A high-entropy metal phosphorus-sulfur compound nanosheet, a preparation method therefor and applications thereof

By preparing high-entropy metal phosphorus sulfide nanosheets and combining them with polar solvents and ultrasonic fragmentation technology, the problem of poor catalytic performance of two-dimensional metal phosphorus sulfides was solved, and a significant improvement in catalytic performance was achieved, especially in electrocatalytic reactions.

CN119320176BActive Publication Date: 2026-05-12HARBIN INST OF TECH
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Patent Information

Authority / Receiving Office
CN · China
Patent Type
Patents(China)
Current Assignee / Owner
HARBIN INST OF TECH
Filing Date
2024-10-16
Publication Date
2026-05-12

AI Technical Summary

Technical Problem

Existing two-dimensional metal phosphorus sulfides have poor catalytic performance. Single or simple element doping cannot effectively improve their basal active sites, thus limiting further improvement in catalytic performance.

Method used

A high-entropy metal phosphorus-sulfur compound nanosheet was prepared by mixing powders of manganese, cobalt, nickel, copper, silver, phosphorus and sulfur for solid-phase synthesis, and then using polar solvents and ultrasonic fragmentation technology to exfoliate the bulk sample to prepare nanosheets with a large specific surface area and abundant active sites.

Benefits of technology

It improves the catalytic performance of two-dimensional metal phosphorus sulfides, especially showing higher activity and efficiency in electrocatalytic hydrogen evolution and oxygen evolution reactions.

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Abstract

The application provides a high-entropy metal phosphorus-sulfur compound nanosheet and a preparation method and application thereof. The preparation method of the high-entropy metal phosphorus-sulfur compound nanosheet comprises the following steps: mixing manganese, cobalt, nickel, copper, silver, phosphorus and sulfur element powders according to a preset mass ratio, uniformly grinding, and then tabletting to obtain a tablet sample; vacuumizing the tablet sample and then packaging; heating the packaged tablet sample to 590-710 DEG C, keeping warm for 150-200 h, and then cooling to obtain a bulk sample; grinding the bulk sample, dispersing in a polar solvent, and then ultrasonic cleaning to obtain a cleaning mixed solution; taking supernatant of the cleaning mixed solution, performing ultrasonic crushing treatment, and then centrifuging to obtain a nanosheet crude product; and cleaning the nanosheet crude product, and then performing vacuum freeze drying to obtain a nanosheet product. The application aims to solve the problem of poor catalytic performance of metal phosphorus-sulfur compounds.
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Description

Technical Field

[0001] This invention relates to the technical field of nanocatalyst materials, and more specifically, to a high-entropy metal phosphorus-sulfur compound nanosheet, its preparation method, and its application. Background Technology

[0002] Two-dimensional metal phosphorus sulfides (MPCh3) are promising catalytic platforms due to their high specific surface area and unique electronic structure. However, the poor basal activity of MPCh3 alone fails to provide sufficient active sites for the reaction, thus limiting further improvement in its catalytic performance.

[0003] Currently, doping MPCh3 with mono- or binary elements is a common material design and preparation strategy to regulate the activity of its basal sites. For example, in related technologies, boron (B) and carbon (C) doping is used to transform the semiconductor NiPS3 into a metallic state, thereby activating the in-plane active sites of NiPS3. However, the activation performance of single or simple element combinations is limited, which is not conducive to further improving the catalyst performance. Summary of the Invention

[0004] The present invention aims to solve the problem of poor catalytic performance of metal phosphorus sulfides.

[0005] To address the above problems, this invention provides a high-entropy metal phosphorus-sulfur compound nanosheet, its preparation method, and its application.

[0006] In a first aspect, the present invention provides a method for preparing high-entropy metal phosphorus-sulfur compound nanosheets, comprising:

[0007] Manganese, cobalt, nickel, copper, silver, phosphorus and sulfur powders are mixed according to a preset mass ratio, ground evenly and then compressed into tablets to obtain tablet samples.

[0008] The compressed sample was vacuum-sealed and then packaged.

[0009] The packaged tablet sample was heated to 590-710℃ and kept at that temperature for 150-200h, then cooled to obtain a block sample.

