CN113097387B - Anti-irradiation photovoltaic energy storage integrated device and preparation method thereof - Google Patents

Anti-irradiation photovoltaic energy storage integrated device and preparation method thereof Download PDF

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CN113097387B
CN113097387B CN202110361565.2A CN202110361565A CN113097387B CN 113097387 B CN113097387 B CN 113097387B CN 202110361565 A CN202110361565 A CN 202110361565A CN 113097387 B CN113097387 B CN 113097387B
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solar cell
packaging
perovskite
energy storage
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CN113097387A (en
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常晶晶
林珍华
王璐
郭雨佳
苏杰
张苗
张进成
郝跃
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Xidian University
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    • H—ELECTRICITY
    • H10—SEMICONDUCTOR DEVICES; ELECTRIC SOLID-STATE DEVICES NOT OTHERWISE PROVIDED FOR
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    • 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
    • H—ELECTRICITY
    • H02—GENERATION; CONVERSION OR DISTRIBUTION OF ELECTRIC POWER
    • H02J—CIRCUIT ARRANGEMENTS OR SYSTEMS FOR SUPPLYING OR DISTRIBUTING ELECTRIC POWER; SYSTEMS FOR STORING ELECTRIC ENERGY
    • H02J7/00—Circuit arrangements for charging or depolarising batteries or for supplying loads from batteries
    • H02J7/34—Parallel operation in networks using both storage and other dc sources, e.g. providing buffering
    • H02J7/35—Parallel operation in networks using both storage and other dc sources, e.g. providing buffering with light sensitive cells
    • 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
    • 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
    • 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
    • H10K30/152—Sensitised wide-bandgap semiconductor devices, e.g. dye-sensitised TiO2 the wide bandgap semiconductor comprising zinc oxide, e.g. ZnO
    • H—ELECTRICITY
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    • H10K—ORGANIC ELECTRIC SOLID-STATE DEVICES
    • H10K30/00—Organic devices sensitive to infrared radiation, light, electromagnetic radiation of shorter wavelength or corpuscular radiation
    • H10K30/80—Constructional details
    • 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
    • H10K30/80—Constructional details
    • H10K30/88—Passivation; Containers; Encapsulations
    • 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
    • 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
    • Y02E10/56—Power conversion systems, e.g. maximum power point trackers

Abstract

The invention discloses an anti-irradiation photovoltaic energy storage integrated device and a preparation method thereof, and mainly solves the problems of low photoelectric conversion efficiency, high cost, long-term stability and poor anti-irradiation capability in the prior art. The solar battery comprises a perovskite solar battery module, a voltage stabilizer, a charge and discharge management assembly, an energy storage battery and a metal halide packaging box. The voltage stabilizer is connected between the solar battery module and the charging and discharging management assembly, and the charging and discharging management assembly is bidirectionally connected with the energy storage battery; a metal halide packaging box is arranged outside the voltage stabilizer, the charge and discharge management assembly and the energy storage battery to prevent radiation damage; each perovskite solar cell forming the solar cell module comprises a transparent conductive substrate, an electron transport layer, a light absorption layer, a hole transport layer, a metal electrode and a double-layer packaging structure. The invention has the advantages of portability, low cost, high efficiency, good radiation resistance and all-weather long-term stable energy storage and power supply all the time, and can be used for artificial satellites, space detectors and spacecrafts.

Description

Anti-irradiation photovoltaic energy storage integrated device and preparation method thereof
Technical Field
The invention belongs to the technical field of electronic devices, and further relates to a photovoltaic energy storage integrated device which can be used for storing and supplying energy for artificial satellites, space detectors, spacecrafts and the like in the aerospace field.
Background
The photovoltaic energy storage integrated device is a device which can convert clean energy of solar energy into electric energy and can be stably used. The device mainly comprises a solar cell, a voltage stabilizer, a charge and discharge management module and an energy storage cell. However, these devices are still in the early stage of development all over the world, and the solar cells mainly adopt two types, namely crystalline silicon cells and thin film cells. The crystalline silicon battery comprises a monocrystalline silicon battery and a polycrystalline silicon battery, occupies the mainstream market, and has the share of more than 90%; the thin film battery mainly comprises a cadmium telluride battery, a nanometer titanium dioxide dye sensitized battery, a copper indium gallium selenide battery, an amorphous silicon thin film battery, a gallium arsenide battery and the like. In recent years, with the continuous development of novel photovoltaic cell technology, a plurality of novel solar cells with better performance are emerging, including perovskite solar cells, quantum dot solar cells and the like, and the novel solar cells have great application potential in photovoltaic energy storage integrated devices.
The perovskite solar cell is a novel solar cell, can be processed by a solution method, and can be combined with a printing process, so that the manufacturing cost is obviously reduced. Meanwhile, the perovskite solar cell has the characteristics of light weight, thinness and small volume, and can be deposited on a flexible substrate to manufacture a flexible solar cell. In addition, the perovskite has strong absorption capacity and stability in a short-wave region, and is a good anti-radiation material. In recent years, perovskite solar cells have remarkable improvements in photoelectric conversion efficiency, preparation methods and device structures. However, the application of the perovskite solar cell is mostly concentrated in the civil photovoltaic market at present, and the application of the perovskite solar cell on the radiation resistance in the aerospace field is not expanded. Meanwhile, at present, research is mostly focused on the device level, research on a micro system applying the perovskite solar cell is not abundant enough, and particularly, a blank exists in the aspect of anti-irradiation application of a photovoltaic energy storage integrated device based on the perovskite solar cell. The device is crucial to realizing the integration of aerospace energy supply and storage with high reliability and low cost.
The patent with the application number of 201720427036.7 discloses a solar photovoltaic power generation and energy storage integrated device which comprises an energy box, a solar photovoltaic assembly plate and a grid-connected inverter. The solar photovoltaic power generation and energy storage integrated device can effectively improve the photovoltaic power generation utilization rate and save the electricity consumption of the traditional municipal power. However, the device has four defects, namely the device has no anti-radiation capability, is only suitable for civil use and cannot meet the requirements on the system in the space radiation environment; secondly, the photoelectric conversion efficiency of the solar cell used by the device is not high enough, which is not beneficial to the energy collection and storage of the whole photovoltaic energy storage device; thirdly, the solar cell used by the device is not light enough, and when the device is applied to a spacecraft, the load of the spacecraft can be increased, so that the device is not beneficial to long-time use; and fourthly, the solar cell used by the device is not beneficial to reducing the system cost.
In the patent application No. 201810933139.X, there is disclosed an anti-radiation solar cell comprising, from top to bottom, a conductive glass electrode layer, an electron transport layer, a perovskite photoactive layer and a carbon electrode. Experimental test results show that the photoelectric performance of the perovskite solar cell after irradiation is not seriously damaged, and the photoelectric conversion efficiency is almost the same as that before irradiation. The cynanchum paniculatum and the like propose a method based on PEN/ITO/SnO in the literature' influence of gamma ray irradiation on flexible perovskite solar cell 2 /FA 0.945 MA 0.025 Cs 0.03 Pb(I 0.975 Br 0.025 ) 3 Perovskite solar cell with/Spiro-OMeTAD/Ag planar heterojunction structureThe research on gamma ray irradiation proves that the perovskite structure has better irradiation resistance and better application prospect in the field of space. However, the two studies on perovskite do not further regulate and control the perovskite components, and an encapsulation layer is not prepared, so that the stability is poor, and the long-term application of the perovskite in space equipment is not facilitated.
Disclosure of Invention
The invention aims to provide an anti-irradiation photovoltaic energy storage integrated device and a preparation method thereof aiming at the defects of the prior art, so as to improve the photoelectric conversion efficiency and the anti-irradiation capability, reduce the cost and the weight and realize the long-term stable power supply of space equipment in the whole time.
