CN110224066A - A kind of translucent perovskite solar battery of no auxiliary layer and preparation method thereof - Google Patents
A kind of translucent perovskite solar battery of no auxiliary layer and preparation method thereof Download PDFInfo
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- CN110224066A CN110224066A CN201910399234.0A CN201910399234A CN110224066A CN 110224066 A CN110224066 A CN 110224066A CN 201910399234 A CN201910399234 A CN 201910399234A CN 110224066 A CN110224066 A CN 110224066A
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- H10K30/15—Sensitised wide-bandgap semiconductor devices, e.g. dye-sensitised TiO2
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Abstract
The invention discloses translucent perovskite solar batteries of a kind of no auxiliary layer and preparation method thereof, wherein, the translucent perovskite solar battery of no auxiliary layer includes: the transparent conductive substrate being sequentially arranged from the bottom up, electron transfer layer, perovskite active layer, hole transmission layer and transparent electrode layer, the material of the transparent electrode layer is ITO, AZO or IZO, is deposited on the hole transport layer by the method for magnetron sputtering or electron beam evaporation.Present invention employs the inorganic material of compatible magnetron sputtering technique as hole transmission layer, it is prepared for not needing the translucent perovskite solar battery of auxiliary layer, solve the problems, such as that auxiliary layer preparation is difficult, repeatability is low, stability is poor, simple process, it is cheap.Meanwhile the inorganic material that the present invention uses also can be improved device stability, substantially reduce the cost of hole transmission layer, be conducive to the commercial applications of perovskite lamination solar cell.
Description
Technical field
The invention belongs to perovskite photoelectric fields, more particularly, to a kind of translucent perovskite solar-electricity of no auxiliary layer
Pond and preparation method thereof.
Background technique
In recent years, organic inorganic hybridization perovskite solar cell is since its absorptivity is high, sub-bandgap absorbs small, ABSORPTION EDGE
The precipitous and adjustable advantage of forbidden bandwidth, receive a lot of attention, high efficiency and low cost in lamination solar cell field
The characteristics of be also beneficial to industrialized application, had at present including silicon/perovskite, CIGS/ perovskite, perovskite/perovskite
Many reports including lamination solar cell.And an important component as lamination solar cell, translucent calcium
The preparation of titanium ore solar battery still has many problems.
Due to needing to guarantee translucency, the top electrode of translucent perovskite solar battery is usually using the transparent oxygen adulterated
Compound conductive film, such as ITO, IZO, AZO or ultra-thin noble metal film, also or noble metal nanocrystalline.Currently, super
Thin noble metal film generallys use thermal evaporation preparation, and it is too low that there are light transmission rates, and thickness is difficult to control with a wide range of precise, cost
The problems such as high.Although noble metal nanocrystalline light transmission rate is higher, difficult complicated, unsuitable large-scale production, while its are prepared
Technique is compatible with perovskite solar battery, and there are also problems.
Comparatively, transparent oxide conductive film can take into account translucency and electric conductivity, with perovskite solar battery
Preparation process compatibility it is also fine, be most common selection.The common preparation means of transparent electrode be magnetron sputtering and
Electron beam evaporation, for organic cavity transmission layer common in perovskite solar battery, often unbearable these are made
A large amount of defects are generated on surface for the bombardment by ions generated in means, seriously affect its contact with transparent electrode.Solution party
Method is in one layer of auxiliary layer of thermal evaporation on hole transmission layer in cell manufacturing process, to play a protective role.However it is common auxiliary
Help layer material, such as MoOX、WOXDeng there are poor repeatability, stability is poor, it is difficult to the shortcomings that large area controls, therefore how not have
It is the project for being worth research that translucent perovskite solar cell is prepared in the case where auxiliary layer.
Summary of the invention
The invention discloses translucent perovskite solar batteries of a kind of no auxiliary layer and preparation method thereof, solve auxiliary
Help the problem that layer preparation is difficult, repeatability is low, stability is poor.
