Trans-perovskite cell with low-dimensional perovskite buried interface and high fill factor and preparation method thereof

By using a 4-(aminomethyl)benzenesulfonamide acetate modification layer in inverted perovskite solar cells, the interface matching between the perovskite layer and the hole transport layer was improved, solving the problems of interface defects and stress release, increasing the fill factor and photoelectric conversion efficiency, and enhancing the stability of the device.

CN121285232APending Publication Date: 2026-01-06CHENGDU UNIVERSITY OF TECHNOLOGY
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Patent Information

Application Number
CN202511347542.0
Authority / Receiving Office
CN · China
Patent Type
Applications(China)
Current Assignee / Owner
Filing Date
2025-09-19
Publication Date
2026-01-06

AI Technical Summary

Technical Problem

In inverted perovskite solar cells, when Me-4PACz is used as a hole transport layer, the interaction between it and the perovskite layer is weak, which leads to the inability to passivate interface defects, insufficient stress release, and severe loss of fill factor FF, thus affecting device efficiency and stability.

Method used

4-(aminomethyl)benzenesulfonamide acetate (4B) was used as the modification layer solution to form a low-dimensional perovskite buried interface on the hole transport layer by spin coating. The modification layer solution consisted of 4B and solvent and was used to improve the interface matching between the perovskite layer and the hole transport layer, and enhance the interface bonding and stability.

Benefits of technology

This improves the stability and hole transport efficiency of perovskite thin films, enhances the fill factor (FF) and photoelectric conversion efficiency of devices, and strengthens the long-term stability of devices.

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Abstract

The invention discloses a trans-perovskite cell with a low-dimensional perovskite buried interface and a high fill factor and a preparation method of the trans-perovskite cell, and belongs to the technical field of trans-perovskite. 4-(aminomethyl) benzenesulfonamide acetate (4B) is used as an interface modification layer between the hole transport layer and the perovskite layer, 4B molecules can improve the surface contact potential difference of the hole transport layer and improve the hole extraction efficiency,-NH2 in the 4B molecules can passivate under-coordinated Pb < 2 + > at a perovskite buried interface, the quality of the perovskite thin film is improved, and the perovskite thin film can be applied to the field of solar cell devices. Furthermore, the acetate can be coordinated with [PbI6] < 4-> at the bottom of the perovskite, so that molecules enter perovskite crystal lattices, and 2D perovskite is formed at the bottom burying interface of the perovskite. By introducing the 4B material into the perovskite cell, the final stability of the device is improved, and the device achieves a high fill factor of 86.65% and a photoelectric conversion efficiency of 26.62%.
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Description

Technical Field

[0001] This invention belongs to the field of perovskite solar cell technology, specifically relating to an inverted perovskite solar cell with a low-dimensional perovskite buried interface and a high fill factor, and its preparation method. Background Technology

[0002] Currently, the world faces severe challenges from energy shortages and the greenhouse effect. Solar energy, with its wide irradiance, high energy output, and pollution-free nature, is a primary resource for achieving this transformation. Solar cells represent the optimal means of utilizing solar energy, directly converting light energy into electrical energy, and have enormous development potential. Among various solar cells, inverted perovskite solar cells have emerged due to their high efficiency, low cost, and compatibility. After more than a decade of development, the efficiency of a single-cell inverted perovskite solar cell can reach 27.3%.

[0003] While inverted perovskite solar cells are developing rapidly, they also face the challenge of further improving efficiency and stability. Inverted perovskite solar cells typically use the organic self-assembled material [4-(3,6-dimethyl-9H-carbazole-9-yl)butyl]phosphonic acid Me-4PACz as the hole transport layer, but the perovskite layer and Me-4PACz have the following problems: (1) The interaction between the top carbazole group of Me-4PACz and the perovskite precursor components is weak, which makes it impossible to passivate the interface defects between the perovskite layer and the hole transport layer, and to alleviate the stress release at the perovskite buried interface, resulting in a decrease in device efficiency.

[0004] (2) The surface contact potential difference of Me-4PACz is relatively high, which is not conducive to hole transport, resulting in increased loss of fill factor FF and seriously affecting device efficiency.

[0005] (3) The 3D perovskite formed at the buried interface has poor stability, which leads to a decrease in device stability. Summary of the Invention

[0006] The purpose of this invention is to overcome the shortcomings of the prior art and provide an inverted perovskite solar cell with a low-dimensional perovskite buried interface and a high fill factor, as well as its preparation method, to solve the problem that when Me-4PACz is used as a hole transport layer in the prior art, it is difficult to achieve a complete match with the perovskite layer, which leads to a decrease in device performance.

[0007] To achieve the above objectives, the present invention employs the following technical solution: A method for preparing an inverted perovskite solar cell with a low-dimensional perovskite buried interface and a high fill factor includes the following steps: S1, Prepare a MgF2 antireflection layer on the back side of FTO; S2, a hole transport layer is prepared on the front side of the FTO, the hole transport layer comprising a NiOx layer and a Me-4PACz layer; S3, A modification layer is prepared on the hole transport layer by spin coating. The modification layer is obtained by spin coating a modification layer solution onto the hole transport layer. The modification layer solution is composed of 4-(aminomethyl)benzenesulfonamide acetate and a solvent. S4, Prepare FA on the modified layer 0.9 Cs 0.05 MA 0.05 PbI3 perovskite light-absorbing layer; S5, in FA 0.9 Cs 0.05 MA 0.05 An electron transport layer, a hole blocking layer, and a metal electrode are sequentially fabricated on a PbI3 perovskite light-absorbing layer.

[0008] A further improvement of the present invention is that: Preferably, in S3, the concentration of the modified layer solution is 1-5 mg / mL.

[0009] Preferably, in S3, the spin coating speed is 5000 rpm and the spin coating time is 30 s.

[0010] Preferably, in S3, the solvent is any one of N,N-dimethylformamide, IPA, or anhydrous ethanol.

[0011] Preferably, the NiOx layer is prepared by spin-coating a NiOx dispersion onto a hole transport layer, wherein the concentration of the NiOx dispersion is 10 mg / mL, the solute of the NiOx dispersion is NiOx powder, and the solvent is deionized water.

[0012] Preferably, the Me-4PACz layer is obtained by spin-coating a Me-4PACz solution onto the surface of a NiOx layer, wherein the solute of the Me-4PACz solution is Me-4PACz powder and the solvent is anhydrous ethanol.

