Perovskite thin film and preparation method therefor, and photoelectric device and preparation method therefor

Abstract

Disclosed in the present invention are a perovskite thin film and a preparation method therefor, and a photoelectric device and a preparation method therefor. The perovskite thin film comprises a perovskite-structure substance and an inorganic metal cyanate, wherein the metal in the inorganic metal cyanate is selected from one or more of an alkali metal, an alkaline earth metal, a transition metal and a rare earth metal. The perovskite thin film of the present invention has a high film-forming quality, and a photoelectric device comprising the perovskite thin film has high efficiency and stability.

Description

Perovskite thin film, preparation method thereof, and optoelectronic device and preparation method thereof TECHNICAL FIELD

[0001] The present application belongs to the field of optoelectronics, and particularly relates to a perovskite thin film, a preparation method thereof, an optoelectronic device and a preparation method thereof. BACKGROUND

[0002] Organic-inorganic hybrid perovskite materials have the material advantages of high absorption coefficient, adjustable band gap, long carrier diffusion length and high defect tolerance, and the industrial advantages of simple preparation process and low material and preparation cost, and are considered to be the most promising new material for commercialization in the photovoltaic market in recent years.

[0003] After only a decade of research, single-junction perovskite solar cells have achieved high photoelectric conversion efficiency, surpassing the currently commercialized cadmium telluride and copper indium gallium selenide cells, and have approached the mainstream crystalline silicon (26.7%) solar cell. The tandem perovskite solar cell has gradually become a hot research direction in the world photovoltaic research field due to its high efficiency, low cost and simple preparation process, and is considered to be one of the technologies that are expected to realize large-scale ground photovoltaic application.

[0004] In the preparation process of single-junction perovskite solar cells, tandem perovskite solar cells and other perovskite devices, how to prepare a perovskite thin film with low defect state density is the key to realizing high-efficiency perovskite device preparation. However, the perovskite components have a large degree of variability, and different components of perovskite require different additives for auxiliary film-forming crystallization. The existing additives have different practicability for different components of perovskite, and cannot be applied to a wide range of perovskite components. Long-chain ammonium salt additives can improve the performance of devices by forming 2D structure perovskite in the bulk phase, but the two-dimensional perovskite diffuses and disappears in the bulk phase during photothermal aging, making it difficult to maintain high efficiency of the device. The presence of methylamino (MA) additives in the annealing process will leave a small amount of residue, which will significantly reduce the stability of the device and affect the practicability of the final product.

[0005] Therefore, it is urgent to develop a perovskite thin film with a new type of additive to improve the efficiency and stability of perovskite devices with different components or different preparation processes. SUMMARY

[0006] To solve the problems in the prior art, the present application provides a perovskite thin film, which comprises perovskite structure material and inorganic metal cyanate, and the film forming quality of the perovskite thin film can be significantly improved by adding inorganic metal cyanate additive into a solution containing perovskite structure material, thereby improving the efficiency of the device; and specific inorganic metal ions can be doped into the perovskite crystal structure to reduce lattice defects and form a more stable crystal structure, thereby improving the stability of the device. In summary, the perovskite thin film of the present application can effectively improve the efficiency and stability of perovskite devices with different components or different preparation processes.

[0007] Specifically, the present application provides a perovskite thin film, which comprises perovskite structure material and inorganic metal cyanate, and the metal in the inorganic metal cyanate is selected from one or more of alkali metal, alkaline earth metal, transition metal and rare earth metal.

[0008] In one or more embodiments, the inorganic metal cyanate is selected from one or more of lithium cyanate, sodium cyanate, potassium cyanate, rubidium cyanate, cesium cyanate, magnesium cyanate, calcium cyanate, barium cyanate, zinc cyanate, cobalt cyanate, copper cyanate, europium cyanate, cerium cyanate and lanthanum cyanate.

[0009] In one or more embodiments, the chemical formula of the perovskite structure material is ABX3, wherein A is a monovalent cation, including one or more of cesium, rubidium, methylamine group and formamidine group, B is a divalent cation, including one or more of lead, copper, zinc, gallium, tin and calcium, and X is a monovalent anion, including one or more of iodine, bromine, chlorine, fluorine, thiocyanate, tetrafluoroborate, hexafluorophosphate, formate and acetate.

[0010] In one or more embodiments, the mass ratio of the inorganic metal cyanate to the perovskite structure material is ≤5.5%, preferably 1:(50-10000000).

[0011] In one or more embodiments, the thickness of the perovskite thin film is 200-10000 nm.

[0012] The present application provides a method for preparing the perovskite thin film of the present application, which comprises the following steps: mixing raw materials of perovskite structure material and inorganic metal cyanate in a solvent to prepare a perovskite precursor solution, and depositing the perovskite precursor solution to obtain a perovskite thin film.

[0013] In one or more embodiments, the solvent in the perovskite precursor solution is selected from one or more of N,N-dimethylformamide, dimethyl sulfoxide, N-methyl pyrrolidone, acetonitrile, 2-methoxyethanol, ethanol and isopropanol.

[0014] In one or more embodiments, the perovskite precursor solution, the method of depositing the perovskite precursor solution is spin coating, doctor blading, electron beam evaporation, thermal evaporation, printing, spray coating, spray pyrolysis or slot-die coating.

