Carbon felt electrode loaded with copper sulfide / graphdiyne composite catalyst as well as preparation method and application of carbon felt electrode

Abstract

The embodiment of the invention discloses a carbon felt electrode loaded with a copper sulfide / graphdiyne composite catalyst as well as a preparation method and application of the carbon felt electrode. The method comprises the following steps: preparing an electroplating solution containing copper sulfate, sodium citrate, sodium tartrate and lauryl sodium sulfate: electroplating in the electroplating solution by taking a pre-oxidized carbon felt as a cathode and a copper sheet as an anode; washing with deionized water to be neutral, and drying to obtain a copper modified carbon felt material; preparing a diethyl ether solution containing a hexaacetylene benzene monomer, and then adding pyridine; soaking the modified carbon felt material in the diethyl ether solution, washing and drying to obtain a copper modified carbon felt material on which graphdiyne grows; preparing a thiourea-containing ethylene glycol solution, soaking the copper modified carbon felt material on which graphdiyne grows in the ethylene glycol solution, and carrying out heat preservation at a preset temperature for a preset time; and washing and drying to obtain the required carbon felt electrode. The limitation of a traditional carbon felt electrode in the aspects of catalytic activity, conductivity and stability is effectively overcome, and the comprehensive performance of the electrode is improved.

Description

Technical Field

[0001] The embodiments of the present disclosure belong to the field of electrochemical technology, and specifically relate to a carbon felt electrode loaded with a copper sulfide / graphene composite catalyst, and a preparation method and application thereof. Background Art

[0002] In recent years, with growing global awareness of sustainable energy and environmental protection, electrocatalytic technology has played an increasingly important role in energy conversion and storage systems, such as fuel cells, water electrolysis to hydrogen production, and carbon dioxide reduction. The core of these technologies lies in efficient and stable electrode materials, which are directly related to energy conversion efficiency and the economic feasibility of the system.

[0003] Carbon materials, particularly carbon nanotubes, graphene, and carbon felt, have become widely used foundational materials in electrocatalysis due to their high surface area, excellent conductivity, and chemical stability. Carbon felt, due to its three-dimensional porous structure and ease of functional modification, has been extensively studied as a basic support for electrode materials, used to load various catalysts to improve electrochemical reaction efficiency.

[0004] However, existing carbon felt electrodes have the following disadvantages:

[0005] Conductive performance limitations: Although carbon felt itself has good conductivity, its internal structure may be uneven, resulting in complex electron transmission paths and affecting the efficiency and speed of electrochemical reactions.

[0006] Limited catalytic activity: When pure carbon materials are used as electrocatalysts, their catalytic activity for specific chemical reactions is relatively low, especially in some electrochemical processes that require highly active catalysts, such as water decomposition and oxygen reduction reaction.

[0007] Stability issues: Under long-term operation or extreme conditions, carbon felt electrodes may face problems of decreased structural stability, including morphological changes, physical damage or chemical corrosion, which will directly affect their service life and performance.

[0008] Difficulty of surface modification: Although the surface of carbon materials can be functionalized to improve their performance, it remains a challenge to find a suitable modification method and achieve efficient and stable modification. Summary of the Invention

[0009] The embodiments of the present disclosure aim to solve at least one of the technical problems existing in the prior art, and disclose a carbon felt electrode loaded with a copper sulfide / graphene composite catalyst, and a preparation method and application thereof.

[0010] In a first aspect, an embodiment of the present disclosure provides a method for preparing a carbon felt electrode loaded with a copper sulfide / graphene composite catalyst, the method comprising:

[0011] Prepare the plating solution: copper sulfate concentration is 20mg / mL to 40mg / mL, sodium citrate concentration is 50mg / mL to 60mg / mL, sodium tartrate concentration is 1mg / mL to 3mg / mL, and sodium lauryl sulfate concentration is 0.5mg / mL to 1mg / mL;

[0012] Using commercial pre-oxidized carbon felt as a cathode and a copper sheet as an anode, electroplating is performed in the electroplating solution at room temperature and a voltage of 4V to 8V; the electroplated carbon felt is washed with deionized water until neutral, and dried in a vacuum oven to obtain a copper-modified carbon felt material;

