High-efficiency large-area perovskite solar cell and preparation method thereof

Abstract

The present application relates to a kind of high-efficiency large-area perovskite solar cells and preparation method, comprising: transparent conductive substrate, hole blocking layer, mesoporous electron transport layer, mesoporous insulating layer, perovskite light absorption layer, hole transport layer, counter electrode and auxiliary frame.The beneficial effects of the present application are: the present application not only makes perovskite particles uniformly distributed in mesoporous film layer, and forms a layer of independent continuous perovskite light absorption layer between hole transport layer (or counter electrode) and mesoporous insulating layer, solves the problem of area expansion of perovskite solar cell.The preparation method of the present application not only reduces the requirement for process environment condition, but also makes perovskite light absorption layer film confined in interstitial space in situ generation, and this kind of confined space in situ film forming method gets rid of the dependence on large-area film forming equipment, so that the preparation of large-area perovskite film becomes very easy, and it is beneficial to obtain large-area high-efficiency perovskite solar cell.

Description

TECHNICAL FIELD

[0001] The application relates to a solar cell, in particular to a high-efficiency large-area perovskite solar cell and a preparation method thereof, and belongs to the technical field of solar cells. BACKGROUND

[0002] Solar energy is a kind of clean energy that can be taken without exhaustion and used without exhaustion. In recent years, perovskite solar cells have developed rapidly, and great breakthroughs have been made in photoelectric conversion efficiency and stability. The efficiency has increased straightly in a few years, and has broken through 25%. Generally, the perovskite solar cell takes an organic-inorganic hybrid perovskite material as a light absorption layer, and takes an organic small molecule material Spiro-OMeTAD as a hole transport layer. The preparation environment is harsh, and raw materials are expensive, which is not conducive to large-scale commercial production. Replacing the expensive metal electrode with a low-cost carbon electrode is one of the currently feasible alternative solutions. The carbon material has good conductivity and long-term stability, and the perovskite solar cell based on the carbon electrode also shows good stability.

[0003] At present, there are two common structures of the carbon electrode perovskite solar cell. One is to prepare a hole blocking layer, an electron transport layer, an insulating layer and a carbon electrode layer by spin coating or screen printing, and then drop the perovskite solution on the carbon electrode, so that the perovskite solution penetrates into the mesoporous electron transport layer, the insulating layer and the carbon electrode layer. The other is to prepare a hole blocking layer, a mesoporous electron transport layer and a perovskite absorption layer respectively, and then print a carbon electrode layer. In the former, the perovskite grains are filled in the mesoporous electron transport layer, the insulating layer and the carbon electrode layer, and the stability is good, and the requirement for the preparation environment is relatively small. However, since the carbon electrode is usually thick, more perovskite particles are filled in the carbon electrode, and the amount of perovskite material is large. In the latter, the perovskite light absorption layer exists independently between the electron transport layer and the carbon electrode, and there is no perovskite particle remaining in the carbon electrode. However, the disadvantage is that the humidity requirement for the preparation environment is high, and it is difficult to prepare a large-area uniform perovskite film. In order to combine the advantages of the two structures, it is urgent to design a high-efficiency large-area perovskite solar cell and a preparation method thereof. SUMMARY

[0004] The purpose of the present application is to overcome the shortcomings of the prior art, and to provide a high-efficiency large-area perovskite solar cell and a preparation method thereof, so that the perovskite nanoparticles are uniformly distributed in the pores of the mesoporous film layer, the filling uniformity of the perovskite grains in the mesoporous pores is improved, and an independent perovskite light absorption layer is formed, so as to improve the photoelectric conversion efficiency of the perovskite solar cell.

