CN107946464A - A kind of perovskite solar cell based on barium titanate interface-modifying layer and preparation method thereof - Google Patents

A kind of perovskite solar cell based on barium titanate interface-modifying layer and preparation method thereof Download PDF

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CN107946464A
CN107946464A CN201711113325.0A CN201711113325A CN107946464A CN 107946464 A CN107946464 A CN 107946464A CN 201711113325 A CN201711113325 A CN 201711113325A CN 107946464 A CN107946464 A CN 107946464A
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solar cell
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perovskite solar
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CN107946464B (en
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张振龙
秦建强
毛艳丽
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Henan University
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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
    • H10K30/10—Organic devices sensitive to infrared radiation, light, electromagnetic radiation of shorter wavelength or corpuscular radiation comprising heterojunctions between organic semiconductors and inorganic semiconductors
    • H10K30/15—Sensitised wide-bandgap semiconductor devices, e.g. dye-sensitised TiO2
    • H10K30/151—Sensitised wide-bandgap semiconductor devices, e.g. dye-sensitised TiO2 the wide bandgap semiconductor comprising titanium oxide, e.g. TiO2
    • 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
    • H—ELECTRICITY
    • H10—SEMICONDUCTOR DEVICES; ELECTRIC SOLID-STATE DEVICES NOT OTHERWISE PROVIDED FOR
    • H10K—ORGANIC ELECTRIC SOLID-STATE DEVICES
    • H10K2102/00—Constructional details relating to the organic devices covered by this subclass
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    • 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
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Abstract

The present invention relates to one kind to be based on BaTiO3The perovskite solar cell of interface-modifying layer, the perovskite solar cell include FTO electro-conductive glass, compacted zone, electron transfer layer, interface-modifying layer, perovskite active layer and the hole transmission layer set gradually from bottom to top.BaTiO is based on the invention also discloses above-mentioned3The preparation method of the perovskite solar cell of interface-modifying layer.Perovskite solar cell of the present invention uses BaTiO3Interface-modifying layer of the film as electron transfer layer and perovskite active layer, applied to perovskite solar cell, reduces the compound of interface light induced electron and hole, improves the photoelectric conversion efficiency of perovskite solar cell.

Description

It is a kind of based on the perovskite solar cell of barium titanate interface-modifying layer and its preparation Method
Technical field
The invention belongs to battery preparation technology field, and in particular to one kind is based on barium titanate（BaTiO3）Interface-modifying layer Perovskite solar cell and preparation method thereof.
Background technology
Perovskite solar cell is due to absorption coefficient is big, absorption region is wide, in the sun the advantages that high conversion efficiency Energy field of batteries is subject to people to pay close attention to extensively.At present, the peak efficiency of perovskite solar cell has reached 22.1% （Science, 2017, 356:1376-1379）.Research shows that the interfacial property of electron transfer layer and perovskite active layer is A key factor for hindering perovskite solar battery efficiency to improve, because state can increase light induced electron and sky the defects of interface Cave it is compound.In order to reduce the compound of interface photogenerated charge, a kind of effective method is exactly that electronics is passed using some materials The defects of defeated layer is modified, reduction interface state, so as to reduce the compound of photogenerated charge, further improves the conversion effect of battery Rate（Adv. Mater., 2016, 28:3966; J. Am. Chem. Soc., 2016, 138:14998; J. Mater. Chem. A, 2015, 3:9160）.Therefore, in order to further improve the transfer efficiency of perovskite solar cell, the task of top priority It is to find a kind of excellent electron transfer layer decorative material, and is applied to perovskite solar cell.
The content of the invention
Present invention aims to overcome that prior art defect, there is provided one kind is based on BaTiO3The perovskite of interface-modifying layer is too Positive energy battery, it uses BaTiO3Film is as electron transfer layer and the interface-modifying layer of perovskite active layer, applied to calcium titanium Ore deposit solar cell, reduces the compound of interface light induced electron and hole, improves the opto-electronic conversion effect of perovskite solar cell Rate.