[0010] The bulk sample was ground and then dispersed in a polar solvent for ultrasonic cleaning to obtain a cleaning mixture.

[0011] The supernatant of the cleaning mixture was subjected to ultrasonic disruption and centrifugation to obtain crude nanosheet product.

[0012] After cleaning the crude nanosheet product, it is subjected to vacuum freeze-drying to obtain the nanosheet product.

[0013] Optionally, the elemental powders are mixed in the following mass proportions: 0.03-0.035 parts manganese, 0.15-0.2 parts cobalt, 0.025-0.035 parts nickel, 0.01-0.025 parts copper, 0.02-0.035 parts silver, 0.17-0.19 parts phosphorus and 0.45-0.55 parts sulfur.

[0014] Optionally, the heating rate of the packaged tablet sample is 1-5℃ / min.

[0015] Optionally, the centrifugation includes:

[0016] First, centrifuge the supernatant at a speed of 3000-4000 r / min, and then take the centrifuged supernatant and centrifuge it at a speed of 9000-10000 r / min.

[0017] Optionally, the vacuum pressure range for the tablet sample is 7 × 10⁻⁶. -4 -9×10 -4 Pa.

[0018] Secondly, the present invention also provides a high-entropy metal phosphorus-sulfur compound nanosheet prepared based on the above preparation method.

[0019] Optionally, the high-entropy metal phosphorus-sulfur compound nanosheets include the following elements: manganese, cobalt, nickel, copper, silver, phosphorus, and sulfur;

[0020] The molar ratio of manganese, cobalt, nickel, copper, silver, phosphorus and sulfur is (0.1-0.2):(0.1-0.2):(0.1-0.2):(0.1-0.2):(0.1-0.2):1:3.

[0021] Optionally, the thickness of the high-entropy metal phosphorus-sulfur compound nanosheets ranges from 1.5 to 4.5 nm.

[0022] Optionally, the high-entropy metal phosphorus-sulfur compound nanosheets have 1-4 layers.

[0023] Thirdly, the present invention also provides the application of the above-mentioned high-entropy metal phosphorus-sulfur compound nanosheets in electrocatalytic hydrogen evolution reaction and electrocatalytic oxygen evolution reaction.

[0024] The advantages of this invention compared to the prior art include:

[0025] This invention involves solid-state synthesis of various high-entropy metal elements and phosphorus and sulfur elements at a temperature of 590-710℃. Then, a polar solvent is used to initially exfoliate the synthesized bulk sample into single-layer or few-layer samples. The polar solvent helps the bulk sample overcome the van der Waals forces between layers, thus facilitating the initial exfoliation. Finally, the initially exfoliated sample is further exfoliated using ultrasonic fragmentation to ensure complete exfoliation. The fully exfoliated nanosheets have a large specific surface area and abundant active sites, promoting catalytic performance. Ultrasonic exfoliation reduces the number of nanosheet layers while also causing them to break, gradually reducing the lateral size of the nanosheets and shortening the migration distance of electrons between the electrode and the catalyst active sites, thereby activating the overall catalytic performance. In summary, this invention prepares high-entropy metal phosphorus-sulfur compound nanosheets through solid-state synthesis and solvent / ultrasonic exfoliation methods, applying a high-entropy alloy formed by various metal elements in a specific ratio to two-dimensional metal phosphorus-sulfides to regulate the basal site activity of the two-dimensional metal phosphorus-sulfides. This combines the advantages of the large specific surface area of ​​two-dimensional metal phosphorus sulfide materials with the advantages of high-entropy alloys in continuous control of surface adsorption performance, thereby improving the catalytic performance of two-dimensional metal phosphorus sulfides. Attached Figure Description

[0026] Figure 1 This is an atomic force microscopy characterization result of the nanosheet product obtained in Example 1 of this invention;

[0027] Figure 2 This is the XRD pattern of the nanosheet product obtained in Example 1 of this invention;

[0028] Figure 3 These are electrochemical characterization diagrams of hydrogen evolution for various embodiments and comparative examples of the present invention;

[0029] Figure 4 These are electrochemical characterization diagrams of oxygen evolution in various embodiments and comparative examples of the present invention. Detailed Implementation

[0030] To make the above-mentioned objects, features, and advantages of the present invention more apparent and understandable, specific embodiments of the present invention will be described in detail below with reference to the accompanying drawings. Although some embodiments of the present invention are shown in the drawings, it should be understood that the present invention can be implemented in various forms and should not be construed as limited to the embodiments set forth herein. Rather, these embodiments are provided to provide a more thorough and complete understanding of the present invention. It should be understood that the accompanying drawings and embodiments of the present invention are for illustrative purposes only and are not intended to limit the scope of protection of the present invention.

