A LaCeGdCoNiO x High-entropy heterojunction catalysts, their preparation methods and applications

Abstract

The application discloses a LaCeGdCoNiO x The application discloses a high-entropy heterojunction catalyst, a preparation method and application thereof, and a catalyst preparation method. The catalyst preparation method comprises the following steps: firstly, obtaining a metal gel precursor by using a microemulsion method; and then, performing high-temperature calcination on the metal gel precursor to obtain a high-entropy oxide nanomaterial with a heterostructure. The high-entropy oxide nanomaterial has the multiplicity of high-entropy material composition and the interface synergistic effect of the heterostructure, can effectively regulate the d-band structure and electronic state of an active center, and can improve the electrocatalytic performance. It can be seen from the test on the electrocatalytic oxygen evolution reaction that the catalyst prepared by the application has excellent catalytic activity and long-term stability, and has a good industrial application prospect.

Description

Technical Field

[0001] This invention relates to the field of electrocatalytic materials technology, and in particular to a LaCeGdCoNiO x High-entropy heterojunction catalysts, their preparation methods, and applications. Background Technology

[0002] The oxygen evolution reaction (OER), a core half-reaction in water electrolysis for hydrogen production, involves complex four-electron transfers and multiple intermediate reaction steps, resulting in slow kinetics and high overpotentials, thus becoming a key bottleneck restricting overall energy conversion efficiency. Currently, highly efficient OER catalysts still heavily rely on precious metals such as iridium (Ir) and ruthenium (Ru), whose high cost and limited reserves severely restrict the large-scale commercial application of OER catalysts. Therefore, developing non-precious metal catalytic materials that combine high activity, high stability, and low cost is of great significance for promoting the development of clean energy technologies.

[0003] In recent years, high-entropy oxide (HEO) nanomaterials have emerged as a new class of catalysts, demonstrating great potential in regulating electronic structure and enhancing catalytic activity due to their unique high-entropy effect, lattice distortion effect, slow diffusion effect, and "cocktail" effect. While catalysts based on abundant transition metals (such as Ni and Co) are relatively inexpensive, they often suffer from problems such as high overpotential and insufficient stability. For example, Chinese patent CN120719331A discloses a two-phase hollow high-entropy oxide catalyst NiCoFeMnCrRuO. Although its metal elements include inexpensive transition metals such as nickel, cobalt, iron, manganese, and chromium, reducing the use of precious metals, the addition of the precious metal Ru is still unavoidable to improve catalytic activity, keeping the catalyst preparation cost relatively high. Furthermore, the catalyst in this patent exhibits high overpotential at 10 mA·cm⁻¹. -2 At the given current density, the OER overpotential is 275mV, which is still relatively high.

[0004] Rare earth elements, due to their unique 4f electron shell structure, are often used to optimize the electronic structure of other materials (such as transition metal oxides), thereby enhancing their intrinsic activity and stability. Therefore, combining transition metals with rare earth elements to construct multiple sets of high-entropy oxide materials is considered an effective strategy to replace noble metal catalysts. Furthermore, constructing heterostructures in materials can effectively introduce abundant interfacial contacts, and their unique interfacial effects can provide a large number of active sites, thereby improving catalytic performance. Simultaneously, the combination of materials with different lattice constants at heterostructure interfaces will generate tensile or compressive strain. This strain can modulate the d-band center position of active sites, optimize the electronic structure, induce interfacial charge redistribution, and enhance electron transfer capabilities, thus affecting the adsorption / desorption behavior of reaction intermediates.

[0005] In summary, constructing high-entropy oxide nanocatalysts with heterogeneous structures can integrate the structural and performance advantages of multiple materials, which has significant scientific value and application prospects for designing next-generation high-performance OER catalysts. Summary of the Invention

[0006] The purpose of this invention is to provide a LaCeGdCoNiO x High-entropy heterojunction catalysts, their preparation methods, and applications are proposed to address the problems of low activity, poor stability, and high cost of the aforementioned OER catalysts.

[0007] To achieve the above objectives, the first aspect of the present invention provides a LaCeGdCoNiO x The preparation method of high-entropy heterojunction catalyst includes the following steps: S1: Preparation of microemulsion A microemulsion was obtained by mixing hexadecyltrimethylammonium bromide, n-butanol, and n-hexane and then sonicating it. S2: Preparation of metal salt solution Lanthanum salt, cerium salt, gadolinium salt, cobalt salt, and nickel salt were dissolved in ultrapure water and subjected to ultrasonic treatment to obtain a metal salt solution; S3: Preparation of gel precursor The metal salt solution was poured into the microemulsion, then potassium hydroxide was added and stirred to carry out the reaction. After centrifugation, washing and drying, the gel precursor was obtained. S4: Catalyst Preparation The gel precursor was calcined and ground to obtain LaCeGdCoNiO x High-entropy heterojunction catalyst.

