Preparation method of low-temperature coating high-entropy alloy composite carbon electrode and perovskite solar cell

Abstract

This invention discloses a method for preparing a low-temperature coated high-entropy alloy composite carbon electrode and a perovskite solar cell, belonging to the technical field of semiconductor device fabrication methods. The preparation method includes mixing a high-entropy alloy, nano-carbon powder, dispersant, binder, functional additives, and solvent to obtain a high-entropy alloy composite carbon slurry; finally, coating the high-entropy alloy composite carbon slurry onto a substrate material, followed by heat treatment and drying to obtain a high-entropy alloy composite carbon electrode with good interfacial contact. This invention is simple to prepare, low in cost, enhances the interfacial contact between the electrode layer and the perovskite layer in perovskite solar cells, and effectively improves the problems of poor electrical contact and energy level matching at the perovskite interface, thereby improving the photoelectric conversion efficiency of the solar cell. It is suitable for perovskite solar cells of various structures.

Description

Technical Field

[0001] This invention relates to the technical field of methods for preparing semiconductor devices, and more particularly to a method for preparing a high-entropy alloy composite carbon electrode that can be coated at low temperatures and a perovskite solar cell. Background Technology

[0002] Solar energy, as the fastest-growing and most dynamic sector in the new energy field, has attracted much attention and favor. As a potential replacement for traditional photovoltaic cells, organic-inorganic lead halide perovskite solar cells have garnered global attention due to their advantages such as high light absorption coefficient, low exciton binding energy, bipolar charge transport, high carrier mobility, and low fabrication cost. In just over a decade, the photoelectric conversion efficiency of perovskite solar cells has rapidly increased from an initial 3.8% to 25.7%, making it comparable to commercially available crystalline silicon solar cells in terms of efficiency. However, almost all high-efficiency perovskite solar cells rely on high-vacuum evaporation of precious metals such as gold and silver to fabricate the counter electrode, resulting in high cost and energy consumption. Furthermore, the reaction of silver with halide ions and the permeation of gold throughout the device can cause performance degradation, negatively impacting long-term stability and commercialization, severely hindering its industrial development.

[0003] To address the aforementioned issues, replacing precious metals such as gold and silver with carbon electrodes is a good approach. Carbon electrodes possess excellent charge transfer properties, and their inherent stability and hydrophobicity can further enhance battery stability. Simultaneously, their low cost and low-temperature processing capabilities further reduce the industrialization cost of the battery. However, their efficiency is far lower than that of metal electrodes, typically around 13%. This is mainly due to the incompatibility between carbon-based perovskite solar cells and organic hole transport materials. Current research largely focuses on carbon-based perovskite solar cells without hole transport materials. Furthermore, the chemical inertness of carbon materials makes it difficult to optimize their energy level matching with perovskite thin films through work function modulation, thus limiting the development of carbon-based perovskite solar cells. Summary of the Invention

[0004] In view of the above-mentioned deficiencies of the prior art, in a first aspect of the present invention, a method for preparing a low-temperature coated high-entropy alloy composite carbon electrode with good interface energy level matching is provided, comprising the following steps:

[0005] 1) Mix high-entropy alloy, nano carbon powder, dispersant, binder, and functional additives to obtain a premix;

[0006] 2) The premixed material is further mixed with a solvent to prepare a high-entropy alloy composite carbon slurry;

[0007] 3) The high-entropy alloy composite carbon slurry is coated onto a substrate material to form a high-entropy alloy composite carbon wet film. The high-entropy alloy composite carbon wet film is dried to obtain a high-entropy alloy composite carbon electrode.

[0008] Preferably, in step 1), the mass percentages of each component in the premix are as follows: high entropy alloy 5%–30%, nano carbon powder 50%–80%, dispersant 0.5%–1%, binder 5%–15%, and functional additives 5%–15%.

