CN116847704B - Perovskite film preparation method and laminated solar cell - Google Patents

Perovskite film preparation method and laminated solar cell Download PDF

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CN116847704B
CN116847704B CN202311099841.8A CN202311099841A CN116847704B CN 116847704 B CN116847704 B CN 116847704B CN 202311099841 A CN202311099841 A CN 202311099841A CN 116847704 B CN116847704 B CN 116847704B
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CN116847704A (en
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请求不公布姓名
易海芒
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Shenzhen Heijing Optoelectronic Technology Co ltd
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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
    • H10K71/15—Deposition of organic active material using liquid deposition, e.g. spin coating characterised by the solvent used
    • H—ELECTRICITY
    • H10—SEMICONDUCTOR DEVICES; ELECTRIC SOLID-STATE DEVICES NOT OTHERWISE PROVIDED FOR
    • H10K—ORGANIC ELECTRIC SOLID-STATE DEVICES
    • H10K39/00—Integrated devices, or assemblies of multiple devices, comprising at least one organic radiation-sensitive element covered by group H10K30/00
    • H10K39/10—Organic photovoltaic [PV] modules; Arrays of single organic PV cells
    • H10K39/15—Organic photovoltaic [PV] modules; Arrays of single organic PV cells comprising both organic PV cells and inorganic PV cells
    • 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
    • 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

According to the perovskite film preparation method provided by the application, a certain proportion of low-boiling-point solvent is added into the perovskite precursor solution, and a film preparation method of hot dipping and annealing is adopted. The method can achieve the effect of uniformly volatilizing the solvent in the process of drying the thick wet film. Compared with the traditional method, the method can effectively reduce the residual organic solvent and additive on the suede substrate, prevent the formation of defects in the film, improve the quality of the perovskite film and improve the performance of the device. The defect density in the film of the laminated solar cell prepared by the method is obviously reduced, the laminated solar cell has higher open-circuit voltage and short-circuit current density, and the stability and the photoelectric conversion efficiency of the device are improved.

Description

Perovskite film preparation method and laminated solar cell
Technical Field
The application mainly relates to the technical field of solar cells, in particular to a perovskite thin film preparation method and a crystalline silicon laminated solar cell.
Background
Solar energy is regarded as one of the new clean energy that is paid attention to, has the advantage that the resource is big, low cost. The use of photovoltaic cells to convert solar energy into electrical energy is currently one of the most efficient ways to utilize solar energy. Among them, solar cells such as monocrystalline silicon and polycrystalline silicon have been industrially produced. In recent years, perovskite solar cells have received a great deal of attention from the scientific and industrial fields, and have advantages such as adjustable band gap, small exciton binding force, and high photoelectric conversion efficiency.
Most of the currently existing crystalline silicon/perovskite stacked solar cells are prepared based on polished crystalline silicon bottom cells. This is because the existing perovskite film forming method is generally directed to polishing a substrate, however, the surface of a crystalline silicon cell which has been commercialized on a large scale at this stage is mostly textured. The suede can greatly reduce the reflection of the device on incident light, improve light absorption, and is one of the conditions indispensable for efficient solar cells. Therefore, currently, crystalline silicon/perovskite stacked solar cells based on polished crystalline silicon bottom cells generally have a large light absorption loss and a low short circuit current density.
In this regard, the use of textured crystalline silicon substrates is an essential option to further improve the performance of crystalline silicon/perovskite stacked solar cells. For example, one patent publication No. CN112151634a discloses a method of coating perovskite material on a textured crystalline silicon solar cell, coating perovskite precursor liquid on the textured crystalline silicon cell layer after cleaning, and annealing to obtain a perovskite layer. However, for textured substrates, it is easy to cause non-uniform distribution of perovskite precursor solution because of its characteristic substrate unevenness. When perovskite is formed into a film on a suede substrate and dried, some organic solvents and additives are more likely to remain in the film, so that a large number of defects are caused, and the performance of the device is affected.
Disclosure of Invention
The application aims to solve the problem that the perovskite layer is formed on a textured crystalline silicon solar cell in the existing crystalline silicon perovskite laminated solar cell and is easy to cause solvent residue, and provides a perovskite film preparation method and a laminated solar cell. The method can achieve the effect of uniformly volatilizing the solvent in the process of drying the thick wet film. Compared with the traditional method, the method can effectively reduce the residual organic solvent and additive on the suede substrate, prevent the formation of defects in the film, improve the quality of the perovskite film and improve the performance of the device.
In order to achieve the above purpose, the present application provides the following specific scheme.
A preparation method of a perovskite thin film comprises the steps.
Providing a textured substrate, heating to 60-80 ℃, then immersing the textured substrate into perovskite precursor liquid completely, taking out the textured substrate, draining residual solution at an angle of 0-90 degrees for 0-600 s, and then performing annealing treatment at an annealing temperature of 50-150 degrees to form a perovskite absorption layer on the textured substrate.
Wherein, a low boiling point solvent is added in the perovskite precursor liquid, and the low boiling point solvent comprises one of gamma-valerolactone, diethyl ether, acetone, methylene dichloride and the like.
