CN112151679B - Nano-crystal composite perovskite solar cell and preparation method thereof - Google Patents
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- 230000031700 light absorption Effects 0.000 claims abstract description 16
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- 238000004528 spin coating Methods 0.000 claims description 25
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Abstract
The invention discloses a nano-crystal composite perovskite solar cell, and relates to the technical field of solar cells. The light absorption layer is arranged on the conductive substrate in a stacking mode; the light absorption layer includes a perovskite thin film, and semiconductor oxide nanoparticles contained in the perovskite thin film. The invention also discloses a preparation method of the nano-crystal composite perovskite solar cell. The nanocrystalline composite perovskite solar cell provided by the invention has high photoelectric conversion efficiency, the photoelectric conversion efficiency is improved from 18% to more than 21%, and the performance and the stability are obviously improved.
Description
Technical Field
The invention belongs to the technical field of solar cells, and relates to a nano-crystal composite perovskite solar cell and a preparation method thereof.
Background
The problems of current carrier recombination, poor stability and the like faced by the perovskite solar cell hinder the practical process of the perovskite solar cell. Therefore, how to further improve the efficiency and stability of the perovskite battery becomes a critical problem to be solved urgently. The lithium salt contained in the hole transport layer material used by the polycrystalline perovskite thin film prepared by the low-temperature solution method can cause lithium ions to permeate at the grain boundary in the perovskite thin film, so that the current carriers are compounded, and the performance of the battery is reduced.
By means of the modification of carbon quantum dots on the perovskite solar cell, the introduction of a material with stronger carrier transmission capability/high conductivity into the film is expected to promote the bulk transmission process of carriers in the perovskite film, and further improve the performance of the perovskite solar cell. The crystal boundary of the perovskite thin film is modified by selecting the nanocrystalline material with high hole migration, the material with high hole migration is introduced into the thin film, the bulk transmission process of holes is hopefully promoted, and the nanocrystalline introduced at the crystal boundary can prevent the penetration of lithium ions so as to improve the long-term stability of the perovskite battery. How to introduce a material with high hole migration into the perovskite thin film is a difficult point for obtaining a high-performance solar cell with excellent long-term stability, which is also a technical problem to be solved by the invention.
Disclosure of Invention
In order to solve the defects, the invention provides the nano-crystal composite perovskite solar cell and the preparation method thereof, the solar cell has high hole mobility and high photoelectric conversion efficiency with excellent long-term stability, and meanwhile, the liquid-phase pulse laser irradiation technology can be adopted to directly prepare the oxide nano-crystal solution with controllable size, monodispersity and stable high hole mobility, and the oxide nano-crystal solution can be directly put into use without complex processes such as solvent/ligand exchange, centrifugal drying and the like.
The invention provides a nanocrystal composite perovskite solar cell, which comprises a conductive substrate, an electron transmission layer, a light absorption layer, a hole transmission layer and a metal electrode layer which are sequentially stacked from bottom to top;
the light absorption layer includes a perovskite thin film, and semiconductor oxide nanoparticles contained in the perovskite thin film.
Preferably, the semiconductor oxide particles are NiO and SmNiO 3 、CuCrO 3 、GaCrO 3 One kind of (1).
More preferably, the light absorption layer is prepared by the following steps:
firstly, uniformly dispersing semiconductor oxide nano particles in an organic liquid phase medium, and irradiating by pulse laser beams to prepare a nano crystal colloidal solution;
secondly, spin-coating a perovskite precursor solution on the electron transport layer, adding the nanocrystalline colloid solution in the spin-coating process, and then carrying out heat treatment at 100-150 ℃ for 10-90 min to obtain the light absorption layer;
wherein the usage ratio of the perovskite precursor to the semiconductor oxide nanoparticles is 1moL: 0.037-4.76 g.
More preferably, the concentration of the nanocrystalline colloidal solution is 0.01-0.5 mg/mL.
More preferably, the concentration of the perovskite precursor solution is 1.05 to 1.35mol/L.