The technical scheme of the invention is realized as follows:
1. the utility model provides an anti irradiation photovoltaic energy storage integrated device, includes solar module 1, stabiliser 2, charge and discharge management subassembly 3 and energy storage battery 4, and stabiliser 2 is connected between solar module 1's output and an input port of charge and discharge management subassembly 3, and the two-way port of input and output of charge and discharge management subassembly 3 meets with the two-way port of input and output of energy storage battery 4, solar module 1 comprises a plurality of perovskite solar cell, and every perovskite solar cell includes transparent conductive substrate 11, electron transport layer 12, light-absorbing layer 13, hole transport layer 14 and metal electrode 15, its characterized in that:
each perovskite solar cell is provided with a double-layer packaging structure 16 for isolating external water and oxygen from entering, protecting the light absorption layer 13 from being corroded and decomposed by water and oxygen and improving the long-term stability of the whole device;
the light absorption layer 13 is made of a three-dimensional perovskite and two-dimensional perovskite composite material so as to improve the long-term stability and the photoelectric conversion efficiency of the material, and the thickness of the light absorption layer is 150-550nm;
the double-layer packaging structure 16 comprises an insulating protection layer 161, a filling protection layer 162, a back plate 163, packaging glue 164 and an interconnection line 165, wherein the insulating protection layer 161, the filling protection layer 162 and the back plate 163 are sequentially stacked above the metal electrode 15, the packaging glue 164 wraps the periphery of all layers between the transparent conductive substrate 11 and the back plate 163, and the interconnection line 165 is respectively led out of the solar cell from the transparent conductive substrate 11 and the metal electrode 15 and is used for completing interconnection between perovskite solar cells;
the metal halide packaging box 5 is arranged outside the voltage stabilizer 2, the charge and discharge management assembly 3 and the energy storage battery 4 and used for eliminating external irradiation;
the metal halide packaging box 5 is formed by bonding six metal halide packaging plates 51 through epoxy resin, each metal halide packaging plate 51 comprises a glass substrate 511, a metal halide layer 512, an inorganic insulating protective layer 513 and a protective packaging adhesive 514 from top to bottom, and the metal halide packaging plate 51 is provided with a through hole 515 used as a wiring channel inside and outside the packaging box.
Further, the perovskite solar cell comprises a positive structure and an inverted structure;
the positive structure comprises a transparent conductive substrate 11, an electron transport layer 12, a light absorption layer 13, a hole transport layer 14, a metal electrode 15 and a double-layer packaging structure 16 from bottom to top;
the inverted structure comprises a transparent conductive substrate 11, a hole transport layer 14, a light absorption layer 13, an electron transport layer 12, a metal electrode 15 and a double-layer packaging structure 16 from bottom to top.
Further, the light absorbing layer 13 material is a three-dimensional perovskite having a molecular formula ABX 3 The different ions in (2) are selected as follows:
positive monovalent cation A, methylamine MA is selected + Formamidine FA + Potassium, K + Rb, rb + Cesium Cs + Any one kind of ion and any combination of several kinds of ions;
a positive divalent metal cation B selected from lead Pb 2+ Germanium Ge 2+ Tin Sn 2+ Any one kind of ion and any combination of several kinds of ions;
a monovalent anion X selected from chlorine Cl - Bromine Br - Iodine I - Any one kind of ion and any combination of several kinds of ions.
Further, the light absorptionTwo-dimensional perovskite of formula A in the material of layer 13 1 2 A n-1 B n X 3n+1 Or A 2 A n-1 B n X 3n+13 The different ions in (1) are selected as follows:
the three ions of positive univalent cations A, positive divalent metal cations B and negative univalent anions X are selected as the three-dimensional perovskite;
monovalent organic cation A 1 Selecting phenylethylamine PEA + Butylamine BA + Ethylamine EA + Dimethylamine DMA + Methyltriethylammonium MTEA + 2-Thienylmethylammonium ThMA + Any one kind of ion and any combination of several kinds of ions;
positive divalent organic cation A 2 3-aminomethylpiperidine 3AMP is selected 2+ 4-Aminomethylpiperidine 4AMP 2+ 3-aminomethylpyridine 3AMPY 2+ 4-aminomethylpyridine 4AMPY 2+ EDA, ethylenediamine 2+ DPA of N, N-dimethylaniline 2+ Propane 1, 3-diammonium PDA 2+ 1, 4-butanediamine BDA 2+ 2, 5-diaminomethylthiophene ThDMA 2+ P-xylylenediamine PDMA 2+ N, N-dimethylethylenediamine DMDEA 2+ Any one kind of ion and any combination of several kinds of ions.
Further, the metal halide layer 512 is made of perovskite or lead halide, wherein the perovskite is selected in the same manner as the light absorbing layer 3, and the lead halide comprises lead fluoride PbF 2 Lead chloride PbCl 2 Lead bromide PbBr 2 And lead iodide PbI 2 One or more of the above;
further, the inorganic insulating protective layer 513 is made of alumina Al 2 O 3 Silicon dioxide SiO 2 Zirconium dioxide ZrO 2 Molybdenum trioxide, moO 3 Silicon nitride Si 3 N 4 Any one or any combination thereof;
further, the protective packaging adhesive 514 is any one or any combination of butyl adhesive, silica gel, thermoplastic polymer material, ultraviolet curing adhesive or AB component adhesive.
2. The preparation method of the anti-irradiation photovoltaic energy storage integrated device is characterized by comprising the following steps of:
1) Preparing a perovskite solar cell:
2) Carrying out double-layer packaging on the perovskite solar cell:
2a) Selecting a metal lead or a conductive adhesive tape or a metal foil as an interconnection line, and fixing the interconnection line on a transparent conductive substrate and a metal electrode of the prepared solar cell to be used as a reserved wiring port;
2b) Selecting an insulating protective layer material, a filling protective layer material and packaging glue, manufacturing an insulating protective layer on the solar cell with a reserved wiring port by using a magnetron sputtering or Atomic Layer Deposition (ALD) or thermal evaporation method, laying a layer of filling protective layer material above the insulating protective layer, ensuring that an interconnection line connected with a metal electrode penetrates through the filling protective layer, filling the packaging glue around the perovskite solar cell with the filling protective layer, and ensuring that all the interconnection lines penetrate through the packaging glue to obtain the perovskite solar cell with the packaging glue;
2c) Selecting a back plate, turning the perovskite solar cells with the packaging glue up and down by one hundred eighty degrees, placing the perovskite solar cells on the back plate, arranging a plurality of perovskite solar cells with the packaging glue on the back plate into an array according to the method, and ensuring that all interconnection lines pass through the back plate to reach the outside of the packaging layer to obtain a stacked perovskite solar cell array;
2d) And (3) placing the stacked perovskite solar cell array into a heating plate of a heated laminating machine for laminating to obtain a laminated perovskite solar cell array, and taking out and cooling the laminated perovskite solar cell array to obtain the double-layer packaged perovskite solar cell array.
3) Carrying out series-parallel connection on interconnection lines of the double-layer packaged perovskite solar cell array according to actual requirements to obtain a double-layer packaged perovskite solar cell module;
4) The voltage stabilizer, the charge and discharge management assembly and the energy storage battery are connected through a wire and packaged by a metal halide packaging box:
4a) Preparing a metal halide packaging plate:
4a1) Taking a glass substrate which is reserved with a through hole according to actual requirements;
4a2) Selecting a metal halide material, and coating the metal halide solution on a glass substrate by a solution coating method to obtain a prepared metal halide layer;
4a3) Selecting an inorganic insulating protective layer material, and preparing an inorganic insulating protective layer on the metal halide layer by using an atomic deposition method or a thermal evaporation method to obtain a prepared inorganic insulating protective layer;
4a4) Selecting a protective packaging adhesive material, preparing a layer of protective packaging adhesive on the insulating protective layer by adopting a solution coating method, and curing the protective packaging adhesive to obtain a metal halide packaging plate;
4b) Connecting the voltage stabilizer, the charge and discharge management assembly and the energy storage battery, and manufacturing a metal halide packaging box to finish packaging:
selecting a voltage stabilizer, a charge and discharge management assembly and an energy storage battery, connecting an output port of the voltage stabilizer with an input port of the charge and discharge management assembly through a wire, connecting an input and output bidirectional port of the charge and discharge management assembly with an input and output bidirectional port of the energy storage battery, respectively connecting the input port of the voltage stabilizer and the output port of the charge and discharge management assembly with the wire, then penetrating through a through hole of a metal halide packaging layer, then forming a metal halide packaging box by six metal halide packaging plates outside the voltage stabilizer, the charge and discharge management assembly and the energy storage battery, ensuring that a glass substrate faces outwards and is bonded by epoxy resin, and obtaining a packaged and connected external device;
5) And connecting an input port of a voltage stabilizer in the packaged and connected external device to an output end of the double-layer packaged perovskite solar cell module to obtain the anti-irradiation photovoltaic energy storage integrated device.
Compared with the prior art, the invention has the following advantages:
firstly, the perovskite solar cell and the energy storage cell are integrated, and the utilization efficiency of solar energy is effectively improved. When the solar battery generates surplus or insufficient electric energy, the storage and continuous power supply of electric quantity can be ensured through the charging and discharging of the energy storage battery.