BaTiO is based on present invention also offers above-mentioned3The preparation method of the perovskite solar cell of interface-modifying layer.
To achieve the above object, the present invention adopts the following technical scheme that：
One kind is based on BaTiO3The perovskite solar cell of interface-modifying layer, the perovskite solar cell are included from bottom to top FTO electro-conductive glass, compacted zone, electron transfer layer, interface-modifying layer, perovskite active layer and the hole transmission layer set gradually.
Specifically, the interface-modifying layer is obtained through following processing：Interface-modifying layer precursor solution is spin-coated on electronics In transport layer, anneal 40 ~ 70 min under the conditions of 450 ~ 550 DEG C；The interface-modifying layer precursor solution is dense for quality Ba (the NO of degree 0.3 ~ 2.4%3)2Aqueous solution.
One kind is above-mentioned to be based on BaTiO3The preparation method of the perovskite solar cell of interface-modifying layer, it includes step as follows Suddenly：
1）Compacted zone precursor solution is spin-coated on clean, dry FTO electro-conductive glass, annealed under the conditions of 450 ~ 500 DEG C 30 ~ 50min, obtains compacted zone；
2）By electron transfer layer slurry for rotary coating on compacted zone, anneal 30 ~ 50min under the conditions of 450 ~ 500 DEG C, obtains electronics and passes Defeated layer；
3）By the spin coating of interface-modifying layer precursor solution on the electron transport layer, the annealing 40 ~ 70 under the conditions of 450 ~ 550 DEG C Min, obtains interface-modifying layer；
4）Perovskite active layer precursor solution is spin-coated on interface-modifying layer, and chlorobenzene is added dropwise before rotation terminates, then Sample is heated into 60 ± 10 min in 100 ± 10 DEG C, obtains perovskite active layer；
5）Hole transmission layer precursor solution is spin-coated on perovskite active layer, then using hot one layer of gold of steaming method coated film deposition Electrode to obtain the final product.
Specifically, step 1）In, the compacted zone precursor solution by 0.25 mL butyl titanates, 5 mL absolute ethyl alcohols, 1 mL concentrated nitric acids and 0.5 mL water, which are mixed, to be obtained.
Further, step 2）In, the electron transfer layer slurry is commercialization TiO2Slurry with absolute ethyl alcohol in mass ratio 1:The dilution of gained after 6 dilutions.
Preferably, step 3）In, interface-modifying layer precursor solution is spin-coated on electricity with 3000 ~ 5000 revs/min of rotating speed In sub- transport layer, 30 ~ 60s of spin coating.
Preferably, step 4）In, the perovskite precursor solution is by iodine carbonamidine（FAI）, lead iodide（PbI2）, bromine first Amine（MABr）And lead bromide（PbBr2）It is added to dimethylformamide（DMF）With dimethyl sulfoxide (DMSO)（DMSO）Mixed solution in Mix and obtain（DMF:DMSO=4:1, volume ratio）, wherein, iodine carbonamidine, lead iodide, the molar concentration difference of bromine methylamine and lead bromide It is 1 M, 1.1 M, 0.2 M and 0.22M.
Preferably, step 5）In, the hole transmission layer precursor solution is by 72.3 mg Spiro-OMeTAD, 28.8 μ The acetonitrile solution dissolving of double (fluoroform sulphonyl) imine lithiums that l 4- tert .-butylpyridines and 17.5 μ l concentration are 520 mg/ml Obtained into 1ml chlorobenzenes.
Present invention also offers using the above method be prepared based on BaTiO3The perovskite sun of interface-modifying layer Can battery.