More preferably, the organic liquid medium is one or more of ethyl formate, ethyl acetate, diethyl ether and diethyl ether.
More preferably, the perovskite precursors are AX and BX 2 A compound of type (I);
wherein A is CH 3 NH 3 + 、HC(＝NH)NH 2 + 、Cs + One or more of (a);
b is Pb 2+ ；
And X is one or more of halogen ions.
More preferably, the wavelength of the pulse laser is 1064nm, 532nm or 355nm, the energy is 50-1000 mJ/pulse, and the irradiation time is 2-30 min.
More preferably, the perovskite precursor solution is spin-coated on the electron transport layer in two steps of low speed 1000rpm/10s and high speed 4000rpm/30s, and the nanocrystalline colloid solution is dropwise added when the residual 5-15 s are left in the high speed spin-coating.
The second purpose of the invention is to provide a preparation method of a nanocrystal composite perovskite solar cell, which comprises the following steps:
spin-coating a perovskite precursor solution on a conductive substrate covered with an electron transport layer, adding a certain amount of nanocrystalline colloid solution while spin-coating, and forming a nanocrystalline composite perovskite thin film after heat treatment; and then spin-coating a hole transport layer and evaporating a metal electrode on the nano-crystal composite perovskite thin film in sequence to obtain the nano-crystal composite perovskite solar cell.
Compared with the prior art, the invention has the beneficial effects that:
the nano-crystal composite perovskite thin-film solar cell provided by the invention has high efficiency and good stability, the photoelectric conversion efficiency is increased to more than 21% from 18% of the basic efficiency, the photoelectric conversion efficiency of the perovskite solar cell prepared by a low-temperature solution method is improved, and the nano-crystal composite perovskite thin-film solar cell has extremely high application prospect.
The invention adopts the liquid-phase pulse laser irradiation technology to directly prepare the oxide nanocrystal solution with controllable size, monodispersity and high hole mobility, can be directly put into use without complex processes such as solvent/ligand exchange, centrifugal drying and the like, and has simple method and mild conditions in the whole preparation process compared with the nanocrystal solution prepared by the traditional preparation method.
Drawings
FIG. 1 shows SmNiO prepared in example 2 3 Transmission spectrum of the nanocrystal.
Fig. 2 is a current-voltage curve of the nanocrystal-composited perovskite solar cell provided in example 1, as well as the pristine perovskite solar cell that was not composited.
Fig. 3 is a current-voltage curve of the nanocrystalline composited perovskite solar cell provided in example 2, as well as the pristine perovskite solar cell that was not composited.
Fig. 4 is a current-voltage curve for the nanocrystalline composited perovskite solar cell provided in example 3, as well as the pristine perovskite solar cell that was not composited.
Detailed Description
In order to make the technical solutions of the present invention better understood and implemented by those skilled in the art, the present invention is further described below with reference to the following specific embodiments and the accompanying drawings, but the embodiments are not meant to limit the present invention.