[0013] A 0.5 mg / mL to 1.5 mg / mL diethyl ether solution of hexaethynylbenzene monomer is prepared, and then 0.5% to 1.5% by volume of pyridine is added; the copper-modified carbon felt material is immersed in the diethyl ether solution, taken out after 3 days, washed, and dried to obtain a copper-modified carbon felt material with graphyne grown thereon;

[0014] A 1 mg / mL to 2 mg / mL thiourea ethylene glycol solution is prepared, the copper-modified carbon felt material with graphyne grown thereon is immersed in the ethylene glycol solution, and the solution is kept at a preset temperature for a preset time; after washing and drying, a carbon felt electrode loaded with a copper sulfide / graphyne composite catalyst is obtained.

[0015] In some possible embodiments, in the step of preparing the electroplating solution, the concentration of copper sulfate is 20 mg / mL, the concentration of sodium citrate is 50 mg / mL, the concentration of sodium tartrate is 1 mg / mL, and the concentration of sodium lauryl sulfate is 0.5 mg / mL.

[0016] In some possible embodiments, in the step of preparing the electroplating solution, the concentration of copper sulfate is 40 mg / mL, the concentration of sodium citrate is 60 mg / mL, the concentration of sodium tartrate is 3 mg / mL, and the concentration of sodium lauryl sulfate is 1 mg / mL.

[0017] In some possible embodiments, in the step of preparing the electroplating solution, the concentration of copper sulfate is 30 mg / mL, the concentration of sodium citrate is 55 mg / mL, the concentration of sodium tartrate is 2 mg / mL, and the concentration of sodium lauryl sulfate is 0.75 mg / mL.

[0018] In some possible embodiments, in the diethyl ether solution, the content of the hexaethynylbenzene monomer is 0.5 mg / mL, and the volume percentage of the pyridine is 0.5%.

[0019] In some possible embodiments, in the diethyl ether solution, the content of the hexaethynylbenzene monomer is 1.5 mg / mL, and the volume percentage of the pyridine is 1.5%.

[0020] In some possible embodiments, in the ethylene glycol solution, the content of thiourea is 1 mg / mL.

[0021] In some possible embodiments, the preset temperature is 70° C. to 90° C., and the preset time is 11 hours to 13 hours.

[0022] In a second aspect, an embodiment of the present disclosure provides a carbon felt electrode loaded with a copper sulfide / graphene composite catalyst, wherein the carbon felt electrode is prepared using the method described above.

[0023] In a third aspect, an embodiment of the present disclosure provides an application of a carbon felt electrode loaded with a copper sulfide / graphene composite catalyst in a liquid flow battery, wherein the carbon felt electrode is prepared using the method described above.

[0024] The carbon felt electrode loaded with copper sulfide / graphene composite catalyst and its preparation method and application in the embodiments of the present disclosure have the following beneficial effects:

[0025] Enhanced catalytic activity: Copper sulfide (CuS), as a semiconductor material, can form efficient catalytic sites when combined with graphyne (GDY), significantly improving the catalytic activity of the electrode for target reactions, especially in reactions involving electron transfer, such as electrochemical synthesis and energy conversion.

[0026] Improved conductivity and electron transfer efficiency: Due to its unique two-dimensional structure and excellent conductivity, graphyne can provide a fast electron transfer channel for the composite material. Combined with the carbon felt substrate, it can effectively improve the conductivity of the entire electrode and accelerate the charge transfer process.

