CN106450001A - Composite laminated perovskite solar cell and manufacturing method therefor - Google Patents

Composite laminated perovskite solar cell and manufacturing method therefor Download PDF

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CN106450001A
CN106450001A CN201610929641.4A CN201610929641A CN106450001A CN 106450001 A CN106450001 A CN 106450001A CN 201610929641 A CN201610929641 A CN 201610929641A CN 106450001 A CN106450001 A CN 106450001A
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perovskite
composite laminate
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light
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向勇
兰洵
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University of Electronic Science and Technology of China
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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
    • H10K85/00—Organic materials used in the body or electrodes of devices covered by this subclass
    • H10K85/30—Coordination compounds
    • 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

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Abstract

The invention belongs to the field of solar cells, and specifically relates to a composite laminated perovskite solar cell and a manufacturing method therefor. According to the invention, CH3NH3PbBr3, CH3NH3PbI3 and NH2CHNH2PbI3 are prepared together according to a degressive sequence of band gap from the top to the bottom, and a composite laminated perovskite light-absorption layer. The introduction of the composite laminated perovskite light-absorption layer remarkably enlarges the spectral response range of the perovskite solar cell to natural light, improves the carrier concentration, and further improves the photoelectric conversion efficiency of the cell. Meanwhile, the main function of the perovskite light-absorption layer is to generate an electron-hole pair, and the generated electron-hole pair can be conducted by an electron transmission layer and a hole transmission layer through an external electrode. Compared with a conventional multijunction solar cell, no multistage solar cell is needed, and no tunnel junction needs to be introduced, thereby simplifying the preparation technology.