[0009] More preferably, the high-entropy alloy includes at least one of FeCoNiMoCr high-entropy alloy, FeCoNiCrP high-entropy alloy, CoCrFeNiAl high-entropy alloy, FeCoNiCrMn high-entropy alloy, NpPtPdAuAgRuAl high-entropy alloy, TaMoWReRu high-entropy alloy, FeCuPtCoNi high-entropy alloy, CoCrFeNiW high-entropy alloy, CoCrFeNiSn high-entropy alloy, AlFeNiCrCoTi high-entropy alloy, and AlCuFeMnNi high-entropy alloy.

[0010] More preferably, the nano-carbon powder includes at least one of graphite, carbon black, graphene, carbon nanotubes, and graphene oxide.

[0011] Furthermore, the particle size of the graphite, carbon black, graphene, and graphene oxide is 10–200 nm; the diameter of the carbon nanotubes is 10–100 nm, and the length is 5–50 μm.

[0012] More preferably, the dispersant includes at least one of polyvinylpyrrolidone and ethylene glycol.

[0013] More preferably, the adhesive comprises at least one of ethyl cellulose, ethylene-vinyl acetate copolymer, acrylic resin, polyvinyl acetate, polyamide, polystyrene, polymethyl methacrylate, and polycarbonate.

[0014] More preferably, the functional additive includes at least one of nickel oxide nanomaterials, tungsten oxide, cuprous iodide, cuprous thiocyanate, and copper phthalocyanine.

[0015] Furthermore, the particle size of the nickel oxide nanomaterial is 5–300 nm.

[0016] Preferably, in step 2), the ratio of the total mass of the high-entropy alloy and nano-carbon powder in the premix to the mass of the solvent is 1 to 5:1.

[0017] More preferably, the solvent includes at least one selected from terpineol, ethylene glycol methyl ether, glycerol, ethyl acetate, glycerol methyl ether, and butyl acetate.

[0018] Preferably, in step 3), the coating method includes screen printing or extrusion coating; the drying temperature is 80-100°C.

[0019] In a second aspect of the present invention, a perovskite solar cell is provided, wherein the perovskite solar cell comprises, from bottom to top, a transparent conductive substrate, an electron transport layer, a perovskite layer, and a high-entropy alloy composite carbon electrode; the high-entropy alloy composite carbon electrode is prepared by the preparation method of the first aspect of the present invention.

[0020] Preferably, the transparent conductive substrate includes an FTO glass substrate, an ITO glass substrate, or an ITO flexible substrate.

[0021] Preferably, the electron transport layer comprises planar TiO2, planar SnO2, planar ZnO, mesoporous TiO2, dense TiO2, and mesoporous Al2O3.

[0022] Compared with the prior art, the present invention has the following advantages and beneficial effects:

[0023] 1. The preparation method of this invention is simple and convenient, and is suitable for preparing high-entropy alloy composite carbon slurries that can be coated at low temperatures. This preparation method introduces a high-entropy alloy with excellent properties. The uniform mixing of multiple elements in the high-entropy alloy leads to an increase in entropy value and a decrease in Gibbs free energy, resulting in good stability. Furthermore, due to variations in atomic radius and the different geometric configurations of the elements, lattice distortion and slow diffusion occur, potentially leading to more active sites in the high-entropy alloy. The cocktail effect resulting from the multi-element mixing can yield performance exceeding the average value of the single elements, giving this method highly controllable and excellent performance.

[0024] 2. The perovskite solar cell provided by this invention includes a high-entropy alloy composite carbon electrode prepared from a high-entropy alloy composite carbon paste. The high-entropy alloy in the high-entropy alloy composite carbon electrode has good conductivity and stability, its work function is adjustable, it optimizes the charge extraction efficiency at the electrode interface, has good energy level matching, and improves the efficiency of the perovskite solar cell. Attached Figure Description

[0025] Figure 1 This is a schematic diagram of the structure of a perovskite solar cell, where 1 is a transparent conductive substrate, 2 is an electron transport layer, 3 is a perovskite layer, and 4 is a high-entropy alloy composite carbon electrode.

