CN111628084A - Perovskite laminated solar cell and preparation method thereof - Google Patents

Perovskite laminated solar cell and preparation method thereof Download PDF

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CN111628084A
CN111628084A CN202010470649.5A CN202010470649A CN111628084A CN 111628084 A CN111628084 A CN 111628084A CN 202010470649 A CN202010470649 A CN 202010470649A CN 111628084 A CN111628084 A CN 111628084A
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solar cell
perovskite
mesoporous
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韩宏伟
胡玥
叶婷
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Huazhong University of Science and Technology
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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
    • H10K30/10—Organic devices sensitive to infrared radiation, light, electromagnetic radiation of shorter wavelength or corpuscular radiation comprising heterojunctions between organic semiconductors and inorganic semiconductors
    • 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
    • H10K30/50—Photovoltaic [PV] devices
    • H10K30/57—Photovoltaic [PV] devices comprising multiple junctions, e.g. tandem PV cells
    • 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
    • H10K30/80—Constructional details
    • H10K30/81—Electrodes
    • H10K30/82—Transparent electrodes, e.g. indium tin oxide [ITO] electrodes
    • 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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    • H10K30/87—Light-trapping means
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Abstract

The invention belongs to the technical field of solar cell preparation, and particularly relates to a perovskite laminated solar cell and a preparation method thereof. Compared with the existing flat plate structure, the mesoporous structure has the advantages of low requirement on preparation environment, simple process, good repeatability and easy large-area preparation. In addition, the electrode with the mesoporous structure has high transparency, strong conductivity and high light utilization rate, the perovskite solar cell based on the mesoporous structure and a silicon-based solar cell or other thin film cells such as CdTe, CIGS, perovskite solar cells and the like can be connected in series to prepare the laminated solar cell in a mode of connecting two ends in series, and the prepared perovskite laminated solar cell is expected to break through the SQ limit.

Description

Perovskite laminated solar cell and preparation method thereof
Technical Field
The invention belongs to the technical field of solar cell preparation, and particularly relates to a perovskite tandem solar cell and a preparation method thereof.
Background
The highest photoelectric conversion efficiency of both silicon solar cells and perovskite solar cells is close to the theoretical limit of 33% of the photoelectric conversion efficiency of single-junction solar cells, and if the efficiency of the solar cells needs to be further improved, the proposal of the laminated cell provides a new idea. The laminated solar cell has wide tunable band gap and dissolution processability, and fully utilizes sunlight to realize efficiency summation, so that the method widens the spectral response range of the cell, improves the efficiency of the solar cell, and reduces the preparation cost. Among them, organic-inorganic hybrid perovskite cells are used in tandem solar cells because of their advantages such as wide forbidden band width, high light absorption coefficient, high photoelectric conversion efficiency, and low manufacturing cost, for example, by combining the advantages of perovskite solar cells and silicon-based solar cells, the conversion efficiency of solar cells is improved, and at the same time, the cost is reduced.
In the perovskite tandem solar cell, a flat perovskite solar cell is generally adopted, the photoelectric conversion efficiency of the flat perovskite solar cell is high, and the flat perovskite solar cell has the problems of poor stability, high preparation cost, incapability of large-area preparation and the like. When the perovskite-based solar cell is applied to a silicon-based solar cell in a cell lamination mode, the preparation method is limited, the area of the perovskite-based solar cell is also limited, and the commercial application of the perovskite-based solar cell is further influenced.
Disclosure of Invention
The invention provides a perovskite tandem solar cell and a preparation method thereof, which are used for solving the technical problem that the performance of the existing perovskite tandem solar cell is limited due to harsh conditions required by the preparation and low light utilization rate.
The technical scheme for solving the technical problems is as follows: the utility model provides a perovskite tandem solar cell, the solar cell that is located the top layer is perovskite solar cell, and it includes from down to the mesoporous electron transport layer, the mesoporous insulating layer that up stacks the setting and is used for increasing absorption spectrum's mesoporous electrode, and every layer of mesoporous structure intussuseption is filled with perovskite material.