The present invention between electron transfer layer and perovskite active layer by adding one layer of BaTiO3Film is repaiied as interface Layer is adornd, to reduce the compound of photogenerated charge, improves the photoelectric conversion efficiency of perovskite solar cell, solves existing traditional calcium Titanium ore solar cell electron transfer layer and the easily compound problem of perovskite active layer interface photogenerated charge.With prior art phase Than the present invention has the following advantages：
1）The present invention is used precursor B a (NO3)2Aqueous solution spin coating prepares BaTiO on the electron transport layer3Interface-modifying layer. The advantages of this method：First, pattern, the thickness of the accurate control interface decorative layer that adjusts the concentration of precursor solution can be passed through Etc. parameter, optimize photoelectric conversion efficiency of the solar battery, obtain the corresponding optimal precursor solution concentration of highest transfer efficiency；Second, The preparation method is easy to operate, is easy to grasp, and is suitably applied the preparation of solar energy in large area battery；
2）The present invention prepare based on BaTiO3Interface-modifying layer can effectively reduce electron transfer layer and perovskite activity bed boundary The light induced electron at place and hole it is compound, improve short circuit current flow, open-circuit voltage and the fill factor, curve factor of solar cell.It is prepared by the present invention Based on BaTiO3The perovskite solar cell of interface-modifying layer is compared with the perovskite solar cell of no interface-modifying layer, battery Transfer efficiency effectively improves, and peak efficiency reaches 17.9%.
Brief description of the drawings
Fig. 1 is the TiO of no interface-modifying layer2With the TiO for having interface-modifying layer2/BaTiO3X-ray diffractogram（XRD）. What is marked in figure belongs to the BaTiO of cubic structure positioned at 31.5 ° of diffraction maximums3；
Fig. 2 is no interface-modifying layer TiO2And have interface-modifying layer TiO2/BaTiO3UV-visible absorption spectrum；With it is unbounded Face decorative layer TiO2Compare, there is interface-modifying layer TiO2/BaTiO3The somewhat red shift of absorption band edge, illustrate its band gap reduce；
In Fig. 3（a）With（b）It is no interface-modifying layer TiO respectively2And have interface-modifying layer TiO2/BaTiO3Scanning electron microscope (SEM) photograph （SEM）；The granular size of film, pattern do not have significant change before and after modification, illustrate BaTiO3It is very thin to modify layer film, without shadow Ring TiO2Pattern；
Fig. 4 is based on no interface-modifying layer TiO2And have interface-modifying layer TiO2/BaTiO3（0.9 wt%）Solar cell Current-voltage（I-V）Curve map.With based on no interface-modifying layer TiO2Battery compare, based on there is interface-modifying layer TiO2/ BaTiO3Solar cell photoelectric performance effectively improve.
Embodiment
Technical scheme is further discussed in detail with reference to embodiments, but protection scope of the present invention It is not limited thereto.
Embodiment 1
One kind is based on BaTiO3The perovskite solar cell of interface-modifying layer, the perovskite solar cell are included from bottom to top FTO electro-conductive glass, compacted zone, electron transfer layer, interface-modifying layer, perovskite active layer and the hole transmission layer set gradually.