[0008] Preferably, in step S1, the amount of hexadecyltrimethylammonium bromide added is 0.01~0.05 mol, the amount of n-butanol added is 5~15 mL, and the amount of n-hexane added is 10~50 mL.

[0009] More preferably, in step S1, the amount of hexadecyltrimethylammonium bromide added is 0.03 mol, the amount of n-butanol added is 10 mL, and the amount of n-hexane added is 30 mL.

[0010] Preferably, in step S1, the frequency of ultrasonic treatment is 20~60KHz and the time is 20~40min.

[0011] More preferably, in step S1, the frequency of ultrasonic treatment is 40 kHz and the time is 30 min.

[0012] Preferably, in step S2, the amount of metal element added to lanthanum salt, cerium salt, gadolinium salt, cobalt salt and nickel salt is 0.2~1.0 mmol, and the amount of ultrapure water added is 0.5~1.5 mL, based on the number of moles of metal element in the metal salt.

[0013] More preferably, the lanthanum salt, cerium salt, gadolinium salt, cobalt salt, and nickel salt are all chloride salts, meaning their anions are chloride ions. Specifically, the amount of lanthanum chloride added is 0.5 mmol, the amount of cerium chloride added is 0.5 mmol, the amount of gadolinium chloride added is 0.5 mmol, the amount of cobalt chloride added is 0.5 mmol, the amount of nickel chloride added is 0.5 mmol, and the amount of ultrapure water added is 1 mL.

[0014] Preferably, in step S2, the frequency of ultrasonic treatment is 20~60KHz and the time is 5~15min.

[0015] More preferably, in step S2, the frequency of ultrasonic treatment is 40 kHz and the time is 10 min.

[0016] Preferably, in step S3, the amount of potassium hydroxide added is 0.01~0.04 mol.

[0017] More preferably, in step S3, the amount of potassium hydroxide added is 0.02 mol.

[0018] It should be noted that the potassium hydroxide used as a precipitant in this invention can also be other alkaline substances, such as sodium hydroxide, and is not limited to the potassium hydroxide used in this invention.

[0019] Preferably, in step S3, the stirring speed is 500~1500 r / min and the stirring time is 1~3 h.

[0020] More preferably, in step S3, the stirring speed is 1000 r / min and the duration is 2 h.

[0021] More preferably, in step S3, the gel product obtained by centrifugation is washed with ethanol and deionized water, requiring 2 to 4 washes, with 3 washes being optimal. The drying process is completed in an oven at a temperature of 50 to 80°C, with 60°C being optimal.

[0022] Preferably, in step S4, the heating rate during calcination is 2~10℃ / min, the calcination temperature is 700~1000℃, and the heating time is 6~10h.

[0023] More preferably, in step S4, the heating rate during calcination is 5°C / min, the calcination temperature is 900°C, and the heating time is 8h.

[0024] A second aspect of the present invention provides a LaCeGdCoNiO xThe high-entropy heterojunction catalyst was prepared by the method described above. The obtained LaCeGdCoNiO x The high-entropy heterojunction catalyst is a black solid.

[0025] A third aspect of the present invention provides a LaCeGdCoNiO x The application of high-entropy heterojunction catalysts will enable the use of LaCeGdCoNiO x High-entropy heterojunction catalysts are used in electrocatalytic oxygen evolution reactions.

[0026] Therefore, the present invention uses the above-mentioned LaCeGdCoNiO x High-entropy heterojunction catalysts, their preparation methods, and applications offer the following beneficial effects: (1) The present invention uses a microemulsion method combined with calcination process, which only requires two steps: mixing of precursor solution and high-temperature calcination to complete the preparation of catalyst. The synthesis process is simple and efficient, which is conducive to the widespread use of catalyst.

[0027] (2) In the preparation process of high-entropy heterojunction catalyst, the present invention obtains high-entropy oxide material by fusing five metal salts, thereby giving it the high-entropy effect, lattice distortion effect, slow diffusion effect and "cocktail" effect unique to high-entropy materials. These properties have advantages in regulating electronic structure and improving catalytic activity.