[0015] In one or more embodiments, the perovskite precursor solution, the concentration of the inorganic metal cyanide salt in the perovskite precursor solution is 0.002-20 mg / mL.

[0016] The present application provides a kind of optoelectronic device, the optoelectronic device includes perovskite film, the perovskite film includes perovskite structure material and inorganic metal cyanide salt;Preferably, the optoelectronic device is perovskite solar cell device, LED device or detector device.

[0017] In one or more embodiments, the perovskite solar cell device includes single-junction perovskite solar cell and / or tandem perovskite solar cell.In one or more embodiments, the single-junction perovskite solar cell is formal single-junction perovskite solar cell or reverse single-junction perovskite solar cell, the formal single-junction perovskite solar cell includes transparent conductive glass, electron transport layer, perovskite film layer, hole transport layer and back electrode from light receiving front to light receiving back in turn;The reverse single-junction perovskite solar cell includes transparent conductive glass, hole transport layer, perovskite film layer, electron transport layer and back electrode from light receiving front to light receiving back in turn.

[0018] In one or more embodiments, the tandem perovskite solar cell is formal tandem perovskite solar cell or reverse tandem perovskite solar cell, the reverse tandem perovskite solar cell includes top electrode, reverse perovskite top cell, tunneling layer, bottom cell and back electrode from light receiving front to light receiving back in turn, the reverse perovskite top cell includes electron transport layer, perovskite film layer, hole transport layer from light receiving front to light receiving back in turn;The formal tandem perovskite solar cell includes top electrode, formal perovskite top cell, tunneling layer, bottom cell and back electrode from light receiving front to light receiving back in turn;The reverse perovskite top cell includes hole transport layer, perovskite film layer, electron transport layer from light receiving front to light receiving back in turn.

[0019] In one or more embodiments, the top electrode comprises a transparent electrode layer; preferably, the top electrode comprises a gate line electrode and a transparent electrode layer in sequence from the light-receiving front side to the light-receiving back side; more preferably, the top electrode comprises a gate line electrode, an anti-reflection layer and a transparent electrode layer in sequence from the light-receiving front side to the light-receiving back side; wherein the material of the transparent electrode layer is preferably selected from one or more of indium tin oxide, indium zinc oxide, cerium-doped indium oxide, tungsten-doped indium oxide, aluminum-doped zinc oxide, antimony-doped tin oxide, zirconium-doped indium oxide and gallium zinc-doped indium oxide; the material of the gate line electrode is preferably silver and / or copper; the material of the anti-reflection layer is preferably selected from one or more of silicon oxide, aluminum oxide, silicon nitride, magnesium fluoride, lithium fluoride, polydimethylsiloxane and ethylene-vinyl acetate copolymer; the thickness of the top electrode is preferably 0.005-201 μm; the thickness of the transparent electrode layer is 5-300 nm; the thickness of the gate line electrode is preferably 0-200 μm; the thickness of the anti-reflection layer is preferably 0-400 nm.

[0020] In one or more embodiments, the transparent conductive glass is indium tin oxide glass, indium zinc oxide glass, cerium-doped indium oxide glass, tungsten-doped indium oxide glass, aluminum-doped zinc oxide glass, antimony-doped tin oxide glass, zirconium-doped indium oxide glass or gallium zinc-doped indium oxide glass.

[0021] In one or more embodiments, the material of the hole transport layer is an inorganic transport material and / or a p-type semiconductor material; preferably, the inorganic transport material is selected from one or more of nickel oxide, cuprous oxide, molybdenum oxide and copper iodide; the p-type semiconductor material is selected from one or more of reduced graphene oxide, poly[bis(4-phenyl)(2,4,6-trimethylphenyl)amine], 2,2',7,7'-tetra[N,N-bis(4-methoxyphenyl)amino]-9,9'-spirobifluorene, poly(3,4-ethylenedioxythiophene), polystyrene sulfonate, poly[bis(4-phenyl)(4-butylphenyl)amine], [2-(9H-carbazol-9-yl)ethyl]phosphonic acid and [2-(3,6-dimethoxy-9H-carbazol-9-yl)ethyl]phosphonic acid.

[0022] In one or more embodiments, the material of the electron transport layer is an n-type semiconductor material; preferably, the n-type semiconductor material is selected from one or more of titanium oxide, tin oxide, zinc oxide, fullerene, graphene and fullerene derivatives.

[0023] In one or more embodiments, the material of the tunneling layer is indium tin oxide, indium zinc oxide, cerium-doped indium oxide, tungsten-doped indium oxide, aluminum-doped zinc oxide, antimony-doped tin oxide, zirconium-doped indium oxide, gallium zinc-doped indium oxide, a combination of heavily doped n-silicon and p-silicon, a combination of n-silicon and other p-type materials; preferably, the other p-type material is MoO3 and / or NiOx.

[0024] In one or more embodiments, the bottom cell is a perovskite bottom cell, a crystalline silicon bottom cell, a copper indium gallium selenide bottom cell, a gallium arsenide bottom cell, a cadmium telluride bottom cell, an organic bottom cell, or a quantum dot bottom cell.