[0026] Figure 2 A flowchart illustrating the preparation method of a low-temperature coated high-entropy alloy composite carbon electrode;

[0027] Figure 3 The current density-voltage curves are shown for the high-entropy alloy composite carbon electrodes prepared in Examples 1-4, respectively, applied to the perovskite solar cell prepared in Example 12. Detailed Implementation

[0028] The present invention is further illustrated below by way of embodiments, but the invention is not limited to the scope of the embodiments described herein. Experimental methods in the following embodiments that do not specify specific conditions were performed according to conventional methods and conditions, or as selected according to the product instructions.

[0029] In the following examples, the particle size of graphite, carbon black, graphene, and graphene oxide is between 10 and 200 nm, the diameter of carbon nanotubes is between 10 and 100 nm, the length is between 5 and 50 μm, and the particle size of nickel oxide nanomaterials is between 5 and 300 nm.

[0030] Example 1

[0031] like Figure 2 As shown, a method for preparing a low-temperature coated high-entropy alloy composite carbon electrode is described below:

[0032] 1) By mass percentage, take 20% FeCoNiCrMn high-entropy alloy, 60% nano-carbon powder formed by mixing graphite and carbon black in a mass ratio of 3:1, 1% ethylene glycol, 5% ethyl cellulose, and 14% nickel oxide nanomaterials and mix them to obtain a premix.

[0033] 2) The premix is ​​further mixed with terpineol, and the ratio of the total mass of FeCoNiCrMn high-entropy alloy and nano carbon powder in the premix to the mass of terpineol is 3:1, to prepare a high-entropy alloy composite carbon slurry;

[0034] 3) The high-entropy alloy composite carbon slurry is screen-printed onto a substrate material to form a high-entropy alloy composite carbon wet film. The high-entropy alloy composite carbon wet film is dried at 90°C to obtain a high-entropy alloy composite carbon electrode.

[0035] Example 2

[0036] like Figure 2 As shown, a method for preparing a low-temperature coated high-entropy alloy composite carbon electrode is described below:

[0037] 1) By mass percentage, take 20% FeCuPtCoNi high-entropy alloy, 60% nano-carbon powder formed by mixing graphite and carbon black in a mass ratio of 3:1, 1% ethylene glycol, 5% ethyl cellulose, and 14% nickel oxide nanomaterials and mix them to obtain a premix.

[0038] 2) The premix is ​​further mixed with terpineol, and the ratio of the total mass of FeCuPtCoNi high-entropy alloy and nano carbon powder in the premix to the mass of terpineol is 3:1, to prepare a high-entropy alloy composite carbon slurry;

[0039] 3) The high-entropy alloy composite carbon slurry is screen-printed onto a substrate material to form a high-entropy alloy composite carbon wet film. The high-entropy alloy composite carbon wet film is dried at 90°C to obtain a high-entropy alloy composite carbon electrode.

[0040] Example 3

[0041] like Figure 2 As shown, a method for preparing a low-temperature coated high-entropy alloy composite carbon electrode is described below:

[0042] 1) By mass percentage, take 20% of CoCrFeNiAl high-entropy alloy, 60% of nano-carbon powder formed by mixing graphite and carbon black in a mass ratio of 3:1, 1% of ethylene glycol, 5% of ethyl cellulose, and 14% of nickel oxide nanomaterials and mix them to obtain a premix.

[0043] 2) The premix is ​​further mixed with terpineol, and the ratio of the total mass of CoCrFeNiAl high-entropy alloy and nano carbon powder in the premix to the mass of terpineol is 3:1, to prepare a high-entropy alloy composite carbon slurry;

[0044] 3) The high-entropy alloy composite carbon slurry is screen-printed onto a substrate material to form a high-entropy alloy composite carbon wet film. The high-entropy alloy composite carbon wet film is dried at 90°C to obtain a high-entropy alloy composite carbon electrode.

