CN113193123B - Double-interface-layer-modified efficient perovskite solar cell and preparation method thereof - Google Patents

Double-interface-layer-modified efficient perovskite solar cell and preparation method thereof Download PDF

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CN113193123B
CN113193123B CN202110380752.5A CN202110380752A CN113193123B CN 113193123 B CN113193123 B CN 113193123B CN 202110380752 A CN202110380752 A CN 202110380752A CN 113193123 B CN113193123 B CN 113193123B
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刘明侦
曾成松
曾鹏
赵海峰
李发明
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University of Electronic Science and Technology of China
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Abstract

The invention provides a double-interface layer modified high-efficiency perovskite solar cell which comprises transparent conductive glass, an electron transmission layer, a perovskite absorption layer, a PMAI layer and CsPbBr which are sequentially arranged 3 Quantum dots, a hole transport layer and a metal electrode; wherein the PMAI layer and CsPbBr 3 The preparation method of the quantum dot comprises the following steps: spin-coating a PMAI solution with isopropanol serving as a solvent and 1-15 mg/mL of concentration on the perovskite absorption layer to obtain a PMAI layer; then the solvent is chlorobenzene and CsPbBr with the concentration of 2-10 mg/mL 3 The quantum dot solution is coated on the PMAI layer in a spin mode to obtain CsPbBr 3 And (4) quantum dots. The invention adopts a PMAI layer and CsPbBr 3 The quantum dots are used as double interface layers to modify a perovskite absorption layer, a PMAI layer and CsPbBr 3 The synergistic effect of the quantum dots improves the charge transmission performance of the interface, and the perovskite solar cell with high efficiency is realized.

Description

Double-interface-layer-modified efficient perovskite solar cell and preparation method thereof
Technical Field
The invention belongs to the technical field of solar cells, and particularly relates to a double-interface-layer-modified efficient perovskite solar cell and a preparation method thereof.
Background
The new energy is the power foundation of scientific development and is an important strategy for solving the problem of energy shortage and environmental pollution. Solar energy is used as renewable clean energy, has the advantages of environmental protection and abundant reserves, and is paid much attention to in a plurality of new energy sources. The solar cell technology is a key technology for directly converting solar energy into electric energy, and is roughly divided into three types, namely a first-generation silicon-based solar cell, a second-generation thin-film solar cell, and a third-generation novel solar cell which is currently and intensively researched, wherein the third-generation novel solar cell is a quantum dot solar cell, an organic solar cell, a Perovskite Solar Cell (PSCs) and the like.
Due to the advantages of excellent photoelectric property, simple preparation process, low preparation cost and the like of the perovskite solar cell, the Photoelectric Conversion Efficiency (PCE) is increased from 3.8% to 25.5% in the short decade, and the perovskite solar cell can almost be comparable to a commercial silicon-based solar cell. The theoretical limit efficiency of Shockley-Queisser (Shockley-Quetiser) of the perovskite solar cell is 33%, and compared with other types of photovoltaic devices, the PCE still has a great promotion space. However, due to the ionic characteristics and preparation processes of perovskite materials, various types of defects exist on the perovskite surface, mainly including iodine ion vacancies, lead ion gaps, pb-I inversion defects, and unbound lead atom defects. These defects can lead to extensive non-radiative recombination, inhibit separation and extraction of interfacial charges, and reduce the efficiency and stability of the device.
Interfacial passivation has proven to be the most effective method to address the above defect problems, and therefore various functional interfacial materials are used for defect passivation of the perovskite surface to improve the efficiency and stability of the perovskite solar cell. At present, most researches are based on an interface layer, or interface layers are respectively deposited on two sides of a perovskite layer, so that the photovoltaic performance of the device is improved. However, the functionality of an interfacial layer is limited and it is difficult to achieve a large increase in efficiency.
Disclosure of Invention
Aiming at the problem of single function of an interface layer in the prior art, the invention provides a double-interface-layer-modified efficient perovskite solar cell and a preparation method thereof, and the efficiency and the stability of the perovskite solar cell are effectively improved by utilizing the synergistic effect of the double interface layers.