[0025] In one or more embodiments, the back electrode material is selected from one or more of gold, palladium, silver, titanium, chromium, nickel, aluminum, copper, indium tin oxide, and indium zinc oxide.

[0026] In one or more embodiments, the thickness of the hole transport layer in the single-junction perovskite solar cell is 0.2-100 nm.

[0027] In one or more embodiments, the thickness of the perovskite thin film layer in the single-junction perovskite solar cell is 200-3000 nm.

[0028] In one or more embodiments, the thickness of the electron transport layer in the single-junction perovskite solar cell is 1-90 nm.

[0029] In one or more embodiments, the thickness of the back electrode in the single-junction perovskite solar cell is 0.04-200 μm.

[0030] In one or more embodiments, the thickness of the hole transport layer in the tandem perovskite solar cell is 0.2-100 nm.

[0031] In one or more embodiments, the thickness of the perovskite thin film layer in the tandem perovskite solar cell is 200-3000 nm.

[0032] In one or more embodiments, the thickness of the electron transport layer in the tandem perovskite solar cell is 0.5-90 nm.

[0033] In one or more embodiments, the thickness of the bottom cell in the tandem perovskite solar cell is 10-600 μm.

[0034] In one or more embodiments, the thickness of the back electrode in the tandem perovskite solar cell is 0.04-100 μm.

[0035] The present application provides a method for preparing the photovoltaic device described herein, the method comprising the following steps:

[0036] (1) depositing a hole transport layer or an electron transport layer on a surface of a transparent conductive glass;

[0037] (2) depositing a perovskite thin film layer on a surface of the hole transport layer or the electron transport layer;

[0038] (3) depositing an electron transport layer or a hole transport layer on the surface of the perovskite thin film layer;

[0039] (4) depositing a back electrode on the surface of the electron transport layer or the hole transport layer, to obtain a single-junction perovskite solar cell; or

[0040] (1') depositing a back electrode material and a tunneling layer on the two surfaces of the bottom cell, respectively;

[0041] (2') depositing a hole transport layer or an electron transport layer on the surface of the tunneling layer

[0042] (3') depositing a perovskite thin film layer on the surface of the hole transport layer or the electron transport layer;

[0043] (4') depositing an electron transport layer or a hole transport layer on the surface of the perovskite thin film layer;

[0044] (5') depositing a top electrode on the surface of the electron transport layer or the hole transport layer, to obtain a stacked perovskite solar cell.

[0045] In one or more embodiments, in step (2) or step (3') of the method for preparing the photoelectric device, a perovskite precursor solution is deposited on the surface of the hole transport layer or the electron transport layer, to obtain a perovskite thin film layer, the perovskite precursor solution comprising raw materials of perovskite structure substances, an inorganic metal cyanate, and a solvent.

[0046] In one or more embodiments, in the method for preparing the photoelectric device, the method for preparing the perovskite precursor solution is mixing the raw materials of perovskite structure substances and the inorganic metal cyanate in the solvent to prepare the perovskite precursor solution.

[0047] In one or more embodiments, in the method for preparing the photoelectric device, the solvent in the perovskite precursor solution is selected from one or more of N,N-dimethylformamide, dimethyl sulfoxide, N-methyl pyrrolidone, acetonitrile, 2-methoxyethanol, ethanol, and isopropanol.

[0048] In one or more embodiments, in the method for preparing the photoelectric device, the concentration of the inorganic metal cyanate in the perovskite precursor solution is 0.002-20 mg / mL.

[0049] The present application provides a method for preparing the single-junction perovskite solar cell described in the present application, the method comprising the following steps:

[0050] (1) depositing a hole transport layer material on the surface of a transparent conductive glass, to obtain a hole transport layer;

[0051] (2) depositing a perovskite precursor solution on the surface of the hole transport layer, to obtain a perovskite thin film layer;

[0052] (3) depositing an electron transport layer material on the surface of the perovskite thin film layer to obtain an electron transport layer;

[0053] (4) depositing a back electrode material on the surface of the electron transport layer to obtain a back electrode and a trans single-junction perovskite solar cell at the same time; or

[0054] (1') depositing an electron transport layer material on the surface of the transparent conductive glass to obtain an electron transport layer;

[0055] (2') depositing a perovskite precursor solution on the surface of the electron transport layer to obtain a perovskite thin film layer;

[0056] (3') depositing a hole transport layer material on the surface of the perovskite thin film layer to obtain a hole transport layer;

[0057] (4') depositing a back electrode material on the surface of the hole transport layer to obtain a back electrode and a formal single-junction perovskite solar cell at the same time.

[0058] In one or more embodiments, in the method for preparing a single-junction perovskite solar cell, the hole transport layer is deposited by spin coating, blade coating, physical vapor deposition, atomic layer deposition, slot coating or immersion; preferably, the physical vapor deposition is magnetron sputtering, reactive plasma deposition, electron beam evaporation or thermal evaporation.

[0059] In one or more embodiments, in the method for preparing a single-junction perovskite solar cell, the perovskite precursor solution is prepared by mixing raw materials of perovskite structure substances and inorganic metal cyanate in a solvent to obtain a perovskite precursor solution.