Description

A kind of composite laminate perovskite solaode and preparation method thereof
Technical field
The invention belongs to area of solar cell and in particular to a kind of perovskite solaode of composite lamainated structure and Its preparation method.
Background technology
Day by day exhausted with fossil energy, energy crisis is increasingly sharpened, and the development and utilization of clean reproducible energy becomes The hot issue of 21 century global concern.Wherein photovoltaic solar cell due to efficiently, cleaning, the advantage such as pollution-free, becoming can The development priority of the renewable sources of energy.Photovoltaic solar cell is the photovoltaic effect using quasiconductor, by the luminous energy of solar radiation Be converted to the device of electric energy.From the differentiation of structure and raw material, photovoltaic solar cell experienced from crystal silicon battery to thin film Solaode arrives the development course of multijunction solar cell again., due to mature preparation process, conversion efficiency is stable for crystal silicon battery And become main photovoltaic solar cell.But due to being affected and relatively low specific absorbance by the internal impurity defect of crystal silicon, its Photoelectric transformation efficiency only up to reach 25% about；Thin-film solar cells are because having higher specific absorbance and relatively low Preparation cost, and become the core force of photovoltaic solar cell development.But because thin-film solar cells are less efficient, decay Larger, conversion efficiency highest only has 15% about；Multijunction solar cell refers to the solar spectral for different-waveband, chooses The semi-conducting material of different bandwidth is prepared into multiple solar subcells, and the lamination multi-junction solar of the formation that is together in series Battery.Due to greatly improving the spectral absorption scope of solaode so that photoelectric transformation efficiency has obtained larger raising, More than 44% can be reached.In order to prevent the reverse bias between each sub- battery, needs add ultra-thin in each sub- battery Tunnel junctions, realize the transport of carrier, along with the preparation of each sub- battery, lead to the preparation technology of multijunction solar cell Extremely complex, constrain the process of its industrialized development.
In recent years, a kind of planar heterojunction perovskite solaode is due to having a higher specific absorbance, relatively low load Flow sub- recombination rate, the advantage such as preparation process is simple and get more and more people's extensive concerning.Perovskite solaode is a kind of employing The perovskite metal halide ABX of organic inorganic hybridization3(A：CH3NH3 +；B：Pb2+；X：Cl-,Br-,I-) as light-absorption layer light Volt solaode.The operation principle of perovskite solaode is：Under illumination condition, calcium titanium ore bed absorbing light, produce electricity Sub- hole pair, electron hole pair is sent out in electron transfer layer and light-absorption layer near interface, light-absorption layer and hole transmission layer near interface Raw electron hole separates, and is transmitted by electron transfer layer and hole transmission layer, and forms conductive path via electrode material. Its primary structure includes：Glass substrate, conductive electrode, electron transfer layer, perovskite light-absorption layer, hole transmission layer and metal electricity Pole.
Continuing to optimize with technique, the conversion efficiency of perovskite solaode is also constantly lifted therewith.From 2013 Document " M.Liu, M.B.Johnston, and H.J.Snaith Nature 2,013 501 395 " adopts coevaporation method to prepare Perovskite thin film, since making the planar heterojunction perovskite solaode that first item conversion efficiency is 15.4%, technique obtains Improve to continuous.To document in 2014 " H.Zhao, Q.Chen, G.Li, S.Luo, T.Song, H-S.Duan, Z.Hong, J.You, and Y.Yang Science 2,014 345 542 " passes through doping and modification electron transfer layer, has obtained leveling off to 20% Conversion efficiency.It is to improve having of perovskite conversion efficiency of solar cell to continuing to optimize of perovskite solar battery structure Effect approach.
Content of the invention
For above-mentioned existing problems or deficiency, the invention provides a kind of composite laminate perovskite solaode and its system Preparation Method.The present invention the adopted technical scheme that solves the above problems is：
A kind of composite laminate perovskite solaode, its structure includes from bottom to up successively：Substrate, conductive electrode, electricity Sub- transport layer, composite laminate perovskite light-absorption layer, hole transmission layer and metal electrode.
Thickness≤the 400nm of described composite laminate perovskite light-absorption layer, its structure sequentially consists of：Ground floor is CH3NH3PbBr3, thickness 100～150nm, to expand the absorption of the ultraviolet portion to solar spectral for the light-absorption layer；The second layer is CH3NH3PbI3, thickness 100～150nm, to absorb the visible light part from solar spectral；Third layer is NH2CHNH2PbI3, thickness 100～150nm, it is beneficial to the red shift to solar spectral response range for the perovskite solaode.
Described substrate is glass material or transparent plastic.The conductive electrode being connected with substrate is transparent conducting glass (ITO Or FTO).Electron transfer layer is TiO2Or the dense film that its alloy is made, in order to improve the surface with perovskite light-absorption layer Contact, its thickness is between 10～100nm.Hole transmission layer is organic material Spiro-MeOTAD, and its thickness is in 50～200nm Between.The metal electrode connecting with hole transmission layer adopts gold, silver, copper or aluminum, and the thickness of metal electrode is 80～150nm.
The preparation method of this composite laminate perovskite solaode, comprises the following steps：
Step 1., to cover the substrate of conductive electrode as substrate, prepares fine and close TiO using spin-coating method2Thin film；
Step 2. is then at above-mentioned TiO2On thin film, CH is sequentially prepared using spin-coating method3NH3PbBr3Layer, CH3NH3PbI3Layer and FAPbI3Layer is composite laminate perovskite light-absorption layer；
Step 3. prepares hole transmission layer using spin-coating method on above-mentioned composite laminate perovskite light-absorption layer；
Step 4. prepares metal electrode using vapour deposition method on above-mentioned hole transmission layer.
CH3NH3PbI3Forbidden band broadband be 1.5eV, its spectral response range mainly includes visible-range. CH3NH3PbBr3Energy gap be 1.9eV, there is good ultraviolet spectra response.By changing the molecular size of A position ion The energy gap of perovskite can be regulated and controled, using NH2CHNH2 +Ion substitution CH3NH3 +The perovskite material of ion NH2CHNH2PbI3Energy gap be 1.4eV, compared to CH3NH3PbI3, there is wider spectral response range.In plane In hetero-junctions perovskite solaode, as group together with perovskite material and the electron transfer layer of light-absorption layer, hole transmission layer Become the heterojunction structure of P-i-N, the Main Function of calcium titanium ore bed is to absorb solar spectral to produce electron hole pair.Based on Upper consideration, the present invention from expand perovskite solaode spectral response range, by CH3NH3PbBr3、CH3NH3PbI3 And NH2CHNH2PbI3According to energy gap by upper under the order successively decreased prepare together, form the perovskite that lamination is combined and inhale Photosphere.Using the perovskite solaode of present invention preparation, significantly improve the spectrum to natural light for the perovskite solaode Response range, can lift carrier concentration, thus lifting the photoelectric transformation efficiency of battery further.Simultaneously because perovskite extinction The Main Function of layer is to produce electron-hole pair, and the electron-hole pair of generation can be directly by electron transfer layer and hole transport Layer realizes conducting by external electrode, compares with traditional multijunction solar cell it is not necessary to prepare multi-level solar battery, no Need to introduce tunnel junctions, preparation technology significantly simplifies.
Brief description
Fig. 1 is the composite laminate perovskite solar battery structure schematic diagram of the present invention.
Specific embodiment
In conjunction with the drawings and specific embodiments, the present invention is described in further detail.
As shown in Figure 1：It is glass substrate, electro-conductive glass FTO, electron transfer layer TiO from bottom to up respectively2, ground floor calcium Titanium ore light-absorption layer CH3NH3PbBr3, second layer perovskite light-absorption layer CH3NH3PbI3, third layer perovskite light-absorption layer FAPbI3, empty Cave transport layer Spiro-MeOTAD and metal electrode.The thickness of wherein glass substrate and electro-conductive glass FTO is 200nm, electronics Transport layer thickness 80nm, the thickness 100nm, CH of hole transmission layer3NH3PbBr3The thickness 130nm, CH of layer3NH3PbI3The thickness of layer Degree 130nm, FAPbI3The thickness 140nm of layer, lamination perovskite light-absorption layer gross thickness 400nm.The thickness of metal Ag electrode is 100nm.
The preparation of step 1. transparency electrode：
Prepare electro-conductive glass FTO film on a glass substrate, form 200nm thickness transparency electrode.
The etch cleaner of step 2. electro-conductive glass：
Protect FTO electro-conductive glass 2/3 thickness with marine glue, put it in Zn powder and the aqueous hydrochloric acid solution of 2mol/L and carry out Etching, after the completion of etching, rinses substrate with water, removes marine glue, ultrasonic clear respectively with the acetone of saturation, ethanol and deionized water Wash, put into air dry oven after the completion of cleaning and be dried.
The preparation of step 3. electron transfer layer：
In the substrate that step 2 is obtained, with 5000rpm spin coating TiO2Precursor solution, heats 40 points at 450 DEG C afterwards Clock, re-annealing is to room temperature.
Step 4. light-absorption layer CH3NH3PbBr3Preparation：
Configuration PbBr2：CH3NH3Br is 1:1.3 precursor solution, is spun on TiO with 3500rpm2On electron transfer layer, Heat 30 minutes at 110 DEG C, re-annealing is to room temperature.CH3NH3PbBr3The thickness of layer is 130nm.
Step 5. light-absorption layer CH3NH3PbI3Preparation：
Configuration PbI2：CH3NH3I is 1:1.3 precursor solution, is spun on light-absorption layer CH with 3500rpm3NH3PbBr3On, Heat 30 minutes at 110 DEG C, re-annealing is to room temperature.CH3NH3PbI3The thickness of layer is 130nm.
Step 6.FAPbI3The preparation of layer：
In N2Under environment, the HI phase mixing of C3H6N2O2 with 8.2g of 3g is reacted 2 hours, precipitate passes through at 0 DEG C After 65 DEG C of revolving half an hour, then replace cleaning with ether and ethanol, can get the white powder of FAI after dried.Join Putting Pb (OH) I with FAI molar ratio is 1:Precursor is spin-coated on CH with 5000rpm by 3 spin coating precursor3NH3PbI3On layer, By FAPbI complete for spin coating3Simultaneously being placed on warm table, be heated to 160 DEG C of half an hour, until darkening, that is, completing FAPbI3 The preparation of layer, thickness is 140nm.
The preparation of step 7. hole transmission layer
Composite laminate perovskite light absorbent is dissolved in concentration in green benzene solvent as 0.17M with 5000rpm spin coating Spiro layer, places in glove box after being solidified within 8 hours, aoxidizes 12 hours in drying tower, and obtaining thickness is 100nm's Hole transmission layer.
The preparation of step 8. metal electrode
Method is steamed using Vacuum Heat and prepares the thick metal Ag electrode of 100nm.

