Defect carbon material loaded molybdenum disulfide-based composite material x-ctab-y and preparation and application thereof

Abstract

The application discloses a kind of defect carbon material load molybdenum disulfide-based composite X-CTAB-Y and its preparation and application.Molybdenum disulfide-based electrocatalyst of the application is composite system comprising the following components: a carbon material and molybdenum disulfide-based composite material;The carbon material is defect carbon material, preferably graphene oxide GO, becomes reduced graphene oxide rGO in the process of compounding;The molybdenum disulfide-based composite material is molybdenum disulfide and nickel monatomic, molybdenum trioxide, sulfur-deficient molybdenum sulfide composite.The graphene load molybdenum disulfide-based electrocatalyst of the application has multiple effects such as high hydrogen evolution performance, high cycle stability and strong corrosion resistance, which can effectively improve the hydrogen evolution performance and cycle stability of electrocatalyst in acidic medium.

Description

Technical Field

[0001] This invention relates to the field of hydrogen energy technology, and in particular to a defective carbon material supported molybdenum disulfide-based composite material X-CTAB-Y and its preparation and application. Background Technology

[0002] With economic development and ever-increasing energy demand, the environmental problems caused by human use of fossil fuels are becoming increasingly serious. However, with the over-exploitation and use of fossil fuels, a series of difficulties and challenges have arisen, including limited crustal reserves, the depletion of surface fossil fuels leading to restrictions and cost constraints on deep-sea extraction. More importantly, the large-scale use of fossil fuels has caused extremely negative environmental problems and impacts on daily human production and life. Harmful gases produced during the use of fossil fuels, such as CO2 and NO... x and SO x However, this will cause irreversible damage to the environment in the long run. Promoting sustainable energy development has become an inevitable trend. my country is committed to energy conservation, emission reduction, and energy structure transformation, but it needs to solve the problems of renewable energy storage and sustainable utilization. Hydrogen energy, as an ideal high-energy-density (142.35 kJ / kg) energy source, offers a solution. -1 Hydrogen energy is a secondary energy source, with water as its only combustion product, unlike fossil fuels which produce byproducts, making it one of the best clean energy sources. Besides its high energy density, hydrogen energy also has the following advantages: abundant raw materials for hydrogen production, as it can be directly produced from water; and convenient storage and transportation, as it can be stored in high-pressure tanks in gaseous or liquid form, or in solid hydrogen storage materials. Therefore, hydrogen energy has immeasurable application prospects in solving the environmental pollution problems and energy shortage crisis caused by fossil fuels. Currently, hydrogen production is still in its early stages, mainly through chemical methods such as water-gas reforming, which generates pollutants and fails to meet the requirements of clean production. Electrolysis of water, as a method for producing high-purity hydrogen, does not produce greenhouse gases during the process, and the purity of the produced hydrogen can reach over 99.7%, sufficient to meet the requirements of actual production. However, large-scale application of water electrolysis is currently not feasible due to the large overpotential compared to the theoretical water decomposition voltage of 1.23V, resulting in high costs and limited promotion.

[0003] Highly efficient electrocatalysts are required for hydrogen production through water electrolysis. These electrocatalysts should possess low overpotentials to achieve efficient electrochemical reactions. Currently, electrocatalysts mainly include noble metal-based electrocatalysts, transition metal-based electrocatalysts, and non-metal-based electrocatalysts. Among them, platinum-based catalysts are commercially used due to their high efficiency and stability. However, their extremely scarce abundance in the Earth's crust makes them prohibitively expensive. Therefore, it is necessary to replace the structure of non-noble metal catalysts. Developing efficient, stable, and scalable low-cost electrocatalysts is key to realizing the "hydrogen economy" blueprint. Rational design of transition metal-based electrocatalysts can solve the critical problems of high prices and limited precious metal resources in current electrocatalysts. However, in acidic media, transition metal-based electrocatalysts suffer from easy corrosion and short lifespan. Therefore, it is necessary to construct acid-resistant carbon support composite materials to increase the corrosion resistance and long lifespan of these electrocatalysts. Summary of the Invention

[0004] To address the above technical problems, this invention provides a defective carbon material-supported molybdenum disulfide-based composite material X-CTAB-Y, its preparation and application.