[0045] Example 4

[0046] like Figure 2 As shown, a method for preparing a low-temperature coated high-entropy alloy composite carbon electrode is described below:

[0047] 1) By mass percentage, take 20% of CoCrFeNiW high-entropy alloy, 60% of nano-carbon powder formed by mixing graphite and carbon black in a mass ratio of 3:1, 1% of ethylene glycol, 5% of ethyl cellulose, and 14% of nickel oxide nanomaterials and mix them to obtain a premix.

[0048] 2) The premix is ​​further mixed with terpineol, and the ratio of the total mass of CoCrFeNiW high-entropy alloy and nano carbon powder in the premix to the mass of terpineol is 3:1, to prepare a high-entropy alloy composite carbon slurry;

[0049] 3) The high-entropy alloy composite carbon slurry is screen-printed onto a substrate material to form a high-entropy alloy composite carbon wet film. The high-entropy alloy composite carbon wet film is dried at 90°C to obtain a high-entropy alloy composite carbon electrode.

[0050] Example 5

[0051] like Figure 2 As shown, a method for preparing a low-temperature coated high-entropy alloy composite carbon electrode is described below:

[0052] 1) By mass percentage, 20% of FeCoNiMoCr high-entropy alloy, 60% of graphite, 1% of ethylene pyrrolidone, 5% of ethylene-vinyl acetate copolymer, and 14% of tungsten oxide are mixed to obtain a premix.

[0053] 2) The premix is ​​further mixed with ethylene glycol methyl ether, and the ratio of the total mass of FeCoNiMoCr high-entropy alloy and graphite in the premix to the mass of ethylene glycol methyl ether is 3:1, to prepare a high-entropy alloy composite carbon slurry;

[0054] 3) The high-entropy alloy composite carbon slurry is coated onto the substrate material by extrusion coating to form a high-entropy alloy composite carbon wet film. The high-entropy alloy composite carbon wet film is dried at 80°C to obtain a high-entropy alloy composite carbon electrode.

[0055] Example 6

[0056] like Figure 2 As shown, a method for preparing a low-temperature coated high-entropy alloy composite carbon electrode is described below:

[0057] 1) By mass percentage, take 20% FeCoNiCrP high-entropy alloy, 60% carbon black, 1% ethylene glycol, 5% acrylic resin and 14% cuprous iodide and mix them to obtain a premix.

[0058] 2) The premix is ​​further mixed with terpineol, and the ratio of the total mass of FeCoNiCrP high-entropy alloy and carbon black in the premix to the mass of terpineol is 3:1, to prepare a high-entropy alloy composite carbon slurry;

[0059] 3) The high-entropy alloy composite carbon slurry is screen-printed onto a substrate material to form a high-entropy alloy composite carbon wet film. The high-entropy alloy composite carbon wet film is dried at 100°C to obtain a high-entropy alloy composite carbon electrode.

[0060] Example 7

[0061] like Figure 2 As shown, a method for preparing a low-temperature coated high-entropy alloy composite carbon electrode is described below:

[0062] 1) By mass percentage, take 20% of NpPtPdAuAgRuAl high-entropy alloy, 60% of carbon nanotubes, 1% of ethylene glycol, 5% of polyvinyl acetate, and 14% of cuprous thiocyanate and mix them to obtain a premix.

[0063] 2) The premix is ​​further mixed with glycerol, and the ratio of the total mass of NpPtPdAuAgRuAl high-entropy alloy and carbon nanotubes in the premix to the mass of glycerol is 3:1, to prepare a high-entropy alloy composite carbon slurry.

[0064] 3) The high-entropy alloy composite carbon slurry is screen-printed onto a substrate material to form a high-entropy alloy composite carbon wet film. The high-entropy alloy composite carbon wet film is dried at 90°C to obtain a high-entropy alloy composite carbon electrode.

[0065] Example 8

[0066] like Figure 2 As shown, a method for preparing a low-temperature coated high-entropy alloy composite carbon electrode is described below:

[0067] 1) By mass percentage, take 20% of TaMoWReRu high-entropy alloy, 60% of graphene oxide, 1% of ethylene glycol, 5% of polyamide, and 14% of copper phthalocyanine and mix them to obtain a premix.