The invention has the beneficial effects that: compared with the existing flat plate structure (the existing flat plate structure has higher requirements on humidity and temperature in the preparation process, is often required to be prepared in a glove box, and has harsh preparation conditions), the mesoporous structure has low requirements on the preparation environment, and the preparation method has the advantages of simple preparation process, good repeatability and easiness in large-area preparation. In addition, the electrode with the mesoporous structure has high transparency, strong conductivity and high sunlight utilization rate, the perovskite solar cell based on the mesoporous structure film and the silicon-based solar cell can be connected in series to prepare the laminated solar cell in a two-end series connection mode, and the prepared laminated solar cell has high photoelectric conversion efficiency.
On the basis of the technical scheme, the invention can be further improved as follows.
Further, the solar cell positioned at the bottom layer is a silicon-based solar cell, a thin film solar cell, a perovskite solar cell, an organic solar cell or a dye-sensitized solar cell.
Further, the solar cell positioned at the bottom layer is connected with the perovskite solar cell through the compact layer.
The invention has the further beneficial effects that: through the connection of the compact layers, the electron transmission rate of the upper and lower layer batteries can be enhanced, and the photoelectric conversion efficiency of the laminated battery is improved.
Furthermore, the mesoporous electrode is made of indium tin oxide.
The invention has the further beneficial effects that: the mesoporous electrode for increasing the absorption spectrum adopts an indium tin oxide electrode, has high transmittance in a visible light region and an infrared region, is an excellent transparent electrode material, and has the advantages of high crystallinity, light transmission, electric conduction and the like. The problem of light transmittance of the infrared part of the mesoporous perovskite solar cell is solved due to high light transmittance, the transparency of the top cell of the laminated cell is realized, and the absorption spectrum of the laminated cell is widened.
The invention also provides a preparation method of the perovskite laminated solar cell, which comprises the following steps:
s1, preparing electron transport material slurry, insulating material slurry and electrode slurry respectively;
s2, preparing a mesoporous electron transmission layer, a mesoporous insulating layer and a mesoporous electrode for increasing absorption spectrum on the upper part of the solar cell at the bottom layer through screen printing in sequence;
s3, dropping the perovskite precursor on the surface of the mesoporous electrode to complete the preparation of the perovskite tandem solar cell.
The invention has the beneficial effects that: and respectively preparing the perovskite material three-layer slurry to prepare the mesoporous structure, wherein the mesoporous structure is prepared simply and quickly by adopting a screen printing mode.
Further, the preparation method of the electrode slurry comprises the following steps:
mixing electrode material powder, pore-forming agent, terpineol and dispersant together and ball-milling to obtain the composite material.
Further, when the mesoporous electrode is made of indium tin oxide, the mass ratio of the indium tin oxide to the pore-forming agent to the terpineol is 1:0.3: 5; the ball milling time is within the range of 12-24 hours, and the ball milling speed is within the range of 100-400 r/h.
Drawings
Fig. 1 is a schematic structural diagram of a perovskite tandem solar cell provided in an embodiment of the present invention;
FIG. 2 is a schematic structural diagram of another perovskite tandem solar cell provided by an embodiment of the invention;
fig. 3 is a positive and negative sweep J-V curve diagram of a transparent mesoporous perovskite cell provided in an embodiment of the invention;
fig. 4 is a light transmittance graph of the ito mesoporous thin film provided by the embodiment of the present invention at different annealing temperatures.
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.
Example one
The perovskite laminated solar cell structurally comprises a perovskite solar cell, a mesoporous electron transmission layer, a mesoporous insulating layer and a mesoporous electrode, wherein the mesoporous electron transmission layer, the mesoporous insulating layer and the mesoporous electrode are stacked from bottom to top, the mesoporous electrode is used for increasing absorption spectrum, and perovskite materials are filled in each layer of mesoporous structure.
