Organic small molecule for improving hydrogen evolution performance of molybdenum sulfide-based catalyst, molybdenum sulfide-based catalyst, preparation method and application thereof

Abstract

The application belongs to the technical field of catalyst preparation, and particularly relates to an organic small molecule for improving hydrogen evolution performance of a molybdenum sulfide-based catalyst, a molybdenum sulfide-based catalyst, a preparation method and application. End groups at two ends of the organic small molecule respectively include a cation and an anion; the anion includes at least one of a carboxylate ion, a sulfonate ion and a phosphate ion; and the cation has a specific structural formula. The organic small molecule can improve the water electrolysis hydrogen evolution performance of an existing molybdenum sulfide catalyst, especially alkaline water electrolysis hydrogen production.

Description

Technical Field

[0001] This invention belongs to the field of catalyst preparation technology, specifically relating to an organic small molecule for improving the hydrogen evolution performance of molybdenum sulfide-based catalysts, a molybdenum sulfide-based catalyst, its preparation method, and its application. Background Technology

[0002] Molybdenum sulfide catalysts theoretically possess superior hydrogen adsorption binding energies, closely comparable to those of the noble metal platinum, making them potential candidates for highly efficient hydrogen evolution catalysts. Furthermore, molybdenum sulfide-based catalysts are simple to prepare, abundant in reserves, and inexpensive. However, when facing the ever-increasing demand for high-efficiency hydrogen evolution catalysts, molybdenum sulfide catalysts still exhibit certain limitations.

[0003] Existing technologies for improving the hydrogen production performance of molybdenum sulfide electrolysis generally include creating defects and constructing heterojunctions. However, these methods have limited effectiveness in improving the hydrogen evolution performance of MoS2-based catalysts, especially under alkaline conditions, and are far from meeting industrial standards. Summary of the Invention

[0004] Therefore, the technical problem to be solved by the present invention is to overcome the defects of existing molybdenum sulfide catalysts, such as the need to further improve hydrogen evolution performance, and to provide an organic small molecule, a molybdenum sulfide-based catalyst, a preparation method and application for improving the hydrogen evolution performance of molybdenum sulfide-based catalysts.

[0005] To this end, the present invention provides the following technical solution.

[0006] This invention provides an organic small molecule for improving the hydrogen evolution performance of molybdenum sulfide-based catalysts. The terminal groups of the organic small molecule include cations and anions, respectively. The anions include at least one of carboxylate ions, sulfonate ions, and phosphate ions. The cations have at least one of the following structural formulas:

[0007]

[0008] Furthermore, the organic small molecule has one of the following structural formulas:

[0009]

[0010] Where n is 1-12. For example, n can be 1, 3, 6, 8, 10, 12 or any value within that range.

[0011] Furthermore, the organic small molecule has one of the following structural formulas:

[0012]

[0013] And / or,

[0014] The value of n is 1-5.

[0015] The present invention also provides a molybdenum sulfide-based catalyst, the molybdenum sulfide-based catalyst comprising molybdenum sulfide, the molybdenum sulfide comprising a 1T phase; the molybdenum sulfide-based catalyst comprising a quaternary ammonium group, and further comprising at least one of a carboxyl group, a sulfonic acid group and a phosphate group.

[0016] Furthermore, the molybdenum sulfide-based catalyst comprises a doped metal, wherein the doped metal comprises a transition metal and / or a noble metal; and / or,

[0017] The molybdenum sulfide-based catalyst also includes a support.

[0018] Further, the doped metal includes at least one selected from nickel, iron, cobalt, platinum, and ruthenium; and / or,

[0019] The carrier includes carbon nanotubes, graphene, or carbon fibers.

[0020] This invention provides a method for preparing a molybdenum sulfide-based catalyst, comprising a molybdenum source and a small organic molecule mixed together and subjected to a hydrothermal reaction; the terminal groups at both ends of the small organic molecule include cations and anions, respectively, wherein the anion includes at least one of carboxylate ions, sulfonate ions, and phosphate ions, and the cation has at least one of the following structural formulas:

[0021]

[0022] Furthermore, the mixing process further includes the addition of a sulfur source and / or a doped metal source; and / or,

[0023] The mixing process also includes the addition of a support, which may include carbon nanotubes, graphene, or carbon fibers; preferably, the mass ratio of the support to the molybdenum source is 1:(6-10); and / or,

[0024] The hydrothermal reaction is carried out at a temperature of 170-220℃ for a duration of 6-20 hours; and / or,

[0025] The organic small molecule has one of the following structural formulas:

[0026]

[0027] Where n is 1-12.