[0027] Improved stability: The introduction of CuS / GDY composite material not only enhances the catalytic performance of the electrode, but also improves the stability and durability of the electrode during repeated use by forming a more stable overall structure, thereby extending its service life;

[0028] Optimized surface properties: The planar structure of graphyne provides an ideal platform for loading catalysts, which helps to evenly distribute catalyst particles, further optimizes the reaction environment on the electrode surface, and improves reaction efficiency and selectivity;

[0029] In summary, the embodiments of the present disclosure not only overcome the limitations of traditional carbon felt electrodes in catalytic activity, conductivity and stability by loading the CuS / GDY composite catalyst onto the carbon felt electrode, but also optimize the comprehensive performance of the electrode through material design, providing a more efficient and stable electrode material solution for fields such as electrochemical reactions, energy storage and conversion. BRIEF DESCRIPTION OF THE DRAWINGS

[0030] The above and other features, advantages, and aspects of the various embodiments of the present disclosure will become more apparent with reference to the following detailed description in conjunction with the accompanying drawings. Throughout the drawings, the same or similar reference numerals represent the same or similar elements. It should be understood that the drawings are schematic and that components and elements are not necessarily drawn to scale.

[0031] Figure 1 The present invention is a flow chart of a method for preparing a carbon felt electrode loaded with a copper sulfide / graphene composite catalyst according to an embodiment of the present invention. DETAILED DESCRIPTION

[0032] To enable those skilled in the art to better understand the technical solutions of the present disclosure, the present disclosure is further described in detail below in conjunction with the accompanying drawings and specific embodiments. It is apparent that the described embodiments are only a portion of the embodiments of the present disclosure, not all of them. Based on the described embodiments of the present disclosure, all other embodiments obtained by those skilled in the art without the need for creative work are within the scope of protection of the present disclosure.

[0033] Unless otherwise specified, the technical terms or scientific terms used in the embodiments of the present disclosure should be understood by people with ordinary skills in the field to which the present disclosure belongs. The "including" or "comprising" used in the embodiments of the present disclosure neither limits the shapes, numbers, steps, actions, operations, components, originals and / or their groups mentioned, nor excludes the appearance or addition of one or more other different shapes, numbers, steps, actions, operations, components, originals and / or their groups, or the addition of these. In addition, the terms "first" and "second" are used for descriptive purposes only and cannot be understood as indicating or implying relative importance or implicitly indicating the number and order of the indicated technical features. Thus, the features defined as "first" and "second" may explicitly or implicitly include one or more of the features. In the description of the embodiments of the present disclosure, the meaning of "multiple" is two or more, unless otherwise clearly and specifically defined.

[0034] Unless otherwise specifically stated, the relative arrangements of the components and steps, numerical expressions, and numerical values ​​set forth in these embodiments do not limit the scope of the present disclosure. At the same time, it should be understood that, for ease of description, the dimensions of the various parts shown in the drawings are not drawn in accordance with actual proportional relationships, and that the techniques, methods, and devices known to those of ordinary skill in the relevant art may not be discussed in detail, but where appropriate, the techniques, methods, and devices shown should be considered part of the authorized specification. In all examples shown and discussed herein, any specific other examples may have different values. It should be noted that similar symbols and letters represent similar items in the following figures, and therefore, once an item is defined in one figure, it does not need to be further discussed in subsequent figures.

[0035] In the description of the embodiments of the present disclosure, the description with reference to the terms "one embodiment", "some embodiments", "example", "specific example", or "some examples" means that the specific features, structures, materials or characteristics described in conjunction with the embodiment or example are included in at least one embodiment or example of the present disclosure. In the embodiments of the present disclosure, the schematic representations of the above terms do not necessarily refer to the same embodiment or example. Moreover, the specific features, structures, materials or characteristics described may be combined in a suitable manner in any one or more embodiments or examples. In addition, those skilled in the art may combine and combine the different embodiments or examples described in the embodiments of the present disclosure and the features of the different embodiments or examples, unless they are contradictory.

[0036] Figure 1 The flowchart of the method for preparing a carbon felt electrode loaded with copper sulfide / graphene composite catalyst according to one embodiment of the present disclosure is shown in FIG. Figure 1 As shown, a method for preparing a carbon felt electrode loaded with a copper sulfide / graphene composite catalyst comprises the following steps S101 to S104:

[0037] Step S101, prepare an electroplating solution: copper sulfate concentration is 20 mg / mL to 40 mg / mL, sodium citrate concentration is 50 mg / mL to 60 mg / mL, sodium tartrate concentration is 1 mg / mL to 3 mg / mL, and sodium lauryl sulfate concentration is 0.5 mg / mL to 1 mg / mL.