[0005] The first objective of this invention is to provide a defective carbon material-supported molybdenum disulfide-based composite material X-CTAB-Y, wherein the defective carbon material is used as a carrier, and the molybdenum disulfide-based composite material is loaded on the surface of the carrier and in the defects, wherein X is the defective carbon material and Y is the molybdenum disulfide-based composite material.

[0006] In this invention, the defective carbon material supported molybdenum disulfide-based composite material X-CTAB-Y includes defective carbon material supported molybdenum disulfide X-CTAB-MoS2, the molybdenum disulfide-based composite material Ni SA / X-CTAB-MoS2 supported with nickel single atoms, the carbon material supported molybdenum disulfide-based composite material X-CTAB-MoS2-MoO3, the carbon material supported molybdenum disulfide-based composite material Ni SA / X-CTAB-MoS2-MoO3, and the carbon material supported molybdenum disulfide-based composite material X-CTAB-MoS2-SD.

[0007] In some embodiments of the present invention, the defective carbon material includes one or more of reduced graphene oxide, nitrogen carbide (C3N4), and carbon nanotubes.

[0008] In some embodiments of the present invention, the molybdenum disulfide-based composite material includes one or more of the following: a molybdenum disulfide-nickel single-atom composite, a molybdenum disulfide-molybdenum trioxide heterojunction, and a molybdenum disulfide-sulfur-defect molybdenum disulfide heterojunction.

[0009] A second objective of this invention is to provide a method for preparing the aforementioned defective carbon material-supported molybdenum disulfide-based composite material X-CTAB-Y, comprising the following steps:

[0010] X-CTAB-S was obtained by mixing defective carbon materials, CTAB, and a sulfur source.

[0011] X-CTAB-MoS2 is obtained by reacting it with a molybdenum source via a hydrothermal method. The obtained X-CTAB-MoS2 is then loaded with single-atom nickel and / or oxidized to form a heterojunction, and / or sulfur vacancies are formed in situ through high-temperature heat treatment to prepare the defective carbon material-supported molybdenum disulfide-based composite material X-CTAB-Y.

[0012] In some embodiments of the present invention, the mass ratio of the defective carbon material, CTAB, and sulfur source is (20:1:80)-(40:1:60);

[0013] The defective carbon materials include one or more of reduced graphene oxide, nitrogen carbide (C3N4), and carbon nanotubes.

[0014] The conditions for the hydrothermal method are: 150-300℃ and 24-48h;

[0015] The molybdenum source is selected from one or more of Na2MoO4·2H2O, K2MoO4, CaMoO4, FeMoO4, (NH4)2MoO4, and MgMoO4;

[0016] The sulfur source is selected from one or more of sublimed sulfur, sodium sulfide, and cysteine.

[0017] In some embodiments of the present invention, the steps for preparing NiSA / X-CTAB-MoS2 by loading single-atom nickel are as follows:

[0018] X-CTAB-S was obtained by mixing defective carbon materials, CTAB, and a sulfur source.

[0019] The defective carbon material-supported molybdenum disulfide composite material X-CTAB-MoS2 was then prepared by reacting it with a molybdenum source via a hydrothermal method.

[0020] The defective carbon material loaded with molybdenum disulfide composite material was mixed with a nickel source and stirred under ultraviolet light to obtain the molybdenum disulfide-based composite material NiSA / X-CTAB-MoS2 loaded with nickel single atoms.

[0021] In some embodiments of the present invention, the mass ratio of X-CTAB-MoS2 to the nickel source is (1:0.05)-(1:0.2);

[0022] The conditions for the hydrothermal method are: 150-300℃ and 24-48h;

[0023] The nickel source is selected from one or more of Ni(NO3)2, nickel chloride, and nickel sulfate;

[0024] The sulfur source is selected from one or more of sublimed sulfur, sodium sulfide, and cysteine;

[0025] The stirring reaction takes 4-8 hours.

[0026] In some embodiments of the present invention, the step of X-CTAB-MoS2 oxidation to form heterojunction X-CTAB-MoS2-MoO3 is as follows:

[0027] X-CTAB-S was obtained by mixing defective carbon materials, CTAB, and a sulfur source.