In order to achieve the above purpose, the invention provides the following technical scheme:
the high-efficiency perovskite solar cell modified by the double interface layers comprises transparent conductive glass, an electron transmission layer, a perovskite absorption layer, a hole transmission layer and metal electrodes which are sequentially arranged from bottom to top, and is characterized in that a benzyl ammonium iodide (PMAI) layer and CsPbBr are sequentially arranged between the perovskite absorption layer and the hole transmission layer 3 And (4) quantum dots.
Further, the thickness of the PMAI layer does not exceed 10nm.
A preparation method of a double-interface layer modified high-efficiency perovskite solar cell is characterized by comprising the following steps:
step 1: depositing an electron transport layer on the transparent conductive glass;
step 2: preparing a perovskite absorption layer on the electron transport layer;
and step 3: dissolving benzyl ammonium iodide (PMAI) in isopropanol to obtain a PMAI solution with the concentration of 1-15 mg/mL, and spin-coating the PMAI solution on the perovskite absorption layer obtained in the step 2 to obtain a PMAI layer;
and 4, step 4: reacting CsPbBr 3 Quantum dots are dissolved in chlorobenzene to obtain CsPbBr with the concentration of 2-10 mg/mL 3 Spin-coating quantum dot solution on the PMAI layer obtained in step 3 to obtain CsPbBr 3 Quantum dots;
and 5: csPbBr obtained in step 4 3 And sequentially preparing a hole transport layer and a metal electrode on the quantum dots.
Further, the material of the electron transport layer in step 1 is tin dioxide or titanium dioxide.
Further, in step 2, the perovskite absorption layer is FA 1-x MA x PbI 3 Perovskite absorption layer, (FAPbI) 3 ) 1-x (MAPbBr 3 ) x Perovskite absorption layer or Cs 0.2 FA 0.8 PbI 3 A perovskite absorption layer.
Further, step 2 preparation of FA 1-x MA x PbI 3 The perovskite absorption layer comprises the following specific steps:
step 2.1: lead iodide (PbI) 2 ) Dissolving in a mixed solvent of DMF (N, N-dimethylformamide) and DMSO (dimethyl sulfoxide) in a volume ratio of 9 2 PbI with a concentration of 1.3 to 1.5M 2 Solution of PbI 2 Spin coating the solution on the electron transport layer obtained in the step 1 to obtain PbI 2 A film;
step 2.2: mixing formamidine iodine (FAI), methylamine iodine (MAI) and methylamine chloride (MACl) according to a mass ratio of 30:2:3 in the ratio of isopropyl alcohol to obtain a mixed solution with the FAI concentration of 90mg/mL, and spin-coating the mixed solution on the PbI obtained in the step 2.1 2 On a film, obtainObtaining a mixed film;
step 2.3: annealing the mixed film obtained in the step 2.2 at 150 ℃ for 15min to prepare FA 1-x MA x PbI 3 A perovskite absorption layer.
Further, the spin coating conditions in step 3 are: spin coating at 4000-6000 rpm for 30s.
Further, the spin coating conditions in step 4 are: spin coating for 30s at a rotation speed of 4000-6000 rpm.
Furthermore, the material of the metal electrode in step 5 is a metal material such as Au, ag, or Cu.
The beneficial effects of the invention are as follows:
1. the invention adopts benzyl ammonium iodide (PMAI) layer and CsPbBr 3 Quantum dots are used as double interface layers to modify a perovskite absorption layer; wherein, the PMAI layer can effectively passivate the surface defects of the perovskite absorption layer, reduce the non-radiative recombination of the interface and is beneficial to the transfer of interface charges, and CsPbBr 3 The quantum dots can further promote the extraction and transmission of carriers, the PMAI layer and the CsPbBr 3 The synergistic effect of the quantum dots improves the charge transmission performance of the interface, realizes the perovskite solar cell with high efficiency, has the efficiency of 22.06 percent and is beneficial to accelerating the commercialization pace of the perovskite solar cell;
2. the invention prepares the PMAI layer and the CsPbBr layer on the surface of the perovskite in sequence by a surface spin coating mode 3 The quantum dots are simple and controllable to operate, and have the advantage of low energy consumption.
