CN105226190B - A kind of planar heterojunction perovskite solar cell and preparation method thereof - Google Patents
A kind of planar heterojunction perovskite solar cell and preparation method thereof Download PDFInfo
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Abstract
The invention discloses a kind of planar heterojunction perovskite solar cell, the planar heterojunction perovskite solar cell includes electron transfer layer, and the electron transfer layer is prepared by n type conjugated polymer materials.In the perovskite solar cell of the present invention, perovskite material absorbs sunlight and generates exciton and isolate hole and electronics.PX PDI are used for the electron transfer layer of perovskite solar cell by the present invention, are collected and are transmitted electronics, significantly improve device performance.The preparation process of the electron transfer layer is simple, is not necessarily to pyroprocess, and of low cost, experimental repeatability is good, is suitable for large-scale industrial production.
Description
Technical field
The invention belongs to perovskite solar cell material and devices fields, and in particular to a kind of planar heterojunction perovskite
Solar cell and preparation method thereof.
Background technology
The perovskite solar cell of rising in recent years becomes solar energy since its is simple in structure, efficient, at low cost
The hot spot of research.The development of perovskite solar cell is very rapid, in the time less than 4 years, battery efficiency by less than
5% is promoted to 21%." perovskite solar cell photoelectric transfer efficiency breaks through 15% " is chosen as 2013 by Science weeklys
One of year ten big technological breakthrough of the world.
Perovskite solar cell refers to specifically with ABO3The perovskite material of structure, such as CH3NH3PbX3(X is
The halogen atoms such as Cl, Br, I).Currently the majority perovskite solar cell is with TiO2, ZnO as electronics collect and electron-transport
Layer, needs by high temperature sintering.High temperature sintering is the process of a highly energy-consuming, is not suitable for large-scale commercial production.It is common
Fullerene derivate PCBM be organic molecule, film forming is poor, is covered to perovskite incomplete, causes device performance bad.
Imidodicarbonic diamide class material has the characteristics that electron mobility height, good film-forming property, is very typical n-type material, in polymer
Excellent electrons transport property is shown in solar cell and organic field effect tube, itself and other conjugate units are total to
It is poly-, it can effectively adjust the HOMO and lumo energy of molecule.
Invention content
The present invention is copolymerized using different conjugate units and imidodicarbonic diamide PDI units, has been obtained a series of with excellent electricity
The n-type conjugated polymer material of sub- transport property, is applied in perovskite solar cell, can perovskite with
Effective heterojunction boundary is formed between imidodicarbonic diamide copolymer, realizes the fast transport of electronics, and the photoelectricity to improve battery turns
Change efficiency and stability.Entire device fabrication process is all accomplished below at 150 DEG C, compared to TiO2, the materials such as ZnO, drop significantly
Low production cost.
A kind of planar heterojunction perovskite solar cell of present invention offer and preparation method thereof.Specific technical solution is such as
Under:
A kind of planar heterojunction perovskite solar cell, which is characterized in that the planar heterojunction perovskite solar energy
Battery includes electron transfer layer, and the electron transfer layer is prepared by n-type conjugated polymer material.
Further, the planar heterojunction perovskite solar cell includes sequentially substrate, transparent conductive metal oxidation
Object anode layer, hole transmission layer, calcium titanium ore bed, electron transfer layer and cathode layer.
Further, the structure of the n-type conjugated polymer material is PX-PDI, and structural formula is
Wherein, R1For n-octyl, R2For 2- ethylhexyls;
It is obtained with imidodicarbonic diamide (PDI) unit by copolymerization by X unit, and the X unit is the Asias 1,2- ethylene
Base (V), thiophene (T), dithieno pyrroles (DTP), fluorenes (F), dibenzo thiophene cough up (DBS) or carbazole (C)
Further, the thickness of the electron transfer layer is 5nm-15nm.