[0028] The carbon-supported molybdenum disulfide-based composite material X-CTAB-MoS2 was then prepared by reacting it with a molybdenum source via a hydrothermal method.

[0029] X-CTAB-MoS2 was stirred and mixed with an oxidant, and then dried to obtain X-CTAB-MoS2-MoO3.

[0030] In this invention, the defective carbon material-supported molybdenum disulfide-based composite material X-CTAB-MoS2-MoO3 is oxidized on the surface of the carbon material-supported molybdenum disulfide composite material to form MoO3, wherein X is the defective carbon material.

[0031] The stirring and mixing reaction time is 12-24 hours.

[0032] In some embodiments of the present invention, the oxidant is selected from one or more of H2O2, KMnO4, NaClO3, and NaClO4;

[0033] The molybdenum source is selected from one or more of Na2MoO4·2H2O, K2MoO4, CaMoO4, FeMoO4, (NH4)2MoO4, and MgMoO4;

[0034] The sulfur source is selected from one or more of sublimed sulfur, sodium sulfide, and cysteine.

[0035] In some embodiments of the present invention, the steps of loading single-atom nickel on X-CTAB-MoS2 and oxidizing it to form a heterojunction Ni SA / X-CTAB-MoS2-MoO3 are as follows: X-CTAB-MoS2 is stirred and mixed with an oxidant and dried to obtain X-CTAB-MoS2-MoO3; the X-CTAB-MoS2-MoO3 is mixed with a nickel source and stirred and reacted under ultraviolet light irradiation to obtain the Ni SA / X-CTAB-MoS2-MoO3.

[0036] In this invention, Ni SA / X-CTAB-MoS2-MoO3 uses X-CTAB-MoS2-MoO3 as a support, with nickel single atoms loaded on the surface of the support.

[0037] In some embodiments of the present invention, the step of forming X-CTAB-MoS2-SD by in-situ sulfur vacancies through high-temperature heat treatment is as follows: X-CTAB-MoS2 is mixed and ground with a molten salt mixture, and then calcined at high temperature in an inert gas atmosphere to obtain X-CTAB-MoS2-SD.

[0038] In this invention, a defective carbon material supported molybdenum disulfide-based composite material X-CTAB-MoS2-SD is provided, wherein sulfur vacancies are formed in situ on the surface of X-CTAB-MoS2 by high-temperature heating. In X-CTAB-MoS2-SD, SD represents sulfur-defective molybdenum disulfide (MoS2). z The sulfur-defect molybdenum sulfide MoS₂ z 1 <Z<2。

[0039] In some embodiments of the present invention, the mass ratio of X-CTAB-MoS2 to the molten salt mixture is (1:2)-(2:1);

[0040] The high-temperature calcination temperature is 400-800℃, and the high-temperature calcination time is 2-6 hours;

[0041] The inert atmosphere contains inactive gases including argon and / or nitrogen.

[0042] The molten salt mixture is selected from two or more of KCl, LiCl, and NaCl.

[0043] A third objective of this invention is to provide the application of the aforementioned defective carbon material-supported molybdenum disulfide-based composite material X-CTAB-Y in the electrocatalytic hydrogen evolution under acidic conditions.

[0044] In some embodiments of the present invention, the acidic pH range is 0-5.

[0045] A fourth objective of this invention is to provide the application of the aforementioned defective carbon material-supported molybdenum disulfide-based composite material X-CTAB-Y in hydrogen electrolyzers and fuel cells.

[0046] The technical solution of the present invention has the following advantages over the prior art:

[0047] 1. The basic raw materials are cheap and readily available, the process is simple and efficient, and it is easy to scale up the production.

[0048] 2. The defective carbon material (such as reduced graphene oxide) supported on molybdenum disulfide-based composite material of the present invention has a large number of active sites. The defective carbon material (such as reduced graphene oxide) supported on molybdenum disulfide-based composite material of the present invention has a low overpotential, good cycle performance, and corrosion resistance in acidic media.