[0060] In one or more embodiments, in the method for preparing a single-junction perovskite solar cell, the solvent in the perovskite precursor solution is selected from one or more of N,N-dimethylformamide, dimethyl sulfoxide, N-methyl pyrrolidone, acetonitrile, 2-methoxyethanol, ethanol and isopropanol.

[0061] In one or more embodiments, in the method for preparing a single-junction perovskite solar cell, the concentration of the inorganic metal cyanate in the perovskite precursor solution is 0.002-20 mg / mL.

[0062] In one or more embodiments, in the method for preparing a single-junction perovskite solar cell, the perovskite thin film layer is deposited by spin coating, blade coating, electron beam evaporation, thermal evaporation, printing, spraying, spray pyrolysis or slot coating.

[0063] In one or more embodiments, in the method for preparing a single-junction perovskite solar cell, the electron transport layer is deposited by spin coating, blade coating, physical vapor deposition, atomic layer deposition, slot coating or immersion; preferably, the physical vapor deposition is magnetron sputtering, reactive plasma deposition, electron beam evaporation or thermal evaporation.

[0064] In one or more embodiments, in the method for preparing a single-junction perovskite solar cell, the back electrode is deposited by physical vapor deposition, printing, spraying or electroplating; preferably, the physical vapor deposition is magnetron sputtering, reactive plasma deposition, electron beam evaporation or thermal evaporation.

[0065] The present application provides a method for preparing the laminated perovskite solar cell described in the present application, the method comprising the following steps:

[0066] (1) depositing a back electrode material and a tunneling layer material on the two surfaces of the bottom cell respectively, to obtain a back electrode and a tunneling layer;

[0067] (2) depositing a hole transport layer material on the surface of the tunneling layer, to obtain a hole transport layer;

[0068] (3) depositing a perovskite precursor solution on the surface of the hole transport layer, to obtain a perovskite thin film layer;

[0069] (4) depositing an electron transport layer material on the surface of the perovskite thin film layer, to obtain an electron transport layer;

[0070] (5) depositing a top electrode material on the surface of the electron transport layer, to obtain a top electrode and a trans-inverted laminated perovskite solar cell; or

[0071] (1') depositing a back electrode material and a tunneling layer material on the two surfaces of the bottom cell respectively, to obtain a back electrode and a tunneling layer;

[0072] (2') depositing an electron transport layer material on the surface of the tunneling layer, to obtain an electron transport layer;

[0073] (3') depositing a perovskite precursor solution on the surface of the electron transport layer, to obtain a perovskite thin film layer;

[0074] (4') depositing a hole transport layer material on the surface of the perovskite thin film layer, to obtain a hole transport layer;

[0075] (5') depositing a top electrode material on the surface of the hole transport layer, to obtain a top electrode and an official laminated perovskite solar cell;

[0076] The top electrode comprises a transparent electrode layer; preferably, the top electrode comprises a gate line electrode and a transparent electrode layer in sequence from the light-receiving front surface to the light-receiving back surface, more preferably, the top electrode comprises a gate line electrode, an anti-reflection layer and a transparent electrode layer in sequence from the light-receiving front surface to the light-receiving back surface.

[0077] In one or more embodiments, in the method for preparing the laminated perovskite solar cell, the back electrode is deposited by physical vapor deposition, printing, spraying or electroplating; preferably, the physical vapor deposition is magnetron sputtering, reactive plasma deposition, electron beam evaporation or thermal evaporation.

[0078] In one or more embodiments, in the method for preparing the laminated perovskite solar cell, the tunneling layer is deposited by physical vapor deposition, monolayer deposition, chemical vapor deposition or plasma-enhanced chemical vapor deposition; preferably, the physical vapor deposition is magnetron sputtering, reactive plasma deposition, electron beam evaporation or thermal evaporation.

[0079] In one or more embodiments, in the method for preparing the laminated perovskite solar cell, the hole transport layer is deposited by spin coating, blade coating, physical vapor deposition, atomic layer deposition, slot coating or immersion; preferably, the physical vapor deposition is magnetron sputtering, reactive plasma deposition, electron beam evaporation or thermal evaporation.

[0080] In one or more embodiments, in the method for preparing the laminated perovskite solar cell, the perovskite precursor solution is prepared by mixing raw materials of perovskite structure substances and inorganic metal cyanate in a solvent to obtain a perovskite precursor solution.

[0081] In one or more embodiments, in the method for preparing the laminated perovskite solar cell, the solvent in the perovskite precursor solution is selected from one or more of N, N-dimethylformamide, dimethyl sulfoxide, N-methyl pyrrolidone, acetonitrile, 2-methoxyethanol, ethanol and isopropanol.

[0082] In one or more embodiments, in the method for preparing the laminated perovskite solar cell, the concentration of the inorganic metal cyanate in the perovskite precursor solution is 0.002-20 mg / mL.

[0083] In one or more embodiments, in the method for preparing the laminated perovskite solar cell, the deposition method of the perovskite thin film layer is spin coating, blade coating, electron beam evaporation, thermal evaporation, printing, spraying, spray pyrolysis or slot coating.

[0084] In one or more embodiments, in the method for preparing a stacked perovskite solar cell, the electron transport layer is deposited by spin coating, blade coating, physical vapor deposition, atomic layer deposition, slot-die coating, or immersion; preferably, the physical vapor deposition is magnetron sputtering, reactive plasma deposition, electron beam evaporation, or thermal evaporation.