[0005] The high-efficiency large-area perovskite solar cell comprises a transparent conductive substrate, a hole blocking layer, a mesoporous electron transport layer, a mesoporous insulating layer, a perovskite light absorption layer, a hole transport layer, a counter electrode and an auxiliary frame. The perovskite solar cell structure comprises the transparent conductive substrate, the hole blocking layer, the mesoporous electron transport layer, the mesoporous insulating layer, the hole transport layer and the counter electrode from bottom to top. A layer of independent continuous perovskite light absorption layer is formed between the hole transport layer and the mesoporous insulating layer, and perovskite grains are uniformly distributed in each mesoporous film layer (mesoporous electron transport layer and mesoporous insulating layer). The auxiliary frame is arranged at the four peripheral edges of the counter electrode and the interval area adjacent to the counter electrode.

[0006] As preferred, the hole transport layer contains micron or sub-micron flake or dendritic structure, which is beneficial to form an interlayer gap between the hole transport layer and the mesoporous insulating layer, and the perovskite light absorption layer is formed in the interlayer gap. The hole transport layer can be omitted at times, and the perovskite light absorption layer is formed in the gap between the mesoporous insulating layer and the counter electrode.

[0007] As preferred, the thickness of the mesoporous electron transport layer is 0.1 μm-3 μm, and the thickness of the mesoporous insulating layer is 0.1 μm-2 μm.

[0008] As preferred, the counter electrode is a carbon-based counter electrode, which is applied in a carbon-based perovskite solar cell. The carbon-based counter electrode is a film with a through-pore structure and takes carbon material as the main material, which is beneficial to guide the perovskite precursor solution into the mesoporous film layer and uniformly distribute in the pores of the mesoporous film layer. Preferably, the carbon material is at least one of flake graphite, carbon black, carbon fiber, few-layer graphene or carbon nanotube and a dopant thereof. The thickness of the counter electrode is 1 μm-200 μm.

[0009] As preferred, the transparent conductive substrate is composed of a transparent substrate and a transparent conductive film, and the transparent conductive substrate is one of fluorine-doped tin oxide transparent conductive substrate or indium tin oxide transparent conductive substrate.

[0010] As preferred, the hole blocking layer is a metal oxide film, which is preferably at least one of titanium oxide and a dopant thereof, zinc oxide and a dopant thereof, tin oxide and a dopant thereof or tungsten oxide and a dopant thereof. Preferably, the thickness of the hole blocking layer is 30 nm-100 nm.

[0011] As preferred, the chemical composition of the perovskite light absorption layer is ABX3, wherein A is at least one of monovalent cations, specifically CH3NH3 + , NH2-CH=NH2 + , C4H9NH3 + , Cs + , K + or Na + , and B is Pb2+ Sn 2+ Ge 2+ Co 2+ Fe 2+ Mn 2 + Cu 2+ or Ni 2+ X is at least one of Cl - Br - I - or SCN - The thickness of the perovskite light absorption layer is about 50-300 nm.

[0012] As a preferred: the thickness of the auxiliary frame around the four edges of the counter electrode and the adjacent spacing area of the counter electrode is 20-150 μm; the auxiliary frame has a certain adhesion with the transparent conductive substrate, and the two are closely attached without gap; in addition, the auxiliary frame neither falls off automatically nor leaves residue after being removed, and the material thereof includes but is not limited to polyimide, polyethylene, polypropylene or polystyrene.

[0013] The preparation method of the high-efficiency large-area perovskite solar cell comprises the following steps:

[0014] 1) coating the hole blocking layer nanosol on the transparent conductive substrate by spin coating, blade coating or screen printing, the calcination temperature is 400-600 ℃, and the calcination time is 20-60 minutes to obtain the hole blocking layer;

[0015] 2) coating the electronic transport layer nanoslurry with a mass fraction of 5%-20% on the hole blocking layer by spin coating, blade coating or screen printing, the calcination temperature is 400-600 ℃, and the calcination time is 20-60 minutes to obtain the mesoporous electronic transport layer;

