CN113193125A - Flexible perovskite solar cell with high power-to-mass ratio and preparation method thereof - Google Patents

Flexible perovskite solar cell with high power-to-mass ratio and preparation method thereof Download PDF

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CN113193125A
CN113193125A CN202110422591.1A CN202110422591A CN113193125A CN 113193125 A CN113193125 A CN 113193125A CN 202110422591 A CN202110422591 A CN 202110422591A CN 113193125 A CN113193125 A CN 113193125A
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solar cell
parylene
perovskite solar
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CN113193125B (en
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朱瑞
李雷
喻茂滔
陈鹏
龚旗煌
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Peking University
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    • H—ELECTRICITY
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    • H10K77/00—Constructional details of devices covered by this subclass and not covered by groups H10K10/80, H10K30/80, H10K50/80 or H10K59/80
    • H10K77/10—Substrates, e.g. flexible substrates
    • H10K77/111—Flexible substrates
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    • H10K—ORGANIC ELECTRIC SOLID-STATE DEVICES
    • H10K71/00—Manufacture or treatment specially adapted for the organic devices covered by this subclass
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    • H10—SEMICONDUCTOR DEVICES; ELECTRIC SOLID-STATE DEVICES NOT OTHERWISE PROVIDED FOR
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    • Y02E10/549—Organic PV cells
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Abstract

The invention discloses a flexible perovskite solar cell with a high power-to-mass ratio and a preparation method thereof. The invention adopts a chemical vapor deposition method and an ion beam polishing technology to prepare a parylene film with the thickness of less than 5 mu m as a flexible substrate, and then a transparent conductive functional layer consisting of a metal grid and a transparent conductive oxide and other functional layers of the perovskite solar cell are prepared on the parylene film, so that the photoelectric conversion efficiency of the obtained flexible perovskite solar cell can exceed 20 percent, the power-mass ratio can exceed 30W/g, the bending radius can be less than 1mm, and the performance attenuation of the cell after 300 cycles of bending is less than 5 percent. The flexible perovskite solar cell with the high power-to-mass ratio has the characteristics of small mass, high flexibility and very high power-to-mass ratio, has great application potential in the fields of aerospace and the like, and has unique advantages in the fields of intelligent equipment, wearable equipment and the like.