In one embodiment, the preparing of the pile substrate comprises:
providing a textured silicon substrate, sequentially preparing a base passivation layer, a P-type base doping layer and a first conductive layer on one surface of the textured silicon substrate, sequentially preparing a base surface passivation layer, an N-type base doping layer, a tunneling layer and a hole transmission layer on the other surface of the textured silicon substrate to obtain the textured substrate, wherein the perovskite absorption layer is formed on the hole transmission layer.
Specifically, the first conductive layer comprises a first conductive transparent layer and a first metal electrode layer which are sequentially formed on the P-type doped layer.
In one embodiment, the perovskite thin film preparation method further comprises sequentially forming a passivation layer, an electron transport layer, a buffer layer and a second conductive layer on the surface of the perovskite absorption layer.
Specifically, the second conductive layer includes a second conductive transparent layer and a second metal electrode layer sequentially formed on the buffer layer.
The application also provides a laminated solar cell prepared by the method, which comprises a suede substrate; and the perovskite absorption layer, the passivation layer, the electron transmission layer, the buffer layer and the second conductive layer are sequentially arranged on the surface of the suede substrate.
Specifically, the second conductive layer comprises a second conductive transparent layer and a second metal electrode layer which are sequentially arranged on the buffer layer.
The suede substrate comprises a suede crystalline silicon layer; the tunneling layer and the hole transmission layer are sequentially arranged on one surface of the suede crystalline silicon layer, and the perovskite absorption layer is arranged on the hole transmission layer; and a first conductive layer disposed on the other surface of the textured crystalline silicon layer.
Specifically, the first conductive layer comprises a first conductive transparent layer and a first metal conductive layer which are sequentially arranged on the surface of the suede-like crystalline silicon layer.
Specifically, the textured crystalline silicon layer comprises a textured silicon substrate; the substrate passivation layer and the P-type substrate doping layer are sequentially arranged on one surface of the textured silicon substrate, and the first conductive layer is arranged on the P-type substrate doping layer; and the substrate surface passivation layer and the N-type substrate doping layer are sequentially prepared on the other surface of the textured silicon substrate, and the tunneling layer is arranged on the N-type substrate doping layer.
According to the perovskite film preparation method provided by the application, a certain proportion of low-boiling-point solvent is added into the perovskite precursor solution, and a film preparation method of hot dipping and annealing is adopted. The method can achieve the effect of uniformly volatilizing the solvent in the process of drying the thick wet film. Compared with the traditional method, the method can effectively reduce the residual organic solvent and additive on the suede substrate, prevent the formation of defects in the film, improve the quality of the perovskite film and improve the performance of the device. By using the method, high-quality thick perovskite thin films with the thickness of 1-10um can be prepared, so that complete coverage is formed on the suede and the substrate, and the method can be applied to preparing the crystalline silicon/perovskite laminated solar cell with the high-performance suede crystalline silicon substrate.
Drawings
FIG. 1 is a schematic diagram showing steps of a perovskite thin film preparation method according to example 1 of the present application.
FIG. 2 is a schematic diagram showing steps of a method for producing a perovskite thin film according to comparative example 1 of the present application.
FIG. 3 is a schematic illustration of steps of a method for producing a perovskite thin film according to comparative example 2 of the present application.
FIG. 4 is a schematic diagram showing steps of a method for producing a perovskite thin film according to comparative example 3 of the present application.
Fig. 5 is a schematic structural diagram of a stacked solar cell according to embodiment 1 of the present application.
1. A pile substrate; 2. a perovskite absorber layer; 3. residual solvent; 4. a scraper; 20. perovskite film layer.
10. A first conductive layer; 11. a textured crystalline silicon layer; 12. a tunneling layer; 13. a hole transport layer; 21. a passivation layer; 22. an electron transport layer; 23. buffer layer, 24, second conductive layer.
101. A first metal electrode layer; 102. a first conductive transparent layer; 111. a P-type substrate doping layer; 112. a base passivation layer; 113. a textured silicon substrate; 114. a passivation layer on the surface of the substrate; 115. an N-type substrate doping layer; 241. a second conductive transparent layer; 242. and a second metal electrode layer.
Detailed Description
The following description of the embodiments of the present application will be made clearly and completely with reference to the accompanying drawings, in which it is apparent that the embodiments described are only some embodiments of the present application, but not all embodiments.
In the description of the present application, unless otherwise indicated, the meaning of "a plurality" is two or more; the terms "center," "longitudinal," "transverse," "upper," "lower," "left," "right," "inner," "outer," "front," "rear," "head," "tail," "vertical," "horizontal," "top," "bottom," "inner," "outer," and the like are used as references to orientations or positional relationships based on the orientation or positional relationships shown in the drawings, merely to facilitate description of the application and simplify the description, and do not indicate or imply that the devices or elements referred to must have a particular orientation, be configured and operated in a particular orientation, and are not to be construed as limiting the application. Furthermore, the terms "first," "second," "third," and the like are used for descriptive purposes only and are not to be construed as indicating or implying relative importance.
Referring to fig. 1, an embodiment of the present application provides a method for preparing a perovskite thin film, including the steps of.
