CN113270548B - Perovskite solar cell with trans-planar structure and preparation method - Google Patents

Perovskite solar cell with trans-planar structure and preparation method Download PDF

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CN113270548B
CN113270548B CN202110372537.0A CN202110372537A CN113270548B CN 113270548 B CN113270548 B CN 113270548B CN 202110372537 A CN202110372537 A CN 202110372537A CN 113270548 B CN113270548 B CN 113270548B
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于华
侯鸿铭
胡滔滔
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Southwest Petroleum University
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Abstract

The invention discloses a trans-planar perovskite solar cell and a preparation method thereof, wherein the trans-planar perovskite solar cell comprises a conductive substrate, a hole transport layer, an ultrathin modification layer, a perovskite light absorption layer, an electron transport layer, an interface modification layer and a metal cathode which are sequentially stacked from bottom to top; the hole transport layer is prepared by doping tributyl phosphate with nickel oxide, and the ultrathin modification layer is LiF with the thickness of 1-5 nm; the invention improves the transmittance of nickel oxide, improves the conductivity, inhibits the interface recombination between a hole transmission layer and a perovskite light absorption layer, improves the transmission efficiency of carriers between interfaces, improves the crystallization quality of perovskite thin films, reduces the defects of perovskite light active layers and improves the performance of perovskite solar cell devices.