[0031] Unless otherwise defined, all technical and scientific terms used in this application have the same meaning as commonly understood by one of ordinary skill in the art to which this application pertains; the terminology used in the description of this application is for the purpose of describing particular embodiments only and is not intended to limit this application.

[0032] The term "comprising" and its variations as used herein are open-ended, meaning "including but not limited to"; the term "based on" means "at least partially based on"; the term "one embodiment" means "at least one embodiment"; the term "another embodiment" means "at least one additional embodiment"; the term "some embodiments" means "at least some embodiments"; and the term "optionally" means "optional embodiments". Definitions of other terms will be given in the description below. It should be noted that the concepts of "first," "second," etc., mentioned in this invention are used to distinguish different objects, not to describe a specific order or hierarchy. Furthermore, the terms "first" and "second" are used for descriptive purposes only and should not be construed as indicating or implying relative importance or implicitly specifying the number of indicated technical features. Thus, a feature defined with "first" or "second" may explicitly or implicitly include one or more of that feature. In the description of this application, unless otherwise stated, "a plurality of" means two or more.

[0033] High-entropy alloys are a novel type of material system that combines multiple elements in equal or near-equal proportions. Due to their rich elemental composition, high-entropy alloys can provide a broad combinatorial space for the design of high-performance catalysts. Furthermore, high-entropy alloys possess continuously tunable adsorption energies, enabling the optimization of the kinetic barriers for intermediate adsorption and desorption during catalysis. However, high-entropy alloys prepared by traditional methods are mostly bulk materials, making it difficult to effectively expose active sites and thus limiting their application in enhancing the catalytic performance of two-dimensional metal phosphorus sulfides.

[0034] This invention provides a method for preparing high-entropy metal phosphorus-sulfur compound nanosheets, comprising:

[0035] Manganese, cobalt, nickel, copper, silver, phosphorus and sulfur powders are mixed according to a preset mass ratio, ground evenly and then compressed into tablets to obtain tablet samples.

[0036] The compressed sample was vacuum-sealed and then packaged.

[0037] The packaged tablet sample was heated to 590-710℃ and kept at that temperature for 150-200h, then cooled to obtain a block sample.

[0038] The bulk sample was ground and then dispersed in a polar solvent for ultrasonic cleaning to obtain a cleaning mixture.

[0039] The supernatant of the cleaning mixture was subjected to ultrasonic disruption and centrifugation to obtain crude nanosheet product.

[0040] After cleaning the crude nanosheet product, it is subjected to vacuum freeze-drying to obtain the nanosheet product.

[0041] In this embodiment of the invention, various high-entropy metal elements and phosphorus and sulfur elements are synthesized in a solid-state manner at a temperature of 590-710℃. Then, a polar solvent is used to initially exfoliate the synthesized bulk sample into single-layer or few-layer samples. The polar solvent helps the bulk sample overcome the van der Waals forces between layers, thus achieving initial exfoliation. Finally, the initially exfoliated sample is further exfoliated using ultrasonic fragmentation to ensure complete exfoliation. The fully exfoliated nanosheets have a large specific surface area and abundant active sites, promoting catalytic performance. Ultrasonic exfoliation reduces the number of nanosheet layers and also causes them to break, gradually reducing the lateral size of the nanosheets and shortening the migration distance of electrons between the electrode and the catalyst active sites, thereby activating the overall catalytic performance. This combines the advantages of the large specific surface area of ​​two-dimensional metal phosphorus sulfide materials with the advantages of continuous control of surface adsorption performance by high-entropy alloys, improving the catalytic performance of two-dimensional metal phosphorus sulfides.