Providing a textured substrate 1, heating to 60-80 ℃, then completely immersing the textured substrate 1 in perovskite precursor liquid, then taking out the textured substrate, draining residual solution at an angle of 0-90 degrees for 0-600 s, then performing annealing treatment at 50-150 ℃ to form a perovskite absorption layer 2 on the textured substrate.
In one embodiment, the perovskite precursor liquid is added with a low-boiling point solvent, wherein the low-boiling point solvent comprises one of gamma valerolactone, diethyl ether, acetone, methylene dichloride and the like.
Specifically, the textured substrate 1 is immersed in the perovskite precursor solution, and due to the textured structure on the surface thereof, the perovskite precursor solution can be well attached thereon, and a perovskite film layer 20 is formed when the perovskite precursor solution is taken out, the film layer is a wet film structure, and after annealing treatment, the solvent volatilizes and the molecules react, so that the perovskite absorption layer 2 is formed.
The perovskite absorption layer 2 is specifically ABX 3 Structure, A is an organic cation including CH 3 NH 3 + (MA + )、NH 2 CH＝NH 2 + (FA + )、CH 3 CH 2 NH 3 + Or Cs + At least one of them.
The B position is a metal cation including Pb 2+ 、Sn 2+ At least one of them.
X is a halogen anion including F - 、Cl - 、Br - 、I - At least one of them.
The preparation of the perovskite precursor liquid comprises the following steps: weighing 0.5-3M perovskite powder, dissolving the perovskite powder in 0.5-5 mL of organic solvent, and then adding 0.5-5 mL of low-boiling-point solvent additive to obtain perovskite precursor liquid.
The organic solvent includes at least one of Dimethylformamide (DMF), G-butyrolactone (GBL), dimethyl sulfoxide (DMSO), and N, N-Dimethylacetamide (DMA).
In this embodiment, the textured substrate 1 is a layer film with a textured structure on the surface, and in the production application of a solar cell, the irregular surface of the textured structure can increase the reflection times of sunlight on the surface, effectively reduce the surface reflectivity of the solar cell, and improve the light absorption coefficient of the device, so as to increase the photoelectric conversion efficiency of the device.
However, in the process of forming the perovskite absorbing layer 2 by using the perovskite precursor solution, due to the suede structure on the suede substrate 1, part of the residual solvent 3 remains at the interface between the suede substrate 1 and the perovskite absorbing layer 2, if the residual solvent cannot be further cleaned, defects in the film may be formed, and the performance of the device is reduced.
In the embodiment of the application, a certain proportion of low boiling point solvent is added into perovskite precursor solution, and a film preparation method of hot dipping and annealing is adopted. The method can achieve the effect of uniformly volatilizing the solvent in the process of drying the thick wet film. Compared with the traditional method, the method can effectively reduce the residual organic solvent and additive on the suede substrate, prevent the formation of defects in the film, improve the quality of the perovskite film and improve the performance of the device.
In one embodiment, the preparing of the pile substrate 1 comprises: providing a textured silicon substrate 113, sequentially preparing a base passivation layer 112, a P-type base doped layer 111 and a first conductive layer 10 on one surface of the textured silicon substrate 113, sequentially preparing a base surface passivation layer 114, an N-type base doped layer 115, a tunneling layer 12 and a hole transport layer 13 on the other surface of the textured silicon substrate 113 to obtain the textured substrate 1, wherein the perovskite absorption layer 2 is formed on the hole transport layer 13, and the first conductive layer 10 comprises a first conductive transparent layer 102 and a first metal electrode layer 101 sequentially formed on the P-type base doped layer 111.
In this embodiment, the textured silicon substrate 113 has a textured surface on its surface, and on this basis, each film layer formed on both surfaces of the textured silicon substrate 113 also has a textured structure; specifically, the textured surface of the textured silicon substrate 113 may be prepared by anisotropically etching a silicon wafer with an alkali solution.
The base passivation layer 112 and the base surface passivation layer 114 formed on the two surfaces of the textured silicon substrate 113 are passivation structures, can saturate dangling bonds on the surface of the semiconductor, reduce surface activity, increase a cleaning procedure of the surface, and avoid forming a recombination center due to the introduction of impurities into the surface layer, thereby reducing the surface recombination rate of minority carriers; specifically, the substrate passivation layer 112 and the substrate surface passivation layer 114 may be formed by vapor deposition, atomic layer deposition, or the like.
In this embodiment, the P-type base doped layer 111 and the N-type base doped layer 115 may be formed by diffusion, specifically, a phosphorus source/nitrogen source is adopted to diffuse on the textured silicon substrate 113 to form a doped structure, so as to obtain the P-type base doped layer 111 and the N-type base doped layer 115 respectively.
The first conductive transparent layer 102 may be formed by using a magnetron sputtering method, placing a substrate sample to be prepared in a magnetron sputtering device, controlling the power between 50 and 200W, setting a target material, and sputtering to form the first conductive transparent layer 102; the first metal electrode layer 101 is prepared by vapor deposition, a substrate sample to be prepared is placed on a mask plate for vapor deposition, and the vacuum degree of vapor deposition is 5×10 -5 ～2×10 -4 Pa, evaporating temp. 500-2000 deg.C, evaporating speedA metal material is evaporated to form the first metal electrode layer 101.
