CN113241411A - FAPBI3 perovskite solar cell based on in-situ reaction and preparation method thereof - Google Patents

FAPBI3 perovskite solar cell based on in-situ reaction and preparation method thereof Download PDF

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CN113241411A
CN113241411A CN202110461288.2A CN202110461288A CN113241411A CN 113241411 A CN113241411 A CN 113241411A CN 202110461288 A CN202110461288 A CN 202110461288A CN 113241411 A CN113241411 A CN 113241411A
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fapbi3
perovskite
thin film
solar cell
vacuum
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陈炜
张文君
蒋昭毅
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Huazhong University of Science and Technology
Ezhou Institute of Industrial Technology Huazhong University of Science and Technology
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Huazhong University of Science and Technology
Ezhou Institute of Industrial Technology Huazhong University of Science and Technology
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    • H—ELECTRICITY
    • H10—SEMICONDUCTOR DEVICES; ELECTRIC SOLID-STATE DEVICES NOT OTHERWISE PROVIDED FOR
    • H10K—ORGANIC ELECTRIC SOLID-STATE DEVICES
    • H10K71/00—Manufacture or treatment specially adapted for the organic devices covered by this subclass
    • H10K71/10—Deposition of organic active material
    • H10K71/12—Deposition of organic active material using liquid deposition, e.g. spin coating
    • H—ELECTRICITY
    • H10—SEMICONDUCTOR DEVICES; ELECTRIC SOLID-STATE DEVICES NOT OTHERWISE PROVIDED FOR
    • H10K—ORGANIC ELECTRIC SOLID-STATE DEVICES
    • H10K30/00—Organic devices sensitive to infrared radiation, light, electromagnetic radiation of shorter wavelength or corpuscular radiation
    • H10K30/30—Organic devices sensitive to infrared radiation, light, electromagnetic radiation of shorter wavelength or corpuscular radiation comprising bulk heterojunctions, e.g. interpenetrating networks of donor and acceptor material domains
    • H—ELECTRICITY
    • H10—SEMICONDUCTOR DEVICES; ELECTRIC SOLID-STATE DEVICES NOT OTHERWISE PROVIDED FOR
    • H10K—ORGANIC ELECTRIC SOLID-STATE DEVICES
    • H10K71/00—Manufacture or treatment specially adapted for the organic devices covered by this subclass
    • H10K71/40—Thermal treatment, e.g. annealing in the presence of a solvent vapour
    • Y—GENERAL TAGGING OF NEW TECHNOLOGICAL DEVELOPMENTS; GENERAL TAGGING OF CROSS-SECTIONAL TECHNOLOGIES SPANNING OVER SEVERAL SECTIONS OF THE IPC; TECHNICAL SUBJECTS COVERED BY FORMER USPC CROSS-REFERENCE ART COLLECTIONS [XRACs] AND DIGESTS
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    • Y02E—REDUCTION OF GREENHOUSE GAS [GHG] EMISSIONS, RELATED TO ENERGY GENERATION, TRANSMISSION OR DISTRIBUTION
    • Y02E10/00—Energy generation through renewable energy sources
    • Y02E10/50—Photovoltaic [PV] energy
    • Y02E10/549—Organic PV cells

Abstract

The invention discloses a preparation method of a FAPBI3 perovskite solar cell based on in-situ reaction, belonging to the field of photoelectric materials and devices. The method comprises the steps of dissolving lead iodide, formamidine iodide and lead formate in a DMF/DMSO mixed solvent according to a certain specific ratio to prepare FAPbI3 perovskite precursor solution, preparing FAPbI3 perovskite thin film on ITO transparent conductive glass sputtered with a hole transport material through a blade coating process, and annealing to form the FAPbI3 perovskite thin film with compact and smooth surface, high crystallinity, low defect state density and good crystal orientation. The FAPBI3 perovskite solar cell prepared by using the perovskite thin film has excellent photoelectric conversion efficiency and excellent device stability.