Drawings
FIG. 1 is a schematic structural diagram of a double-interface layer modified high-efficiency perovskite solar cell obtained in example 1 of the present invention;
FIG. 2 shows the preparation of FA in example 1 of the present invention 1-x MA x PbI 3 Perovskite absorption layer, PMAI layer and CsPbBr 3 A flow diagram of quantum dots;
FIG. 3 is a time resolved photoluminescence spectrum TRPL profile of perovskite absorbing layers in example 1, comparative example 1 and comparative example 2 of the present invention;
FIG. 4 is an EIS diagram of electrochemical impedance spectra of perovskite solar cells in example 1, comparative example 1 and comparative example 2 of the present invention
FIG. 5 is a statistical plot of photovoltaic parameters of perovskite solar cells obtained in example 1, comparative example 1 and comparative example 2 of the present invention;
fig. 6 is a positive and negative current density-voltage curve diagram of the double-interface layer modified high-efficiency perovskite solar cell obtained in example 1 of the invention.
Detailed Description
The principles and features of the present invention are explained in detail below with reference to the embodiments and the accompanying drawings of the specification:
example 1
In this embodiment, a double-interface layer modified high-efficiency perovskite solar cell (PMAI + QDs) is prepared, and a schematic structural diagram of the device is shown in fig. 1, which sequentially comprises from bottom to top: ITO conductive glass (ITO), snO 2 Electron transport layer (SnO) 2 )、 FA 1- x MA x PbI 3 Perovskite light absorbing layer (Perovskite), PMAI layer (PMAI), csPbBr 3 Quantum dots (CsPbBr) 3 QDs), hole transport layer (Spiro-OMeTAD), metal electrode (Au); the preparation method specifically comprises the following steps:
step 1: cleaning a substrate:
in this embodiment, ITO conductive glass is used as the substrate, i.e., indium-doped tin dioxide (SnO) 2 :In)；
Firstly, primarily cleaning ITO conductive glass by using a detergent and nano sponge, then washing the ITO conductive glass for a plurality of times by using deionized water, sequentially carrying out ultrasonic treatment on a washed substrate by using acetone, absolute ethyl alcohol and deionized water as solvents, blow-drying the ITO conductive glass after ultrasonic treatment by using nitrogen, and then treating the ITO conductive glass for 12min by using oxygen plasma so as to further remove organic matters on the surface of the substrate and simultaneously enhance the bonding force and adhesive force on the surface of the substrate material;
and 2, step: preparing an electron transport layer:
tin dioxide SnO is selected for use in this example 2 The film is used as an electron transport layer;
SnO purchased from a company with a volume fraction of 15% 2 The volume ratio of the aqueous solution to the deionized water is 1Mixing in proportion to obtain SnO 2 Solution, then SnO 2 The solution is placed on a stirring table to be stirred for 30min at normal temperature; mixing the stirred SnO 2 And (2) spin-coating the solution on the substrate obtained in the step (1) by a spin-coating method with uniform glue, wherein the spin-coating procedure comprises the following steps: the spin-coating speed is 4000rpm, the acceleration is 4000rpm, and the spin-coating time is 30s; then sintering for 30min at the temperature of 150 ℃ to obtain SnO 2 An electron transport layer;
and 3, step 3: preparation of FA 1-x MA x PbI 3 Perovskite absorption layer:
step 3.1: preparation of PbI 2 Solution: 691.5mg of PbI were weighed on an electronic balance 2 Powder, dissolved in 1mL of a mixed solvent of DMF and DMSO at a volume ratio of 9 2 A solution;
step 3.2: preparation of a mixed solution a of FAI, MAI, and MACl: weighing 90mg of FAI, 6mg of MAI and 9mg of MACl by using an electronic balance, dissolving the FAI, the MAI and the MACl in 1mL of isopropanol, and stirring the mixture for 30min at normal temperature to obtain a mixed solution A of the FAI, the MAI and the MACl;