Description

Flexible perovskite solar cell with high power-to-mass ratio and preparation method thereof
Technical Field
The invention belongs to the field of photoelectric functional devices, and particularly relates to a flexible perovskite solar cell and a preparation method thereof.
Background
The flexible solar cell has the unique advantages of small weight, less unit material consumption, flexibility, scalability and the like compared with the traditional rigid solar cell, has urgent needs in the fields of aerospace, military equipment and the like, and also has wide application prospects in the civil fields of intelligent equipment, wearable equipment and the like. The power-to-mass ratio is a very important parameter for flexible solar cells, and represents the strength of the power generation capacity of a solar cell per unit mass. Taking the fields of aerospace and the like which are sensitive to quality as an example, the high power-to-quality ratio means that less emission quality can be occupied, more electric energy can be generated, more fuel and equipment can be loaded, and therefore the pursuit of the power-to-quality ratio is not limited.
Silicon-based solar cells have always occupied a large share of the solar cell market with their relatively high photoelectric conversion efficiency and good stability, but are limited by the inherent properties of their materials, poor flexibility, low power-to-mass ratio (typically below 0.5W/g), and little potential for development in the flexible field. At present, the technical route adopted by flexible solar cells is generally a thin film solar cell using a flexible substrate, and the thin film solar cell mainly comprises Copper Indium Gallium Selenide (CIGS), cadmium telluride (CdTe), gallium arsenide (GaAs) and other materials. Among them, flexible solar cells based on Copper Indium Gallium Selenide (CIGS), cadmium telluride (CdTe) materials are also low in power to mass ratio due to their low efficiency. The flexible solar cell based on gallium arsenide (GaAs) materials has high energy conversion efficiency, the power-to-mass ratio of the multijunction GaAs solar cell can reach 3W/g, but the preparation cost is high, and large-scale application is difficult.
In recent years, organic-inorganic hybrid perovskite materials have attracted much attention in the application fields of solar cells, photoelectric transceivers and the like due to low preparation cost, simple process, long carrier diffusion distance, high carrier mobility and strong absorption capacity in visible and infrared bands. The solar cell prepared based on the perovskite material has high photoelectric conversion efficiency, and is a thin-film solar cell, and the thin-film preparation process of the solar cell has the characteristics of small mass and capability of being combined with a flexible substrate. Therefore, the perovskite material is used for preparing the flexible solar cell with high power-to-mass ratio.
In order to realize a flexible solar cell with a high power-to-mass ratio, a flexible transparent substrate must be used, and in addition to satisfying characteristics such as high flexibility, high light transmittance, and the like, such a substrate must have high flatness and a small mass thickness. The substrate materials commonly used in the current flexible solar cell, such as flexible substrates of PET (polyethylene terephthalate), PEN (polyethylene naphthalate) and the like, have a great tendency of spontaneous curling when the thickness is thin due to the process reason of the biaxial stretching-based preparation, and the increase of the thickness of the film to inhibit the spontaneous curling thereof will result in a great thickness and quality, so that the requirement of the device on high power-to-quality ratio is difficult to meet.
Disclosure of Invention
In order to overcome the defects of the prior art, the invention provides an ultra-thin and ultra-light flexible perovskite solar cell with ultra-high power-to-mass ratio and prepared based on a Parylene substrate and a transparent conductive oxide electrode, and a preparation method thereof.
The parylene material substrate used by the invention is prepared by a Chemical Vapor Deposition (CVD) method, a compact and uniform film can be obtained within the thickness range of 0.1-100 mu m, and the problem of spontaneous curling of the ultrathin film can be solved by a deposition process based on a smooth substrate. However, the parylene prepared based on the vapor deposition technology has the problem of overlarge surface roughness, the ion beam polishing technology is used for improving the surface roughness, the parylene film with the thickness of less than 5 microns is finally used as the flexible substrate, the photoelectric conversion efficiency of the perovskite solar cell prepared by the substrate can exceed 20%, the power-mass ratio can exceed 30W/g, the power-mass ratio is far higher than that of the multijunction gallium arsenide cell reported in the prior art, the bending radius of the multijunction gallium arsenide cell can be less than 1mm, and the performance of the cell is attenuated by less than 5% after the multijunction gallium arsenide cell is bent for 300 cycles. The invention can provide a technical cushion for the application of the flexible perovskite solar cell in aerospace and other similar fields.
Specifically, the technical scheme of the invention is as follows:
a flexible perovskite solar cell comprises a substrate and a perovskite solar cell functional layer on the substrate, and is characterized in that the substrate is a Parylene (Parylene) ultrathin film, the Parylene ultrathin film is a compact and uniform Parylene film prepared by adopting a chemical vapor deposition method, and then the surface of the Parylene film is improved by using an ion beam polishing technology to obtain the Parylene film with the thickness of less than 5 microns; and a transparent conductive functional layer and other functional layers of the perovskite solar cell are sequentially arranged on the substrate, wherein the transparent conductive functional layer consists of a metal grid and a transparent conductive oxide.
In the flexible perovskite solar cell, the Parylene film material can be Parylene-C (poly 2-chloro-p-xylene), Parylene-D (poly 2, 5-dichloro-p-xylene), Parylene-N (Parylene) and other Parylene derivatives, such as Parylene HT, Parylene F, Parylene AF4, Parylene AF8, and the like.