Description

FAPBI3 perovskite solar cell based on in-situ reaction and preparation method thereof
Technical Field
The invention relates to the field of new material solar cells, in particular to a FAPBI3 perovskite solar cell based on in-situ reaction and a preparation method thereof.
Background
At present, the demand of economic society for energy is continuously increased, and the traditional energy cannot adapt to the requirements of social development more and more due to the self limitation. But the problem of environmental pollution caused by the combustion of fossil energy is also receiving more and more attention. The development of renewable and environment-friendly new energy is imperative. Therefore, the development of renewable energy sources such as water energy, wind energy, solar energy, biomass energy, geothermal energy, tidal energy and the like is widely regarded. The solar energy has the advantages of inexhaustibility, economy, environmental protection and the like, and is important for the sustainable development of the society. Therefore, solar energy is expected as an important energy supply for human beings in the future, and development of a novel solar cell having low cost and high efficiency has become a research hotspot in recent years.
In recent years, research on novel solar cells with low price, high efficiency and large area is rapidly advanced, wherein the development of the novel solar cells belongs to perovskite type solar cells most rapidly, and the photoelectric conversion efficiency is improved from 3.8% to 25.2% in less than ten years and exceeds that of crystalline silicon solar cells. The perovskite material has the characteristics of excellent photoelectric property, simple preparation process, low production cost and the like, so that the perovskite material has the potential of being commercially applied as an ideal photoelectric device.
However, the efficiency of perovskite solar cells is much lower than the schottky-queither efficiency of single cell cells. Broadening the absorption spectrum of the cell by lowering the band width of the film has proven to be an effective strategy to improve the photovoltaic performance of the device. The combination of methyl ammonium lead iodide (MAPbI3) with formamide lead iodide (FAPbI3) and mixtures thereof in perovskite solar cells has been extensively studied. Compared with MAPbI3, FAPbI3 has better thermal stability and the forbidden band distance is closer to the Shockley-Queisser limit, which makes FAPbI3 the most ideal perovskite layer of unijunction PSCs, but FAPbI3 has the problem of instability of the black phase at room temperature, and previous methods for solving this problem include mixing FAPbI3 with a combination of methylammonium (MA +), cesium (Cs +) and bromide (Br-), however, at the cost of blue-shift absorption and phase separation.
Disclosure of Invention
The embodiment of the application provides a preparation method of the FAPBI3 perovskite solar cell based on in-situ reaction, and improves the photoelectric conversion performance and stability of the FAPBI3 perovskite solar cell.
The embodiment of the application provides a preparation method of a FAPBI3 perovskite solar cell based on in-situ reaction, which comprises the following steps:
dissolving lead iodide, formamidine iodide and lead formate in a DMF/DMSO mixed solvent to prepare an FAPbI3 perovskite precursor solution;
step (2), sputtering a hole transport layer on the ITO transparent conductive glass;
step (3), coating the FAPBI3 perovskite precursor solution on the hole transport layer, and annealing to obtain a FAPBI3 perovskite thin film;
step (4), evaporating an electron transport layer on the FAPBI3 perovskite film in vacuum;
and (5) evaporating an interface modification layer and a metal electrode on the electron transport layer in vacuum.
Furthermore, the adding ratio of lead iodide, formamidine iodide and lead formate in the FAPBI3 perovskite precursor solution in the step (1) is 1 (1.04-1.1) to (0.015-0.05).
Further, the concentration of the FAPBI3 perovskite precursor solution in the step (1) is 0.8-1.5M.
Further, the material of the hole transport layer in the step (2) is NixCu1-xThe doping ratio of O and Cu is 0-5%, and the sputtering vacuum degree is 1 multiplied by 10-4～5×10-4(ii) a The sputtering working air pressure is 1mbar to 10 mbar; the sputtering power is 60-150W.
Further, the FAPBI3 perovskite precursor solution is coated in the step (3), the blade coating speed is 5-30 mm/s, the blowing pressure is 0-20 pis, the annealing temperature is 125-150 ℃, and the annealing time is 10-60 min.
Further, the electron transport layer in the step (4) is made of a fullerene film, the fullerene film is C60, the thickness of the fullerene film is 20-80 nm, and the evaporation vacuum degree reaches 1 × 10-5～5×10-4Pa。
Further, the step (5) isThe interface modification layer is made of LiF or BCP, LiF or BCP powder is deposited on the FAPbI3 perovskite film in a vacuum evaporation mode, the thickness of the interface modification layer is 3-10 nm, and the evaporation vacuum degree is 1 multiplied by 10-5～5×10-4Pa。
Further, in the step (5), a metal electrode is vacuum-evaporated on the interface modification layer, the thickness of the metal electrode is 50-300 nm, and the evaporation vacuum degree is 1 × 10-5～5×10-4Pa。