[0013] Preferably, the electron transport layer is C 60 .

[0014] Preferably, the hole blocking layer is a BCP.

[0015] Preferably, the metal electrode is Ag.

[0016] An inverted perovskite solar cell with a low-dimensional perovskite buried interface and a high fill factor, prepared by any of the above methods, comprises, from one side to the other, a MgF2 antireflection layer, an FTO layer, a NiOx layer, a Me-4PACz layer, a 4-(aminomethyl)benzenesulfonamide acetate modification layer, a perovskite light-absorbing layer, an electron transport layer, a hole-blocking layer, and a metal electrode.

[0017] Compared with the prior art, the present invention has the following beneficial effects: This invention develops a method for constructing a low-dimensional perovskite phase buried interface and preparing a high-fill-factor inverted perovskite solar cell. 4-(aminomethyl)benzenesulfonamide acetate (4B) is a multifunctional small organic molecule containing -NH2, acetate Ac-, and an organic macromolecular backbone (benzenesulfonic acid). For the first time, 4B is used to modify the hole transport layer and perovskite layer interface of an inverted perovskite solar cell. (1) The -NH2 in 4B can passivate the undercoordinated Pb on the buried perovskite surface. 2+ Defects induce perovskite nucleation and crystallization, releasing residual stress at the perovskite buried interface, which helps to obtain higher quality perovskite films; (2) Acetate Ac- in 4B reacts with [PbI6] in the perovskite 4- It has stronger binding force and can break down [PbI6] 4- The structure makes it easier for the main body of 4B to enter the perovskite lattice, forming a 2D perovskite at the buried interface of the perovskite, which improves the stability of the perovskite film. In addition, the acetate group in 4B provides an acidic environment, making Me-4PACz at the lower interface more stable in an acidic environment. (3) The hole transport layer modified by 4B has a smoother surface roughness and a more negative surface contact potential difference under the combined action of the organic macromolecular framework benzenesulfonic acid and -NH2, which optimizes the interface contact and is conducive to the extraction of holes from the perovskite layer to the hole transport layer, thereby improving the fill factor FF of the device. Attached Figure Description

[0018] Figure 1 This is a schematic diagram of the device structure of the FAMACsPbI3 perovskite solar cell in Embodiment 1 of the present invention. From top to bottom, they are: MgF2 layer, NiO... x Layer, SAM layer, lower interface modification layer, perovskite layer, upper surface passivation layer, electron transport layer, hole blocking layer, metal electrode; Figure 2 This is a GIWAXS image of the perovskite thin film modified with 4B material in Example 1 of the present invention; Figure 3 This is a SEM image of the bottom of the perovskite film modified with 4B material in Example 1 of the present invention. Figure 4 This is the GIXRD pattern of the perovskite thin film modified with 4B material in Example 1 of the present invention; Figure 5 This is a KPFM diagram of the hole transport layer modified with 4B material in Embodiment 1 of the present invention. Figure 6 The 4B-modified and unmodified perovskite solar cells in Example 1 of this invention JV curve; Figure 7 This is a stability test of the 4B-modified and unmodified perovskite solar cells in Example 1 of the present invention. Detailed Implementation

[0019] The present invention will now be described in further detail with reference to the accompanying drawings: To enable those skilled in the art to understand the features and effects of the present invention, the terms and expressions used in the specification and claims are explained and defined in general below. Unless otherwise specified, all technical and scientific terms used herein have the ordinary meaning understood by those skilled in the art regarding the present invention, and in case of conflict, the definitions in this specification shall prevail.

[0020] In this article, unless otherwise specified, “contains,” “includes,” “containing,” “has,” or similar terms cover the meanings of “composed of” and “mainly composed of,” for example, “A contains a” covers the meanings of “A contains a and others” and “A contains only a.”

[0021] The present invention will be further illustrated below with reference to specific embodiments. It should be understood that these embodiments are for illustrative purposes only and are not intended to limit the scope of the invention. Furthermore, it should be understood that after reading the teachings of this invention, those skilled in the art can make various alterations or modifications to the invention, and these equivalent forms also fall within the scope defined by the appended claims.

[0022] The following examples use instruments and equipment conventional in the art. Experimental methods in the following examples, unless otherwise specified, are generally performed under conventional conditions or as recommended by the manufacturer. All raw materials used in the following examples are conventional commercially available products with specifications conventional in the art. In this specification and the following examples, unless otherwise specified, "%" refers to weight percentage, "parts" refers to parts by weight, and "ratio" refers to weight proportion.

[0023] The first aspect of this invention discloses a method for constructing a low-dimensional perovskite phase buried interface and preparing a high-fill-factor inverse perovskite solar cell, comprising the following steps: Step 1: Preparation of FTO glass and magnesium fluoride (MgF2) antireflection layer; The FTO glass was ultrasonically cleaned with conductive glass cleaning solution, acetone, and ethanol, and then dried with a nitrogen gas gun. The cleaned FTO conductive glass was placed in a vacuum evaporation apparatus, and a 110 nm thick MgF2 antireflection layer was deposited on the back of the FTO at a rate of 0.3 Å / s. After the deposition was completed, the glass was stored in anhydrous ethanol.

[0024] Step 2, Preparation method of NiOx and SAM; Add 1 mL of deionized water to a glass bottle containing 10 mg of NiOx powder (nickel oxide nanoparticles) to prepare a 10 mg / mL NiOx dispersion. Place the glass bottle in an ultrasonic cleaner and sonicate for 40 minutes to ensure the NiOx powder is fully dispersed in the deionized water. Treat the FTO glass cleaned in step 1 with ultraviolet ozone for 15 min. Spin-coat the 10 mg / mL NiOx dispersion onto the FTO glass surface at a spin speed of 2000 rpm (acceleration of 1000 rpm / s) for 30 s. Then anneal on a constant temperature hot plate at 150 °C for 10 min. 1 mg of [4-(3,6-dimethoxy-9H-carbazole-9-yl)butyl]phosphonic acid Me-4PACz solid powder was dissolved in 2 mL of anhydrous ethanol to obtain a Me-4PACz solution with a concentration of 0.5 mg / mL. The solution was stirred for 3 h and then set aside. The solution was then spin-coated onto the surface of a NiOx layer at a spin speed of 4000 rpm for 30 s. Annealing was then performed at a temperature of 100 ℃ for 10 min. After annealing, unbound molecules were removed by rinsing with ethanol to obtain the NiOx and Me-4PACz layers.