[0038] Step S102: using commercial pre-oxidized carbon felt as the cathode and the copper sheet as the anode, electroplating is performed in the electroplating solution at room temperature and a plating voltage of 4V to 8V; washing the electroplated carbon felt with deionized water until it is neutral, and drying it in a vacuum oven to obtain a copper-modified carbon felt material.

[0039] Step S103, preparing a 0.5 mg / mL to 1.5 mg / mL ether solution of hexaethynylbenzene monomer, and then adding 0.5% to 1.5% by volume of pyridine; immersing the copper-modified carbon felt material in the ether solution, taking it out after 3 days, washing it, and drying it to obtain a copper-modified carbon felt material with graphyne grown on it.

[0040] Step S104: preparing a 1 mg / mL to 2 mg / mL thiourea ethylene glycol solution, immersing the copper-modified carbon felt material on which graphyne is grown in the ethylene glycol solution, and keeping the solution at a preset temperature for a preset time; after washing and drying, a carbon felt electrode loaded with a copper sulfide / graphyne composite catalyst is obtained.

[0041] The method for preparing a carbon felt electrode loaded with a copper sulfide / graphene (CuS / GDY) composite catalyst according to the embodiment of the present disclosure has the following beneficial effects:

[0042] Enhanced catalytic activity: Copper sulfide (CuS), as a semiconductor material, can form efficient catalytic sites when combined with graphyne (GDY), significantly improving the catalytic activity of the electrode for the target reaction, especially in reactions involving electron transfer, such as electrochemical synthesis, energy conversion and other fields.

[0043] Improved conductivity and electron transfer efficiency: Due to its unique two-dimensional structure and excellent conductivity, graphyne can provide a fast electron transfer channel for composite materials. Combined with the carbon felt substrate, it can effectively improve the conductivity of the entire electrode and accelerate the charge transfer process.

[0044] Improved stability: The introduction of CuS / GDY composite materials not only enhances the catalytic performance of the electrode, but also improves the stability and durability of the electrode during repeated use and extends its service life by forming a more stable overall structure.

[0045] Optimized surface properties: The planar structure of graphyne provides an ideal platform for loading catalysts, which helps to evenly distribute catalyst particles, further optimizes the reaction environment on the electrode surface, and improves reaction efficiency and selectivity.

[0046] In summary, the embodiments of the present disclosure not only overcome the limitations of traditional carbon felt electrodes in catalytic activity, conductivity and stability by loading the CuS / GDY composite catalyst onto the carbon felt electrode, but also optimize the comprehensive performance of the electrode through material design, providing a more efficient and stable electrode material solution for fields such as electrochemical reactions, energy storage and conversion.

[0047] In some possible embodiments, in the step of preparing the electroplating solution, the concentration of copper sulfate is 20 mg / mL, the concentration of sodium citrate is 50 mg / mL, the concentration of sodium tartrate is 1 mg / mL, and the concentration of sodium lauryl sulfate is 0.5 mg / mL.

[0048] In some possible embodiments, in the step of preparing the electroplating solution, the concentration of copper sulfate is 40 mg / mL, the concentration of sodium citrate is 60 mg / mL, the concentration of sodium tartrate is 3 mg / mL, and the concentration of sodium lauryl sulfate is 1 mg / mL.

[0049] In some possible embodiments, in the step of preparing the electroplating solution, the concentration of copper sulfate is 30 mg / mL, the concentration of sodium citrate is 55 mg / mL, the concentration of sodium tartrate is 2 mg / mL, and the concentration of sodium lauryl sulfate is 0.75 mg / mL.

[0050] In some possible embodiments, in the diethyl ether solution, the content of the hexaethynylbenzene monomer is 0.5 mg / mL, and the volume percentage of the pyridine is 0.5%.