The technical scheme provided in the embodiment of the application has at least the following technical effects:
the invention provides a preparation method of an FAPBI3 perovskite solar cell based on in-situ reaction based on an additive adding mode, wherein formamidine acetate is introduced through the in-situ reaction to prepare formamidine formate, so that main lattice defect halide vacancies in an FAPBI3 perovskite film are removed, and non-radiative recombination in the cell is reduced. By introducing formamidine formate into a precursor solution in situ, the FAPBI3 perovskite thin film with higher crystallinity and larger grain size is prepared, and the photoelectric conversion performance and stability of the FAPBI3 perovskite solar cell are improved.
Drawings
FIG. 1 is a schematic diagram of a perovskite solar cell structure;
FIG. 2 in situ reaction addition reaction equation;
fig. 3 is an SEM image of FAPbI3 perovskite thin film prepared by the methods of the present application;
fig. 4 is an XRD pattern of FAPbI3 perovskite thin film prepared by the process of the present application;
FIG. 5 is a comparison of cell efficiencies of FAPBI3 perovskite thin film prepared by in situ reaction with introduction of formamidine acetate preparation and FAPBI3 perovskite thin film prepared by post-addition.
Detailed Description
In order to make the objects, technical solutions and advantages of the present invention more apparent, the present invention is described in further detail below with reference to the accompanying drawings and embodiments. It should be understood that the specific embodiments described herein are merely illustrative of the invention and are not intended to limit the invention. In addition, the technical features involved in the embodiments of the present invention described below may be combined with each other as long as they do not conflict with each other.
Fig. 1 is a schematic diagram of a perovskite solar cell structure. As shown in fig. 1, the solar cell is composed of an ITO transparent conductive glass 1, a hole transport layer 2, a perovskite thin film 3, an electron transport layer 4, an interface modification layer 5, and a metal electrode 6 from bottom to top.
The perovskite film is an FAPbI3 film prepared by introducing formamidine formate through in-situ reaction, the addition ratio of lead iodide, formamidine iodide and lead formate is 1 (1.04-1.1): 0.015-0.05), the FAPbI3 perovskite film with higher crystallinity and larger grain size is prepared by introducing formamidine formate in-situ reaction, and the non-radiative recombination in a battery is reduced;
wherein the sheet resistance of the ITO conductive glass is 5-25 omega, and the transmittance is 85-95%;
optionally, the hole transport layer is NixCu1-xThe doping proportion of O and Cu is 0-5%, and the thickness is 10-50 nm;
optionally, the electron transport layer is a fullerene film, the fullerene film is C60;
optionally, the interface modification layer is LiF (with a thickness of 0.5-5 nm), BCP (with a thickness of 1-20 nm), or the like.
Optionally, the metal electrode is Cu and Ag, and the thickness is 50-300 nm;
the application provides a preparation method of a FAPBI3 perovskite solar cell based on in-situ reaction, which comprises the following steps:
dissolving lead iodide, formamidine iodide and lead formate in a DMF/DMSO mixed solvent to prepare an FAPbI3 perovskite precursor solution;
step (2), sputtering a hole transport layer on the ITO transparent conductive glass;
step (3), coating FAPBI3 perovskite precursor solution on the hole transport layer, and annealing to obtain a FAPBI3 perovskite film;
step (4), evaporating an electron transport layer on the FAPBI3 perovskite film in vacuum;
and (5) evaporating an interface modification layer and a metal electrode on the electron transport layer in vacuum.
Optionally, the adding ratio of lead iodide, formamidine iodide and lead formate in the FAPBI3 perovskite precursor solution in the step (1) is 1 (1.04-1.1) to (0.015-0.05).
Optionally, the concentration of the FAPbI3 perovskite precursor solution in the step (1) is 0.8M-1.5M.
Optionally, the material of the hole transport layer in the step (2) is NixCu1-xThe doping ratio of O and Cu is 0-5%, and the sputtering vacuum degree is 1 multiplied by 10-4～5×10-4(ii) a The sputtering working air pressure is 1mbar to 10 mbar; the sputtering power is 60-150W.
Optionally, the FAPBI3 perovskite precursor solution is coated in the step (3), the blade coating speed is 5-30 mm/s, the blowing pressure is 0-20 pis, the annealing temperature is 125-150 ℃, and the annealing time is 10-60 min.
Optionally, in the step (4), the electron transport layer is made of a fullerene film, the fullerene film is C60, the thickness is 20-80 nm, and the evaporation vacuum degree reaches 1 × 10-5～5×10-4Pa。
Optionally, the material of the interface modification layer in the step (5) is LiF or BCP, LiF or BCP powder is deposited on the FAPbI3 perovskite film in a vacuum evaporation mode, the thickness of the interface modification layer is 3-10 nm, and the evaporation vacuum degree is 1 × 10-5～5×10-4Pa。
In the step (5), a metal electrode is evaporated on the interface modification layer in vacuum, the thickness of the metal electrode is 50-300 nm, and the evaporation vacuum degree is 1 multiplied by 10-5～5×10-4Pa。