In the embodiment, the mesoporous structure is introduced into the tandem solar cell, and compared with the existing flat plate structure (the existing flat plate structure has higher requirements on humidity and temperature in the preparation process, often needs to be prepared in a glove box, and has harsh preparation conditions), the mesoporous structure has low requirements on the preparation environment, the preparation process is simple, the repeatability is good, and the large-area preparation is easy. In addition, the electrode with the mesoporous structure has high transparency, strong conductivity and high sunlight utilization rate, the perovskite solar cell based on the mesoporous structure film and the silicon-based solar cell can be connected in series in a two-end series connection mode to prepare the laminated solar cell, the prepared laminated solar cell has high photoelectric conversion efficiency, and the laminated solar cell is expected to break through SQ (Shockley-Queisser limit or S-Q limit).
Preferably, the solar cell located at the bottom layer is a silicon-based solar cell, a thin film solar cell, a perovskite solar cell, an organic solar cell or a dye-sensitized solar cell.
Solar energy is used as renewable clean energy and has important significance for the sustainable development of human beings. The solar cell can directly convert solar energy into electric energy, and the photoelectric conversion efficiency and the preparation cost are key factors for determining the industrial application of the solar cell. At present, silicon-based solar cells are the mainstream of solar cells, occupy 90% of the photovoltaic market, have the efficiency of 25.6%, but the preparation cost is high. Therefore, the laminated cell can be formed by superposing the wide-band-gap perovskite material on the top layer of the silicon cell, so that the solar energy is utilized to the maximum extent, the efficiency of the solar cell is improved, and the preparation cost is reduced. The theoretical ultimate efficiency based on silicon-based laminate cells, which has been reported to date, can be increased from 29% to 42.5%, and the selection of the top cell of the laminate cell needs to meet the following requirements: the silicon solar cell has the advantages of band gap matching with the bottom silicon cell, high photoelectric conversion efficiency and low manufacturing cost. However, organic-inorganic hybrid perovskite solar cells completely meet the above requirements, are receiving much attention due to the advantages of low cost, easy preparation, high light absorption coefficient and the like, and are rapidly developed, the cell conversion efficiency has been improved from 3.8% in 2009 to 25.2% in 2020, and perovskite materials are also considered as light absorption materials of next-generation low-cost solar cells. Since perovskites and silicon have different absorption ranges, in order to fully utilize the solar spectrum, perovskite solar cells can be used as top cells to form tandem solar cells with silicon cells, i.e., perovskite/silicon-based tandem solar cells.
Preferably, the solar cell located at the bottom layer is connected with the perovskite solar cell through the dense layer. Through the connection of the compact layers, the electron transmission rate of the upper and lower layer batteries can be enhanced, and the photoelectric conversion efficiency of the laminated battery is improved.
Preferably, the perovskite solar cell does not comprise a hole transport layer.
The hole transport layer is removed, so that the stability of the perovskite solar cell in the air is improved, the perovskite solar cell is easy to store, and the perovskite solar cell is low in manufacturing cost and convenient to manufacture.
Preferably, the mesoporous electrode is made of indium tin oxide.
The mesoporous electrode for increasing the absorption spectrum adopts an indium tin oxide electrode, the indium tin oxide is an n-type semiconductor, has a wide band gap of 4.3eV, has high transmittance in a visible light region and an infrared region, is an excellent transparent electrode material, and has the advantages of high crystallinity, light transmission, electric conduction and the like. The problem of light transmittance of the infrared part of the mesoporous perovskite solar cell is solved due to high light transmittance, the transparency of the top cell of the laminated cell is realized, the absorption spectrum of the laminated cell is widened, and other mesoporous conductive materials can be used as materials of mesoporous electrodes.
Example two
A method of fabricating a perovskite tandem solar cell as described in the first embodiment above, comprising:
s1, preparing electron transport material slurry, insulating material slurry and electrode slurry respectively;
s2, preparing a mesoporous electron transmission layer, a mesoporous insulating layer and a mesoporous electrode for increasing absorption spectrum on the upper part of the solar cell at the bottom layer through screen printing in sequence;
and S3, dropping the perovskite precursor on the surface of the mesoporous electrode to complete the preparation of the perovskite tandem solar cell.