[0028] (3) In the preparation process of high-entropy heterojunction catalyst, the present invention uses a multi-element combination of transition metals and rare earth metals to carry out high-entropy design without the use of precious metals, which reduces the preparation cost of the catalyst and has good industrial application prospects.

[0029] (4) The heterostructure formed inside the catalyst prepared by the present invention generates strong lattice distortion at the interface, which can finely control the d-band center of the active site and induce the redistribution of the interface charge, thereby optimizing the adsorption / desorption behavior of the reaction intermediate, achieving further improvement of catalytic performance, and significantly improving the stability of the catalyst.

[0030] The technical solution of the present invention will be further described in detail below with reference to the accompanying drawings and embodiments. Attached Figure Description

[0031] Figure 1 LaCeGdCoNiO in Example 1 x TEM image of a high-entropy heterojunction catalyst; Figure 2 LaCeGdCoNiO in Example 1 x Elemental distribution diagram in high-entropy heterojunction catalysts; Figure 3LaCeGdCoNiO in Example 1 x HRTEM morphology of high-entropy heterojunction catalyst; Figure 4 LaCeGdCoNiO in Example 1 x XRD pattern of high-entropy heterojunction catalyst; Figure 5 TEM images of the catalysts prepared in Examples 2-5; Figure 6 The graphs show the OER performance test results for Examples 1 and 5 and the commercial catalyst. Figure 7 LaCeGdCoNiO x High-entropy heterojunction catalysts at 50 mA·cm -2 Stability test under current density. Detailed Implementation

[0032] The present invention will be further described below. It should be noted that this embodiment is based on the present technical solution and provides detailed implementation methods and specific operation processes, but the present invention is not limited to this embodiment.

[0033] Example 1 A LaCeGdCoNiO x The preparation method of high-entropy heterojunction catalyst includes the following steps: (1) Preparation of microemulsion: Add 0.03 mol of cetyltrimethylammonium bromide (CTAB), 10 mL of n-butanol and 30 mL of n-hexane to a flask and sonicate at 40 kHz for 30 min to obtain microemulsion.

[0034] (2) Preparation of metal salt solution: Dissolve 0.5 mmol lanthanum chloride, 0.5 mmol cerium chloride, 0.5 mmol gadolinium chloride, 0.5 mmol cobalt chloride and 0.5 mmol nickel chloride in 1 mL of ultrapure water, and sonicate at 40 kHz for 10 min. After all the metal salts are completely dissolved, the metal salt solution can be obtained.

[0035] (3) Preparation of gel precursor: The prepared metal salt solution was poured into a flask containing the microemulsion, and 0.02 mol of potassium hydroxide was added to obtain a mixed solution. The mixed solution was then stirred on a stirrer for 2 hours at a speed of 1000 r / min. After the reaction was completed, the gel product was separated by centrifugation and washed three times with ethanol and deionized water. Then, it was dried in an oven at 60°C to obtain the gel precursor.

[0036] (4) Catalyst preparation: The dried gel precursor was placed in a crucible and then placed in a muffle furnace for high-temperature calcination. The heating rate was 5℃ / min, the calcination temperature was 900℃, and the heating time was 10h. After the system cooled naturally to room temperature, the black solid was removed and ground into powder to obtain the high-entropy heterojunction catalyst. The catalyst in this example was named LaCeGdCoNiO x .

[0037] Example 2 A LaCoNiO x The preparation method of the catalyst differs from that in Example 1 in that the types of metal elements in the metal salt solution are different, and specifically includes the following steps: (1) Preparation of microemulsion: Add 0.03 mol of cetyltrimethylammonium bromide (CTAB), 10 mL of n-butanol and 30 mL of n-hexane to a flask and sonicate at 40 kHz for 30 min to obtain microemulsion.

[0038] (2) Preparation of metal salt solution: Dissolve 0.5 mmol lanthanum chloride, 0.5 mmol cobalt chloride and 0.5 mmol nickel chloride in 1 mL of ultrapure water, and sonicate at 40 kHz for 10 min. After all the metal salts are completely dissolved, the metal salt solution can be obtained.

[0039] (3) Preparation of gel precursor: The prepared metal salt solution was poured into a flask containing the microemulsion, and 0.02 mol of potassium hydroxide was added to obtain a mixed solution. The mixed solution was then stirred on a stirrer for 2 hours at a speed of 1000 r / min. After the reaction was completed, the gel product was separated by centrifugation and washed three times with ethanol and deionized water. Then, it was dried in an oven at 60°C to obtain the gel precursor.

