CN112366277A - Perovskite solar cell charge transport layer material and preparation method thereof - Google Patents
Perovskite solar cell charge transport layer material and preparation method thereof Download PDFInfo
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Abstract
The invention discloses a perovskite solar cell charge transport layer material and a preparation method thereof, wherein the charge transport layer material is prepared by coating a layer of polymethyl methacrylate (PMMA), poly [ bis (4-phenyl) (2,4, 6-trimethylphenyl) amine (PTAA) and Polystyrene (PS) mixed organic spin coating on a NiOx nanocrystalline coating on ITO glass for modification. The preparation method comprises the steps of adding nickel nitrate into deionized water, stirring, dropwise adding sodium hydroxide to adjust the pH value, filtering, drying and calcining to obtain NiOx nanocrystals; adding the NiOx nanocrystal into ethylenediamine, stirring, spin-coating on ITO glass, and annealing; polymethyl methacrylate, poly [ bis (4-phenyl) (2,4, 6-trimethylphenyl) amine and polystyrene are added into a toluene solution and are spin-coated on ITO glass of a NiOx nanocrystalline substrate to obtain the charge transport layer material. The charge transport layer material is more matched with the energy level of the perovskite layer, so that the energy loss is reduced, and the charge transport is facilitated, so that the photoelectric conversion efficiency of the perovskite layer is improved.
Description
Technical Field
The invention belongs to the technical field of solar cells, and particularly relates to a perovskite solar cell charge transport layer material and a preparation method thereof.
Background
Organic-inorganic hybrid perovskite materials are receiving attention due to their advantages of excellent photoelectric properties, low cost and solution processability. Since Mihasaka and the like introduce perovskite materials into the photovoltaic field for the first time, the photoelectric conversion efficiency of perovskite solar cells is rapidly improved, and the latest certification record of 25.2% is reached and is close to the theoretical limit. Low cost, high efficiency and high stability are key indicators to consider when converting this technology from laboratory to commercial products.
The stability of perovskite solar cells is affected by a variety of factors, mainly divided into internal and external factors. Internal factors include the instability of the perovskite material itself and the instability of the interface between the perovskite and the charge transport layer. The use of inorganic charge transport materials such as metal oxides has proven to be an effective method for improving device stability. The metal oxide can be prepared at low temperature by evaporation or by corresponding precursor solution and nanocrystalline dispersion liquid, the process is simple, the cost is low, and the metal oxide material has higher carrier mobility and good stability, so the metal oxide material is widely researched. In recent years, some groups have attempted to replace these organic transport layers with inorganic materials (e.g., CuSCN, CuI, and NiOx) as charge transport layers. The selection of the charge transport layer material is one of the key factors influencing the performance of the device, but the inorganic semiconductor material NiOx and the perovskite layer material have poor energy level matching and interface contact, so that the energy loss of the interface is inhibited, and the charge transport is not facilitated.
Disclosure of Invention
In view of the above problems, the present invention provides a perovskite solar cell charge transport layer material and a preparation method thereof.
The invention aims to provide a perovskite solar cell charge transport layer material, which is modified by selectively coating a layer of polymethyl methacrylate (PMMA), poly [ bis (4-phenyl) (2,4, 6-trimethylphenyl) amine (PTAA) and Polystyrene (PS) mixed organic spin coating on a NiOx nanocrystalline coating spin-coated on ITO glass.
Wherein the polymethyl methacrylate (PMMA) has a structural formula:
the structural formula of the poly [ bis (4-phenyl) (2,4, 6-trimethylphenyl) ] amine (PTAA) is as follows:
the structural formula of the Polystyrene (PS) is as follows:
the invention also aims to provide a preparation method of the perovskite solar cell charge transport layer material, which comprises the following steps:
s1: adding nickel nitrate hexahydrate into deionized water, stirring for 30-45 min, then dropwise adding a sodium hydroxide solution to adjust the pH value of the solution, continuously stirring for 20-30 min, filtering, washing precipitates with deionized water, drying at 80-90 ℃ for 10-15 h, placing the precipitates in a tubular furnace, and calcining at 280-300 ℃ for 2.5-3 h to obtain the NiOx nanocrystal.
S2: adding the NiOx nanocrystal into ethylenediamine, uniformly stirring, wherein the molar ratio of the NiOx nanocrystal to the ethylenediamine is 1:1, spin-coating the obtained precursor solution on ITO glass, annealing at 160-180 ℃ for 0.5-1 h, further annealing at 300-320 ℃ for 1.5-2 h, cooling, and preparing for the next step.