[0085] In one or more embodiments, in the method for preparing a stacked perovskite solar cell, the transparent electrode layer is deposited by physical vapor deposition; preferably, the physical vapor deposition is magnetron sputtering, reactive plasma deposition, electron beam evaporation, or thermal evaporation.

[0086] In one or more embodiments, in the method for preparing a stacked perovskite solar cell, the anti-reflection layer is deposited by physical vapor deposition; preferably, the physical vapor deposition is magnetron sputtering, reactive plasma deposition, electron beam evaporation, or thermal evaporation.

[0087] In one or more embodiments, in the method for preparing a stacked perovskite solar cell, the grid electrode is deposited by thermal evaporation, printing, or electroplating. BRIEF DESCRIPTION OF DRAWINGS

[0088] Figure 1(a) is a schematic diagram of the structure of a single-junction perovskite solar cell according to some embodiments of the present application.

[0089] Figure 1(b) is a schematic diagram of the structure of a stacked perovskite solar cell according to some embodiments of the present application.

[0090] Figure 1(c) is a schematic diagram of the detailed structure of a stacked perovskite solar cell according to some embodiments of the present application.

[0091] Figure 2 is a schematic diagram of inorganic metal cyanate according to some embodiments of the present application; in Figure 2, (a) lithium cyanate, (b) sodium cyanate, (c) potassium cyanate, (d) rubidium cyanate, (e) cesium cyanate, (f) magnesium cyanate, (g) calcium cyanate, (h) barium cyanate, (i) zinc cyanate, (j) copper cyanate, (k) cobalt cyanate, (1) europium cyanate, (m) cerium cyanate, (n) lanthanum cyanate.

[0092] Figure 3 is a schematic diagram of a crystalline silicon / perovskite stacked solar cell according to some embodiments of the present application.

[0093] Figure 4 is an X-ray diffraction pattern (XRD) of perovskite thin films prepared in Examples 1-3, Example 6, Examples 8-9, and Comparative Example 1 according to the present application.

[0094] Figure 5 is a fluorescence image of perovskite thin films prepared in Examples 1-9 and Comparative Example 1 according to the present application. DETAILED DESCRIPTION

[0095] To enable persons skilled in the art to understand the features and effects of the present application, the following is a general description and definition of the terms and phrases mentioned in the specification and claims. Unless otherwise specified, all technical and scientific words used herein are understood to have the common meaning to those skilled in the art of the present application, and in the event of conflict, the definitions in the specification shall prevail.

[0096] Theories and mechanisms described and disclosed herein, whether correct or not, should not be considered limiting of the scope of the present application, which is limited only by the claims. The present application can be implemented in ways other than those specifically described herein.

[0097] In this document, "comprise", "include", "contain" and similar words are used in a inclusive sense and are intended to mean "consist essentially of" and "consist of", for example, when it is disclosed herein that "A comprises B and C", it should be considered that "A consists essentially of B and C" and "A consists of B and C" are disclosed herein.

[0098] In this document, all features of a numerical range or a percentage range, such as values, amounts, contents and concentrations, are only for the sake of brevity and convenience. Therefore, the description of a numerical range or a percentage range should be considered to have encompassed and specifically disclosed all possible sub-ranges and individual values within the range (including integers and fractions).

[0099] In this document, unless otherwise specified, percentages refer to mass percentages and ratios refer to mass ratios.

[0100] In this document, when describing embodiments or examples, it should be understood that they are not intended to limit the present application to these embodiments or examples. On the contrary, all alternatives, modifications and equivalents of the methods and materials described herein that are within the scope of the claims are intended to be encompassed by the present application.

[0101] In this document, for the sake of brevity, not all possible combinations of the technical features in each embodiment or example are described. Therefore, as long as the combinations of the technical features do not conflict, the technical features in each embodiment or example can be combined arbitrarily, and all possible combinations should be considered to be within the scope of the present application.

[0102] The application provides a perovskite thin film, which comprises perovskite structure substances and inorganic metal cyanate, and the metal in the inorganic metal cyanate can be one or more selected from alkali metals, alkaline earth metals, transition metals and rare earth metals.

[0103] In the application, the inorganic metal cyanate can be one or more selected from lithium cyanate, sodium cyanate, potassium cyanate, rubidium cyanate, cesium cyanate, magnesium cyanate, calcium cyanate, barium cyanate, zinc cyanate, cobalt cyanate, copper cyanate, europium cyanate, cerium cyanate and lanthanum cyanate, and the structure is shown in Figure 2.

[0104] In the application, the chemical formula of the perovskite structure substance can be ABX3, wherein A can be one or more selected from monovalent cations including cesium (Cs + ), rubidium (Rb + ), methylamine (CH3NH3 + , MA) and formamidinium (CH(NH)NH2 + , FA), B can be one or more selected from divalent cations including lead (Pb 2+ ), copper (Cu 2+ ), zinc (Zn 2+ ), gallium (Ga 2+ ), tin (Sn 2+ ) and calcium (Ca 2+ ), and X can be one or more selected from monovalent anions including iodine (I - ), bromine (Br - ), chlorine (Cl - ), fluorine (F - ), thiocyanate (SCN - ), tetrafluoroborate (BF4 - ), hexafluorophosphate (PF6 - ), formate (COO - ) and acetate (CH3COO -One or more of the following. The inorganic metal cyanate of the present invention improves the quality of film formation and crystallization of perovskite-structured materials with different compositions, and further significantly improves the efficiency and stability of devices composed of thin films with different perovskite-structured materials.