The transparent conductive functional layer is composed of a metal grid and a transparent conductive oxide, wherein the metal material forming the metal grid can be gold (Au), silver (Ag), aluminum (Al), nickel (Ni), titanium (Ti) or other metals which do not react with the perovskite material, and can also be alloy materials or nano materials of the metals. The transparent conductive oxide can be ITO (indium tin oxide), FTO (fluorine-doped tin oxide) or other transparent conductive oxides.
The thickness of the transparent conductive functional layer is preferably 100-300 nm.
The flexible perovskite solar cell of the invention may be of a formal or trans structure. Generally, for a perovskite solar cell with a formal structure, an electron transport layer, a perovskite light absorption layer, a hole transport layer and a metal electrode are sequentially arranged on the transparent conductive functional layer; for the trans-structure perovskite solar cell, a hole transport layer, a perovskite light absorption layer, an electron transport layer and a metal electrode are sequentially arranged on the transparent conductive functional layer. The perovskite light absorption layer is preferably made of an organic-inorganic perovskite material.
The invention also provides a preparation method of the flexible perovskite solar cell, which comprises the following steps:
1) preparing a compact and uniform parylene film on a hard substrate by adopting a chemical vapor deposition method;
2) using an ion beam polishing technology to improve the surface of the parylene film;
3) preparing a transparent conductive functional layer on the surface of the improved parylene film to obtain a flexible transparent conductive electrode;
4) the preparation of other functional layers of the perovskite solar cell is completed on the flexible transparent conductive electrode;
5) and (3) taking off the prepared perovskite solar thin film cell from the hard substrate to finish the preparation of the flexible perovskite solar cell.
In the step 1), the hard substrate may be a glass substrate, a quartz substrate, a silicon substrate, or the like.
In the step 2), the surface roughness of the parylene film is preferably controlled to 8nm or less by an ion beam polishing technique.
In the step 3), a layer of metal is plated on the surface of the parylene film, then a metal grid is formed through photoetching and etching, and then a transparent conductive oxide film is prepared on the parylene film with the metal grid to form a flexible transparent conductive electrode consisting of the metal grid and the transparent conductive oxide. The transparent conductive oxide film is prepared from the transparent conductive oxide material by magnetron sputtering, thermal evaporation, laser deposition, atomic layer deposition and other methods.
The P-I-N type and N-I-P type solar cells can be prepared in the step 4), and the preparation process of each functional layer can be a spin coating method, an evaporation method, a spraying method, a blade coating method or other process modes.
Compared with the prior art, the invention has the technical advantages that:
1. the flexible perovskite solar cell with the high power-to-mass ratio has the characteristics of small mass, high flexibility, especially very high power-to-mass ratio, has great application potential in the fields of aerospace and the like, and has unique advantages in the fields of intelligent equipment, wearable equipment and the like.
2. According to the flexible perovskite solar cell with the high power-to-mass ratio, the parylene material is used for replacing materials such as PET (polyethylene terephthalate), PEN (PEN) and the like commonly used in the field of flexible solar cells in the aspect of the flexible transparent substrate. Compared with materials such as PET, PEN and the like, the parylene material greatly reduces the thickness and the quality of the flexible substrate, so that the ultrathin flexible substrate (<5 mu m) can be applied to the field of flexible solar cells.
3. The flexible perovskite solar cell with the high power-to-mass ratio provided by the invention uses the organic and inorganic perovskite material as the light absorption active layer material, compared with the traditional silicon-based and III-V group semiconductor materials, the organic and inorganic hybrid perovskite material has the advantages of low preparation cost, simple process and the like, and the organic and inorganic hybrid perovskite material is a hot material currently researched in the academic world, and the photoelectric conversion efficiency of the organic and inorganic hybrid perovskite material is still a great promotion space, so that the battery power-to-mass ratio emphasized by the invention is not limited to the degree reached by the invention along with the development of the organic and inorganic perovskite material.
Drawings
Fig. 1 is a schematic structural diagram of a high power to mass ratio flexible perovskite solar cell according to the present invention.
In the figure: the light absorption layer comprises a 1-parylene film substrate, a 2-transparent conductive functional layer, a 3-electron (formal) or hole (trans) transmission layer, a 4-perovskite light absorption layer, a 5-hole (formal) or electron (trans) transmission layer and a 6-metal electrode.
FIG. 2 is a J-V curve diagram of a high power to mass ratio flexible perovskite solar cell prepared by the invention.
Detailed Description
The present invention will be described in detail below with reference to the accompanying drawings and specific embodiments, but the present invention is not limited to the following embodiments.
Example 1:
(1) and immersing the glass substrate into a detergent for ultrasonic cleaning, rinsing the detergent by using deionized water, and sequentially immersing the glass substrate into the deionized water, acetone and isopropanol for ultrasonic cleaning.
(2) A Parylene-C film was deposited on a glass substrate to a thickness of 2 μm.
(3) The surface roughness of Parylene (Parylene) film is improved by ion beam polishing technology, and the surface roughness of the film surface is controlled below 8 nm.
(4) And plating a Ni metal layer with the thickness of 200nm on the surface of the polished Parylene-C film.
(5) And spin-coating photoresist on the Ni metal layer, and performing photoetching after prebaking and curing.
(6) And obtaining a grid pattern formed by the photoresist through development after photoetching.
(7) The conductive metal grid is formed by removing unwanted metal portions by wet etching.
(8) And washing the photoresist.
(9) And sputtering a layer of ITO with the thickness of 250nm on the Parylene-C film with the conductive metal grid.