[0042] Optionally, when preparing high-entropy metal phosphorus-sulfur compound nanosheets, the elemental powders can be mixed in the following mass proportions: 0.03-0.035 parts manganese, 0.15-0.2 parts cobalt, 0.025-0.035 parts nickel, 0.01-0.025 parts copper, 0.02-0.035 parts silver, 0.17-0.19 parts phosphorus and 0.45-0.55 parts sulfur.

[0043] In this embodiment, the elemental powders are mixed, ground, and then compressed into tablets according to the above-mentioned mass ratio. The tableting process ensures sufficient contact between the elemental powders during the solid-phase reaction, improving reaction efficiency. Ultimately, a chemically homogeneous product with nearly equal proportions of each metal element is obtained. This approach minimizes raw material consumption and reduces production costs while ensuring product quality.

[0044] In some optional embodiments, the tablet sample is vacuum-sealed, including: placing the tablet sample into a quartz tube and vacuuming it to a pressure of 7 × 10⁻⁶. -4 -9×10 -4 Pa is then used for encapsulation with a flame torch. This avoids interference from other gaseous impurities and other contaminants on the solid-phase reaction, ensuring the homogeneity of the high-entropy alloy and achieving excellent mechanical properties and chemical stability.

[0045] In some optional embodiments, when heating the packaged tablet sample, the heating rate of the tablet sample is 1-5℃ / min. Slow heating is conducive to the uniform growth of the material and avoids the segregation of a single phase.

[0046] In some optional embodiments, after the bulk sample is ground, it is dispersed in a polar solvent for ultrasonic cleaning. The polar solvent includes an aqueous solution of ethanol or isopropanol, preferably an aqueous solution of ethanol. The polar solvent helps the bulk sample overcome the interlayer van der Waals forces, thereby initially exfoliating the bulk sample into a few-layer or monolayer sample.

[0047] Optionally, after ultrasonic disruption, the centrifugation process specifically includes: first centrifuging the supernatant at 3000-4000 r / min, and then centrifuging the supernatant at 9000-10000 r / min. This removes large, incompletely dissected sample fragments, ensuring the acquisition of high-quality few-layer or single-layer nanosheets.

[0048] Optionally, the cleaning process for the crude nanosheet product includes: first cleaning the surface of the crude nanosheet product with an aqueous solution of ethanol to remove residual polar solvents, and then cleaning with water.

[0049] Secondly, embodiments of the present invention provide a high-entropy metal phosphorus-sulfur compound nanosheet prepared based on the above preparation method, comprising the following elements: manganese, cobalt, nickel, copper, silver, phosphorus and sulfur; wherein the molar ratio of manganese, cobalt, nickel, copper, silver, phosphorus and sulfur is (0.1-0.2):(0.1-0.2):(0.1-0.2):(0.1-0.2):(0.1-0.2):1:3.

[0050] In this embodiment, the high-entropy metal phosphorus-sulfur compound nanosheets contain a variety of high-entropy metal elements in equal or nearly equal proportions, exhibiting high overall uniformity. Furthermore, the combination of the advantages of two-dimensional phosphorus-sulfur compounds and a large surface area, along with the continuous control of surface adsorption performance by high-entropy alloys, significantly enhances the overall catalytic performance of the nanosheets.

[0051] Optionally, the thickness of the high-entropy metal phosphorus-sulfur compound nanosheets ranges from 1.5 to 4.5 nm, and the nanosheets have a layered structure with 1 to 4 layers. Specifically, the main thickness distribution of the nanosheets is 3 to 4 layers, while the sample also contains 1 to 2 monolayers, with a uniform overall layer distribution. Compared to bulk samples, the thickness of the high-entropy metal phosphorus-sulfur compound nanosheets in this embodiment is significantly reduced, and the layered structure of the nanosheets has a large specific surface area and abundant active sites. This is beneficial for reducing the material size, and the prepared nanosheets retain a large number of edge active sites while maintaining the advantage of controllable morphology and layer number, thus promoting the catalytic performance.

[0052] This invention also provides an application of the above-mentioned high-entropy metal phosphorus-sulfur compound nanosheets in electrocatalytic hydrogen evolution reaction and electrocatalytic oxygen evolution reaction.

[0053] The present invention will be described in detail below through specific embodiments and comparative examples.