[0016] 3) coating the insulating layer nanoslurry with a mass fraction of 5%-20% on the mesoporous electronic transport layer by spin coating, blade coating or screen printing, so that it completely covers the mesoporous electronic transport layer, the calcination temperature is 400-600 ℃, and the calcination time is 20-60 minutes to obtain the mesoporous insulating layer;

[0017] 4) coating the hole transport layer slurry containing micron or submicron flake or dendritic structure with a mass fraction of 5%-20% on the mesoporous insulating layer by spin coating, blade coating or screen printing, the calcination temperature is 400-600 ℃, and the calcination time is 20-60 minutes to obtain the hole transport layer;

[0018] 5) The counter electrode slurry with solid content of 20%~60% is coated on the hole transport layer by means of doctor blading, spin coating or screen printing, the calcination temperature is 350~500℃, and the calcination time is 20~60 minutes, to obtain the counter electrode;

[0019] 6) An auxiliary outer frame is pasted on the substrate coated with the mesoporous membrane layer, along the four peripheral edges of the counter electrode and the interval area adjacent to the counter electrode, and the height of the auxiliary outer frame is greater than the height of the top edge of the counter electrode;

[0020] 7) The perovskite precursor solution is drop-coated or doctor-bladed on the counter electrode by using the drainage function of the counter electrode channel structure, so that the perovskite precursor solution is immersed in the channel of the mesoporous membrane layer and the gap between the mesoporous insulating layer and the hole transport layer, and is annealed at 40~100℃ for 30min~100min.

[0021] As preferred: in step 7), the molar concentration of the perovskite precursor solution is 0.5mol / L~1.5mol / L; after the auxiliary outer frame is added, the dropwise addition amount of the perovskite precursor solution is 1.5μL / cm 2 ~7.5μL / cm 2 .

[0022] The beneficial effects of the present application are:

[0023] 1) The present application not only makes the perovskite particles uniformly distributed in the mesoporous membrane layer, but also forms an independent continuous perovskite light absorption layer between the hole transport layer (or the counter electrode) and the mesoporous insulating layer, solving the problem of area expansion of the perovskite solar cell. The preparation method of the present application not only reduces the requirements for process environmental conditions, but also makes the perovskite light absorption layer film confined in the interlayer gap to generate in situ, which breaks the dependence on large-area film forming equipment, making the preparation of large-area perovskite film very easy, and being conducive to obtaining large-area high-efficiency perovskite solar cells.

[0024] 2) The present application pastes an auxiliary outer frame on the substrate around the mesoporous membrane layer, so that the perovskite precursor solution penetrates more fully in the limited range; at the same time, the dropwise addition amount of the perovskite solution is accurately controlled, the crystallization quality of the perovskite particles and the filling uniformity in the mesoporous channel are improved, so as to improve the photoelectric conversion efficiency of the perovskite solar cell.

[0025] 3) The perovskite solar cell of the present application has low preparation cost, simple preparation process and low requirement for environmental conditions. BRIEF DESCRIPTION OF DRAWINGS

[0026] Figure 1 A schematic diagram of a device prepared by drop-coating perovskite solution without adding an outer frame;

[0027] Figure 2Schematic diagram of device prepared by drop-coating perovskite solution after adding outer frame;

[0028] Figure 3 Schematic diagram of structure profile and auxiliary outer frame of perovskite solar cell module;

[0029] Figure 4 Schematic diagram of structure plane and auxiliary outer frame of perovskite solar cell module;

[0030] Figure 5 Schematic diagram of structure profile and auxiliary outer frame of small-area perovskite solar cell;

[0031] Figure 6 I-V characteristic curve of cell assembled in Example 1 and Comparative Example 1;

[0032] Figure 7 I-V characteristic curve of cell assembled in Example 2 and Comparative Example 2.