[0049] 3. The composite material obtained in this invention exhibits excellent electrocatalytic performance due to the synergistic effect of defective carbon materials (such as reduced graphene oxide rGO) with Ni single atoms, molybdenum disulfide, molybdenum trioxide, and sulfur-defective molybdenum sulfide. The 1T phase MoS2 better anchors Ni single atoms on the composite material and provides a larger specific surface area. Attached Figure Description

[0050] To make the content of this invention easier to understand, the invention will be further described in detail below with reference to specific embodiments and accompanying drawings, wherein...

[0051] Figure 1 This is a TEM image of the Ni SA / rGO-CTAB-MoS2 composite material prepared in Example 1 of the present invention;

[0052] Figure 2 The aberration diagram of the Ni SA / rGO-CTAB-MoS2 composite material prepared in Example 1 of this invention;

[0053] Figure 3 The three-dimensional reconstruction and mapping diagram of the Ni SA / rGO-CTAB-MoS2 composite material prepared in Example 1 of this invention;

[0054] Figure 4 The graph shows the HER performance of the Ni SA / rGO-CTAB-MoS2 composite material prepared in Example 1 of this invention in acidic medium.

[0055] Figure 5 The image shows the XRD pattern of the rGO-CTAB-MoS2-MoO3 composite material prepared in Example 5 of this invention.

[0056] Figure 6 This is a SEM image of the rGO-CTAB-MoS2-MoO3 composite material prepared in Example 5 of the present invention;

[0057] Figure 7 The graph shows the HER performance of the Ni SA / rGO-CTAB-MoS2-MoO3 composite material prepared in Example 5 of this invention in an acidic medium.

[0058] Figure 8 This is a SEM image of the SD-rGO-CTAB-MoS2-MoO3 composite material prepared in Example 7 of the present invention;

[0059] Figure 9 The image shows the XRD pattern of the SD-rGO-CTAB-MoS2-MoO3 composite material prepared in Example 7 of this invention.

[0060] Figure 10 The image shows the HER performance of the SD-rGO-CTAB-MoS2-MoO3 composite material prepared in Example 7 of this invention in an acidic medium.

[0061] Figure 11 The images show the XRD patterns of the rGO-CTAB-MoS2 and NiSA / rGO-CTAB-MoS2 composite materials prepared in Example 1 of this invention. Detailed Implementation

[0062] The present invention will be further described below with reference to the accompanying drawings and specific embodiments, so that those skilled in the art can better understand and implement the present invention. However, the embodiments described are not intended to limit the present invention.

[0063] Example 1

[0064] This embodiment provides a method for preparing a reduced graphene oxide-supported molybdenum disulfide-based composite electrocatalyst NiSA / rGO-CTAB-MoS2, as detailed below:

[0065] I. Preparation of rGO-CTAB-MoS2:

[0066] Step (1): Take 70 mL of 1 mg / mL graphene oxide suspension (GO) and 66 mg of CTAB powder and stir for 2 hours.

[0067] Step (II): Stir 787.5 mg of Na2S·9H2O with 315 mg of sublimed sulfur for 2 hours, and set aside for later use;

[0068] Step (3): Mix the solutions from Step (1) and Step (2) and stir overnight. Then add HCOOH dropwise to this mixture and stir for 2 hours. Filter with acetone and water to obtain rGO-CTAB-S for later use.

[0069] Step (IV): Take 100 mg of the rGO-CTAB-S powder obtained in Step (III), add 302 mg of molybdenum source Na2MoO4·2H2O and 70 mL of deionized water, and carry out a hydrothermal reaction at 200℃ for 24 h. The resulting solution is filtered and dried to obtain rGO-CTAB-MoS2. The structure of the obtained material is characterized as follows: Figure 11 .

[0070] II. Preparation of Ni SA / rGO-CTAB-MoS2: The above-obtained rGO-CTAB-MoS2 was dispersed in deionized water to form a mixed solution, and then mixed with Ni(NO3)2·6H2O at a mass ratio of 1:0.05 and stirred for 4 hours. Then, it was stirred under ultraviolet light for 4 hours, filtered with ethanol and deionized water, and dried overnight in an oven at 60°C to obtain Ni SA / rGO-CTAB-MoS2.