[0028] Further, the molybdenum source comprises molybdate and / or dimolybdate; preferably, the dimolybdate comprises (NH4)6Mo7O 24 The molybdate comprises at least one of (NH4)2MoO4, Na2MoO4, and K2MoO4; and / or,

[0029] The sulfur source includes a sulfur-containing compound, preferably, the sulfur-containing compound includes at least one of thiourea, thioether, and thioacetamide; and / or,

[0030] The metal in the doped metal source includes at least one of nickel, iron, cobalt, platinum, and ruthenium; and / or,

[0031] The doped metal source is a water-soluble salt of a doped metal; and / or,

[0032] The molar ratio of molybdenum in the molybdenum source, the doped metal in the doped metal source, the organic small molecule, and the sulfur source is 1:(0.05-0.2):(0.1-0.5):(2-4); and / or,

[0033] The molar ratio of molybdenum, organic small molecules and sulfur source in the molybdenum source is 1:(0.1-0.5):(2-4).

[0034] Furthermore, the organic small molecule has one of the following structural formulas:

[0035]

[0036] Where n is 1-12.

[0037] The doped metal source is a water-soluble salt of the doped metal. Specifically, the nickel source includes water-soluble nickel salts, including at least one of nickel sulfate, nickel nitrate, or nickel chloride. The iron source includes water-soluble iron salts, including ferrous and ferric salts; the ferrous salt includes at least one of ferrous chloride, ferrous sulfate, or ferrous nitrate; the ferric salt includes at least one of ferric chloride, ferric sulfate, or ferric nitrate. The cobalt source includes water-soluble cobalt salts, including at least one of cobalt chloride, cobalt sulfate, or cobalt nitrate. The platinum source includes soluble platinum sources, such as H₂PtCl₆·(H₂O)₆. The ruthenium source includes soluble ruthenium salts, such as RuCl₃·3H₂O.

[0038] It should be noted that before the hydrothermal reaction, water is needed to dissolve the various components. The amount of water added is a well-known amount in the art and can be obtained according to actual needs. This invention does not limit the amount of water added.

[0039] This invention provides an application of the above-mentioned molybdenum sulfide-based catalyst in the electrolysis of water to produce hydrogen.

[0040] The technical solution of this invention has the following advantages:

[0041] 1. This invention provides an organic small molecule for improving the hydrogen evolution performance of molybdenum sulfide-based catalysts. The terminal groups of this organic small molecule include cations and anions, respectively. The anions include at least one of carboxylate ions, sulfonate ions, and phosphate ions. The cations have a specific structural formula. This organic small molecule can improve the hydrogen evolution performance of existing molybdenum sulfide catalysts in water electrolysis, especially in alkaline water electrolysis, including but not limited to liquid alkaline water electrolysis (AWE), anion exchange membrane water electrolysis (AEMWE), and proton exchange water electrolysis (PEMWE). Modifying the surface of the molybdenum sulfide catalyst with the organic small molecule of this invention allows the molybdenum sulfide to form a 1T phase with better conductivity, reducing overpotential, increasing current density, and thus improving the hydrogen evolution performance of the catalyst. Furthermore, the organic small molecule provided by this invention significantly improves the hydrogen evolution performance of both 2H and 1T phase molybdenum sulfide catalysts. The anionic terminals of the organic small molecule mainly act as anchoring groups, coordinating with metal cations in the molybdenum sulfide-based catalyst, such as molybdenum ions, thereby fixing the small molecule to the surface of the molybdenum sulfide. The cation end is a functional end, which improves the hydrogen bond network of interfacial water, promotes water dissociation, and enhances the hydrogen evolution performance of the catalyst.

[0042] 2. The molybdenum sulfide-based catalyst provided by the present invention includes quaternary ammonium groups, which helps to form a 1T phase with better conductivity of molybdenum sulfide, resulting in a lower overpotential, higher current density, and better hydrogen evolution performance.