[0051] In some possible embodiments, in the diethyl ether solution, the content of the hexaethynylbenzene monomer is 1.5 mg / mL, and the volume percentage of the pyridine is 1.5%.

[0052] In some possible embodiments, in the ethylene glycol solution, the content of thiourea is 1 mg / mL.

[0053] In some possible embodiments, the preset temperature is 70° C. to 90° C., and the preset time is 11 hours to 13 hours.

[0054] The preparation method of the carbon felt electrode loaded with copper sulfide / graphene composite catalyst disclosed in the present invention will be specifically described below with reference to several embodiments.

[0055] Example 1

[0056] A method for preparing a carbon felt electrode loaded with a copper sulfide / graphene composite catalyst, the method comprising the following steps:

[0057] Prepare the plating solution: copper sulfate concentration is 20 mg / mL, sodium citrate concentration is 50 mg / mL, sodium tartrate concentration is 1 mg / mL, and sodium lauryl sulfate concentration is 0.5 mg / mL.

[0058] Commercial pre-oxidized carbon felt was used as a cathode and a copper sheet was used as an anode. Electroplating was carried out in the electroplating solution at room temperature and a plating voltage of 4 V. The electroplated carbon felt was washed with deionized water until neutral, and dried in a vacuum oven to obtain a copper-modified carbon felt material.

[0059] A 0.5 mg / mL ether solution of hexaethynylbenzene monomer was prepared, and then 0.5% by volume of pyridine was added; the copper-modified carbon felt material was immersed in the ether solution, taken out after 3 days, washed, and dried to obtain a copper-modified carbon felt material with graphyne grown thereon.

[0060] A 1 mg / mL thiourea ethylene glycol solution was prepared, and the copper-modified carbon felt material with graphyne grown thereon was immersed in the ethylene glycol solution and kept warm at 70° C. for 11 hours. After washing and drying, a carbon felt electrode loaded with a copper sulfide / graphyne composite catalyst was obtained.

[0061] Example 2

[0062] A method for preparing a carbon felt electrode loaded with a copper sulfide / graphene composite catalyst, the method comprising the following steps:

[0063] Prepare the plating solution: copper sulfate concentration is 40 mg / mL, sodium citrate concentration is 60 mg / mL, sodium tartrate concentration is 3 mg / mL, and sodium dodecyl sulfate concentration is 1 mg / mL.

[0064] Commercial pre-oxidized carbon felt was used as a cathode and a copper sheet was used as an anode. Electroplating was carried out in the electroplating solution at room temperature and a plating voltage of 8 V. The electroplated carbon felt was washed with deionized water until neutral, and dried in a vacuum oven to obtain a copper-modified carbon felt material.

[0065] A 1.5 mg / mL ether solution of hexaethynylbenzene monomer was prepared, and then 1.5% by volume of pyridine was added; the copper-modified carbon felt material was immersed in the ether solution, taken out after 3 days, washed, and dried to obtain a copper-modified carbon felt material with graphyne grown thereon.

[0066] A 2 mg / mL thiourea ethylene glycol solution was prepared, and the copper-modified carbon felt material with graphyne grown thereon was immersed in the ethylene glycol solution and kept warm at 90° C. for 13 h. After washing and drying, a carbon felt electrode loaded with a copper sulfide / graphyne composite catalyst was obtained.

[0067] Example 3

[0068] A method for preparing a carbon felt electrode loaded with a copper sulfide / graphene composite catalyst, the method comprising the following steps:

[0069] Prepare the plating solution: copper sulfate concentration is 30 mg / mL, sodium citrate concentration is 55 mg / mL, sodium tartrate concentration is 2 mg / mL, and sodium lauryl sulfate concentration is 0.75 mg / mL.

[0070] Commercial pre-oxidized carbon felt was used as a cathode and a copper sheet was used as an anode. Electroplating was carried out in the electroplating solution at room temperature and a plating voltage of 6 V. The electroplated carbon felt was washed with deionized water until neutral, and dried in a vacuum oven to obtain a copper-modified carbon felt material.