[0071] Structural characterization:

[0072] The structures of the rGO-CTAB-MoS2 and NiSA / rGO-CTAB-MoS2 prepared above were characterized, and the experimental results are shown in the figure. Figures 1-3 and Figure 11 Through XRD ( Figure 11 ), TEM Figure 1 ), Spherical Aberration Diagram ( Figure 2 ), 3D reconstruction and mapping diagram ( Figure 3 This proves that Ni single atoms were successfully loaded onto rGO-CTAB-MoS2, indicating that Ni SA / rGO-CTAB-MoS2 was successfully prepared.

[0073] Performance testing:

[0074] The electrocatalytic performance of the NiSA / rGO-CTAB-MoS2, rGO-CTAB-MoS2, and control group pristineMoS2 and 20wt% Pt / C prepared above was tested in 0.5M H2SO4 medium, as detailed below:

[0075] Step 1: Take 5 mg of rGO-CTAB-MoS2, NiSA / rGO-CTAB-MoS2 and control group pristineMoS2, 20 wt% Pt / C and 2 mL of isopropanol, 460 μL of deionized water and 20 μL of Nafion, and mix them evenly by sonication to prepare a 2 mg / mL ink solution for later use.

[0076] Step 2: Drop-coat this ink onto a glassy carbon electrode and characterize its electrochemical performance in an acidic medium of 0.5 M H₂SO₄. The experimental results are shown below. Figure 4 ,Depend on Figure 4 It can be seen that NiSA / rGO-CTAB-MoS2 exhibits a lower overpotential and stronger hydrogen evolution performance than rGO-CTAB-MoS2 and MoS2.

[0077] Example 2

[0078] Similar to Example 1, the difference lies in the conditions of the hydrothermal method in step one: 200°C and 30 hours.

[0079] Example 3

[0080] Similar to Example 1, except that in step one, the graphene oxide suspension GO is replaced with nitrogen carbide C3N4.

[0081] Example 4

[0082] Similar to Example 1, the difference is that in step two, the mass ratio of rGO-CTAB-MoS2 to the nickel source is (1:0.2).

[0083] Example 5

[0084] Similar to Example 1, the difference is that in step one, the molybdenum source is replaced with K2MoO4.

[0085] Example 6

[0086] This embodiment provides a method for preparing a reduced graphene oxide-supported molybdenum disulfide-based electrocatalyst NiSA / rGO-CTAB-MoS2-MoO3, as detailed below:

[0087] 1. Disperse the rGO-CTAB-MoS2 obtained in Example 1 in deionized water to form a solution, stir with 2.5wt% H2O2 for 12h, filter the resulting mixed solution with ethanol and deionized water, place it in a vacuum drying oven, and dry it overnight at 60°C to obtain rGO-CTAB-MoS2-MoO3.

[0088] Structural characterization:

[0089] The obtained rGO-CTAB-MoS2-MoO3 was characterized by XRD and SEM, and the results are shown in the figure. Figure 5 and Figure 6 ,Depend on Figure 5 It can be seen that the heterostructure composite material rGO-CTAB-MoS2-MoO3 has the coexistence of MoO3 and MoS2, which is due to... Figure 6 It can be seen that the composite material rGO-CTAB-MoS2-MoO3 was successfully constructed.

[0090] 2. The obtained rGO-CTAB-MoS2-MoO3 and Ni(NO3)2·6H2O were mixed at a mass ratio of 1:0.05 and stirred for 4 hours; then stirred for 4 hours under ultraviolet light irradiation, filtered with ethanol and deionized water, and dried overnight in an oven at 60°C to obtain Ni SA / rGO-CTAB-MoS2-MoO3.

[0091] Structural characterization:

[0092] The obtained NiSA / rGO-CTAB-MoS2-MoO3 was structurally characterized by XRD. Figure 5 SEM and mapping Figure 6 Characterized by ) Figure 5 , 6 It can be concluded that the material was successfully prepared.

[0093] Performance testing:

[0094] The electrocatalytic performance of the obtained NiSA / rGO-CTAB-MoS2-MoO3, rGO-CTAB-MoS2-MoO3, and control groups rGO, pristine MoS2, 20wt% Pt / C, and rGO-CTAB-MoS2 was tested in 0.5M H2SO4 medium, as detailed below:

[0095] Step 1: Take 5 mg of Ni SA / rGO-CTAB-MoS2-MoO3, rGO-CTAB-MoS2-MoO3, and control group pristine MoS2, 20 wt% Pt / C, 2 mL of isopropanol, 460 μL of deionized water, and 20 μL of Nafion, and mix them evenly by sonication to prepare a 2 mg / mL ink solution for later use.

