CN109244249A - The perovskite solar cell device and preparation method thereof that hole transmission layer is modified - Google Patents
The perovskite solar cell device and preparation method thereof that hole transmission layer is modified Download PDFInfo
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- CN109244249A CN109244249A CN201811196681.8A CN201811196681A CN109244249A CN 109244249 A CN109244249 A CN 109244249A CN 201811196681 A CN201811196681 A CN 201811196681A CN 109244249 A CN109244249 A CN 109244249A
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- H—ELECTRICITY
- H10—SEMICONDUCTOR DEVICES; ELECTRIC SOLID-STATE DEVICES NOT OTHERWISE PROVIDED FOR
- H10K—ORGANIC ELECTRIC SOLID-STATE DEVICES
- H10K30/00—Organic devices sensitive to infrared radiation, light, electromagnetic radiation of shorter wavelength or corpuscular radiation
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- H—ELECTRICITY
- H10—SEMICONDUCTOR DEVICES; ELECTRIC SOLID-STATE DEVICES NOT OTHERWISE PROVIDED FOR
- H10K—ORGANIC ELECTRIC SOLID-STATE DEVICES
- H10K71/00—Manufacture or treatment specially adapted for the organic devices covered by this subclass
- H10K71/10—Deposition of organic active material
- H10K71/12—Deposition of organic active material using liquid deposition, e.g. spin coating
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- Y—GENERAL TAGGING OF NEW TECHNOLOGICAL DEVELOPMENTS; GENERAL TAGGING OF CROSS-SECTIONAL TECHNOLOGIES SPANNING OVER SEVERAL SECTIONS OF THE IPC; TECHNICAL SUBJECTS COVERED BY FORMER USPC CROSS-REFERENCE ART COLLECTIONS [XRACs] AND DIGESTS
- Y02—TECHNOLOGIES OR APPLICATIONS FOR MITIGATION OR ADAPTATION AGAINST CLIMATE CHANGE
- Y02E—REDUCTION OF GREENHOUSE GAS [GHG] EMISSIONS, RELATED TO ENERGY GENERATION, TRANSMISSION OR DISTRIBUTION
- Y02E10/00—Energy generation through renewable energy sources
- Y02E10/50—Photovoltaic [PV] energy
- Y02E10/549—Organic PV cells
Abstract
The invention discloses the perovskite solar cell devices and preparation method thereof that a kind of pair of hole transmission layer is modified, the solar cell device is by the transparent substrates that are sequentially overlapped, anode, hole transmission layer, absorbed layer, electron transfer layer, decorative layer and cathode composition, the ethanol solution of present invention ethyl acetate carries out moditied processing to hole transport layer surface, so that its surface is with certain effective group, the crystallization of perovskite thin film can be effectively facilitated, advantageously form the perovskite thin film of more smooth densification, improve carrier mobility and diffusion length, improve charge transfer efficiency, effectively improve short circuit current, improve device efficiency, so as to improve the performance of the luminescent devices such as solar battery, it is widely applied preparing perovskite battery device field.
Description
Technical field
The invention belongs to technical field of solar batteries, and in particular to the perovskite sun modified hole transmission layer
Energy battery device and preparation method thereof.
Background technique
2009, people were for the first time with CH3NH3PbI3, CH3NH3PbBr3Sensitizer as dye-sensitized solar cells is real
About 4% photovoltaic efficiency is showed.Hereafter, people using this material prepare partial size be 2~3nm nanocrystalline introducing dye sensitization too
In positive energy battery, 6% or more photoelectric conversion efficiency is realized, wherein perovskite material is deposited on TiO in the form of quantum dot2
Surface, still, this battery use liquid electrolyte, and perovskite material can gradually dissolve in the electrolytic solution, therefore battery
Service life it is very short, efficiency also cannot very big promotion.
2012, with CH3NH3PbI3With CH3NH3I3- XClx be representative perovskite material realize respectively 9.7% with
10.9% photoelectric conversion efficiency for the first time improves the efficiency of such battery to 10%, so as to cause the extensive concern of people,
This is also the beginning that perovskite material composes new page in area of solar cell.Only after 1 year, perovskite solar-electricity
The efficiency in pond has just broken through 15%, and with deepening continuously to perovskite solar battery research, the photoelectricity of such battery turns
It changes efficiency and persistently rises to 15.9%, ended for the end of the year 2013, efficiency is up to 16.2%, and in 2013 by " science " magazine
It is chosen as one of annual ten big Progress & New Products.
