A large-area perovskite assembly based on slit coating and vacuum flash process and a preparation method thereof

Abstract

This invention relates to the field of optoelectronic materials and devices, specifically to a large-area perovskite module based on slit coating and vacuum flash evaporation processes and its fabrication method. From bottom to top, it comprises a transparent conductive substrate, a hole transport layer, a perovskite photoactive layer, a passivation layer, an electron transport layer, a buffer layer, and a metal electrode. The hole transport layer is a self-assembled monolayer containing TEPY and MeO4PACz molecules. TEPY inhibits the self-aggregation of MeO4PACz through π-π interactions and passivates uncoordinated Pb at the buried interface through tridentate PbN coordination bonds. 2+ Defects. The perovskite photoactive layer is deposited using slot coating combined with vacuum flash evaporation to achieve large-area uniform film formation and controlled crystallization. The entire layer is coated using a slot coating process, suitable for 1 cm thicknesses. 2 Up to 100 cm 2 Component fabrication. This approach effectively suppresses nonradiative recombination and releases residual stress in the thin film through synergistic optimization of interfacial chemical bonding and crystallization kinetics, enabling the component to possess both high photoelectric conversion efficiency and excellent operational stability.

Description

Technical Field

[0001] This invention relates to the field of optoelectronic materials and devices, specifically to a large-area perovskite component based on slit coating and vacuum flash evaporation processes and its preparation method. Background Technology

[0002] Perovskite solar cells (PSCs) have shown great potential in the photovoltaic field due to their high photoelectric conversion efficiency and low-temperature solution processing characteristics. Inverted structure devices are particularly suitable for large-area fabrication and industrial production. Self-assembled monolayers (SAMs), as hole transport layers, have significantly improved device efficiency; however, SAM molecules are prone to self-aggregation, leading to uneven substrate coverage and dense defects at the buried interface, especially uncoordinated Pb. 2+ Defects become the main source of non-radiative recombination, severely limiting device performance and long-term stability.

[0003] Traditional spin-coating processes are only suitable for small-area samples and suffer from problems such as poor film uniformity, significant edge effects, and uncontrollable solvent evaporation, failing to meet the needs of large-area component fabrication. Currently, there is a lack of integrated fabrication solutions that can simultaneously achieve SAM anti-agglomeration, efficient interface passivation, large-area uniform film formation, and rapid high-quality crystallization.

[0004] To overcome the above problems, this invention introduces an interfacial tridentate chelation strategy, using 2,2′:6′,2″-terpyridine (TERPY) as a bifunctional molecule to simultaneously inhibit SAM aggregation and passivate interfacial defects. Furthermore, slit coating is used to achieve uniform film formation over a large area across the entire layer, and vacuum flash evaporation is employed to achieve rapid drying and crystallization control of the perovskite precursor, ultimately resulting in a high-efficiency, high-stability large-area perovskite module. Summary of the Invention

[0005] The purpose of this invention is to provide a large-area perovskite module and its preparation method based on slit coating and vacuum flash evaporation processes. A composite hole transport layer is constructed using TERPY molecules and MeO4PACz, and the perovskite layer is prepared by combining slit coating and vacuum flash evaporation processes, thereby achieving large-area uniform film formation and passivation of interface defects, and improving the efficiency and stability of the module.

[0006] To achieve the above-mentioned technical objectives and effects, the present invention is implemented through the following technical solution: A large-area perovskite module based on slot coating and vacuum flash evaporation process is characterized in that, from bottom to top, it comprises: a transparent conductive substrate, a hole transport layer, a perovskite photoactive layer, a passivation layer, an electron transport layer, a buffer layer, and a metal electrode. The hole transport layer is a self-assembled monolayer containing TERPY molecules and MeO-4PACz molecules.

[0007] Furthermore, the TERPY molecule inhibits the self-aggregation of MeO-4PACz molecules through π-π interactions, and passivates the uncoordinated Pb at the perovskite buried interface through tridentate Pb-N coordination bonds. 2+ defect.

