CN113113541A - Method for passivating perovskite solar cell interface defects by using sodium bis (trifluoromethyl) sulfonyl imide - Google Patents
Method for passivating perovskite solar cell interface defects by using sodium bis (trifluoromethyl) sulfonyl imide Download PDFInfo
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Abstract
The invention discloses a method for passivating perovskite solar cell interface defects by using sodium bistrifluoromethylsulfonyl imide, belonging to the technical field of perovskite solar cells and comprising the following steps: s1, cleaning the etched FTO conductive glass, S2, and removing TiO2Uniformly spreading the quantum dot solution on the surface of FTO conductive glass to prepare an electron transport layer, transferring the spin-coated film into a muffle furnace, sintering at 450 ℃ for 30min, S3, cooling to room temperature, and performing TiO deposition2The film was spin coated with NaTFSI acetonitrile solution. In the invention, solution spin coating is adopted to coat on plane TiO2A layer of NaTFSI is prepared on the film and used for modifying the interface between the electron transport layer and the perovskite and assembling the electron transport layer and the perovskite into PSCs, the NaTFSI modification layer can not only improve the crystallinity of the perovskite film,the non-radiative recombination loss of the perovskite thin film is reduced, and the energy level structure of the surface of the ETL can be optimized to be more matched with the energy level of the perovskite, so that the extraction and transmission efficiency of electrons between interfaces is accelerated.
Description
Technical Field
The invention relates to the technical field of perovskite solar cells, in particular to a method for passivating interface defects of perovskite solar cells by using sodium bistrifluoromethylsulfonyl imide.
Background
Organic-inorganic hybrid Perovskite Solar Cells (PSCs) are considered as one of the most promising new solar cells, with a rapid increase in Photoelectric Conversion Efficiency (PCE) from the first reported 3.8% to the present 25.5%. Perovskite type crystal (ABX)3) There are many perovskite crystals whose a-site ion includes organic cation methylamine (CH), which is a light-absorbing active material in solar cells3NH3 +,MA+) Formamidine (NH ═ CHNH)3 +,FA+) Inorganic cation Cs+Etc.; the divalent metal ion B includes Pb2+、Sn2+Etc., and X ions are generally halide ions, e.g. I-、Br-Cl-, etc. The perovskite material has the advantages of high absorption coefficient, long carrier diffusion length, wide absorption range and the like, so that the perovskite material has wide application in photoelectric devices.
In addition to the perovskite photoactive layer, a conductive glass substrate, an Electron Transport Layer (ETL), a Hole Transport Layer (HTL), a metal electrode, and the like are known in conventional PSCs device structures. The ETL can promote the extraction of electrons, effectively reduce the energy barrier for the electrons to jump from the perovskite light absorption layer to the anode, and play a role in blocking holes, and the quality of the ETL is one of the main factors determining the performance of the PSCs. TiO 22Due to its high electron injection rate, stable chemical properties and low price, the material is the most common electron transport material in PSCs. Solution process of preparing TiO2Film watchThe surface has a large number of defects, and the defects can cause carriers to generate non-radiative recombination at the interface of the perovskite layer and the ETL and block charge transmission, so that the further improvement of the PCE of the device is severely restricted, and in addition, the non-radiative recombination can also induce the attenuation and hysteresis phenomena of the device efficiency.
Disclosure of Invention
The invention aims to provide a method for passivating perovskite solar cell interface defects by using sodium bistrifluoromethylsulfonyl imide, which adopts a solution spin coating method to carry out a planar TiO coating process2The NaTFSI modification layer can not only improve the crystallinity of the perovskite thin film and reduce the non-radiative recombination loss of the perovskite thin film, but also optimize the energy level structure of the ETL surface to enable the energy level structure to be more matched with the energy level of the perovskite, thereby accelerating the extraction and transmission efficiency of electrons between interfaces.
In order to achieve the above effects, the present invention provides the following technical solutions: a method for passivating perovskite solar cell interface defects by sodium bistrifluoromethylsulfonyl imide, comprising the steps of:
and S1, cleaning the etched FTO conductive glass.
S2, mixing TiO2And uniformly spreading the quantum dot solution on the surface of the FTO conductive glass to prepare an electron transport layer, and transferring the spin-coated film into a muffle furnace to be sintered for 30min at 450 ℃.
S3, cooling to room temperature, and dissolving in TiO2The film was spin coated with NaTFSI acetonitrile solution.