[0054] Example 1

[0055] This embodiment provides a method for preparing the above-mentioned high-entropy metal phosphorus-sulfur compound nanosheets, including:

[0056] S1: Mix the powdered elements according to the following mass: 0.0325g manganese, 0.175g cobalt, 0.03g nickel, 0.0175g copper, 0.0275g silver, 0.18g phosphorus, and 0.5g sulfur. After grinding the powders evenly, press them into tablets using a ring-shaped mold to ensure sufficient contact between the elements during the subsequent reaction.

[0057] S2: Place the compressed sample into a quartz tube and evacuate until the air pressure inside the tube reaches 7 × 10⁻⁶. -4 When Pa is applied, it is sealed with a flame torch.

[0058] S3: Place the quartz tube in a muffle furnace and heat it to 610°C at a heating rate of 1°C / min. Then, keep the quartz tube at 610°C for 168 hours and cool it with the furnace.

[0059] S4: After grinding the block sample, disperse it in an aqueous solution of ethanol and ultrasonically clean it for 2 hours in an ultrasonic cleaner.

[0060] S5: Take the supernatant of the mixed solution and further process it with an ultrasonic disruptor for 3 hours. Then put the solution into a centrifuge and centrifuge it at 3000 r / min. Then take the supernatant after centrifugation and further centrifuge it at 9000 r / min to obtain the crude nanosheet product.

[0061] S6: The crude product is washed with ethanol and water in sequence, and then freeze-dried in a vacuum freeze dryer for 24 hours to obtain the nanosheet product.

[0062] The nanosheet product in this embodiment includes the following elements: manganese, cobalt, nickel, copper, silver, phosphorus and sulfur, wherein the molar ratio of manganese, cobalt, nickel, copper, silver, phosphorus and sulfur is 0.15:0.15:0.15:0.15:0.15:1:3.

[0063] The atomic force microscopy characterization results of the nanosheet product prepared in this embodiment are as follows: Figure 1 As shown, the high-entropy metal phosphorus-sulfur compound nanosheets prepared in this embodiment have a thickness range of 1.5-4.5 nm, a layered structure, and 1-4 layers.

[0064] The XRD pattern of the nanosheet product prepared in this embodiment is shown in the figure below. Figure 2 As shown, it should be noted that, for ease of representation, the chemical formula of the nanosheet products prepared in the embodiments of this invention is all represented by MnCoNiCuAgPS3. Figure 2 It can be seen that the MnCoNiCuAgPS3 nanosheets prepared in the embodiments of the present invention have a monoclinic phase crystal structure, indicating that the high-entropy material was successfully synthesized without segregation.

[0065] Example 2

[0066] The difference between this embodiment and Embodiment 1 is that in the high-entropy metal phosphorus-sulfur compound nanosheets of this embodiment, the molar ratio of manganese, cobalt, nickel, copper, silver, phosphorus and sulfur is 0.1:0.1:0.1:0.1:0.1:1:3.

[0067] Methods for preparing high-entropy metal phosphorus-sulfur compound nanosheets include:

[0068] S1: Mix the powdered elements according to the following mass: 0.03g manganese, 0.15g cobalt, 0.025g nickel, 0.01g copper, 0.02g silver, 0.17g phosphorus, and 0.45g sulfur. After grinding the powders evenly, press them into tablets using a ring-shaped mold to ensure sufficient contact between the elements during subsequent reactions.

[0069] S2: Place the compressed sample into a quartz tube and evacuate until the air pressure inside the tube reaches 8.5 × 10⁻⁶. -4 When Pa is applied, it is sealed with a flame torch.

[0070] S3: Place the quartz tube in a muffle furnace and heat it to 590°C at a heating rate of 3°C / min. Then, keep the quartz tube at 590°C for 200 hours and cool it with the furnace.

[0071] S4: After grinding the block sample, disperse it in an aqueous solution of ethanol and ultrasonically clean it for 2 hours in an ultrasonic cleaner.

[0072] S5: Take the supernatant of the mixed solution and further process it with an ultrasonic disruptor for 3 hours. Then put the solution into a centrifuge and centrifuge it at 4000 r / min. Then take the supernatant after centrifugation and centrifuge it at 10000 r / min to obtain the crude nanosheet product.