[0033] Explanation of reference numerals: 1, transparent substrate; 2, transparent conductive film; 3a, silver lead; 3b, silver lead; 4, etching line; 5, hole blocking layer; 6, mesoporous electron transport layer; 7, mesoporous insulating layer; 8, perovskite light absorption layer; 9, hole transport layer; 10, counter electrode; 11, auxiliary outer frame; 12, perovskite precursor solution. DETAILED DESCRIPTION

[0034] The application will be further described below in conjunction with examples. The following examples are only used to help understand the application. It should be pointed out that for those skilled in the art, some improvements and modifications can be made to the application without departing from the principles of the application, and these improvements and modifications also fall within the scope of protection of the claims of the application.

[0035] An outer frame is pasted on the substrate around the mesoporous film layer of the perovskite solar cell, which provides a confined space for the precursor solution, so that the perovskite precursor solution is uniformly distributed in the mesoporous film layer, especially the filling uniformity of the edge of the mesoporous film is achieved, while avoiding the precursor solution overflowing out of the edge of the mesoporous film layer to cause short circuit, thereby improving the conversion efficiency of the perovskite cell. This method is not only suitable for small-area perovskite solar cells, but also suitable for large-area perovskite solar cells, so that the enlargement of the area of the perovskite film is not affected by the preparation equipment, thereby large-area high-efficiency perovskite solar cells can be prepared.

[0036] Example 1:

[0037] (1) 1.5 cm x 2.2 cm FTO glass is divided into two parts by laser etching as the two poles of the cell. The FTO glass is cleaned with acetone, alkaline, deionized water, and acetone for 10 min, respectively, and then dried by blowing. An appropriate amount of nano-titanium oxide sol is coated on the clean FTO conductive substrate, a film is formed by spin coating, and then sintered in a muffle furnace at 510°C for 30 min to obtain a hole blocking layer 5;

[0038] (2) A nano-titanium oxide slurry with a mass fraction of 7.5% is printed on the hole blocking layer 5 by screen printing to form a titanium oxide film, and then sintered in a muffle furnace at 510°C for 30 min to obtain a mesoporous electron transport layer 6;

[0039] (3) A nano-zirconium oxide slurry with a mass fraction of 15% is printed on the titanium oxide mesoporous layer by screen printing to form a zirconium oxide film, and then sintered in a muffle furnace at 510°C for 30 min to obtain a mesoporous insulating layer 7;

[0040] (4) A nickel oxide slurry with a mass fraction of 10% containing 800 nm flaky nickel oxide and 50 nm nano nickel oxide mixed particles is printed on the mesoporous insulating layer 7 by screen printing to form a nickel oxide film, and then sintered in a muffle furnace at 510°C for 30 min to obtain a hole transport layer 9;

[0041] (5) A carbon slurry is deposited on the hole transport layer 9 by screen printing to form a carbon film, and then sintered in a muffle furnace at 430°C for 30 min to obtain a counter electrode 10;

[0042] (6) A frame with a thickness of 34 μm is attached to the substrate around the mesoporous film layer;

[0043] (7) 2.88 g of PbI2, 0.95 g of MAI, and 0.076 g of 5-AVAI are dissolved in 5 ml of a mixed solvent of ethanol and γ-butyrolactone (Vethanol:Vγ-butyrolactone = 1:4), stirred at 60°C for 6 hours, then 3.5 μL of perovskite solution is dropped on the counter electrode 10, and then annealed at 50°C for 1 h to obtain a perovskite solar cell.