S4, placing the obtained product into a muffle furnace after spin coating, sintering the obtained product for 30min at the temperature of 450 ℃, cooling the obtained product to room temperature, transferring the obtained product into a plasma cleaning instrument, and carrying out plasma treatment for 10 min.
S5, feeding the treated FTO conductive glass into a glove box, and dropwise adding the perovskite precursor solution on the NaTFSI interface layer to prepare a perovskite layer.
S6, transferring the film to a heating table, and treating for 60min at the temperature of 100 ℃.
And S7, cooling to room temperature, spreading the Spiro-OMeTAD solution on the perovskite film for spin coating, and after the spin coating is finished, placing the film in a moisture-proof cabinet with the humidity of less than 15% for oxidation for 12 hours.
Further, the method also comprises the following steps:
oxidizing in a damp-proof cabinet for 12h, and then putting the damp-proof cabinet into a high vacuum coating machine, wherein the vacuum degree is less than 6.0 multiplied by 10-4And (5) evaporating an 80nm gold counter electrode in a Pa state to complete the assembly of the battery.
Further, in step S1, the cleaning of the etched FTO conductive glass includes the following steps:
s101, cleaning the etched FTO conductive glass with a cleaning agent, then sequentially placing the FTO conductive glass in absolute ethyl alcohol, acetone and isopropanol for ultrasonic cleaning for 30min each time, taking out the FTO conductive glass, and drying the residual solvent on the surface with nitrogen.
S102, placing the dried FTO conductive glass into an ultraviolet ozone cleaning machine, treating for 20min, then placing the FTO conductive glass into a plasma cleaning instrument, cleaning for 5min, and taking out for later use.
Further, in the step S2, spin coating is performed for 5S at 700rpm and 20S at 4000rpm, respectively.
Further, in step S5, the perovskite precursor liquid is prepared by:
0.5290g of PbI are weighed in a glove box respectively2，0.0743g PbBr20.0176g of CsI, 0.1874g of FAI and 0.0157g of MABr were dissolved in a mixed solution of 0.2mL of DMSO and 0.8mL of DMF, and the solution was stirred until the solution was completely dissolved to prepare a perovskite precursor solution.
Further, in step S7, the preparation method of the Spiro-OMeTAD solution is:
72.3mg of Spiro-OMeTAD was weighed in a glove box, dissolved in 1mL of chlorobenzene, and after completely dissolved by stirring, 17.5. mu.L of LiTFSI solution and 28.8. mu.L of 4-tBP were added and stirred uniformly to obtain a Spiro-OMeTAD solution.
Further, in the step S7, spin coating is performed for 10S at 1000rpm, 20S at 6500rpm, and the anti-solvent chlorobenzene is added dropwise at 25S.
The invention provides a method for passivating perovskite solar cell interface defects by using sodium bistrifluoromethylsulfonyl imide, which has the following beneficial effects:
in the invention, solution spin coating is adopted to coat on plane TiO2And preparing a layer of NaTFSI on the film, modifying an interface between the electron transport layer and the perovskite, and assembling the electron transport layer and the perovskite into PSCs. The NaTFSI modification layer can improve the crystallinity of the perovskite thin film, reduce the non-radiative recombination loss of the perovskite thin film, and optimize the energy level structure of the surface of the ETL to enable the energy level structure to be more matched with the energy level of the perovskite, so that the extraction and transmission efficiency of electrons between interfaces is accelerated.
Drawings
FIG. 1 is a flow chart of a method for passivating perovskite solar cell interface defects with sodium bistrifluoromethylsulfonylimide.
Detailed Description
The technical solution in the embodiments of the present invention will be clearly and completely described below with reference to the accompanying drawings in the embodiments of the present invention; it is obvious that the described embodiments are only a part of the embodiments of the present invention, and not all embodiments, and all other embodiments obtained by those skilled in the art without any inventive work are within the scope of the present invention.
The invention provides a technical scheme that: referring to fig. 1, a method for passivating perovskite solar cell interface defects by sodium bistrifluoromethylsulfonylimide comprises the following steps:
step one, cleaning the etched FTO conductive glass.
Cleaning the etched FTO conductive glass, comprising the following steps:
101) and cleaning the etched FTO conductive glass by using a cleaning agent, then sequentially placing the FTO conductive glass into absolute ethyl alcohol, acetone and isopropanol for ultrasonic cleaning for 30min each time, taking out the FTO conductive glass, and drying the residual solvent on the surface by using nitrogen.