Secondly, the solar cell adopted by the invention uses perovskite as a light absorption layer. The perovskite material has the advantages of strong irradiation resistance, high light absorption coefficient, long carrier diffusion length and high mobility, and the perovskite solar cell prepared from the perovskite material can obtain high photoelectric conversion efficiency and has the characteristics of small volume and light weight. The integrated device is well applied to a power supply system in irradiation environments such as aerospace and the like.
Thirdly, the perovskite solar cell adopted by the invention has low preparation cost and simple preparation process, can effectively reduce the cost of the integrated device, is favorable for expanding the application range and the scene, and is particularly favorable for reducing the cost expenditure of an aerospace power supply system.
Fourthly, the metal halide material is used as the anti-irradiation metal halide packaging box to protect all parts except the solar cell in the device, and the excellent anti-irradiation capability is obtained at extremely low cost, so that the stability of the integrated device is well improved.
Fifth, the invention adopts the double-layer packaging layer to isolate the external water and oxygen from entering, protects the light absorption layer from being corroded and decomposed by water, and uses the composite material of the two-dimensional perovskite and the three-dimensional perovskite as the light absorption layer, thereby improving the environmental stability of the light absorption layer and ensuring high long-term stability and reliability.
Drawings
FIG. 1 is a system diagram of an integrated radiation-resistant photovoltaic energy storage device according to the present invention;
FIG. 2 is a schematic structural view of a single perovskite solar cell of the present invention in a face-up configuration;
FIG. 3 is a schematic diagram of a single perovskite solar cell of the present invention with an inverted structure;
FIG. 4 is a schematic view of a metal halide enclosure of the present invention;
FIG. 5 is a general flow chart of the present invention for preparing an integrated radiation-resistant photovoltaic energy storage device;
FIG. 6 is a sub-flow diagram of the present invention for making a single perovskite solar cell of a front-up configuration;
fig. 7 is a sub-flow diagram of the present invention for fabricating a single perovskite solar cell of an inverted structure.
Detailed Description
The invention is further described below with reference to the accompanying drawings and examples.
Referring to fig. 1, the anti-irradiation photovoltaic energy storage integrated device of the invention comprises a solar cell module 1, a voltage stabilizer 2, a charging and discharging management assembly 3, an energy storage cell 4 and a metal halide packaging box 5. The solar battery module 1 has an output port, the voltage stabilizer 2 has an output port and an input port, the charge and discharge management assembly 3 has an output port, an input port and an input and output bidirectional port, and the energy storage battery 4 has an input and output bidirectional port. The output port of the charge/discharge management module 3 is not connected to any module in the apparatus, and functions as an output port of the entire apparatus. The voltage stabilizer 2 is connected between the output end of the solar battery module 1 and an input port of the charge and discharge management assembly 3, and an input and output bidirectional port of the charge and discharge management assembly 3 is connected with an input and output bidirectional port of the energy storage battery 4. The voltage stabilizer 2, the charging and discharging management assembly 3 and the energy storage battery 4 are placed in the metal halide packaging box 5, and input port wiring of the voltage stabilizer 2 and output port wiring of the charging and discharging management assembly 3 respectively penetrate through the metal halide packaging box 5.
The solar cell module 1 is formed by arranging a plurality of perovskite solar cells according to actual requirements and connecting the perovskite solar cells in series and parallel, and each perovskite solar cell can be of an upright structure or an inverted structure at will.
The energy storage battery 4 is one of a lithium battery, a sodium battery and a nickel battery.
Referring to fig. 2, the single perovskite solar cell of the front-mounted structure includes, from bottom to top, a transparent conductive substrate 11, an electron transport layer 12, a light absorption layer 13, a hole transport layer 14, a metal electrode 15, and a double-layered encapsulation structure 16; the double-layer packaging structure comprises an insulating protection layer 161, a filling protection layer 162, a back plate 163, packaging glue 164 and an interconnection line 165, wherein the insulating protection layer 161, the filling protection layer 162 and the back plate 163 are sequentially stacked above the metal electrode 15, the packaging glue 164 wraps the periphery of all layers between the transparent conductive substrate 11 and the back plate 163, and the interconnection line 165 is led out to the outside of the solar cell from the transparent conductive substrate 11 and the metal electrode 15 respectively and is used for completing interconnection between perovskite solar cells.
The transparent conductive substrate 11 is made of an Indium Tin Oxide (ITO) material or a fluorine-doped tin oxide (FTO) material with the thickness of 300-800 nm.
The electron transport layer 12 is made of titanium dioxide (TiO) 2 Zinc oxide ZnO, tin dioxide SnO 2 、C 60 、[6,6]-phenyl radical C 61 Any one of methyl butyrate with the thickness of 70-150nm.
The light absorption layer 13 is made of a composite material of three-dimensional perovskite and two-dimensional perovskite, and the thickness is 150-550nm.
The three-dimensional perovskite has a molecular formula ABX 3 Selecting different ions, wherein:
a monovalent cation A, methylamine MA is selected + Formamidine FA + Potassium, K + Rubidium Rb + Cesium Cs + Any one kind of ion and any combination of several kinds of ions in the ion;
positive divalent metal cation B, lead Pb 2+ Germanium Ge 2+ Tin Sn 2+ Any one kind of ion and any combination of several kinds of ions;
a monovalent anion X selected from chlorine Cl - Bromine Br - Iodine I - Any one kind of ion and any combination of several kinds of ions.
The two-dimensional perovskite being of the formula A 1 2 A n-1 B n X 3n+1 Or A 2 A n-1 B n X 3n+13 Selecting different ions, wherein:
the three ions of positive univalent cation A, positive divalent metal cation B and negative univalent anion X are selected as the three-dimensional perovskite;
monovalent organic cation A 1 Selecting phenylethylamine PEA + Butylamine BA + Ethylamine EA + Dimethylamine DMA + Methyltriethylammonium MTEA + 2-Thienylmethylammonium ThMA + Any one kind of ion and any combination of several kinds of ions;
a divalent organic cation A 2 3-aminomethyl piperidine 3AMP is selected 2+ 4-Aminomethylpiperidine 4AMP 2+ 3-aminomethylpyridine 3AMPY 2+ 4-aminomethylpyridine 4AMPY 2+ EDA, ethylenediamine 2+ DPA of N, N-dimethylaniline 2+ Propane 1, 3-diammonium PDA 2+ 1, 4-butanediamine BDA 2+ 2, 5-diaminomethylthiophene ThDMA 2+ P-xylylenediamine (PDMA) 2+ N, N-dimethylethylenediamine DMDEA 2+ Any one kind of ion and any combination of several kinds of ions.
The hole transport layer 14, which uses triphenylamine derivatives, 2, 7-tetrakis [ N, N-bis (4-methoxyphenyl) amino ] -9, 9-spirobifluorene Spiro-OMeTAD, poly 3, 4-ethylenedioxythiophene, polystyrene sulfonate PEDOT: PSS, poly (3-hexylthiophene) P3HT, 2,3,5, 6-tetrafluoro-7, 8-tetracyanodimethane-doped polytriazoloamine PTAA: F4-TCNQ, poly [ bis (4-phenyl) (2, 4, 6-trimethylphenyl) amine ] PTAA, cuprous thiocyanate CuSCN and nickel oxide NiO, wherein the thickness of the mixture is 50-200nm.
The metal electrode 15 is made of any one of gold Au, silver Ag, copper Cu and carbon electrodes, and the thickness of the metal electrode is 90-300nm.
The insulating protective layer 161 is made of alumina Al 2 O 3 Silicon dioxide SiO 2 Zirconium dioxide ZrO 2 Molybdenum trioxide, moO 3 Silicon nitride Si 3 N 4 Any one or any combination thereof.
The filling protection layer 162 is made of any one or any combination of polyethylene octene co-elastomer, ethylene-vinyl acetate copolymer, polyvinyl butyral, organic silicon resin and epoxy resin.
The back plate 163 is made of any one of ultra-white glass, tempered glass, soda-lime glass, a metal substrate, or a fluorine-containing flexible substrate.
The periphery packaging adhesive 164 is any one or any combination of butyl adhesive, silica gel, thermoplastic polymer material, ultraviolet curing adhesive or AB component adhesive.
The interconnecting wire 165 is made of any one or any combination of a metal wire, a conductive tape or a metal foil, wherein the metal wire or the metal foil is made of one of gold Au, silver Ag, copper Cu and aluminum Al.