It is above-mentioned to be based on BaTiO3The preparation method of the perovskite solar cell of interface-modifying layer, it specifically includes following step Suddenly：
1）The preparation of compacted zone：The FTO electro-conductive glass of etching is sequentially placed into acetone, isopropanol and ethanol, it is each to be cleaned by ultrasonic 20 minutes, finally irradiated 20 minutes with UV.Compacted zone precursor solution is spin-coated on 3500 revs/min of rotating speed clean, dry On dry FTO electro-conductive glass, anneal 40 min under the conditions of 500 DEG C, obtains compacted zone；The compacted zone precursor solution by 0.25 mL butyl titanates, 5 mL absolute ethyl alcohols, 1 mL concentrated nitric acids and 0.5 mL water, which are mixed, to be obtained；
2）The preparation of electron transfer layer：Electron transfer layer slurry is spin-coated on compacted zone with 4000 revs/min of rotating speed, in Anneal 40 min under the conditions of 450 DEG C, obtains electron transfer layer；The electron transfer layer slurry is commercialization TiO2Slurry（Dyesol, 30NR-D）With absolute ethyl alcohol in mass ratio 1:The dilution of gained after 6 dilutions；
3）The preparation of interface-modifying layer：Interface-modifying layer precursor solution is spin-coated on electronics with 5000 revs/min of rotating speed to pass On defeated layer（Spin coating 30s）, anneal 60min under the conditions of 500 DEG C, obtains interface-modifying layer；The interface-modifying layer presoma is molten Liquid is the Ba (NO of mass concentration 0.3%3)2Aqueous solution；
4）The preparation of perovskite active layer：By perovskite active layer precursor solution in 1000 rpm 10s and 6000 rpm 20s Under conditions of be spin-coated on interface-modifying layer, and 100 μ l chlorobenzenes are added dropwise in 10s before rotation terminates, then by sample in 100 DEG C plus 60 min are heated in hot plate, obtain perovskite active layer；The perovskite precursor solution is by iodine carbonamidine（FAI）, lead iodide （PbI2）, bromine methylamine（MABr）And lead bromide（PbBr2）It is added to dimethylformamide（DMF）With dimethyl sulfoxide (DMSO)（DMSO）'s Mix and obtain in mixed solution（DMF:DMSO=4:1, volume ratio）, wherein, iodine carbonamidine, lead iodide, bromine methylamine and lead bromide rub Your concentration is 1 M, 1.1 M, 0.2 M and 0.22M respectively；
5）The preparation of hole transmission layer：Hole transmission layer precursor solution is spin-coated on perovskite with 4000 revs/min of speed On active layer, the gold electrode that hot steaming method coated film deposition a layer thickness is about 80nm is then used on hole transmission layer to obtain the final product.Institute It is dense by 72.3 mg Spiro-OMeTAD, 28.8 μ l 4- tert .-butylpyridines and 17.5 μ l to state hole transmission layer precursor solution The acetonitrile solution for spending double (fluoroform sulphonyl) imine lithiums for 520 mg/ml is dissolved into 1ml chlorobenzenes and obtains.
Embodiment 2 to 5
One kind is based on BaTiO3The perovskite solar cell of interface-modifying layer, the perovskite solar cell are included from bottom to top FTO electro-conductive glass, compacted zone, electron transfer layer, interface-modifying layer, perovskite active layer and the hole transmission layer set gradually.
It is above-mentioned to be based on BaTiO3The preparation method reference embodiment 1 of the perovskite solar cell of interface-modifying layer, wherein, Difference is, step 3）In when preparing interface-modifying layer, the interface-modifying layer precursor solution is respectively mass concentration 0.6%th, 0.9%, 1.2%, 2.4% Ba (NO3)2Aqueous solution.
Reference examples
Perovskite solar cell and the difference of embodiment 1 are：Without interface-modifying layer.
The photo electric of above-described embodiment preparation gained battery is tested using the solar cell test system of this area routine Can, test result is shown in Table 1.
1 various concentrations precursor solution of table prepares BaTiO3The photovoltaic performance ginseng of solar cell obtained by interface-modifying layer Number
Table 1 is based on no interface-modifying layer and has interface-modifying layer（The BaTiO prepared by the precursor solution of various concentrations3Boundary Face decorative layer）Perovskite solar cell photovoltaic performance parameter.As can be seen from Table 1：With the sun of no interface-modifying layer Energy battery is compared, based on BaTiO3The photovoltaic performance parameter of modifying interface layer solar cell is obtained for raising.When interface is repaiied When decorations layer precursor solution concentration is 0.9 wt%, cell photovoltaic performance improves most, photoelectric conversion efficiency（PCE）By no interface The 16.1% of decorative layer brings up to 17.9%, short circuit current flow（Isc）, open-circuit voltage（Voc）And fill factor, curve factor（FF）Respectively by no interface 21.9 mA/cm of decorative layer2, 1.06 V and 69.3% bring up to 22.5 mA/cm2, 1.10 V and 71.7%.Test result indicates that BaTiO3The introducing of interface-modifying layer is effectively improved the transfer efficiency of perovskite solar cell.

