A fuel cell and hydrogen production dual-function catalyst and preparation method thereof

Abstract

The present application provides a preparation method of a dual-function catalyst for a fuel cell and hydrogen production, comprising the following steps: S01, adding a stabilizer to a solvent, mixing evenly, and obtaining a mixed solution; adding an Ir precursor and a Ru precursor to the mixed solution in sequence, mixing evenly, and obtaining a precursor mixed solution; S02, heating the precursor mixed solution of step S01 to 100°C to 200°C and keeping it warm for 1min to 60min, and then reacting at 100°C to 200°C to obtain a reaction solution; filtering the reaction solution, taking the filter residue, washing and drying to obtain a powder; S03, annealing the powder of step S02 to obtain a dual-function catalyst for a fuel cell and hydrogen production. The preparation method of the present application is simple and easy, can be mass-produced, and has low production cost. The prepared catalyst has the dual functions of catalyzing oxygen evolution at the electrolytic water anode OER and hydrogen oxidation at the fuel cell anode HOR.

Description

Technical Field

[0001] The invention belongs to the technical field of batteries, and in particular relates to a fuel cell and a hydrogen production dual-function catalyst and a preparation method thereof. Background Art

[0002] A proton exchange membrane fuel cell (PEMFC) is a device that converts chemical energy stored in hydrogen into electrical energy. Its components include membrane electrode, bipolar plate, current collecting plate and end plate. The membrane electrode is composed of a proton exchange membrane, an anode catalyst layer, a cathode catalyst layer, an anode diffusion layer and a cathode diffusion layer. The proton membrane and the catalyst layer are sealed with a frame, and the two sides of the catalyst layer are covered with diffusion layers.

[0003] The Unitized Regenerative Fuel Cell (URFC) is a highly efficient energy storage device derived from PEMFC technology. When voltage is applied to both ends of the current collector, it can operate in the water electrolysis hydrogen production mode. When hydrogen is introduced into the anode and air is introduced into the cathode, it can enter the fuel cell mode to generate electricity. Hydrogen energy is used for backup power supply, energy storage, etc., and URFC has great application potential. Traditional hydrogen energy storage devices include three modules: water electrolysis hydrogen production, hydrogen storage, and fuel cells. The URFC device integrates the hydrogen production electrolyzer and the fuel cell stack to achieve dual functions. The system is more compact, more integrated, and easy to maintain.

[0004] In the water electrolysis mode, oxygen evolution reaction (OER) occurs at the anode and hydrogen evolution reaction (HOR) occurs at the cathode. In the fuel cell mode, hydrogen oxidation reaction (HOR) occurs at the anode and oxygen reduction reaction (ORR) occurs at the cathode.

[0005] The document Energy Environ. Sci., 2020, 13, 4872 discloses a design scheme for URFC, dissolving Pt black and Ir black catalysts in a solvent and combining ultrasonic spraying technology to prepare OER and ORR dual-functional catalytic layers. However, Ir black and Pt black particles are large, with low catalytic activity and low utilization rate. At the same time, it is difficult to ensure the uniformity of the catalytic layer by physical mixing alone. Moreover, the potential is high in the electrolytic water working mode, and Pt is easily oxidized, losing ORR oxygen reduction activity, thereby reducing the performance of the fuel cell mode. Summary of the invention

[0006] The embodiment of the present invention provides a fuel cell and hydrogen production bifunctional catalyst and a preparation method thereof, aiming to solve the problems of poor catalytic performance of existing catalysts, low catalyst utilization, easy oxidation at high potential resulting in decreased oxygen reduction (ORR) catalytic performance, and short switching life between the two working modes of hydrogen production and fuel cell.

[0007] To achieve the above objectives, on the one hand, an embodiment of the present invention provides a method for preparing a fuel cell and a hydrogen production bifunctional catalyst, comprising the following steps:

[0008] S01, adding a stabilizer to a solvent, mixing uniformly, and obtaining a mixed solution; adding an Ir precursor and a Ru precursor to the mixed solution in sequence, mixing uniformly, and obtaining a precursor mixed solution;

[0009] S02, heating the precursor mixture of step S01 to 100° C. to 200° C. and keeping the temperature for 1 min to 60 min, and then reacting at 100° C. to 200° C. to obtain a reaction solution; filtering the reaction solution, taking the filter residue, washing and drying it to obtain a powder;

[0010] S03, annealing the powder of step S02 to obtain a fuel cell and hydrogen production dual-function catalyst (ie, IrRu alloy catalyst).