[0025] It should be noted that the common range of x in NiOx is 0.8–1.3, and in practical applications it is mostly 1.0–1.2. Variations in the x value represent oxygen vacancies or high-valence Ni (such as Ni...). 3+ The introduction of ) affects its electrical properties and interface behavior.

[0026] Step 3: Prepare the modification layer solution; The method for preparing the modified layer solution is as follows: Dissolve 4B (4-(aminomethyl)benzenesulfonamide acetate) solid powder in a solvent with a concentration of 1-5 mg / mL. The solvent is... N,N The modified layer solution is prepared by stirring in any one of the following solvents: dimethylformamide (DMF), IPA, or anhydrous ethanol for 4 hours; the chemical structural formula of 4B is:

[0027] Step 4, Prepare the modification layer: The 1 mg / mL 4B modification solution prepared in step 3 was spin-coated onto the NiOx / Me-4PACz surface at a spin-coating speed of 5000 rpm for 30 s to obtain the modification layer.

[0028] In this step, if the concentration of the 1 mg / mL modified layer solution is too low, it can only passivate defects and cannot form a low-dimensional phase at the buried interface. By limiting the appropriate concentration, without annealing, 4B can both passivate the buried interface defects and enter the perovskite lattice to form a low-dimensional phase.

[0029] Step 5, prepare FA 0.9 Cs 0.05 MA 0.05 PbI3 perovskite precursor solution FA preparation 0.9 Cs 0.05 MA 0.05 The process for preparing the PbI3 perovskite precursor solution was as follows: 232.16 mg of formamidinium hydroiodate (FAI), 11.92 mg of methylamine hydroiodate (MAI), 19.48 mg of cesium iodide (CsI), and 691.51 mg of lead iodide (PbI2) were dissolved in a mixed solvent of DMF and DMSO (V / V = 4:1) to prepare a 1.5 M FA solution. 0.9 Cs 0.05 MA 0.05 PbI3 perovskite precursor solution: The perovskite precursor solution was stirred for 6 h and then filtered using a 0.45 μm syringe for later use.

[0030] In the above process, the perovskite precursor solution is directly spin-coated onto the modified layer, which improves the wettability of the perovskite and the modified interface. Furthermore, without annealing, the anchoring force between the 4B modified layer and the underlying layer is relatively weak, allowing it to penetrate into the perovskite during the spin-coating process and thus form a low-dimensional phase.

[0031] Step 6: Prepare the perovskite light-absorbing layer (PVK). The perovskite precursor solution prepared in step 5 was spin-coated onto the surface of the 4B modified layer. The spin-coating process consisted of two stages: in the first stage, the spin speed was 1000 rpm for 10 s; in the second stage, the spin speed was 5000 rpm for 30 s. Five seconds before the end of the spin-coating process, 120 μL of the anti-solvent anisole was applied to the perovskite surface, followed by an annealing process at 110℃ for 20 min. After annealing, FTO / NiOx / Me-4PACz / 4B / PVK was obtained. The prepared perovskite light-absorbing layer was approximately 500 nm in size.

[0032] Step 7: Prepare the electron transport layer; The perovskite film prepared in step 6 has a C layer with a thickness of approximately 20 nm deposited on its surface. 60 As an electron transport layer, FTO / NiOx / Me-4PACz / 4B / PVK / C was fabricated. 60 .

[0033] Step 8: Prepare the hole blocking layer; C obtained in step 7 60 A BCP (bath copper alloy) layer with a thickness of approximately 6 nm was deposited on the surface as a hole-blocking layer to prepare FTO / NiOx / Me-4PACz / 4B / PVK / C. 60 / BCP.

[0034] Step 9: Prepare the metal electrode; In step 8, a silver electrode with a thickness of approximately 110 nm is deposited on the surface of the hole-blocking layer to obtain the final structure FTO / NiOx / Me-4PACz / 4B / PVK / C. 60 FACsMAPbI3 perovskite solar cells with / BCP / Ag.

[0035] The following description, in conjunction with specific embodiments, provides further details.

[0036] Example 1 Step 1, Preparation of FTO glass and magnesium fluoride (MgF2) antireflective layer; [The text abruptly ends here, likely due to an incomplete sentence or missing information.] 2 The FTO glass was ultrasonically cleaned with conductive glass cleaning solution, acetone, and ethanol, and then dried with a nitrogen gas gun. The cleaned FTO conductive glass was placed in a vacuum evaporation apparatus, and a 110 nm thick MgF2 antireflection layer was deposited on the back of the FTO at a rate of 0.3 Å / s. After the deposition was completed, the glass was stored in anhydrous ethanol.

[0037] Step 2: Add 1 mL of deionized water to a glass bottle containing 10 mg of NiOx powder to prepare a 10 mg / mL NiOx dispersion. Place the glass bottle in an ultrasonic cleaner and sonicate for 40 minutes to ensure the NiOx powder is fully dispersed in the deionized water for later use. Treat the FTO glass cleaned in Step 1 with ultraviolet ozone for 15 min. Spin-coat the 10 mg / mL NiOx dispersion onto the FTO glass surface at a spin speed of 2000 rpm (acceleration of 1000 rpm / s) for 30 s. Then, anneal the glass on a constant temperature hot plate at 150 °C for 10 min. 1 mg of [4-(3,6-dimethoxy-9H-carbazole-9-yl)butyl]phosphonic acid Me-4PACz solid powder was dissolved in 2 mL of anhydrous ethanol to prepare a 0.5 mg / mL solution. The solution was stirred for 3 h and then set aside. The solution was then spin-coated onto the surface of NiOx at a speed of 4000 rpm for 30 s. Annealing was then performed at a temperature of 100 °C for 10 min. After annealing, unbound molecules were removed by rinsing with ethanol to obtain a NiOx and Me-4PACz layer.

[0038] Step 3: Prepare the 4B modified layer DMF solution. The 4B modified layer solution is prepared by dissolving 2 mg of 4B solid powder in 1 mL of DMF and stirring for 4 h.