Claims (8)

  1. A kind of 1. perovskite solar cell based on barium titanate interface-modifying layer, it is characterised in that the perovskite solar-electricity Pond includes FTO electro-conductive glass, compacted zone, electron transfer layer, interface-modifying layer, the perovskite active layer set gradually from bottom to top And hole transmission layer.
  2. 2. the perovskite solar cell based on barium titanate interface-modifying layer as claimed in claim 1, it is characterised in that described Interface-modifying layer is obtained through following processing：By the spin coating of interface-modifying layer precursor solution on the electron transport layer, at 450 ~ 550 DEG C Under the conditions of anneal 40 ~ 70 min；The interface-modifying layer precursor solution is the Ba (NO of mass concentration 0.3 ~ 2.4%3)2Water Solution.
  3. 3. the preparation method of the perovskite solar cell based on barium titanate interface-modifying layer, its feature exist described in claim 1 In including the following steps：
    1）Compacted zone precursor solution is spin-coated on clean, dry FTO electro-conductive glass, annealed under the conditions of 450 ~ 500 DEG C 30-50min, obtain compacted zone；
    2）By electron transfer layer slurry for rotary coating on compacted zone, anneal 30 ~ 50min under the conditions of 450 ~ 500 DEG C, obtains electronics and passes Defeated layer；
    3）By the spin coating of interface-modifying layer precursor solution on the electron transport layer, the annealing 40 ~ 70 under the conditions of 450 ~ 550 DEG C Min, obtains interface-modifying layer；
    4）Perovskite active layer precursor solution is spin-coated on interface-modifying layer, and chlorobenzene is added dropwise before rotation terminates, then Sample is heated into 60 ± 10 min in 100 ± 10 DEG C, obtains perovskite active layer；
    5）Hole transmission layer solution is spin-coated on perovskite active layer, is then using hot one layer of gold electrode of steaming method coated film deposition .
  4. 4. the preparation method of the perovskite solar cell based on barium titanate interface-modifying layer as claimed in claim 3, its feature It is, step 1）In, the compacted zone precursor solution is by 0.25 mL butyl titanates, 5 mL absolute ethyl alcohols, 1 mL concentrated nitric acids It is mixed and obtains with 0.5 mL water.
  5. 5. the preparation method of the perovskite solar cell based on barium titanate interface-modifying layer as claimed in claim 3, its feature It is, step 2）In, the electron transfer layer slurry is commercialization TiO2Slurry absolute ethyl alcohol in mass ratio 1:Gained after 6 dilutions Dilution.
  6. 6. the preparation method of the perovskite solar cell based on barium titanate interface-modifying layer as claimed in claim 3, its feature It is, step 3）In, interface-modifying layer precursor solution with 3000 ~ 5000 revs/min of rotating speed spin coating on the electron transport layer, 30 ~ 60s of spin coating.
  7. 7. the preparation method of the perovskite solar cell based on barium titanate interface-modifying layer as claimed in claim 3, its feature It is, step 4）In, the perovskite precursor solution is to be added to diformazan by iodine carbonamidine, lead iodide, bromine methylamine and lead bromide Mix and obtain in the mixed solution of base formamide and dimethyl sulfoxide (DMSO), wherein, iodine carbonamidine, lead iodide, bromine methylamine and lead bromide Molar concentration is 1 M, 1.1 M, 0.2 M and 0.22M respectively.
  8. 8. the preparation method of the perovskite solar cell based on barium titanate interface-modifying layer as claimed in claim 3, its feature It is, step 5）In, the hole transmission layer precursor solution is by 72.3 mg Spiro-OMeTAD, the 28.8 μ l 4- tert-butyl groups The acetonitrile solution of double (fluoroform sulphonyl) imine lithiums that pyridine and 17.5 μ l concentration are 520 mg/ml is dissolved into 1ml chlorobenzenes Middle acquisition.