[0096] Step 2: Drop-coat this ink onto a glassy carbon electrode, and characterize its electrochemical performance in an acidic medium of 0.5 M H₂SO₄. The results are shown in [Figure 2]. Figure 7 The successfully constructed heterostructure rGO-CTAB-MoS2-MoO3 exhibits superior performance compared to pristine MoS2 and rGO-CTAB-MoS2. Further loading a single atom of Ni onto the heterostructure results in the composite material rGO-CTAB-MoS2-MoO3, which demonstrates even better performance, stable cycling in acidic media, and efficient long-term hydrogen evolution.

[0097] Example 7

[0098] Similar to Example 6, the difference is that in step two, the nickel source is replaced with nickel sulfate.

[0099] Example 8

[0100] This invention provides a method for preparing rGO-CTAB-MoS2-SD, as detailed below:

[0101] 1.50 g of rGO-CTAB-MoS2 obtained in Example 1 was ground using the molten salt method with 1.35 g of KCl and 1.15 g of LiCl. After thorough grinding, the mixture was placed in a tube furnace and calcined at 500 °C for 4 h in an Ar atmosphere. The mixture was then filtered with deionized water and dried overnight in a drying oven at 60 °C to obtain rGO-CTAB-MoS2-SD with sulfur vacancies. SD is molybdenum sulfide with sulfur defects (MoS2). <Z<2)。

[0102] Structural characterization:

[0103] The obtained rGO-CTAB-MoS2-SD was structurally characterized using SEM and mapping. Figure 8 ), XRD Figure 9 Characterized by ) Figure 8 , 9 It can be seen that sulfur vacancies were successfully prepared in the material.

[0104] Performance testing:

[0105] The electrocatalytic performance of the obtained rGO-CTAB-MoS2-SD, rGO-CTAB-MoS2, and control group MoS2 and Pt / C was tested in 0.5M H2SO4 medium, as detailed below:

[0106] Step 1: Take 5 mg of rGO-CTAB-MoS2-SD, rGO-CTAB-MoS2, control group MoS2, Pt / C, 2 mL of isopropanol, 460 μL of deionized water, and 20 μL of Nafion, and mix them evenly by sonication to prepare a 2 mg / mL ink solution for later use.

[0107] Step 2: The ink was drop-coated onto a glassy carbon electrode, and its electrochemical performance was characterized in an acidic medium of 0.5 M H₂SO₄. Experimental results are shown below. Figure 10 The composite material SD-rGO-CTAB-MoS2 with sulfur vacancies exhibits low overpotential, small Tafel slope, and large electrochemical surface area in acidic media, and can stably and efficiently evolve hydrogen.

[0108] 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. A defective carbon material-supported molybdenum disulfide-based composite material X-CTAB-Y, characterized in that, Using a defective carbon material as a carrier, a molybdenum disulfide-based composite material is loaded onto the surface of the carrier and into the defects, where X is the defective carbon material and Y is the molybdenum disulfide-based composite material; The defective carbon materials include one or more of reduced graphene oxide, nitrogen carbide (C3N4), and carbon nanotubes. The molybdenum disulfide-based composite material includes one or more of the following: molybdenum disulfide and nickel single-atom complex, molybdenum disulfide and molybdenum trioxide heterojunction, and molybdenum disulfide and sulfur-defect molybdenum disulfide heterojunction. The preparation method of the defective carbon material-supported molybdenum disulfide-based composite material X-CTAB-Y includes the following steps: Step (1): Take a suspension of graphene oxide, nitrogen carbide (C3N4) or carbon nanotubes and stir it with CTAB powder; Step (II): The Na2S·9H2O solution is stirred with sublimed sulfur; where both Na2S·9H2O and sublimed sulfur are sulfur sources. Step (3): Mix the mixtures from Step (1) and Step (2) and stir overnight; then add HCOOH dropwise to the mixture and stir; then filter with acetone and water to obtain X-CTAB-S for later use. Step (iv): X-CTAB-S is reacted with a molybdenum source via a hydrothermal method to obtain X-CTAB-MoS2. The obtained X-CTAB-MoS2 is loaded with single-atom nickel and / or oxidized to form a heterojunction, and / or sulfur vacancies are formed in situ through high-temperature heat treatment to prepare the defective carbon material-supported molybdenum disulfide-based composite material X-CTAB-Y.