[0008] Furthermore, the concentration of TERPY molecules in the hole transport layer is 0.1 mg / mL to 1.0 mg / mL, and the mass concentration ratio of TERPY molecules to MeO-4PACz molecules is 1:0.5 to 1:2.

[0009] Preferably, the concentration of TERPY molecules in the hole transport layer is 0.5 mg / mL, and the concentration of MeO4PACz molecules is 0.5 mg / mL.

[0010] Furthermore, the material of the perovskite photoactive layer includes formamidinium ions, cesium ions, lead ions, bromide ions, and iodide ions, and also includes chloride ions as a crystallization regulating component.

[0011] Furthermore, the perovskite photoactive layer is prepared using a combination of slit coating and vacuum flash evaporation processes.

[0012] On the other hand, the present invention proposes a method for preparing the above-mentioned large-area perovskite component, comprising the following steps: The transparent conductive substrate is cleaned and activated. Prepare a self-assembled monolayer precursor solution, a perovskite precursor solution, a passivation layer precursor solution, an electron transport layer precursor solution, and a buffer layer precursor solution containing TERPY molecules and MeO-4PACz molecules. The self-assembled monolayer precursor solution was deposited on a substrate using a slot coating process and then annealed to form a hole transport layer. The perovskite precursor solution was deposited onto the hole transport layer using a slot coating process. The solution was then removed by vacuum flash evaporation to remove the solvent and induce nucleation. Finally, the solution was annealed and crystallized to form a perovskite photoactive layer. A passivation layer precursor solution was deposited onto a perovskite photoactive layer using a slot coating process, followed by annealing to form the passivation layer. An electron transport layer precursor solution and a buffer layer precursor solution are sequentially deposited using a slot coating process to form the electron transport layer and the buffer layer, respectively. Vacuum evaporation metal electrode.

[0013] Furthermore, the coating parameters of the slit coating process are: flow rate 20~100 μL / min, coating gap 20~100 μm, and coating travel speed 10~60 cm / min.

[0014] Furthermore, the conditions for the vacuum flash evaporation treatment are: pressure 5~200 Pa, treatment time 20~180 s.

[0015] Furthermore, the effective area of ​​the component is 1 cm². 2 ~100 cm 2 And 1 cm 2 The photoelectric conversion efficiency of the component is not less than 25.4%.

[0016] Furthermore, after the unpackaged component has been operating continuously for no less than 1200 hours under the ISOS-L-2 protocol, its initial efficiency retention rate is no less than 82%.

[0017] The beneficial effects of this invention are: This invention constructs a composite hole transport layer by combining TERPY molecules with MeO4PACz, solving the dual technical problems of easy aggregation of self-assembled monolayers and enrichment of defects at buried interfaces at the molecular level. TERPY molecules possess a large π-conjugated structure, forming π-π stacking interactions with MeO4PACz. Quantitative data on dynamic light scattering particle size distribution and molecular dynamics simulation coverage (such as...) are available. Figure 1 (g) and (h) show that this effect significantly inhibits the self-aggregation behavior of SAMs molecules in solution and during film formation, resulting in a uniform and dense coverage of the hole transport layer on a large-area substrate. The surface potential distribution of KPFM (as shown in (g)) indicates that this effect significantly inhibits the self-aggregation behavior of SAMs molecules in solution and during film formation, resulting in a uniform and dense coverage of the hole transport layer on a large-area substrate. Figure 1 (i) and (j) further confirm the improvement in film uniformity. The three pyridine nitrogen atoms of the TERPY molecule form a tripentate chelate structure, and its electrostatic potential distribution (as shown in Figure 1) further confirms the improvement in film uniformity. Figure 2 (a) shows that the nitrogen atom has strong coordination activity, forming a PbN coordination bond with the uncoordinated lead ions exposed at the perovskite buried interface. The chemical shift of the Pb 4f characteristic peak in XPS (as shown in Figure 1) Figure 2 (f) shows the change in the characteristic peaks of the pyridine ring in FTIR (as shown in f). Figure 2 (d) and 1 The shift of the pyridine hydrogen signal in H NMR (e.g. Figure 2 (g) together verify the existence of this coordination effect. This tripentate chelate transforms the deep-level defect at the buried interface into a chemically inert species, as evidenced by the decrease in reverse saturation current density in the dark-state JV curve (as shown in g). Figure 4 (d) shows that the ideal factor approaches 1 (as shown in the figure). Figure 4 As shown in (h), the nonradiative recombination at the interface is significantly suppressed, which directly contributes to the improvement of the device open-circuit voltage and fill factor.