The efficiency of perovskite solar battery has broken through 20% at present, and designing and developing for perovskite material is constantly updated,
The preparation method of perovskite material also tends to multiplicity, and the design of solar cell device structure is continued to optimize.With to its inside
The further research of micro kinetics process, the photoelectric characteristic of perovskite solar battery are able to more clearly show.
For using perovskite thin film for the device of active layer, the structure cell growing state and surface topography of perovskite thin film
To using perovskite thin film as the series of parameters of the device of active layer, the voltage-current density including luminescent device, Qi Liang electricity
Open-circuit voltage, short-circuit current density, fill factor and the photoelectric conversion effect of pressure, luminous efficiency and solar cell device
Rate plays a crucial role.And perovskite ABX3The preparation method of film is to its structure, pattern, charge mobility, electronics
Service life and photoelectric conversion performance are affected.Current prevailing paradigm be perovskite thin film surfacing, densification be obtain it is high-quality
The key of perovskite thin film is measured, the main preparation methods of perovskite thin film include a step spin-coating method, two cloth solwution methods, vapor deposition
Method and gas phase assisted solution method etc., these methods are all to obtain the perovskite thin film of surfacing densification as target.
Meanwhile because in this perovskite solar battery absorbed layer crystallization rate and pattern etc. be difficult to control, and limit
The efficiency of perovskite solar battery improves.How primary study is formed more fine and close smooth perovskite thin film by the present invention
To greatly improve perovskite solar cell device performance.
Summary of the invention
In view of the above problems, the present invention is intended to provide the perovskite sun that a kind of pair of hole transmission layer is modified
Energy battery device and preparation method thereof.The present invention is repaired by the ethanol solution of spin coating ethyl acetate on the hole transport layer
Decorations, spin coating perovskite precursor liquid on this basis, the perovskite solar cell device prepared due to modification, device
Short circuit current and fill factor are significantly improved, and improve device efficiency, so as to improve photoelectric converters such as solar batteries
The performance of part.
To achieve the goals above, the technical solution adopted in the present invention is as follows:
The perovskite solar cell device that a kind of pair of hole transmission layer is modified by be sequentially overlapped transparent substrates, sun
Pole, hole transmission layer, absorbed layer, electron transfer layer, decorative layer and cathode form, on the hole transport layer spin coating acetic acid second
The ethanol solution of ester is modified, and spin coating perovskite precursor liquid forms absorbed layer on the hole transmission layer after modification.
Further, the anode is located on the inner surface of the transparent substrates, and composition material is indium tin oxide
(ITO, Indi μm of Tin Oxides), fluorine tin-oxide (FTO, Fl μ orine doped Tin Oxides) or aluminium zinc oxide
Common transparent electrode materials such as (AZO, Al μm of ini μm of doped Zinc Oxides).
Further, the hole transmission layer is made of organic material and/or inorganic material, and the organic material includes
PEDOT:PSS, Spiro-MeOTAD and PTAA；The inorganic material includes metal oxide, such as nickel oxide, copper oxide, oxidation
One of cuprous or a variety of, effect is mainly transporting holes.
Further, the electron transfer layer is made of organic material and/or inorganic material, and the organic material includes
PCBM、C60And TPBi；The inorganic material includes titanium oxide, zinc oxide and zirconium oxide.
Further, the decorative layer is BCP or LiF, and the effect of decorative layer mainly improves electrode and hole transmission layer
Or the Ohmic contact of electron-transport interlayer, while preventing electrode from directly contacting with perovskite active layer, thickness is usually 1~
10nm。
Further, the cathode is metal electrode or conductive carbon material electrode with higher work-functions.
The preparation method for the perovskite solar cell device that a kind of pair of hole transmission layer is modified, specifically comprising following
Step:
1) preparation of perovskite precursor liquid: the MAI and PbI for being 1:1 by molar ratio2The mixing for being dissolved in GBL and DMSO is molten
Perovskite precursor liquid is used as in liquid, the final concentration of 1.4mol/L of the perovskite precursor liquid, magnetic stirrer over night is stand-by；
2) preparation of hole transmission layer: hole transport layer material is spun to transparent substrates surface, is carried out at annealing later
Reason, with a thickness of 30~70nm, the transparent substrates, respectively with acetone, deionized water and EtOH Sonicate processing, are dried before spin coating,
3-10min is handled with plasma again；
3) preparation and spin coating of solution are modified: ethyl acetate being dissolved in ethyl alcohol and forms modification solution, solution will be modified
According to the speed of 2000-4000rpm on the hole transmission layer prepared spin coating 10-30s, natural drying；
4) preparation of absorbed layer: be added dropwise on the hole transmission layer after modification described in 30~60 μ L after perovskite precursor liquid with
The rate substep spin coating of 900rpm/15s and 4000rpm/25s, and in the 10-20s in second step spin coating process perpendicular to
Dispersion anti-solvent is at the uniform velocity added dropwise in the transparent substrates surface, and the flushing of duration 1s is carried out to perovskite surface, and spin coating process terminates
It is placed in 100 DEG C of thermal station the 10min that anneals, forms absorbed layer；
5) preparation of electron transfer layer: take the mode of vacuum vapor deposition that C is deposited60Or directly spin coating PCBM solution preparation
Electron transfer layer, with a thickness of 20~40nm；
6) preparation of electrode: before electrode, using the method vapor deposition BCP 5-10nm of vacuum vapor deposition as modification
Ag 100nm is deposited in layer later.