Technical scheme is as follows:
A kind of translucent perovskite solar battery of no auxiliary layer, including the electrically conducting transparent base being sequentially arranged from the bottom up
Plate, electron transfer layer, perovskite active layer, hole transmission layer and transparent electrode layer, the material of the transparent electrode layer are
ITO, AZO or IZO, on the hole transport layer by the method for magnetron sputtering or electron beam evaporation deposition.
The transparent conductive substrate is the glass or plastics for covering ITO, AZO, IZO or FTO film.
Further, the transparent conductive substrate is ITO material, and on the glass substrate, square resistance is 8~15 to deposition
Ω, light transmittance are 85~90%, and thickness of glass is 1.1~2.2mm.
The material of the electron transfer layer is TiO2、SnO2Or ZnO.Further, the electron transfer layer is SnO2It is thin
Film, with a thickness of 30~40nm.
The preparation process of the electron transfer layer are as follows:
The SnO for being 15~40mg/mL by concentration2、TiO2, PCBM or ZnO precursor solution be spin-coated on ITO, AZO, IZO
Or on FTO electro-conductive glass, revolving speed is 3000~5000rpm, and the time is 30~60s；Glass is heated to 180 using warm table later
~270 DEG C and 0.5~2h of heat preservation, 5~15min then is handled with UV ozone.
The perovskite active layer is by ABX3Type perovskite material is formed, wherein A is selected from Cs+、CH3NH3 +、CH(NH2)2 +Or
Its mixture, B are selected from Pb2 +、Sn2 +Or mixtures thereof, X is selected from Br-、I-、Cl-Or mixtures thereof.
Further, the perovskite active layer CH3NH3PbI3, with a thickness of 400~600nm.
The preparation process of the perovskite active layer are as follows:
By A, B and X by 1:(1~1.2): the molar ratio of (1~1.2) is dissolved in DMF solution, concentration be 1.25~
1.6mol/ml；After dissolution, on the electron transport layer by perovskite precursor solution drop, the spin coating at 3000~5000rpm,
The ether of 600~1000 μ L is added dropwise when 20~22s；The good perovskite thin film of spin coating is placed on 100~120 DEG C of warm table
It is heat-treated 5~30min.
The hole transmission layer is NiO, Cu2O, CuSCN or CuI.Further, the hole transmission layer is to incite somebody to action
The ethyl sulfide solution of CuSCN is spin-coated on perovskite active layer, 100~120nm.
The preparation process of the hole transmission layer are as follows:
By NiO, Cu of 20~60mg2O, CuO, CuSCN or CuI are dissolved in the ethyl sulfide solvent of 1mL, glass with
3000~6000rpm is added drop-wise on glass while rotation, continues 30~60s of rotation.
The transparent electrode layer by the method for magnetron sputtering deposition on the hole transport layer, deposition process are as follows: 0.1~
Under the vacuum condition of 1Pa, with the transparent electrode layer material of 100~150nm of power magnetron sputtering of 20~60W in hole transmission layer
On.
Further, the transparent electrode is ITO, is deposited on the hole transport layer by the method for magnetron sputtering,
With a thickness of 100~150nm, square resistance is 30~40 Ω.