Claims (7)

1. a kind of composite laminate perovskite solaode, include successively from bottom to up substrate, conductive electrode, electron transfer layer, Composite laminate perovskite light-absorption layer, hole transmission layer and metal electrode it is characterised in that：
The structure of described composite laminate perovskite light-absorption layer thickness≤400nm sequentially consists of：Ground floor is CH3NH3PbBr3, thickness 100～150nm, to expand the absorption of the ultraviolet portion to solar spectral for the light-absorption layer；The second layer is CH3NH3PbI3, thickness 100～150nm, to absorb the visible light part from solar spectral；Third layer is NH2CHNH2PbI3, thickness 100～150nm, it is beneficial to the red shift to solar spectral response range for the perovskite solaode.
2. composite laminate perovskite solaode as claimed in claim 1 it is characterised in that：Described substrate be glass material or Transparent plastic.
3. composite laminate perovskite solaode as claimed in claim 1 it is characterised in that：Described conductive electrode is transparent leading Electric glass ITO or FTO.
4. composite laminate perovskite solaode as claimed in claim 1 it is characterised in that：Described electron transfer layer is TiO2 Or the dense film that its alloy is made, thickness 10～100nm.
5. composite laminate perovskite solaode as claimed in claim 1 it is characterised in that：Described hole transmission layer is organic Material Spiro-MeOTAD, thickness 50～200nm.
6. composite laminate perovskite solaode as claimed in claim 1 it is characterised in that：Described metal electrode employing gold, Silver, copper or aluminum, thickness 80～150nm.
7. composite laminate perovskite solaode as claimed in claim 1, its preparation method, comprise the following steps：
Step 1., to cover the substrate of conductive electrode as substrate, prepares fine and close TiO using spin-coating method2Thin film；
Step 2. is then at TiO2On thin film, CH is sequentially prepared using spin-coating method3NH3PbBr3Layer, CH3NH3PbI3Layer and FAPbI3Layer I.e. composite laminate perovskite light-absorption layer；
Step 3. prepares hole transmission layer using spin-coating method on above-mentioned composite laminate perovskite light-absorption layer；
Step 4. prepares metal electrode using vapour deposition method on above-mentioned hole transmission layer.
CN201610929641.4A 2016-10-31 2016-10-31 Composite laminated perovskite solar cell and manufacturing method therefor Pending CN106450001A (en)