[0011] As a preferred embodiment, in step S01,

[0012] For every 5 mL of the solvent, 0.01 g to 0.5 g of the stabilizer is added; for every 60 mL of the solvent, the amount of the Ir substance contained in the Ir precursor added is 0.1 mmol to 3 mmol.

[0013] The ratio of the amount of the Ir substance contained in the Ir precursor to the amount of the Ru substance contained in the Ru precursor is (1 to 10): (1 to 10).

[0014] The stabilizer is preferably one of citric acid, sodium citrate, polyvinyl pyrrolidone, cyclopentane, oleic acid or sodium hydroxide, or a mixture of at least two thereof.

[0015] The solvent is preferably one of methanol, ethanol, propylene glycol, glycerol, ethylene glycol, polyvinyl alcohol or oleylamine, or a mixture of at least two thereof.

[0016] The Ir precursor is preferably iridium chloride (including IrCl3 or IrCl3·xH2O), iridium acetylacetonate (C 15 H 21IrO6), chloroiridic acid (including H2IrCl6 or H2IrCl6·xH2O), ammonium chloroiridate (H8Cl6IrN2), potassium chloroiridate (K2IrCl6) or sodium chloroiridate (including Na3IrCl6·xH2O or Na2IrCl6·6H2O) or a mixture of at least two of them.

[0017] The Ru precursor is preferably ruthenium chloride (including RuCl3 or RuCl3·xH2O), ruthenium acetylacetonate (C 15 H 21 O6Ru), ammonium hexachlororuthenate ((NH4)2RuCl6), hexaammineruthenium chloride (Ru(NH3)6Cl3) or potassium hexachlororuthenate (K3RuCl6) or a mixture of at least two of them.

[0018] Preferably, the precursor mixture also contains a carrier; the carrier is a metal oxide carrier. The embodiment of the present application may not add a carrier, or may use a metal oxide carrier resistant to high potential and acid corrosion; the carrier helps to improve the dispersibility and stability of the IrRu alloy nanoparticles and inhibit the agglomeration of the particles.

[0019] The metal oxide support includes at least one of niobium oxide (Nb2O5), titanium suboxide (Ti4O7), tantalum oxide (Ta2O5) or antimony tin oxide (ATO).

[0020] As a preferred embodiment, in step S02,

[0021] The heating is achieved by microwave heating; the heating is preferably carried out under an inert atmosphere. Inert gas can be selected as a protective gas or no inert gas can be used during the reaction.

[0022] The reaction time is preferably 1 h to 2 h.

[0023] The washing is preferably performed with deionized water; and the drying is performed by vacuum drying.

[0024] As a preferred embodiment, in step S03,

[0025] The temperature of the annealing treatment is 100° C. to 300° C., and the time of the annealing treatment is 10 min to 120 min.

[0026] The annealing treatment is carried out in an inert gas containing hydrogen; the volume fraction of the hydrogen is 1% to 100%.

[0027] The inert gas is at least one of Ar or N2.

[0028] The annealing treatment is carried out in a tube furnace.

[0029] The fuel cell and hydrogen production bifunctional catalyst contain an IrxRuy alloy; in the IrxRuy alloy, the ratio of the amount of Ir to the amount of Ru is x / y=(1-10) / (1-10).

[0030] On the other hand, an embodiment of the present invention further provides a fuel cell and a hydrogen production bifunctional catalyst, wherein the fuel cell and the hydrogen production bifunctional catalyst are prepared by the above-mentioned preparation method.

[0031] The fuel cell and hydrogen production bifunctional catalyst prepared by the method of the present application has the dual functions of catalyzing oxygen evolution at the water electrolysis anode OER and hydrogen oxidation at the fuel cell anode HOR, and can be used as an anode catalyst for an integrated recoverable fuel cell URFC.

[0032] Compared with the simple physical mixture of the traditional Ir-based and Pt-based catalysts, the catalytic layer prepared by the IrxRuy alloy catalyst of the present application is more uniform and has a longer life span in switching between hydrogen production and fuel cell working modes.