The preparation method of above-mentioned planar heterojunction perovskite solar cell, includes the following steps:
A. transparent conductive metal oxide anode layer is prepared:Splash-proofing sputtering metal aoxidizes on the substrate of glass or polyester film
Object obtains transparent conductive metal oxide anode layer;
B. hole transmission layer is prepared:The transparent conductive metal oxide anode layer that step a is obtained is through ultraviolet-ozone table
The conducting polymer or metal oxide of spin coating high work content, hole transmission layer is obtained through thermal annealing after surface treatment;
C. calcium titanium ore bed is prepared:Lead source and iodide are dissolved in solvent, it is molten to obtain perovskite precursor for heating stirring
Liquid, which is spun on the hole transmission layer that step b is obtained, and calcium titanium ore bed is obtained through thermal annealing;
D. electron transfer layer is prepared:PX-PDI diimide derivatives are dissolved in solvent, obtain PX-PDI solution, it will
Acquired solution is spun on the calcium titanium ore bed that step c is obtained and obtains electron transfer layer;
E. cathode layer is prepared:The vacuum evaporation metal electrode on the electron transfer layer that step d is obtained, as cathode layer.
Further, the conducting polymer in the step b is PEDOT and PSS.
Further, the solvent in the step d is the mixed solvent that chlorobenzene and chloroform are formed.
Further, the volume ratio of the in the mixed solvent, chlorobenzene and chloroform is 1:1.
Further, in the step d PX-PDI solution a concentration of 6~10mg/ml.
Further, spin coating rotating speed is 800~1200rpm in the step d.
Beneficial effects of the present invention are:
In perovskite solar cell, perovskite material absorbs sunlight and generates exciton and isolate hole and electronics,
PX-PDI is used for the electron transfer layer of perovskite solar cell by the present invention, is collected and is transmitted electronics, significantly improve device
Performance.The preparation process of electron transfer layer of the present invention is simple, is not necessarily to pyroprocess, of low cost, experimental repeatability is good, is suitable for
Large-scale industrial production.
Description of the drawings
Fig. 1 is the atomic force microscope shape appearance figure for the perovskite film that the present invention generates.
Fig. 2 is the perovskite film scanning electron microscope shape appearance figure that the present invention generates.
Fig. 3 is the PV-PDI electron transfer layer atomic force microscope shape appearance figures that the method for the present invention obtains.
Fig. 4 is the PV-PDI electron transfer layer scanning electron microscope shape appearance figures that the method for the present invention obtains.
Fig. 5 is the current-voltage characteristic curve of perovskite solar cell prepared by embodiment 1, and obtained device structure is
FTO/PEDOT:PSS/CH3NH3PbI3/PC60BM/Al。
Fig. 6 is the current-voltage characteristic curve of perovskite solar cell prepared by embodiment 2, and obtained device structure is
FTO/PEDOT:PSS/CH3NH3PbI3/PV-PDI/Al。
Fig. 7 is the current-voltage characteristic curve of perovskite solar cell prepared by embodiment 3, and obtained device structure is
FTO/PEDOT:PSS/CH3NH3PbI3/PT-PDI/Al。
Fig. 8 is the current-voltage characteristic curve of perovskite solar cell prepared by embodiment 4, and obtained device structure is
FTO/PEDOT:PSS/CH3NH3PbI3/PDTP-PDI/Al。
Fig. 9 is the current-voltage characteristic curve of perovskite solar cell prepared by embodiment 5, and obtained device structure is
FTO/PEDOT:PSS/CH3NH3PbI3/PF-PDI/Al。
Figure 10 is the current-voltage characteristic curve of perovskite solar cell prepared by embodiment 6, and obtained device structure is
FTO/PEDOT:PSS/CH3NH3PbI3/PDBS-PDI/Al。
Figure 11 is the current-voltage characteristic curve of perovskite solar cell prepared by embodiment 7, and obtained device structure is
FTO/PEDOT:PSS/CH3NH3PbI3/PC-PDI/Al。
Specific implementation mode
The present invention provides a kind of perovskite solar cells and preparation method thereof, in the following with reference to the drawings and specific embodiments
The present invention will be further described.