Referring to fig. 3, the single perovskite solar cell of the inverted structure includes, from bottom to top, a transparent conductive substrate 11, a hole transport layer 14, a light absorbing layer 13, an electron transport layer 12, a metal electrode 15, and a double-layered encapsulation structure 16; the double-layer packaging structure 16 comprises an insulating protection layer 161, a filling protection layer 162, a back plate 163, packaging glue 164 and an interconnection line 165, and the connection relation and the position of each layer in the double-layer packaging structure 16 are the same as those of the upright structure; the range and thickness of the materials of all layers in the single perovskite solar cell with the inverted structure are the same as those of the positive structure.
Referring to fig. 4, the metal halide package box 5 is formed by bonding six metal halide package plates 51 through epoxy resin, each metal halide package plate 51 includes, from top to bottom, a glass substrate 511, a metal halide layer 512, an inorganic insulating protective layer 513 and a protective package adhesive 514, and the metal halide package plate 51 is provided with a through hole 515 for serving as a routing channel inside and outside the package box.
The metal halide layer 512 is made of perovskite or lead halide, wherein the perovskite is selected in the same way as the light absorbing layer 3, and the lead halide comprises lead fluoride PbF 2 Lead chloride PbCl 2 Lead bromide PbBr 2 And lead iodide PbI 2 One or more of them.
The inorganic insulating protective layer 513 is made of alumina Al 2 O 3 Silicon dioxide SiO 2 Zirconium dioxide ZrO 2 Molybdenum trioxide, moO 3 Silicon nitride Si 3 N 4 Any one or any combination thereof.
The protective packaging adhesive 514 is any one or any combination of butyl adhesive, silica gel, thermoplastic polymer material, ultraviolet curing adhesive or AB component adhesive.
Referring to fig. 5, three examples of the method for preparing the irradiation-resistant integrated photovoltaic energy storage device according to the present invention are shown below.
Example 1: MAPbI was used for preparing the light-absorbing layer 13 3 And (4 AMPY) MA n-1 Pb n I (3n-1)(1-y) Cl (3n-1)y The metal halide layer 512 is lead chloride PbCl 2 The perovskite solar cell is of a positive structure, and the anti-irradiation photovoltaic energy storage integrated device is based on the solar cell module.
Step 1, preparing a positive solar cell.
Referring to fig. 6, the specific implementation of this step is as follows:
1.1 A transparent conductive substrate is selected and pretreated:
1.1.1 Indium Tin Oxide (ITO) with the thickness of 400nm is selected as a transparent conductive substrate;
1.1.2 Respectively ultrasonically cleaning the selected substrate for 20min at 50 ℃ by using glass cleaning solution, deionized water, acetone, isopropanol solution and deionized water in sequence;
1.1.3 The ultrasonically cleaned substrate was blow-dried on the glass surface using nitrogen gas, and the glass surface was irradiated with ultraviolet ozone for 20 minutes to obtain a pretreated transparent conductive substrate.
1.2 Preparation of electron transport layers for perovskite solar cells:
in a glove box first 20mg of [6, 6' ]]-phenyl radical C 61 Methyl butyrate is dissolved in 1mL of chlorobenzene, the chlorobenzene is stirred for 8 hours by a magnetic stirring table to be fully dissolved, the solution is uniformly dripped on a substrate by using a spin coater, and the prepared electron transport layer with the thickness of 170nm is obtained by spin coating for 42s at the rotating speed of 2000 rpm.
1.3 Preparation of perovskite light-absorbing layers:
1.3.1 Prepared perovskite precursor solution according to dimethylsulfoxide DMSO γ -hydroxybutyrate lactone GBL =3:7, preparing a mixed solvent, and after mixing, slightly shaking to fully mix the mixed solvent;
1.3.2 215mg of MAI was dissolved in the above 1mL of the mixed solvent to obtain a MAI solution, 640mg of MAI solution was addedLead iodide PbI 2 Mixing with 1mL of MAI solution, heating at 75 deg.C and stirring to dissolve completely to obtain MAPbI 3 A solution; 0.06mmol of 4-aminomethylpyridine chloride (4 AMPY) Cl 2 The powder was dissolved in 1mL of DMSO to give 4-aminomethylpyridinium chloride (4 AMPY) Cl 2 Precursor solution;
1.3.3 The prepared solution is placed on a hot table to be heated at 60 ℃, spin-coated for 20s at the rotating speed of 1000rpm, accelerated to 4000rpm and then spin-coated for 30s, toluene is dropwise added when the total time is 30s, and then the solution is placed on a hot table at 100 ℃ to be annealed for 20min to obtain MAPbI 3 A film;
1.3.4 ) then at 6000rpm in the prepared MAPbI 3 100ml of 4-aminomethyl pyridinium chloride (4 AMPY) Cl was spin-coated on the film 2 Precursor solution is annealed for 10min at the temperature of 100 ℃ for 40s to obtain MAPbI 3 And (4 AMPY) MA n- 1 Pb n I (3n-1)(1-y) Cl (3n-1)y A mixed perovskite light absorbing layer.
1.4 Preparation of hole transport layers for perovskite solar cells:
1.4.1 170mg of lithium bis (trifluoromethanesulfonyl) imide Li-TFSI powder is dissolved in 1mL of acetonitrile solution to obtain a Li-TFSI solution; dissolving 1.014g of tert-butylpyridine tBP powder in 1mL of acetonitrile solution to obtain a tBP solution; dissolving 11.27g of Co (III) complex FK209 powder in 1mL of acetonitrile solution to obtain a Co (III) complex FK209 solution;
1.4.2 90mg of 2, 7-tetrakis [ N, N-bis (4-methoxyphenyl) amino ] -9, 9-spirobifluorene Spiro-OMeTAD powder, 45. Mu.L of Li-TFSI solution, 10. Mu.L of tBP solution, and 75. Mu.L of Co (III) complex FK209 solution were Co-dissolved in 1mL of chlorobenzene to give a2, 7-tetrakis [ N, N-bis (4-methoxyphenyl) amino ] -9, 9-spirobifluorene Spiro-OMeTAD solution;
1.4.3 Spin coating the prepared Spiro-OMeTAD solution on the perovskite light absorption layer by adopting spin coater equipment, firstly spin coating for 12s at the speed of 1000rpm, and then spin coating for 30s at the speed of 4000rpm to obtain the hole transport layer.
1.5 Preparation of metal electrodes for perovskite solar cells:
under the condition of vacuum degree of a chamber being 10 -5 Pa or less, at 1.1
Figure BDA0003005818470000101
And (4) evaporating 100nm silver Ag at a speed of/s to obtain a metal electrode, and finishing the preparation of the positive perovskite solar cell.
Step 2, carrying out double-layer packaging on the perovskite solar cell:
2.1 Copper Cu leads are selected as interconnection wires and fixed on a transparent conductive substrate and a metal electrode of the prepared positive solar cell to be used as reserved wiring ports;
2.2 By magnetron sputtering of 210nm of silicon dioxide SiO on the back electrode of the prepared solar cell 2 Obtaining the positive perovskite solar cell with the insulating protective layer;
2.3 0.9mm of polyethylene octene co-elastomer is selected as a filling protective layer, butyl rubber is used as packaging rubber, and 1mm of ultra-white glass is used as a back plate;
2.4 A layer of filling protective layer material is laid above the insulating protective layer, the interconnection lines connected with the metal electrodes are ensured to pass through the filling protective layer, the periphery of the positive perovskite solar cell filled with the protective layer is filled with packaging glue, and all the interconnection lines are ensured to pass through the packaging glue, so that the perovskite solar cell with the packaging glue is obtained;
2.5 The positive perovskite solar cells with the packaging glue are placed on the back plate after being turned over for 180 degrees up and down, then a plurality of positive perovskite solar cells with the packaging glue are arranged on the back plate to form an array according to the method, and all interconnection lines are ensured to pass through the back plate to reach the outside of the packaging layer, so that the stacked positive perovskite solar cell array is obtained;
2.6 The stacked positive perovskite solar cell array is placed into a heating plate of a laminating machine which is heated to 90 ℃ for lamination to obtain a laminated perovskite solar cell array, and then the laminated perovskite solar cell array is taken out and cooled to obtain a double-layer packaged positive perovskite solar cell array.
And 3, completing the connection in the perovskite solar cell module.