[0105] In this invention, the mass ratio of inorganic metal cyanate to perovskite structural material can be ≤5.5%, preferably ≤2.0%, and more preferably 1:(50~10,000,000), for example 1:50, 1:100, 1:200, 1:300, 1:500, 1:1000, 1:1500, 1:2000, 1:3000, 1:4000, 1:5000, 1:10000, 1:50000, 1:100000, 1:500000, 1:1000000, 1:500000, 1:1000000, 1:5000000, 1:10000000. By controlling the mass ratio of inorganic metal cyanate to perovskite structural material within the above-mentioned preferred range, this invention improves the crystallization quality of perovskite thin films, and further enhances the efficiency and stability of optoelectronic devices containing perovskite thin films.

[0106] In this invention, the thickness of the perovskite thin film can be 200 to 10000 nm, for example 200 nm, 500 nm, 1000 nm, 2000 nm, 4000 nm, 4000 nm, 5000 nm, 6000 nm, 7000 nm, 8000 nm, 9000 nm, and 10000 nm.

[0107] This invention provides a method for preparing the perovskite thin film of this invention, the method comprising the following steps: mixing the raw material of the perovskite structure and the inorganic metal cyanate in a solvent to obtain a perovskite precursor solution, depositing the perovskite precursor solution to obtain a perovskite thin film.

[0108] In the method for preparing the perovskite thin film of the present invention, the solvent may be one or more selected from N,N-dimethylformamide (DMF), dimethyl sulfoxide (DMSO), N-methylpyrrolidone, acetonitrile, 2-methoxyethanol, ethanol and isopropanol.

[0109] In the method for preparing the perovskite thin film of this invention, the perovskite precursor solution deposition method can be spin coating, blade coating, electron beam evaporation, thermal evaporation, printing, spraying, spray pyrolysis, or slot coating. The inorganic metal cyanate of this invention improves the quality of film formation and crystallization of perovskite thin films prepared by different processes. Furthermore, it significantly improves the efficiency and stability of devices composed of perovskite thin films prepared by different processes.

[0110] In the present application, the concentration of inorganic metal cyanate in the perovskite precursor solution is 0.002-20 mg / mL, for example, 0.005 mg / mL, 0.01 mg / mL, 0.05 mg / mL, 0.1 mg / mL, 0.5 mg / mL, 1 mg / mL, 2 mg / mL, 3 mg / mL, 5 mg / mL, 10 mg / mL, 15 mg / mL, or 20 mg / mL. The present application controls the concentration of inorganic metal cyanate in the perovskite precursor solution within the above range, which is beneficial to the film forming and crystallization quality of the perovskite thin film, and further improves the efficiency and stability of the optoelectronic device containing the perovskite thin film.

[0111] The present application provides an optoelectronic device containing the perovskite thin film of the present application; preferably, the optoelectronic device is a perovskite solar cell device, an LED device, or a detector device; more preferably, the perovskite solar cell device is a single-junction perovskite solar cell or a tandem perovskite solar cell. In some embodiments, the tandem perovskite solar cell is a perovskite / perovskite tandem cell, a perovskite / crystalline silicon tandem cell, a perovskite / copper indium gallium selenide tandem cell, a perovskite / gallium arsenide tandem cell, a perovskite / cadmium telluride tandem cell, a perovskite / organic tandem cell, or a perovskite / quantum dot tandem cell. In the present application, the single-junction perovskite solar cell is a formam single-junction perovskite solar cell or an inverse single-junction perovskite solar cell, the formam single-junction perovskite solar cell comprises, from the light-receiving front surface to the light-receiving back surface, a transparent conductive glass, an electron transport layer, a perovskite thin film layer, a hole transport layer, and a back electrode (as shown in FIG. 1(a)); the inverse single-junction perovskite solar cell comprises, from the light-receiving front surface to the light-receiving back surface, a transparent conductive glass, a hole transport layer, a perovskite thin film layer, an electron transport layer, and a back electrode (as shown in FIG. 1(a)). The single-junction perovskite solar cell of the present application has a perovskite thin film layer containing inorganic metal cyanate, which is beneficial to improve the efficiency and stability of the single-junction perovskite solar cell.

[0112] In the present application, the laminated perovskite solar cell is a formal laminated perovskite solar cell or a reverse laminated perovskite solar cell, the reverse laminated perovskite solar cell sequentially comprises a top electrode, a reverse perovskite top cell, a tunneling layer, a bottom cell and a back electrode from a light-receiving front surface to a light-receiving back surface (as shown in FIG. 1(b)), and the reverse perovskite top cell sequentially comprises an electron transport layer, a perovskite thin film layer and a hole transport layer from the light-receiving front surface to the light-receiving back surface (as shown in FIG. 1(c)); the formal laminated perovskite solar cell sequentially comprises a top electrode, a formal perovskite top cell, a tunneling layer, a bottom cell and a back electrode from a light-receiving front surface to a light-receiving back surface (as shown in FIG. 1(b)); and the reverse perovskite top cell sequentially comprises a hole transport layer, a perovskite thin film layer and an electron transport layer from the light-receiving front surface to the light-receiving back surface (as shown in FIG. 1(c)). The laminated perovskite solar cell of the present application has a perovskite thin film layer containing inorganic metal cyanate, which is beneficial to improving the efficiency and stability of the laminated perovskite solar cell.