2. The X-CTAB-Y composite material supported on defective carbon materials according to claim 1, characterized in that, The mass ratio of the graphene oxide, nitrogen carbide C3N4 or carbon nanotubes, CTAB and sulfur source is (20:1:80)-(40:1:60); The conditions for the hydrothermal method are: 150-300℃ and 24-48h; The molybdenum source is selected from one or more of Na2MoO4·2H2O, K2MoO4, CaMoO4, FeMoO4, (NH4)2MoO4, and MgMoO4.

3. The X-CTAB-Y composite material supported on defective carbon materials according to claim 1, characterized in that, The steps for preparing NiSA / X-CTAB-MoS2 by loading single-atom nickel are as follows: X-CTAB-MoS2 is mixed with a nickel source and stirred under ultraviolet light to obtain a molybdenum disulfide-based composite material loaded with single nickel atoms. The mass ratio of X-CTAB-MoS2 to the nickel source is (1:0.05)-(1:0.2); The nickel source is selected from one or more of Ni(NO3)2, nickel chloride, and nickel sulfate; The stirring reaction takes 4 to 8 hours.

4. The X-CTAB-Y composite material supported on defective carbon materials according to claim 1, characterized in that, The steps for forming heterojunction X-CTAB-MoS2-MoO3 by oxidation of X-CTAB-MoS2 are as follows: X-CTAB-MoS2 is stirred and mixed with an oxidant and then dried to obtain X-CTAB-MoS2-MoO3. The oxidant is selected from one or more of H2O2, KMnO4, NaClO3, and NaClO4; The stirring and mixing reaction time is 12 to 24 hours.

5. The X-CTAB-Y composite material supported on defective carbon materials according to claim 1, characterized in that, The steps for forming a heterojunction Ni SA / X-CTAB-MoS2-MoO3 by loading single-atom nickel with X-CTAB-MoS2 and oxidizing it are as follows: X-CTAB-MoS2 is stirred and mixed with an oxidant and dried to obtain X-CTAB-MoS2-MoO3. The X-CTAB-MoS2-MoO3 is then mixed with a nickel source and stirred under ultraviolet light irradiation to obtain the Ni SA / X-CTAB-MoS2-MoO3. The oxidant is selected from one or more of H2O2, KMnO4, NaClO3, and NaClO4; The stirring and mixing reaction takes 12–24 hours; The stirring reaction takes 4 to 8 hours.

6. The X-CTAB-Y composite material supported on defective carbon materials according to claim 1, characterized in that, The steps for forming X-CTAB-MoS2-SD by in-situ sulfur vacancies through high-temperature heat treatment are as follows: X-CTAB-MoS2 is mixed and ground with a molten salt mixture, and then calcined at high temperature in an inert gas atmosphere to obtain X-CTAB-MoS2-SD. The mass ratio of X-CTAB-MoS2 to the molten salt mixture is (1:2)-(2:1); The high-temperature calcination temperature is 400-800℃, and the high-temperature calcination time is 2-6 hours; The inert gas atmosphere includes argon and / or nitrogen. The molten salt mixture is selected from two or more of KCl, LiCl, and NaCl; In the X-CTAB-MoS2-SD, SD represents sulfur-defective molybdenum sulfide (MoS2). z The sulfur-defect molybdenum sulfide MoS₂ z 1 <Z<2。 7. The application of the defective carbon material supported molybdenum disulfide-based composite material X-CTAB-Y as described in any one of claims 1 to 6 in the electrocatalytic hydrogen evolution under acidic conditions.

8. The application of the defective carbon material supported molybdenum disulfide-based composite material X-CTAB-Y as described in any one of claims 1 to 6 in a hydrogen electrolyzer or fuel cell.

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