Example 1
A nanocrystal composite perovskite solar cell comprises a conductive substrate, an electron transmission layer, a light absorption layer, a hole transmission layer and a metal electrode layer which are sequentially stacked from bottom to top;
the light absorption layer includes a perovskite thin film, and semiconductor oxide nanoparticles contained in the perovskite thin film. The semiconductor oxide particles are NiO;
the specific preparation method of the nano-crystal composite perovskite solar cell comprises the following steps:
s1, under the assistance of ultrasound, irradiating 3mL of NiO-ethyl acetate suspension solvent with the concentration of 0.1mg/mL by using pulse laser with the wavelength of 355nm and the energy of 100mJ for 10min to prepare NiO nanocrystalline ethyl acetate colloidal solution with the size of about 3nm and the concentration of 0.1mg/m L;
s2, preparing concentrate in a nitrogen glove boxLead iodide methylamine (MAPbI) at a concentration of 1.25mol/L 3 ) Perovskite precursor solution: weighing 1.25mmol of CH in a reagent bottle 3 NH 3 I. 1.25mmol of PbI 2 Adding 700 mu L of dimethylformamide and 300 mu L of dimethyl sulfoxide, stirring the mixed solution at 60 ℃ for 2 hours, and filtering by using an organic filter head to obtain 1mL of 1.25mol/L perovskite precursor solution for experiment;
s3, taking 30 mu L of perovskite precursor solution prepared in S2, spin-coating the perovskite precursor solution on an FTO conductive substrate covered with a 70nm TiO2 electronic transmission layer, spin-coating at a low speed (1000 rmp) for 10S, then spin-coating at a high speed (5000 rmp) for 30S, immediately dropwise adding 200 mu L of NiO nanocrystalline ethyl acetate colloidal solution prepared by S1 when the residual 10S is spin-coated at a high speed, and after dropwise adding, carrying out heat treatment at 100 ℃ for 30min to prepare the NiO nanocrystalline composite MAPbI 3 The perovskite thin film layer is uniform and flat in surface and 550nm in thickness;
s4, coating a hole transport layer material Spiro-OMeTAD on the perovskite thin film layer prepared in the S3 in a spinning mode, and oxidizing in the air for 12 hours to obtain a hole transport layer with the thickness of 120 nm;
s5, evaporating and plating a layer with the area of 0.1cm on the hole transport layer of the S4 2 And an Au electrode with the thickness of 100nm to obtain the NiO nanocrystal compounded MAPbI 3 A perovskite solar cell;
this example provides a cell with a photoelectric conversion efficiency of 19.7%.
Example 2
A nanocrystal composite perovskite solar cell comprises a conductive substrate, an electron transmission layer, a light absorption layer, a hole transmission layer and a metal electrode layer which are sequentially stacked from bottom to top;
the light absorption layer includes a perovskite thin film, and semiconductor oxide nanoparticles contained in the perovskite thin film. The semiconductor oxide particles are SmNiO 3 ；
The specific preparation method of the nano-crystal composite perovskite solar cell comprises the following steps:
s1, under the assistance of ultrasound, irradiating pulse laser with the wavelength of 1064nm and the energy of 1000mJAccording to 3mL of SmNiO with the concentration of 0.03mg/mL 3 Diethyl ether suspension solvent for 10min to prepare SmNiO with the size of about 5-10nm and the concentration of 0.03mg/m L 3 A nanocrystalline diethyl ether colloidal solution; FIG. 1 shows SmNiO prepared in example 2 3 The transmission spectrum of the nanocrystal can be clearly seen from FIG. 1, smNiO 3 The nano-crystals are dispersed uniformly, and the particle size is uniform;
s2, preparing 1.25mol/L lead methylamine iodide (MAPbI) in a nitrogen glove box 3 ) Perovskite precursor solution: weighing 1.25mmol of CH in a reagent bottle 3 NH 3 I. 1.25mmol of PbI 2 Adding 700 mu L of dimethylformamide and 300 mu L of dimethyl sulfoxide, stirring the mixed solution at 60 ℃ for 2 hours, and filtering by using an organic filter head to obtain 1mL of 1.25mol/L perovskite precursor solution for experiment;
s3, taking 30 mu L of perovskite precursor solution prepared in S2 to spin coat on an FTO conductive substrate covered with a 70nm TiO2 electronic transmission layer, firstly spin-coating at low speed (1000 rmp) for 10S, then spin-coating at high speed (5000 rmp) for 30S, and immediately dropwise adding 200 mu L of SmNiO prepared in S1 when the residual 10S is spin-coated at high speed 3 The nanocrystalline diethyl ether colloidal solution is thermally treated for 30min at 100 ℃ after the dripping is finished, and the SmNiO is prepared 3 Nanocrystalline compounded MAPbI 3 The perovskite thin film layer is uniform and flat in surface and 550nm in thickness;
s4, spin-coating a hole transport material Spiro-OMeTAD on the perovskite thin film layer prepared in the S3, and oxidizing in the air for 12 hours to obtain a hole transport layer with the thickness of 120 nm;
s5, evaporating and plating a layer with the area of 0.1cm on the hole transport layer of the S4 2 And an Au electrode with the thickness of 100nm to obtain SmNiO 3 Nanocrystalline compounded MAPbI 3 Perovskite solar cell.