[0068] 2) The premix is ​​further mixed with ethyl acetate, and the ratio of the total mass of TaMoWReRu high-entropy alloy and graphene oxide in the premix to the mass of ethyl acetate is 3:1, to prepare a high-entropy alloy composite carbon slurry;

[0069] 3) The high-entropy alloy composite carbon slurry is screen-printed onto a substrate material to form a high-entropy alloy composite carbon wet film. The high-entropy alloy composite carbon wet film is dried at 90°C to obtain a high-entropy alloy composite carbon electrode.

[0070] Example 9

[0071] like Figure 2 As shown, a method for preparing a low-temperature coated high-entropy alloy composite carbon electrode is described below:

[0072] 1) By mass percentage, take 5% of CoCrFeNiSn high-entropy alloy, 80% of nano-carbon powder formed by mixing graphite and carbon black in a mass ratio of 3:1, 0.5% of ethylene glycol, 5% of polystyrene, and 9.5% of nickel oxide nanomaterials and mix them to obtain a premix.

[0073] 2) The premix is ​​further mixed with glycerol methyl ether, and the ratio of the total mass of CoCrFeNiSn high-entropy alloy and nano carbon powder in the premix to the mass of glycerol methyl ether is 1:1, to prepare a high-entropy alloy composite carbon slurry;

[0074] 3) The high-entropy alloy composite carbon slurry is screen-printed onto a substrate material to form a high-entropy alloy composite carbon wet film. The high-entropy alloy composite carbon wet film is dried at 90°C to obtain a high-entropy alloy composite carbon electrode.

[0075] Example 10

[0076] like Figure 2 As shown, a method for preparing a low-temperature coated high-entropy alloy composite carbon electrode is described below:

[0077] 1) By mass percentage, take 30% of AlFeNiCrCoTi high-entropy alloy, 50% of nano-carbon powder formed by mixing graphite and carbon black in a mass ratio of 3:1, 1% of ethylene glycol, 14% of polymethyl methacrylate, and 5% of nickel oxide nanomaterials and mix them to obtain a premix.

[0078] 2) The premix is ​​further mixed with terpineol, and the ratio of the total mass of AlFeNiCrCoTi high-entropy alloy and nano carbon powder in the premix to the mass of terpineol is 3:1, to prepare a high-entropy alloy composite carbon slurry;

[0079] 3) The high-entropy alloy composite carbon slurry is screen-printed onto a substrate material to form a high-entropy alloy composite carbon wet film. The high-entropy alloy composite carbon wet film is dried at 90°C to obtain a high-entropy alloy composite carbon electrode.

[0080] Example 11

[0081] like Figure 2 As shown, a method for preparing a low-temperature coated high-entropy alloy composite carbon electrode is described below:

[0082] 1) By mass percentage, take 19% of AlCuFeMnNi high-entropy alloy, 50% of nano-carbon powder formed by mixing graphite and carbon black in a mass ratio of 3:1, 1% of ethylene glycol, 15% of polycarbonate, and 15% of nickel oxide nanomaterials and mix them to obtain a premix.

[0083] 2) The premix is ​​further mixed with butyl acetate, and the ratio of the total mass of AlCuFeMnNi high-entropy alloy and nano carbon powder in the premix to the mass of butyl acetate is 5:1, to prepare a high-entropy alloy composite carbon slurry;

[0084] 3) The high-entropy alloy composite carbon slurry is screen-printed onto a substrate material to form a high-entropy alloy composite carbon wet film. The high-entropy alloy composite carbon wet film is dried at 90°C to obtain a high-entropy alloy composite carbon electrode.

[0085] Example 12

[0086] like Figure 1 As shown, a perovskite solar cell comprises, from bottom to top, a transparent conductive substrate, an electron transport layer, a perovskite layer, and a high-entropy alloy composite carbon electrode; the high-entropy alloy composite carbon electrode is prepared by the preparation methods of Examples 1 to 4.