Embodiment 1 (comparative example)
Sputtering there is into doping fluorine SnO2(FTO) transparent conducting glass uses liquid detergent, tap water, deionized water, third successively
Ketone, isopropanol are cleaned by ultrasonic twice, and nitrogen drying is immediately placed in processing 15 minutes in UV ozone surface processing equipment (UVO),
Then spin coating PEDOT and the PSS solution under 2000rpm rotating speeds obtains hole transport after 150 DEG C of thermal annealing 15min in air
Layer 3, thickness is about 30nm.Then by PbI2And CH3NH3I in molar ratio 1:1 is dissolved in DFM (N, N-METHYLFORMAMIDE) solution
In, PbI in solution2And CH3NH3The mass ratio of I is 45wt%, and 70 DEG C are heated 5 hours, and perovskite precursor solution is made.By calcium
Titanium ore precursor solution is spun under the rotating speed of 5000rpm on hole transmission layer, and thermal annealing 15~20 minutes obtains perovskite
Layer, thickness are 320nm~380nm.Later the PC of a concentration of 20mg/ml60Rotating speed backspin of the chlorobenzene solution of BM in 1000rpm
It is coated on above-mentioned calcium titanium ore bed, obtains the electron transfer layer that thickness is about 5nm~15nm.Finally in 5x10-5Pa or less vacuum is steamed
The Al that plating thickness is 50nm~60nm does cathode.Obtained device structure is FTO/PEDOT:PSS/CH3NH3PbI3/PC60BM/Al,
Open-circuit voltage is 0.83v, short circuit current 14.71mA/cm under the simulated solar irradiation irradiation every square centimeter of 100 milliwatts2, fill out
It is 59.62% to fill the factor, transfer efficiency 7.29%.Fig. 5 gives the device without light irradiation and through 100 every square of milliwatts
Centimetre simulated solar irradiation irradiation under current -voltage curve.
Embodiment 2 (PV-PDI)
Sputtering there is into doping fluorine SnO2(FTO) transparent conducting glass uses liquid detergent, tap water, deionized water, third successively
Ketone, isopropanol are cleaned by ultrasonic twice, and nitrogen drying is immediately placed in processing 15 minutes in UV ozone surface processing equipment (UVO),
Then spin coating PEDOT and the PSS solution under 2000rpm rotating speeds obtains hole transport after 150 DEG C of thermal annealing 15min in air
Layer 3, thickness is about 30nm.Then by PbI2And CH3NH3I in molar ratio 1:1 is dissolved in DFM (N, N-METHYLFORMAMIDE) solution
In, PbI in solution2And CH3NH3The mass ratio of I is 45wt%, and 70 DEG C are heated 5 hours, and perovskite precursor solution is made.By calcium
Titanium ore precursor solution is spun under the rotating speed of 5000rpm on hole transmission layer, and thermal annealing 15~20 minutes obtains perovskite
Layer, thickness are 320nm~380nm.The solution of the PV-PDI of a concentration of 6mg/ml, (solvent is chlorobenzene and chloroform volume ratio later
It is 1:1 mixed solution) it is spin-coated under the rotating speed of 800rpm on above-mentioned calcium titanium ore bed, it obtains the electronics that thickness is about 5nm and passes
Defeated layer.Finally in 5x10-5Pa or less vacuum evaporation thickness is that the Al of 50nm~60nm does cathode.Obtained device structure is FTO/
PEDOT:PSS/CH3NH3PbI3/ PV-PDI/Al, open-circuit voltage is under the simulated solar irradiation irradiation every square centimeter of 100 milliwatts
0.96v, short circuit current 21.32mA/cm2, fill factor 57.10%, transfer efficiency 11.69%.Fig. 6 gives the device
Part is without the current -voltage curve under light irradiation and the simulated solar irradiation every square centimeter through 100 milliwatts irradiation.