[0039] Step 4: Prepare the 4B modification layer; spin-coat the 2 mg / mL 4B DMF solution prepared in Step 3 onto the NiOx / Me-4PACz surface at a spin-coating speed of 5000 rpm for 30 s, without annealing.

[0040] Step 5, prepare 1.5 M FA 0.9 Cs 0.05 MA 0.05 The PbI3 perovskite precursor solution was prepared by dissolving formamidinium hydroiodide (FAI), CsI, MAI, and PbI2 in a stoichiometric ratio in a mixed solvent of DMF and DMSO (V / V = 4:1), stirring at room temperature for 6 h, and then filtering using a 0.45 μm syringe for later use.

[0041] Step 6: Prepare the perovskite absorbing layer (PVK). The perovskite precursor solution prepared in Step 5 is spin-coated onto the surface of the 4B modified layer. The spin-coating process consists of two stages: the first stage uses a spin speed of 1000 rpm for 8 s; the second stage uses a spin speed of 4000 rpm for 25 s. Five seconds before the end of the spin-coating, the antisolvent anisole is applied to the perovskite surface, followed by annealing at 110 ℃ for 20 min. After annealing, FTO / NiOx / Me-4PACz / 4B / PVK is formed. The prepared perovskite absorbing layer is approximately 500 nm in size.

[0042] Step 7: Prepare the electron transport layer; The perovskite film prepared in step 6 has a C layer with a thickness of approximately 20 nm deposited on its surface. 60 As an electron transport layer, FTO / NiOx / Me-4PACz / 4B / PVK / C was fabricated. 60 .

[0043] Step 8: Prepare the hole blocking layer; C obtained in step 7 60 A BCP (bath copper alloy) layer with a thickness of approximately 6 nm was deposited on the surface as a hole-blocking layer to prepare FTO / NiOx / Me-4PACz / 4B / PVK / C. 60 / BCP.

[0044] Step 9: Prepare the metal electrode; In step 8, a silver electrode with a thickness of approximately 110 nm is deposited on the surface of the hole-blocking layer to obtain the final structure FTO / NiOx / Me-4PACz / 4B / PVK / C. 60 FACsMAPbI3 perovskite solar cells with / BCP / Ag.

[0045] In this embodiment, a perovskite solar cell with a 2 mg / mL lower interface modification layer 4B was prepared.

[0046] Comparative Example 1 differs from Example 1 only in steps 3 and 4. In Comparative Example 1, a 4B DMF solution was not prepared in step 3, and a 4B modification layer was not spin-coated in step 4. All other steps and parameters are the same.

[0047] like Figure 1 The device structure of the FAMACsPbI3 perovskite solar cell shown, from bottom to top, consists of a MgF2 antireflection layer, a NiOx layer, a Me-4PACz layer, a lower interface modification layer 4B, a perovskite light-absorbing layer, and an electron transport layer C. 60 Hole blocking layer (BCP) and metal electrode (Ag).

[0048] like Figure 2 As shown in the GIWAXS test images of 4B-modified and unmodified perovskite films, it can be seen that the 4B-modified perovskite film exhibits... q z = 1.0 Å -1 The presence of sharp and discrete Bragg points indicates a high degree of crystal orientation along the (001) direction, confirming the orientation-regulating effect of 4B modification on the growth of the perovskite film. Furthermore, compared to the control film, the 4B-modified perovskite film exhibits higher GIWAXS spectra in the 4B-modified perovskite film due to the interaction between 4B and the perovskite. q z = 0.4 Å -1 and 0.7 Å -1 The presence of a distinct diffraction peak indicates that the acetate group in the 4B material disrupts the [PbI6] morphology of the 3D perovskite. 4- The resulting 2D perovskite is beneficial for improving the stability of perovskite films.

[0049] like Figure 3 As shown in the SEM images of the bottom of the 4B-modified and unmodified perovskite films, it can be seen that the bottom of the 4B-modified perovskite is more uniform and dense, and the grain size is also larger, which enables the device to absorb light energy more fully.

[0050] like Figure 4 As shown, the GIXRD test patterns of the 4B-modified and unmodified perovskite films at the lower interface are shown. 4B can induce perovskite nucleation and crystallization, and the -NH2 in 4B interacts with the lead iodide at the bottom of the perovskite, causing the bottom lattice to shrink, thereby releasing the residual stress at the buried interface of the perovskite.

[0051] like Figure 5 As shown, KPFM tests were performed on the hole transport layer with and without 4B modification. 4B modification significantly reduced the surface contact potential difference of the hole transport layer. The lower surface contact potential difference is conducive to hole transport, reduces nonradiative recombination at the interface, improves the fill factor of the device, and thus improves the photoelectric conversion efficiency.

[0052] like Figure 6 Perovskite solar cells with modified and unmodified interfaces. JV The curves and specific parameters are shown in Table 1. The open-circuit voltage and fill factor of the perovskite solar cell improved after the lower interface modification. The modified perovskite solar cell achieved a high fill factor of 86.65%, and the photoelectric conversion efficiency increased from 24.80% to 26.62%.

[0053] Table 1 Performance Comparison of Comparative Example and Example 1

[0054] like Figure 7 As shown, the stability of the modified film was tested. After 1250 h of operation under air conditions, the 4B-modified battery device maintained 93.98% of its initial efficiency, which is higher than that of the unmodified device.

[0055] Example 2 Step 1, Preparation of FTO glass and magnesium fluoride (MgF2) antireflective layer; [The text abruptly ends here, likely due to an incomplete sentence or missing information.] 2 The FTO glass was ultrasonically cleaned with conductive glass cleaning solution, acetone, and ethanol, and then dried with a nitrogen gas gun. The cleaned FTO conductive glass was placed in a vacuum evaporation apparatus, and a 110 nm thick MgF2 antireflection layer was deposited on the back of the FTO at a rate of 0.3 Å / s. After the deposition was completed, the glass was stored in anhydrous ethanol.