[0044] Example 2:

[0045] (1) 125 cm x 125 cm FTO glass is divided into 8 modules by laser etching for series connection. The FTO glass is cleaned with acetone, alkaline detergent, deionized water, and acetone for 10 min, respectively, and then dried by blowing. An appropriate amount of nano-titanium oxide sol is coated on the clean FTO conductive substrate, a film is formed by screen printing, and then sintered in a muffle furnace at 510°C for 30 min to obtain a hole blocking layer 5;

[0046] (2) The nano-titanium oxide slurry with a mass fraction of 9% is printed on the hole-blocking layer 5 by screen printing to form a titanium oxide film, and then sintered at 510°C for 30 min in a muffle furnace to obtain the mesoporous electron transport layer 6;

[0047] (3) The nano-zirconium oxide slurry with a mass fraction of 13% is printed on the titanium oxide mesoporous layer by screen printing to form a zirconium oxide film, and then sintered at 510°C for 30 min in a muffle furnace to obtain the mesoporous insulating layer 7;

[0048] (4) The nickel oxide slurry with a mass fraction of 10% containing 800 nm flaky nickel oxide and 50 nm nano-nickel oxide mixed particles is printed on the mesoporous insulating layer 7 by screen printing to form a nickel oxide film, and then sintered at 510°C for 30 min in a muffle furnace to obtain the hole transport layer 9;

[0049] (5) The silver slurry is printed on both sides of the transparent conductive substrate by screen printing process to form a film, and then sintered at 510°C for 30 min in a muffle furnace to obtain the silver lead;

[0050] (6) The carbon slurry is deposited on the hole transport layer 9 by screen printing to form a carbon film, and then sintered at 430°C for 30 min in a muffle furnace to obtain the counter electrode 10;

[0051] (7) A frame is attached to the substrate between the two adjacent single cells and around the battery module, and the thickness of the frame is 34 μm;

[0052] (8) 2.88 g of PbI2, 0.95 g of MAI and 0.076 g of 5-AVAI are dissolved in 5 ml of a mixed solvent of ethanol and γ-butyrolactone (Vethanol:Vγ-butyrolactone = 1:4), stirred at 60°C for 6 hours, and then 16.5 μL of the solution is dropped on the counter electrode 10. After annealing at 50°C for 1 h, a perovskite solar cell is obtained.

[0053] Comparative Example 1:

[0054] (1) The FTO glass with a size of 1.5 cm x 2.2 cm is divided into two parts by laser etching as the two poles of the cell. The FTO glass is ultrasonically cleaned with acetone, lye, deionized water and acetone for 10 min, and then dried by blowing. An appropriate amount of nano-titanium oxide sol is coated on the clean FTO conductive substrate, a film is formed by spin coating, and then sintered at 510°C for 30 min in a muffle furnace to obtain the hole-blocking layer 5;

[0055] (2) The nano-titanium oxide slurry with a mass fraction of 7.5% is printed on the hole-blocking layer 5 by screen printing to form a titanium oxide film, and then sintered at 510°C for 30 min in a muffle furnace to obtain the mesoporous electron transport layer 6;

[0056] (3) The zirconium oxide slurry with a mass fraction of 15% is printed on the titanium oxide mesoporous layer by screen printing to form a zirconium oxide film, and then sintered at 510°C for 30 min in a muffle furnace to obtain the mesoporous insulating layer 7;

[0057] (4) The nickel oxide slurry with a mass fraction of 10% containing mixed particles of 800 nm flaky nickel oxide and 50 nm nano nickel oxide is printed on the mesoporous insulating layer 7 by screen printing to form a nickel oxide film, and then sintered at 510°C for 30 min in a muffle furnace to obtain the hole transport layer 9;

[0058] (5) The carbon slurry is deposited on the hole transport layer 9 by screen printing to form a carbon film, and then sintered at 430°C for 30 min in a muffle furnace to obtain the counter electrode 10;

[0059] (6) 2.88 g of PbI2, 0.95 g of MAI and 0.076 g of 5-AVAI are dissolved in 5 ml of a mixed solvent of ethanol and γ-butyrolactone (Vethanol:Vγ-butyrolactone = 1:4), stirred at 60°C for 6 hours, and then 3.5 μL of perovskite solution is dropped on the counter electrode 10, and after annealing at 50°C for 1 h, a perovskite solar cell is obtained.