Connecting the interconnection lines of the double-layer packaged positive perovskite solar cell array in series and parallel according to actual requirements to obtain a double-layer packaged perovskite solar cell module;
step 4, connecting the voltage stabilizer, the charge and discharge management assembly and the energy storage battery through a lead, and packaging the voltage stabilizer, the charge and discharge management assembly and the energy storage battery by using a metal halide packaging box:
4.1 Preparation of metal halide package panels:
4.1.1 Taking a glass substrate with a through hole reserved according to actual requirements;
4.1.2 Preparing a metal halide precursor solution and preparing a metal halide layer by a blade coating method;
0.5mmol of lead chloride PbCl is taken 2 Dissolving in 1mL dimethyl sulfoxide DMSO solution, heating and stirring at 75 ℃ until the solution is completely dissolved to obtain lead chloride PbCl 2 Precursor solution, and preparing the metal halide layer by adopting a blade coating method.
4.1.3 By atomic layer deposition of a layer of Si on a metal halide layer 3 N 4 An insulating protective layer;
4.1.4 By knife coating on Si 3 N 4 Preparing a layer of ultraviolet curing adhesive on the insulating protective layer, and irradiating the ultraviolet curing adhesive under ultraviolet to cure the ultraviolet curing adhesive to obtain a metal halide packaging plate;
4.2 Selecting an energy storage battery, connecting the voltage stabilizer, the charging and discharging management assembly and the energy storage battery, and manufacturing a metal halide packaging box to finish packaging:
4.2.1 The energy storage battery is a nickel battery;
4.2.2 Connecting a voltage stabilizer, a charging and discharging management assembly and an energy storage battery, and manufacturing a metal halide packaging box to finish packaging:
connecting an output port of the voltage stabilizer with an input port of the charge and discharge management assembly through a wire, connecting an input and output bidirectional port of the charge and discharge management assembly with an input and output bidirectional port of the energy storage battery, respectively connecting the input port of the voltage stabilizer and the output port of the charge and discharge management assembly with the wire, then penetrating through a through hole of a metal halide packaging layer, then forming a metal halide packaging box by six metal halide packaging plates outside the voltage stabilizer, the charge and discharge management assembly and the energy storage battery, ensuring that the glass substrate faces outwards and is bonded by epoxy resin, and obtaining a packaged and connected external device;
and 5, assembling the photovoltaic energy storage integrated device.
And connecting an input port of a voltage stabilizer in the packaged and connected external device to an output end of the double-layer packaged perovskite solar cell module to obtain the anti-irradiation photovoltaic energy storage integrated device.
Example 2: MAPbI was used for preparing the light-absorbing layer 13 3 And (4 AMPY) MA n-1 Pb n I (3n-1)(1-y) Cl (3n-1)y The metal halide layer 512 is lead chloride PbCl 2 The positive structure perovskite solar cell and the anti-irradiation photovoltaic energy storage integrated device based on the solar cell module.
Step one, preparing a positive solar cell.
Referring to fig. 6, the specific implementation of this step is as follows:
1a) Selecting a transparent conductive substrate, and carrying out pretreatment on the transparent conductive substrate:
1a1) Indium Tin Oxide (ITO) with the thickness of 450nm is selected as a transparent conductive substrate;
1a2) The selected substrate is pretreated in the same manner as in steps 1.1.2) and 1.1.3) of example 1;
1b) Preparing an electron transport layer of the perovskite solar cell:
1b1) 0.2mol/L of titanium dioxide TiO 2 The solution is coated on an Indium Tin Oxide (ITO) substrate in a spinning mode for 45s at the speed of 4000rpm, and then annealing is carried out for 5min at the temperature of 125 ℃;
1b2) 0.4mol/L of titanium dioxide TiO 2 Spin coating the solution on the substrate obtained in 1b 1) at 4000rpm for 45s, and then annealing at 125 ℃ for 5min;
1b3) After repeating the step 1b 2) twice, annealing the obtained substrate at 450 ℃ for 15min;
1b4) After the substrate obtained in 1b 3) had cooled to room temperature, it was immersed in 40mmol/L titanium TiCl chloride at a temperature of 70 deg.C 4 Soaking in water solution for 45min, and annealing at 450 deg.C for 20min to obtain electron transfer materialConveying a layer;
1b5) 1, 0mg, 6]-phenyl radical C 61 Methyl butyrate was dissolved in 1mL chlorobenzene to give PC 61 And (3) carrying out spin coating on the BM solution at the speed of 6000rpm for 45s above the prepared electron transport layer, and then annealing at the temperature of 100 ℃ for 5min to obtain the passivated electron transport layer.
1c) Preparing a perovskite light absorption layer:
1c1) 1mmol of PbBr 2 The powder was dissolved in 1mL dimethylsulfoxide DMSO and stirred at 75 deg.C for 8 hours to give PbBr 2 Precursor solution; then 0.42mmol CsBr powder is dissolved in 6mL DMSO to obtain CsBr precursor solution;
1c2) Spin-coating PbBr on the prepared electron transmission layer at 2000rpm by spin coater 2 Precursor solution is annealed for 60min at 90 ℃ for 30s to obtain PbBr 2 A film; then the prepared PbBr is stirred at the rotating speed of 2000rpm 2 Spin-coating CsBr precursor solution on the film for 30s, annealing at 250 ℃ for 5min, and repeating the steps for 3-8 times to obtain CsPbBr 3 A perovskite light absorbing layer.
1d) Preparing a hole transport layer of the perovskite solar cell:
1d1) Dissolving 2mg of poly [ bis (4-phenyl) (2, 4, 6-trimethylphenyl) amine ] PTAA in 1ml of toluene to obtain a solution of poly [ bis (4-phenyl) (2, 4, 6-trimethylphenyl) amine ] PTAA;
1d2) Spin-coating poly [ bis (4-phenyl) (2, 4, 6-trimethylphenyl) amine ] PTAA solution on the prepared perovskite light absorption layer for 30s at the rotating speed of 3000rpm by adopting spin coater equipment, and then annealing at the temperature of 90 ℃ for 30min to obtain a hole transport layer with the thickness of 160 nm.
1e) Preparing a metal electrode of the perovskite solar cell:
under the condition of vacuum degree of the chamber being 10 -5 Pa below, 1.8
Figure BDA0003005818470000121
And (3) evaporating gold Au with the thickness of 140nm at the speed of/s to obtain a metal electrode, thereby completing the preparation of the positive perovskite solar cell.
Step two, carrying out double-layer packaging on the perovskite solar cell:
2a) Selecting a gold foil as an interconnection line, and fixing the gold foil on a transparent conductive substrate and a metal electrode of the prepared positive solar cell to be used as a reserved wiring port;
2b) 160nm of aluminum oxide Al is formed on the back electrode of the prepared solar cell through magnetron sputtering 2 O 3 Obtaining the positive perovskite solar cell with the insulating protective layer;
2c) 1mm of organic silicon resin is selected as a filling protective layer, a thermoplastic high polymer material is packaging glue, and 1mm of soda-lime glass is used as a back plate;
2d) Preparing a filling protective layer and packaging glue on the insulating protective layer:
the specific implementation of this step is the same as step 2.4) in example 1.
2e) Arranging a perovskite solar cell array on a back sheet:
the specific implementation of this step is the same as step 2.5) in example 1.
2f) Laminating and cooling the perovskite solar cell array:
the specific implementation of this step is the same as step 2.6) in example 1.
And step three, completing the connection in the perovskite solar cell module.
The specific implementation of this step is the same as step 3 in example 1.
And step four, connecting the voltage stabilizer, the charge-discharge management assembly and the energy storage battery through a lead, and packaging the voltage stabilizer, the charge-discharge management assembly and the energy storage battery by using a metal halide packaging box.
4a) Preparing a metal halide packaging plate:
4a1) Taking a glass substrate which is reserved with a through hole according to actual requirements;
4a2) Preparing metal halide precursor solution and preparing metal halide layer by slit coating method, i.e. taking 1mmol BAI powder and 0.5mmol PbI 2 Dissolving the powder in 0.9mml mixed solution of dimethyl sulfoxide DMSO and 0.1ml dimethyl formamide DMF, heating and stirring at 75 deg.C until completely dissolving to obtain BA 2 PbI 4 Perovskite precursor solution, then adopting slit typePreparing a metal halide layer by a coating method;
4a3) Depositing a layer of aluminum oxide Al on a metal halide layer by atomic layer deposition 2 O 3 An insulating protective layer;
4a4) Applying a blade coating method on aluminum oxide Al 2 O 3 Preparing a layer of thermoplastic polymer material on the insulating protective layer, and curing the thermoplastic polymer material to obtain a metal halide packaging plate;
4b) Selecting an energy storage battery, connecting the voltage stabilizer, the charging and discharging management assembly and the energy storage battery, and manufacturing a metal halide packaging box to finish packaging:
4b1) Selecting a nickel battery as an energy storage battery;
4b2) Connecting the voltage stabilizer, the charge-discharge management assembly and the energy storage battery, and manufacturing a metal halide packaging box to complete packaging:
the specific implementation in this step is the same as step 4.2.2) in example 1.
