CN116367562A - Modification method of n/i interface of perovskite solar cell - Google Patents

Modification method of n/i interface of perovskite solar cell Download PDF

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CN116367562A
CN116367562A CN202310364607.7A CN202310364607A CN116367562A CN 116367562 A CN116367562 A CN 116367562A CN 202310364607 A CN202310364607 A CN 202310364607A CN 116367562 A CN116367562 A CN 116367562A
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perovskite
fafa
interface
solar cell
layer
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丁毅
王雅
韩梅斗雪
侯国付
赵颖
张晓丹
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Nankai University
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    • H—ELECTRICITY
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    • H10K30/00—Organic devices sensitive to infrared radiation, light, electromagnetic radiation of shorter wavelength or corpuscular radiation
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    • H10K30/865—Intermediate layers comprising a mixture of materials of the adjoining active layers
    • H—ELECTRICITY
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    • H10K30/00—Organic devices sensitive to infrared radiation, light, electromagnetic radiation of shorter wavelength or corpuscular radiation
    • H10K30/40—Organic devices sensitive to infrared radiation, light, electromagnetic radiation of shorter wavelength or corpuscular radiation comprising a p-i-n structure, e.g. having a perovskite absorber between p-type and n-type charge transport layers
    • H—ELECTRICITY
    • H10—SEMICONDUCTOR DEVICES; ELECTRIC SOLID-STATE DEVICES NOT OTHERWISE PROVIDED FOR
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    • H10K30/00—Organic devices sensitive to infrared radiation, light, electromagnetic radiation of shorter wavelength or corpuscular radiation
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    • H10—SEMICONDUCTOR DEVICES; ELECTRIC SOLID-STATE DEVICES NOT OTHERWISE PROVIDED FOR
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    • H10K85/00—Organic materials used in the body or electrodes of devices covered by this subclass
    • H10K85/50—Organic perovskites; Hybrid organic-inorganic perovskites [HOIP], e.g. CH3NH3PbI3
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Abstract

The invention provides a modification method of an n/i interface of a perovskite solar cell, which comprises a transparent conductive substrate, an electron transport layer, an n/i interface modification layer, a perovskite active layer, a hole transport layer and a metal electrode, wherein the n/i interface modification layer is a formamidine formate material, and the formamidine formate material is a modification layer simultaneously comprising carboxyl and amino compounds. The interface modification layer can effectively improve the electrical property of the electron transport material and passivate the defects on the surface of the electron transport layer. In addition, formamidine formate can also improve interface contact performance by constructing a chemical bridge at the n/i interface, and obtain a high-quality perovskite film by regulating the perovskite growth process. Meanwhile, the modification layer has remarkable improvement effect on the open-circuit voltage, the short-circuit current density, the filling factor and the photoelectric conversion efficiency of the device; the modification method provided by the invention provides a broad prospect for preparing high-efficiency conventional perovskite solar cells.

Description

Modification method of n/i interface of perovskite solar cell
Technical Field
The invention relates to the technical field of photoelectric functional materials and devices. The invention relates to a modification method of an n/i interface of a perovskite solar cell, wherein the introduction of an n/i interface modification layer can greatly improve the performance of the perovskite solar cell device, and more importantly, the optimization problem of a perovskite bottom interface is related.
Background
Among emerging solar cells, perovskite solar cells have experienced a rapid development in recent decades. The efficiency of single junction perovskite solar cells is rapidly increasing from 3.8% in 2009 to 25.7% today, almost approaching that of single crystal silicon cells where the fabrication technology is already very mature. Because of excellent photoelectric semiconductor properties, such as high light absorption coefficient, adjustable band gap, low exciton binding energy, longer carrier life and diffusion length, and low cost which can be prepared by low-temperature solution, the perovskite solar cell has very wide application prospect in the photoelectric field.
The two most commonly used inorganic Electron Transport Layer (ETL) materials in n-i-p type perovskite solar cells today are: titanium dioxide (TiO) 2 ) And tin dioxide (SnO) 2 ). Compared with TiO which needs high-temperature annealing and has obvious hysteresis effect 2 ，SnO 2 Because of up to 240 cm 2 V -1 s -1 Is considered to be a more potential electron transport layer material due to its excellent properties such as electron mobility, low-temperature preparation, and good chemical stability.