In this embodiment, the tunneling layer 12 is prepared by using one of an atomic layer deposition method, a magnetron sputtering method or a wet chemical method, so that the problems of electrical mismatch and unstable devices caused by direct serial connection of the crystalline silicon cell and the perovskite cell can be eliminated.
In this embodiment, the hole transport layer 13 is prepared by spin coating, the dispersion of the hole transport layer is uniformly coated on the surface of the tunneling layer 12, the spin coating speed is 1000-5000rpm, the spin coating time is 10-100s, and after the spin coating is finished, annealing operation is performed, the annealing temperature is 300-600 ℃, and the annealing time is 10-50min, so as to obtain the hole transport layer 13.
In this embodiment, the hole transport layer 13 may also be prepared by using a magnetron sputtering method, and the substrate sample to be prepared is placed in a magnetron sputtering device, the power is controlled to be 30-90W, and the hole transport layer 13 is obtained by sputtering.
In one embodiment, the perovskite thin film preparation method further includes sequentially forming a passivation layer 21, an electron transport layer 22, a buffer layer 23, and a second conductive layer 24 on the surface of the perovskite absorption layer 2, wherein the second conductive layer 24 includes a second conductive transparent layer 241 and a second metal electrode layer 242 sequentially formed on the buffer layer 23.
The passivation layer 21 can be prepared by vapor deposition, the passivation layer material is evaporated onto the surface of the perovskite absorption layer 2, and the vapor deposition vacuum degree is 1-5×10 -4 Pa, evaporating temp. is 50-400 deg.C, evaporating speed isAnd after the evaporation is finished, carrying out annealing operation, wherein the annealing temperature is 0-150 ℃, and the annealing time is 0-30min, so as to obtain the passivation layer 21.
The passivation layer 21 can also be prepared by adopting a spin coating method, the passivation layer dispersion liquid is uniformly coated on the surface of the perovskite absorption layer 2, ultrasonic dissolution and spin coating are carried out, the ultrasonic time is 0-30min, the spin coating rotating speed is 1000-7000rpm, and the spin coating time is 20-120s; and after spin coating, carrying out annealing operation, wherein the annealing temperature is 40-160 ℃, and the annealing time is 5-40min, so as to obtain the passivation layer 21.
The passivation layer 21 can also be prepared by adopting a spraying method, the passivation layer dispersion liquid is sprayed on the surface of the perovskite absorption layer, the spraying speed is 1-100cm/s, after the spraying is finished, annealing operation is carried out, the annealing temperature is 20-170 ℃, and the annealing time is 0-30min, so that the passivation layer 21 is obtained.
The passivation layer 21 is used for reducing the surface activity of the perovskite absorption layer, so that the carrier recombination efficiency of the surface is reduced, and the photoelectric conversion efficiency of the device is improved.
The electron transport layer 22 is prepared by spin coating, the dispersion liquid of the electron transport layer is uniformly coated on the surface of the passivation layer 21, the spin coating rotation speed is 500-4000rpm, and the spin coating time is 10-80s, so that the electron transport layer 22 is obtained.
The electron transport layer 22 may also be prepared by vapor deposition, in which the electron transport layer material is evaporated onto the surface of the passivation layer 21 with a vapor deposition vacuum of 5×10 -5 ～5×10 -4 Pa, evaporating temperature of 100-400 deg.C, evaporating rate ofThe electron transport layer 22 is obtained.
The buffer layer 23 is prepared by atomic layer deposition, and the buffer layer material is deposited on the surface of the electron transport layer 22 by atomic layer deposition equipment with a deposition vacuum degree of 0-1×10 4 Pa, the temperature of the deposition pipeline is between 50 and 150 ℃, the temperature of the deposition chamber is between 40 and 150 ℃, and the buffer layer 23 is obtained.
The buffer layer 23 may also be prepared by vapor deposition, by evaporating the buffer layer material onto the surface of the electron transport layer 22, with a vapor deposition vacuum degree of 6X10 -5 ～4×10 -4 Pa, evaporating temperature of 100-500 deg.C, evaporating rate ofThe buffer layer 23 is obtained.
In this embodiment, the second conductive layer 24 may be prepared by the same method as the first conductive layer 10, specifically, the second conductive transparent layer 241 may be prepared by using a magnetron sputtering method, placing a substrate sample to be prepared in a magnetron sputtering device, controlling the power to be between 50 and 200W, setting a target, and sputtering to form the second conductive transparent layer 241; the first metal electrode layer 242 is formed by vapor deposition, and the substrate sample to be prepared is placed on a mask plate for vapor deposition, wherein the vacuum degree of vapor deposition is 5×10 -5 ～2×10 -4 Pa, evaporating temp. 500-2000 deg.C, evaporating speedA metal material is evaporated to form the second metal electrode layer 242.
According to the perovskite film preparation method provided by the embodiment, the low-boiling point solvent is added into the perovskite precursor liquid, so that volatilization of the solvent on the suede structure is more uniform, solvent residues in the suede structure are reduced, meanwhile, the film layer structure of the interface is further improved, and formation of defects in the film is reduced, so that performance and stability of a device are improved.