[0018] This invention constructs a synergistic process route of slot coating and vacuum flash evaporation in the preparation of perovskite photoactive layers. Slot coating, through precise control of flow rate, coating gap, and travel speed, forms a uniformly thick precursor wet film on a wide substrate, overcoming the area limitations and edge effects of spin coating. The wet film is then subjected to vacuum flash evaporation in a low-pressure environment. Utilizing the vapor pressure difference between different solvents, a solvent-directed extraction effect is induced, achieving rapid solvent removal before macroscopic solvent flow occurs, thus inducing instantaneous and uniform nucleation of perovskite components in a supersaturated state. SEM images (e.g.) Figure 3 As shown in (a)-3(d), after this process and combined with TERPY interface modification, the perovskite film exhibits morphological characteristics of increased grain size, denser grain boundaries, and a significant reduction in pinhole defects. GIWAXS testing (as shown in Figures 1-3) confirms this. Figure 3 (e) and (f) further confirm the ordered crystal orientation. The residual strain fitting results of GIXRD at different ψ angles (as shown in Figures 3(e) and 3(f)) further confirm the ordered crystal orientation. Figure 3 (k) and (l) show that the PbN chemical anchoring layer formed by TERPY molecules at the buried interface has moderate flexibility and deformability, plays a buffering role in the perovskite crystallization shrinkage process, and significantly releases the residual stress caused by the mismatch of the thermal expansion coefficients between the perovskite and the substrate material, providing a key guarantee for the structural stability of the film.

[0019] This invention incorporates the hole transport layer, perovskite photoactive layer, passivation layer, electron transport layer, and buffer layer into a slot coating process framework, establishing a complete all-solution method (excluding metal electrodes) platform for large-area component fabrication. The solution rheological properties of the TEPY / MeO4PACz blend in the hole transport layer are highly compatible with the slot coating process, enabling large-area uniform coverage at the nanoscale thickness. The passivation layer, electron transport layer, and buffer layer are deposited sequentially through slot coating, avoiding the radial thickness unevenness caused by spin coating and eliminating the risk of cross-contamination between different functional layers due to process switching. Effective area starts from 1 cm². 2 Enlarged to 100 cm 2 Performance retention rate during the process, and the forward and reverse JV scan curves of the champion device (e.g.) Figure 5 The extremely low hysteresis factor shown in (d) jointly verifies that the process platform has good area scaling effect and process tolerance.

[0020] This invention utilizes the synergistic effect of TERPY interfacial tridentate chelation and vacuum flash evaporation to construct intrinsically stable perovskite components at multiple scales: molecular, interface, and thin film. At the interface chemistry level, TERPY stably chelates uncoordinated lead ions at the buried interface through PbN coordination bonds, and the appearance of coordination states in XPS and N 1s spectra (such as...) Figure 2(e) indicates that this effect blocks the chemical reaction pathways that catalyze the migration of halide ions or induce perovskite decomposition at the active sites. At the film stress level, GIXRD residual stress analysis results (e.g.) Figure 3 As shown in (k) and 3(l), the TERPY interface anchoring layer and the vacuum flash evaporation process synergistically release the residual stress of the perovskite film, reducing the thermodynamic driving force for grain boundary cracking and interlayer delamination caused by stress concentration within the film. At the film morphology and crystallography level, the rapid and uniform nucleation induced by vacuum flash evaporation and the grain growth promoted by the TERPY interface work synergistically to form a film structure with dense grain boundaries, low defect density, and good grain penetration, thus extending the diffusion path for ion migration. As described in Example 2, the unencapsulated component still maintains an efficiency of 82.75% after 1300 hours of continuous operation under the ISOSL2 protocol (e.g., ...). Figure 5 (g) shown), and maintained 92% of its initial efficiency for 1000 hours in a dark thermal aging test in a nitrogen atmosphere at 85 °C (as shown in the figure). Figure 5 As shown in (h), the synergistic effect of the above three levels provides a complete mechanistic support for this stability improvement.