Figure 2 in situ reaction addition reaction equation. As shown in figure 2, the invention provides a preparation method of FAPBI3 perovskite solar cell based on in-situ reaction based on an additive adding mode, wherein formamidine acetate is introduced through the in-situ reaction to prepare formamidine formate, so that main lattice defect halide vacancies in a FAPBI3 perovskite thin film are removed, and non-radiative recombination in the cell is reduced. By introducing formamidine formate into a precursor solution in situ, the FAPBI3 perovskite thin film with higher crystallinity and larger grain size is prepared, and the photoelectric conversion performance and stability of the FAPBI3 perovskite solar cell are improved.
Example one
And (1) sequentially carrying out ultrasonic treatment on the etched ITO conductive glass in ultrapure water, a cleaning agent, ultrapure water, acetone and ethanol for 15min respectively, blow-drying by nitrogen and then putting the ITO conductive glass into the reactor to obtain a clean ITO substrate.
Dissolving lead iodide, formamidine iodide and lead formate in the proportion of 1 (1.04-1.1): 0.02 in a DMF/DMSO mixed solvent to prepare an FAPbI3 perovskite precursor solution, and stirring at room temperature for 6-24 hours;
step (3) carrying out ultraviolet ozone treatment on the ITO substrate cleaned in the step (1) for 15 minutes;
the sputtering vacuum degree of the step (4) is 1 x 10-4The sputtering working pressure is controlled between 3mbar, the sputtering power is 100W, and Ni is added0.97Cu0.03O is sputtered on the ITO;
step (5) sputtering Ni in the step (4)0.97Cu0.03Putting the ITO of O on blade coating equipment, adding the solution obtained in the step (2) and dropwise adding the solution on an ITO substrate to be coated, wherein the blade coating speed is 10mm/s, the air blowing pressure is 20pis, the annealing temperature is 150 ℃, and the annealing time is 30 min;
step (6) vacuum evaporating C60 on the perovskite thin film obtained in step (5), wherein the vacuum degree reaches 3 x 10-4Pa, thickness of 30 nm;
and (7) performing vacuum evaporation on the electron transmission layer in the step (6) by adopting a vacuum evaporation technology to perform vacuum evaporation on 5nm BCP, and then performing evaporation on 100nm metal electrode Cu to prepare the perovskite solar cell.
And (8) testing the photoelectric conversion efficiency of the cell under the standard test condition (AM 1.5G illumination).
Fig. 3 is an SEM image of FAPbI3 perovskite thin film prepared by the methods of the present application; fig. 4 is an XRD pattern of FAPbI3 perovskite thin film prepared by the process of the present application. As shown in fig. 3 and fig. 4, by introducing formamidine formate into the precursor solution in situ, a FAPbI3 perovskite thin film with higher crystallinity and larger grain size is prepared, and the photoelectric conversion performance and stability of the FAPbI3 perovskite solar cell are improved.
Comparative example
And (1) sequentially carrying out ultrasonic treatment on the etched ITO conductive glass in ultrapure water, a cleaning agent, ultrapure water, acetone and ethanol for 15min respectively, blow-drying by nitrogen and then putting the ITO conductive glass into the reactor to obtain a clean ITO substrate.
Step (2), mixing lead iodide, formamidine iodide 1: dissolving 1 and 2 mol% of formamidine formate in a DMF/DMSO mixed solvent to prepare an FAPbI3 perovskite precursor solution, and stirring at room temperature for 6-24 hours;
step (3) carrying out ultraviolet ozone treatment on the ITO substrate cleaned in the step (1) for 15 minutes;
the sputtering vacuum degree of the step (4) is 1 x 10-4The sputtering working pressure is controlled between 3mbar, the sputtering power is 100W, and Ni is added0.97Cu0.03O is sputtered on the ITO;
step (5) sputtering Ni in the step (4)0.97Cu0.03Putting the ITO of O on blade coating equipment, adding the solution obtained in the step (2) and dropwise adding the solution on an ITO substrate to be coated, wherein the blade coating speed is 10mm/s, the air blowing pressure is 20pis, the annealing temperature is 150 ℃, and the annealing time is 30 min;
step (6) vacuum evaporating C60 on the perovskite thin film obtained in step (5), wherein the vacuum degree reaches 3 x 10-4Pa, thickness of 30 nm;
and (7) performing vacuum evaporation on the electron transmission layer in the step (6) by adopting a vacuum evaporation technology to perform vacuum evaporation on 5nm BCP, and then performing evaporation on 100nm metal electrode Cu to prepare the perovskite solar cell.
And (8) testing the photoelectric conversion efficiency of the cell under the standard test condition (AM 1.5G illumination).
The implementation effect is as follows: the perovskite solar cell samples were tested for change over time under continuous irradiation of standard solar light intensity for 1000 hours.
FIG. 5 is a comparison of cell efficiencies of FAPBI3 perovskite thin film prepared by introducing formamidine acetate preparation agent in situ reaction and FAPBI3 perovskite thin film prepared by post-addition.
It will be understood by those skilled in the art that the foregoing is merely a preferred embodiment of the present invention, and is not intended to limit the invention, and that any modification, equivalent replacement, or improvement made within the spirit and principle of the present invention should be included within the scope of the present invention.