step 3.3: will PbI 2 Filtering the solution and the mixed solution of FAI, MAI and MACl in a glove box in a nitrogen atmosphere by using a filter head with the diameter of 0.22 μm;
step 3.4: taking 40 mu L of PbI obtained in step 3.1 in a glove box in nitrogen atmosphere by using a spin coater 2 Solution spin coating on the SnO obtained in step 2 2 On the electron transport layer to obtain PbI 2 A film; the spin coating program was set up as follows: the rotating speed is 1500rpm, the acceleration is 1500rpm, and the spin coating time is 30s;
step 3.5: 80 μ L of the mixed solution A of FAI, MAI and MACl obtained in step 3.2 was spin-coated on the PbI obtained in step 3.4 using a spin coater in a glove box under nitrogen atmosphere 2 Obtaining a mixed film on the film; the spin coating program was set up as follows: the rotating speed is 2000rpm, the acceleration is 2000rpm, and the spin coating time is 30s;
step 3.6: annealing the mixed film obtained in the step 3.5, setting the annealing temperature at 150 ℃ and the annealing time at 15min to obtain FA 1-x MA x PbI 3 A perovskite absorption layer;
and 4, step 4: preparing a PMAI layer:
firstly, weighing 9mg of PMAI powder by using an electronic balance, dissolving the PMAI powder in 1mL of isopropanol, and stirring for 30min at normal temperature to obtain a PMAI solution; then spin-coating PMAI solution on FA obtained in step 3.6 1-x MA x PbI 3 Obtaining a PMAI layer on the perovskite absorption layer; the spin coating program was set up as: the rotating speed is 5000rpm, the acceleration is 5000rpm, and the spin coating time is 30s;
and 5: preparation of CsPbBr 3 Quantum dot:
60 mu L of CsPbBr with the solvent of chlorobenzene and the concentration of 5mg/mL 3 Spin coating the quantum dot solution on the PMAI layer obtained in the step 4 to obtain CsPbBr 3 Quantum dots; the spin coating program was set up as follows: the rotating speed is 5000rpm, the acceleration is 5000rpm, and the spin coating time is 30s;
step 6: preparing a hole transport layer:
the invention does not limit the selection of the hole transport layer material, and can be any suitable hole transport layer material; in this example, a composite film formed by 2,2', 7' -tetrakis [ N, N-bis (4-methoxyphenyl) amino ] -9,9' -spirobifluorene, lithium bistrifluoromethanesulfonylimide, and 4-t-butylpyridine was used as a hole transport layer;
73.4mg of 2,2', 7' -tetrakis [ N, N-di (4-methoxyphenyl) amino are weighed out]9,9' -spirobifluorene, 17.5 mu L of bis (trifluoromethanesulfonimide) lithium acetonitrile solution with the concentration of 520mg/mL of bis (trifluoromethanesulfonimide) lithium, and 28 mu L of 4-tert-butylpyridine, and dissolving the three in 1mL of chlorobenzene to prepare a mixed solution B; spin-coating 40 μ L of the mixed solution B on the CsPbBr obtained in step 5 3 Forming a hole transport layer on the quantum dots;
and 7: preparing a metal electrode:
in this embodiment, a metal Au with a thickness of 100nm is vapor-deposited on the hole transport layer obtained in step 6 by using a vapor deposition method to serve as a metal electrode, and finally the double-interface layer modified high-efficiency perovskite solar cell is prepared.
FA preparation for this example as shown in FIG. 2 1-x MA x PbI 3 Perovskite absorption layer, PMAI layer and CsPbBr 3 A flow chart for preparing Quantum Dots (QDs).
Example 2
This example a high efficiency perovskite solar cell modified with a double interface layer was prepared according to the procedure of example 1, differing from example 1 only in that 9mg of PMAI powder was dissolved in 1mL of isopropanol during the preparation of the PMAI layer in step 4, adjusted to 1mg of PMAI powder in 1mL of isopropanol; the other steps are unchanged.
Example 3
This example a high efficiency perovskite solar cell modified with a double interface layer was prepared according to the procedure of example 1, differing from example 1 only in that 9mg of PMAI powder was dissolved in 1mL of isopropanol and adjusted to 15mg of PMAI powder was dissolved in 1mL of isopropanol during the preparation of the PMAI layer in step 4; the other steps are unchanged.