Description

Perovskite solar cell with trans-planar structure and preparation method
Technical Field
The invention relates to the technical field of perovskite solar cells, in particular to a trans-form planar structure perovskite solar cell and a preparation method thereof.
Background
In the 21 st century, the demand of economic society for energy is increasing, and the traditional energy cannot adapt to the demand of social development due to the self limitation. Solar energy is used as a renewable energy source, has the advantages of inexhaustibility, economy, environmental protection and the like, develops a solar energy, particularly a cheap solar cell technology, promotes the solar cell to generate electricity at a low price, and is an important trend for the development of a new energy technology.
In recent years, perovskite solar cells are particularly concerned in academia and industry as a new generation of replaceable cheap solar cells due to low material cost, simple preparation process and rapid increase of cell efficiency to the level close to that of the traditional crystalline silicon solar cells. Metal halide Perovskite Solar Cells (PSCs) are based on p-i-n junctions, with a perovskite absorber layer sandwiched between n-type and p-type semiconductors as the selective layer. The efficiency of Power Conversion (PCE) is improved to more than 25% due to adjustable optical band gap, high absorption coefficient and long photocarrier life.
NiOx is considered to be the most promising inorganic p-type hole-selective layer due to its conversion efficiency (PCE) of 22.1% and its excellent stability in a NiOx-based organic-inorganic hybrid perovskite solar cell. However, the existing NiOx-based organic-inorganic hybrid perovskite solar cell has two main problems, namely, the existence of nickel oxide surface defects and poor permeability, so that the conductivity of the nickel oxide solar cell is poor; second, the open circuit voltage (Voc) of the NiOx-based device is relatively low due to the high surface roughness of nickel oxide and the presence of a large number of pinholes, which causes the perovskite thin film to be insufficiently coated on the surface thereof, resulting in interfacial recombination with the release of the electron transport layer.
Disclosure of Invention
Aiming at the problems in the prior art, the invention provides the trans-planar perovskite solar cell and the preparation method thereof, wherein the trans-planar perovskite solar cell improves the transmittance of nickel oxide, improves the conductivity, inhibits the interface recombination between a hole transport layer and a perovskite light absorption layer, improves the transmission efficiency of carriers between interfaces, improves the crystallization quality of a perovskite thin film, reduces the defects of a perovskite light active layer and improves the performance of a perovskite solar cell device.
The technical scheme adopted by the invention is as follows:
a trans-planar perovskite solar cell comprises a conductive substrate, a hole transport layer, an ultrathin modification layer, a perovskite light absorption layer, an electron transport layer, an interface modification layer and a metal cathode which are sequentially stacked from bottom to top; the hole transport layer is prepared by doping tributyl phosphate with nickel oxide, and the ultrathin modification layer is LiF with the thickness of 1-5 nm.
Further, the perovskite light absorption layer is APbI3 -A is CH3NH3 +、CH(NH2)2 +、Cs+Mixtures of any proportion.
Further, the conductive substrate is one of FTO glass, ITO glass, ICO glass, IWO glass, IZO glass and AZO glass; the electron transport layer is a fullerene derivative film; the interface modification layer is one of bathocuproine, lithium fluoride and titanium oxide; the metal cathode is one of silver, copper or gold.
Furthermore, the thickness of the conductive substrate is 500-600 nm, the thickness of the hole transmission layer is 20-50 nm, the thickness of the perovskite light absorption layer is 400-500 nm, the thickness of the electron transmission layer is 15-35 nm, the thickness of the interface modification layer is 2-5 nm, and the thickness of the metal cathode is 70-120 nm.
A preparation method of a trans-planar perovskite solar cell comprises the following steps:
step 1: depositing a nickel oxide precursor solution doped with tributyl phosphate on a conductive substrate by a spin coating method, and annealing to obtain a hole transport layer;
step 2: spin-coating and depositing a LiF aqueous solution on the hole transport layer, and carrying out annealing treatment to obtain an ultrathin modification layer;
and step 3: spin-coating and depositing a perovskite precursor solution on the ultrathin modification layer, and carrying out annealing treatment to obtain a perovskite light absorption layer;
and 4, step 4: spin-coating and depositing a fullerene derivative solution on the perovskite light absorption layer, and carrying out annealing treatment to obtain an electron transmission layer;
and 5: depositing a precursor solution of the interface modification layer on the electron transport layer through spin coating, and carrying out annealing treatment to obtain the interface modification layer;
step 6: and plating a cathode metal plating layer on the interface modification layer to obtain the required trans-planar perovskite solar cell.
Further, the preparation process of the nickel oxide precursor solution doped with tributyl phosphate in the step 1 is as follows:
dissolving 0.1g of nickel acetate in 4mL of ethanol, and adding 24uL of ethanolamine; then stirring and reacting for 6-10 h under the condition of water bath at 60 ℃; obtaining a nickel oxide precursor solution; then adding tributyl phosphate solution to obtain the required precursor solution; the volume ratio of tributyl phosphate to nickel oxide precursor solution is 1-4: 200.