Further, the volume ratio of GBL and DMSO is 7:3 in the step 1).
Further, the annealing temperature in the step 2) is 120-150 DEG C, annealing time 10-20min.
Further, the anti-solvent in the step 4) includes toluene, chlorobenzene and ether.
The beneficial effects of the present invention are: the ethanol solution of present invention ethyl acetate modifies hole transport layer surface
Processing, so that its surface can effectively facilitate the crystallization of perovskite thin film, advantageously form more with certain effective group
The perovskite thin film of smooth densification improves carrier mobility and diffusion length, improves charge transfer efficiency, effectively improves short circuit
Electric current improves device efficiency so as to improve the performance of the luminescent devices such as solar battery and is preparing perovskite battery device field
It is widely applied.
Detailed description of the invention
Fig. 1 is the structure chart of the perovskite solar cell device disclosed by the invention modified hole transmission layer；
Fig. 2 is the J-V curve for two kinds of solar cell devices that the embodiment of the present invention one obtains；
Fig. 3 is prepared after the modification solution for the various concentration that the embodiment of the present invention two obtains modifies hole transmission layer
A variety of solar cell devices J-V curve graph.
Specific embodiment
In order to make those skilled in the art be better understood on technical solution of the present invention, with reference to the accompanying drawing and
Embodiment is further described technical solution of the present invention.
Embodiment one:
(1) preparation of perovskite precursor liquid
The PbI of the MAI and 645.4mg of 222.6mg are weighed respectively2Mixing is poured into air-tight bottle, is fallen in said mixture
Enter the DMSO of the GBL and 300 μ L of 700 μ L as solvent, the molar concentration of solution is 1.4mol/L, and room temperature is stood about in glove box
20min is completely dissolved to solute and perovskite precursor liquid can be obtained.
(2) preparation of perovskite solar device
Handled by ito glass piece acetone, deionized water, EtOH Sonicate, then with plasma, by PEDOT:PSS with
The rate of 4000rpm/30s is spun on ito glass, 130 DEG C of annealing 15min.Ethyl acetate is dissolved according to volume ratio 10%
In ethyl alcohol, modification solution is spin-coated on the hole transmission layer prepared according to the speed of 4000rpm/30s, natural drying；It takes
35 μ L of precursor liquid in step (1) is added drop-wise on PEDOT:PSS film, with the rate of 900rpm/15s and 4000rpm/25s point
Spin coating is walked, and the anti-solution of dispersion is at the uniform velocity added dropwise perpendicular to the transparent substrates surface by the 15s in second step spin coating process, it is right
Perovskite surface carries out the flushing of duration 1s, and spin coating process terminates to be placed in 100 DEG C of thermal station the 10min that anneals, and forms absorbed layer；
Then electron transfer layer is prepared using solwution method, i.e., be spin-coated on the PCBM that concentration is 30mg/mL with the rate of 2500rpm/30s
On calcium titanium ore bed, the Ag of the BCP and 100nm of 10nm is finally deposited respectively under condition of negative pressure.
(3) another to prepare to be contrasted experiment using the device that the hole transmission layer without modification is prepared into.
Fig. 2 is hole transmission layer by modification and without the two kinds of solar cell devices prepared in the case of two kinds of modification
J-V curve graph, modifying the volume accounting of ethyl acetate in ethanol in solution is 10%.
Figure it is seen that after being modified using the ethanol solution of ethyl acetate hole transmission layer, solar energy device
The numerical value of the photoelectric conversion efficiency (PCE) of part, short circuit current (Jsc) and fill factor (FF) is all significantly improved, solar energy
The property of battery has promotion largely.
Embodiment 2
(1) preparation of perovskite precursor liquid
The PbI of the MAI and 645.4mg of 222.6mg are weighed respectively2Mixing is poured into air-tight bottle, is fallen in said mixture
Enter the DMSO of the GBL and 300 μ L of 700 μ L as solvent, the molar concentration of solution is 1.4mol/L, and room temperature is stood about in glove box
20min is completely dissolved to solute and perovskite precursor liquid can be obtained.