[0043] 3. The method for preparing molybdenum sulfide-based catalysts provided by this invention uses molybdenum source and small organic molecules as raw materials. During the preparation of molybdenum sulfide-based catalysts, this method helps to form a 1T phase with better conductivity, resulting in lower overpotential, higher current density, and better hydrogen evolution performance. The small organic molecules of this invention can improve the hydrogen evolution performance of any molybdenum sulfide catalyst, including molybdenum sulfide, doped molybdenum sulfide, and supported molybdenum sulfide catalysts.

[0044] 4. The preparation method of the molybdenum sulfide-based catalyst provided by this invention utilizes the synergistic effect of the doped metal and metallic molybdenum to further improve the hydrogen evolution performance of molybdenum sulfide. Thiourea and other sulfur-containing compounds primarily provide the sulfur source for the catalyst. Graphene, carbon nanotubes, and other supports have better conductivity, which can enhance the overall conductivity of the catalyst. Attached Figure Description

[0045] To more clearly illustrate the specific embodiments of the present invention or the technical solutions in the prior art, the drawings used in the description of the specific embodiments or the prior art will be briefly introduced below. Obviously, the drawings described below are some embodiments of the present invention. For those skilled in the art, other drawings can be obtained from these drawings without creative effort.

[0046] Figure 1This is a schematic diagram illustrating the hydrophilicity and hydrophobicity of the molybdenum sulfide catalysts in Example 1 and Control Group 1 of the present invention;

[0047] Figure 2 These are SEM images of the molybdenum sulfide catalysts in Example 1 and Control Group 1 of the present invention;

[0048] Figure 3 These are the XRD patterns of the molybdenum sulfide catalysts in Example 1 and Control Group 1 of this invention;

[0049] Figure 4 This is the energy dispersive X-ray spectrum of the molybdenum sulfide catalyst in Example 1 of the present invention;

[0050] Figure 5 These are the linear voltammetric scan (LSV) curves of the molybdenum sulfide catalysts in Example 1 and Control Group 1 of this invention;

[0051] Figure 6 These are the LSV curves of the molybdenum sulfide catalysts in Example 2 and Control Group 2 of this invention;

[0052] Figure 7 These are the LSV curves of the molybdenum sulfide catalysts in Example 3 and Control Group 3 of this invention;

[0053] Figure 8 These are the LSV curves of the molybdenum sulfide catalysts in Example 4 and Control Group 4 of this invention;

[0054] Figure 9 These are the LSV curves of the molybdenum sulfide catalysts in Example 5 and Control Group 5 of this invention;

[0055] Figure 10 These are the LSV curves of the molybdenum sulfide catalysts in Example 6 and Control Group 6 of this invention;

[0056] Figure 11 These are the LSV curves of the molybdenum sulfide catalysts in Example 7 and Comparative Example 1 of this invention. Detailed Implementation

[0057] The following embodiments are provided to better understand the present invention and are not limited to the preferred embodiments described. They do not constitute a limitation on the content and scope of protection of the present invention. Any product that is the same as or similar to the present invention, derived by any person under the guidance of the present invention or by combining the features of the present invention with other prior art, falls within the protection scope of the present invention.

[0058] For experiments not specifically described in the examples, the procedures or conditions should be followed according to the conventional experimental procedures described in the literature in this field. Reagents or instruments whose manufacturers are not specified are all commercially available conventional reagent products.

[0059] Example 1

[0060] This embodiment provides a method for preparing a molybdenum sulfide-based catalyst, including the following steps:

[0061] (NH4)2MoO4, nickel nitrate, organic small molecule A and thiourea were mixed in a molar ratio of 1:0.05:0.5:2.5 and water was added to prepare a mixture. The mixture was then subjected to hydrothermal reaction at 220℃ for 15 h to obtain Ni-MoS2 catalyst.

[0062] The preparation method of organic small molecule A includes: reacting trimethylamine and bromopropionic acid in isopropanol, stirring, heating to reflux at 90°C to form a precipitate, followed by filtration, washing, and drying to obtain organic small molecule A. The reaction process and the structural formula of organic small molecule A are as follows:

[0063]

[0064] Based on this embodiment, a molybdenum sulfide-based catalyst obtained without the addition of organic small molecules was used as control group 1.