[0060] Comparative Example 2:

[0061] (1) The FTO glass with a size of 125 cm x 125 cm is divided into 8 modules connected in series by laser etching. The FTO glass is cleaned with acetone, alkali, deionized water and acetone ultrasonic cleaning for 10 min, and then dried. An appropriate amount of titanium oxide sol is used to form a film on the FTO by screen printing, and then sintered at 510°C for 30 min in a muffle furnace to obtain the TiO2 hole blocking layer;

[0062] (2) The nano titanium oxide slurry with a mass fraction of 9% is printed on the hole blocking layer 5 by screen printing to form a titanium oxide film, and then sintered at 510°C for 30 min in a muffle furnace to obtain the mesoporous electron transport layer 6;

[0063] (3) The nano zirconium oxide slurry with a mass fraction of 13% is printed on the mesoporous electron transport layer 6 by screen printing to form a zirconium oxide film, and then sintered at 510°C for 30 min in a muffle furnace to obtain the mesoporous insulating layer 7;

[0064] (4) The nickel oxide slurry with a mass fraction of 10% containing mixed particles of 800 nm flaky nickel oxide and 50 nm nano nickel oxide is printed on the mesoporous insulating layer 7 by screen printing to form a nickel oxide film, and then sintered at 510°C for 30 min in a muffle furnace to obtain the hole transport layer 9;

[0065] (5) The silver paste was screen-printed on both sides of the transparent conductive substrate to form a thin film, and then sintered in a muffle furnace at 510°C for 30 min to obtain the silver lead;

[0066] (6) The carbon paste was screen-printed on the hole transport layer 9 to form a mesoporous carbon thin film, and then sintered in a muffle furnace at 430°C for 30 min to obtain the counter electrode 10;

[0067] (7) 2.88 g of PbI2, 0.975 g of MAI and 0.076 g of 5-AVAI were dissolved in 5 mL of a mixed solvent of ethanol and γ-butyrolactone (Vethanol:Vγ-butyrolactone = 1:4), stirred at 60°C for 6 hours, and then 16.5 μL of the solution was dropped on the counter electrode 10 of the single cell, and after annealing at 50°C for 1 h, a perovskite solar cell was obtained.

[0068] The following table shows the photoelectric conversion parameters of perovskite solar cells with different carbon electrodes.

[0069] Table 1 Photoelectric conversion parameters of perovskite solar cells with different carbon electrodes

[0070]

Claims

1. A high-efficiency, large-area perovskite solar cell, characterized in that: The perovskite solar cell structure comprises a transparent conductive substrate, a hole blocking layer (5), a mesoporous electron transport layer (6), a mesoporous insulating layer (7), a perovskite light absorption layer (8), a hole transport layer (9), a counter electrode (10), and an auxiliary frame (11). From bottom to top, the perovskite solar cell structure comprises a transparent conductive substrate, a hole blocking layer (5), a mesoporous electron transport layer (6), a mesoporous insulating layer (7), a hole transport layer (9), and a counter electrode (10). An independent and continuous perovskite light absorption layer (8) is formed between the hole transport layer (9) and the mesoporous insulating layer (7), and perovskite grains are uniformly distributed in each mesoporous film layer. An auxiliary frame (11) is provided around the periphery of the counter electrode (10) and in the space between adjacent counter electrodes. The hole transport layer (9) contains micron or submicron scale sheet-like or dendritic structures; The thickness of the mesoporous electron transport layer (6) is 0.1 μm to 3 μm; the thickness of the mesoporous insulating layer (7) is 0.1 μm to 2 μm; The counter electrode (10) is a carbon-based counter electrode, which is a thin film with a through-hole structure and carbon material as the main material; the carbon material is at least one of sheet graphite, carbon black, carbon fiber, few-layer graphene or carbon nanotubes and their dopants; the thickness of the counter electrode (10) is 1 μm to 200 μm. The thickness of the auxiliary frame (11) is 20μm to 150μm; the auxiliary frame (11) is tightly bonded to the transparent conductive substrate; the material of the auxiliary frame (11) includes polyimide, polyethylene, polypropylene or polystyrene.