Embodiment 3 (PT-PDI)
Sputtering there is into doping fluorine SnO2(FTO) transparent conducting glass uses liquid detergent, tap water, deionized water, third successively
Ketone, isopropanol are cleaned by ultrasonic twice, and nitrogen drying is immediately placed in processing 15 minutes in UV ozone surface processing equipment (UVO),
Then the spin coating PEDOT under 2000rpm rotating speeds:PSS solution obtains hole transmission layer after 150 DEG C of thermal annealing 15min in air
3, thickness is about 30nm.Then by PbI2And CH3NH3I in molar ratio 1:1 is dissolved in DFM (N, N-METHYLFORMAMIDE) solution
In, PbI in solution2And CH3NH3The mass ratio of I is 45wt%, and 70 DEG C are heated 5 hours, and perovskite precursor solution is made.By calcium
Titanium ore precursor solution is spun under the rotating speed of 5000rpm on hole transmission layer, and thermal annealing 15~20 minutes obtains perovskite
Layer, thickness are 320nm~380nm.The solution of the PT-PDI of a concentration of 8mg/ml, (solvent is chlorobenzene and chloroform volume ratio later
It is 1:1 mixed solution) it is spin-coated under the rotating speed of 900rpm on above-mentioned calcium titanium ore bed, it obtains the electronics that thickness is about 15nm and passes
Defeated layer.Finally in 5x10-5Pa or less vacuum evaporation thickness is that the Al of 50nm~60nm does cathode.Obtained device structure is FTO/
PEDOT:PSS/CH3NH3PbI3/ PT-PDI/Al, open-circuit voltage is under the simulated solar irradiation irradiation every square centimeter of 100 milliwatts
0.90v, short circuit current 19.44mA/cm2, fill factor 56.80%, transfer efficiency 9.88%.Fig. 7 gives the device
Part is without the current -voltage curve under light irradiation and the simulated solar irradiation every square centimeter through 100 milliwatts irradiation.
Embodiment 4 (PDTP-PDI)
Sputtering there is into doping fluorine SnO2(FTO) transparent conducting glass uses liquid detergent, tap water, deionized water, third successively
Ketone, isopropanol are cleaned by ultrasonic twice, and nitrogen drying is immediately placed in processing 15 minutes in UV ozone surface processing equipment (UVO),
Then the spin coating PEDOT under 2000rpm rotating speeds:PSS solution obtains hole transmission layer after 150 DEG C of thermal annealing 15min in air
3, thickness is about 30nm.Then by PbI2And CH3NH3I in molar ratio 1:1 is dissolved in DFM (N, N-METHYLFORMAMIDE) solution
In, PbI in solution2And CH3NH3The mass ratio of I is 45wt%, and 70 DEG C are heated 5 hours, and perovskite precursor solution is made.By calcium
Titanium ore precursor solution is spun under the rotating speed of 5000rpm on hole transmission layer, and thermal annealing 15~20 minutes obtains perovskite
Layer, thickness are 320nm~380nm.The solution of the PDTP-PDI of a concentration of 10mg/ml, (solvent is chlorobenzene and chloroform body later
Product is than being 1:1 mixed solution) it is spin-coated under the rotating speed of 1000rpm on above-mentioned calcium titanium ore bed, it is about 10nm's to obtain thickness
Electron transfer layer.Finally in 5x10-5Pa or less vacuum evaporation thickness is that the Al of 50nm~60nm does cathode.Obtained device structure is
FTO/PEDOT:PSS/CH3NH3PbI3/ PDTP-PDI/Al opens a way under the simulated solar irradiation irradiation every square centimeter of 100 milliwatts
Voltage is 0.90v, short circuit current 19.89mA/cm2, fill factor 59.01%, transfer efficiency 10.59%.Fig. 8 is provided
The device is without the current -voltage curve under light irradiation and the simulated solar irradiation every square centimeter through 100 milliwatts irradiation.