[0073] S6: The crude product is washed with ethanol and water in sequence, and then freeze-dried in a vacuum freeze dryer for 24 hours to obtain the nanosheet product.

[0074] In this embodiment, high-entropy metal phosphorus-sulfur compound nanosheets were successfully synthesized. The thickness of the nanosheet products ranged from 2 to 4.5 nm, with a layered structure and 1 to 4 layers.

[0075] Example 3

[0076] The difference between this embodiment and Embodiment 1 is that in the high-entropy metal phosphorus-sulfur compound nanosheets of this embodiment, the molar ratio of manganese, cobalt, nickel, copper, silver, phosphorus and sulfur is 0.2:0.2:0.2:0.2:0.2:1:3.

[0077] Methods for preparing high-entropy metal phosphorus-sulfur compound nanosheets include:

[0078] In step S1, the element powders are mixed according to the following masses: 0.035g manganese, 0.2g cobalt, 0.035g nickel, 0.025g copper, 0.035g silver, 0.19g phosphorus, and 0.55g sulfur.

[0079] In step S2, the compressed sample is placed in a quartz tube and a vacuum is drawn until the air pressure inside the tube reaches 9 × 10⁻⁶. -4 When Pa is applied, it is sealed with a flame torch.

[0080] In step S3, the quartz tube is placed in a muffle furnace and heated to 590°C at a heating rate of 5°C / min. The quartz tube is then held at 710°C for 150 hours and cooled with the furnace. The other steps are the same.

[0081] In this embodiment, high-entropy metal phosphorus-sulfur compound nanosheets were successfully synthesized. The thickness of the nanosheet products ranged from 2 to 4 nm, and they had a layered structure with 1 to 4 layers.

[0082] Comparative Example 1

[0083] The difference between Comparative Example 1 and Example 1 is that in step S1 of the method for preparing high-entropy metal phosphorus-sulfur compound nanosheets, the elemental powders in the following mass ratio are mixed: 0.027 g vanadium, 0.03 g manganese, 0.191 g cobalt, 0.032 g nickel, 0.035 g zinc, 0.167 g phosphorus, and 0.518 g sulfur. The other steps are the same.

[0084] Comparative Example 2

[0085] The difference between Comparative Example 2 and Example 1 is that in step S1 of the method for preparing high-entropy metal phosphorus-sulfur compound nanosheets, the elemental powders in the following mass ratio are mixed: 0.034 g vanadium, 0.035 g manganese, 0.21 g cobalt, 0.035 g nickel, 0.038 g zinc, 0.173 g phosphorus, and 0.532 g sulfur. The other steps are the same.

[0086] Comparative Example 3

[0087] The difference between Comparative Example 3 and Example 1 is that in step S1 of the method for preparing high-entropy metal phosphorus-sulfur compound nanosheets, the elemental powders in the following mass ratio are mixed: 0.038 g vanadium, 0.037 g manganese, 0.24 g cobalt, 0.052 g nickel, 0.04 g zinc, 0.185 g phosphorus, and 0.57 g sulfur. The other steps are the same.

[0088] Electrochemical tests were conducted on the nanosheet products prepared in Examples 1-3 and Comparative Examples 1-3. The test solution was a 1M KOH aqueous solution, the reference electrode was Hg / HgO, and the counter electrode was a graphite rod.

[0089] Electrochemical characterization of hydrogen evolution in each embodiment and comparative example is as follows: Figure 3 As shown. By Figure 3 It can be seen that the nanosheet products in Examples 1-3 exhibit excellent alkaline hydrogen evolution activity. Specifically, at a current density of 10 mA / cm², 2 Under the same conditions, compared to -93.3mV, -122.5mV, and -187.9mV in Comparative Examples 1-3, and Tafel slopes of 76.4mV / dec, 81.5mV / dec, and 93.1mV / dec, the overpotentials of the nanosheet products in Examples 1-3 were -51.8mV, -60.1mV, and -67.6mV, respectively, and the Tafel slopes were 61.5mV / dec, 65.7mV / dec, and 70.9mV / dec, respectively. These lower overpotentials indicate that the nanosheet products prepared in the embodiments of this invention exhibit higher catalytic activity in the electrocatalytic hydrogen evolution reaction.