[0033] Compared with conventional Pt catalysts, the IrxRuy alloy catalyst of the present application has CO resistance and lower requirements for hydrogen purity. The preparation method of the present application is simple and easy to implement. Combined with a continuous liquid supply device, microwave continuous preparation can be achieved to realize batch production, and the batch production cost is low. BRIEF DESCRIPTION OF THE DRAWINGS

[0034] In order to more clearly illustrate the embodiments of the present invention or the technical solutions in the prior art, the drawings required for use in the embodiments or the description of the prior art will be briefly introduced below. Obviously, the drawings described below are only some embodiments of the present invention. For ordinary technicians in this field, other drawings can be obtained based on the structures shown in these drawings without paying creative work.

[0035] Figure 1 The XRD diagram of the fuel cell and hydrogen production bifunctional catalyst of Example 1 of the present invention;

[0036] Figure 2 TEM image of the fuel cell and hydrogen production bifunctional catalyst of Example 1;

[0037] Figure 3 Element distribution diagram of the fuel cell and hydrogen production bifunctional catalyst of Example 1;

[0038] Figure 4 This is a hydrogen production performance diagram of a membrane electrode composed of a fuel cell and a hydrogen production bifunctional catalyst combined with a Pt / C cathode catalyst layer in Example 1;

[0039] Figure 5This is a performance diagram of a fuel cell that is a membrane electrode composed of a fuel cell and a hydrogen production bifunctional catalyst in Example 1 combined with a Pt / C cathode catalyst layer.

[0040] The realization of the purpose, functional features and advantages of the present invention will be further explained in conjunction with embodiments and with reference to the accompanying drawings. DETAILED DESCRIPTION

[0041] The technical solutions in the embodiments of the present invention are described clearly and completely below. Obviously, the described embodiments are only part of the embodiments of the present invention, not all of the embodiments. Based on the embodiments of the present invention, all other embodiments obtained by ordinary technicians in this field without creative work are within the scope of protection of the present invention.

[0042] It should be noted that if the embodiments of the present invention involve directional indications (such as up, down, left, right, front, back, top, bottom...), the directional indications are only used to explain the relative position relationship, movement status, etc. between the components in a certain specific posture. If the specific posture changes, the directional indication will also change accordingly.

[0043] In this application, unless otherwise clearly specified and limited, the terms "installed", "connected", "connected", "fixed" and the like should be understood in a broad sense, for example, it can be a fixed connection, a detachable connection, or an integral connection; it can be a mechanical connection or an electrical connection; it can be a direct connection or an indirect connection through an intermediate medium, it can be the internal connection of two elements or the interaction relationship between two elements, unless otherwise clearly defined. For ordinary technicians in this field, the specific meanings of the above terms in this application can be understood according to specific circumstances.

[0044] It should be noted that when an element is referred to as being "fixed to" or "disposed on" another element, it may be directly on the other element or there may be an intermediate element. When an element is considered to be "connected to" another element, it may be directly connected to the other element or there may be an intermediate element at the same time.

[0045] In addition, if there are descriptions involving "first", "second", etc. in the embodiments of the present invention, the descriptions of "first", "second", etc. are only used for descriptive purposes and cannot be understood as indicating or suggesting their relative importance or implicitly indicating the number of the indicated technical features. Therefore, the features defined as "first" and "second" may explicitly or implicitly include at least one of the features. In addition, the technical solutions between the various embodiments can be combined with each other, but they must be based on the ability of ordinary technicians in the field to implement them. When the combination of technical solutions is contradictory or cannot be implemented, it should be deemed that such a combination of technical solutions does not exist and is not within the scope of protection required by the present invention.

[0046] Current URFCs usually use oxygen electrodes with OER and ORR on the same side, which are mainly mechanical mixtures of Ir and Pt-based catalysts or alloy catalysts containing Ir and Pt, with poor catalytic performance and low catalyst utilization. In addition, in the water electrolysis mode, OER is at a high potential (≥1.5V), and the Pt-based catalyst used for the ORR reaction is easily oxidized at such a high potential, resulting in a decrease in the oxygen reduction ORR catalytic performance and a low switching life between the two working modes of hydrogen production and fuel cells.

[0047] The catalyst prepared in this application has high-performance OER and HOR dual-functional catalysis, and can be used as the anode-side catalytic layer of water electrolysis to produce hydrogen and fuel cells. The cathode uses commercial Pt / C, and the prepared membrane electrode can operate in two modes: water electrolysis to produce hydrogen and fuel cell power generation.

