dispersing in 200mL of absolute ethyl alcohol, adding 1.25g of chloroplatinic acid, stirring and reacting for 1 hour, washing the reaction product with water for multiple times, washing with diluted acid at 80 ℃, then washing with water for multiple times, and drying at 50 ℃. The catalyst of structure "3" in FIG. 1 was obtained.
Example 6
Preparing 200mL of 0.025mol/L tungsten oxide solution, then adding sodium citrate with the mass fraction of 0.05%, adding hydrochloric acid to adjust the pH value of the solution to 3, stirring uniformly, adding FeCl with the mass fraction of 0.025mol/L3Adding 0.5mol/L hydrazine hydrate into 100mL of solution after uniformly stirring, reacting for 2 hours at the temperature of 80 ℃ under stirring, enabling the solution to turn black, separating precipitates, washing the precipitates for multiple times by using water, and drying at the temperature of 50 ℃.
Taking 1g of the product and 1g of polypyrrole, dispersing in absolute ethyl alcohol, reacting for 72 hours at 200 ℃ in an autoclave, taking out, drying, heating to 1100 ℃ under an inert atmosphere, keeping the temperature for 2 hours, then cooling to below 50 ℃, and taking out the product.
Taking 0.5g of the product, dispersing in 200mL of deionized water, adding 0.8g of silver nitrate, stirring for reaction for 1 hour, washing the reaction product with water for multiple times, washing with diluted acid at 80 ℃, then washing with water for multiple times, and drying at 50 ℃. The catalyst of structure "3" in FIG. 1 was obtained.
Example 7
Preparing 200mL of 0.025mol/L tungsten oxide solution, then adding Arabic gum with the mass fraction of 0.05%, adding sulfuric acid to adjust the pH value of the solution to be 5, stirring uniformly, adding FeCl with the mass fraction of 0.025mol/L3And NiCl2The solution is 100mL, Fe and Ni are equal to 1: 1, after even stirring, hydrazine hydrate is added in 0.5mol/L, reaction is carried out for 2 hours under the stirring at 80 ℃, the solution color is changed to black, precipitate is separated, the precipitate is washed by water for a plurality of times, and drying is carried out at 50 ℃.
Taking 1g of the product, 1g of glucose and 0.5g of hexamethylenediamine, dispersing in absolute ethyl alcohol, reacting for 72 hours at 200 ℃ in an autoclave, taking out, drying, heating to 800 ℃ under an inert atmosphere, keeping the temperature for 2 hours, heating to 1000 ℃, keeping the temperature for 1 hour, then cooling to below 50 ℃, and taking out the product.
Taking 0.5g of the product, dispersing in 200mL of water, adding 1.25g of chloroplatinic acid, stirring and reacting for 1 hour, washing the reaction product with water for multiple times, washing with diluted acid at 80 ℃, then washing with water for multiple times, and drying at 50 ℃. The catalyst of structure "3" in FIG. 1 was obtained.
Example 8
Preparing 200mL of 0.025mol/L tungsten oxide solution, then adding 0.05 mass percent sodium dodecyl sulfate, adding sulfuric acid to adjust the pH value of the solution to 5, stirring uniformly, and adding 0.025mol/L CuCl2And (3) uniformly stirring 100mL of solution, adding 0.5mol/L of sodium borohydride, stirring for reacting for 2 hours, enabling the solution to turn black, separating precipitates, washing the precipitates for multiple times by using water, and drying at 50 ℃.
Taking 1g of the product, 1g of glucose and 0.5g of hexamethylenediamine, dispersing in absolute ethyl alcohol, reacting for 72 hours at 200 ℃ in an autoclave, taking out, drying, heating to 800 ℃ under an inert atmosphere, keeping the temperature for 2 hours, heating to 1000 ℃, keeping the temperature for 1 hour, then cooling to below 50 ℃, and taking out the product.
Taking 0.5g of the product, dispersing in 200mL of water, adding 0.5g of palladium chloride, stirring for reaction for 1 hour, washing the reaction product with water for multiple times, washing with dilute acid at room temperature, then washing with water for multiple times, and drying at 50 ℃. The catalyst of structure "3" in FIG. 1 was obtained.

Claims (9)

1. A preparation method of a fuel cell catalyst with a moisture retention function is characterized by comprising the following steps:
(1) dispersing nano inorganic oxide in water, adding a surfactant, adjusting the pH value of the solution to 1-6, uniformly stirring, adding one or more transition metal salts, uniformly stirring, adding a reducing agent sodium borohydride or hydrazine hydrate, and reducing and depositing metal on the surface of the inorganic oxide; washing the product with absolute ethyl alcohol or water for several times, and drying to obtain the transition metal-loaded inorganic oxide;
(2) dispersing inorganic oxide loaded with transition metal in water or ethanol, adding nitrogen-containing organic matter, stirring and mixing uniformly, transferring into a high-pressure kettle, and heating at 100-200 ℃ for 1-72 hours; taking out and drying, heating to 500-1100 ℃ in an inert atmosphere for 0.5-3 hours; then cooling to below 50 ℃, and taking out a product;
(3) dispersing the product obtained in the step (2) in water or absolute ethyl alcohol, stirring uniformly, adding noble metal acid or salt, adding sodium borohydride or hydrazine hydrate reducing agent, stirring for reaction for 0.5-2 hours, filtering and washing the product, and washing the product for 0.5-2 hours at room temperature-100 ℃ by using dilute acid; and washing with water, and drying to obtain the final product.
2. The method of producing a fuel cell catalyst according to claim 1, wherein the transition metal salt is a nitrate, chloride or sulfate of a transition metal; the transition metal is iron, cobalt, nickel or copper, and the noble metal is platinum, gold, silver or palladium.
3. The method of producing a fuel cell catalyst according to claim 1, characterized in that the surfactant is an anionic surfactant or an amphoteric surfactant containing a sulfonic acid group or a carboxylic acid group.
4. The method of preparing a fuel cell catalyst according to claim 3, wherein the surfactant is sodium dodecylbenzenesulfonate, sodium dodecylsulfonate, sodium octane sulfonate, sodium vinyl sulfonate, sodium citrate, or gum arabic.
5. The method of preparing a fuel cell catalyst according to claim 1, wherein the nitrogen-containing organic substance is urea, melamine, dicyandiamide, hexamethylenediamine, polyvinyl pyrrole, polyvinyl pyrrolidone, polyaniline, or polypyrrole.
6. The method for preparing a fuel cell catalyst according to claim 1, wherein in the step (1), the concentration of the transition metal salt is 0.001 to 1.0mol/L, and the mass fraction of the surfactant in the solution is 0.001 to 5%.
7. The method for preparing a fuel cell catalyst according to claim 1, wherein in the step (1) or the step (3), the molar ratio of the amount of the sodium borohydride or the hydrazine hydrate added to the transition metal salt or the noble metal salt added to the reaction is (1-10): 1.
8. The method for producing a fuel cell catalyst according to claim 1, wherein in the step (2), the mass ratio of the transition metal-supporting inorganic oxide to the nitrogen-containing organic substance is (50 to 0.001): 1.
9. The method for producing a fuel cell catalyst according to claim 1, wherein the mass of the noble metal in the obtained catalyst is 0 to 70% of the mass of the catalyst.
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