102) And putting the dried FTO conductive glass into an ultraviolet ozone cleaning machine, treating for 20min, putting into a plasma cleaning instrument, cleaning for 5min, and taking out for later use.
Step two, TiO is added2And uniformly spreading the quantum dot solution on the surface of the FTO conductive glass to prepare an electron transport layer, and transferring the spin-coated film into a muffle furnace to be sintered for 30min at 450 ℃.
During the spin coating, 5s of spin coating is carried out under the condition of 700rpm, and 20s of spin coating is carried out under the condition of 4000 rpm.
Step three, cooling to room temperature, and dissolving in TiO2The film was spin coated with NaTFSI acetonitrile solution.
And step four, after spin coating, placing the mixture into a muffle furnace, sintering the mixture for 30min at the temperature of 450 ℃, cooling the mixture to room temperature, transferring the mixture into a plasma cleaning instrument, and carrying out plasma treatment for 10 min.
And fifthly, feeding the treated FTO conductive glass into a glove box, and dropwise adding the perovskite precursor solution on the NaTFSI interface layer to prepare a perovskite layer.
The preparation method of the perovskite precursor liquid comprises the following steps:
0.5290g of PbI are weighed in a glove box respectively2，0.0743g PbBr20.0176g of CsI, 0.1874g of FAI and 0.0157g of MABr were dissolved in a mixed solution of 0.2mL of DMSO and 0.8mL of DMF, and the solution was stirred until the solution was completely dissolved to prepare a perovskite precursor solution.
And step six, transferring the film to a heating table, and treating for 60min at the temperature of 100 ℃.
And seventhly, cooling to room temperature, spreading the Spiro-OMeTAD solution on the perovskite film for spin coating, and after the spin coating is finished, placing the film in a moisture-proof cabinet with the humidity of less than 15% for oxidation for 12 hours.
The preparation method of the Spiro-OMeTAD solution comprises the following steps:
72.3mg of Spiro-OMeTAD was weighed in a glove box, dissolved in 1mL of chlorobenzene, stirred until completely dissolved, and then 17.5. mu.L of LiTFSI solution and 28.8. mu.L of 4-tBP were added and stirred uniformly to obtain a Spiro-OMeTAD solution.
Wherein, spin coating 10s at 1000rpm, 20s at 6500rpm, and dripping chlorobenzene as anti-solvent at 25 s.
Eighthly, after oxidizing for 12 hours in a damp-proof cabinet, putting the damp-proof cabinet into a high vacuum coating machineVacuum degree less than 6.0 × 10-4And (5) evaporating an 80nm gold counter electrode in a Pa state to complete the assembly of the battery.
TiO before and after modification of NaTFSI2The properties of the electron transport layers were compared and are shown in table 1:
table 1: TiO before and after NaTFSI modification2Energy level parameter of electron transport layer
As can be seen from Table 1, NaTFSI modified TiO2Defect reduction and energy level matching at the interface of the electron transport layer and the perovskite layer.
The perovskite thin film processed by the NaTFSI becomes more uniform, and has larger-sized crystal grains and fewer crystal boundaries, the existence of the NaTFSI can favorably influence the growth of perovskite crystals, so that the quality of the perovskite thin film is improved, the cross sections of devices before and after the NaTFSI processing are respectively analyzed, the perovskite particle size in the processed device is obviously improved, and part of crystal grains longitudinally penetrating through the whole perovskite thin film are formed, so that the number of the crystal boundaries in the device is reduced, the reduction of the crystal boundaries in the device means the reduction of a carrier recombination center, the improvement of the transmission efficiency of a carrier is facilitated, and the improvement of the performance of a perovskite solar cell is of great importance.
By modifying titanium dioxide ETL with the NaTFSI interface layer, the size of perovskite crystal grains on the upper layer can be increased, grain boundaries are reduced, so that interface carrier recombination is reduced, conductivity of the ETL modified by NaTFSI is enhanced, work function is reduced, and the efficiency of the device is remarkably improved from 18.62% to 19.83% by optimizing the NaTFSI interface layer.
In the invention, solution spin coating is adopted to coat on plane TiO2Preparing a layer of NaTFSI on the film for modifying the interface between the electron transport layer and the perovskite and assembling the electron transport layer and the perovskitePSCs. The NaTFSI modification layer can improve the crystallinity of the perovskite thin film, reduce the non-radiative recombination loss of the perovskite thin film, and optimize the energy level structure of the surface of the ETL to enable the energy level structure to be more matched with the energy level of the perovskite, so that the extraction and transmission efficiency of electrons between interfaces is accelerated.
