CN117355190A - Perovskite passivation method based on ultrasonic technology and laminated solar cell - Google Patents
Perovskite passivation method based on ultrasonic technology and laminated solar cell Download PDFInfo
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- WFWMQVKKOITTHO-UHFFFAOYSA-N propane-1,2-diamine;hydrobromide Chemical compound Br.CC(N)CN WFWMQVKKOITTHO-UHFFFAOYSA-N 0.000 claims description 2
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- JYMITAMFTJDTAE-UHFFFAOYSA-N aluminum zinc oxygen(2-) Chemical compound [O-2].[Al+3].[Zn+2] JYMITAMFTJDTAE-UHFFFAOYSA-N 0.000 description 1
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- PWLNAUNEAKQYLH-UHFFFAOYSA-N butyric acid octyl ester Natural products CCCCCCCCOC(=O)CCC PWLNAUNEAKQYLH-UHFFFAOYSA-N 0.000 description 1
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- AMGQUBHHOARCQH-UHFFFAOYSA-N indium;oxotin Chemical compound [In].[Sn]=O AMGQUBHHOARCQH-UHFFFAOYSA-N 0.000 description 1
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- UUIQMZJEGPQKFD-UHFFFAOYSA-N n-butyric acid methyl ester Natural products CCCC(=O)OC UUIQMZJEGPQKFD-UHFFFAOYSA-N 0.000 description 1
- 229910052757 nitrogen Inorganic materials 0.000 description 1
- PQQKPALAQIIWST-UHFFFAOYSA-N oxomolybdenum Chemical compound [Mo]=O PQQKPALAQIIWST-UHFFFAOYSA-N 0.000 description 1
- GNRSAWUEBMWBQH-UHFFFAOYSA-N oxonickel Chemical compound [Ni]=O GNRSAWUEBMWBQH-UHFFFAOYSA-N 0.000 description 1
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Classifications
-
- 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
- H10K10/00—Organic devices specially adapted for rectifying, amplifying, oscillating or switching; Organic capacitors or resistors having potential barriers
- H10K10/80—Constructional details
- H10K10/88—Passivation; Containers; Encapsulations
-
- 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
- Y02—TECHNOLOGIES OR APPLICATIONS FOR MITIGATION OR ADAPTATION AGAINST CLIMATE CHANGE
- 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
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- Engineering & Computer Science (AREA)
- Manufacturing & Machinery (AREA)
- Photovoltaic Devices (AREA)
Abstract
According to the perovskite passivation method based on the ultrasonic process, the battery substrate of the prepared perovskite absorption layer is immersed in the passivating agent solution, and the passivating agent is infiltrated into the perovskite film by assistance of ultrasonic treatment, so that the internal crystal boundary and the surface of the perovskite absorption layer can be passivated on the premise of not changing the film forming characteristic of the perovskite absorption layer, the generation of internal defects is reduced, the quality of the perovskite film is improved, and the laminated solar cell obtained by the method has higher photoelectric conversion efficiency and stability.
Description
Technical Field
The invention mainly relates to the technical field of solar cells, in particular to a perovskite passivation method based on an ultrasonic process and a 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.
The photoelectric conversion efficiency of the current crystalline silicon/perovskite laminated solar cell exceeds 32%, and although the photoelectric conversion efficiency is different from the theoretical value, a great progress space still exists compared with that of a single-junction solar cell, wherein the passivation process of the perovskite is also an important factor influencing the performance and stability of the whole device. In the traditional method, a passivation layer is deposited on the prepared perovskite film for one time, so that the passivation effect is realized, however, the method lacks effective passivation on the crystal boundary in the perovskite film, so that defects in the film are still much, and the photoelectric conversion efficiency and stability of the crystalline silicon/perovskite laminated solar cell are affected; or adding a passivating agent into the perovskite precursor liquid to passivate crystal boundaries, and changing the film forming property of the perovskite to form a low-quality perovskite film although the generation of internal defects can be reduced.