Although the conversion efficiency of perovskite solar cells has achieved significant advances, there is still a large space for improvement beyond the theoretical limit of the Shockley-Queisser of 30% and the long-term operational stability of the device has not been thoroughly addressed, which also hinders large-scale commercialization of perovskite solar cells. In the important characterization parameters of perovskite solar cells, the current short-circuit current density is already close to the theoretical value, so that the conversion efficiency is wanted to be further improved, and the open-circuit voltage and the filling factor will need to be improved by reducing non-radiative recombination. Previous studies have shown that a large number of defects at the surface interface are important factors in non-radiative recombination and open circuit voltage loss. Currently, there are already very well established methods and a wide variety of materials for perovskite upper surface passivation, such as ammonium salts, lewis acid bases, polymers, etc., and there are few related studies on perovskite bottom interface passivation.
However, it has been reported that even higher defect densities at the bottom interface of perovskite than at the top surface of perovskite can severely hamper carrier transport and result in significant energy loss. In addition, in SnO 2 A number of defects, such as surface dangling bonds, hydroxyl groups, and two typical O vacancies and Sn interstitial impurities, are also inevitably introduced during the preparation process of (a), which not only results in non-radiative recombination, but also hinders efficient extraction and transport of electrons. At the same time, snO 2 The morphology and wettability of the surface can affect the quality of the perovskite thin film deposited thereon, and the unmatched physical properties with the perovskite can also cause significant interfacial residual stress, thereby affecting the efficiency and stability of the perovskite solar cell. In summary, effective regulation of perovskite bottom interfaces is critical to further improve device performance.
Studies have shown that perovskite bottom interface passivation helps to improve device efficiency. However, these methods have certain limitations. For example, the passivation mechanism is not completely understood due to the lack of a technique for directly characterizing the perovskite bottom interface; due to the strong polarity of the perovskite solvent, the passivating molecules at the bottom interface may be destroyed upon subsequent deposition of the perovskite. It is therefore important and challenging to explore a simple passivation method and to study its mechanism.
Disclosure of Invention
Object of the invention
The invention aims at introducing a formamidine formate (FAFa) modification layer at an n/i interface, and discovers that the formamidine formate (FAFa) modification layer not only can passivate interface defects and improve interface contact performance, but also can improve the crystallization quality of a perovskite film and the conductivity of an electron transport layer, so that the performance of a perovskite solar cell is further improved.
(II) technical scheme
The invention adopts the following technical scheme to realize the aim:
a perovskite solar cell comprises a transparent conductive substrate, an electron transport layer, an n/i interface modification layer, a perovskite active layer, a hole transport layer and a metal electrode, wherein the n/i interface modification layer is formamidine formate material, and the molecular structure of the formamidine formate material is that
Figure SMS_1
。
The perovskite solar cell is a conventional perovskite solar cell, and the n/i interface modification layer is prepared between the electron transport layer and the perovskite active layer.
The preparation method of the perovskite solar cell, wherein the n/i interface modification layer FAFa comprises the following steps:
s1: respectively weighing formamidine formate materials of 1-20 mg by a precision balance, dissolving in an organic solvent of 1 mL until the formamidine formate materials are completely dissolved, and preparing FAFa solutions with different concentrations for comparison; the organic solvents include, but are not limited to, IPA;
s2: spin-coating the prepared FAFa solution on the prepared electron transport layer at 1000-4000 rpm for 20-60 s, and annealing at 80-150deg.C for 5-20 min.
The perovskite solar cell, wherein FAFa modification can effectively improve photovoltaic parameters such as short-circuit current, open-circuit voltage, filling factor, photoelectric conversion efficiency and the like of the device.
The FAFa modification layer can effectively reduce the SnO of the electron transport layer 2 The surface roughness of the film is easier to deposit on to obtain high quality perovskite film.
The FAFa modification layer can effectively reduce the SnO of the electron transport layer 2 The surface defect of the film can improve the conductivity of the electron transport layer.
The FAFa modification layer can obtain a high-quality perovskite film by adjusting the growth process, so that the pores on the bottom surface of the perovskite film are reduced, the roughness of the surface interface is reduced, and meanwhile, the perovskite crystallization quality is improved.
The FAFa modification layer, wherein, can construct chemical bridge at n/i interface so as to raise interface contact performance.
The FAFa modification layer can effectively reduce defect density in the perovskite film and inhibit non-radiative recombination.