This example provides a cell with a photoelectric conversion efficiency of 21.3%.
Example 3
A nanocrystal composite perovskite solar cell comprises a conductive substrate, an electron transmission layer, a light absorption layer, a hole transmission layer and a metal electrode layer which are sequentially stacked from bottom to top;
the light absorption layer includes a perovskite thin film, and semiconductor oxide nanoparticles contained in the perovskite thin film. The semiconductor oxide particles are CuCrO 3 ；
The specific preparation method of the nano-crystal composite perovskite solar cell comprises the following steps:
s1, under the assistance of ultrasound, irradiating 3mL of CuCrO with the concentration of 0.03mg/mL by using pulse laser with the wavelength of 355nm and the energy of 100mJ 3 Ethyl acetate suspension solvent for 10min to prepare CuCrO with size of about 3nm and concentration of 0.03mg/m L 3 A nanocrystalline ethyl acetate colloidal solution;
s2, preparing 1.2mol/L lead methylamine iodide (MAPbI) in a nitrogen glove box 3 ) Perovskite precursor solution: weighing 1.2mmol of CH in a reagent bottle 3 NH 3 I. 1.2mmol of PbI 2 Adding 700 mu L of dimethylformamide and 300 mu L of dimethyl sulfoxide, stirring the mixed solution at 60 ℃ for 2h, and filtering by using an organic filter head to obtain 1mL of 1.2mol/L perovskite precursor solution for experiments;
s3, taking 30 mu L of perovskite precursor solution prepared in S2, spin-coating the perovskite precursor solution on an FTO conductive substrate covered with a 70nm TiO2 electronic transmission layer, spin-coating at a low speed (1000 rmp) for 10S, then spin-coating at a high speed (5000 rmp) for 30S, and immediately dropwise adding 200 mu L of CuCrO prepared in S1 when the residual 10S is left in the high-speed spin-coating 3 The nanocrystalline ethyl acetate colloidal solution is thermally treated for 60min at 100 ℃ after the dripping is finished, and the CuCrO is prepared 3 Nanocrystalline compounded MAPbI 3 The perovskite thin film layer is uniform and flat in surface and 550nm in thickness;
s4, spin-coating a hole transport material Spiro-OMeTAD on the perovskite thin film layer prepared in the S3, and oxidizing in the air for 12 hours to obtain a hole transport layer with the thickness of 120 nm;
s5, evaporating and plating a layer with the area of 0.1cm on the hole transport layer of the S4 2 And an Au electrode with the thickness of 100nm to obtain the CuCrO 3 Nanocrystalline compounded MAPbI 3 Perovskite solar cell.
This example provides a cell having a photoelectric conversion efficiency of 20.7%.
In order to illustrate the nanocrystal composite perovskite solar cell and the preparation method provided by the invention, the performance parameters of the nanocrystal composite perovskite solar cell prepared in the embodiments 1 to 3 are shown in tables 1 to 3; and the current-voltage curves of the nanocrystal-composited perovskite solar cells provided in examples 1 to 3, the relevant properties of the un-composited original perovskite solar cells were taken as the original control groups, see fig. 2 to 4.
Table 1: performance parameters of the batteries prepared in example 1
Table 2: performance parameters of the batteries prepared in example 2
Table 3: performance parameters of the batteries prepared in example 3
As can be seen from tables 1 to 3 and fig. 2 to 4, the open-circuit voltage, the short-circuit current and the fill factor of the nanocrystal composite perovskite solar cell are significantly improved compared with those of the original perovskite solar cell, because the nanocrystals with high hole rate in the nanocrystal composite perovskite thin film promote the extraction of holes in the perovskite thin film and facilitate the transmission of the holes generated in the perovskite thin film to the hole transport layer, the photoelectric conversion efficiency of the nanocrystal composite perovskite solar cell is improved from 18% to more than 21% of that of the original perovskite solar cell.