[0056] Step 2: Add 1 mL of deionized water to a glass bottle containing 10 mg of NiOx powder to prepare a 10 mg / mL NiOx dispersion. Place the glass bottle in an ultrasonic cleaner and sonicate for 40 minutes to ensure the NiOx powder is fully dispersed in the deionized water for later use. Treat the FTO glass cleaned in Step 1 with ultraviolet ozone for 15 min. Spin-coat the 10 mg / mL NiOx dispersion onto the FTO glass surface at a spin speed of 2000 rpm (acceleration of 1000 rpm / s) for 30 s. Then, anneal the glass on a constant temperature hot plate at 150 °C for 10 min. 1 mg of Me-4PACz solid powder was dissolved in 2 mL of anhydrous ethanol at a concentration of 0.5 mg / mL and stirred for 3 h. The solution was then spin-coated onto the surface of NiOx at a speed of 4000 rpm for 30 s. Annealing was then performed at 100 °C for 10 min. After annealing, unbound molecules were removed by rinsing with ethanol to obtain the NiOx and Me-4PACz layers.

[0057] Step 3: Prepare the 4B modified layer DMF solution. The 4B modified layer solution is prepared by dissolving 10 mg of 4B solid powder in 2 mL of DMF and stirring for 4 h.

[0058] Step 4: Prepare the 4B modified layer; spin-coat the 5 mg / mL 4B DMF solution prepared in Step 3 onto the NiOx / Me-4PACz surface at a spin-coating speed of 5000 rpm for 30 s, and then anneal for 10 min.

[0059] Step 5, prepare 1.5 M FA 0.9 Cs 0.05 MA 0.05The PbI3 perovskite precursor solution was prepared by dissolving formamidinium hydroiodide (FAI), CsI, MAI, and PbI2 in a stoichiometric ratio in a mixed solvent of DMF and DMSO (V / V = 4:1), stirring at room temperature for 6 h, and then filtering using a 0.45 μm syringe for later use.

[0060] Step 6: Prepare the perovskite absorbing layer (PVK). The perovskite precursor solution prepared in Step 5 is spin-coated onto the surface of the 4B modified layer. The spin-coating process consists of two stages: the first stage uses a spin speed of 1000 rpm for 8 s; the second stage uses a spin speed of 4000 rpm for 25 s. Five seconds before the end of the spin-coating, the antisolvent anisole is applied to the perovskite surface, followed by annealing at 110 ℃ for 20 min. After annealing, FTO / NiOx / Me-4PACz / 4B / PVK is formed. The prepared perovskite absorbing layer is approximately 500 nm in size.

[0061] Step 7: Prepare the electron transport layer; The perovskite film prepared in step 6 has a C layer with a thickness of approximately 20 nm deposited on its surface. 60 As an electron transport layer, FTO / NiOx / Me-4PACz / 4B / PVK / C was fabricated. 60 .

[0062] Step 8: Prepare the hole blocking layer; C obtained in step 7 60 A BCP (bath copper alloy) layer with a thickness of approximately 6 nm was deposited on the surface as a hole-blocking layer to prepare FTO / NiOx / Me-4PACz / 4B / PVK / C. 60 / BCP.

[0063] Step 9: Prepare the metal electrode; In step 8, a silver electrode with a thickness of approximately 110 nm is deposited on the surface of the hole-blocking layer to obtain the final structure FTO / NiOx / Me-4PACz / 4B / PVK / C. 60 FACsMAPbI3 perovskite solar cells with / BCP / Ag.

[0064] In this embodiment, a perovskite solar cell was prepared by applying a 2 mg / mL lower interface modification layer 4B, followed by annealing. The device achieved an open-circuit voltage of 1.175 V and a current of 25.87 mA / cm². 2 Short-circuit current, fill factor of 85.32%, photoelectric conversion efficiency of 25.94%.

[0065] Example 3 Step 1, Preparation of FTO glass and magnesium fluoride (MgF2) antireflective layer; [The text abruptly ends here, likely due to an incomplete sentence or missing information.] 2 The FTO glass was ultrasonically cleaned with conductive glass cleaning solution, acetone, and ethanol, and then dried with a nitrogen gas gun. The cleaned FTO conductive glass was placed in a vacuum evaporation apparatus, and a 110 nm thick MgF2 antireflection layer was deposited on the back of the FTO at a rate of 0.3 Å / s. After the deposition was completed, the glass was stored in anhydrous ethanol.

[0066] Step 2: Add 1 mL of deionized water to a glass bottle containing 10 mg of NiOx powder to prepare a 10 mg / mL NiOx dispersion. Place the glass bottle in an ultrasonic cleaner and sonicate for 40 minutes to ensure the NiOx powder is fully dispersed in the deionized water for later use. Treat the FTO glass cleaned in Step 1 with ultraviolet ozone for 15 min. Spin-coat the 10 mg / mL NiOx dispersion onto the FTO glass surface at a spin speed of 2000 rpm (acceleration of 1000 rpm / s) for 30 s. Then, anneal the glass on a constant temperature hot plate at 150 °C for 10 min. 1 mg of Me-4PACz solid powder was dissolved in 2 mL of anhydrous ethanol at a concentration of 0.5 mg / mL and stirred for 3 h. The solution was then spin-coated onto the surface of NiOx at a speed of 4000 rpm for 30 s. Annealing was then performed at 100 °C for 10 min. After annealing, unbound molecules were removed by rinsing with ethanol to obtain the NiOx and Me-4PACz layers.

[0067] Step 3: Prepare the 4B modified layer DMF solution. The 4B modified layer solution is prepared by dissolving 2 mg of 4B solid powder in 2 mL of DMF and stirring for 4 h.

[0068] Step 4: Prepare the 4B modification layer; spin-coat the 1 mg / mL 4B DMF solution prepared in Step 3 onto the NiOx / Me-4PACz surface at a spin-coating speed of 5000 rpm for 30 s without annealing.

[0069] Step 5, prepare 1.5 M FA 0.9 Cs 0.05 MA 0.05 The PbI3 perovskite precursor solution was prepared by dissolving formamidinium hydroiodide (FAI), CsI, MAI, and PbI2 in a stoichiometric ratio in a mixed solvent of DMF and DMSO (V / V = 4:1), stirring at room temperature for 6 h, and then filtering using a 0.45 μm syringe for later use.

[0070] Step 6: Prepare the perovskite absorbing layer (PVK). The perovskite precursor solution prepared in Step 5 is spin-coated onto the surface of the 4B modified layer. The spin-coating process consists of two stages: the first stage uses a spin speed of 1000 rpm for 8 s; the second stage uses a spin speed of 4000 rpm for 25 s. Five seconds before the end of the spin-coating, the antisolvent anisole is applied to the perovskite surface, followed by annealing at 110 ℃ for 20 min. After annealing, FTO / NiOx / Me-4PACz / 4B / PVK is formed. The prepared perovskite absorbing layer is approximately 500 nm in size.