Embodiment 5 (PF-PDI)
Sputtering there is into doping fluorine SnO2(FTO) transparent conducting glass uses liquid detergent, tap water, deionized water, third successively
Ketone, isopropanol are cleaned by ultrasonic twice, and nitrogen drying is immediately placed in processing 15 minutes in UV ozone surface processing equipment (UVO),
Then the spin coating PEDOT under 2000rpm rotating speeds:PSS solution obtains hole transmission layer after 150 DEG C of thermal annealing 15min in air
3, thickness is about 30nm.Then by PbI2And CH3NH3I in molar ratio 1:1 is dissolved in DFM (N, N-METHYLFORMAMIDE) solution
In, PbI in solution2And CH3NH3The mass ratio of I is 45wt%, and 70 DEG C are heated 5 hours, and perovskite precursor solution is made.By calcium
Titanium ore precursor solution is spun under the rotating speed of 5000rpm on hole transmission layer, and thermal annealing 15~20 minutes obtains perovskite
Layer, thickness are 320nm~380nm.The solution of the PF-PDI of a concentration of 8mg/ml, (solvent is chlorobenzene and chloroform volume ratio later
It is 1:1 mixed solution) it is spin-coated under the rotating speed of 800rpm on above-mentioned calcium titanium ore bed, it obtains the electronics that thickness is about 8nm and passes
Defeated layer.Finally in 5x10-5Pa or less vacuum evaporation thickness is that the Al of 50nm~60nm does cathode.Obtained device structure is FTO/
PEDOT:PSS/CH3NH3PbI3/ PF-PDI/Al, open-circuit voltage is under the simulated solar irradiation irradiation every square centimeter of 100 milliwatts
0.94v, short circuit current 19.03mA/cm2, fill factor 58.01%, transfer efficiency 10.4%.Fig. 9 gives the device
Part is without the current -voltage curve under light irradiation and the simulated solar irradiation every square centimeter through 100 milliwatts irradiation.
Embodiment 6 (PDBS-PDI)
Sputtering there is into doping fluorine SnO2(FTO) transparent conducting glass uses liquid detergent, tap water, deionized water, third successively
Ketone, isopropanol are cleaned by ultrasonic twice, and nitrogen drying is immediately placed in processing 15 minutes in UV ozone surface processing equipment (UVO),
Then the spin coating PEDOT under 2000rpm rotating speeds:PSS solution obtains hole transmission layer after 150 DEG C of thermal annealing 15min in air
3, thickness is about 30nm.Then by PbI2And CH3NH3I in molar ratio 1:1 is dissolved in DFM (N, N-METHYLFORMAMIDE) solution
In, PbI in solution2And CH3NH3The mass ratio of I is 45wt%, and 70 DEG C are heated 5 hours, and perovskite precursor solution is made.By calcium
Titanium ore precursor solution is spun under the rotating speed of 5000rpm on hole transmission layer, and thermal annealing 15~20 minutes obtains perovskite
Layer, thickness are 320nm~380nm.The solution of the PDBS-PDI of a concentration of 8mg/ml, (solvent is chlorobenzene and chloroform volume later
Than being 1:1 mixed solution) it is spin-coated under the rotating speed of 1200rpm on above-mentioned calcium titanium ore bed, obtain the electricity that thickness is about 12nm
Sub- transport layer.Finally in 5x10-5Pa or less vacuum evaporation thickness is that the Al of 50nm~60nm does cathode.Obtained device structure is
FTO/PEDOT:PSS/CH3NH3PbI3/ PDBS-PDI/Al opens a way under the simulated solar irradiation irradiation every square centimeter of 100 milliwatts
Voltage is 0.92v, short circuit current 20.14mA/cm2, fill factor 54.97%, transfer efficiency 10.19%.Figure 10 gives
The device is gone out bent without the current-voltage under light irradiation and the simulated solar irradiation every square centimeter through 100 milliwatts irradiation
Line.