(III) beneficial effects
According to the modification method of the perovskite solar cell n/i interface, provided by the invention, the formamidine formate (FAFa) modification layer is introduced between the electron transport layer and the perovskite active layer, defects on the surface of the electron transport layer can be passivated through electrostatic interaction, the conductivity of the electron transport layer is improved, the perovskite crystallization process can be regulated, a high-quality perovskite film with high crystallinity and low defect density is obtained, in addition, the interface contact performance can be optimized through chemically bridging the electron transport layer and the perovskite active layer, and the performance of a solar cell device is greatly improved. The invention provides a new thought for n/i interface modification of the conventional perovskite solar cell and a wide prospect for further improving the performance of the conventional perovskite solar cell.
Drawings
FIG. 1 is a schematic diagram of the structure of a perovskite solar cell of the present invention;
FIG. 2 shows the SnO before and after modification of FAFa at different concentrations in the preferred embodiment of the present invention 2 Roughness of the surface;
FIG. 3 is a graph showing FTIR spectra and conductivity before and after FAFa modification in a preferred embodiment of the present invention;
FIG. 4 is an SEM image of perovskite thin films before and after modification with different concentrations of FAFa in a preferred embodiment of the invention;
FIG. 5 is an AFM image of perovskite thin films before and after modification with different concentrations of FAFa in a preferred embodiment of the invention;
FIG. 6 is a cross-sectional SEM of a device before and after modification of FAFa at different concentrations in a preferred embodiment of the present invention;
FIG. 7 is a graph showing the PL and TRPL spectra of perovskite thin films before and after FAFa modification at various concentrations in a preferred embodiment of the invention;
FIG. 8 is a J-V curve of a device before and after FAFa modification at different concentrations in a preferred embodiment of the present invention.
Description of the embodiments
The present invention will be described in further detail with reference to the preferred embodiments and the complete test results, and in the following description, further details are set forth in order to provide a thorough understanding of the present invention, and persons skilled in the art may make similar generalizations and deductions according to the practical circumstances without departing from the spirit of the invention, and therefore should not limit the scope of the present invention in the context of this particular embodiment.
The perovskite solar cell provided by the invention, as shown in figure 1, comprises a transparent conductive substrate 1, an electron transport layer 2, a formamidine formate modification layer 3, a perovskite active layer 4, a hole transport layer 5 and a metal electrode 6.
The formamidine formate modification layer is a material simultaneously comprising carboxyl and amino, wherein the carboxyl and the amino can deactivate charge defects through electrostatic interaction, so that different defects can be simultaneously deactivated by utilizing a bifunctional molecule. According to previous literature reports, there are a large number of holes and deep level traps at the perovskite bottom interface, with defect densities even higher than on the perovskite top surface. In addition, the electron transport layer 2 is an inorganic compound SnO 2 Many defects, such as surface dangling bonds, hydroxyl groups, and two typical O vacancies and Sn interstitial impurities, are inevitably introduced during the preparation process, which not only results in non-radiative recombination, but also hinders efficient extraction and transport of electrons. According to the invention, by providing a unique strategy, the formamidine formate modification layer is added between the electron transport layer and the perovskite active layer, so that the interface performance can be effectively optimized, and the high-quality perovskite solar cell is obtained, and the performance of the solar cell is greatly improved. Therefore, the research of the passivation of the bottom interface of the perovskite by the formamidine formate has great research prospect.
The preparation method of the formamidine formate solution comprises the following steps: the formamidine formate will be dissolved using IPA as the solvent. Firstly, 1 mg,5 mg and 10 mg of formamidine formate are respectively weighed by a precise balance, put into a small bottle, and thenTo the vial was added 1 mL IPA and stirred until formamidine formate was completely dissolved to give 1 mg mL each -1 ，5 mg mL -1 ，10 mg mL -1 The present invention designates different concentrations of FAFa solution as 1-FAFa,5-FAFa,10-FAFa, respectively.
The FAFa modification layer can change SnO 2 For the study of FAFa treatment on the surface of the film on SnO 2 Influence of film surface morphology, the invention modifies the SnO with different concentration of FAFa 2 The film surface was subjected to Atomic Force Microscope (AFM) testing. As shown in FIG. 2, it can be seen that SnO is not treated with FAFa solution 2 The film has larger surface roughness, and SnO is obtained after spin coating FAFa solution 2 Reduced surface roughness, wherein 5-FAFa modified SnO 2 The roughness is most obviously reduced, and the flatter and denser film surface is beneficial to the subsequent deposition of the high-quality perovskite film.