Example 4
This example prepares a double interface layer modified high efficiency perovskite solar cell according to the procedure of example 1, and compared with example 1, the difference is only that: the rotation speed in the process of preparing the PMAI layer in the step 4 is 5000rpm, the rotation speed is adjusted to 4000rpm, and CsPbBr is prepared in the step 5 3 The rotation speed in the process of quantum dots is 5000rpm, and the rotation speed is adjusted to 4000rpm; the other steps are unchanged.
Example 5
This example prepares a double interface layer modified high efficiency perovskite solar cell according to the procedure of example 1, and compared with example 1, the difference is only that: the rotation speed in the process of preparing the PMAI layer in the step 4 is 5000rpm, the rotation speed is adjusted to 6000rpm, and the CsPbBr prepared in the step 5 3 The rotation speed in the process of quantum dots is 5000rpm, and is adjusted to be 6000rpm; the other steps are unchanged.
Example 6
This example prepares a double interfacial layer modified high efficiency perovskite solar cell according to the procedure of example 1, which differs from example 1 only in that CsPbBr is prepared at step 5 3 In the process of quantum dots, the concentration is5mg/mL CsPbBr 3 The quantum dot solution is adjusted to CsPbBr with the concentration of 2mg/mL 3 A quantum dot solution; the other steps are unchanged.
Example 7
This example a double-interface layer modified high-efficiency perovskite solar cell was prepared according to the procedure of example 1, and compared with example 1, the difference is only that CsPbBr was prepared at step 5 3 In the process of quantum dots, csPbBr with the concentration of 5mg/mL is added 3 The quantum dot solution is adjusted to CsPbBr with the concentration of 10mg/mL 3 A quantum dot solution; the other steps are unchanged.
Comparative example 1
This comparative example a perovskite solar cell (Control) was prepared according to the procedure of example 1, differing from example 1 only in that: no PMAI layer and CsPbBr were prepared 3 Quantum dots, i.e. the perovskite solar cell comprises ITO conduction band glass and SnO which are arranged from bottom to top in sequence 2 The electron transport layer, the Perovskite light absorption layer Perovskite, the hole transport layer Spiro-OMeTAD and the metal electrode Au; the other steps are unchanged.
Comparative example 2
This comparative example a perovskite solar cell (PMAI) was prepared according to the procedure of example 1, differing from example 1 only in that: csPbBr was not prepared 3 Quantum dot, i.e. the perovskite solar cell comprises ITO conduction band glass and SnO which are arranged from bottom to top in sequence 2 The electron transport layer, the Perovskite light absorption layer Perovskite, the PMAI layer, the hole transport layer Spiro-OMeTAD and the metal electrode Au; the other steps are unchanged.
The above examples and comparative examples were analytically tested as follows:
for example 1 (PMAI + QDs) with a PMAI layer and CsPbBr 3 Quantum dot modified FA 1-x MA x PbI 3 Perovskite absorber layer, unmodified FA in comparative example 1 (Control) 1-x MA x PbI 3 Perovskite absorber layer, FA modified with PMAI layer in comparative example 2 (PMAI) 1-x MA x PbI 3 Time-resolved photoluminescence spectroscopy TRPL analysis of the perovskite absorption layer is shown in FIG. 3, and without interface modificationCompared with the perovskite absorption layer, the surface of the perovskite absorption layer is modified by the PMAI layer, has longer carrier life, and is further added with CsPbBr 3 After quantum dots, the carrier lifetime is shortened. The change result of the TRPL carrier lifetime shows that the PMAI layer can effectively reduce the non-radiative recombination of the interface carrier, csPbBr 3 The quantum dots facilitate the transport of carriers.
The electrochemical impedance spectroscopy EIS analysis of the double-interface-layer-modified high-efficiency perovskite solar cell obtained in example 1 (PMAI + QDs), the perovskite solar cell obtained in comparative example 1 (Control) and the perovskite solar cell obtained in comparative example 2 (PMAI) is carried out, and the results are shown in FIG. 4, compared with the perovskite solar cell of comparative example 1, the charge transfer resistance of the PMAI-interface-modified perovskite solar cell of comparative example 2 is obviously reduced, and CsPbBr is added 3 After quantum dots are formed, the charge transmission resistance of the perovskite solar cell modified by the PMAI + QDs double interface layer is further reduced, and the charge transmission performance of the interface is remarkably improved.