[0071] A 1 mg / mL ether solution of hexaethynylbenzene monomer was prepared, and then 1% by volume of pyridine was added; the copper-modified carbon felt material was immersed in the ether solution, taken out after 3 days, washed, and dried to obtain a copper-modified carbon felt material with graphyne grown thereon.

[0072] A 1.5 mg / mL thiourea ethylene glycol solution was prepared, and the copper-modified carbon felt material with graphyne grown thereon was immersed in the ethylene glycol solution and kept warm at 80° C. for 12 h. After washing and drying, a carbon felt electrode loaded with a copper sulfide / graphyne composite catalyst was obtained.

[0073] Based on the same inventive concept, an embodiment of the present disclosure provides a carbon felt electrode loaded with a copper sulfide / graphene composite catalyst. The carbon felt electrode is prepared using the method described above. For details, please refer to the relevant records above and will not be repeated here.

[0074] The carbon felt electrode loaded with a copper sulfide / graphene (CuS / GDY) composite catalyst according to the embodiment of the present disclosure has the following beneficial effects:

[0075] Enhanced catalytic activity: Copper sulfide (CuS), as a semiconductor material, can form efficient catalytic sites when combined with graphyne (GDY), significantly improving the catalytic activity of the electrode for the target reaction, especially in reactions involving electron transfer, such as electrochemical synthesis, energy conversion and other fields.

[0076] Improved conductivity and electron transfer efficiency: Due to its unique two-dimensional structure and excellent conductivity, graphyne can provide a fast electron transfer channel for composite materials. Combined with the carbon felt substrate, it can effectively improve the conductivity of the entire electrode and accelerate the charge transfer process.

[0077] Improved stability: The introduction of CuS / GDY composite materials not only enhances the catalytic performance of the electrode, but also improves the stability and durability of the electrode during repeated use and extends its service life by forming a more stable overall structure.

[0078] Optimized surface properties: The planar structure of graphyne provides an ideal platform for loading catalysts, which helps to evenly distribute catalyst particles, further optimizes the reaction environment on the electrode surface, and improves reaction efficiency and selectivity.

[0079] In summary, the embodiments of the present disclosure not only overcome the limitations of traditional carbon felt electrodes in catalytic activity, conductivity and stability by loading the CuS / GDY composite catalyst onto the carbon felt electrode, but also optimize the comprehensive performance of the electrode through material design, providing a more efficient and stable electrode material solution for fields such as electrochemical reactions, energy storage and conversion.

[0080] Based on the same inventive concept, an embodiment of the present disclosure provides an application of a carbon felt electrode loaded with a copper sulfide / graphene composite catalyst in a liquid flow battery. The carbon felt electrode is prepared using the method described above. For details, please refer to the relevant records above and will not be repeated here.

[0081] The application of the carbon felt electrode loaded with copper sulfide / graphene composite catalyst in a flow battery according to the embodiment of the present disclosure has the following beneficial effects:

[0082] Enhanced catalytic activity: Copper sulfide (CuS), as a semiconductor material, can form efficient catalytic sites when combined with graphyne (GDY), significantly improving the catalytic activity of the electrode for the target reaction, especially in reactions involving electron transfer, such as electrochemical synthesis, energy conversion and other fields.

[0083] Improved conductivity and electron transfer efficiency: Due to its unique two-dimensional structure and excellent conductivity, graphyne can provide a fast electron transfer channel for composite materials. Combined with the carbon felt substrate, it can effectively improve the conductivity of the entire electrode and accelerate the charge transfer process.

[0084] Improved stability: The introduction of CuS / GDY composite materials not only enhances the catalytic performance of the electrode, but also improves the stability and durability of the electrode during repeated use and extends its service life by forming a more stable overall structure.

[0085] Optimized surface properties: The planar structure of graphyne provides an ideal platform for loading catalysts, which helps to evenly distribute catalyst particles, further optimizes the reaction environment on the electrode surface, and improves reaction efficiency and selectivity.