[0048] In the preparation method of the embodiment of the present application, the selection and dosage of each component can be selected according to the actual use needs, as long as it is within the limited range of the above requirements, the present application scheme can be realized. In addition, by controlling the dosage ratio of each component and the preparation conditions within the limited range of the requirements of the present application, the catalytic activity of the prepared catalyst can be effectively guaranteed.

[0049] Example 1

[0050] A method for preparing a fuel cell and a hydrogen production bifunctional catalyst comprises the following steps:

[0051] S01, adding 0.24g of stabilizer to 60mL of solvent, mixing evenly to obtain a mixed solution; adding 267.0mg of Ir precursor and 101.1mg of Ru precursor to the mixed solution in sequence, dispersing evenly by ultrasonication, and then stirring and mixing for 30min to obtain a precursor mixed solution;

[0052] S02, heating the precursor mixture of step S01 to 170° C. and keeping the temperature for 30 minutes, and then reacting at 170° C. to obtain a reaction solution; filtering the reaction solution, taking the filter residue, washing and drying it to obtain a powder;

[0053] S03, annealing the powder of step S02 to obtain a fuel cell and hydrogen production dual-function catalyst (ie, Ir1Ru1 alloy catalyst).

[0054] In step S01,

[0055] The ratio of the amount of Ir contained in the Ir precursor to the amount of Ru contained in the Ru precursor is 1:1.

[0056] The stabilizer is sodium hydroxide. The solvent is ethylene glycol.

[0057] The Ir precursor is chloroiridic acid (H2IrCl6·xH2O, Ir content 36%). The Ru precursor is ruthenium chloride (RuCl3, Ru content 50%, M=207.43, Ru:M=101.07).

[0058] In step S02,

[0059] The heating is achieved by microwave heating; the heating is carried out under a N2 inert atmosphere.

[0060] The reaction time is 2h.

[0061] The washing is performed 4 times with deionized water; and the drying is performed by vacuum drying.

[0062] In step S03,

[0063] The temperature of the annealing treatment is 200° C., and the time of the annealing treatment is 60 minutes.

[0064] The annealing treatment is carried out in an inert gas containing hydrogen; the volume fraction of the hydrogen is 10%.

[0065] The inert gas is N2. The annealing treatment is carried out in a tube furnace.

[0066] The fuel cell and hydrogen production bifunctional catalyst contain an IrxRuy alloy; in the IrxRuy alloy, the ratio of the amount of Ir to the amount of Ru is x / y=1.

[0067] Figure 1 The XRD diagram of the fuel cell and hydrogen production bifunctional catalyst of this embodiment is shown in FIG. Figure 1 It can be seen that the diffraction peaks clearly correspond to the characteristic peaks of iridium and ruthenium. Figure 2 TEM image of the fuel cell and hydrogen production bifunctional catalyst of this embodiment; Figure 3 The element distribution diagram of the fuel cell and hydrogen production bifunctional catalyst of this embodiment is shown in FIG. The obtained Ir1Ru1 alloy catalyst is prepared into the anode catalyst layer of the membrane electrode, and the cathode catalyst layer adopts a commercial Pt / C catalyst. The membrane electrode is tested for performance under the tooling. Figure 4 The hydrogen production performance diagram of the fuel cell and hydrogen production bifunctional catalyst combined with the Pt / C cathode catalyst layer to form a membrane electrode in this embodiment; in the hydrogen production mode, the current density can reach 2.2A / cm under 80°C and 1.75V. 2 . Figure 5The fuel cell performance diagram of the fuel cell and hydrogen production bifunctional catalyst combined with the Pt / C cathode catalyst layer to form a membrane electrode in this embodiment; in the fuel cell mode, the temperature is 80C, the anode cathode humidity is 40% / 60%, the back pressure is 140 / 120Kpa, and the stoichiometric ratio is 1.6 / 2.2, and the single cell polarization performance is 2A / cm 2 The voltage was 0.62V at the current density.