S3: adding polymethyl methacrylate (PMMA), poly [ bis (4-phenyl) (2,4, 6-trimethylphenyl) ] amine (PTAA) and Polystyrene (PS) into a toluene solution, wherein the prepared concentration is 1.9-2.2 mol/L, and then spin-coating on the ITO glass of the NiOx nanocrystalline substrate in the step S2 at the rotating speed of 5000-6000 rpm/min to obtain the charge transport layer material.
Preferably, the mass-to-volume ratio of the nickel nitrate hexahydrate to the deionized water is (260-296) g, (180-210) mL.
Preferably, the molar concentration of the sodium hydroxide solution is 9.2-10.6 mol/L; adjusting the pH value to 10.3-11.1.
Preferably, the mass ratio of the polymethyl methacrylate (PMMA), the poly [ bis (4-phenyl) (2,4, 6-trimethylphenyl) amine (PTAA) and the Polystyrene (PS) is (0.34-0.46): (0.66-0.82): 0.41-047).
The invention has the following beneficial effects:
in the invention, polymethyl methacrylate (PMMA) and poly [ bis (4-phenyl) (2,4, 6-trimethylphenyl) are adopted according to a certain mass ratio]Amine (PTAA) and Polystyrene (PS) modified NiOx films in which the insulating polymer PS, without any functional groups, carries a functional group capable of reacting with Pb2+An insulating polymer PMMA of C ═ O and methoxy groups (OMe groups) and a semiconductor polymer PTAA, all of which are capable of reducing the surface roughness of the NiOx thin film, thereby improving the interfacial contact between NiOx and perovskite, suppressing the device dark current, reducing the interfacial defects, and a PMMA in which C ═ O and OMe groups and Pb are reacted2+Facilitates passivation of defects, thereby achieving higher V than PS-modified devicesoc(ii) a After the surface of NiOx is modified by the PTAA, the NiOx has a deeper HOMO energy level which is more matched with the energy level of the perovskite layer, so that the energy loss is reduced, the charge transmission is facilitated, and the photoelectric conversion efficiency is improved.
Drawings
FIG. 1 is an SEM image of a charge transport layer material prepared in example 1 of the present invention;
Detailed Description
The following embodiments of the present invention are described in detail, and the embodiments are implemented on the premise of the technical solution of the present invention, and a detailed implementation manner and a specific operation process are given, it should be noted that, for those skilled in the art, a plurality of modifications and decorations can be made without departing from the principle of the present invention, and these modifications and decorations should also be regarded as the protection scope of the present invention.
Example 1
A perovskite solar cell charge transport layer material and a preparation method thereof specifically comprise the following steps:
s1: adding nickel nitrate hexahydrate into deionized water, stirring for 30min, wherein the mass-to-volume ratio of the nickel nitrate hexahydrate to the deionized water is 260g:180mL, then dropwise adding a sodium hydroxide solution with the molar concentration of 9.2mol/L to adjust the pH value of the solution to 10.3, continuously stirring for 20min, filtering, washing precipitates with deionized water, drying at 80 ℃ for 10h, placing the precipitates in a tubular furnace, and calcining at 280 ℃ for 2.5h to obtain the NiOx nanocrystals.
S2: adding the NiOx nanocrystal into ethylenediamine, stirring uniformly, wherein the molar ratio of the NiOx nanocrystal to the ethylenediamine is 1:1, spin-coating the obtained precursor solution on ITO glass, annealing at 160 ℃ for 0.5h, further annealing at 300 ℃ for 1.5h, cooling, and preparing for the next step.
S3: adding polymethyl methacrylate (PMMA), poly [ bis (4-phenyl) (2,4, 6-trimethylphenyl) amine (PTAA) and Polystyrene (PS) into a toluene solution, wherein the mass ratio of the polymethyl methacrylate (PMMA), the poly [ bis (4-phenyl) (2,4, 6-trimethylphenyl) ] amine (PTAA) and the Polystyrene (PS) is 0.34:0.66:0.41, the prepared concentration is 1.9mol/L, and then spin-coating on ITO glass of the NiOx nanocrystalline substrate in the step S2 at the rotating speed of 5000rpm/min to obtain the charge transport layer material.