Further, in the step 1, the annealing temperature is 270-310 ℃, and the annealing time is 40-60 min; in the step 2, the annealing temperature is 70-150 ℃, and the annealing time is 5-15 min; in the step 3, the annealing temperature is 100 ℃, and the annealing time is 40-60 min; the annealing temperature in the step 4 is 70 ℃, the annealing time is 15min, the annealing temperature in the step 5 is 70 ℃, and the annealing time is 10 min.
Further, the perovskite precursor solution in the step 2 is prepared as follows:
mixing 29.12mg CsI and 42.72mg PbI2、553.2mg MABr、319.68mg FAI、918.24mg PbI2And 139.84mg of PbBr2Dissolving in a mixed solution composed of N, N-dimethylformamide and dimethyl sulfoxide; wherein the volume ratio of the N, N-dimethylformamide to the dimethyl sulfoxide is 7: 3; stirring the mixed solution at 60 ℃ for 8h to obtain the required FA1.17MA0.24Cs0.07Pb1.48I3.73Br0.72And (3) precursor solution.
Further, the coating in the step 6 is prepared by vacuum evaporation coating, and the vacuum degree is 6 multiplied by 10-4Pa。
The invention has the beneficial effects that:
(1) according to the invention, small-molecule tributyl phosphate is doped with nickel oxide, so that the prepared hole transport layer has low surface roughness, high conductivity and high transmittance;
(2) according to the invention, a layer of ultrathin modification layer lithium fluoride is deposited on the hole transport layer, so that the interface defect of the hole layer and the perovskite layer is passivated, and the perovskite film with uniform grain size, compact film, smooth surface and mirror surface effect is obtained.
Drawings
Fig. 1 is a schematic structural view of a solar cell according to the present invention.
FIG. 2 is an SEM image and an AFM image of a perovskite light absorption layer thin film obtained in an example of the present invention.
Fig. 3 is a J-V curve of a battery obtained in an example of the present invention.
Detailed Description
The invention is further described with reference to the following figures and specific embodiments.
A trans-planar perovskite solar cell is shown in figure 1 and comprises a conductive substrate 1, a hole transport layer 2, an ultrathin modification layer 3, a perovskite light absorption layer 4, an electron transport layer 5, an interface modification layer 6 and a metal cathode 7 which are sequentially stacked from bottom to top; the hole transport layer 2 is prepared by doping tributyl phosphate with nickel oxide, and the ultrathin modification layer 3 is LiF with the thickness of 1-5 nm.
The perovskite light absorption layer is APbI3 -A is CH3NH3 +、CH(NH2)2 +、Cs+Mixtures of any proportion. The conductive substrate 1 is one of FTO glass, ITO glass, ICO glass, IWO glass, IZO glass and AZO glass; the electron transport layer 5 is a fullerene derivative film, and is one of PC60BM, PC61BM or PC71 BM; the interface modification layer 6 is one of bathocuproine, lithium fluoride and titanium oxide; the metal cathode 7 is one of silver, copper or gold. The thickness of the conductive substrate 1 is 500-600 nm, the thickness of the hole transport layer 2 is 20-50 nm, the thickness of the perovskite light absorption layer 4 is 400-500 nm, the thickness of the electron transport layer 5 is 15-35 nm, the thickness of the interface modification layer 6 is 2-5 nm, and the thickness of the metal cathode 7 is 70-120 nm.
Example 1
Preparing a trans-planar perovskite solar cell according to the following steps:
step 1: placing FTO conductive glass with the size of 2cm multiplied by 2cm into a cleaning frame, sequentially adopting a detergent, deionized water, acetone, isopropyl alcohol and absolute ethyl alcohol for ultrasonic cleaning, and then blowing the FTO conductive glass by using nitrogen.
0.1g of nickel acetate is dissolved in 4mL of ethanol solution, 24uL of ethanolamine is added, and the mixture is stirred in a water bath kettle at the temperature of 60 ℃ for 6-10 hours. And filtering to obtain the nickel oxide precursor solution. And then adding 50ul of tributyl phosphate tBP solution into 4mL of nickel oxide solution to obtain a hole transport layer precursor solution. And spin-coating a hole transport layer precursor solution on the surface of the pretreated FTO glass. The spin coating speed is 4000rpm, the time is 40s, and then the annealing is carried out at 280 ℃ for 60min, so as to obtain the nickel oxide hole transport layer.
Step 2: dissolving 2mg LiF in 1mL deionized water, and stirring for 12-36 h. And spin-coating LiF solution on the hole transport layer to serve as an ultrathin modification layer. The spin coating speed is 4000rpm, the time is 40s, and after the spin coating is finished, the ultrathin modification layer is obtained by annealing for 10min on a hot bench at the temperature of 100 ℃.
And step 3: mixing 29.12mg CsI and 42.72mg PbI2、553.2mg MABr、319.68mg FAI、918.24mg PbI2And 139.84mg of PbBr2Dissolved in 1.6mL of a mixed solution of DMF and DMSO. The volume ratio of the DMF to the DMSO in the mixed solution is 7: 3. Stirring at 60 deg.C for 8h to obtainFA concentration of 1.48mmol/mL1.17MA0.24Cs0.07Pb1.48I3.73Br0.72And (3) precursor solution. Spin coating FA on the ultrathin modification layer obtained in the step 21.17MA0.24Cs0.07Pb1.48I3.73Br0.72And (3) precursor solution. The spin coating speed is 4000rpm, the time is 35s, 200uL chlorobenzene is punched after 25s of spin coating is started, and then annealing is carried out for 60min at 100 ℃, so that FA with high coverage, large grains and mirror surface effect can be obtained1.17MA0.24Cs0.07Pb1.48I3.73Br0.72Perovskite light absorption layer film.