The high-efficiency perovskite solar cell modified by the double interface layer obtained in the example 1 (PMAI + QDs), the perovskite solar cell obtained in the comparative example 1 (Control) and the perovskite solar cell obtained in the comparative example 2 (PMAI) are placed in a nitrogen glove box for photoelectric test, the effective active area is 0.09 square centimeter, the test condition is standard simulated sunlight AM 1.5, and the temperature is 25 ℃. Photovoltaic parameter statistical plots as shown in fig. 5, open circuit voltage V for the PMAI interface modified perovskite solar cell of comparative example 2 compared to the perovskite solar cell of comparative example 1 OC Remarkably improves the quality and is further added with CsPbBr 3 After quantum dots, open-circuit voltage V of perovskite solar cell modified by PMAI + QDs double interface layer OC Further promoted and higher efficiency PCE is obtained. The current density-voltage curve diagram is shown in fig. 6, the photoelectric conversion efficiency PCE is as high as 22.06%, which indicates that the efficiency PCE of the device is significantly improved under the synergistic effect of the double interface layers of the perovskite solar cell.

Claims (8)

1. A double-interface layer modified high-efficiency perovskite solar cell comprises transparent conductive glass, an electron transmission layer and a perovskite absorber which are sequentially arranged from bottom to topThe perovskite-type solar cell comprises a perovskite absorption layer, a hole transport layer and a metal electrode, and is characterized in that a PMAI layer and CsPbBr are sequentially arranged between the perovskite absorption layer and the hole transport layer 3 The PMAI layer is obtained by dissolving PMAI in isopropanol to obtain a PMAI solution with the concentration of 1-15 mg/mL, and then spin-coating the PMAI solution on the perovskite absorption layer.
2. The double interfacial layer modified high efficiency perovskite solar cell according to claim 1, wherein the thickness of the PMAI layer is no more than 10nm.
3. A preparation method of a double-interface layer modified high-efficiency perovskite solar cell is characterized by comprising the following steps:
step 1: depositing an electron transport layer on the transparent conductive glass;
step 2: preparing a perovskite absorption layer on the electron transport layer;
and 3, step 3: dissolving PMAI in isopropanol to obtain a PMAI solution with the concentration of 1-15 mg/mL, and spin-coating the PMAI solution on the perovskite absorption layer to obtain a PMAI layer;
and 4, step 4: mixing CsPbBr 3 Quantum dots are dissolved in chlorobenzene to obtain CsPbBr with the concentration of 2-10 mg/mL 3 Quantum dot solution is coated on the PMAI layer in a spin way to obtain CsPbBr 3 Quantum dots;
and 5: in CsPbBr 3 And sequentially preparing a hole transport layer and a metal electrode on the quantum dots.
4. The preparation method of the double interfacial layer modified high-efficiency perovskite solar cell as claimed in claim 3, wherein the spin coating condition in the step 3 is spin coating for 30s at a rotation speed of 4000-6000 rpm.
5. The preparation method of the double interfacial layer modified high-efficiency perovskite solar cell as claimed in claim 3, wherein the spin coating condition in the step 4 is spin coating for 30s at a rotation speed of 4000-6000 rpm.
6. The method for preparing a high-efficiency perovskite solar cell modified by a double interface layer according to claim 3, wherein the material of the electron transport layer in the step 1 is tin dioxide or titanium dioxide.
7. The method for preparing a high-efficiency perovskite solar cell modified by double interfacial layers according to claim 3, wherein the perovskite absorption layer in the step 2 is FA 1-x MA x PbI 3 Perovskite absorption layer, (FAPbI) 3 ) 1-x (MAPbBr 3 ) x Perovskite absorption layers or Cs 0.2 FA 0.8 PbI 3 A perovskite absorption layer.
8. The method for preparing a high-efficiency perovskite solar cell modified by a double interface layer according to claim 3, wherein the metal electrode in the step 5 is made of Au, ag or Cu.
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