The invention also discloses a kind of translucent perovskite preparation method of solar battery of no auxiliary layer, including following step
It is rapid:
(1) cleaning of transparent conductive substrate: ITO, AZO, IZO or FTO electro-conductive glass successively deionized water, dish washing liquid,
It is cleaned by ultrasonic 5~10min in acetone, ethanol solution, is dried up electro-conductive glass with nitrogen, uses UV ozone cleaning machine processing 10
~20min；
(2) preparation of electron transfer layer: it is 15~40mg/mL by concentration, is dissolved in the SnO of ethyl alcohol2、TiO2Or ZnO forerunner
Liquid solution is spin-coated on ITO, AZO, IZO or FTO electro-conductive glass, and revolving speed is 3000~5000rpm, and the time is 30~60s；Later
To 180~270 DEG C and 0.5~2h is kept the temperature using warm table heating glass, then handles 5~15min with UV ozone；
(3) it is molten that A, B and X by the molar ratio of 1:1~1.2:1~1.2 preparation of perovskite active layer: are dissolved in DMF
In liquid, concentration is 1.25~1.6mol/ml；Wherein, A is selected from Cs+, CH3NH3 +、CH(NH2)2 +Or mixtures thereof, B is selected from Pb2 +、
Sn2 +Or mixtures thereof, X is selected from Br-、I-、Cl-Or mixtures thereof；
After dissolution, on the electron transport layer by obtained perovskite precursor solution drop, in 3000~5000rpm backspin
It applies, the ether of 600~1000 μ L is added dropwise in 20~22s；By the good perovskite thin film of spin coating be placed on 100~120 DEG C plus
5~30min is heat-treated in thermal station；
(4) preparation of hole transmission layer: by NiO, Cu of 20~60mg2O, CuO, CuSCN or CuI are dissolved in the second of 1mL
In thioether solvent, in glass to be added drop-wise on the perovskite thin film on glass while 3000~6000rpm rotation, continue to rotate
30~60s；
(5) preparation of transparent electrode: under the vacuum condition of 0.1~1Pa, with the power magnetron sputtering 100 of 20~60W~
ITO, AZO or IZO of 150nm is on above-mentioned hole transmission layer.
Compared with prior art, the invention has the following advantages:
It is compared with common translucent perovskite solar battery, by the present invention in that, tolerance transparent electricity good with stability
The inorganic hole-transporting layer of pole film forming procedure replaces common organic cavity transmission layer, has been prepared without the semi-transparent of auxiliary layer
Bright perovskite solar battery, photoelectric conversion efficiency has bright compared with no auxiliary layer, using the battery of organic cavity transmission layer
Aobvious promotion.The present invention can substantially reduce the cost of translucent perovskite solar battery, simplify technique, improve device and stablize
Property, it is advantageously implemented the large-scale application of two-sided extinction perovskite solar battery and perovskite lamination solar cell.
Detailed description of the invention
Fig. 1 is the device architecture and working principle diagram of translucent perovskite solar battery in the embodiment of the present invention 1；
Fig. 2 is I-V curve figure of the translucent perovskite solar battery under AM1.5 illumination in the embodiment of the present invention 1；
Fig. 3 is I-V curve figure of the translucent perovskite solar battery under AM1.5 illumination in the embodiment of the present invention 2；
Fig. 4 is I-V curve figure of the translucent perovskite solar battery under AM1.5 illumination in the embodiment of the present invention 3.
Specific embodiment
The invention will be described in further detail with reference to the accompanying drawings and examples, it should be pointed out that reality as described below
It applies example to be intended to convenient for the understanding of the present invention, and does not play any restriction effect to it.
Embodiment 1
As shown in Figure 1, a kind of translucent perovskite solar battery of no auxiliary layer, including what is be sequentially arranged from the bottom up
Transparent conductive substrate, electron transfer layer, perovskite active layer, hole transmission layer and transparent electrode layer.
In the present embodiment, transparent conductive substrate is the glass for covering ito thin film, and the material of electron transfer layer is SnO2, calcium
Titanium ore active layer is perovskite material CH3NH3PbI3, hole transmission layer CuSCN, transparent electrode layer ITO.Specific preparation side
Method is as follows:
Step 1, the cleaning of ito glass: selecting square resistance for 10 Ω, light transmittance 90%, with a thickness of the ITO glass of 1.1mm
ITO electro-conductive glass is successively cleaned by ultrasonic in deionized water, dish washing liquid, acetone, ethanol solution 5min, then uses nitrogen by glass
Ito glass is dried up, 20min is handled using UV ozone cleaning machine.
Step 2, electron transfer layer SnO2Preparation: by the SnCl of 20mg2·2H2O is dissolved in the ethanol solution of 1mL, molten
Solution is spin-coated in ITO substrate after solution is complete, revolving speed 3000rpm, spin-coating time 30s.Finally, the film that spin coating is good
230 DEG C of heating 1h on warm table are placed on, is put into UV ozone handles 5min after cooling.
Step 3, the preparation of perovskite thin film: by PbI2、CH3NH3It is molten that I and DMSO by the molar ratio of 1:1:1 is dissolved in DMF
In liquid, concentration 1.45mol/mL.After solution is completely dissolved, perovskite precursor solution is dripped in SnO2On.In 1000rpm
5000rpm is accelerated to after lower spin coating 10s, the ether of 600 μ L is added dropwise in 20~22s.The good perovskite thin film of spin coating is put
10min is heat-treated on 100 DEG C of warm table.