And 4, step 4:20 mg of PCBM was added to 1mL of chlorobenzene solution to give a 20mg/mL solution of PCBM. And preparing the PCBM electron transport layer on the surface of the obtained perovskite light absorption layer film by adopting a one-step spin coating method. The spin coating speed was 4000rpm for 40s, and annealing was carried out on a hot plate at 70 ℃ for 10 min. The purities of PCBM and chlorobenzene are both more than 99%.
And 5: 0.5mg of BCP was added to 1mL of isopropanol solution to give a 5mg/mL BCP solution. And preparing a BCP interface modification layer on the surface of the obtained electron transport layer film by adopting a one-step spin coating method. The spin coating speed was 4000rpm for 40s, and annealing was carried out on a hot plate at 70 ℃ for 10 min.
Step 6: putting the prepared substrate into vacuum evaporation coating equipment with the vacuum degree of 6 multiplied by 10-4Pa, and obtaining the silver electrode through the silver electrode coating with the thickness of 100 nm.
Example 2
Preparing a trans-planar perovskite solar cell according to the following steps:
step 2 is not included in this example, and the other steps are the same as the preparation method of the example.
Example 3
Preparing a trans-planar perovskite solar cell according to the following steps:
the preparation processes of the step 2, the step 3, the step 4, the step 5 and the step 6 are the same as the embodiment.
Step 1: placing FTO conductive glass with the size of 2cm multiplied by 2cm into a cleaning frame, sequentially adopting a detergent, deionized water, acetone, isopropyl alcohol and absolute ethyl alcohol for ultrasonic cleaning, and then blowing the FTO conductive glass by using nitrogen.
0.1g of nickel acetate is dissolved in 4mL of ethanol solution, 24uL of ethanolamine is added, and the mixture is stirred in a water bath kettle at the temperature of 60 ℃ for 6-10 hours. And filtering to obtain the nickel oxide precursor solution. And spin-coating a nickel oxide precursor solution on the surface of the pretreated FTO glass. The spin coating speed is 4000rpm, the time is 40s, and then the annealing is carried out at 280 ℃ for 60min, so as to obtain the nickel oxide hole transport layer.
And observing the surface appearance and the surface roughness of the obtained perovskite light absorption layer film by using a scanning electron microscope SEM and an atomic force microscope AFM. And (4) characterizing the photoelectric characteristics of the prepared perovskite solar cell by using a J-V testing instrument.
FIG. 2 is SEM and AFM images of perovskite light absorbing layer thin films. Wherein a and d are SEM image and AFM image of the unmodified perovskite thin film in example 3 respectively. b. e is the SEM and AFM images of the tBP-modified perovskite thin film obtained in example 2, respectively. c. f is the SEM image and AFM image of the tBP and LiF co-modified perovskite thin film (scale: 3um) obtained in example 1, respectively.
As can be seen from the figure, the pictures shown in c and f, namely the film obtained by the method of the invention, have smooth surface and low roughness; the film is compact and has no pinholes; the crystal grains are large and uniformly distributed. It can be seen from the figure that the obtained film is of high quality.
FIG. 3 shows the results of the J-V test. a is the J-V test result of the battery obtained in example 3, b is the J-V test result of the battery obtained in example 2, and c is the J-V test result of the battery obtained in example 3. A is the front side and B is the back side.
As can be seen from the graph c, the open-circuit voltage Voc of the battery obtained by the method of the present invention is 1.056, and the short-circuit current Jsc is 22.66mA/cm2The fill factor FF is 77.9% and the energy conversion efficiency PCE is 18.54%.
The open-circuit voltage Voc of the battery obtained in example 3 was 1.048, and the short-circuit current Jsc was 22.17mA/cm2The fill factor FF is 74.67% and the energy conversion efficiency PCE is 17.35%. The open-circuit voltage Voc and the short-circuit current Jsc of the battery obtained in example 2 were 1.081 and 22.54mA/cm, respectively2The fill factor FF is 74.71% and the energy conversion efficiency PCE is 18.09%. The test results show that the battery obtained by the method has more excellent performance.
According to the invention, the micromolecule tBP is doped with nickel oxide, and the obtained hole transport layer has low surface roughness, so that the interface contact between the perovskite layer and the nickel oxide layer is improved, and the non-radiative recombination between the interfaces is reduced. In addition, the conductivity and the transmittance are obviously improved, and the extraction capability of the nickel oxide hole transport layer to charge carriers is enhanced. Finally, the photoelectric conversion efficiency of the perovskite solar cell is improved from 17.35% to 18.09%. On the basis, an ultrathin modification layer of lithium fluoride is deposited on the doped hole transport layer, so that the defect between the hole layer and the perovskite layer interface is passivated, and the non-radiative recombination between the interfaces is inhibited. Meanwhile, the transmission efficiency of current carriers between interfaces is improved, and the crystallization quality of the perovskite thin film is improved, so that the photoelectric conversion efficiency is further improved to 18.54 percent. The work in this chapter proves the possibility that organic micromolecule doped nickel oxide and ultrathin insulating layer modified nickel oxide improve the hole transmission performance of the organic micromolecule doped nickel oxide and the ultrathin insulating layer modified nickel oxide, and provides a new method for improving the energy photoelectric conversion efficiency of the trans-form planar perovskite solar cell.