Referring to fig. 5, the embodiment of the application further provides a stacked solar cell obtained by the perovskite thin film preparation method, which comprises a suede substrate 1; and a perovskite absorption layer 2, a passivation layer 21, an electron transport layer 22, a buffer layer 23 and a second conductive layer 24 which are sequentially disposed on the textured substrate surface.
Specifically, the second conductive layer 24 includes a second conductive transparent layer 241 and a second metal electrode layer 242 sequentially disposed on the buffer layer 23.
In this embodiment, the surface of the textured substrate 1 is textured, so the perovskite absorption layer 2, the passivation layer 21, the electron transport layer 22, the buffer layer 23 and the second conductive layer 24 formed on the surface of the textured substrate 1 are also film layers with textured structures, and the irregular surface of the textured structures can increase the reflection times of sunlight on the surface, effectively reduce the surface reflectivity of the solar cell, and improve the light absorption coefficient of the device, thereby increasing the photoelectric conversion efficiency of the device.
In the present embodiment, the perovskite absorption layer 2 is specifically ABX 3 Structure, A is an organic cation including CH 3 NH 3 + (MA + )、NH 2 CH＝NH 2 + (FA + )、CH 3 CH 2 NH 3 + Or Cs + At least one of them.
The B position is a metal cation including Pb 2+ 、Sn 2+ At least one of them.
X is a halogen anion including F - 、Cl - 、Br - 、I - At least one of them.
The passivation layer 21 on the perovskite absorption layer 2 can reduce the surface activity of the perovskite absorption layer 2, so that the carrier recombination efficiency on the surface is reduced, and the photoelectric conversion efficiency of the device is improved; specifically, the passivation layer 21 is at least one of propylenediamine iodine (PDADBr), butylammonium chloride (BACl), butylammonium bromide (BABr), butylammonium iodide (BAI), N-dimethyl-1, 3-propylenediamine hydrochloride (DMePDADCl), dodecylenediamine bromine (DDDADBr), magnesium fluoride, lithium fluoride (LiF), and sodium fluoride (NaF).
The electron transport layer 22 can effectively transport electrons and block holes, and specifically, the electron transport layer adopts zinc oxide (ZnO), tin dioxide (SnO 2 ) Titanium dioxide (TiO) 2 )、[6,6]Phenyl C61 methyl butyrate (PC) 61 BM), carbon 60 (C 60 ) At least one of 2, 9-dimethyl-4, 7-diphenyl-1, 10-phenanthroline (BCP).
The buffer layer 23 can effectively improve the problems of energy band mismatch, carrier recombination, chemical reaction and the like between interfaces, further improve the charge separation and collection efficiency in the perovskite battery, and realize the effective improvement of the problems of interfaces and stability, and specifically, the buffer layer 23 is formed by at least one of zinc oxide (ZnO), tin dioxide (SnO 2) and titanium dioxide (TiO 2).
The second conductive layer 24 is composed of a second conductive transparent layer 241 and a second metal electrode layer 242, and plays a role of conducting electrons and outputting current, specifically, the second metal electrode layer 242 is composed of at least one of silver (Ag), gold (Au), copper (Cu), aluminum (Al) and carbon (C); the second conductive transparent layer 241 adopts at least one of Indium Tin Oxide (ITO), indium Zinc Oxide (IZO), and zinc aluminum oxide (AZO).
In this embodiment, the textured substrate 1 includes a textured crystalline silicon layer 11; the tunneling layer 12 and the hole transmission layer 13 are sequentially arranged on one surface of the suede crystalline silicon layer 11, and the perovskite absorption layer 2 is arranged on the hole transmission layer 13; and a first conductive layer 10 disposed on the other surface of the textured silicon layer 11, wherein the first conductive layer 10 includes a first conductive transparent layer 102 and a first metal conductive layer 101 sequentially disposed on the surface of the textured silicon layer 11.
Specifically, the textured crystalline silicon layer 11 includes a textured silicon substrate 113; the substrate passivation layer 112 and the P-type substrate doping layer 111 are sequentially arranged on one surface of the textured silicon substrate 113, and the first conductive layer 10 is arranged on the P-type substrate doping layer 111; and a base surface passivation layer 114 and an N-type base doping layer 115 which are sequentially prepared on the other surface of the textured silicon substrate 113, wherein the tunneling layer 12 is disposed on the N-type base doping layer 115.
The tunneling layer 12 may be made of oxide such as silicon dioxide, and may generate tunneling current at the contact position of the stacked cells to connect the two sub-cells.
The hole transport layer 13 is poly [ bis (4 phenyl) (2, 4,6 trimethylphenyl) amine](PTAA), poly-3-hexylthiophene (P) 3 HT), nickel oxide (NiO) x ) Molybdenum oxide (MoO) x ) At least one of cuprous iodide (CuI) and cuprous thiocyanate (CuSCN) can play a role in transporting holes and blocking electron transport.