[0065] Figure 1 This diagram illustrates the hydrophilicity / hydrophobicity of the molybdenum sulfide catalysts in Example 1 and Control Group 1, obtained using a contact angle meter. a represents the catalyst in Control Group 1, and b represents the catalyst in Example 1. As can be seen from the diagram, the catalyst in Control Group 1 is hydrophobic, while the catalyst in Example 1, modified with small organic molecules, is hydrophilic, significantly improving its hydrophilicity. This enhances the mass transfer efficiency between water and the catalyst during water electrolysis for hydrogen production, facilitates bubble detachment, and allows hydrogen to rapidly escape from the catalyst, thus increasing the contact between water and the catalyst and ultimately improving the efficiency of water electrolysis for hydrogen production.

[0066] Figure 2 These are SEM images of the molybdenum sulfide catalysts from Example 1 and Control Group 1. a) is the catalyst from Control Group 1, and b) is the catalyst from Example 1. Figure 2 It can be seen that the addition of small organic molecules causes MoS2 to change from the 2H phase to the 1T phase. The 1T phase MoS2 has better conductivity, which is beneficial to improving electron transport efficiency, reducing catalyst internal resistance, increasing current density, and thus improving the hydrogen evolution performance of water electrolysis.

[0067] Figure 3 These are the XRD patterns of the molybdenum sulfide catalysts in Example 1 and Control Group 1. As can be seen from the figures, the molybdenum sulfide changes from a 2H phase to a 1T phase after the introduction of small organic molecules. Specifically, Ni-MoS2-Z is the XRD pattern of the molybdenum sulfide catalyst in Example 1, and Ni-MoS2 is the XRD pattern of the molybdenum sulfide catalyst in Control Group 1.

[0068] Figure 4This is the energy-dispersive X-ray spectroscopy (EDSX) spectrum of the molybdenum sulfide catalyst from Example 1. The figure shows that the molybdenum sulfide-based catalyst synthesized in Example 1 contains elements such as Mo, Ni, S, N, and O, and these elements are uniformly distributed, indicating that the Ni dopant is uniformly dispersed in MoS2. The N and O are mainly derived from small organic molecules, proving that the small organic molecules were successfully modified on the surface of MoS2 and are uniformly distributed.

[0069] Example 2

[0070] This embodiment provides a method for preparing a molybdenum sulfide-based catalyst. The difference from Example 1 is that ferrous sulfate is used instead of nickel nitrate, and the molar amount of iron in ferrous sulfate is the same as the molar amount of nickel in nickel nitrate; organic small molecule B is used in equal molar amounts to replace organic small molecule A to obtain the Fe-MoS2 catalyst.

[0071] The synthesis method of organic small molecule B is the same as that of organic small molecule A in Example 1. The structural formula of organic small molecule B is as follows:

[0072]

[0073] Based on this embodiment, a molybdenum sulfide-based catalyst obtained without the addition of organic small molecules was used as control group 2.

[0074] Example 3

[0075] This embodiment provides a method for preparing a molybdenum sulfide-based catalyst. The difference from Example 1 is that cobalt sulfate is used instead of nickel nitrate, and organic small molecule C is used instead of organic small molecule A. (NH4)2MoO4, cobalt sulfate, organic small molecule C and thiourea are mixed in a molar ratio of 1:0.1:0.3:2.5 to obtain a Co-MoS2 catalyst.

[0076] The synthesis method of organic small molecule C is the same as that of organic small molecule A in Example 1. The structural formula of organic small molecule C is as follows:

[0077]

[0078] Based on this embodiment, a molybdenum sulfide-based catalyst obtained without the addition of organic small molecules was used as control group 3.

[0079] Example 4

[0080] This embodiment provides a method for preparing a molybdenum sulfide-based catalyst. The difference from Example 1 is that H2PtCl6·(H2O)6 is used instead of nickel nitrate, and organic small molecule D is used instead of organic small molecule A. (NH4)2MoO4, H2PtCl6·(H2O)6, organic small molecule D and thiourea are mixed in a molar ratio of 1:0.2:0.5:2 to obtain the Pt-MoS2 catalyst.

[0081] The synthesis method of organic small molecule D is the same as that of organic small molecule A in Example 1. The structural formula of organic small molecule D is as follows:

[0082]

[0083] Based on this embodiment, a molybdenum sulfide-based catalyst obtained without the addition of organic small molecules was used as control group 4.

[0084] Example 5

[0085] This embodiment provides a method for preparing a molybdenum sulfide-based catalyst. The difference from Example 1 is that Na2MoO4 is used instead of (NH4)2MoO4, RuCl3·3H2O is used instead of nickel nitrate, and organic small molecule E is used instead of organic small molecule A. Na2MoO4, RuCl3·3H2O, organic small molecule E and thiourea are mixed in a molar ratio of 1:0.05:0.5:4 to obtain the Ru-MoS2 catalyst.