And fifthly, assembling the photovoltaic energy storage integrated device.
The specific implementation in this step is the same as step 5 in example 1.
Example 3: preparation of the light-absorbing layer 13 with MAPbI 3 And (PEA) 2 MA n-1 Pb n I (3n-1)(1-y) Cl (3n-1)y The metal halide layer 512 adopts MAPbI 3 The perovskite solar cell with the inverted structure and the anti-irradiation photovoltaic energy storage integrated device based on the solar cell module are disclosed.
And step A, preparing the inverted solar cell.
Referring to fig. 7, the specific implementation of this step is as follows:
a1 A transparent conductive substrate is selected and pretreated:
a11 Fluorine-doped tin oxide FTO with the thickness of 450nm is selected as a transparent conductive substrate;
a12 ) pre-treatment of the selected substrate, the procedure being the same as in steps 1.1.2) and 1.1.3) of example 1;
a2 Preparation of hole transport layers for perovskite solar cells:
a21 In magnetism12.885g of NiCl are stirred vigorously 2 ·6H 2 Dissolving O in 100mL of deionized water, dropwise adding 10M NaOH solution until the pH value reaches 10, centrifuging the obtained turbid green solution, washing the precipitate with deionized water twice, and drying the powder at 80 ℃ to obtain NiO x A nanoparticle;
a22 150mgNiO was added x The nanoparticles were added to 5mL of isopropanol, and the mixed liquid was then sonicated in an ultrasonic cleaner at a power of 100W for a total duration of about 8 hours. Filtering the obtained solution through a polytetrafluoroethylene TPFE filter of 0.45 um;
a23 The obtained solution was spin-coated on a pretreated fluorine-doped tin oxide FTO substrate at 2000rpm for 30s using a spin coating method, and then annealed at 120 ℃ for 20min to obtain a prepared hole transport layer.
A3 Preparation of perovskite light-absorbing layers:
a31 Prepared perovskite precursor solution according to dimethylsulfoxide DMSO γ -hydroxybutyrate lactone GBL =3:7 preparing a mixed solvent according to the volume ratio;
a32 215mg of MAI is dissolved in the 1mL of mixed solvent to obtain MAI solution; 640mg of 461 lead iodide PbI is taken 2 Mixing with 1mL of MAI solution, heating at 75 deg.C and stirring to dissolve completely to obtain MAPbI 3 A solution;
a33 24.9mg of phenethyl amine iodide PEAI powder is dissolved in 1ml of isopropanol IPA solvent to obtain PEAI solution;
a34 Prepared MAPbI) 3 Heating the solution on a hot table at 60 ℃, spin-coating the solution at the rotating speed of 1000rpm for 20s, then accelerating to 4000rpm, spin-coating the solution for 30s, dropwise adding toluene when the total time is 30s, and then placing the solution on a hot table at 100 ℃ for annealing for 20min to obtain a three-dimensional perovskite layer;
a35 100ml of PEAI solution is spin-coated on the three-dimensional perovskite layer at a rotation speed of 4000rpm for 20s and then annealed at a temperature of 90 ℃ for 10min to obtain MAPbI 3 And (PEA) 2 MA n-1 Pb n I (3n-1)(1-y) Cl (3n-1)y A mixed perovskite light absorbing layer.
A4 Preparation of hole transport layers for perovskite solar cells:
a41 2.95g of zinc acetate powder is added into 125mL of methanol solution, the temperature is immediately raised to 70 ℃, and the mixture is continuously stirred to obtain transparent liquid A;
a42 1.48g of potassium hydroxide powder was dissolved in 65mL of a methanol solution at 70 ℃ and continuously stirred to obtain a mixed solution B;
a43 Dropwise adding the mixed solution B into the transparent solution A while stirring, stirring for 2h, standing to cool to room temperature, removing supernatant, washing the precipitate with methanol, adding 70mL of n-butanol, 5mL of methanol and 5mL of chloroform into the precipitate, stirring at constant speed, and filtering to obtain a zinc oxide nano particle solution;
a44 Zinc oxide nanoparticle solution was spin-coated on the pretreated transparent conductive substrate ITO at a rotation speed of 3000rmp for 30s, and the spin-coating was repeated three times to obtain a prepared electron transport layer 170nm thick.
A5 Preparation of metal electrodes for perovskite solar cells:
under the condition of vacuum degree of the chamber being 10 -5 Pa below, 1.8
Figure BDA0003005818470000151
And (3) evaporating copper Cu with the thickness of 140nm at the speed of/s to obtain a metal electrode, and finishing the preparation of the inverted perovskite solar cell.
And step B, carrying out double-layer packaging on the perovskite solar cell.
B1 Copper Cu foil is selected as an interconnection line and is fixed on a transparent conductive substrate and a metal electrode of the prepared inverted solar cell to be used as a reserved wiring port;
b2 Silicon nitride Si of 160nm by magnetron sputtering on the back electrode of the prepared solar cell 3 N 4 Obtaining the inverted perovskite solar cell with the insulating protective layer;
b3 1.1mm of polyvinyl butyral is selected as a filling protective layer, silica gel is used as packaging adhesive, and a 1.2mm metal substrate is used as a back plate;
b4 Preparing a filling protective layer and a packaging adhesive on the insulating protective layer:
the specific implementation of this step is the same as step 2.4) in example 1.
B5 Perovskite solar cell array on a back sheet:
the specific implementation of this step is the same as step 2.5) in example 1.
B6 Laminate and cool perovskite solar cell arrays:
the specific implementation of this step is the same as step 2.6) in example 1.
And C, completing the connection in the perovskite solar cell module.
The specific implementation of this step is the same as step 3 in example 1.
Step D, connecting the voltage stabilizer, the charge and discharge management assembly and the energy storage battery through a lead, and packaging the voltage stabilizer, the charge and discharge management assembly and the energy storage battery by using a metal halide packaging box:
d1 Preparation of metal halide package boards:
d11 Take a glass substrate with a through hole reserved according to actual requirements;
d12 Preparing a metal halide precursor solution and preparing a metal halide layer by a slit coating method, i.e., taking 1mmol MAI powder and 1mmol PbI powder 2 Dissolving the powder in a mixed solution of 0.9mml dimethyl sulfoxide DMSO and 0.1ml dimethylformamide DMF, heating and stirring at 75 ℃ until the powder is completely dissolved to obtain MAPbI 3 Preparing a metal halide layer by adopting a perovskite precursor solution and then adopting an ultrasonic spraying method;
d13 By atomic layer deposition of a layer of silicon dioxide SiO on a metal halide layer 2 An insulating protective layer;
d14 By knife coating on silicon dioxide SiO 2 Preparing a layer of AB component glue on the insulating protective layer, and curing the glue to obtain a metal halide packaging plate;
d2 Manufacturing a metal halide packaging box to complete packaging:
d21 Selecting a sodium battery as an energy storage battery;
d22 Connecting the voltage stabilizer, the charging and discharging management assembly and the energy storage battery in sequence, and manufacturing a metal halide packaging box to finish packaging:
the specific implementation in this step is the same as step 4.2.2) in example 1.
And E, assembling the photovoltaic energy storage integrated device.
The specific implementation in this step is the same as step 5 in example 1.