Disclosure of Invention
The invention aims to solve the problem that the inner film of the crystalline silicon/perovskite laminated solar cell cannot be effectively passivated in the existing crystalline silicon/perovskite laminated solar cell, and provides a perovskite passivation method based on an ultrasonic process and a laminated solar cell. Compared with the traditional method, the method can effectively enable the passivating agent to permeate into the perovskite film, reduce defects in the film, especially at the perovskite crystal interface, improve the quality of the perovskite film and improve the device performance.
In order to achieve the above purpose, the present invention provides the following specific scheme.
A perovskite passivation method based on an ultrasonic process, comprising the steps of:
providing a battery substrate, coating perovskite precursor liquid on the surface of the battery substrate, carrying out annealing treatment to obtain a perovskite absorption layer, wherein the annealing temperature is 50-80 ℃, the annealing time is 5-40 min, then immersing the battery substrate in a passivating agent solution, carrying out ultrasonic treatment for 120-360 s, taking out the battery substrate, draining, carrying out second annealing treatment, and the annealing temperature is 100-160 ℃, and the annealing time is 5-40 min, so that a passivation layer is formed on the inner crystal boundary and the surface of the perovskite absorption layer;
the passivating agent solution is a solution obtained by dissolving propylenediamine iodine in an organic solvent, the concentration is 0.1-6 mg/ml, and the organic solvent comprises at least one of methanol, ethanol or isopropanol.
After the perovskite precursor liquid is coated on the battery substrate, spin coating treatment can be carried out, the spin coating rotating speed is 1000-6000 rpm, and the spin coating time is 20-120 s.
In one embodiment, the preparation of the battery substrate comprises:
providing a silicon substrate, sequentially preparing a base passivation layer, a P-type base doping layer and a first conductive layer on one surface of the 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 silicon substrate, and obtaining the battery 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 substrate doping layer.
In one embodiment, the perovskite passivation method based on the ultrasonic process further comprises sequentially forming an electron transport layer, a buffer layer and a second conductive layer on the surface of the passivation 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 invention also provides a laminated solar cell prepared by the method, which comprises a cell 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 battery 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 battery substrate includes: a crystalline silicon layer; the perovskite absorption layer is arranged on the hole transmission layer; and a first conductive layer provided on the other surface of the crystalline silicon layer.
Specifically, the first conductive layer comprises a first conductive transparent layer and a first metal electrode layer which are sequentially arranged on the surface of the crystalline silicon layer.
Specifically, the crystalline silicon layer includes: a silicon substrate; the substrate passivation layer and the P-type substrate doping layer are sequentially arranged on one surface of the silicon substrate, and the first conductive layer is arranged on the P-type substrate doping layer; and the tunneling layer is arranged on the N-type base doping layer.
According to the perovskite passivation method based on the ultrasonic process, the battery substrate of which the perovskite absorption layer is prepared is immersed in the passivating agent solution, and the passivating agent is infiltrated into the perovskite film by assistance of ultrasonic treatment, so that the internal crystal boundary and the surface of the perovskite absorption layer can be passivated on the premise of not changing the film forming characteristic of the perovskite absorption layer, the generation of internal defects is reduced, the quality of the perovskite film is improved, the device performance is improved, and the laminated solar cell obtained by the method has higher photoelectric conversion efficiency and stability.
Drawings
Fig. 1 is a schematic diagram of steps of a perovskite passivation method based on an ultrasonic process according to an embodiment of the invention.
Fig. 2 is a schematic structural diagram of a stacked solar cell according to an embodiment of the invention.
1. A battery substrate; 2. a perovskite absorber layer;
10. a first conductive layer; 11. a 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 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 invention 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 invention, but not all embodiments.