In this embodiment, the hole transport layer 13, the perovskite absorption layer 2, the passivation layer 21 and the electron transport layer 22 form a perovskite cell; the P-type base doped layer 111, the base passivation layer 112, the textured silicon substrate 113, the base surface passivation layer 114 and the N-type base doped layer 115 form a textured crystalline silicon layer 11, and the textured crystalline silicon layer 11 is a crystalline silicon cell, specifically, a crystalline silicon cell formed by monocrystalline silicon, polycrystalline silicon or amorphous silicon semiconductor can be selected. The tunneling layer 12 connects the two cells to form a series structure, which can achieve excellent surface passivation and selective collection of carriers, thereby improving the performance of the device.
The application provides a laminated solar cell which comprises a textured substrate 1, a perovskite absorption layer 2, a passivation layer 21, an electron transmission layer 22, a buffer layer 23 and a second conductive layer 24, wherein a low-boiling-point additive is added into a perovskite precursor liquid to achieve the effect of uniformly volatilizing a solvent, so that the solvent residue at the contact interface of the perovskite absorption layer 2 and the textured substrate 1 is reduced, the in-film defect is reduced, the structure of the contact interface of the perovskite absorption layer 2 and the textured substrate 1 is further improved, and the performance and stability of a device are improved.
Specific examples and comparative examples are provided below to clearly and fully describe the technical aspects of the present application. It will be apparent that the described embodiments are some, but not all, embodiments of the application. All other embodiments, which can be made by those skilled in the art based on the embodiments of the application without making any inventive effort, are intended to be within the scope of the application.
Example 1
There is provided a laminated solar cell including a first metal electrode layer 101, a first conductive transparent layer 102, a P-type base doped layer 111, a base passivation layer 112, a textured silicon substrate 113, a base surface passivation layer 114, an N-type base doped layer 115, a tunneling layer 12, a hole transport layer 13, a perovskite absorption layer 2, a passivation layer 21, an electron transport layer 22, a buffer layer 23, a second conductive transparent layer 241, and a second metal electrode layer 242, prepared by a method comprising the steps of:
step one: a textured silicon substrate 113 is provided, a base passivation layer 112 and a P-type base doping layer 111 are sequentially prepared on the back surface of the textured silicon substrate 113, and a base surface passivation layer 114 and an N-type base doping layer 115 are sequentially prepared on the other surface.
Step two: an ITO target was set by a magnetron sputtering method, the power was controlled to be 60W, the running time was 1.5h, and the first conductive transparent layer 102 was formed on the P-type base doping layer 111.
Step three: the substrate sample wafer prepared in the previous step is put into a chamber of an evaporator by an evaporation method, and the vacuum degree of the evaporation is 2 multiplied by 10 -4 Evaporating in Pa, regulating evaporating voltage to evaporating temperature, and controlling evaporating rate atSilver is evaporated onto the first conductive transparent layer 102 to obtain a first metal electrode layer 101.
Step four: and (3) placing the substrate sample wafer prepared in the previous step in a magnetron sputtering device after placing the substrate sample wafer in a mask by utilizing a magnetron sputtering method, controlling the power to be 60W, and controlling the running time to be 1h, and forming a tunneling layer 12 on the N-type substrate doped layer 115, wherein the tunneling layer 12 is silicon dioxide.
Step five: treating the substrate sample wafer prepared in the previous step with UV-Ozone for 15min, preparing a hole transport layer dispersion liquid by using a spin coating method, weighing 0.05mol of NiOx powder to dissolve in 1ml of ultrapure water, and performing ultrasonic vibration for 20min; uniformly coating the hole transport layer dispersion liquid on the surface of the tunneling layer 12, setting the spin coating rotation speed to 2000rpm, the spin coating time to 40s and the solution amount to 100ul; after spin coating was completed, an annealing operation was performed at 450 ℃ for 30min to obtain the hole transport layer 13.
Step six: weigh 1.7M perovskite powder dissolved in 1ml DMF and DMSO solvent. The solvent ratio is 8:2, adding 0.2mL of gamma-valerolactone as a low boiling point solvent additive to obtain perovskite precursor liquid; and heating the substrate sample wafer prepared in the previous step to 60 ℃, and taking out the substrate sample wafer inclined at 45 degrees to drain the residual solvent after the substrate sample wafer is completely immersed in the perovskite precursor liquid for 30s. Then annealing treatment is carried out, wherein the annealing temperature is 110 ℃, and the annealing time is 20min; a perovskite absorption layer 2 having a thickness of 5um was formed on the hole transport layer 13.
Step seven: 3mg of propylenediamine iodine is weighed by an evaporation method and placed in a crucible, a substrate sample prepared in the previous step is placed on a mask plate, and is placed in a chamber of an evaporator until the vacuum degree of evaporation is 2 multiplied by 10 -4 Evaporating in Pa, regulating evaporating voltage to evaporating temperature, and controlling evaporating rate atAnd evaporating propylenediamine iodine on the perovskite absorption layer 2, setting the temperature of an annealing table to 100 ℃ after the evaporation, and carrying out annealing operation for 8min to obtain the passivation layer 21.