Claims (9)

1. A preparation method of a FAPBI3 perovskite solar cell based on in-situ reaction is characterized by comprising the following steps:
step (1): dissolving lead iodide, formamidine iodide and lead formate in a DMF/DMSO mixed solvent to prepare FAPbI3 perovskite precursor solution;
step (2): sputtering a hole transport layer on the ITO transparent conductive glass;
and (3): coating the FAPBI3 perovskite precursor solution on the hole transport layer, and annealing to obtain a FAPBI3 perovskite thin film;
and (4): vacuum evaporating an electron transport layer on the FAPBI3 perovskite film;
and (5): and vacuum evaporating an interface modification layer and a metal electrode on the electron transport layer.
2. The preparation method according to claim 1, wherein the addition ratio of lead iodide, formamidine iodide and lead formate in the FAPBI3 perovskite precursor solution in the step (1) is 1 (1.04-1.1) to (0.015-0.05).
3. The method according to claim 1, wherein the concentration of the FAPbI3 perovskite precursor solution in step (1) is 0.8M to 1.5M.
4. The method according to claim 1, wherein the material of the hole transport layer in the step (2) is Ni0.97Cu0.03The doping ratio of O and Cu is 0-5%, and the sputtering vacuum degree is 1 multiplied by 10-4～5×10-4(ii) a The sputtering working air pressure is 1mbar to 10 mbar; the sputtering power is 60-150W.
5. The method of claim 1, wherein the FAPBI3 perovskite precursor solution is coated in the step (3), the blade coating speed is 5-30 mm/s, the air blowing pressure is 0-20 pis, the annealing temperature is 125-150 ℃, and the annealing time is 10-60 min.
6. The method according to any one of claims 1 to 5, wherein the electron transport layer in step (4) is a fullerene thin film, the fullerene thin film is C60, the fullerene thin film has a thickness of 20 to 80nm, and the degree of vacuum for evaporation is 1 x 10-5～5×10-4Pa。
7. The method according to any one of claims 1 to 5, wherein the interface modification layer in the step (5) is made of LiF or BCP, LiF or BCP powder is deposited on the FAPBI3 perovskite film in a vacuum evaporation mode, the thickness of the interface modification layer is 3-10 nm, the evaporation vacuum degree is 1 x 10-5～5×10-4Pa。
8. The method according to any one of claims 1 to 5, wherein in the step (5), a metal electrode is vacuum-evaporated on the interface modification layer, the thickness of the metal electrode is 50 to 300nm, and the evaporation vacuum degree is 1 x 10-5～5×10-4Pa。
9. An FAPBI3 perovskite solar cell based on in-situ reaction, characterized in that the FAPBI3 perovskite solar cell is prepared by the preparation method of any one of claims 1 to 8.
CN202110461288.2A 2021-04-27 2021-04-27 FAPBI3 perovskite solar cell based on in-situ reaction and preparation method thereof Pending CN113241411A (en)

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Application publication date: 20210810