Claims (8)

1. The perovskite solar cell with the trans-form planar structure is characterized by comprising a conductive substrate (1), a hole transport layer (2), an ultrathin modification layer (3), a perovskite light absorption layer (4), an electron transport layer (5), an interface modification layer (6) and a metal cathode (7) which are sequentially stacked from bottom to top; the hole transport layer (2) is prepared by doping tributyl phosphate with nickel oxide, and the ultrathin modification layer (3) is LiF with the thickness of 1-5 nm;
the hole transport layer (2) is obtained by spin coating a nickel oxide precursor solution doped with tributyl phosphate to form a film and then annealing;
the preparation process of the nickel oxide precursor solution doped with tributyl phosphate comprises the following steps:
dissolving 0.1g of nickel acetate in 4mL of ethanol, and adding 24uL of ethanolamine; then stirring and reacting for 6-10 h under the condition of water bath at 60 ℃ to obtain a nickel oxide precursor solution; then adding tributyl phosphate solution to obtain the required precursor solution; the volume ratio of tributyl phosphate to nickel oxide precursor solution is 1-4: 200.
2. The trans-planar perovskite solar cell according to claim 1, wherein the perovskite light absorption layer is APbI3A is CH3NH3 +、CH(NH2)2 +、Cs+Mixtures of any proportion.
3. The trans-planar perovskite solar cell according to claim 1, wherein the conductive substrate (1) is one of FTO glass, ITO glass, ICO glass, IWO glass, IZO glass, AZO glass; the electron transport layer (5) is a fullerene derivative film; the interface modification layer (6) is one of bathocuproine, lithium fluoride and titanium oxide; the metal cathode (7) is one of silver, copper or gold.
4. The trans-planar perovskite solar cell according to claim 1, wherein the thickness of the conductive substrate (1) is 500-600 nm, the thickness of the hole transport layer (2) is 20-50 nm, the thickness of the perovskite light absorption layer (4) is 400-500 nm, the thickness of the electron transport layer (5) is 15-35 nm, the thickness of the interface modification layer (6) is 2-5 nm, and the thickness of the metal cathode (7) is 70-120 nm.
5. The method for preparing the trans-planar perovskite solar cell according to any one of claims 1 to 4, which is characterized by comprising the following steps:
step 1: depositing a nickel oxide precursor solution doped with tributyl phosphate on a conductive substrate (1) by a spin coating method, and annealing to obtain a hole transport layer (2);
step 2: spin-coating and depositing a LiF aqueous solution on the hole transport layer (2), and carrying out annealing treatment to obtain an ultrathin modification layer (3);
and step 3: spin-coating and depositing a perovskite precursor solution on the ultrathin modification layer (3), and carrying out annealing treatment to obtain a perovskite light absorption layer (4);
and 4, step 4: spin-coating and depositing a fullerene derivative solution on the perovskite light absorption layer (4), and carrying out annealing treatment to obtain an electron transmission layer (5);
and 5: depositing the precursor solution of the interface modification layer on the electron transport layer (5) through spin coating, and carrying out annealing treatment to obtain an interface modification layer (6);
step 6: and plating a cathode metal plating layer on the interface modification layer (6) to obtain the required trans-planar perovskite solar cell.
6. The method for preparing a trans-planar perovskite solar cell according to claim 5, wherein in the step 1, the annealing temperature is 270-310 ℃, and the annealing time is 40-60 min; in the step 2, the annealing temperature is 70-150 ℃, and the annealing time is 5-15 min; in the step 3, the annealing temperature is 100 ℃, and the annealing time is 40-60 min; the annealing temperature in the step 4 is 70 ℃, the annealing time is 15min, the annealing temperature in the step 5 is 70 ℃, and the annealing time is 10 min.
7. The method for preparing a trans-planar perovskite solar cell according to claim 5, wherein the perovskite precursor solution in the step 2 is prepared by the following steps:
mixing 29.12mg CsI and 42.72mg PbI2、553.2mg MABr、319.68mg FAI、918.24mg PbI2And 139.84mg of PbBr2Dissolving in a mixed solution composed of N, N-dimethylformamide and dimethyl sulfoxide; wherein the volume ratio of the N, N-dimethylformamide to the dimethyl sulfoxide is 7: 3; and stirring the mixed solution at 60 ℃ for 8h to obtain the required precursor solution.
8. The method for preparing a trans-planar perovskite solar cell as claimed in claim 5, wherein the coating layer in the step 6 is prepared by vacuum evaporation coating with a vacuum degree of 6 x 10-4Pa。
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CN111223990A (en) * 2019-11-29 2020-06-02 西南石油大学 Inverted perovskite solar cell containing alkali metal halide hole modification layer and preparation method

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* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
CN111223990A (en) * 2019-11-29 2020-06-02 西南石油大学 Inverted perovskite solar cell containing alkali metal halide hole modification layer and preparation method

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