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Cited By (10)

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Publication number Priority date Publication date Assignee Title
CN107565024A (en) * 2017-08-24 2018-01-09 宁波大学 A kind of perovskite solar cell of staged absorbent layer structure and preparation method thereof
CN107845730A (en) * 2017-12-25 2018-03-27 湖南师范大学 A kind of perovskite solar cell of Cheap highly effective and preparation method thereof
CN108447992A (en) * 2018-04-03 2018-08-24 常州大学 A method of improving organic metal halide perovskite solar cell stability and efficiency
CN108550705A (en) * 2018-06-30 2018-09-18 浙江浙能技术研究院有限公司 A kind of perovskite solar cell module
CN109378385A (en) * 2018-10-08 2019-02-22 电子科技大学 A kind of organic perovskite combination solar battery based on full spectral absorption
CN110335946A (en) * 2019-06-26 2019-10-15 上海黎元新能源科技有限公司 A kind of the perovskite extinction layer material and solar battery of perovskite solar battery
CN110491998A (en) * 2019-08-23 2019-11-22 通威太阳能（成都）有限公司 A kind of plane non-impurity-doped hetero-junctions-perovskite laminated cell and preparation method thereof
CN111211230A (en) * 2020-01-22 2020-05-29 苏州大学 Full-spectrum absorption multilayer perovskite/quantum dot solar cell device and preparation method
CN111916561A (en) * 2020-07-22 2020-11-10 隆基绿能科技股份有限公司 Perovskite solar cell, tandem solar cell and battery pack
WO2024050662A1 (en) * 2022-09-05 2024-03-14 宁德时代新能源科技股份有限公司 Perovskite solar cell, manufacturing method therefor and electric apparatus

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Cited By (14)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
CN107565024A (en) * 2017-08-24 2018-01-09 宁波大学 A kind of perovskite solar cell of staged absorbent layer structure and preparation method thereof
CN107565024B (en) * 2017-08-24 2020-04-14 宁波大学 Perovskite solar cell with stepped absorption layer structure and preparation method thereof
CN107845730A (en) * 2017-12-25 2018-03-27 湖南师范大学 A kind of perovskite solar cell of Cheap highly effective and preparation method thereof
CN107845730B (en) * 2017-12-25 2024-03-08 湖南师范大学 Perovskite solar cell and preparation method thereof
CN108447992B (en) * 2018-04-03 2021-07-27 常州大学 Method for improving stability and efficiency of organic metal halide perovskite solar cell
CN108447992A (en) * 2018-04-03 2018-08-24 常州大学 A method of improving organic metal halide perovskite solar cell stability and efficiency
CN108550705A (en) * 2018-06-30 2018-09-18 浙江浙能技术研究院有限公司 A kind of perovskite solar cell module
CN109378385A (en) * 2018-10-08 2019-02-22 电子科技大学 A kind of organic perovskite combination solar battery based on full spectral absorption
CN110335946A (en) * 2019-06-26 2019-10-15 上海黎元新能源科技有限公司 A kind of the perovskite extinction layer material and solar battery of perovskite solar battery
CN110491998A (en) * 2019-08-23 2019-11-22 通威太阳能（成都）有限公司 A kind of plane non-impurity-doped hetero-junctions-perovskite laminated cell and preparation method thereof
CN111211230B (en) * 2020-01-22 2023-04-18 苏州大学 Full-spectrum absorption multilayer perovskite/quantum dot solar cell device and preparation method
CN111211230A (en) * 2020-01-22 2020-05-29 苏州大学 Full-spectrum absorption multilayer perovskite/quantum dot solar cell device and preparation method
CN111916561A (en) * 2020-07-22 2020-11-10 隆基绿能科技股份有限公司 Perovskite solar cell, tandem solar cell and battery pack
WO2024050662A1 (en) * 2022-09-05 2024-03-14 宁德时代新能源科技股份有限公司 Perovskite solar cell, manufacturing method therefor and electric apparatus

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