[0113] In the present application, the top electrode can comprise a transparent electrode layer; preferably, the top electrode sequentially comprises a grid line electrode and a transparent electrode layer from a light-receiving front surface to a light-receiving back surface; more preferably, the top electrode sequentially comprises a grid line electrode, an anti-reflection layer and a transparent electrode layer from a light-receiving front surface to a light-receiving back surface.

[0114] In the top electrode of the present application, the material of the transparent electrode layer can be one or more selected from indium tin oxide (ITO), indium zinc oxide (IZO), cerium-doped indium oxide (ICO), tungsten-doped indium oxide (IWO), aluminum-doped zinc oxide (AZO), antimony-doped tin oxide (ATO), zirconium-doped indium oxide (IZrO) and gallium zinc-doped indium oxide (IGZO).

[0115] In the top electrode of the present application, the grid line electrode can be silver and / or copper.

[0116] In the top electrode of the present application, the anti-reflection layer can be one or more selected from silicon oxide, aluminum oxide, silicon nitride, magnesium fluoride, lithium fluoride, polydimethylsiloxane (PDMS) or ethylene-vinyl acetate copolymer (EVA).

[0117] In the top electrode of the present application, the thickness of the transparent electrode layer can be 5-300 nm, for example, 5 nm, 10 nm, 30 nm, 60 nm, 90 nm, 120 nm, 150 nm, 180 nm, 210 nm, 240 nm, 270 nm or 300 nm.

[0118] In the top electrode of the present application, the thickness of the grid line electrode can be 0-200 μm, for example, 20 μm, 40 μm, 60 μm, 80 μm, 100 μm, 120 μm, 140 μm, 160 μm, 180 μm or 200 μm.

[0119] The thickness of the anti-reflection layer in the top electrode can be 0-400 nm, such as 50 nm, 100 nm, 150 nm, 200 nm, 250 nm, 300 nm, 150 nm, 180 nm, 210 nm, 240 nm, 270 nm, 300 nm.

[0120] The thickness of the top electrode can be 0.005-201 μm. In some embodiments, the top electrode is composed of a transparent electrode layer, in which case the thickness of the top electrode is the thickness of the transparent electrode layer, which is in the range of 5-300 nm. In some embodiments, the top electrode is composed of a gate line electrode and a transparent electrode layer, in which case the thickness of the top electrode is the sum of the thicknesses of the gate line electrode and the transparent electrode layer, which is in the range of 0.005-200.3 μm. In some embodiments, the top electrode is composed of a gate line electrode, an anti-reflection layer, and a transparent electrode layer, in which case the thickness of the top electrode is the sum of the thicknesses of the gate line electrode, the anti-reflection layer, and the transparent electrode layer, which is in the range of 0.005-200.7 μm.

[0121] In the present application, the transparent conductive glass can be indium tin oxide glass, indium zinc oxide glass, cerium-doped indium oxide glass, tungsten-doped indium oxide glass, aluminum-doped zinc oxide glass, antimony-doped tin oxide glass, zirconium-doped indium oxide glass, or gallium zinc-doped indium oxide glass.

[0122] In the present application, the hole transport layer material can be an inorganic transport material and / or a p-type semiconductor material; preferably, the inorganic transport material can be one or more selected from nickel oxide (NiO), cuprous oxide (Cu2O), molybdenum trioxide (MoO3), and copper iodide (CuI); the p-type semiconductor material can be one or more selected from reduced graphene oxide, poly[bis(4-phenyl)(2,4,6-trimethylphenyl)amine] (PTAA), 2,2',7,7'-tetrakis[N,N-di(4-methoxyphenyl)amino]-9,9'-spirobifluorene (Spiro-OMeTAD), poly(3,4-ethylenedioxythiophene) (PEDOT), polystyrene sulfonate (PSS), poly[bis(4-phenyl)(4-butylphenyl)amine] (Ploy-TPD), [2-(9H-carbazol-9-yl)ethyl]phosphonic acid, and [2-(3,6-dimethoxy-9H-carbazol-9-yl)ethyl]phosphonic acid (MeO-2PACZ).

[0123] In the present application, the material of the electron transport layer can be an n-type semiconductor material; preferably, the n-type semiconductor material can be one or more selected from titanium oxide (TiO2), tin oxide (SnO2), zinc oxide (ZnO), fullerene (C60), graphene and fullerene derivative (PCBM). In some embodiments, the fullerene derivative is [6,6]-phenyl-C61-butyric acid methyl ester (

[0060] PCBM); in some embodiments, the fullerene derivative is [6,6]-phenyl-C71-butyric acid methyl ester (

[0070] PCBM).