Although embodiments of the present invention have been shown and described, it will be appreciated by those skilled in the art that changes, modifications, substitutions and alterations can be made in these embodiments without departing from the principles and spirit of the invention, the scope of which is defined in the appended claims and their equivalents.
Claims (7)
1. A method for passivating perovskite solar cell interface defects by using sodium bistrifluoromethylsulfonyl imide is characterized by comprising the following steps:
s1, cleaning the etched FTO conductive glass;
s2, mixing TiO2Uniformly spreading the quantum dot solution on the surface of FTO conductive glass to prepare an electron transport layer, and transferring the spin-coated film into a muffle furnace to be sintered for 30min at 450 ℃;
s3, cooling to room temperature, and dissolving in TiO2Spinning and coating NaTFSI acetonitrile solution on the film;
s4, placing the obtained product into a muffle furnace after spin coating, sintering the obtained product for 30min at the temperature of 450 ℃, cooling the obtained product to room temperature, transferring the obtained product into a plasma cleaning instrument, and carrying out plasma treatment for 10 min;
s5, feeding the treated FTO conductive glass into a glove box, and dropwise adding a perovskite precursor solution on the NaTFSI interface layer to prepare a perovskite layer;
s6, transferring the film to a heating table, and treating for 60min at the temperature of 100 ℃;
and S7, cooling to room temperature, spreading the Spiro-OMeTAD solution on the perovskite film for spin coating, and after the spin coating is finished, placing the film in a moisture-proof cabinet with the humidity of less than 15% for oxidation for 12 hours.
2. The method for passivating perovskite solar cell interface defects with sodium bistrifluoromethylsulfonylimide according to claim 1, further comprising:
oxidizing in a damp-proof cabinet for 12h, and then putting the damp-proof cabinet into a high vacuum coating machine, wherein the vacuum degree is less than 6.0 multiplied by 10-4And (5) evaporating an 80nm gold counter electrode in a Pa state to complete the assembly of the battery.
3. The method for passivating perovskite solar cell interface defects by sodium bistrifluoromethylsulfonyl imide according to claim 1, wherein in the step S1, the cleaning of the etched FTO conductive glass comprises the following steps:
s101, cleaning the etched FTO conductive glass with a cleaning agent, then sequentially placing the FTO conductive glass in absolute ethyl alcohol, acetone and isopropanol for ultrasonic cleaning, performing ultrasonic cleaning for 30min each time, taking out the FTO conductive glass, and drying the residual solvent on the surface with nitrogen;
s102, placing the dried FTO conductive glass into an ultraviolet ozone cleaning machine, treating for 20min, then placing the FTO conductive glass into a plasma cleaning instrument, cleaning for 5min, and taking out for later use.
4. The method for passivating perovskite solar cell interface defects by using sodium bistrifluoromethylsulfonyl imide according to claim 1, wherein in the step S2, the spin coating is performed for 5S at 700rpm and 20S at 4000 rpm.
5. The method for passivating perovskite solar cell interface defects by using sodium bistrifluoromethylsulfonyl imide according to claim 1, wherein in the step S5, the perovskite precursor solution is prepared by:
0.5290g of PbI are weighed in a glove box respectively2，0.0743g PbBr20.0176g of CsI, 0.1874g of FAI and 0.0157g of MABr are dissolved in a mixed solution of 0.2ml of DMSO and 0.8ml of DMMF, and the solution is stirred until the solution is completely dissolved to prepare the perovskite precursor solution.
6. The method for passivating perovskite solar cell interface defects by using sodium bistrifluoromethylsulfonylimide according to claim 1, wherein in the step S7, a Spiro-OMeTAD solution is prepared by:
72.3mg of Spiro-OMeTAD was weighed in a glove box, dissolved in 1mL of chlorobenzene, and after completely dissolved by stirring, 17.5. mu. LLITFSI solution and 28.8. mu.L of 4-tBP were added and stirred uniformly to obtain a Spiro-OMeTAD solution.
7. The method for passivating perovskite solar cell interface defects by using sodium bistrifluoromethylsulfonyl imide according to claim 1, wherein in the step S7, 10S of spin coating is performed at 1000rpm, 20S of spin coating is performed at 6500rpm, and the anti-solvent chlorobenzene is added dropwise at 25S.
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