The foregoing description is only three specific examples of the present invention and is not intended to limit the invention in any way, and it will be apparent to those skilled in the art that, having the benefit of this disclosure, various modifications and changes in form and detail can be made without departing from the principles and arrangements of the invention, including, for example, the following materials in addition to those used in the three examples described above:
the electron transport layer: also comprises tin dioxide SnO 2 、C 60 ；
Three-dimensional perovskite material ABX in the light absorption layer 3 And a two-dimensional perovskite material A 1 2 A n-1 B n X 3n+1 、A 2 A n-1 B n X 3n+1 The selection scheme of various ions in (1):
monovalent cation A also includes formamidine FA + Potassium, K + Rb, rb + One or more of the above;
monovalent organic cation A 1 Also comprises butylamine BA + Ethylamine EA + Dimethylamine DMA + Methyltriethylammonium MTEA + 2-Thienylmethylammonium ThMA + One or more of the above;
positive divalent organic cation A 2 Also included is 3-aminomethylpiperidine 3AMP 2+ 4-Aminomethylpiperidine 4AMP 2+ 3-aminomethylpyridine 3AMPY 2+ EDA, ethylenediamine 2+ DPA of N, N-dimethylaniline 2+ Propane 1, 3-diammonium PDA 2+ 1, 4-butanediamine BDA 2+ 2, 5-diaminomethylthiophene ThDMA 2+ P-xylylenediamine (PDMA) 2+ N, N-dimethylethylenediamine DMDEA 2+ One or more of the above;
the positive divalent cation B also includes germanium Ge 2+ Sn, sn 2+ One or more of the above;
the hole transport layer: also included are triphenylamine derivatives, poly-3 hexylthiophene P3HT, poly (3-hexylthiophene) P3HT, 2,3,5, 6-tetrafluoro-7, 8-tetracyanodimethane-doped polytriazoloylamines PTAA: F4-TCNQ and cuprous thiocyanate CuSCN;
the metal electrode comprises carbon;
the inorganic insulating protective layer: also comprises zirconium dioxide ZrO 2 Molybdenum trioxide, moO 3 One or more of the above;
the filling protective layer: also comprises one or more of ethylene-vinyl acetate copolymer and epoxy resin;
the packaging adhesive is characterized in that: also comprises one or more of ultraviolet curing glue or AB component glue;
the back plate: the flexible glass substrate also comprises toughened glass or a fluorine-containing flexible substrate;
the interconnection line: also comprises a lead of aluminum Al or silver Ag, a conductive adhesive tape or a foil.
Three-dimensional perovskite material ABX in the metal halide layer 3 And a two-dimensional perovskite material A 1 2 A n-1 B n X 3n+1 、A 2 A n-1 B n X 3n+1 The selection scheme of various ions in (1):
monovalent cations A also include formamidine FA + Potassium, K + Rb, rb + Cesium Cs + One or more of the above;
monovalent organic cation A 1 Also comprises phenethylamine PEA + Ethylamine EA + Dimethylamine DMA + Methyltriethylammonium MTEA + Guanidine GA + 2-Thienylmethylammonium ThMA + One or more of the above;
a divalent organic cation A 2 Also included is 3-aminomethylpiperidine 3AMP 2+ 4-Aminomethylpiperidine 4AMP 2+ 3-aminomethylpyridine 3AMPY 2+ 4-aminomethylpyridine 4AMPY 2+ EDA, ethylenediamine 2+ DPA of N, N-dimethylaniline 2+ Propane 1, 3-diammonium PDA 2 + 1, 4-DingDiamine BDA 2+ 2, 5-diaminomethylthiophene ThDMA 2+ P-xylylenediamine (PDMA) 2+ N, N-dimethylethylenediamine DMDEA 2+ One or more of the above;
the positive divalent cation B also includes germanium Ge 2+ Tin Sn 2+ One or more of the above;
the monovalent anion X also includes bromine Br - ；
A lead halide material in the metal halide layer: also comprises lead fluoride PbF 2 Lead bromide PbBr 2 And lead iodide PbI 2 One or more of the above;
the inorganic insulating protective layer: also comprises zirconium dioxide ZrO 2 Molybdenum trioxide, moO 33 Any one or any combination thereof;
the protection packaging adhesive: any one or any combination of butyl rubber and silica gel is also included.
In addition to the preparation methods used in the above three examples, the preparation method for preparing the insulating protective layer further includes a thermal evaporation method. Such modifications and variations are within the spirit of the invention and the scope of the appended claims.

Claims (10)

1. The utility model provides an anti irradiation photovoltaic energy storage integrated device, includes solar module (1), stabiliser (2), charge and discharge management subassembly (3) and energy storage battery (4), and stabiliser (2) are connected between the output of solar module (1) and an input port of charge and discharge management subassembly (3), and the two-way port of an input/output of charge and discharge management subassembly (3) meets with the two-way port of input/output of energy storage battery (4), solar module (1) comprises a plurality of perovskite solar cell, and every perovskite solar cell includes transparent conductive substrate (11), electron transport layer (12), light-absorption layer (13), hole transport layer (14) and metal electrode (15), its characterized in that:
each perovskite solar cell is provided with a double-layer packaging structure (16) for isolating external water and oxygen from entering, protecting the light absorption layer (13) from being corroded and decomposed by the water and oxygen and improving the long-term stability of the whole device;
the light absorption layer (13) is made of a three-dimensional perovskite and two-dimensional perovskite composite material so as to improve the long-term stability and the photoelectric conversion efficiency of the material, and the thickness of the light absorption layer is 150-550nm;
the double-layer packaging structure (16) comprises an insulating protection layer (161), a filling protection layer (162), a back plate (163), packaging glue (164) and interconnection lines (165), wherein the insulating protection layer (161), the filling protection layer (162) and the back plate (163) are sequentially stacked above the metal electrode (15), the packaging glue (164) wraps the periphery of all layers between the transparent conductive substrate (11) and the back plate (163), and the interconnection lines (165) are respectively led out of the solar cell from the transparent conductive substrate (11) and the metal electrode (15) and are used for completing interconnection between the perovskite solar cells;
the metal halide packaging box (5) is arranged outside the voltage stabilizer (2), the charge-discharge management assembly (3) and the energy storage battery (4) and used for eliminating external irradiation;
the metal halide packaging box (5) is formed by bonding six metal halide packaging plates (51) through epoxy resin, each metal halide packaging plate (51) comprises a glass substrate (511), a metal halide layer (512), an inorganic insulating protective layer (513) and protective packaging glue (514) from top to bottom, and the metal halide packaging plates (51) are provided with through holes (515) used as wiring channels inside and outside the packaging box.
2. The device according to claim 1, wherein the perovskite solar cell comprises both an inverted structure and an inverted structure;
the positive structure comprises a transparent conductive substrate (11), an electron transport layer (12), a light absorption layer (13), a hole transport layer (14), a metal electrode (15) and a double-layer packaging structure (16) from bottom to top;
the inverted structure comprises a transparent conductive substrate (11), a hole transport layer (14), a light absorption layer (13), an electron transport layer (12), a metal electrode (15) and a double-layer packaging structure (16) from bottom to top.
3. Device according to claim 1, characterized by a three-dimensional perovskite in the material of the light-absorbing layer (13) of formula ABX 3 The different ions in (2) are selected as follows:
positive monovalent cation A, methylamine MA is selected + Formamidine FA + Potassium, K + Rubidium Rb + Cesium Cs + Any one kind of ion and any combination of several kinds of ions;
positive divalent metal cation B, lead Pb 2+ Germanium Ge 2+ Sn, sn 2+ Any one kind of ion and any combination of several kinds of ions in the ion;
a monovalent anion X selected from chlorine Cl - Bromine Br - Iodine I - Any one kind of ion and any combination of several kinds of ions.
4. The device according to claim 1, wherein the light absorbing layer (13) material is a two-dimensional perovskite of formula a 1 2 A n-1 B n X 3n+1 Or A 2 A n-1 B n X 3n+13 The different ions in (1) are selected as follows:
the three ions of positive univalent cation A, positive divalent metal cation B and negative univalent anion X are selected as the three-dimensional perovskite;
monovalent organic cation A 1 Selecting phenylethylamine PEA + Butylamine BA + Ethylamine EA + Dimethylamine DMA + Methyltriethylammonium MTEA + Guanidine GA + 2-Thienylmethylammonium ThMA + Any one kind of ion and any combination of several kinds of ions in the ion;
positive divalent organic cation A 2 3-aminomethylpiperidine 3AMP is selected 2+ 4-Aminomethylpiperidine 4AMP 2+ 3-aminomethylpyridine 3AMPY 2+ 4-aminomethylpyridine 4AMPY 2+ EDA, ethylenediamine 2+ DPA of N, N-dimethylaniline 2+ Propane 1, 3-diammonium PDA 2+ 1, 4-butanediamine BDA 2+ 2, 5-diaminomethylthiophene ThDMA 2+ P-xylylenediamine (PDMA) 2+ N, N-dimethylethylenediamine DMDEA 2+ Any one ion and any combination of several ions.