[0068] Example 2

[0069] A method for preparing a fuel cell and a hydrogen production bifunctional catalyst comprises the following steps:

[0070] S01, adding 0.24g of stabilizer to 60mL of solvent, mixing evenly to obtain a mixed solution; adding 801.0mg of Ir precursor and 101.1mg of Ru precursor to the mixed solution in sequence, dispersing evenly by ultrasonication, and then stirring and mixing for 30min to obtain a precursor mixed solution;

[0071] S02, heating the precursor mixture of step S01 to 170° C. and keeping the temperature for 30 minutes, and then reacting at 170° C. to obtain a reaction solution; filtering the reaction solution, taking the filter residue, washing and drying it to obtain a powder;

[0072] S03, annealing the powder of step S02 to obtain a fuel cell and hydrogen production dual-function catalyst (i.e., Ir3Ru1 alloy catalyst).

[0073] In step S01,

[0074] The ratio of the amount of Ir contained in the Ir precursor to the amount of Ru contained in the Ru precursor is 3:1.

[0075] The stabilizer is sodium hydroxide. The solvent is ethylene glycol.

[0076] The Ir precursor is chloroiridic acid (H2IrCl6·xH2O, Ir content 36%). The Ru precursor is ruthenium chloride (RuCl3, Ru content 50%, M=207.43, Ru:M=101.07).

[0077] In step S02,

[0078] The heating is achieved by microwave heating; the heating is carried out under a N2 inert atmosphere.

[0079] The reaction time is 2 hours. The washing is performed 4 times with deionized water; and the drying is performed by vacuum drying.

[0080] In step S03,

[0081] The temperature of the annealing treatment is 200° C., and the time of the annealing treatment is 60 minutes.

[0082] The annealing treatment is carried out in an inert gas containing hydrogen; the volume fraction of the hydrogen is 10%.

[0083] The inert gas is N2. The annealing treatment is carried out in a tube furnace.

[0084] The fuel cell and hydrogen production bifunctional catalyst contain an IrxRuy alloy; in the IrxRuy alloy, the ratio of the amount of Ir to the amount of Ru is x / y=3.

[0085] Example 3

[0086] A method for preparing a fuel cell and a hydrogen production bifunctional catalyst comprises the following steps:

[0087] S01, adding 0.24g of stabilizer to 60mL of solvent, mixing evenly to obtain a mixed solution; adding 267.0mg of Ir precursor and 101.1mg of Ru precursor to the mixed solution in sequence, dispersing evenly by ultrasonication, and then stirring and mixing for 30min to obtain a precursor mixed solution;

[0088] S02, heating the precursor mixture of step S01 to 170° C. and keeping the temperature for 30 minutes, and then reacting at 170° C. to obtain a reaction solution; filtering the reaction solution, taking the filter residue, washing and drying it to obtain a powder;

[0089] S03, annealing the powder of step S02 to obtain a fuel cell and hydrogen production dual-function catalyst (i.e., Ir1Ru1@Nb2O5 carrier-type alloy catalyst).

[0090] In step S01,

[0091] The ratio of the amount of Ir contained in the Ir precursor to the amount of Ru contained in the Ru precursor is 1:1.

[0092] The stabilizer is sodium hydroxide. The solvent is ethylene glycol.

[0093] The Ir precursor is chloroiridic acid (H2IrCl6·xH2O, Ir content 36%). The Ru precursor is ruthenium chloride (RuCl3, Ru content 50%, M=207.43, Ru:M=101.07).

[0094] The precursor mixture also contains 100 mg of a carrier, which is niobium oxide (Nb2O5). The carrier helps to improve the dispersibility and stability of the IrRu alloy nanoparticles and inhibit the agglomeration of the particles.

[0095] In step S02,

[0096] The heating is achieved by microwave heating; the heating is carried out under a N2 inert atmosphere.

[0097] The reaction time is 2h.

[0098] The washing is performed 4 times with deionized water; and the drying is performed by vacuum drying.

[0099] In step S03,

[0100] The temperature of the annealing treatment is 200° C., and the time of the annealing treatment is 60 minutes.

[0101] The annealing treatment is carried out in an inert gas containing hydrogen; the volume fraction of the hydrogen is 10%.

[0102] The inert gas is N2. The annealing treatment is carried out in a tube furnace.

[0103] The fuel cell and hydrogen production bifunctional catalyst contain an IrxRuy alloy; in the IrxRuy alloy, the ratio of the amount of Ir to the amount of Ru is x / y=1.

[0104] In the description of this specification, the description with reference to the terms "an embodiment", "example", etc. means that the specific features, structures, materials or characteristics described in conjunction with the embodiment or example are included in at least one embodiment or example of the present invention. In this specification, the schematic representation of the above terms does not necessarily refer to the same embodiment or example.