[0071] Step 7: Prepare the electron transport layer; deposit a C layer with a thickness of approximately 20 nm on the surface of the perovskite prepared in Step 6. 60 As an electron transport layer, FTO / NiOx / Me-4PACz / 4B / perovskite light-absorbing layer / C was fabricated. 60 .

[0072] Step 8, prepare the hole blocking layer; the C obtained in step 7 60 A BCP (bath copper alloy) layer with a thickness of approximately 6 nm was deposited on the surface as a hole-blocking layer to prepare FTO / NiOx / Me-4PACz / 4B / PVK / C. 60 / BCP.

[0073] Step 9: Fabrication of the metal electrode; A silver layer with a thickness of approximately 110 nm is deposited on the surface of the hole-blocking layer prepared in step 8 as the metal electrode, ultimately yielding a structure of FTO / NiOx / Me-4PACz / 4B / PVK / C. 60 FACsMAPbI3 perovskite solar cells with / BCP / Ag.

[0074] In this embodiment, a perovskite solar cell with a 1.0 mg / mL lower interface modification layer 4B was prepared. The perovskite solar cell achieved an open-circuit voltage of 1.171 V and a voltage of 26.04 mA / cm². 2 Short-circuit current, 85.75% fill factor, 26.14% photoelectric conversion efficiency.

[0075] Example 4 Step 1, Preparation of FTO glass and magnesium fluoride (MgF2) antireflective layer; [The text abruptly ends here, likely due to an incomplete sentence or missing information.] 2 The FTO glass was ultrasonically cleaned with conductive glass cleaning solution, acetone, and ethanol, and then dried with a nitrogen gas gun. The cleaned FTO conductive glass was placed in a vacuum evaporation apparatus, and a 110 nm thick MgF2 antireflection layer was deposited on the back of the FTO at a rate of 0.3 Å / s. After the deposition was completed, the glass was stored in anhydrous ethanol.

[0076] Step 2: Add 1 mL of deionized water to a glass bottle containing 10 mg of NiOx powder to prepare a 10 mg / mL NiOx dispersion. Place the glass bottle in an ultrasonic cleaner and sonicate for 40 minutes to ensure the NiOx powder is fully dispersed in the deionized water for later use. Treat the FTO glass cleaned in Step 1 with ultraviolet ozone for 15 min. Spin-coat the 10 mg / mL NiOx dispersion onto the FTO glass surface at a spin speed of 2000 rpm (acceleration of 1000 rpm / s) for 30 s. Then, anneal the glass on a constant temperature hot plate at 150 °C for 10 min. 1 mg of Me-4PACz solid powder was dissolved in 2 mL of anhydrous ethanol at a concentration of 0.5 mg / mL and stirred for 3 h. The solution was then spin-coated onto the surface of NiOx at a speed of 4000 rpm for 30 s. Annealing was then performed at 100 °C for 10 min. After annealing, unbound molecules were removed by rinsing with ethanol to obtain the NiOx and Me-4PACz layers.

[0077] Step 3: Prepare the 4B modified layer DMF solution. The 4B modified layer solution is prepared by dissolving 3 mg of 4B solid powder in 1 mL of DMF and stirring for 4 h.

[0078] Step 4: Prepare the 4B modification layer; spin-coat the 3 mg / mL 4B DMF solution prepared in Step 3 onto the NiOx / Me-4PACz surface at a spin-coating speed of 5000 rpm for 30 s without annealing.

[0079] Step 5, prepare 1.5 M FA 0.9 Cs 0.05 MA 0.05 The PbI3 perovskite precursor solution was prepared by dissolving formamidinium hydroiodide (FAI), CsI, MAI, and PbI2 in a stoichiometric ratio in a mixed solvent of DMF and DMSO (V / V = 4:1), stirring at room temperature for 6 h, and then filtering using a 0.45 μm syringe for later use.

[0080] Step 6: Prepare the perovskite absorbing layer (PVK). The perovskite precursor solution prepared in Step 5 is spin-coated onto the surface of the 4B modified layer. The spin-coating process consists of two stages: the first stage uses a spin speed of 1000 rpm for 8 s; the second stage uses a spin speed of 4000 rpm for 25 s. Five seconds before the end of the spin-coating, the antisolvent anisole is applied to the perovskite surface, followed by annealing at 110 ℃ for 20 min. After annealing, FTO / NiOx / Me-4PACz / 4B / PVK is formed. The prepared perovskite absorbing layer is approximately 500 nm in size.

[0081] Step 7: Prepare the electron transport layer; deposit a C layer with a thickness of approximately 20 nm on the surface of the perovskite prepared in Step 6. 60 As an electron transport layer, FTO / NiOx / Me-4PACz / 4B / perovskite light-absorbing layer / C was fabricated. 60 .

[0082] Step 8, prepare the hole blocking layer; the C obtained in step 7 60 A BCP (bath copper alloy) layer with a thickness of approximately 6 nm was deposited on the surface as a hole-blocking layer to prepare FTO / NiOx / Me-4PACz / 4B / PVK / C. 60 / BCP.

[0083] Step 9: Fabrication of the metal electrode; A silver layer with a thickness of approximately 110 nm is deposited on the surface of the hole-blocking layer prepared in step 8 as the metal electrode, ultimately yielding a structure of FTO / NiOx / Me-4PACz / 4B / PVK / C. 60 FACsMAPbI3 perovskite solar cells with / BCP / Ag.

[0084] In this embodiment, a perovskite solar cell with a 3 mg / mL lower interface modification layer 4B was prepared.

[0085] Example 5 Step 1, Preparation of FTO glass and magnesium fluoride (MgF2) antireflective layer; [The text abruptly ends here, likely due to an incomplete sentence or missing information.] 2 The FTO glass was ultrasonically cleaned with conductive glass cleaning solution, acetone, and ethanol, and then dried with a nitrogen gas gun. The cleaned FTO conductive glass was placed in a vacuum evaporation apparatus, and a 110 nm thick MgF2 antireflection layer was deposited on the back of the FTO at a rate of 0.3 Å / s. After the deposition was completed, the glass was stored in anhydrous ethanol.