[0040] (4) Catalyst preparation: The dried gel precursor was placed in a crucible and then placed in a muffle furnace for high-temperature calcination. The heating rate was 5℃ / min, the calcination temperature was 900℃, and the heating time was 10h. After the system cooled naturally to room temperature, the black solid was removed and ground into powder to obtain the catalyst. The catalyst in this example was named LaCoNiO. x .

[0041] Example 3 A CeCoNiO x The preparation method of the catalyst differs from that in Example 1 in that the types of metal elements in the metal salt solution are different, and specifically includes the following steps: (1) Preparation of microemulsion: Add 0.03 mol of cetyltrimethylammonium bromide (CTAB), 10 mL of n-butanol and 30 mL of n-hexane to a flask and sonicate at 40 kHz for 30 min to obtain microemulsion.

[0042] (2) Preparation of metal salt solution: Dissolve 0.5 mmol cerium chloride, 0.5 mmol cobalt chloride and 0.5 mmol nickel chloride in 1 mL ultrapure water, and sonicate at 40 kHz for 10 min. After all the metal salts are completely dissolved, the metal salt solution can be obtained.

[0043] (3) Preparation of gel precursor: The prepared metal salt solution was poured into a flask containing the microemulsion, and 0.02 mol of potassium hydroxide was added to obtain a mixed solution. The mixed solution was then stirred on a stirrer for 2 hours at a speed of 1000 r / min. After the reaction was completed, the gel product was separated by centrifugation and washed three times with ethanol and deionized water. Then, it was dried in an oven at 60°C to obtain the gel precursor.

[0044] (4) Catalyst preparation: The dried gel precursor was placed in a crucible and then placed in a muffle furnace for high-temperature calcination. The heating rate was 5℃ / min, the calcination temperature was 900℃, and the heating time was 10h. After the system cooled naturally to room temperature, the black solid was removed and ground into powder to obtain the catalyst. The catalyst in this example was named CeCoNiO. x .

[0045] Example 4 A GdCoNiO x The preparation method of the catalyst differs from that in Example 1 in that the types of metal elements in the metal salt solution are different, and specifically includes the following steps: (1) Preparation of microemulsion: Add 0.03 mol of cetyltrimethylammonium bromide (CTAB), 10 mL of n-butanol and 30 mL of n-hexane to a flask and sonicate at 40 kHz for 30 min to obtain microemulsion.

[0046] (2) Preparation of metal salt solution: Dissolve 0.5 mmol gadolinium chloride, 0.5 mmol cobalt chloride and 0.5 mmol nickel chloride in 1 mL of ultrapure water, and sonicate at 40 kHz for 10 min. After all the metal salts are completely dissolved, the metal salt solution can be obtained.

[0047] (3) Preparation of gel precursor: The prepared metal salt solution was poured into a flask containing the microemulsion, and 0.02 mol of potassium hydroxide was added to obtain a mixed solution. The mixed solution was then stirred on a stirrer for 2 hours at a speed of 1000 r / min. After the reaction was completed, the gel product was separated by centrifugation and washed three times with ethanol and deionized water. Then, it was dried in an oven at 60°C to obtain the gel precursor.

[0048] (4) Catalyst preparation: The dried gel precursor was placed in a crucible and then placed in a muffle furnace for high-temperature calcination. The heating rate was 5℃ / min, the calcination temperature was 900℃, and the heating time was 10h. After the system cooled naturally to room temperature, the black solid was removed and ground into powder to obtain the catalyst. The catalyst in this example was named GdCoNiO. x .

[0049] Example 5 A method for preparing a CoNiO2 catalyst differs from Example 1 in that the type of metal element in the metal salt solution is different, and specifically includes the following steps: (1) Preparation of microemulsion: Add 0.03 mol of cetyltrimethylammonium bromide (CTAB), 10 mL of n-butanol and 30 mL of n-hexane to a flask and sonicate at 40 kHz for 30 min to obtain microemulsion.

[0050] (2) Preparation of metal salt solution: Dissolve 0.5 mmol cobalt chloride and 0.5 mmol nickel chloride in 1 mL of ultrapure water, and sonicate at 40 kHz for 10 min. After all metal salts are completely dissolved, the metal salt solution can be obtained.