Step eight: placing the substrate sample wafer prepared in the previous step on a mask plate by utilizing an evaporation method, and placing the mask plate into a chamber of an evaporation machine until the vacuum degree of evaporation is 1 multiplied by 10 -4 Evaporating in Pa, regulating evaporating voltage to evaporating temperature, and controlling evaporating rate atAnd evaporating C60 on the passivation layer 21 to obtain the electron transport layer 22.
Step nine: setting the vacuum degree of the atomic layer deposition equipment to be 0.5X10 by using an atomic layer deposition method 4 Pa, the temperature of a deposition pipeline is 60 ℃, the temperature of a deposition chamber is 70 ℃, and SnO is processed 2 Evaporating to the endOn the electron transport layer 22, a buffer layer 23 is obtained.
Step ten: an IZO target was set using a magnetron sputtering method, the power was controlled to 50W, the running time was 1h, and a second conductive transparent layer 241 was formed on the buffer layer 23.
Step eleven: the substrate sample wafer prepared in the previous step is put into a chamber of an evaporator by an evaporation method, and the vacuum degree of evaporation is equal toEvaporating, regulating evaporating voltage to evaporating temperature, and controlling evaporating rate at +.>And evaporating silver on the second conductive transparent layer 241 to obtain a second metal electrode layer 242, and finally obtaining the laminated solar cell.
Comparative example 1
A laminated solar cell was provided, which had the same device structure as in example 1, but was different from example 1 in that no gamma valerolactone was added as a low boiling point solvent additive to the perovskite precursor liquid in step six, as shown in FIG. 2.
Comparative example 2
There is provided a laminated solar cell having the same device structure as in example 1, but the manufacturing method is different from example 1 in that in step six, a perovskite absorption layer 2 is manufactured by a conventional method, a perovskite precursor solution is prepared by a flash evaporation method, and perovskite powder is weighed and dissolved in 1ml of DMF and DMSO solvent, the solvent ratio being 8:2, magnetically stirring for 30min, then placing the sample on a spin Tu Yi base, setting the spin speed to be 1000rpm, the spin time to be 10s, the solution amount of the perovskite precursor solution to be 120ul, coating the surface of the sample, placing the sample on a flash evaporation table after spin coating, setting the flash evaporation time to be 30s, setting the flash evaporation temperature to be 30 ℃, carrying out annealing treatment after flash evaporation, setting the annealing temperature to be 100 ℃, setting the annealing time to be 15min, and the thickness to be about 5um, thus obtaining the perovskite absorption layer 2; in addition, the perovskite precursor liquid can be coated on the suede structure in a doctor blade coating, spraying, printing and other modes, as shown in fig. 3.
Comparative example 3
There is provided a laminated solar cell having the same device structure as in example 1, but the manufacturing method is different from example 1 in that the perovskite absorber layer 2 is manufactured by a conventional method in the sixth step, the perovskite precursor solution is prepared by a flash evaporation method instead, and the perovskite powder is weighed and dissolved in 1ml of DMF and DMSO solvent in a solvent ratio of 8:2, magnetically stirring for 30min, then placing the sample on a spin Tu Yi base, setting the spin speed to 3000rpm, the spin time to 30s, the perovskite precursor solution amount to 120ul, coating the surface of the sample, placing the sample on a flash evaporation table after spin coating, setting the flash evaporation time to 30s, the flash evaporation temperature to 30 ℃, carrying out annealing treatment after flash evaporation, setting the annealing temperature to 100 ℃, the annealing time to 15min, and the thickness to about 700 nm; in addition, the perovskite precursor liquid can be coated on the suede structure by a doctor blade coating, spraying, printing and the like, as shown in fig. 4.
The above-mentioned comparative examples 3 and 4 were prepared in a substantially identical manner, with the emphasis that the perovskite film layer 20 (i.e., the wet film formed by the attachment of the perovskite precursor solution) was on top of the textured structure, and the spin-coating speed was high in comparative example 4, and the resulting perovskite film layer 20 substantially covered the textured structure and had a low thickness.
Using a solar simulator to calibrate standard solar light intensity and 1.0cm area 2 The devices obtained in the above examples and comparative examples were subjected to IV test, the initial voltage was set to 1.95V, the cut-off voltage was set to 0V, the measuring range was 100mA, and the results were kept in two decimal places, and the test results are shown in the following table:
perovskite solution with low boiling point solvent, evaporation of perovskite solvent during film formation
It is divided into two steps. 1. In the process of forming a liquid film at an inclined angle, the low-boiling-point solvent slowly evaporates in a first step, takes away organic impurities partially dissolved in the low-boiling-point solvent, and enables perovskite to be uniformly re-textured for nucleation without affecting perovskite film formation. 2. In the annealing film forming process, all solvents are quickly evaporated again to form a high-quality film.
Whereas in the case of solutions without addition of low boiling solvents, the perovskite solvents can only evaporate rapidly at the time of the final annealing step. Thus, perovskite cannot slowly and uniformly nucleate, and thus film formation is not uniform. And because the process speed from liquid state to solid state is too fast, many organic impurities cannot be effectively taken away by solvent evaporation, thereby influencing the film quality.