The FAFa modification layer can reduce SnO 2 Surface defects increase the conductivity of the electron transport layer. The invention relates to the SnO modified by FAFa 2 Fourier transform infrared spectroscopy (FTIR) testing was performed as shown in fig. 3 a. With SnO 2 Compared with SnO 2 The stretching vibration peak of C=O belonging to FAFa appears on the FAFa film, and the peak position is from original 1732 cm -1 Move to 1724 cm -1 Indicating that FAFa is indeed identical to SnO 2 Interaction occurs. Furthermore, snO 2 548 and cm of the Sn-O stretching vibration -1 The peak position at the position 568 cm after FAFa modification -1 Higher wavenumber shifts at. This means that Fa anions coordinate to uncomplexed Sn by electrostatic coupling or Lewis acid base complexation 4+ Bonding to thereby cause SnO 2 Surface defects are reduced. To further investigate FAFa treatment versus SnO 2 Influence of film conductivity, the invention is characterized in that ITO/Au/SnO 2 SnO modified by FAFa with different concentration under dim light condition based on/Au structure 2 The film was subjected to current density-voltage (J-V) measurements as shown in FIG. 3 b. Unmodified SnO 2 The conductivity of the film was 1.04×10 -3 mS cm -1 When the concentration is 5 mg mL -1 After FAFa modification, the conductivity is significantly improvedUp to 1.72×10 - 3 mS cm -1 . The electron transport layer with higher conductivity is beneficial to promoting the extraction and transport of carriers, thereby improving the device performance.
The FAFa interface modification can obtain a high-quality perovskite film by regulating the growth process. The invention characterizes SnO under the modification of FAFa with different concentrations by a Scanning Electron Microscope (SEM) and an AFM 2 Surface morphology of perovskite thin films deposited on the thin films. FIG. 4 shows 1 mg mL of unmodified -1 、5 mg mL -1 、10 mg mL -1 The surface morphology of the perovskite film on the FAFa interface modification layer. It can be seen that the surface morphology of the perovskite modified by the FAFa is cleaner and more uniform, which indicates that the FAFa interface modification is beneficial to the growth of perovskite crystals. FIG. 5 also shows that the perovskite thin film surface roughness is determined by SnO-based 2 Is reduced to 39.0 nm based on SnO 2 30.9. 30.9 nm of 5-FAFa, a more planar and dense film is advantageous for reducing non-radiative recombination caused by defects. FIG. 6 shows SnO with FAFa interface modification 2 The cross-section SEM of the perovskite film prepared above the film can see that the perovskite film has obvious and more crystal boundaries under the condition of no modification, and after being processed by FAFa, the perovskite film has larger crystal grains and shallower crystal boundary ravines corresponding to the film thickness and fewer holes at the interface of the perovskite bottom, which is beneficial to reducing the recombination loss at the crystal boundary, accelerating the extraction and transmission of photo-generated carriers and reducing the defect state density, and further proves that the FAFa modification is beneficial to improving the film forming quality of the perovskite film.
The FAFa interface modification is capable of constructing chemical bridges at the n/i interface to enhance interface contact performance. Research has shown that Fa anions are more prone to SnO 2 Surface bonding, so SnO 2 The surface-repulsive FA cations may preferentially react with PbI in the perovskite precursor 2 Interact and act as nucleation sites for perovskite growth. Thus, FAFa treatment can be achieved by treatment with SnO 2 And a chemical bridge is established between the perovskite and the perovskite to repair structural defects (such as gaps), so that the contact characteristic at the bottom interface of the perovskite is improved.
The FAFa interface modification can effectively reduce the defect density of the perovskite film and inhibit non-radiative recombination of carriers. The present invention measures Photoluminescence (PL) and Time Resolved Photoluminescence (TRPL) spectra of perovskite thin films modified with FAFa at different concentrations, as shown in fig. 7 a. Compared with a non-modified control perovskite film, the PL intensity of the perovskite film on the 5-FAFa interface modification layer is obviously improved, and the FAFa can fully show that the defect of the perovskite film can be effectively reduced and the non-radiative recombination is inhibited. Furthermore, it was observed that after 5-FAFa modification, the PL peak blue shifted from 820 nm to 795 nm, verifying effective annihilation of the tail defects. TRPL also demonstrates similar results, as shown in fig. 7b, TRPL decay curves can be well fitted with a bi-exponential decay function, while the present invention also estimates the average carrier lifetime from the fitting results. In the case of 5-FAFa modification, the average carrier lifetime of the perovskite increased significantly from 219.57 ns to 230.35 ns, which means that manipulation of the growth process with FAFa can significantly improve the crystalline quality of the perovskite, effectively inhibiting the non-radiative recombination pathway of the perovskite thin film.