[0051] (3) Preparation of gel precursor: The prepared metal salt solution was poured into a flask containing the microemulsion, and 0.02 mol of potassium hydroxide was added to obtain a mixed solution. The mixed solution was then stirred on a stirrer for 2 hours at a speed of 1000 r / min. After the reaction was completed, the gel product was separated by centrifugation and washed three times with ethanol and deionized water. Then, it was dried in an oven at 60°C to obtain the gel precursor.

[0052] (4) Catalyst preparation: The dried gel precursor was placed in a crucible and then placed in a muffle furnace for high-temperature calcination at a heating rate of 5°C / min, a calcination temperature of 900°C, and a heating time of 10 h. After the system cooled naturally to room temperature, the black solid was removed and ground into powder to obtain the catalyst. The catalyst in this example was named CoNiO2.

[0053] Test case (1) The catalysts prepared in Examples 1 and 2-5 were characterized.

[0054] The catalyst prepared in Example 1 was characterized by TEM, elemental distribution, HRTEM, and XRD. The results are shown in the figure. Figure 1 , 2 As shown in Figures 3 and 4. Figure 1 The TEM images clearly show that the catalyst prepared in Example 1 has obvious heterogeneous structural features. Figure 2 The elemental distribution diagram further shows that lanthanum, cerium, gadolinium, cobalt, and nickel are uniformly distributed in the catalyst, confirming its high-entropy heterostructure. Figure 3 HRTEM images clearly show the grain boundary structure in the catalyst, and the lattice distortion caused by this structure helps to improve the catalytic performance of the material. Furthermore, Figure 4 The sharp diffraction peaks appearing in the XRD pattern also confirm that the catalyst prepared in Example 1 has good crystallinity.

[0055] The catalysts of Examples 2-5 were characterized by TEM. Figure 5 As can be seen from the results, compared to the LaCeGdCoNiO prepared in Example 1, x The high-entropy heterojunction catalysts, synthesized in Examples 2-5 with different rare earth elements, exhibit drastically different morphologies and structural characteristics. Specifically, without the introduction of rare earth elements, the CoNiO2 catalyst in Example 5 has a nanoparticle morphology; when rare earth elements are doped, the LaCoNiO2 catalyst in Example 2... x The catalyst transforms into an irregular bulk morphology, as seen in CeCoNiO in Example 3. x The catalyst is transformed into core-shell structured nanosheets, such as CeCoNiO in Example 4. x The catalyst is transformed into a nanosheet structure.

[0056] (2) The oxygen evolution reaction (OER) performance of the catalysts prepared in Examples 1-5 was tested.

[0057] OER performance testing process: The OER test was conducted using a traditional three-electrode system on a Chenhua workstation, where the working electrode was a carbon paper (1 cm²) loaded with the catalyst. -2 The reference electrode was Hg / HgO, and the counter electrode was a stone rod. The catalyst ink was prepared by adding 5 mg of freshly prepared catalyst, 5 mg of conductive carbon black, 0.5 mL of ultrapure water, 0.5 mL of ethanol, and 20 μL of ethanol-Nafion solution (0.5 wt.%). During the preparation of the working electrode, 50 μL of the prepared ink was added dropwise onto carbon paper, resulting in a catalyst loading of 0.25 mg / cm³. -2 OER performance was obtained by linear scanning in 1M KOH electrolyte at a scan rate of 5mV / s.

[0058] In terms of OER catalytic performance, catalyst activity is closely related to the type of rare earth element added. For example... Figure 6 The OER polarization curves of LaCeGdCoNiO are shown in Table 1 below. Under the same test conditions, the polarization curves of LaCeGdCoNiO are shown in Table 1 below. x The high-entropy heterojunction catalyst (Example 1) exhibited optimal catalytic activity at 10 mA / cm². 2 The overpotential at the current density is only 199 mV, which is significantly lower than that of the commercial catalyst RuO2 (297 mV) and superior to that of currently reported mainstream transition metal-based catalysts (typically above 200 mV). Furthermore, its experimental results are also significantly better than the catalysts in Examples 2-5 that incorporate a rare earth element, such as LaCoNiO in Example 2. x The overpotential is 285mV, and in Example 3, CeCoNiO x The overpotential is 206mV. In Example 4, GdCoNiO x The overpotential was 219 mV. In Example 5, the CoNiO2 catalyst without rare earth elements had the weakest performance, with an overpotential as high as 361 mV. The above results indicate that the high-entropy heterostructure catalyst with multi-rare earth element synergistic optimization involved in this invention has significant advantages in the OER process. It is speculated that its excellent catalytic performance is mainly due to: (1) the high-entropy effect unique to high-entropy oxides can effectively regulate the electronic structure of active sites; (2) the grain boundaries formed by the heterostructure and the lattice distortion it causes can adjust the position of the d-band of the active center through stress effect, further optimizing the electronic structure.