(2) preparation of perovskite solar device
Handled by ito glass piece acetone, deionized water, EtOH Sonicate, then with plasma, by PEDOT:PSS with
The rate of 4000rpm/30s is spun on ito glass, 130 DEG C of annealing 15min.It prepares ethyl acetate and ethyl alcohol volume ratio is distinguished
For 10%, 15%, 20%, 25% modification solution, it is spin-coated on to the hole prepared according to the speed of 4000rpm/30s and is passed
On defeated layer, natural drying；Take the 35 μ L of precursor liquid in step (1) to be added drop-wise on PEDOT:PSS film, with 900rpm/15s and
The rate substep spin coating of 4000rpm/25s, and the 15s in second step spin coating process is even perpendicular to the transparent substrates surface
Anti- solution is added dropwise in speed, the flushing of duration 1s is carried out to perovskite surface, spin coating process, which terminates to be placed in 100 DEG C of thermal station, anneals
10min forms absorbed layer；Then electron transfer layer is prepared using solwution method, i.e., by PCBM that concentration is 30mg/mL with
The rate of 2500rpm/30s is spin-coated on calcium titanium ore bed, and the BCP and 100nm of 10nm is finally deposited respectively under condition of negative pressure
Ag.
(3) another to prepare to be contrasted experiment using the device that the hole transmission layer without modification is prepared into.
Fig. 3 is a variety of solar cell devices prepared after the modification solution of various concentration modifies hole transmission layer
J-V curve graph, the volume accounting of ethyl acetate in ethanol is respectively 10%, 15%, 20%, 25%, and using without repairing
The device that the hole transmission layer of decorations is prepared into is compared as normal component.
As can be seen from Figure 3 the relationship of device performance and modification solution concentration.When the body of ethyl acetate in modification solution
When product accounting is stepped up, device efficiency is also increased, and when volume accounting reaches 20%, device efficiency reaches peak
14.53%, when volume accounting is further increased to 25%, apparent decline is had occurred in device efficiency.Illustrate when volume accounting
It is best to the modification effect of hole transmission layer when being 20%.
In summary: the electricity that can significantly improve device is modified hole transmission layer with the ethanol solution of ethyl acetate
Stream and fill factor, and then improve efficiency, when volume accounting is 20%, device efficiency reaches peak 14.53%.
Basic principles and main features and advantage of the invention have been shown and described above.But the foregoing is merely this hairs
Bright specific embodiment, technical characteristic of the invention are not limited thereto, and any those skilled in the art is not departing from this hair
The other embodiments obtained under bright technical solution should all cover within the scope of the patent of the present invention.
Claims (10)
1. the perovskite solar cell device that a kind of pair of hole transmission layer is modified, which is characterized in that the solar battery
Device is made of transparent substrates, anode, hole transmission layer, absorbed layer, electron transfer layer, decorative layer and the cathode being sequentially overlapped,
The ethanol solution of spin coating ethyl acetate is modified on the hole transport layer, spin coating calcium on the hole transmission layer after modification
Titanium ore precursor liquid forms absorbed layer.
2. the perovskite solar cell device that a kind of pair of hole transmission layer as described in claim 1 is modified, feature
It is, the anode is located on the inner surface of the transparent substrates, and composition material includes ITO, FTO and AZO.
3. the perovskite solar cell device modified as described in claim 1 hole transmission layer, which is characterized in that
The hole transmission layer is made of organic material and/or inorganic material, and the organic material includes PEDOT:PSS, Spiro-
MeOTAD and PTAA；The inorganic material includes metal oxide, such as one of nickel oxide, copper oxide, cuprous oxide or more
Kind.
4. the perovskite solar cell device modified as described in claim 1 hole transmission layer, which is characterized in that
The electron transfer layer is made of organic material and/or inorganic material, and the organic material includes PCBM, C60And TPBi；It is described
Inorganic material includes titanium oxide, zinc oxide and zirconium oxide.
5. the perovskite solar cell device modified as described in claim 1 hole transmission layer, which is characterized in that
The decorative layer is BCP or LiF, with a thickness of 1~10nm.
6. the perovskite solar cell device modified as described in claim 1 hole transmission layer, which is characterized in that
The cathode is metal electrode or conductive carbon material electrode with higher work-functions.