In the description of the present invention, 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 invention 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 invention. 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 invention provides a perovskite passivation method based on an ultrasonic process, including the steps of:
providing a battery substrate 1, coating perovskite precursor liquid on the surface of the battery substrate 1, performing annealing treatment to obtain a perovskite absorption layer 2, wherein the annealing temperature is 50-80 ℃ and the annealing time is 5-40 min, then immersing the battery substrate 1 in a passivating agent solution and performing ultrasonic treatment for 120-360 s, taking out the battery substrate 1, draining, performing second annealing treatment, and the annealing temperature is 100-160 ℃ and the annealing time is 5-40 min, thereby forming a passivation layer 2 on the inner crystal boundary and the surface of the perovskite absorption layer 2;
the passivating agent solution is a solution obtained by dissolving propylenediamine iodine in an organic solvent, the concentration is 0.1-6 mg/ml, and the organic solvent comprises at least one of methanol, ethanol or isopropanol.
In other embodiments, the passivating agent solution may be prepared by dissolving at least one of propylenediamine bromide (PDADBr), butylammonium chloride (BACl), butylammonium bromide (BABr), butylammonium iodide (BAI), N-dimethyl-1, 3-propylenediamine hydrochloride (DMePDADCl), dodecylenediamine bromide (DDDADBr), magnesium fluoride, lithium fluoride (LiF) and sodium fluoride (NaF) in an organic solvent, wherein the concentration is 0.1-6 mg/ml, and the organic solvent comprises at least one of methanol, ethanol or isopropanol.
When the perovskite film is passivated by the traditional method, a passivation layer is prepared above the perovskite film, the passivation material is difficult to permeate into the perovskite film, and the addition of the passivating agent in the perovskite precursor liquid influences the crystallization effect of the perovskite, so that the film forming quality is influenced.
The method adopts the ultrasonic process to assist the passivation process of the perovskite, so that the structure of the perovskite crystal is not influenced, meanwhile, the perovskite film can be infiltrated into the interior to passivate the crystal boundary, the passivation effect is improved, and the performance and the stability of the perovskite film are improved.
In order to further improve the passivation effect and not destroy the result of the formed perovskite film, the process adopts twice annealing treatment in the preparation process, the passivation solvent is dried at low temperature for the first annealing, and the purpose of the second annealing is to enable the passivating agent to react with the perovskite crystal boundary and the surface, so that the passivating agent can completely passivate defects.
After the perovskite precursor liquid is coated on the battery substrate 1, spin coating treatment can be further carried out, the spin coating rotating speed is 1000-6000 rpm, and the spin coating time is 20-120 s.
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: and weighing 0.5-3M perovskite powder, and dissolving the perovskite powder in 0.5-5 mL of organic solvent 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 other embodiments, the battery substrate 1 may also be provided with a layer film having a textured structure on a surface, and in the production application of the solar cell, the irregular surface of the textured structure may increase the reflection times of sunlight on the surface, so as to 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 one embodiment, the preparation of the battery substrate 1 includes: providing a 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 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 silicon substrate 113 to obtain the battery 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.
The base passivation layer 112 and the base surface passivation layer 114 formed on the two surfaces of the 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 used to diffuse on the 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 to be 50-200 w, setting a target, 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, the evaporation temperature is 500-2000 ℃, the evaporation rate is 0.1-5A/S, and the 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 10-50 min, 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 passivation method based on the ultrasonic process further includes sequentially forming an electron transport layer 22, a buffer layer 23 and a second conductive layer 24 on the surface of the passivation layer 21, 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 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 at 100-400 ℃ and evaporating rate at 0.05-1A/S to obtain the electron transport layer 22.
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 50-150 ℃, the temperature of the deposition chamber is 40-150 ℃, 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, the evaporation temperature is 100-500 ℃, the evaporation rate is 0.05-1A/S, and the 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 50-200 w, setting a target, and sputtering to form the second conductive transparent layer 241; the first metal electrode layer 101 is formed by vapor deposition, and a 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, the evaporation temperature is 500-2000 ℃, the evaporation rate is 0.1-5A/S, and the metal material is evaporated to form the second metal electrode layer 242.