[0086] Step 2: Add 1 mL of deionized water to a glass bottle containing 10 mg of NiOx powder to prepare a 10 mg / mL NiOx dispersion. Place the glass bottle in an ultrasonic cleaner and sonicate for 40 minutes to ensure the NiOx powder is fully dispersed in the deionized water for later use. Treat the FTO glass cleaned in Step 1 with ultraviolet ozone for 15 min. Spin-coat the 10 mg / mL NiOx dispersion onto the FTO glass surface at a spin speed of 2000 rpm (acceleration of 1000 rpm / s) for 30 s. Then, anneal the glass on a constant temperature hot plate at 150 °C for 10 min. 1 mg of Me-4PACz solid powder was dissolved in 2 mL of anhydrous ethanol at a concentration of 0.5 mg / mL and stirred for 3 h. The solution was then spin-coated onto the surface of NiOx at a speed of 4000 rpm for 30 s. Annealing was then performed at 100 °C for 10 min. After annealing, unbound molecules were removed by rinsing with ethanol to obtain the NiOx and Me-4PACz layers.

[0087] Step 3: Prepare the 4B modified layer DMF solution. The 4B modified layer solution is prepared by dissolving 4 mg of 4B solid powder in 2 mL of IPA and stirring for 4 h.

[0088] Step 4: Prepare the 4B modification layer; spin-coat the 2 mg / mL 4B IPA solution prepared in Step 3 onto the NiOx / Me-4PACz surface at a spin-coating speed of 5000 rpm for 30 s without annealing.

[0089] Step 5, prepare 1.5 M FA 0.9 Cs 0.05 MA 0.05 The PbI3 perovskite precursor solution was prepared by dissolving formamidinium hydroiodide (FAI), CsI, MAI, and PbI2 in a stoichiometric ratio in a mixed solvent of DMF and DMSO (V / V = 4:1), stirring at room temperature for 6 h, and then filtering using a 0.45 μm syringe for later use.

[0090] Step 6: Prepare the perovskite absorbing layer (PVK). The perovskite precursor solution prepared in Step 5 is spin-coated onto the surface of the 4B modified layer. The spin-coating process consists of two stages: the first stage uses a spin speed of 1000 rpm for 8 s; the second stage uses a spin speed of 4000 rpm for 25 s. Five seconds before the end of the spin-coating, the antisolvent anisole is applied to the perovskite surface, followed by annealing at 110 ℃ for 20 min. After annealing, FTO / NiOx / Me-4PACz / 4B / PVK is formed. The prepared perovskite absorbing layer is approximately 500 nm in size.

[0091] Step 7: Prepare the electron transport layer; deposit a C layer with a thickness of approximately 20 nm on the surface of the perovskite prepared in Step 6. 60 As an electron transport layer, FTO / NiOx / Me-4PACz / 4B / perovskite light-absorbing layer / C was fabricated. 60 .

[0092] Step 8, prepare the hole blocking layer; the C obtained in step 7 60 A BCP (bath copper alloy) layer with a thickness of approximately 6 nm was deposited on the surface as a hole-blocking layer to prepare FTO / NiOx / Me-4PACz / 4B / PVK / C. 60 / BCP.

[0093] Step 9: Fabrication of the metal electrode; A silver layer with a thickness of approximately 110 nm is deposited on the surface of the hole-blocking layer prepared in step 8 as the metal electrode, ultimately yielding a structure of FTO / NiOx / Me-4PACz / 4B / PVK / C. 60 FACsMAPbI3 perovskite solar cells with / BCP / Ag.

[0094] In this embodiment, a perovskite solar cell with a 2 mg / mL lower interface modification layer 4B was prepared using IPA solvent. The perovskite solar cell achieved an open-circuit voltage of 1.172 V and an open-circuit voltage of 25.66 mA / cm². 2 Short-circuit current, fill factor of 85.31%, photoelectric conversion efficiency of 25.67%.

[0095] Example 6 Step 1, Preparation of FTO glass and magnesium fluoride (MgF2) antireflective layer; [The text abruptly ends here, likely due to an incomplete sentence or missing information.] 2 The FTO glass was ultrasonically cleaned with conductive glass cleaning solution, acetone, and ethanol, and then dried with a nitrogen gas gun. The cleaned FTO conductive glass was placed in a vacuum evaporation apparatus, and a 110 nm thick MgF2 antireflection layer was deposited on the back of the FTO at a rate of 0.3 Å / s. After the deposition was completed, the glass was stored in anhydrous ethanol.

[0096] Step 2: Add 1 mL of deionized water to a glass bottle containing 10 mg of NiOx powder to prepare a 10 mg / mL NiOx dispersion. Place the glass bottle in an ultrasonic cleaner and sonicate for 40 minutes to ensure the NiOx powder is fully dispersed in the deionized water for later use. Treat the FTO glass cleaned in Step 1 with ultraviolet ozone for 15 min. Spin-coat the 10 mg / mL NiOx dispersion onto the FTO glass surface at a spin speed of 2000 rpm (acceleration of 1000 rpm / s) for 30 s. Then, anneal the glass on a constant temperature hot plate at 150 °C for 10 min. 1 mg of Me-4PACz solid powder was dissolved in 2 mL of anhydrous ethanol at a concentration of 0.5 mg / mL and stirred for 3 h. The solution was then spin-coated onto the surface of NiOx at a speed of 4000 rpm for 30 s. Annealing was then performed at 100 °C for 10 min. After annealing, unbound molecules were removed by rinsing with ethanol to obtain the NiOx and Me-4PACz layers.

[0097] Step 3: Prepare an anhydrous ethanol solution for the 4B modified layer. The 4B modified layer solution is prepared by dissolving 2 mg of 4B solid powder in 4 mL of anhydrous ethanol and stirring for 4 h.

[0098] Step 4: Prepare the 4B modified layer; spin-coat the 2 mg / mL anhydrous ethanol solution of 4B prepared in Step 3 onto the surface of NiOx / Me-4PACz at a spin-coating speed of 5000 rpm for 30 s, followed by annealing at 100℃ for 10 min to obtain the 4B modified layer.