[0021] Of course, any product implementing this invention does not necessarily need to achieve all of the advantages described above at the same time. Attached Figure Description

[0022] To more clearly illustrate the technical solutions of the embodiments of the present invention, the accompanying drawings used in the description of the embodiments will be briefly introduced below. Obviously, the drawings described below are only some embodiments of the present invention. For those skilled in the art, other drawings can be obtained based on these drawings without creative effort.

[0023] Figure 1 (a) Schematic diagram of the molecular regulation mechanism of SAMs assembly process; (b) Chemical structure of MeO-4PACz and TERPY; (c) Schematic diagram of the deposition of MeO-4PACz and TERPY-MeO; (d) Top view of NiO / SAMs / NiO heterojunction model used for MD simulation; (e) and (f) Side view of the heterojunction model; (g) Partial coverage of MeO-4PACz sample on NiOx substrate determined by MD simulation; (h) Particle size distribution of DLS in SAMs precursor solution; (i) KPFM image of MeO-4PACz film; (j) KPFM image of TERPY-doped MeO-4PACz film.

[0024] Figure 2(a) Schematic diagram of the tridentate chelation mechanism of TERPY; (b) ESP distribution diagram of TERPY; (c) Differential charge density diagram of the adsorption configuration of TERPY on the perovskite (100) crystal plane and corresponding adsorption energy; (d) FTIR spectrum of the perovskite buried interface; (e) N 1s XPS spectrum of the perovskite buried interface; (f) Pb 4f XPS spectrum of the perovskite buried interface; (g) TERPY in PbI2 / DMSO-d6 solution. 1 H NMR spectrum; (h) is a schematic diagram of the perovskite / HTL interface mechanism without TERPY; (i) is a schematic diagram of the perovskite / HTL interface mechanism with TERPY.

[0025] Figure 3 (a) Morphology and residual stress diagram of the perovskite embedded interface; (b) SEM image of the perovskite film deposited on MeO-4PACz; (c) SEM image of the perovskite film deposited on MeO-4PACz; (d) SEM image of the perovskite film deposited on MeO-4PACz; (e) Two-dimensional GIWAXS pattern of the perovskite film deposited on MeO-4PACz; (f) Two-dimensional GIWAXS pattern of the perovskite film deposited on MeO-4PACz. (g) GIXRD spectrum of perovskite film deposited on MeO-4PACz during annealing; (h) GIXRD spectrum of perovskite film deposited on TERPY-MeO during annealing; (i) GIXRD spectrum of perovskite film deposited on MeO-4PACz at different ψ angles (10°-50°); (j) GIXRD spectrum of perovskite film deposited on TERPY-MeO at different ψ angles (10°-50°); (k) Residual strain and sin(θ) based on GIXRD results. 2 ψ relationship curve; (l) is a comparison diagram of residual stress in perovskite films.

[0026] Figure 4 (a) Interfacial carrier dynamics and nonradiative recombination suppression plots; (b) FS-TAS spectra of perovskite films on MeO-4PACz at different delay times; (c) TA kinetic curves corresponding to (a) and (b); (d) dark-state JV curves; (e) TPC decay curves; (f) TPV decay curves; (g) EIS Nyquist plots and fitting curves; (h) Ideal factor comparison plots; (i) Mott-Schottky curves.