[0086] In summary, the embodiments of the present disclosure not only overcome the limitations of traditional carbon felt electrodes in catalytic activity, conductivity and stability by loading the CuS / GDY composite catalyst onto the carbon felt electrode, but also optimize the comprehensive performance of the electrode through material design, providing a more efficient and stable electrode material solution for fields such as electrochemical reactions, energy storage and conversion.

[0087] It is understood that the above embodiments are merely exemplary embodiments for illustrating the principles of the present disclosure, and the present disclosure is not limited thereto. Those skilled in the art may make various modifications and improvements without departing from the spirit and substance of the present disclosure, and such modifications and improvements are also considered to be within the scope of protection of the present disclosure.

Claims

1. A method for preparing a carbon felt electrode loaded with a copper sulfide / graphene composite catalyst, characterized in that: The method comprises: Prepare the plating solution: copper sulfate concentration is 20mg / mL to 40mg / mL, sodium citrate concentration is 50mg / mL to 60mg / mL, sodium tartrate concentration is 1mg / mL to 3mg / mL, and sodium lauryl sulfate concentration is 0.5mg / mL to 1mg / mL; Using commercial pre-oxidized carbon felt as a cathode and a copper sheet as an anode, electroplating is performed in the electroplating solution at room temperature and a voltage of 4V to 8V; the electroplated carbon felt is washed with deionized water until neutral, and dried in a vacuum oven to obtain a copper-modified carbon felt material; A 0.5 mg / mL to 1.5 mg / mL diethyl ether solution of hexaethynylbenzene monomer is prepared, and then 0.5% to 1.5% by volume of pyridine is added; the copper-modified carbon felt material is immersed in the diethyl ether solution, taken out after 3 days, washed, and dried to obtain a copper-modified carbon felt material with graphyne grown thereon; A 1 mg / mL to 2 mg / mL thiourea ethylene glycol solution is prepared, the copper-modified carbon felt material with graphyne grown thereon is immersed in the ethylene glycol solution, and the solution is kept at a preset temperature for a preset time; after washing and drying, a carbon felt electrode loaded with a copper sulfide / graphyne composite catalyst is obtained.

2. The method according to claim 1, characterized in that In the step of preparing the electroplating solution, the concentration of copper sulfate is 20 mg / mL, the concentration of sodium citrate is 50 mg / mL, the concentration of sodium tartrate is 1 mg / mL, and the concentration of sodium lauryl sulfate is 0.5 mg / mL.

3. The method according to claim 1, characterized in that In the step of preparing the electroplating solution, the concentration of copper sulfate is 40 mg / mL, the concentration of sodium citrate is 60 mg / mL, the concentration of sodium tartrate is 3 mg / mL, and the concentration of sodium lauryl sulfate is 1 mg / mL.

4. The method according to claim 1, wherein In the step of preparing the electroplating solution, the concentration of copper sulfate is 30 mg / mL, the concentration of sodium citrate is 55 mg / mL, the concentration of sodium tartrate is 2 mg / mL, and the concentration of sodium lauryl sulfate is 0.75 mg / mL.

5. The method according to any one of claims 1 to 4, characterized in that In the diethyl ether solution, the content of the hexaethynylbenzene monomer is 0.5 mg / mL, and the volume percentage of the pyridine is 0.5%.

6. The method according to any one of claims 1 to 4, characterized in that In the diethyl ether solution, the content of the hexaethynylbenzene monomer is 1.5 mg / mL, and the volume percentage of the pyridine is 1.5%.

7. The method according to any one of claims 1 to 4, characterized in that In the ethylene glycol solution, the content of thiourea is 1 mg / mL.

8. The method according to any one of claims 1 to 4, characterized in that The preset temperature is 70° C. to 90° C., and the preset time is 11 hours to 13 hours.

9. A carbon felt electrode loaded with a copper sulfide / graphene composite catalyst, characterized in that: The carbon felt electrode is prepared by the method according to any one of claims 1 to 8.

10. Application of a carbon felt electrode loaded with a copper sulfide / graphene composite catalyst in a flow battery, characterized in that: The carbon felt electrode is prepared by the method according to any one of claims 1 to 8.

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