Embodiment 7 (PC-PDI)
Sputtering there is into doping fluorine SnO2(FTO) transparent conducting glass uses liquid detergent, tap water, deionized water, third successively
Ketone, isopropanol are cleaned by ultrasonic twice, and nitrogen drying is immediately placed in processing 15 minutes in UV ozone surface processing equipment (UVO),
Then the spin coating PEDOT under 2000rpm rotating speeds:PSS solution obtains hole transmission layer after 150 DEG C of thermal annealing 15min in air
3, thickness is about 30nm.Then by PbI2And CH3NH3I in molar ratio 1:1 is dissolved in DFM (N, N-METHYLFORMAMIDE) solution
In, PbI in solution2And CH3NH3The mass ratio of I is 45wt%, and 70 DEG C are heated 5 hours, and perovskite precursor solution is made.By calcium
Titanium ore precursor solution is spun under the rotating speed of 5000rpm on hole transmission layer, and thermal annealing 15~20 minutes obtains perovskite
Layer, thickness are 320nm~380nm.The solution of the PC-PDI of a concentration of 10mg/ml, (solvent is chlorobenzene and chloroform volume later
Than being 1:1 mixed solution) it is spin-coated under the rotating speed of 1000rpm on above-mentioned calcium titanium ore bed, it is about 10.5nm's to obtain thickness
Electron transfer layer.Finally in 5x10-5Pa or less vacuum evaporation thickness is that the Al of 50nm~60nm does cathode.Obtained device structure is
FTO/PEDOT:PSS/CH3NH3PbI3/ PC-PDI/Al, electricity of opening a way under the simulated solar irradiation irradiation every square centimeter of 100 milliwatts
Pressure is 0.91v, short circuit current 19.33mA/cm2, fill factor 59.09%, transfer efficiency 10.35%.Figure 11 is provided
The device is without the current -voltage curve under light irradiation and the simulated solar irradiation every square centimeter through 100 milliwatts irradiation.
Claims (2)
1. a kind of preparation method of planar heterojunction perovskite solar cell, which is characterized in that include the following steps:
(1) sputtering there is into doping fluorine SnO2(FTO) transparent conducting glass successively use liquid detergent, tap water, deionized water, acetone,
Isopropanol is cleaned by ultrasonic twice, and nitrogen drying is immediately placed in processing 15 minutes in UV ozone surface processing equipment (UVO), so
The spin coating PEDOT under 2000rpm rotating speeds afterwards:PSS solution obtains hole transmission layer after 150 DEG C of thermal annealing 15min in air,
Its thickness is about 30nm;
(2) by PbI2And CH3NH3I in molar ratio 1:1 is dissolved in DFM (N, N-METHYLFORMAMIDE) solution, PbI in solution2With
CH3NH3The mass ratio of I is 45wt%, and 70 DEG C are heated 5 hours, and perovskite precursor solution is made;
(3) perovskite precursor solution is spun under the rotating speed of 5000rpm on hole transmission layer, 15~20 points of thermal annealing
Clock, obtains calcium titanium ore bed, and thickness is 320nm~380nm;
(4) the solution of the PV-PDI of a concentration of 6mg/ml, solvent is chlorobenzene and chloroform volume ratio is 1:1 mixed solution,
It is spin-coated under the rotating speed of 800rpm on above-mentioned calcium titanium ore bed, obtains the electron transfer layer that thickness is about 5nm;
(5) in vacuum degree 5x10-5Pa is hereinafter, vacuum evaporation thickness is the Al of 50nm~60nm as cathode on the electron transport layer
Layer;
Wherein, PV-PDI structural formulas are in step (4)
I.e. X unit is 1,2- ethenylidenes.
2. a kind of preparation method of planar heterojunction perovskite solar cell according to claim 1, which is characterized in that institute
It is FTO/PEDOT to obtain device architecture:PSS/CH3NH3PbI3/ PV-PDI/Al, in 100 milliwatts simulated solar irradiation every square centimeter
The lower open-circuit voltage of irradiation is 0.96v, short circuit current 21.32mA/cm2, fill factor 57.10%, transfer efficiency is
11.69%.
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