[0059] Table 1. OER test results of the catalysts prepared in Examples 1-5

[0060] (3) LaCeGdCoNiO prepared in Example 1 x Stability testing of high-entropy heterojunction catalysts Stability testing procedure: The stability testing conditions are the same as the OER performance testing procedure, but the testing method used is the time-potential method, and the constant test current set during the test is 50mA / cm. -2 .

[0061] Depend on Figure 7 The long-term stability test results show that LaCeGdCoNiO x High-entropy heterostructure catalysts at 50 mA / cm 2 It can operate stably for more than 600 hours at current density, exhibiting excellent electrochemical stability, which is mainly due to the stable structural characteristics of this high-entropy heterostructure in an alkaline environment.

[0062] Finally, it should be noted that the above embodiments are only used to illustrate the technical solutions of the present invention and not to limit them. Although the present invention has been described in detail with reference to preferred embodiments, those skilled in the art should understand that modifications or equivalent substitutions can still be made to the technical solutions of the present invention, and these modifications or equivalent substitutions cannot cause the modified technical solutions to deviate from the spirit and scope of the technical solutions of the present invention.

Claims

1. A LaCeGdCoNiO x A method for preparing a high-entropy heterojunction catalyst, characterized in that: Includes the following steps: S1: Preparation of microemulsion A microemulsion was obtained by mixing hexadecyltrimethylammonium bromide, n-butanol, and n-hexane and then sonicating it. S2: Preparation of metal salt solution Lanthanum salt, cerium salt, gadolinium salt, cobalt salt, and nickel salt were dissolved in ultrapure water and subjected to ultrasonic treatment to obtain a metal salt solution; S3: Preparation of gel precursor The metal salt solution was poured into the microemulsion, then potassium hydroxide was added and stirred to carry out the reaction. After centrifugation, washing and drying, the gel precursor was obtained. S4: Catalyst Preparation The gel precursor was calcined and ground to obtain LaCeGdCoNiO x High-entropy heterojunction catalyst.

2. The LaCeGdCoNiO according to claim 1 x A method for preparing a high-entropy heterojunction catalyst, characterized in that: In step S1, the amount of hexadecyltrimethylammonium bromide added is 0.01~0.05 mol, the amount of n-butanol added is 5~15 mL, and the amount of n-hexane added is 10~50 mL.

3. The LaCeGdCoNiO according to claim 1 x A method for preparing a high-entropy heterojunction catalyst, characterized in that: In step S1, the frequency of ultrasonic treatment is 20~60KHz and the time is 20~40min.

4. The LaCeGdCoNiO according to claim 1 x A method for preparing a high-entropy heterojunction catalyst, characterized in that: In step S2, the amount of metal element added to lanthanum salt, cerium salt, gadolinium salt, cobalt salt and nickel salt is 0.2~1.0 mmol, and the amount of ultrapure water added is 0.5~1.5 mL, based on the number of moles of metal element in the metal salt.

5. The LaCeGdCoNiO according to claim 1 x A method for preparing a high-entropy heterojunction catalyst, characterized in that: In step S2, the frequency of ultrasonic treatment is 20~60KHz and the time is 5~15min.

6. The LaCeGdCoNiO according to claim 1 x A method for preparing a high-entropy heterojunction catalyst, characterized in that: In step S3, the amount of potassium hydroxide added is 0.01~0.04 mol.

7. The LaCeGdCoNiO according to claim 1 x A method for preparing a high-entropy heterojunction catalyst, characterized in that: In step S3, the stirring speed is 500~1500 r / min and the stirring time is 1~3 h.

8. The LaCeGdCoNiO according to claim 1 x A method for preparing a high-entropy heterojunction catalyst, characterized in that: In step S4, the heating rate during calcination is 2~10℃ / min, the calcination temperature is 700~1000℃, and the heating time is 6~10h.

9. A LaCeGdCoNiO x High-entropy heterojunction catalyst, characterized in that: It is prepared by the preparation method according to any one of claims 1 to 8.

10. A LaCeGdCoNiO according to claim 9 x The application of high-entropy heterojunction catalysts is characterized by: LaCeGdCoNiO x High-entropy heterojunction catalysts are used in electrocatalytic oxygen evolution reactions.

Images