[0086] The synthesis method of organic small molecule E is the same as that of organic small molecule A in Example 1. The structural formula of organic small molecule E is as follows:

[0087]

[0088] Based on this embodiment, a molybdenum sulfide-based catalyst obtained without the addition of organic small molecules was used as control group 5.

[0089] Example 6

[0090] This embodiment provides a method for preparing a molybdenum sulfide-based catalyst, including the following steps:

[0091] (NH4)2MoO4, organic small molecule A (same as in Example 1), and thiourea were mixed in a molar ratio of 1:0.5:2.5 and water was added to prepare a mixture. Carbon nanotubes were added to the mixture, with a mass ratio of carbon nanotubes to (NH4)2MoO4 of 1:6, and the mixture was ultrasonically dispersed evenly. Then, the mixture was hydrothermally reacted at 220°C for 15 h to obtain a carbon nanotube-supported MoS2-CNT-Z catalyst.

[0092] Based on this embodiment, a molybdenum sulfide-based catalyst obtained without the addition of organic small molecules was used as control group 6.

[0093] Example 7

[0094] This embodiment provides a method for preparing a molybdenum sulfide-based catalyst, which differs from Example 1 in that nickel nitrate is not added.

[0095] Comparative Example 1

[0096] This comparative example provides a method for preparing molybdenum sulfide, which differs from Example 7 in that: succinic acid and dimethylformamide in a molar ratio of 1:1 are used instead of organic small molecule A, and the total molar amount of succinic acid and dimethylformamide is the same as that of organic small molecule A.

[0097] Test case

[0098] This test case provides performance tests for the catalysts in each embodiment, control group, and comparative example, as detailed below:

[0099] A three-electrode testing method was employed, using 1M KOH as the electrolyte, a mercury / mercury oxide electrode as the reference electrode, and a graphite electrode as the counter electrode. The working electrode was based on nickel foam, with the catalyst to be tested sprayed onto the surface of the nickel foam at a catalyst loading of 2 mg / cm³. 2 .

[0100] Figure 5 These are the linear voltammetric scan (LSV) curves of molybdenum sulfide catalysts in Example 1 and Control Group 1; where Ni-MoS2-Z is Example 1 and Ni-MoS2 is Control Group 1. Figure 6 These are the LSV curves of the molybdenum sulfide catalysts in Example 2 and Control Group 2; where Fe-MoS2-Z is Example 2 and Fe-MoS2 is Control Group 2. Figure 7 These are the LSV curves of molybdenum sulfide catalysts in Example 3 and Control Group 3; where Co-MoS2-Z is Example 3 and Co-MoS2 is Control Group 3. Figure 8 These are the LSV curves of molybdenum sulfide catalysts in Example 4 and Control Group 4; where Pt-MoS2-Z is Example 4 and Pt-MoS2 is Control Group 4. Figure 9 These are the LSV curves of molybdenum sulfide catalysts in Example 5 and Control Group 5; where Ru-MoS2-Z is Example 5 and Ru-MoS2 is Control Group 5. Figure 10 These are the LSV curves of the molybdenum sulfide catalysts in Example 6 and Control Group 6; where MoS2-CNT-Z is Example 6 and MoS2-CNT is Control Group 6. Figure 11 These are the LSV curves of the molybdenum sulfide catalysts in Example 7 and Comparative Example 1; where MoS2-Z is Example 7 and MoS2-B is Comparative Example 1.

[0101] from Figure 5-9It can be seen that, compared with the control group, the surface modification of the molybdenum sulfide-based catalyst of the present invention with organic small molecules results in a lower overpotential, higher current density, and increased gas production, indicating better hydrogen evolution performance of the catalyst. Example 6 illustrates that adding a support, such as carbon nanotubes, to the molybdenum sulfide catalyst can still improve the hydrogen evolution performance of the supported catalyst. Examples 7 and Comparative Example 1 show that the improvement in hydrogen evolution performance of molybdenum sulfide catalysts by modification with organic small molecules is not only due to the phase transition and hydrophilicity / hydrophobicity of MoS2, but also because the quaternary ammonium cations in the organic small molecules are key to improving the hydrogen evolution performance of the molybdenum sulfide catalyst surface. The addition of succinic acid and dimethylformamide in Comparative Example 1 further verifies this conclusion. In summary, the various examples, the control group, and Comparative Example 1 show that the improvement in hydrogen evolution performance of molybdenum sulfide-based catalysts with quaternary ammonium cations is universal, including pure molybdenum sulfide, doped molybdenum sulfide, and supported molybdenum sulfide catalysts.