[0099] Step 5, prepare 1.5 M FA 0.9 Cs 0.05 MA 0.05 The PbI3 perovskite precursor solution was prepared by dissolving formamidinium hydroiodide (FAI), CsI, MAI, and PbI2 in a stoichiometric ratio in a mixed solvent of DMF and DMSO (V / V = 4:1), stirring at room temperature for 6 h, and then filtering using a 0.45 μm syringe for later use.

[0100] Step 6: Prepare the perovskite absorbing layer (PVK). The perovskite precursor solution prepared in Step 5 is spin-coated onto the surface of the 4B modified layer. The spin-coating process consists of two stages: the first stage uses a spin speed of 1000 rpm for 8 s; the second stage uses a spin speed of 4000 rpm for 25 s. Five seconds before the end of the spin-coating, the antisolvent anisole is applied to the perovskite surface, followed by annealing at 110 ℃ for 20 min. After annealing, FTO / NiOx / Me-4PACz / 4B / PVK is formed. The prepared perovskite absorbing layer is approximately 500 nm in size.

[0101] Step 7: Prepare the electron transport layer; deposit a C layer with a thickness of approximately 20 nm on the surface of the perovskite prepared in Step 6. 60 As an electron transport layer, FTO / NiOx / Me-4PACz / 4B / perovskite light-absorbing layer / C was fabricated. 60 .

[0102] Step 8, prepare the hole blocking layer; the C obtained in step 7 60 A BCP (bath copper alloy) layer with a thickness of approximately 6 nm was deposited on the surface as a hole-blocking layer to prepare FTO / NiOx / Me-4PACz / 4B / PVK / C. 60 / BCP.

[0103] Step 9: Fabrication of the metal electrode; A silver layer with a thickness of approximately 110 nm is deposited on the surface of the hole-blocking layer prepared in step 8 as the metal electrode, ultimately yielding a structure of FTO / NiOx / Me-4PACz / 4B / PVK / C. 60 FACsMAPbI3 perovskite solar cells with / BCP / Ag.

[0104] In this embodiment, anhydrous ethanol was used to dissolve and prepare a perovskite solar cell with a 2 mg / mL lower interface modification layer 4B. The perovskite solar cell achieved an open-circuit voltage of 1.171 V and a voltage rating of 25.79 mAcm⁻¹. -2 It has a short-circuit current of 84.49%, a fill factor of 84.49%, and a photoelectric conversion efficiency of 25.51%.

[0105] The above description is only a preferred embodiment of the present invention and is not intended to limit the present invention. Any modifications, equivalent substitutions, improvements, etc., made within the spirit and principles of the present invention should be included within the protection scope of the present invention.

Claims

1. A method for preparing a trans -perovskite cell with low dimensional perovskite buried interface and high fill factor, characterized in that, The method comprises the following steps: S1, preparing a MgF2 anti-reflection layer on the back of FTO; S2, preparing a hole transport layer on the front of FTO, wherein the hole transport layer comprises a NiOx layer and a Me-4PACz layer; S3, preparing a modification layer on the hole transport layer by a spin coating method, wherein the modification layer is obtained by spin coating a modification layer solution on the hole transport layer, and the modification layer solution is composed of 4-(aminomethyl)benzenesulfonamide acetate and a solvent; S4, preparing FA on the modification layer 0.9 Cs 0.05 MA 0.05 PbI3perovskite light-absorbing layer; S5, in the FA 0.9 Cs 0.05 MA 0.05 An electron transport layer, a hole blocking layer and a metal electrode are sequentially prepared on the PbI3 perovskite light absorption layer.

2. The method of claim 1, wherein the method further comprises: depositing a first layer of a perovskite material on the substrate; depositing a second layer of a perovskite material on the first layer; and depositing a third layer of a perovskite material on the second layer. In S3, the concentration of the modification layer solution is 1-5 mg / mL.

3. The method of claim 1, wherein the method further comprises: depositing a first layer of a perovskite material on the substrate; depositing a second layer of a perovskite material on the first layer; and depositing a third layer of a perovskite material on the second layer. In S3, the spin coating speed of the spin coating method is 5000 rpm, and the spin coating time is 30 s.

4. The method of claim 1, wherein the method further comprises: depositing a first layer of a perovskite material on the substrate; depositing a second layer of a perovskite material on the first layer; and depositing a third layer of a perovskite material on the second layer. In S3, the solvent is N,N - any of dimethylformamide, IPA or anhydrous ethanol.

5. The method of claim 1, wherein the method further comprises: depositing a first layer of a perovskite material on the substrate; depositing a second layer of a perovskite material on the first layer; and depositing a third layer of a perovskite material on the second layer. The NiOx layer is prepared by spin coating a NiOx dispersion liquid on the hole transport layer, wherein the concentration of the NiOx dispersion liquid is 10 mg / mL, the solute of the NiOx dispersion liquid is NiOx powder, and the solvent is deionized water.

6. The method of claim 1, wherein the method further comprises: depositing a first layer of a perovskite material on the substrate; depositing a second layer of a perovskite material on the first layer; and depositing a third layer of a perovskite material on the second layer. The Me-4PACz layer is obtained by spin coating a Me-4PACz solution on the surface of the NiOx layer, wherein the solute of the Me-4PACz solution is Me-4PACz powder, and the solvent is anhydrous ethanol.

7. The method of claim 1, wherein the method further comprises: depositing a first layer of a perovskite material on the substrate; depositing a second layer of a perovskite material on the first layer; and depositing a third layer of a perovskite material on the second layer. The electron transport layer is C 60 .

8. The method of claim 1, wherein the method further comprises: depositing a first layer of a perovskite material on the substrate; depositing a second layer of a perovskite material on the first layer; and depositing a third layer of a perovskite material on the second layer. The hole blocking layer is BCP.

9. The method of claim 1, wherein the method further comprises: depositing a first layer of a perovskite material on the substrate; depositing a second layer of a perovskite material on the first layer; and depositing a third layer of a perovskite material on the second layer. The metal electrode is Ag.

10. A trans perovskite cell with low dimensional perovskite buried interface and high fill factor, prepared by the method of any one of claims 1-9, characterized in that, The device comprises, from one side to the other, a MgF2 anti-reflection layer, FTO, a NiOx layer, a Me-4PACz layer, a 4-(aminomethyl)benzenesulfonamide acetate modification layer, a perovskite light-absorbing layer, an electron transport layer, a hole blocking layer, and a metal electrode.