[0027] Figure 5 The figures show the photovoltaic performance and stability of the PSC; (a) a schematic diagram of the pin structure PSC; (b) inverse JV curves of the champion devices based on MeO-4PACz and TERPY-MeO; (c) inverse JV curves of the champion device with a wide bandgap (1.68 eV); and (d) the inverse JV curves of the champion device based on TERPY-MeO (effective area 1 cm²). 2 (e) is the forward and reverse JV curves of the champion device; (f) is the EQE spectrum and integral JSC of the champion device; (g) is the steady-state output curve of the device at the maximum power point (MPP) for 300 s; (h) is the MPPT curve of the packaged device in an air environment (55-65 °C, AM 1.5G illumination); (f) is the thermal stability curve of the unpackaged device in a dark state and an 85 °C nitrogen environment. Detailed Implementation

[0028] The technical solutions of the embodiments of the present invention will be clearly and completely described below with reference to the accompanying drawings. Obviously, the described embodiments are only some embodiments of the present invention, and not all embodiments. Based on the embodiments of the present invention, all other embodiments obtained by those skilled in the art without creative effort are within the scope of protection of the present invention. Example 1

[0029] This embodiment provides a large-area perovskite module based on slot coating and vacuum flash evaporation processes and its preparation method, specifically including the following steps: S1, Substrate Cleaning and Activation A patterned large-area ITO glass substrate (effective area 1 cm²) 2 ~ 100 cm 2 The substrate was then ultrasonically cleaned for 15 minutes each with glass cleaner, isopropanol, deionized water, and anhydrous ethanol, followed by drying with high-purity nitrogen. The cleaned substrate was then treated in a UV-ozone cleaner for 30 minutes to increase its surface energy and remove organic residues.

[0030] S2, Solution preparation The following precursor solutions for each functional layer were prepared under constant temperature conditions of 60℃: (1) Hole transport layer precursor solution: MeO-4PACz was weighed and dissolved in anhydrous ethanol to prepare a solution with a concentration of 0.5 mg / mL. Then, TERPY molecules were added to make the concentration 0.5 mg / mL, and the mixture was stirred at 60 °C for 60 minutes until it was completely dissolved to obtain a TERPY-doped MeO-4PACz mixed solution.

[0031] (2) Perovskite precursor solution: Weigh the raw material in a molar ratio of CsI:PbI2:FAI:PbBr2:MABr:MACl = 0.05:1:1.1:0.2:0.2:0.6, dissolve it in a mixed solvent of N,N-dimethylformamide (DMF) and dimethyl sulfoxide (DMSO) in a volume ratio of 8:2, and stir at 60°C for 60 minutes to obtain CsI with a concentration of 1.5 M. 0.05 (FA) 0.95 MA 0.05 ) 0.95 Pb(I) 0.95 Br 0.05 3. Perovskite precursor solution.

[0032] (3) Passivation layer precursor solution: Dissolve PEAI in isopropanol to prepare a solution of 1 mg / mL.

[0033] (4) Electron transport layer precursor solution: PC 61 BM was dissolved in chlorobenzene to prepare a solution of 20 mg / mL.

[0034] (5) Buffer layer precursor solution: Dissolve BCP in anhydrous ethanol to prepare a solution of 1 mg / mL.

[0035] S3. Slit coating for preparing hole transport layer The UV-ozone treated ITO substrate was placed on the stage of a slot coating apparatus, and the substrate temperature was set to room temperature. The TERPY-doped MeO4PACz solution prepared in step S2 was deposited onto the substrate using a slot coating process. The coating parameters were: solution flow rate 50 μL / min, coating gap 50 μm, and coating speed 30 cm / min. After coating, the sample was transferred to a nitrogen-atmosphere heated stage and annealed at 100°C for 10 minutes to form a dense hole transport layer.

[0036] S4. Preparation of perovskite photoactive layer by slit coating and vacuum flash evaporation (1) Using a slot coating process, the perovskite precursor solution prepared in step S2 is uniformly coated onto the hole transport layer obtained in step S3. The coating process parameters are the same as those in step S3.

[0037] (2) After coating, immediately transfer the substrate with the wet film of perovskite precursor to the vacuum flash evaporation chamber. Reduce the chamber pressure to 30 Pa and maintain this pressure for 60 seconds to induce uniform nucleation of the perovskite components by rapidly removing the solvent from the wet film. After flash evaporation, immediately remove the sample and transfer it to a hot stage under a nitrogen atmosphere to avoid exposure to air.

[0038] (3) Under a nitrogen atmosphere, the sample was annealed at 100°C for 50 minutes to form a black, dense, and well-crystallized perovskite photoactive layer, and then allowed to cool to room temperature.