And respectively preparing the perovskite material three-layer slurry to prepare the mesoporous structure, wherein the mesoporous structure is prepared simply and quickly by adopting a screen printing mode.
Preferably, the preparation method of the electrode slurry comprises the following steps: mixing electrode material powder, pore-forming agent, terpineol and dispersant together and ball-milling to obtain the composite material.
Preferably, when the mesoporous electrode is made of indium tin oxide, the mass ratio of the indium tin oxide to the pore-forming agent to the terpineol is 1:0.3: 5; the ball milling time is within the range of 12-24 hours, and the ball milling speed is within the range of 100-; the screen printing pressure for screen printing was between 6.0-8.0 kg.
The conductive indium tin oxide slurry prepared from indium tin oxide is a conductive material with high conductivity and high light transmittance, and the problem of light transmittance of the infrared part of the mesoporous perovskite solar cell is solved due to the high light transmittance, so that the transparentization of the top cell of the laminated cell is realized. The conductive indium tin oxide slurry can be sintered to be used as a transparent back electrode of a mesoporous perovskite solar cell to prepare an indium tin oxide transparent mesoporous film with high conductivity and high transparency.
For example, in the preparation of indium tin oxide slurry, the siliceous mortar is cleaned with industrial alcohol and dried for later use. 3g of indium tin oxide powder, 0.9g of pore-forming agent and 15g of terpineol are respectively weighed by a ten-thousandth electronic balance and put into a zirconia ball-milling tank. The ball milling speed is 350r/h, the ball milling is carried out for 48 hours, then the ball is taken out, and a rotary steaming instrument is opened to prepare rotary steaming. And (4) performing rotary evaporation at 40 ℃ under the air pressure of 10mbar until no liquid drops, finishing the rotary evaporation, collecting the slurry, and cleaning a rotary evaporation bottle.
Further printing of an indium tin oxide layer was performed. And cleaning and drying the indium tin oxide screen printing plate and the indium tin oxide scraper for later use. And (4) placing the indium tin oxide silk-screen printing plate into a silk-screen printing machine for fixing. And then sending the film brushed with the zirconium peroxide into the screen printing plate, adjusting the position of the screen printing plate to enable the upper and lower positions of the brushed indium tin oxide to be positioned in the middle of the zirconium oxide, then putting a proper amount of indium tin oxide slurry on the screen printing plate, adjusting the pressure of a screen printing machine to be 7.0, and brushing the film. And after drying the film, putting the film into a hot bench for annealing, setting the target temperature to be 500 ℃, annealing at 500 ℃, and keeping the heating rate at 10 ℃ per minute.
And after a compact layer is sprayed on the bottom solar cell, sequentially printing a mesoporous film structure of a nano crystal layer, an insulating layer and a porous electrode, specifically, referring to the printing of the indium tin oxide layer in the printing process, and then, dripping perovskite precursor liquid onto the surface of the indium tin oxide layer to prepare the perovskite laminated solar cell based on the mesoporous film structure.
As shown in table 1 below, the test stability was tested for 30 days, with a maximum Photoelectric Conversion Efficiency (PCE) of 8.86% and a drop in efficiency within 15% within 30 days. The transparent mesoporous perovskite battery device has good stability in the air.
Table 1 dark state stability test of transparent mesoporous perovskite cell within 30 days
Time (sky) Voc(mV) Jsc(mA/cm2) FF PCE(％)
1 897.88 21.82 0.40 7.92
4 937.08 22.97 0.41 8.86
20 898.63 22.00 0.42 8.36
21 927.66 21.41 0.41 8.24
22 899.59 21.94 0.41 8.08
23 904.27 22.06 0.41 8.12
24 902.28 21.62 0.40 7.83
26 909.19 21.69 0.39 7.63
27 888.16 21.78 0.38 7.35
29 875.44 21.67 0.36 6.84
31 924.90 22.00 0.39 8.00
As shown in table 2 below, the data in the figure is positive and negative scanning data obtained by testing a transparent mesoporous perovskite solar cell, the difference between the photoelectric conversion efficiencies of the positive and negative scanning is not large, and it can be seen from fig. 3 intuitively that the obtained hysteresis factor is small, and it is known that the performance of the cell device is relatively stable.