According to the perovskite passivation method based on the ultrasonic process, the battery substrate of which the perovskite absorption layer is prepared is immersed in the passivating agent solution, and the passivating agent is infiltrated into the perovskite film by assistance of ultrasonic treatment, so that the internal crystal boundary and the surface of the perovskite absorption layer can be passivated on the premise of not changing the film forming characteristic of the perovskite absorption layer, the generation of internal defects is reduced, the quality of the perovskite film is improved, and the device performance is improved.
Referring to fig. 2, the embodiment of the present invention further provides a stacked solar cell obtained by the perovskite passivation method based on the ultrasonic process, including a cell 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 sequentially disposed on the surface of the battery substrate 1.
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 other embodiments, the surface of the battery substrate 1 may be configured as a textured structure, 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 battery substrate 1 may be also a film layer with a textured structure, and the irregular surface of the textured structure may increase the number of reflection times of sunlight on the surface, so that the surface reflectivity of the solar cell may be effectively reduced, and the light absorption coefficient of the device may be improved, 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 the present embodiment, the battery substrate 1 includes a crystalline silicon layer 11; a tunneling layer 12 and a hole transport layer 13 sequentially arranged on one surface of the crystalline silicon layer 11, wherein the perovskite absorption layer 2 is arranged on the hole transport layer 13; and a first conductive layer 10 disposed on the other surface of the crystalline silicon layer 11, the first conductive layer 10 including a first conductive transparent layer 102 and a first metal electrode layer 101 sequentially disposed on the surface of the crystalline silicon layer 11.
Specifically, the crystalline silicon layer 11 includes a silicon substrate 113; a base passivation layer 112 and a P-type base doping layer 111 sequentially arranged on one surface of the silicon substrate 113, wherein the first conductive layer 10 is arranged on the P-type base doping layer 111; and a base surface passivation layer 114 and an N-type base doping layer 115 sequentially prepared on the other surface of the 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 silicon substrate 113, the base surface passivation layer 114 and the N-type base doped layer 115 form a crystalline silicon layer 11, and the crystalline silicon layer 11 is a crystalline silicon cell, specifically, a crystalline silicon cell formed by monocrystalline silicon, polycrystalline silicon or amorphous silicon semiconductor may 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 invention provides a laminated solar cell, which comprises a cell 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 the passivation layer 21 penetrates into the crystal boundary and the surface in the perovskite absorption layer 2 in an ultrasonic mode, so that a perovskite film can be effectively passivated, the defects in the film are reduced, and the performance and the 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 invention. It will be apparent that the described embodiments are some, but not all, embodiments of the invention. All other embodiments, which can be made by those skilled in the art based on the embodiments of the invention without making any inventive effort, are intended to be within the scope of the invention.
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 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, a second metal electrode layer 242, prepared by a method comprising the steps of:
step one: a 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 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 And (3) performing evaporation at Pa, adjusting the evaporation voltage to the evaporation temperature, controlling the evaporation rate to be 2.5A/S, and evaporating silver to the first conductive transparent layer 102 to obtain the 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 15 min, preparing a hole transport layer dispersion liquid by using a spin coating method, weighing 0.05 mol of NiOx powder to dissolve in 1 ml ultrapure water, and performing ultrasonic vibration for 20 min; 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 30 min to obtain the hole transport layer 13.
Step six: weigh 1.7M perovskite powder dissolved in 1 ml DMF and DMSO solvent. The solvent ratio is 8:2, obtaining perovskite precursor liquid; coating 120ul of perovskite precursor liquid on the surface of a substrate sample wafer prepared in the previous step, and then performing spin coating treatment, wherein the spin coating rotating speed is 3500rpm; then annealing treatment is carried out, wherein the annealing temperature is 80 ℃, and the annealing time is 15 min; a perovskite absorption layer 2 having a thickness of 500nm was formed on the hole transport layer 13.