[0087] Perovskite solar cells are fabricated in the following way:

[0088] S1. Preparation of transparent conductive substrate: Cut ITO glass into 1.5cm×1.3cm pieces, and ultrasonically clean them in deionized water, acetone and ethanol for 30min each, then blow them dry to prepare ITO glass substrates for later use.

[0089] S2. Preparation of electron transport layer: 2.5% SnO2 hydrocolloid dispersion was spin-coated onto an ITO glass substrate by solution spin coating, and then annealed on a hot plate at 140℃ for 30 min to obtain a planar SnO2 structure. The spin coating speed was 4000 rpm and the spin coating time was 45 s to obtain the electron transport layer.

[0090] S3. Preparation of perovskite layer precursor solution: Add 1.3 mol / L methylammonium iodide and 1.3 mol / L lead iodide to a mixed solution of N,N-dimethylformamide and dimethyl sulfoxide. The final concentrations of methylammonium iodide and lead iodide are both 1.3 mol / L, and the volume ratio of N,N-dimethylformamide to dimethyl sulfoxide is 9:1 to obtain the perovskite layer precursor solution.

[0091] S4. Preparation of perovskite layer: The perovskite layer precursor solution is spin-coated onto the hole transport layer by spin coating at a speed of 4500 rpm for 40 s. During this process, diethyl ether is rapidly dropped onto the substrate in 14 s. Then, the substrate is annealed at 100 °C for 12.5 min to obtain the perovskite layer.

[0092] S5. Coating high-entropy alloy composite carbon electrode: Following the preparation methods of Examples 1 to 4, a layer of high-entropy alloy composite carbon slurry is coated on the perovskite layer by screen printing, and then annealed at 90°C for 30 min to obtain the high-entropy alloy composite carbon electrode.

[0093] The parameters, methods, and types of substances actually used in the above steps are preferred options in this embodiment. In other embodiments, other parameters, methods, and types of substances can be selected as needed.

[0094] The photovoltaic performance of perovskite solar cells fabricated using different high-entropy alloy composite carbon electrode methods was tested. The tests were conducted under AM 1.5G standard solar spectrum and an effective active layer area of ​​0.06 cm². The test results are shown in the graph below. Figure 3 As shown, the corresponding performance results are shown in Table 1.

[0095] Table 1: Photovoltaic performance results of perovskite solar cells fabricated using different high-entropy alloy composite carbon electrodes

[0096]

[0097] Depend on Figure 3As shown, with the two ends open, the battery output voltage of Example 1 is 1.049V. Theoretically, the more photons absorbed, the greater the short-circuit current. With a fixed effective area, the corresponding short-circuit current density is also greater. The current density at zero voltage, i.e., the short-circuit current density, is 21.15 mA / cm². 2 The fill factor is the ratio of the maximum output power to the product of the open-circuit voltage and the short-circuit current. The fill factor of Example 1 is 0.7333, which is relatively less than the interface defects of the device. The maximum energy conversion efficiency when the optimal load resistance is connected on the external circuit is 16.27%, which is higher than the general efficiency of carbon electrode perovskite cells.

[0098] The battery output voltage of Example 2 is 1.065V, which is higher than that of other examples; the short-circuit current density is 21.27mA / cm². 2 The fill factor was 0.7712; the conversion efficiency was 17.47%, higher than the general efficiency of carbon electrode perovskite cells and superior to other embodiments. The cell output voltage of Example 3 was 1.025V; the short-circuit current density was 20.49 mA / cm². 2 The fill factor was 0.7251; the conversion efficiency was 15.23%, which, although lower than other examples, was still higher than the general efficiency of carbon electrode perovskite cells. The cell output voltage of Example 4 was 1.025, lower than that of Examples 1 and 2; the short-circuit current density was 21.07 mA / cm². 2 The fill factor was 0.7566; the conversion efficiency was 16.34%, second only to Example 2.