2. The high-efficiency large-area perovskite solar cell according to claim 1, characterized in that: The transparent conductive substrate is composed of a transparent substrate (1) and a transparent conductive film (2). The transparent conductive substrate is either a fluorine-containing tin oxide transparent conductive substrate or an indium tin oxide transparent conductive substrate.

3. The high-efficiency large-area perovskite solar cell according to claim 1, characterized in that: The hole blocking layer (5) is a metal oxide film, specifically at least one of titanium oxide and its dopants, zinc oxide and its dopants, tin oxide and its dopants, or tungsten oxide and its dopants; the thickness of the hole blocking layer (5) is 30nm to 100nm.

4. The high-efficiency large-area perovskite solar cell according to claim 1, characterized in that: The chemical composition of the perovskite light-absorbing layer (8) is ABX3, where A is a monovalent cation and A is CH3NH3. + NH2-CH=NH2 + C4H9NH3 + Cs + K + Or Na + At least one of them, B is Pb 2+ Sn 2+ 、Ge 2+ Co 2+ Fe 2+ Mn 2+ Cu 2+ or Ni 2+ At least one of them, X is Cl - ,Br - I - or SCN - At least one of the following; the thickness of the perovskite light-absorbing layer (8) is 50 nm to 300 nm.

5. A method for fabricating a high-efficiency large-area perovskite solar cell as described in claim 1, characterized in that, Includes the following steps: 1) The hole blocking layer nanosol is coated onto a transparent conductive substrate by spin coating, scraping or screen printing. The calcination temperature is 400-600℃ and the calcination time is 20-60 minutes to obtain the hole blocking layer (5). 2) Electron transport layer nano-slurry with a mass fraction of 5% to 20% is coated onto hole blocking layer (5) by spin coating, scraping or screen printing. The calcination temperature is 400 to 600°C and the calcination time is 20 to 60 minutes to obtain mesoporous electron transport layer (6). 3) Apply 5% to 20% of insulating layer nano paste by spin coating, scraping or screen printing onto the mesoporous electron transport layer (6) to completely cover the mesoporous electron transport layer (6). The calcination temperature is 400 to 600°C and the calcination time is 20 to 60 minutes to obtain the mesoporous insulating layer (7). 4) A hole transport layer slurry containing micron or submicron scale sheet-like or dendritic structures with a mass fraction of 5% to 20% is coated onto a mesoporous insulating layer (7) by spin coating, scraping or screen printing. The calcination temperature is 400 to 600℃ and the calcination time is 20 to 60 minutes to obtain a hole transport layer (9). 5) A counter electrode slurry with a solid content of 20% to 60% is coated onto the hole transport layer (9) by scraping, spin coating or screen printing. The calcination temperature is 350 to 500°C and the calcination time is 20 to 60 minutes to obtain the counter electrode (10). 6) On the substrate coated with the mesoporous membrane layer, an auxiliary frame (11) is attached along the periphery of the counter electrode (10) and the interval between adjacent counter electrodes. The height of the auxiliary frame (11) is greater than the height of the top edge of the counter electrode (10). 7) Using the drainage of the electrode channel structure, drop or scrape the perovskite precursor liquid (12) above the electrode (10) so that it can be immersed in the channels of the mesoporous film layer and the gap between the mesoporous insulating layer (7) and the hole transport layer (9), and anneal at 40 to 100°C for 30 to 100 minutes.

6. The method for fabricating a high-efficiency large-area perovskite solar cell according to claim 5, characterized in that: In step 7), the molar concentration of the perovskite precursor solution (12) is 0.5 mol / L to 1.5 mol / L; the dropping volume of the perovskite precursor solution (12) is 1.5 μL / cm. 2 ~7.5μL / cm 2 .

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