It will be apparent to those skilled in the art that various changes and modifications may be made in the present invention without departing from the spirit and scope of the invention. Thus, if such modifications and variations of the present invention fall within the scope of the claims of the present invention and their equivalents, the present invention is also intended to include such modifications and variations.
Claims (8)
1. A nanocrystal composite perovskite solar cell is characterized by comprising a conductive substrate, an electron transmission layer, a light absorption layer, a hole transmission layer and a metal electrode layer which are sequentially stacked from bottom to top;
the light absorption layer comprises a perovskite thin film, and semiconductor oxide nano-particles contained in the perovskite thin film;
the semiconductor oxide nanoparticles are NiO and SmNiO 3 、CuCrO 3 、GaCrO 3 One of (a) and (b);
the light absorption layer is prepared by the following steps:
firstly, uniformly dispersing semiconductor oxide nano particles in an organic liquid medium, and irradiating by pulse laser beams to prepare a nano-crystalline colloidal solution;
secondly, spin-coating a perovskite precursor solution on the electron transport layer, adding the nanocrystalline colloid solution in the spin-coating process, and then carrying out heat treatment at 100-150 ℃ for 10-90 min to obtain the light absorption layer;
wherein the usage ratio of the perovskite precursor to the semiconductor oxide nanoparticles is 1moL: 0.037-4.76 g.
2. The nanocrystalline composite perovskite solar cell of claim 1, wherein the nanocrystalline colloidal solution has a concentration of 0.01-0.5 mg/mL.
3. The nanocrystalline composite perovskite solar cell according to claim 1, wherein the concentration of the perovskite precursor solution is 1.05 to 1.35mol/L.
4. The nanocrystalline composite perovskite solar cell of claim 1, wherein the organic liquid medium is one or more of ethyl formate, ethyl acetate, diethyl ether.
5. The nanocrystalline composite perovskite solar cell of claim 1, wherein the perovskite precursors are AX and BX 2 A compound of type (I);
wherein A is CH 3 NH 3 + 、HC(＝NH)NH 2 + 、Cs + One or more of (a), (b);
b is Pb 2+ ；
And X is one or more of halogen ions.
6. The nanocrystalline composite perovskite solar cell according to claim 1, wherein the pulsed laser has one of a wavelength of 1064nm, a wavelength of 532nm and a wavelength of 355nm, an energy of 50-1000 mJ/pulse, and an irradiation time of 2-30 min.
7. The nanocrystalline composite perovskite solar cell according to claim 1, wherein spin coating a perovskite precursor solution on the electron transport layer adopts two-step spin coating at a low speed of 1000rpm/10s and a high speed of 4000rpm/30s, and the nanocrystalline colloid solution is added dropwise when the high speed spin coating is left for 5-15 s.
8. A method of manufacturing a nanocrystalline composite perovskite solar cell according to claim 1, comprising the steps of:
spin-coating a perovskite precursor solution on a conductive substrate covered with an electron transport layer, adding a certain amount of nanocrystalline colloid solution while spin-coating, and forming a nanocrystalline composite perovskite thin film after heat treatment; and then spin-coating a hole transport layer and evaporating a metal electrode on the nano-crystal composite perovskite thin film in sequence to obtain the nano-crystal composite perovskite solar cell.
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| CN113782684B (en) * | 2021-09-10 | 2022-10-21 | 华能新能源股份有限公司 | Perovskite thin film and preparation method thereof |
| CN113889574B (en) * | 2021-12-03 | 2022-03-22 | 中国华能集团清洁能源技术研究院有限公司 | Preparation method and application of perovskite material layer in concentrating perovskite solar cell |
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| CN107994122A (en) * | 2017-11-27 | 2018-05-04 | 济南大学 | Zinc doping nickel oxide nanoparticle hole transmission layer is just putting perovskite solar cell and preparation method |
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