[0105] In addition, it should be understood that although this specification is described according to implementation methods, not every implementation method contains only one independent technical solution. This narrative method of the specification is only for the sake of clarity. Those skilled in the art should regard the specification as a whole. The technical solutions in each embodiment may also be appropriately combined to form other implementation methods that can be understood by those skilled in the art.

[0106] The above description is only a preferred embodiment of the present invention and is not intended to limit the present invention. Any modifications, equivalent substitutions and improvements made within the spirit and principles of the present invention should be included in the protection scope of the present invention.

Claims

1. A method for preparing a fuel cell and hydrogen production bifunctional catalyst, characterized in that: The steps include: S01, adding a stabilizer to a solvent, mixing uniformly, and obtaining a mixed solution; adding an Ir precursor and a Ru precursor to the mixed solution in sequence, mixing uniformly, and obtaining a precursor mixed solution; S02, heating the precursor mixture of step S01 to 100° C. to 200° C. and keeping the temperature for 1 min to 60 min, and then reacting at 100° C. to 200° C. to obtain a reaction solution; filtering the reaction solution, taking the filter residue, washing and drying it to obtain a powder; S03, annealing the powder of step S02 to obtain a dual-function catalyst for fuel cell and hydrogen production; In step S02, the heating is achieved by microwave heating; the heating is performed under an inert atmosphere; and the drying is vacuum drying; In step S03, the temperature of the annealing treatment is 100°C to 300°C, and the time of the annealing treatment is 10min to 120min; The annealing treatment is carried out in an inert gas containing hydrogen; the volume fraction of the hydrogen is 1% to 100%; The fuel cell and hydrogen production bifunctional catalyst contain an IrxRuy alloy; in the IrxRuy alloy, the ratio of the amount of Ir to the amount of Ru is x / y=(1-10) / (1-10).

2. The method for preparing a fuel cell and hydrogen production bifunctional catalyst according to claim 1, characterized in that: In step S01, 0.01 g to 0.5 g of the stabilizer is added to every 5 mL of the solvent; the amount of the Ir substance contained in the Ir precursor added to every 60 mL of the solvent is 0.1 mmol to 3 mmol; The ratio of the amount of the Ir substance contained in the Ir precursor to the amount of the Ru substance contained in the Ru precursor is (1 to 10): (1 to 10).

3. The method for preparing a fuel cell and hydrogen production bifunctional catalyst according to claim 1, characterized in that: In step S01, The stabilizer is one or a mixture of at least two of citric acid, sodium citrate, polyvinyl pyrrolidone, cyclopentane, oleic acid or sodium hydroxide; The solvent is one of methanol, ethanol, propylene glycol, glycerol, ethylene glycol, polyvinyl alcohol or oleylamine, or a mixture of at least two of them.

4. The method for preparing a fuel cell and hydrogen production bifunctional catalyst according to claim 1, characterized in that: In step S01, The Ir precursor is one or a mixture of at least two of iridium chloride, iridium acetylacetonate, chloroiridic acid, ammonium chloroiridate, potassium chloroiridate or sodium chloroiridate; The Ru precursor is one of ruthenium chloride, ruthenium acetylacetonate, ammonium hexachlororuthenate, hexaammineruthenium chloride or potassium hexachlororuthenate, or a mixture of at least two of them.

5. The method for preparing a fuel cell and hydrogen production bifunctional catalyst according to claim 1, characterized in that: In step S01, the precursor mixture also contains a carrier; the carrier is a metal oxide carrier.

6. The method for preparing a fuel cell and hydrogen production bifunctional catalyst according to claim 5, characterized in that: The metal oxide support includes at least one of niobium oxide, titanium oxide, tantalum oxide or antimony tin oxide.

7. The method for preparing a fuel cell and hydrogen production bifunctional catalyst according to claim 1, characterized in that: In step S02, The reaction time is 1 h to 2 h; the washing is performed with deionized water.

8. The method for preparing a fuel cell and hydrogen production bifunctional catalyst according to claim 1, characterized in that: The inert gas is at least one of Ar and N2; and the annealing treatment is carried out in a tube furnace.

9. A fuel cell and hydrogen production bifunctional catalyst, characterized in that: The fuel cell and hydrogen production bifunctional catalyst is prepared by the preparation method according to any one of claims 1 to 8.

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