Example 2
A perovskite solar cell charge transport layer material and a preparation method thereof specifically comprise the following steps:
s1: adding nickel nitrate hexahydrate into deionized water, stirring for 45min, wherein the mass-to-volume ratio of the nickel nitrate hexahydrate to the deionized water is 296g:210mL, then dropwise adding a sodium hydroxide solution with the molar concentration of 10.6mol/L to adjust the pH value of the solution to 11.1, continuously stirring for 30min, filtering, washing precipitates with the deionized water, drying for 15h at 90 ℃, placing the precipitates in a tubular furnace, and calcining for 3h at 300 ℃ to obtain the NiOx nanocrystals.
S2: adding the NiOx nanocrystal into ethylenediamine, uniformly stirring, wherein the molar ratio of the NiOx nanocrystal to the ethylenediamine is 1:1, spin-coating the obtained precursor solution on ITO glass, annealing at 180 ℃ for 1h, further annealing at 320 ℃ for 2h, cooling, and preparing for the next step.
S3: adding polymethyl methacrylate (PMMA), poly [ bis (4-phenyl) (2,4, 6-trimethylphenyl) amine (PTAA) and Polystyrene (PS) into a toluene solution, wherein the mass ratio of the polymethyl methacrylate (PMMA), the poly [ bis (4-phenyl) (2,4, 6-trimethylphenyl) ] amine (PTAA) and the Polystyrene (PS) is 0.46:0.82:047, the prepared concentration is 2.2mol/L, and then spin-coating on the ITO glass of the NiOx nanocrystalline substrate in the step S2 at the rotating speed of 6000rpm/min to obtain the charge transport layer material.
Example 3
A perovskite solar cell charge transport layer material and a preparation method thereof specifically comprise the following steps:
s1: adding nickel nitrate hexahydrate into deionized water, stirring for 40min, wherein the mass-to-volume ratio of the nickel nitrate hexahydrate to the deionized water is 276g:195mL, then dropwise adding a sodium hydroxide solution with the molar concentration of 10mol/L to adjust the pH value range of the solution to 10.8, continuously stirring for 25min, filtering, washing precipitates with the deionized water, drying for 13h at 85 ℃, placing the precipitates in a tubular furnace, and calcining for 2.5-3 h at 290 ℃ to obtain the NiOx nanocrystal.
S2: adding the NiOx nanocrystal into ethylenediamine, uniformly stirring, wherein the molar ratio of the NiOx nanocrystal to the ethylenediamine is 1:1, spin-coating the obtained precursor solution on ITO glass, annealing at 170 ℃ for 1h, further annealing at 310 ℃ for 2h, cooling, and preparing for the next step.
S3: adding polymethyl methacrylate (PMMA), poly [ bis (4-phenyl) (2,4, 6-trimethylphenyl) ] amine (PTAA) and Polystyrene (PS) into a toluene solution, wherein the mass ratio of the polymethyl methacrylate (PMMA), the poly [ bis (4-phenyl) (2,4, 6-trimethylphenyl) amine (PTAA) and the Polystyrene (PS) is 0.39:0.77:0.45, the prepared concentration is 2mol/L, and then spin-coating on ITO glass of the NiOx nanocrystalline substrate in the step S2 at the rotating speed of 5500rpm/min to obtain the charge transport layer material.
Comparative example 1
This comparative example is the same as the preparation method described in example 1 except that NiOx was modified using only poly [ bis (4-phenyl) (2,4, 6-trimethylphenyl) amine (PTAA).
Performance test experiments:
a perovskite battery device: a perovskite layer was sequentially coated on the charge transport layers prepared in examples 1 to 3, wherein the perovskite layer was (MAPbI)3)0.95(MAPbCIBr2)0.05，[6，6]-phenyl-C61A layer of methyl butyrate, a layer of tin dioxide and a layer of silver electrode, using a solar simulator (100 mW/cm)2AM 1.5G) irradiating the PSCs, recording measured J-V and power-voltage (P-V) characteristic curves by using a Keithley (2601A, USA) digital source table, representing the device performance, and obtaining the open-circuit voltage V according to the I-V characteristic curveocShort-circuit current JscAccording to the formula: FF is Pmax/(Voc×Jsc) Obtaining a fill factor FF of the strain; according to the formula: PCE ═ Pmax/PincGiving it a photoelectric conversion efficiency wherein PmaxAt maximum output power, PincThe results are shown in Table 1 for incident light power, Table 1. test results:
as can be seen from table 1, the photoelectric conversion efficiency PCE of the charge transport material prepared in examples 1 to 3 is about 21.66%, and is 19.43% compared to the photoelectric conversion efficiency PCE of the charge transport material prepared in comparative example 1, which indicates that the energy levels of the charge transport material and the perovskite layer are more matched, thereby reducing energy loss, facilitating charge transport, and further improving the photoelectric conversion efficiency thereof.