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CN109545972A (en) * 2018-11-23 2019-03-29 浙江昱辉阳光能源江苏有限公司 A kind of high stability perovskite solar battery and preparation method
CN109638163A (en) * 2018-12-17 2019-04-16 齐齐哈尔大学 It is a kind of using phosphotungstic acid as the perovskite solar battery and preparation method of boundary layer
CN110299454A (en) * 2019-07-04 2019-10-01 湖南师范大学 A kind of perovskite thin film solar battery and preparation method thereof using barium titanate as electron transport material
CN110311041A (en) * 2019-06-25 2019-10-08 宁波大学科学技术学院 A kind of SnO of ZnO modification2Based perovskite solar battery and preparation method
CN110676388A (en) * 2019-10-14 2020-01-10 海南大学 Perovskite solar cell modified based on 3,4,9, 10-perylene tetracarboxylic dianhydride and preparation method
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CN113113541A (en) * 2021-04-08 2021-07-13 华侨大学 Method for passivating perovskite solar cell interface defects by using sodium bis (trifluoromethyl) sulfonyl imide
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CN109103339A (en) * 2018-08-16 2018-12-28 深圳市前海首尔科技有限公司 A kind of preparation method of perovskite solar battery
CN109545972B (en) * 2018-11-23 2022-12-02 浙江昱辉阳光能源江苏有限公司 High-stability perovskite solar cell and preparation method
CN109545972A (en) * 2018-11-23 2019-03-29 浙江昱辉阳光能源江苏有限公司 A kind of high stability perovskite solar battery and preparation method
CN109638163A (en) * 2018-12-17 2019-04-16 齐齐哈尔大学 It is a kind of using phosphotungstic acid as the perovskite solar battery and preparation method of boundary layer
CN109638163B (en) * 2018-12-17 2020-10-09 齐齐哈尔大学 Perovskite solar cell with phosphotungstic acid as interface layer and preparation method
CN110311041A (en) * 2019-06-25 2019-10-08 宁波大学科学技术学院 A kind of SnO of ZnO modification2Based perovskite solar battery and preparation method
CN110311041B (en) * 2019-06-25 2023-06-13 宁波大学科学技术学院 ZnO modified SnO 2 Perovskite-based solar cell and preparation method thereof
CN110299454A (en) * 2019-07-04 2019-10-01 湖南师范大学 A kind of perovskite thin film solar battery and preparation method thereof using barium titanate as electron transport material
CN110676388A (en) * 2019-10-14 2020-01-10 海南大学 Perovskite solar cell modified based on 3,4,9, 10-perylene tetracarboxylic dianhydride and preparation method
CN110993803A (en) * 2019-12-05 2020-04-10 常州大学 Interface modification method of solar cell based on all-inorganic metal halide perovskite material
CN110993803B (en) * 2019-12-05 2023-03-21 常州大学 Interface modification method of solar cell based on all-inorganic metal halide perovskite material
CN113113541A (en) * 2021-04-08 2021-07-13 华侨大学 Method for passivating perovskite solar cell interface defects by using sodium bis (trifluoromethyl) sulfonyl imide
CN113113541B (en) * 2021-04-08 2023-06-06 华侨大学 Method for passivating perovskite solar cell interface defects by using sodium bistrifluoromethylsulfonylimide
CN114050189A (en) * 2021-11-10 2022-02-15 苏州腾晖光伏技术有限公司 Selenium antimony sulfide thin film solar cell with 3D structure and preparation method thereof
CN114369459B (en) * 2022-01-10 2022-12-09 吉林大学 Preparation method of lead-free rare earth perovskite quantum dot, product and application thereof
CN114369459A (en) * 2022-01-10 2022-04-19 吉林大学 Preparation method of lead-free rare earth perovskite quantum dot, product and application thereof

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