[0099] As shown in Table 1, the perovskite solar cell of the present invention has good conversion efficiency and stability.

[0100] The preferred embodiments of the present invention have been described in detail above. It should be understood that those skilled in the art can make numerous modifications and variations based on the concept of the present invention without creative effort. Therefore, all technical solutions that can be obtained by those skilled in the art based on the concept of the present invention through logical analysis, reasoning, or limited experimentation on the basis of existing technology should be within the scope of protection defined by the claims.

Claims

1. A method for preparing a low-temperature coatable high-entropy alloy composite carbon electrode, characterized in that, Includes the following steps: 1) Mix high-entropy alloy, nano carbon powder, dispersant, binder, and functional additives to obtain a premix; The mass percentages of each component in the premix are as follows: high entropy alloy 5%~30%, nano carbon powder 50%~80%, dispersant 0.5%~1%, binder 5%~15%, and functional additives 5%~15%; The high-entropy alloy is at least one of the following: FeCoNiMoCr high-entropy alloy, FeCoNiCrP high-entropy alloy, CoCrFeNiAl high-entropy alloy, FeCoNiCrMn high-entropy alloy, NpPtPdAuAgRuAl high-entropy alloy, TaMoWReRu high-entropy alloy, FeCuPtCoNi high-entropy alloy, CoCrFeNiW high-entropy alloy, CoCrFeNiSn high-entropy alloy, AlFeNiCrCoTi high-entropy alloy, and AlCuFeMnNi high-entropy alloy. 2) The premixed material is further mixed with a solvent to prepare a high-entropy alloy composite carbon slurry; 3) The high-entropy alloy composite carbon slurry is coated onto a substrate material to form a high-entropy alloy composite carbon wet film. The high-entropy alloy composite carbon wet film is dried to obtain a high-entropy alloy composite carbon electrode.

2. The method of claim 1, wherein: In step 1), the nano-carbon powder includes at least one of graphite, carbon black, graphene, carbon nanotubes, and graphene oxide; wherein the particle size of graphite, carbon black, graphene, and graphene oxide is 10~200nm; and the diameter of carbon nanotubes is 10~100nm and the length is 5~50μm.

3. The method of claim 1, wherein: In step 1), the dispersant includes at least one of polyvinylpyrrolidone and ethylene glycol; the binder includes at least one of ethyl cellulose, ethylene-vinyl acetate copolymer, acrylic resin, polyvinyl acetate, polyamide, polystyrene, polymethyl methacrylate, and polycarbonate.

4. The method of claim 1, wherein: In step 1), the functional additive includes at least one of nickel oxide nanomaterials, tungsten oxide, cuprous iodide, cuprous thiocyanate, and copper phthalocyanine; wherein the particle size of the nickel oxide nanomaterials is 5~300nm.

5. The method of claim 1, wherein: In step 2), the ratio of the total mass of the high-entropy alloy and nano-carbon powder in the premix to the mass of the solvent is 1~5:1; the solvent includes at least one of terpineol, ethylene glycol methyl ether, glycerol, ethyl acetate, glycerol methyl ether, and butyl acetate.

6. The method of claim 1, wherein: In step 3), the coating method includes screen printing or extrusion coating; the drying temperature is 80~100℃.

7. A perovskite solar cell, characterized by: The perovskite solar cell comprises, from bottom to top, a transparent conductive substrate, an electron transport layer, a perovskite layer, and a high-entropy alloy composite carbon electrode; the high-entropy alloy composite carbon electrode is prepared by the preparation method described in any one of claims 1 to 6.

8. The perovskite solar cell according to claim 7, characterized in that: The transparent conductive substrate includes any one of FTO glass substrate, ITO glass substrate, and ITO flexible substrate; the electron transport layer includes any one of planar TiO2, planar SnO2, planar ZnO, mesoporous TiO2, dense TiO2, and mesoporous Al2O3.

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