Step seven: immersing the substrate sample wafer prepared in the previous step into a passivating agent solution, carrying out ultrasonic treatment for 60 seconds, taking out, draining and annealing, wherein the annealing temperature is 100 ℃, and the annealing time is 10 minutes, so as to obtain the passivation layer 21; the passivating agent solution is prepared by dissolving propylenediamine iodine in a methanol solvent, and the concentration is 2mg/ml.
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 And (3) performing evaporation in Pa, adjusting the evaporation voltage to the evaporation temperature, controlling the evaporation rate to be 0.1-0.15A/S, and performing evaporation of C60 onto 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 Vapor deposition is performed on the electron transport layer 22 to obtain a buffer layer 23.
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 utilizing an evaporation method,vacuum degree to be evaporated is 2 x 10 -4 And (3) performing evaporation at Pa, adjusting the evaporation voltage to the evaporation temperature, controlling the evaporation rate to be 2.5A/S, and evaporating silver to the second conductive transparent layer 241 to obtain a second metal electrode layer 242, thereby finally obtaining the laminated solar cell.
Example 2
A laminated solar cell was provided, which had the same device structure as in example 1, but the manufacturing method was different from example 1 in that the ultrasonic treatment time in step seven was 120s.
Example 3
A laminated solar cell was provided, which had the same device structure as in example 1, but the manufacturing method was different from example 1 in that the ultrasonic treatment time in step seven was 240s.
Example 4
A stacked solar cell was provided having the same device structure as in example 1, but the manufacturing method was different from example 1 in that the ultrasonic treatment time in step seven was 360s.
Example 5
A laminated solar cell was provided, which had the same device structure as in example 1, but the manufacturing method was different from example 1 in that no ultrasonic treatment was used in step seven.
Example 6
A laminated solar cell was provided, which had the same device structure as in example 1, but was different from example 1 in that step seven was removed, and in step six, 0.5mol%/mL of propylenediamine iodine was added to the perovskite precursor solution.
A standard solar light intensity calibration was performed using a solar simulator and the area was 1.0. 1.0 cm 2 The device obtained in the above examples was subjected to IV test, the initial voltage was set to 1.95V, the cut-off voltage was set to 0V, and the range was set to 100 mA, and the test results are shown in the following table:
| device and method for manufacturing the same | Open circuit voltage (V) | Short-circuit current (mA/cm) 2 ） | Photoelectric conversion efficiency (%) | Efficiency decay Rate (%/year) |
| Example 1 | 1.96 | 20.4 | 30.2 | 0.8 |
| Example 2 | 1.98 | 20.8 | 32.4 | 0.3 |
| Example 3 | 1.98 | 20.6 | 32.1 | 0.2 |
| Example 4 | 1.98 | 20.7 | 32.2 | 0.3 |
| Example 5 | 1.92 | 20.6 | 29.4 | 3.6 |
| Example 6 | 1.90 | 20.2 | 28.8 | 4.4 |
The invention aims to provide a perovskite passivation method based on an ultrasonic process, which can simultaneously complete high-quality perovskite film interface passivation and perovskite film internal grain boundary passivation under the condition that the film forming property of perovskite from precursor solution to a film is not changed and a high-quality perovskite film is reserved.
The invention also aims to optimize the ultrasonic time of the ultrasonic passivation process, and among examples 1-4 adopting the ultrasonic passivation process, example 1 has the lowest photoelectric conversion efficiency and open-circuit voltage, which shows that the ultrasonic time is 60s insufficient to enable passivating agent solution to permeate into crystal boundaries inside a film to complete passivation, and examples 2,3 and 4 all have similar photoelectric conversion efficiency and open-circuit voltage, which shows that the ultrasonic time is 120s to enable a device to complete higher-quality passivation, and further prolongs the ultrasonic time to 240s and 360s, compared with 120s, no obvious difference is generated; however, in examples 5 and 6, the passivation effect was poor and the photoelectric conversion efficiency and stability were not good, and example 6 further illustrates that the addition of the passivation agent in the preparation of the perovskite thin film also affects the overall film formation quality of the perovskite absorption layer, thereby affecting the photoelectric conversion efficiency and stability.