The FAFa interface modification can optimize the performance of a perovskite solar cell device, and the invention prepares a conventional planar perovskite solar cell by adopting a two-step method, and the device structure is ITO/SnO 2 Formamidine formate modification layer/FAPbI 3 perovskite/Spiro-OMeTAD/Au. FIG. 8 is a typical J-V curve of a device without modification and modified n/i interface with different concentrations of FAFa under one sun light (AM1.5G, 100 mW/cm 2 ) An effective area of 0.089 cm 2 Is a perovskite solar cell of (a). An efficiency of 21.48% and a 23.34 mA cm was finally obtained -2 An open circuit voltage of 1.112V and a fill factor of 82.74%. The performance of the device can be obviously improved by introducing the FAFa interface modification layer, and the optimal concentration of the FAFa solution is 5 mg mL -1 . The invention provides a thinking for further improving the performance of the conventional perovskite solar cell.
The following text refers to the abbreviations used in the present application:
IPA （isopropyl alcohol）
FAFa （formamidine formate）
ITO（Indium tin oxide）
MAI（methylammouniumiodide）
FAI（formamidiniumiodide）
Spiro-OMeTAD （2,2’,7,7’-tetrakis (N,N-di-p-methoxyphenyl -amine)-9,9’-spirobifluorene ）
the above description is illustrative of the preferred embodiments of the invention, which helps those skilled in the art to more fully understand the technical solution of the invention, and also can excite new ideas in the perovskite solar cell field, change the original thinking mode, and make great contribution to the improvement of the performance of conventional perovskite solar cells. It should be understood that, to those skilled in the art to which the present invention pertains, several simple deductions and changes can be made without departing from the inventive concept, and these should be considered as falling within the scope of the present invention.

Claims (8)

1. A perovskite solar cell comprises a transparent conductive substrate, an electron transport layer, an n/i interface modification layer, a perovskite active layer, a hole transport layer and a metal electrode, and is characterized in that,
the n/i interface modification layer is formamidine formate material (FAFa for short), and the molecular structure of the formamidine formate material is
Figure QLYQS_1
；
The perovskite solar cell is a conventional perovskite solar cell, and the n/i interface modification layer is prepared between the electron transport layer and the perovskite active layer.
2. The perovskite solar cell according to claim 1, wherein the preparation method of the n/i interface modification layer FAFa comprises the following steps:
s1: respectively weighing formamidine formate materials of 1-20 mg by a precision balance, dissolving in an organic solvent of 1 mL until the formamidine formate materials are completely dissolved, and preparing FAFa solutions with different concentrations for comparison; the organic solvents include, but are not limited to, IPA;
s2: spin-coating the prepared FAFa solution on the prepared electron transport layer at 1000-4000 rpm for 20-60 s, and annealing at 80-150deg.C for 5-20 min.
3. The perovskite solar cell of claim 1, wherein FAFa modification is effective to increase photovoltaic parameters such as short circuit current, open circuit voltage, fill factor, photoelectric conversion efficiency, etc. of the device.
4. The perovskite solar cell of claim 1, wherein FAFa is effective to reduce electron transport layer SnO 2 The surface roughness of the film is easier to deposit on to obtain high quality perovskite film.
5. The perovskite solar cell of claim 1, wherein FAFa significantly reduces the electron transport layer SnO 2 The surface defect of the film can improve the conductivity of the electron transport layer.
6. The perovskite solar cell according to claim 1, wherein FAFa interface modification can obtain a high quality perovskite thin film by adjusting the growth process, so that the pores on the bottom surface of the perovskite thin film are reduced, the roughness of the surface interface is reduced, and meanwhile, the perovskite crystallization quality is improved.
7. The perovskite solar cell of claim 1, wherein FAFa interface modification is capable of constructing chemical bridges at the n/i interface to enhance interface contact performance.
8. The perovskite solar cell of claim 1, wherein the FAFa interface modification is effective to reduce defect density in the perovskite thin film and inhibit non-radiative recombination.
CN202310364607.7A 2023-04-07 2023-04-07 Modification method of n/i interface of perovskite solar cell Pending CN116367562A (en)

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