Step 4, the preparation of hole transmission layer: 35mg CuSCN is dissolved in the ethyl sulfide solvent of 1mL, glass with
CuSCN solution is added drop-wise to perovskite thin film surface when 5000rpm rotates, continues to rotate 30s.
Step 5, the preparation of transparent electrode layer: under the vacuum condition of 0.2Pa, with the power magnetron sputtering 150nm's of 60W
ITO is on CuSCN film.
The performance of the translucent perovskite solar battery obtained in this example is as shown in Figure 2.The solar battery
It is 13.91% that photoelectric efficiency, which is just being swept, and counter sweep is 12.79%.
Embodiment 2
In the present embodiment, transparent conductive substrate is the glass for covering FTO film, and the material of electron transfer layer is SnO2, calcium
Titanium ore active layer is perovskite material CH3NH3PbI3, hole transmission layer CuI, transparent electrode layer ITO.Specific preparation method
It is as follows:
Step 1, the cleaning of FTO glass: selecting square resistance for 10 Ω, light transmittance 90%, with a thickness of the FTO glass of 1.1mm
FTO electro-conductive glass is successively cleaned by ultrasonic in deionized water, dish washing liquid, acetone, ethanol solution 5min, then uses nitrogen by glass
FTO glass is dried up, 20min is handled using UV ozone cleaning machine.
Step 2, electron transfer layer SnO2Preparation: by the SnCl of 20mg2·2H2O is dissolved in the ethanol solution of 1mL, molten
Solution is spin-coated in FTO substrate after solution is complete, revolving speed 3000rpm, spin-coating time 30s.Finally, the film that spin coating is good
230 DEG C of heating 1h on warm table are placed on, is put into UV ozone handles 5min after cooling.
Step 3, the preparation of perovskite thin film: by PbI2、CH3NH3It is molten that I and DMSO by the molar ratio of 1:1:1 is dissolved in DMF
In liquid, concentration 1.45mol/mL.After solution is completely dissolved, perovskite precursor solution is dripped in SnO2On.In 1000rpm
5000rpm is accelerated to after lower spin coating 10s, the ether of 600 μ L is added dropwise in 20~22s.The good perovskite thin film of spin coating is put
10min is heat-treated on 100 DEG C of warm table.
Step 4, the preparation of hole transmission layer: 40mg CuI is dissolved in the acetonitrile solvent of 1mL, glass with
CuI solution is added drop-wise to perovskite thin film surface when 5000rpm rotates, continues to rotate 30s.
Step 5, the preparation of transparent electrode layer: under the vacuum condition of 0.2Pa, with the power magnetron sputtering 150nm's of 60W
ITO is on CuI film.
The performance of the translucent perovskite solar battery obtained in this example is as shown in Figure 3.The solar battery
It is 12.03% that photoelectric efficiency, which is just being swept, and counter sweep is 10.48%.
Embodiment 3
In the present embodiment, transparent conductive substrate is the glass for covering ito thin film, and the material of electron transfer layer is PCBM, calcium
Titanium ore active layer is perovskite material CH (NH2)2PbI3, hole transmission layer CuSCN, transparent electrode layer ITO.Specific preparation
Method is as follows:
Step 1, the cleaning of ito glass: selecting square resistance for 10 Ω, light transmittance 90%, with a thickness of the ITO glass of 1.1mm
ITO electro-conductive glass is successively cleaned by ultrasonic in deionized water, dish washing liquid, acetone, ethanol solution 5min, then uses nitrogen by glass
Ito glass is dried up, 20min is handled using UV ozone cleaning machine.