The above examples are only preferred embodiments of the present invention, 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 invention, and these equivalents should be substituted for the claims set forth herein without departing from the scope of the invention as defined by the appended claims and their equivalents.
Claims (10)
1. A perovskite passivation method based on an ultrasonic process, comprising the steps of:
providing a battery substrate, coating perovskite precursor liquid on the surface of the battery substrate, carrying out annealing treatment to obtain a perovskite absorption layer, wherein the annealing temperature is 50-80 ℃, the annealing time is 5-40 min, then immersing the battery substrate in a passivating agent solution, carrying out ultrasonic treatment for 120-360 s, taking out the battery substrate, draining, carrying out second annealing treatment, and the annealing temperature is 100-160 ℃, and the annealing time is 5-40 min, so that a passivation layer is formed on the inner crystal boundary and the surface of the perovskite absorption layer;
the passivating agent solution is a solution obtained by dissolving propylenediamine iodine in an organic solvent, the concentration is 0.1-6 mg/ml, and the organic solvent comprises at least one of methanol, ethanol or isopropanol.
2. The ultrasonic process-based perovskite passivation method according to claim 1, wherein the preparation of the perovskite precursor liquid comprises:
weighing 0.5-3M perovskite powder, dissolving the perovskite powder in 0.5-5 mL of organic solvent to obtain perovskite precursor liquid,
the organic solvent includes at least one of Dimethylformamide (DMF), G-butyrolactone (GBL), dimethyl sulfoxide (DMSO), or N, N-Dimethylacetamide (DMA).
3. The ultrasonic process-based perovskite passivation method according to claim 1, wherein the passivating agent solution is prepared by dissolving at least one of propylenediamine bromide (PDADBr), butylammonium chloride (BACl), butylammonium bromide (BABr), butylammonium iodide (BAI), N-dimethyl-1, 3-propylenediamine hydrochloride (dmepdbdcl), dodecylenediamine bromide (DDDADBr), magnesium fluoride, lithium fluoride (LiF), sodium fluoride (NaF) in an organic solvent, wherein the concentration is 0.1-6 mg/ml, and the organic solvent comprises at least one of methanol, ethanol, or isopropanol.
4. The perovskite passivation method based on the ultrasonic process according to claim 1, wherein after the perovskite precursor liquid is coated on the battery substrate, spin coating treatment is performed, the spin coating speed is 1000-6000 rpm, and the spin coating time is 20-120 s.
5. The ultrasonic process-based perovskite passivation method according to any one of claims 1 to 4, wherein the preparation of the battery substrate comprises:
providing a silicon substrate, sequentially preparing a base passivation layer, a P-type base doping layer and a first conductive layer on one surface of the 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 silicon substrate, and obtaining the battery substrate, wherein the perovskite absorption layer is formed on the hole transmission layer.
6. The ultrasonic process-based perovskite passivation method according to claim 5, wherein the first conductive layer comprises a first conductive transparent layer and a first metal electrode layer sequentially formed on the P-type substrate doped layer.
7. The ultrasonic process-based perovskite passivation method according to any one of claims 1 to 4, further comprising sequentially forming an electron transport layer, a buffer layer and a second conductive layer on the passivation layer.
8. The ultrasonic process-based perovskite passivation method according to claim 7, wherein the second conductive layer comprises a second conductive transparent layer and a second metal electrode layer sequentially formed on the buffer layer.
9. A laminated solar cell prepared by the perovskite passivation method based on the ultrasonic process according to any one of claims 1 to 8, comprising a cell 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 battery substrate.
10. The laminated solar cell of claim 9, wherein the cell substrate comprises a crystalline silicon layer; the perovskite absorption layer is arranged on the hole transmission layer; and a first conductive layer provided on the other surface of the crystalline silicon layer.
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