[0039] S5. Slit coating to prepare passivation layer A slit coating process was used to deposit the PEAI solution prepared in step S2 onto the perovskite photoactive layer obtained in step S4. The coating process parameters were the same as in step S3. After coating, the layer was annealed at 100°C for 10 minutes to form a passivation layer.

[0040] S6. Slit coating for electron transport and buffer layers (1) Using a slot coating process, the PC prepared in step S2 is coated with PC. 61 The BM solution is deposited on the passivation layer obtained in step S5, and the coating process parameters are the same as in step S3, forming an electron transport layer. After coating, it is left to stand for 15 minutes.

[0041] (2) Using a slit coating process, the BCP solution prepared in step S2 is deposited on the electron transport layer. The coating process parameters are the same as in step S3 to form a buffer layer.

[0042] S7, Vacuum Evaporated Metal Electrode The sample prepared according to the above steps is placed under a mask, and a portion of the active layer is scraped off to expose the electrode leads. The sample is then transferred to a vacuum evaporator, where a vacuum level below 1 × 10⁻⁶ is applied. -5 Under the condition of Pa, a silver electrode with a thickness of about 120 nm was deposited by thermal evaporation to finally obtain the large-area perovskite component.

[0043] In this embodiment, TERPY is a tripentate chelating ligand that binds to uncoordinated Pb at the perovskite buried interface via three pyridine nitrogen atoms. 2+ Stable Pb-N coordination bonds are formed, achieving efficient synergistic passivation of the buried interface. The relevant mechanism is as follows: Figure 2 As shown. Simultaneously, the large π-conjugated structure of the TERPY molecule can form π-π stacking interactions with the MeO-4PACz molecule, effectively inhibiting the self-aggregation behavior of SAM molecules in solution and during film formation, and improving the coverage and uniformity of the hole transport layer on large-area substrates. The relevant molecular regulatory mechanisms are as follows: Figure 1 As shown.

[0044] Figure 3 This paper presents a comparison of the morphology and residual stress of perovskite films prepared using the method of this embodiment (TERPY-MeO) and a control group without TERPY (MeO-4PACz). Figure 3As can be seen from the SEM images (a)-3 (d), the perovskite thin film prepared in this embodiment has increased grain size, denser grain boundaries, and significantly reduced pinhole defects. Figure 3 The GIXRD residual stress analysis results of (k) and 3(l) show that the method in this embodiment effectively releases the residual stress of the perovskite film. Figure 4 The carrier dynamics test results further confirm that the TERPY interface modification in this embodiment significantly suppressed nonradiative recombination and reduced the dark-state current density and ideality factor of the device.

[0045] Example 2: Component Performance Testing The 1 cm prepared in Example 1 2 Photoelectric performance and stability tests were conducted on large-area perovskite modules.

[0046] (1) Photoelectric performance testing Under standard test conditions (AM 1.5G, 100 mW / cm²), 2 (25℃) The JV characteristics of the device were tested using a solar simulator, and the results are as follows: Figure 5 As shown. Testing revealed that the champion device fabricated in this embodiment achieved a photoelectric conversion efficiency (PCE) of 25.43%, an open-circuit voltage (Voc) of 1.16 V, and a short-circuit current density (Jsc) of 25.52 mA / cm². 2 The fill factor (FF) is 85.90%. The hysteresis factor of the device's forward and reverse scan curves is extremely small, indicating that the interface defects have been effectively passivated.

[0047] (2) Stability test Unpackaged devices were subjected to continuous operation stability testing under ISOS-L-2 protocol (55~65℃, AM 1.5G illumination, maximum power point tracking), such as... Figure 5 As shown in (g). The results show that after 1300 hours of continuous operation, the device retains 82.75% of its initial efficiency. Furthermore, the unpackaged device was subjected to dark-state thermal stability testing in a nitrogen atmosphere at 85°C, as shown in (g). Figure 5 As shown in (h), the device efficiency remains at 92% of the initial value after 1000 hours, demonstrating excellent long-term thermal stability.