7. such as the perovskite solar cell device of any of claims 1-6 modified hole transmission layer
Preparation method, which is characterized in that comprising the following steps:
1) preparation of perovskite precursor liquid: the MAI and PbI for being 1:1 by molar ratio2It is dissolved in the mixed solution of GBL and DMSO and makees
For perovskite precursor liquid, the final concentration of 1.4mol/L of the perovskite precursor liquid, magnetic stirrer over night is stand-by；
2) preparation of hole transmission layer: being spun to transparent substrates surface for hole transport layer material, made annealing treatment later, thick
Degree is 30~70nm, and the transparent substrates, respectively with acetone, deionized water and EtOH Sonicate processing, are dried, then use before spin coating
Plasma handles 3-10min；
3) modify solution preparation and spin coating: by ethyl acetate be dissolved in ethyl alcohol formed modification solution, will modification solution according to
The speed of 2000-4000rpm spin coating 10-30s, natural drying on the hole transmission layer prepared；
4) preparation of absorbed layer: be added dropwise on the hole transmission layer after modification described in 30~60 μ L after perovskite precursor liquid with
The rate substep spin coating of 900rpm/15s and 4000rpm/25s, and in the 10-20s in second step spin coating process perpendicular to
Dispersion anti-solvent is at the uniform velocity added dropwise in the transparent substrates surface, and the flushing of duration 1s is carried out to perovskite surface, and spin coating process terminates
It is placed in 100 DEG C of thermal station the 10min that anneals, forms absorbed layer；
5) preparation of electron transfer layer: take the mode of vacuum vapor deposition that C is deposited60Or directly spin coating PCBM solution prepares electronics
Transport layer, with a thickness of 20~40nm；
6) preparation of electrode: before electrode, using the method vapor deposition BCP 5-10nm of vacuum vapor deposition as decorative layer, it
Ag 100nm is deposited afterwards.
8. the preparation method for the perovskite solar cell device that hole transmission layer is modified as claimed in claim 7,
It is characterized in that, the volume ratio of GBL and DMSO is 7:3 in the step 1).
9. the preparation method for the perovskite solar cell device that hole transmission layer is modified as claimed in claim 7,
It is characterized in that, the annealing temperature in the step 2) is 120-150 DEG C, annealing time 10-20min.
10. the preparation method for the perovskite solar cell device that hole transmission layer is modified as claimed in claim 7,
It is characterized in that, the anti-solvent in the step 4) includes toluene, chlorobenzene and ether.
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| CN110311042A (en) * | 2019-05-31 | 2019-10-08 | 南京邮电大学 | A kind of preparation method and perovskite solar battery of self assembled monolayer and perovskite solar battery |
| CN110429180A (en) * | 2019-07-16 | 2019-11-08 | 上海黎元新能源科技有限公司 | A kind of solar battery and preparation method thereof |
| CN110931645A (en) * | 2019-12-18 | 2020-03-27 | 南开大学 | Perovskite solar cell and preparation method thereof |
| CN111092160A (en) * | 2019-11-27 | 2020-05-01 | 中国科学院金属研究所 | Method for passivating lower interface of perovskite solar cell with inverse structure |
| 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 |
| CN112349849A (en) * | 2020-11-13 | 2021-02-09 | 新余学院 | Method for quickly evaporating perovskite solar cell electrode and device preparation thereof |
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| CN110311042A (en) * | 2019-05-31 | 2019-10-08 | 南京邮电大学 | A kind of preparation method and perovskite solar battery of self assembled monolayer and perovskite solar battery |
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| CN110429180A (en) * | 2019-07-16 | 2019-11-08 | 上海黎元新能源科技有限公司 | A kind of solar battery and preparation method thereof |
| CN111092160A (en) * | 2019-11-27 | 2020-05-01 | 中国科学院金属研究所 | Method for passivating lower interface of perovskite solar cell with inverse structure |
| CN111092160B (en) * | 2019-11-27 | 2022-04-05 | 中国科学院金属研究所 | Method for passivating lower interface of perovskite solar cell with inverse structure |
| 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 |
| CN110931645A (en) * | 2019-12-18 | 2020-03-27 | 南开大学 | Perovskite solar cell and preparation method thereof |
| CN110931645B (en) * | 2019-12-18 | 2021-04-13 | 南开大学 | Perovskite solar cell and preparation method thereof |
| CN112349849A (en) * | 2020-11-13 | 2021-02-09 | 新余学院 | Method for quickly evaporating perovskite solar cell electrode and device preparation thereof |
| CN112349849B (en) * | 2020-11-13 | 2023-06-23 | 新余学院 | Method for rapidly evaporating perovskite solar cell electrode and device preparation thereof |
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Application publication date: 20190118 |