Claims (8)
1. The perovskite solar cell charge transport layer material is NiOx nanocrystalline, and is characterized in that a NiOx nanocrystalline coating which is spin-coated on ITO glass is further coated with a layer of polymethyl methacrylate (PMMA), poly [ bis (4-phenyl) (2,4, 6-trimethylphenyl) amine (PTAA) and Polystyrene (PS) mixed organic spin coating for modification.
2. The perovskite solar cell charge transport layer material as claimed in claim 1, wherein the polymethyl methacrylate (PMMA) has a structural formula:
3. the perovskite solar cell charge transport layer material of claim 1, wherein the poly [ bis (4-phenyl) (2,4, 6-trimethylphenyl) amine (PTAA) has the formula:
4. the perovskite solar cell charge transport layer material as claimed in claim 1, wherein the Polystyrene (PS) has the formula:
5. the method for preparing a perovskite solar cell charge transport layer material as claimed in claim 1, wherein the method for preparing the perovskite solar cell charge transport layer material comprises the following steps:
s1: adding nickel nitrate hexahydrate into deionized water, stirring for 30-45 min, then dropwise adding a sodium hydroxide solution to adjust the pH value of the solution, continuously stirring for 20-30 min, filtering, washing precipitates with deionized water, drying at 80-90 ℃ for 10-15 h, placing the precipitates in a tubular furnace, and calcining at 280-300 ℃ for 2.5-3 h to obtain NiOx nanocrystals;
s2: adding NiOx nanocrystals into ethylenediamine, uniformly stirring, wherein the molar ratio of the NiOx nanocrystals to the ethylenediamine is 1:1, spin-coating the obtained precursor solution on ITO glass, annealing at 160-180 ℃ for 0.5-1 h, further annealing at 300-320 ℃ for 1.5-2 h, cooling, and preparing for the next step;
s3: adding polymethyl methacrylate (PMMA), poly [ bis (4-phenyl) (2,4, 6-trimethylphenyl) amine (PTAA) and Polystyrene (PS) into a toluene solution, wherein the prepared concentration is 1.9-2.2 mol/L, and then spin-coating on the ITO glass of the NiOx nanocrystalline substrate in the step S2 at the rotating speed of 5000-6000 rpm/min to obtain the charge transport layer material.
6. The preparation method of the perovskite solar cell charge transport layer material as claimed in claim 5, wherein the mass volume ratio of the nickel nitrate hexahydrate and the deionized water is (260-296) g (180-210) mL.
7. The method for preparing a perovskite solar cell charge transport layer material as claimed in claim 5, wherein the molar concentration of the sodium hydroxide solution is 9.2-10.6 mol/L; adjusting the pH value to 10.3-11.1.
8. The method for preparing a perovskite solar cell charge transport layer material as claimed in claim 5, wherein the mass ratio of polymethyl methacrylate (PMMA), poly [ bis (4-phenyl) (2,4, 6-trimethylphenyl) ] amine (PTAA) and Polystyrene (PS) is (0.34-0.46): (0.66-0.82): 0.41-047).
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Cited By (2)
| Publication number | Priority date | Publication date | Assignee | Title |
|---|---|---|---|---|
| CN112802965A (en) * | 2021-04-01 | 2021-05-14 | 太原理工大学 | Interface modification-based perovskite solar cell preparation method |
| CN113299833A (en) * | 2021-04-15 | 2021-08-24 | 暨南大学 | Interface-contacted trans-perovskite solar cell module and preparation method and application thereof |
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Cited By (3)
| Publication number | Priority date | Publication date | Assignee | Title |
|---|---|---|---|---|
| CN112802965A (en) * | 2021-04-01 | 2021-05-14 | 太原理工大学 | Interface modification-based perovskite solar cell preparation method |
| CN113299833A (en) * | 2021-04-15 | 2021-08-24 | 暨南大学 | Interface-contacted trans-perovskite solar cell module and preparation method and application thereof |
| CN113299833B (en) * | 2021-04-15 | 2022-08-02 | 麦耀华 | Interface-contacted trans-perovskite solar cell module and preparation method and application thereof |
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