5. The integrated photovoltaic energy storage device of claim 1, wherein:
the transparent conductive substrate (11) is made of one of Indium Tin Oxide (ITO) or fluorine-doped tin oxide (FTO), and the thickness of the transparent conductive substrate is 300-600nm;
the electron transport layer (12) adopts titanium dioxide TiO 2 SnO, tin dioxide 2 Zinc oxide ZnO, C 60 Solution, [6,6 ] C]-phenyl radical C 61 Any one of methyl butyrate solutions with the thickness of 70-150nm;
the hole transport layer (14) is prepared from triphenylamine derivative, 2, 7-tetra [ N, N-di (4-methoxyphenyl) amino ] -9, 9-spirobifluorene Spiro-OMeTAD, poly 3, 4-ethylenedioxythiophene, polystyrene sulfonate PEDOT, PSS, poly (3-hexylthiophene) P3HT, 2,3,5, 6-tetrafluoro-7, 8-tetracyanodimethane doped poly-tricarboxyamine PTAA: any one of F4-TCNQ, poly [ bis (4-phenyl) (2, 4, 6-trimethylphenyl) amine ] PTAA, cuprous thiocyanate CuSCN and nickel oxide NiO, wherein the thickness of the mixture is 50-200nm;
the metal electrode (15) is one of gold Au, silver Ag, copper Cu and carbon electrodes, and the thickness of the metal electrode is 90-300nm.
6. The apparatus of claim 1, wherein:
the insulating protective layer (161) is made of an inorganic material, and is made of alumina Al 2 O 3 Silicon dioxide SiO 2 Zirconium dioxide ZrO 2 Molybdenum trioxide, moO 3 Silicon nitride Si 3 N 4 Any one or any combination thereof;
the filling protection layer (162) is made of organic materials, and any one or any combination of polyethylene octene co-elastomer, ethylene-vinyl acetate copolymer, polyvinyl butyral, organic silicon resin and epoxy resin is adopted;
the back plate (163) is made of any one of ultra-white glass, toughened glass, soda-lime glass, a metal substrate or a fluorine-containing flexible substrate;
the packaging glue (164) is any one or any combination of butyl glue, silica gel, thermoplastic high polymer material, ultraviolet curing glue or AB component glue;
the interconnecting wire (165) is a metal wire, a conductive adhesive tape or a metal foil made of any one of gold Au, silver Ag and copper Cu.
7. The apparatus of claim 1, wherein:
the metal halide layer (512) is made of perovskite or lead halide material, wherein the perovskite material is selected in the same way as the absorption layer (3), and the lead halide material comprises lead fluoride PbF 2 Lead chloride PbCl 2 Lead bromide PbBr 2 And lead iodide PbI 2 One or more of the above;
the inorganic insulating protective layer (513) is made of aluminum oxide Al 2 O 3 Silicon dioxide SiO 2 Zirconium dioxide ZrO 2 Molybdenum trioxide (MoO) 3 Silicon nitride Si 3 N 4 Any one or any combination thereof;
the protective packaging adhesive (514) is any one or any combination of butyl adhesive, silica gel, thermoplastic high polymer material, ultraviolet curing adhesive or AB component adhesive.
8. The device according to claim 1, characterized in that the energy storage battery (4) is one of a lithium battery, a sodium battery and a nickel battery.
9. The preparation method of the anti-irradiation photovoltaic energy storage integrated device is characterized by comprising the following steps of:
1) Preparing a perovskite solar cell:
2) Carrying out double-layer packaging on the perovskite solar cell:
2.1 A metal wire or a conductive adhesive tape or a metal foil is selected as an interconnecting wire and is fixed on a transparent conductive substrate and a metal electrode of the prepared solar cell to be used as a reserved wiring port;
2.2 Selecting an insulating protective layer material, a filling protective layer material and packaging glue, manufacturing an insulating protective layer on the solar cell with a reserved wiring port by using a magnetron sputtering or Atomic Layer Deposition (ALD) or thermal evaporation method, laying a layer of filling protective layer material above the insulating protective layer, ensuring that an interconnection line connected with a metal electrode passes through the filling protective layer, filling the packaging glue around the perovskite solar cell with the filling protective layer, and ensuring that all the interconnection lines pass through the packaging glue to obtain the perovskite solar cell with the packaging glue;
2.3 Selecting a back plate, turning the perovskite solar cells with the packaging glue up and down by one hundred and eighty degrees, placing the perovskite solar cells on the back plate, arranging a plurality of perovskite solar cells with the packaging glue on the back plate to form an array according to the method, and ensuring that all interconnection lines pass through the back plate to reach the outside of the packaging layer to obtain a stacked perovskite solar cell array;
2.4 The stacked perovskite solar cell array is placed into a heating plate of a heated laminating machine for lamination to obtain a laminated perovskite solar cell array, and then the laminated perovskite solar cell array is taken out and cooled to obtain a double-layer packaged perovskite solar cell array;
3) Connecting the interconnection lines of the double-layer packaged perovskite solar cell array in series and parallel according to actual requirements to obtain a double-layer packaged perovskite solar cell module;
4) The voltage stabilizer, the charge and discharge management assembly and the energy storage battery are connected through a wire and are packaged by a metal halide packaging box:
4.1 Preparation of metal halide package panels:
4.1.1 Taking a glass substrate with a through hole reserved according to actual requirements;
4.1.2 Selecting a metal halide material, and coating the metal halide solution on a glass substrate by a solution coating method to obtain a prepared metal halide layer;
4.1.3 Selecting an inorganic insulating protective layer material, and preparing an inorganic insulating protective layer on the metal halide layer by utilizing an atomic layer deposition method or a thermal evaporation method to obtain a prepared inorganic insulating protective layer;
4.1.4 Selecting a protective packaging adhesive material, preparing a layer of protective packaging adhesive on the insulating protective layer by adopting a solution coating method, and curing the protective packaging adhesive to obtain a metal halide packaging plate;
4.2 Connecting a voltage stabilizer, a charging and discharging management assembly and an energy storage battery, and manufacturing a metal halide packaging box to finish packaging:
selecting a voltage stabilizer, a charge and discharge management assembly and an energy storage battery, connecting an output port of the voltage stabilizer with an input port of the charge and discharge management assembly through a wire, connecting an input and output bidirectional port of the charge and discharge management assembly with an input and output bidirectional port of the energy storage battery, respectively connecting the input port of the voltage stabilizer and the output port of the charge and discharge management assembly with the wire, then penetrating through a through hole of a metal halide packaging layer, then forming a metal halide packaging box by six metal halide packaging plates outside the voltage stabilizer, the charge and discharge management assembly and the energy storage battery, ensuring that a glass substrate faces outwards and is bonded by epoxy resin, and obtaining a packaged and connected external device;
5) And connecting an input port of a voltage stabilizer in the packaged and connected external device to an output end of the double-layer packaged perovskite solar cell module to obtain the anti-irradiation photovoltaic energy storage integrated device.
10. The method according to claim 9, wherein 1) the perovskite solar cell is prepared in any one of an upside-down structure and a front-up structure;
the preparation method of the perovskite solar cell with the positive structure comprises the following steps:
1.1 Selecting a transparent conductive substrate, and carrying out ultrasonic cleaning and ultraviolet ozone pretreatment;
1.2 Selecting an electron transport layer material, preparing the electron transport layer on the pretreated substrate by adopting a solution coating method, and then annealing the substrate to obtain the prepared electron transport layer;
1.3 Selecting a perovskite material, coating a perovskite solution on the prepared electron transport layer by adopting a one-step method or a two-step method, and annealing the coated sample piece to obtain a prepared perovskite absorption layer;
1.4 Selecting a hole transport layer material, and preparing a hole transport layer on the prepared perovskite absorption layer by adopting a solution coating method to obtain the prepared hole transport layer;
1.5 Selecting a metal electrode material, and evaporating the metal electrode on the hole transport layer by using a vacuum coating instrument to obtain a prepared metal electrode, thereby completing the preparation of the perovskite solar cell with the positive structure;
the preparation method of the perovskite solar cell with the inverted structure comprises the following steps:
1a) Selecting a transparent conductive substrate, and carrying out ultrasonic cleaning and ultraviolet ozone pretreatment;
1b) Selecting a hole transport layer material, preparing a hole transport layer on the pretreated substrate by adopting a solution coating method, and annealing the substrate to obtain the prepared hole transport layer;
1c) Coating a perovskite solution on the prepared hole transport layer by adopting a perovskite material through a one-step method or a two-step method, and annealing the coated sample piece to obtain a prepared perovskite absorption layer;
1d) Selecting an electron transport layer material, and preparing an electron transport layer on the prepared perovskite absorption layer by adopting a solution coating method to obtain the prepared electron transport layer;
1e) And (3) selecting a metal electrode material, and evaporating the metal electrode on the hole transport layer by using a vacuum coating instrument to obtain the prepared metal electrode, thereby completing the preparation of the inverted structure perovskite solar cell.
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