The application aims to provide a high-efficiency perovskite film forming method based on a textured crystalline silicon substrate, which is used for preparing a high-efficiency perovskite/crystalline silicon laminated solar cell based on the textured substrate. The perovskite thin film prepared by the traditional method cannot form a high-quality thick perovskite thin film on a suede substrate. If a 5um thick film is prepared by a conventional method, a large number of defects are formed in the film due to organic solvent residues, thereby affecting device performance. Comparative example and comparative example 2 it was found that the thick perovskite thin film-based device prepared by the conventional method was low in efficiency, low in open circuit voltage, and greater in attenuation rate. The conventional method can be used to prepare a high quality thin perovskite film, however, in comparative example 3, when the film thickness is reduced to 700nm, the perovskite film cannot completely cover the textured crystalline silicon, thus causing the device in comparative example 3 to be short-circuited, the photoelectric conversion efficiency is only 3.2%, and the open circuit voltage is lower than 1V.
Comparative example 1 and comparative example 1 we have added a low boiling point solvent additive in the hot dip coating process. The additive volatilizes in advance in the hot dipping and draining process, so that the organic solvent and additive residues in the film are removed better. Thus, the device manufactured in example 1 had the best photoelectric conversion efficiency of 31.25%, the highest open circuit voltage of 1.99V, and the lowest attenuation rate of 0.3% at a film thickness of 5um. These high properties all benefit from their lower in-film defects. The application aims to provide a perovskite film preparation method based on a textured crystalline silicon substrate and a crystalline silicon/perovskite laminated solar cell, wherein a certain proportion of low-boiling-point solvent is added into a perovskite precursor solution, and a film preparation method of hot dipping and annealing is adopted, so that the residual organic solvent and additive on the textured substrate are reduced, the formation of defects in the film is prevented, the quality of the perovskite film is improved, and the performance and stability of a device are improved.
The above examples are only preferred embodiments of the present application, it being noted that: it will be apparent to those skilled in the art that various changes, modifications, substitutions and alterations can be made to these embodiments without departing from the principles of the present application, and these equivalents should be substituted for the claims set forth herein without departing from the scope of the application as defined by the appended claims and their equivalents.

Claims (9)

1. The preparation method of the perovskite thin film is characterized by comprising the following steps:
providing a suede substrate, heating to 60-80 ℃, then completely immersing the suede substrate in perovskite precursor liquid, then taking out the suede substrate, draining residual solution at an angle of 0-90 degrees, continuously performing annealing treatment for 0-600 s, wherein the annealing temperature is 50-150 ℃, and forming a perovskite absorption layer on the suede substrate;
the preparation of the perovskite precursor liquid comprises the following steps:
weighing 0.5-3M perovskite powder, dissolving the perovskite powder in 0.5-5 mL of organic solvent, and then adding 0.5-5 mL of low-boiling-point solvent additive to obtain perovskite precursor liquid.
2. The method for preparing a perovskite thin film according to claim 1, wherein a low boiling point solvent is added to the perovskite precursor liquid, and the low boiling point solvent comprises one of gamma valerolactone, diethyl ether, acetone and methylene dichloride.
3. The method of producing a perovskite thin film according to any one of claims 1 to 2, wherein the production of the textured substrate comprises:
providing a textured silicon substrate, sequentially preparing a base passivation layer, a P-type base doping layer and a first conductive layer on one surface of the textured silicon substrate, sequentially preparing a base surface passivation layer, an N-type base doping layer, a tunneling layer and a hole transmission layer on the other surface of the textured silicon substrate to obtain the textured substrate, wherein the perovskite absorption layer is formed on the hole transmission layer.
4. The method of claim 3, wherein the first conductive layer comprises a first conductive transparent layer and a first metal electrode layer sequentially formed on the P-type doped substrate layer.
5. The method according to any one of claims 1 to 2, further comprising sequentially forming a passivation layer, an electron transport layer, a buffer layer, and a second conductive layer on the surface of the perovskite absorption layer.
6. The method of manufacturing a perovskite thin film according to claim 5, wherein the second conductive layer comprises a second conductive transparent layer and a second metal electrode layer sequentially formed on the buffer layer.
7. A laminated solar cell prepared by the perovskite thin film preparation method according to any one of claims 1 to 6, which is characterized by comprising a textured substrate; and the perovskite absorption layer, the passivation layer, the electron transmission layer, the buffer layer and the second conductive layer are sequentially arranged on the surface of the suede substrate.
8. The laminated solar cell of claim 7, wherein the textured substrate comprises a textured crystalline silicon layer; the tunneling layer and the hole transmission layer are sequentially arranged on one surface of the suede crystalline silicon layer, and the perovskite absorption layer is arranged on the hole transmission layer; and a first conductive layer disposed on the other surface of the textured crystalline silicon layer.
9. The stacked solar cell of claim 8, wherein the textured crystalline silicon layer comprises a textured silicon substrate; the substrate passivation layer and the P-type substrate doping layer are sequentially arranged on one surface of the textured silicon substrate, and the first conductive layer is arranged on the P-type substrate doping layer; and the substrate surface passivation layer and the N-type substrate doping layer are sequentially prepared on the other surface of the textured silicon substrate, and the tunneling layer is arranged on the N-type substrate doping layer.
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