[0048] In summary, this invention proposes a large-area perovskite component and its fabrication method based on slit coating and vacuum flash evaporation processes. From bottom to top, it comprises a transparent conductive substrate, a hole transport layer, a perovskite photoactive layer, a passivation layer, an electron transport layer, a buffer layer, and a metal electrode. The hole transport layer is a self-assembled monolayer containing TEPY and MeO4PACz molecules. TEPY inhibits the self-aggregation of MeO4PACz through π-π interactions and passivates uncoordinated Pb at the buried interface through tridentate PbN coordination bonds.2+ Defects. The perovskite photoactive layer is deposited using slot coating combined with vacuum flash evaporation to achieve large-area uniform film formation and controlled crystallization. The entire layer is coated using a slot coating process, suitable for 1 cm thicknesses. 2 Up to 100 cm 2 Component fabrication. This approach effectively suppresses nonradiative recombination and releases residual stress in the thin film through synergistic optimization of interfacial chemical bonding and crystallization kinetics, enabling the component to possess both high photoelectric conversion efficiency and excellent operational stability.

[0049] The preferred embodiments of the present invention disclosed above are merely illustrative of the invention. These preferred embodiments do not exhaustively describe all details, nor do they limit the invention to the specific implementations described. Clearly, many modifications and variations can be made based on the content of this specification. This specification selects and specifically describes these embodiments to better explain the principles and practical applications of the invention, thereby enabling those skilled in the art to better understand and utilize the invention. The invention is limited only by the claims and their full scope and equivalents.

Claims

1. A large area perovskite module based on slot-die coating and vacuum flash-off process, characterized in that, From bottom to top, it includes: a transparent conductive substrate, a hole transport layer, a perovskite photoactive layer, a passivation layer, an electron transport layer, a buffer layer, and a metal electrode. The hole transport layer is a self-assembled monolayer formed by blending TERPY molecules and MeO4PACz molecules, wherein the TERPY molecules stack with the MeO4PACz molecules through ππ interactions, and the TERPY molecules are used to form tridentate PbN coordination bonds with uncoordinated lead ions in the perovskite photoactive layer. The perovskite photoactive layer is a thin film deposited using a slot coating process and dried and crystallized using a vacuum flash evaporation process.

2. The large area perovskite assembly of claim 1, wherein, The concentration of TERPY molecules in the hole transport layer is 0.1 mg / mL to 1.0 mg / mL, and the mass concentration ratio of TERPY molecules to MeO-4PACz molecules is 1:0.5 to 1:

2.

3. The large area perovskite assembly of claim 1, wherein, The perovskite photoactive layer contains formamidinium ions, cesium ions, lead ions, bromide ions, and iodide ions, and also contains chloride ions as a crystallization regulating component.

4. A method for producing a large-area perovskite assembly according to any one of claims 1 to 3, characterized in that Includes the following steps: The transparent conductive substrate is cleaned and activated. Prepare a self-assembled monolayer precursor solution, a perovskite precursor solution, a passivation layer precursor solution, an electron transport layer precursor solution, and a buffer layer precursor solution containing TERPY molecules and MeO-4PACz molecules. The self-assembled monolayer precursor solution was deposited on a substrate using a slot coating process and then annealed to form a hole transport layer. The perovskite precursor solution was deposited onto the hole transport layer using a slot coating process. The solution was then removed by vacuum flash evaporation to remove the solvent and induce nucleation. Finally, the solution was annealed and crystallized to form a perovskite photoactive layer. A passivation layer precursor solution was deposited onto a perovskite photoactive layer using a slot coating process, followed by annealing to form the passivation layer. An electron transport layer precursor solution and a buffer layer precursor solution are sequentially deposited using a slot coating process to form the electron transport layer and the buffer layer, respectively. Vacuum evaporation metal electrode.

5. The production method according to claim 4, wherein The coating parameters for the slot coating process are: flow rate 30~80 μL / min, coating gap 20~100 μm, and coating travel speed 10~60 cm / min.

6. The production method according to claim 5, wherein The conditions for the vacuum flash evaporation treatment are: pressure 10~100 Pa, treatment time 20~180 s.

Images