Step 2, the preparation of electron transfer layer PCBM: the PCBM of 20mg is dissolved in the chlorobenzene solution of 1mL, and dissolution is complete
Solution is spin-coated in ITO substrate afterwards, revolving speed 4000rpm, spin-coating time 30s.
Step 3, the preparation of perovskite thin film: by PbI2、CH2N2H3It is molten that I and DMSO by the molar ratio of 1:1:1 is dissolved in DMF
In liquid, concentration 1.55mol/mL.After solution is completely dissolved, by perovskite precursor solution drop on PCBM.In 1000rpm
5000rpm is accelerated to after lower spin coating 10s, the chlorobenzene of 600 μ L is added dropwise in 20~22s.The good perovskite thin film of spin coating is put
10min is heat-treated on 100 DEG C of warm table.
Step 4, the preparation of hole transmission layer: 50mg CuSCN is dissolved in the ethyl sulfide solvent of 1mL, glass with
CuSCN solution is added drop-wise to perovskite thin film surface when 6000rpm rotates, continues to rotate 30s.
Step 5, the preparation of transparent electrode layer: under the vacuum condition of 0.3Pa, with the power magnetron sputtering 120nm's of 40W
AZO is on CuSCN film.
The performance of the translucent perovskite solar battery obtained in this example is as shown in Figure 4.The solar battery
It is 13.84% that photoelectric efficiency, which is just being swept, and counter sweep is 13.01%.
Technical solution of the present invention and beneficial effect is described in detail in embodiment described above, it should be understood that
Above is only a specific embodiment of the present invention, it is not intended to restrict the invention, it is all to be done in spirit of the invention
Any modification, supplementary, and equivalent replacement, should all be included in the protection scope of the present invention.
Claims (10)
1. a kind of translucent perovskite solar battery of no auxiliary layer, which is characterized in that including what is be sequentially arranged from the bottom up
Transparent conductive substrate, electron transfer layer, perovskite active layer, hole transmission layer and transparent electrode layer, the transparent electrode layer
Material be ITO, AZO or IZO, by the method for magnetron sputtering or electron beam evaporation deposition on the hole transport layer.
2. the translucent perovskite solar battery of no auxiliary layer according to claim 1, which is characterized in that described transparent
Electrically-conductive backing plate is the glass or plastics for covering ITO, AZO, IZO or FTO film.
3. the translucent perovskite solar battery of no auxiliary layer according to claim 1, which is characterized in that the electricity
The material of sub- transport layer is TiO2、SnO2, PCBM or ZnO.
4. the translucent perovskite solar battery of no auxiliary layer according to claim 3, which is characterized in that the electronics
The preparation process of transport layer are as follows:
The SnO for being 15~40mg/mL by concentration2、TiO2, PCBM or ZnO precursor solution be spin-coated on ITO, AZO, IZO or FTO
On electro-conductive glass, revolving speed is 3000~5000rpm, and the time is 30~60s；Glass is heated to 180~270 using warm table later
DEG C and keep the temperature 0.5~2h, then with UV ozone handle 5~15min.
5. the translucent perovskite solar battery of no auxiliary layer according to claim 1, which is characterized in that the calcium titanium
Mine active layer is by ABX3Type perovskite material is formed, wherein A is selected from Cs+、CH3NH3 +、CH(NH2)2 +Or mixtures thereof, B is selected from
Pb2 +、Sn2 +Or mixtures thereof, X is selected from Br-、I-、Cl-Or mixtures thereof.
6. the translucent perovskite solar battery of no auxiliary layer according to claim 5, which is characterized in that the calcium titanium
The preparation process of mine active layer are as follows:
A, B and X are dissolved in DMF solution by the molar ratio of 1:1~1.2:1~1.2, concentration is 1.25~1.6mol/ml；It is molten
Xie Hou, on the electron transport layer by perovskite precursor solution drop, the spin coating at 3000~5000rpm is dripped in 20~22s
Add the ether of 600~1000 μ L；By the good perovskite thin film of spin coating be placed on 100~120 DEG C of warm table heat treatment 5~
30min。
7. the translucent perovskite solar battery of no auxiliary layer according to claim 1, which is characterized in that the sky
Cave transport layer is NiO, Cu2O, CuO, CuSCN or CuI.