Table 2 positive and negative scanning data of transparent mesoporous perovskite cell
Voc(mV) Jsc(mA/cm2) FF PCE(％) Rs(ohm cm2) Rsh(ohm cm2)
Reverse sweeping 899.59 21.94 0.41 8.08 19.15 240.35
Positive sweep 842.26 22.29 0.37 7.00 21.91 482.86
In addition, as shown in table 3 below, when the annealing temperature is 500 degrees celsius, the indium tin oxide mesoporous thin film has the lowest carrier density and the highest hall mobility and conductivity, which indicates that the indium tin oxide mesoporous thin film has high conductivity at the annealing temperature of 500 degrees celsius.
TABLE 3 mesoporous ITO film Carrier concentration, Hall mobility and conductivity at different annealing temperatures
Annealing temperature carrier concentration(*10^19cm-3) hall mobility(cm2/Vs) Conductivity(1/ohm cm)
9.03 0.12 10.78
6.17 0.11 10.73
400℃ 6.72 0.92 10.71
17.99 0.13 10.69
13.96 0.09 10.68
1.26 6.77 13.65
11.89 0.71 13.58
450℃ 2.31 3.67 13.61
4.86 1.73 13.44
2.43 3.49 13.55
2.32 4.47 16.61
7.19 1.40 16.15
500℃ 2.70 3.73 16.12
1.78 5.65 16.08
1.33 7.53 16.09
8.73 1.13 15.74
5.99 1.63 15.67
550℃ 8.69 1.12 15.59
1.17 8.31 15.55
3.98 2.44 15.57
As shown in fig. 4, the transmittance of the indium tin oxide mesoporous thin film at different annealing temperatures is higher between 800 nm and 1200nm, and the average transmittance can reach 87%, so that the indium tin oxide mesoporous thin film has higher transmittance at the infrared part.
The choice of the numerical ranges of the specific parameters therein does not limit the invention, and the above annealing temperature may be between 400 ℃ and 550 ℃.
The solvent in the present invention is not limited to terpineol, and is a solvent that is well compatible with perovskite, i.e., does not dissolve perovskite, based on the solvent properties and experimental phenomena. Thus, the solvent may be terpineol, N-dimethylformamide, N-dimethylacetamide, N-dimethylpropionamide, N-diethylformamide, N-diethylacetamide, N-diethylpropionamide, dimethyl sulfoxide, tetramethylene sulfoxide, pentamethylene sulfoxide, hexamethylene sulfoxide, tetramethylene urea, N-dimethylacrylic acid urea, hexamethylphosphoramide, N-methylpyrrolidone, N-ethylpyrrolidone, methylene chloride, benzene, toluene, xylene, methane, ethane, propane, butane, pentane, hexane, octane, cyclohexane, cyclohexanone, tolucyclohexanone, diethyl ether, acetone, methyl ethyl ketone, acetic acid, acetic anhydride, dioxane, chloroform, carbon tetrachloride, ethyl acetate, tetrahydrofuran, pyridine, petroleum ether, methanol, ethanol, N-butanol, isopropanol, nitrobenzene, chlorobenzene, dichlorobenzene, dichloromethane, diethyl ether, propylene oxide, methyl acetate, ethyl acetate, propyl acetate, isopropyl acetate, methyl n-acetone, isobutyl acetate, 2-nitropropane, n-butyl acetate, propylene glycol methyl ether, methyl isoamyl ketone, methyl amyl acetate, n-butyl propionate, propylene glycol methyl ether acetate, amyl acetate, methyl n-amyl ketone, isobutyl isobutyrate, hydroxyethyl diethyl ether, cyclohexanone, propylene glycol monobutyl ether, propylene glycol monopropyl ether, ethylene glycol ethyl ether acetate, diisobutyl ketone, ethylene glycol propyl ether, diacetone alcohol, ethylene glycol butyl ether, propylene glycol butyl ether, 2-ethylhexyl formate, ethylene glycol butyl ether acetate, dipropylene glycol methyl ether, glycol diacetate, diethylene glycol methyl ether, diethylene glycol ethyl ether, diethylene glycol propyl ether, diethylene glycol butyl ether, Ethylene glycol hexyl ether, diethylene glycol ethyl ether acetate, diethylene glycol butyl ether, ethylene glycol-2-ethylhexyl ether, diethylene glycol butyl ether acetate, propylene glycol monophenyl ether, methyl butanone, methyl isobutyl ketone, ethylene glycol monomethyl ether, ethylene glycol monoethyl ether, ethylene glycol monobutyl ether, acetonitrile, pyridine, phenol, methanol, ethanol, isopropanol, n-propanol, 2-butanol, isobutanol, methyl isobutyl methanol, pentanol, cyclohexanol, naphtha, 100# solvent oil, 150# solvent oil, 200# solvent oil, styrene, perchloroethylene, trichloroethylene, ethylene glycol ether, triethanolamine, and the like.