[0090] The electrochemical characterization of oxygen evolution in each embodiment and comparative example is as follows: Figure 4 As shown. By Figure 4 It can be seen that the nanosheet products in Examples 1-3 exhibit excellent alkaline oxygen evolution activity. Specifically, at a current density of 10 mA / cm², 2 Under the same conditions, compared to 350mV, 380mV, and 430mV in Comparative Examples 1-3, with Tafel slopes of 170.8mV / dec, 126.2mV / dec, and 143.2mV / dec, the overpotentials of the nanosheet products in Examples 1-3 were 230mV, 280mV, and 320mV, respectively, with Tafel slopes of 83.7mV / dec, 81.4mV / dec, and 103.2mV / dec, respectively. These lower overpotentials indicate that the nanosheet products prepared in the embodiments of this invention exhibit higher catalytic activity in the electrocatalytic oxygen evolution reaction.

[0091] While the present invention has been disclosed above, its scope of protection is not limited thereto. Those skilled in the art can make various changes and modifications without departing from the spirit and scope of the present invention, and all such changes and modifications will fall within the scope of protection of the present invention.

Claims

1. A method for preparing high-entropy metal phosphorus-sulfur compound nanosheets, characterized in that, include: Manganese, cobalt, nickel, copper, silver, phosphorus, and sulfur powders were mixed according to a preset mass ratio, ground evenly, and then compressed into tablets to obtain tablet samples. The powders of each element were mixed in the following mass proportions: 0.03-0.035 parts manganese, 0.15-0.2 parts cobalt, 0.025-0.035 parts nickel, 0.01-0.025 parts copper, 0.02-0.035 parts silver, 0.17-0.19 parts phosphorus, and 0.45-0.55 parts sulfur. The compressed sample was vacuum-sealed and then packaged. The packaged tablet sample was heated to 590-710℃ and kept at that temperature for 150-200h, then cooled to obtain a block sample. The bulk sample was ground and then dispersed in a polar solvent for ultrasonic cleaning to obtain a cleaning mixture. The supernatant of the cleaning mixture was subjected to ultrasonic disruption and centrifugation to obtain crude nanosheet product. After cleaning the crude nanosheet product, it is subjected to vacuum freeze-drying to obtain the nanosheet product.

2. The method for preparing high-entropy metal phosphorus-sulfur compound nanosheets according to claim 1, characterized in that, The heating rate of the packaged tablet sample is 1-5℃ / min.

3. The method for preparing high-entropy metal phosphorus-sulfur compound nanosheets according to claim 1, characterized in that, The centrifugation includes: First, centrifuge the supernatant of the cleaning mixture at a speed of 3000-4000 r / min, and then take the supernatant after centrifugation and centrifuge it at a speed of 9000-10000 r / min.

4. The method for preparing high-entropy metal phosphorus-sulfur compound nanosheets according to claim 1, characterized in that, The pressure range for vacuuming the tablet sample is 7×10⁻⁴-9×10⁻⁴ Pa.

5. A high-entropy metal phosphorus-sulfur compound nanosheet prepared by the preparation method according to any one of claims 1-4, wherein the high-entropy metal phosphorus-sulfur compound nanosheet comprises the following elements: manganese, cobalt, nickel, copper, silver, phosphorus and sulfur; in, The molar ratio of manganese, cobalt, nickel, copper, silver, phosphorus and sulfur is (0.1-0.2):(0.1-0.2):(0.1-0.2):(0.1-0.2):(0.1-0.2):1:

3.

6. The high-entropy metal phosphorus-sulfur compound nanosheets according to claim 5, characterized in that, The thickness of the high-entropy metal phosphorus-sulfur compound nanosheets ranges from 1.5 to 4.5 nm.

7. The high-entropy metal phosphorus-sulfur compound nanosheets according to claim 5, characterized in that, The high-entropy metal phosphorus-sulfur compound nanosheets have 1-4 layers.

8. The application of high-entropy metal phosphorus-sulfur compound nanosheets as described in any one of claims 5-7 in electrocatalytic hydrogen evolution reaction and electrocatalytic oxygen evolution reaction.