8. the translucent perovskite solar battery of no auxiliary layer according to claim 7, which is characterized in that the hole
The preparation process of transport layer are as follows:
By NiO, Cu of 20~60mg2O, CuO, CuSCN or CuI are dissolved in the ethyl sulfide solvent of 1mL, glass with 3000~
6000rpm is added drop-wise on glass while rotation, continues 30~60s of rotation.
9. the translucent perovskite solar battery of no auxiliary layer according to claim 1, which is characterized in that described transparent
Electrode layer is deposited on the hole transport layer by the method for magnetron sputtering, deposition process are as follows: under the vacuum condition of 0.1~1Pa,
On the hole transport layer with the transparent electrode layer material of 100~150nm of power magnetron sputtering of 20~60W.
10. a kind of translucent perovskite preparation method of solar battery of no auxiliary layer, which comprises the following steps:
(1) cleaning of transparent conductive substrate: ITO, AZO, IZO or FTO electro-conductive glass successively deionized water, dish washing liquid, acetone,
In ethanol solution be cleaned by ultrasonic 5~10min, electro-conductive glass is dried up with nitrogen, using UV ozone cleaning machine processing 10~
20min；
(2) preparation of electron transfer layer: the SnO for being 15~40mg/mL by concentration2、TiO2, PCBM or ZnO precursor solution rotation
It is coated on ITO, AZO, IZO or FTO electro-conductive glass, revolving speed is 3000~5000rpm, and the time is 30~60s；Later using heating
Platform heats glass to 180~270 DEG C and keeps the temperature 0.5~2h, then handles 5~15min with UV ozone；
(3) preparation of perovskite active layer: A, B and X are dissolved in DMF solution by the molar ratio of 1:1~1.2:1~1.2,
Concentration is 1.25~1.6mol/ml；Wherein, A is selected from or mixtures thereof Cs+, CH3NH3+, CH (NH2) 2+, and B is selected from Pb2 +、Sn2 +
Or mixtures thereof, X is selected from Br-、I-、Cl-Or mixtures thereof；
After dissolution, on the electron transport layer by obtained perovskite precursor solution drop, the spin coating at 3000~5000rpm,
The ether of 600~1000 μ L is added dropwise when 20~22s；The good perovskite thin film of spin coating is placed on 100~120 DEG C of warm table
It is heat-treated 5~30min；
(4) preparation of hole transmission layer: by NiO, Cu of 20~60mg2O, CuO, CuSCN or CuI be dissolved in 1mL ethyl sulfide it is molten
In agent, glass with 3000~6000rpm rotation while be added drop-wise on the perovskite thin film on glass, continue rotation 30~
60s；
(5) preparation of transparent electrode: under the vacuum condition of 0.1~1Pa, with the power magnetron sputtering 100 of 20~60W~
ITO, AZO or IZO of 150nm is on above-mentioned hole transmission layer.
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Cited By (5)
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| CN112909173A (en) * | 2021-01-18 | 2021-06-04 | 香港科技大学深圳研究院 | Perovskite material, preparation method and application thereof, and semitransparent perovskite solar cell |
| CN113394343A (en) * | 2021-01-07 | 2021-09-14 | 湖州师范学院 | Back-incident p-i-n structure perovskite solar cell and preparation method thereof |
| CN113555451A (en) * | 2020-04-23 | 2021-10-26 | 南方科技大学 | Preparation method of transparent photoelectric device and transparent photoelectric device |
| CN113707817A (en) * | 2021-08-26 | 2021-11-26 | 浙江浙能技术研究院有限公司 | Preparation method of inorganic hole transport layer of perovskite solar cell |
| CN114583011A (en) * | 2022-03-02 | 2022-06-03 | 江西沃格光电股份有限公司 | Manufacturing method of perovskite solar cell based on all-inorganic material |
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| CN114583011A (en) * | 2022-03-02 | 2022-06-03 | 江西沃格光电股份有限公司 | Manufacturing method of perovskite solar cell based on all-inorganic material |
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