[0102] Obviously, the above embodiments are merely illustrative examples for clear explanation and are not intended to limit the implementation. Those skilled in the art will recognize that other variations or modifications can be made based on the above description. It is neither necessary nor possible to exhaustively list all possible implementations here. However, obvious variations or modifications derived therefrom are still within the scope of protection of this invention.

Claims

1. The application of an organic small molecule in a molybdenum sulfide-based catalyst, characterized in that, The terminal groups at both ends of the organic small molecule include cations and anions, respectively; the anions include at least one of carboxylate ions, sulfonate ions, and phosphate ions; the cations have at least one of the following structural formulas: 。 2. The application according to claim 1, characterized in that, The organic small molecule has one of the following structural formulas: Where n is 1-12.

3. The application according to claim 2, characterized in that, The value of n is 1-5.

4. The application according to claim 2, characterized in that, The organic small molecule has one of the following structural formulas: 、 、 、 、 。 5. A molybdenum sulfide-based catalyst, characterized in that, The molybdenum sulfide-based catalyst comprises molybdenum sulfide, which includes a 1T phase; the molybdenum sulfide-based catalyst includes quaternary ammonium groups, and further includes at least one of carboxyl groups, sulfonic acid groups, and phosphate groups.

6. The molybdenum sulfide-based catalyst according to claim 5, characterized in that, The molybdenum sulfide-based catalyst comprises a doped metal, which includes transition metals and / or noble metals; and / or, The molybdenum sulfide-based catalyst also includes a support.

7. The molybdenum sulfide-based catalyst according to claim 6, characterized in that, The doped metal includes at least one of nickel, iron, cobalt, platinum, and ruthenium; and / or, The carrier includes carbon nanotubes, graphene, or carbon fibers.

8. A method for preparing a molybdenum sulfide-based catalyst, characterized in that, The reaction involves a molybdenum source and a mixture of small organic molecules followed by a hydrothermal reaction. The small organic molecules have terminal groups comprising cations and anions, respectively. The anions include at least one of carboxylate ions, sulfonate ions, and phosphate ions. The cations have at least one of the following structural formulas: 、 、 。 9. The preparation method according to claim 8, characterized in that, The mixing process also includes the addition of a sulfur source and / or a doped metal source; and / or, The mixing process also includes the addition of a carrier, which comprises carbon nanotubes, graphene, or carbon fibers; and / or, The hydrothermal reaction is carried out at a temperature of 170-220℃ for a duration of 6-20 hours; and / or, The organic small molecule has one of the following structural formulas: Where n is 1-12.

10. The preparation method according to claim 9, characterized in that, The mass ratio of the carrier to the molybdenum source is 1:(6-10).

11. The preparation method according to any one of claims 8-10, characterized in that, The molybdenum source includes molybdate and / or dimolybdate; and / or, The sulfur source includes sulfur-containing compounds; and / or, The metal in the doped metal source includes at least one of nickel, iron, cobalt, platinum, and ruthenium; and / or, The doped metal source is a water-soluble salt of a doped metal; and / or, The molar ratio of molybdenum in the molybdenum source, the doped metal in the doped metal source, the organic small molecule, and the sulfur source is 1:(0.05-0.2):(0.1-0.5):(2-4); and / or, The molar ratio of molybdenum, organic small molecules and sulfur source in the molybdenum source is 1:(0.1-0.5):(2-4).

12. The preparation method according to claim 11, characterized in that, The dimolybdate comprises (NH4)6Mo7O 24 The molybdate comprises at least one of (NH4)2MoO4, Na2MoO4, and K2MoO4; and / or, The sulfur-containing compound includes at least one of thiourea, thioether, and thioacetamide.

13. The application of the molybdenum sulfide-based catalyst according to any one of claims 5-7 or the molybdenum sulfide-based catalyst prepared by any one of claims 8-12 in the electrolysis of water to produce hydrogen.

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