The preparation method is simple in process, the prepared conductive indium tin oxide slurry is a conductive material with high conductivity and high light transmittance, the conductive indium tin oxide slurry can be sintered to be used as a transparent back electrode of the mesoporous solar cell, the problem of light transmittance of the infrared part of the mesoporous perovskite solar cell is solved, and the transparentization of the top cell of the laminated cell is realized. And finally, the transparent mesoporous perovskite solar cell is prepared and is connected with the bottom solar cell in series at four ends to form a novel laminated solar cell structure.
It will be understood by those skilled in the art that the foregoing is only 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 in the scope of the present invention.

Claims (7)

1. The perovskite laminated solar cell is characterized in that the solar cell positioned at the top layer is a perovskite solar cell, the perovskite solar cell comprises a mesoporous electron transmission layer, a mesoporous insulating layer and a mesoporous electrode, the mesoporous electron transmission layer and the mesoporous insulating layer are stacked from bottom to top, the mesoporous electrode is used for increasing absorption spectrum, and perovskite materials are filled in each layer of mesoporous structure.
2. The perovskite tandem solar cell according to claim 1, wherein the underlying solar cell is a silicon-based solar cell, a thin-film solar cell, a perovskite solar cell, an organic solar cell or a dye-sensitized solar cell.
3. The perovskite tandem solar cell according to claim 1, wherein the underlying solar cell is connected to the perovskite solar cell through a dense layer.
4. The perovskite tandem solar cell according to any one of claims 1 to 3, wherein the mesoporous electrode is made of indium tin oxide.
5. A method of manufacturing a perovskite tandem solar cell as defined in any one of claims 1 to 4, comprising:
s1, preparing electron transport material slurry, insulating material slurry and electrode slurry respectively;
s2, preparing a mesoporous electron transmission layer, a mesoporous insulating layer and a mesoporous electrode for increasing absorption spectrum on the upper part of the solar cell at the bottom layer through screen printing in sequence;
s3, dropping the perovskite precursor on the surface of the mesoporous electrode to complete the preparation of the perovskite tandem solar cell.
6. The method of manufacturing a perovskite tandem solar cell according to claim 5, wherein the electrode paste is prepared by:
mixing electrode material powder, pore-forming agent, terpineol and dispersant together and ball-milling to obtain the composite material.
7. The method according to claim 6, wherein when the mesoporous electrode is made of indium tin oxide, the mass ratio of indium tin oxide to pore former to terpineol is 1:0.3: 5; the ball milling time is within the range of 12-24 hours, and the ball milling speed is within the range of 100-400 r/h.
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Cited By (1)

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Application publication date: 20200904