(10) SnO diluted by water according to the volume ratio of 1:2 is coated on a Parylene/(Ni, ITO) substrate in a spin mode2The water dispersion was spin-coated at 4000 rpm for 30 seconds, and was kept at 150 ℃ for 30 minutes after the completion of the spin-coating.
(11) And (4) transferring and placing the mixture in an ultraviolet-ozone cleaning machine for cleaning for 20 minutes, then transferring and placing the mixture in a glove box for natural cooling to room temperature to finish annealing, and finishing the preparation of the electron transport layer.
(12) Mixing lead iodide (PbI)2) Dissolving the mixture in a mixed solvent of DMSO and DMF, wherein the volume ratio of DMSO to DMF is 1:9, heating at 70 ℃ to completely dissolve the mixture, then spin-coating the mixture on the electron transport layer prepared in the previous step, wherein the spin-coating speed is 2000 revolutions per minute, the spin-coating time is 30 seconds, keeping the temperature at 70 ℃ for 1 minute after the spin-coating is finished, then naturally cooling to room temperature to finish annealing, and completing the preparation of the perovskite light absorption layer.
(13) Spiro-OMeTAD was dissolved in Chlorobenzene (CB) solvent at a concentration of 72.3mg/mL, and vigorously stirred to completely dissolve it. Then, 28.8. mu.L of 4-tert-butylpyridine (4-tert-butylpyridine) and 17.5. mu.L of a solution of Li-TFSI in acetonitrile (concentration: 520mg/mL) were added to 1mL of the solution in this order, and the mixture was stirred well. And then spin-coating the perovskite light absorption layer prepared in the previous step at the spin-coating speed of 4000 revolutions per minute for 30 seconds, and finishing the preparation of the hole transport layer after the spin-coating is finished.
(14) And transferring the semi-finished product of the battery with the hole transport layer prepared in the previous step into a metal evaporation cabin, preparing a gold (Au) electrode with the thickness of 80nm by using a vacuum thermal evaporation method and matching with a mask plate, and finally removing the thin film battery from the substrate to complete the preparation of the formal flexible perovskite solar battery.
Example 2:
(1) and immersing the glass substrate into a detergent for ultrasonic cleaning, rinsing the detergent by using deionized water, and sequentially immersing the glass substrate into the deionized water, acetone and isopropanol for ultrasonic cleaning.
(2) A Parylene-C film was deposited on a glass substrate to a thickness of 2 μm.
(3) The surface roughness of Parylene (Parylene) film is improved by ion beam polishing technology, and the surface roughness of the film surface is controlled below 8 nm.
(4) And plating a Ni metal layer with the thickness of 200nm on the surface of the polished Parylene-C film.
(5) And spin-coating photoresist on the Ni metal layer, and performing photoetching after prebaking and curing.
(6) And obtaining a grid pattern formed by the photoresist through development after photoetching.
(7) The conductive metal grid is formed by removing unwanted metal portions by wet etching.
(8) And washing the photoresist.
(9) And sputtering a layer of ITO with the thickness of 250nm on the Parylene-C film with the conductive metal grid.
(10) Dissolving PTAA in Chlorobenzene (CB) with the concentration of 2mg/mL, spin-coating the solution on a Parylene/(Ni, ITO) substrate in a glove box at the spin-coating speed of 4000 rpm for 30 seconds, heating the solution at the temperature of 150 ℃ for 20 minutes after the spin-coating is finished, and naturally cooling the solution to room temperature for annealing to finish the preparation of the hole transport layer.
(11) Weighing lead iodide (PbI) according to the required proportion2) Lead bromide (PbBr)2) Five powders of formamidine iodine (FAI), methylamine bromide (MABr) and cesium iodide (CsI) are put into the same reagent bottle, a mixed solvent of DMSO and DMF is added, the volume ratio of the two is 1:4, and the concentration of lead ions in the final precursor solution is controlled to be 1.41 mmor/mL. Then the mixture is placed on a heating table at 90 ℃ to be heated to be fully dissolved, and then the mixture is cooled to room temperature for standby.
(12) The solution was spin coated on the hole transport layer in a two-step process, with a first spin coating speed of 2000 rpm for 10 seconds, a second spin coating speed of 6000 rpm for 30 seconds, and 100 μ l of anti-solvent was dropped onto the substrate 15 seconds before the end of the second spin coating. And after the spin coating is finished, heating and keeping the temperature at 100 ℃ for 60 minutes, and then naturally cooling and annealing to finish the preparation of the perovskite light absorption layer.
(13) Will PC61BM was dissolved in Chlorobenzene (CB) solvent at a concentration of 20mg/mL and stirred on a hot plate at 60 ℃ for 2 hours. And then spin-coating the perovskite light absorption layer on the prepared perovskite light absorption layer, wherein the spin-coating speed is 1000 revolutions per minute, and the spin-coating time is 30 seconds, so that the preparation of the electron transmission layer can be completed.
(14) And spin-coating an isopropanol saturated solution of BCP on the electron transmission layer to form a buffer layer, wherein the spin-coating speed is 1000 rpm, the spin-coating time is 30 seconds, then transferring the buffer layer into a metal evaporation chamber, preparing a copper (Cu) electrode with the thickness of 80nm by using a vacuum thermal evaporation method and matching with a mask, and finally removing the thin film battery from the substrate to finish the preparation of the trans-form flexible perovskite solar cell.
As shown in FIG. 2, the open-circuit voltage of the flexible perovskite solar cell prepared by the invention is 1.102V, and the short-circuit current density is 31.744mA/cm2The Photoelectric Conversion Efficiency (PCE) reaches 20.2%, the power-to-mass ratio per unit area reaches 30.9W/g, and the photoelectric conversion device has the characteristics of light weight, flexibility and high power-to-mass ratio.
It is noted that the disclosed embodiments are intended to aid in further understanding of the invention, but those skilled in the art will appreciate that: various substitutions and modifications are possible without departing from the spirit and scope of the invention and appended claims. Therefore, the invention should not be limited to the embodiments disclosed, but the scope of the invention is defined by the appended claims.

Claims (10)

1. A flexible perovskite solar cell comprises a substrate and a perovskite solar cell functional layer on the substrate, and is characterized in that the substrate is a parylene ultrathin film, the parylene ultrathin film is a compact and uniform parylene film prepared by adopting a chemical vapor deposition method, and then the surface of the parylene ultrathin film is improved by using an ion beam polishing technology to obtain a parylene film with the thickness of less than 5 microns; and a transparent conductive functional layer and other functional layers of the perovskite solar cell are sequentially arranged on the substrate, wherein the transparent conductive functional layer consists of a metal grid and a transparent conductive oxide.
2. The flexible perovskite solar cell as defined in claim 1, wherein the parylene film is of a material selected from one or more of the following materials: Parylene-C, Parylene-D, Parylene-N, Parylene HT, Parylene F, Parylene AF4, and Parylene AF 8.
3. The flexible perovskite solar cell of claim 1, wherein the material of the metal mesh is selected from an alloy of one or more of gold, silver, aluminum, nickel, titanium, and other metals that do not react with the perovskite material; the transparent conductive oxide is ITO, FTO or other transparent conductive oxides.
4. The flexible perovskite solar cell of claim 1, wherein the flexible perovskite solar cell is in a formal or trans structure; for the perovskite solar cell with a formal structure, an electron transport layer, a perovskite light absorption layer, a hole transport layer and a metal electrode are sequentially arranged on the transparent conductive functional layer; for the trans-structure perovskite solar cell, a hole transport layer, a perovskite light absorption layer, an electron transport layer and a metal electrode are sequentially arranged on the transparent conductive functional layer.
5. The flexible perovskite solar cell of claim 1, wherein a perovskite light absorbing layer in the flexible perovskite solar cell is made of an organic-inorganic perovskite material.
6. A method of manufacturing a flexible perovskite solar cell as claimed in any one of claims 1 to 5, comprising the steps of:
1) preparing a compact and uniform parylene film on a hard substrate by adopting a chemical vapor deposition method;
2) using an ion beam polishing technology to improve the surface of the parylene film;
3) preparing a transparent conductive functional layer on the surface of the improved parylene film to obtain a flexible transparent conductive electrode;
4) the preparation of other functional layers of the perovskite solar cell is completed on the flexible transparent conductive electrode;
5) and (3) taking off the prepared perovskite solar thin film cell from the hard substrate to finish the preparation of the flexible perovskite solar cell.
7. The production method according to claim 6, wherein in step 1), the hard base is a glass substrate, a quartz substrate, or a silicon substrate.
8. The production method according to claim 6, wherein the surface roughness of the parylene film in the step 2) is controlled to 8nm or less by an ion beam polishing technique.
9. The method according to claim 6, wherein in step 3), a layer of metal is plated on the surface of the parylene film, then a metal grid is formed by photoetching and etching, and then a transparent conductive oxide film is prepared on the parylene film with the metal grid to form the flexible transparent conductive electrode consisting of the metal grid and the transparent conductive oxide.
10. The method of claim 9, wherein the transparent conductive oxide thin film is prepared by magnetron sputtering, thermal evaporation, laser deposition, or atomic layer deposition in step 3).
CN202110422591.1A 2021-04-15 2021-04-15 Flexible perovskite solar cell with high power-mass ratio and preparation method thereof Active CN113193125B (en)

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CN114335216B (en) * 2022-01-17 2022-10-28 北京大学长三角光电科学研究院 Four-end laminated perovskite solar cell and preparation method thereof
CN115295666A (en) * 2022-07-15 2022-11-04 国家电投集团科学技术研究院有限公司 Substrate-free perovskite battery and preparation method thereof
CN115811919A (en) * 2023-02-02 2023-03-17 无锡极电光能科技有限公司 Perovskite thin film, preparation method thereof and perovskite solar cell

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