[0124] In the present application, the material of the tunneling layer can be indium tin oxide, indium zinc oxide, cerium-doped indium oxide, tungsten-doped indium oxide, aluminum-doped zinc oxide, antimony-doped tin oxide, zirconium-doped indium oxide, gallium zinc-doped indium oxide, a combination of heavily doped n-silicon and p-silicon, a combination of n-silicon and other p-type materials; preferably, the other p-type material is MoO3 and / or NiOx.

[0125] In the present application, the bottom cell can be a perovskite bottom cell, a crystalline silicon bottom cell, a copper indium gallium selenide bottom cell, a gallium arsenide bottom cell, a cadmium telluride bottom cell, an organic bottom cell or a quantum dot bottom cell.

[0126] In the present application, the material of the back electrode can be one or more selected from gold, palladium, silver, titanium, chromium, nickel, aluminum, copper, indium tin oxide (ITO) and indium zinc oxide (IZO).

[0127] In the present application, the thickness of the hole transport layer in the single-junction perovskite solar cell can be 0.2-100 nm, such as 0.5 nm, 1 nm, 10 nm, 20 nm, 30 nm, 40 nm, 50 nm, 60 nm, 70 nm, 80 nm, 90 nm or 100 nm.

[0128] In the present application, the thickness of the perovskite thin film layer in the single-junction perovskite solar cell can be 200-3000 nm, such as 200 nm, 400 nm, 600 nm, 800 nm, 1000 nm, 1200 nm, 1400 nm, 1600 nm, 1800 nm, 2000 nm, 2200 nm, 2400 nm, 2600 nm, 2800 nm or 3000 nm.

[0129] In the present application, the thickness of the electron transport layer in the single-junction perovskite solar cell can be 1-90 nm, such as 1 nm, 5 nm, 10 nm, 20 nm, 30 nm, 40 nm, 50 nm, 60 nm, 70 nm, 80 nm or 90 nm.

[0130] The thickness of the back electrode in the single-junction perovskite solar cell can be 0.04-200μm, for example, 0.1μm, 0.5μm, 1μm, 5μm, 10μm, 20μm, 50μm, 100μm, 150μm, 200μm.

[0131] The thickness of the hole transport layer in the stacked perovskite solar cell can be 0.2-100nm, for example, 0.5nm, 1nm, 10nm, 20nm, 30nm, 40nm, 50nm, 60nm, 70nm, 80nm, 90nm, 100nm.

[0132] The thickness of the perovskite thin film layer in the stacked perovskite solar cell can be 200-3000nm, for example, 200nm, 400nm, 600nm, 800nm, 1000nm, 1200nm, 1400nm, 1600nm, 1800nm, 2000nm.

[0133] The thickness of the electron transport layer in the stacked perovskite solar cell can be 0.5-90nm, for example, 1nm, 5nm, 10nm, 20nm, 30nm, 40nm, 50nm, 60nm, 70nm, 80nm, 90nm.

[0134] The thickness of the bottom cell in the stacked perovskite solar cell can be 10-600μm, for example, 20μm, 50μm, 100μm, 150μm, 200μm, 250μm, 300μm, 350μm, 400μm, 450μm, 500μm, 550μm, 600μm.

[0135] The thickness of the back electrode in the stacked perovskite solar cell can be 0.04-100μm, for example, 0.1μm, 0.5μm, 1μm, 5μm, 10μm, 20μm, 50μm, 100μm, 150μm, 200μm.

[0136] The present application provides a method for preparing a photoelectric device, which comprises the following steps:

[0137] (1) depositing a hole transport layer or an electron transport layer on the surface of a transparent conductive glass;

[0138] (2) depositing a perovskite thin film layer on the surface of the hole transport layer or the electron transport layer;

[0139] (3) depositing an electron transport layer or a hole transport layer on the surface of the perovskite thin film layer;

[0140] (4) depositing a back electrode on the surface of the electron transport layer or the hole transport layer to obtain a single-junction perovskite solar cell; or

[0141] (1') depositing a back electrode material and a tunneling layer on two surfaces of a bottom cell, respectively;

[0142] (2') depositing a hole transport layer or an electron transport layer on the surface of the tunneling layer

[0143] (3') depositing a perovskite thin film layer on the surface of the hole transport layer or the electron transport layer;

[0144] (4') depositing an electron transport layer or a hole transport layer on the surface of the perovskite thin film layer;

[0145] (5') depositing a top electrode on the surface of the electron transport layer or the hole transport layer to obtain a stacked perovskite solar cell.

[0146] In step (2) or step (3') of the method for preparing the photoelectric device, a perovskite precursor solution is deposited on the surface of the hole transport layer or the electron transport layer to obtain a perovskite thin film layer, and the perovskite precursor solution comprises raw materials of perovskite structure substances, an inorganic metal cyanate, and a solvent.

[0147] In the method for preparing the photoelectric device, the perovskite precursor solution can be prepared by mixing the raw materials of perovskite structure substances and the inorganic metal cyanate in the solvent.

[0148] In the method for preparing the photoelectric device, the solvent in the perovskite precursor solution can be one or more selected from N,N-dimethylformamide, dimethyl sulfoxide, N-methyl pyrrolidone, acetonitrile, 2-methoxyethanol, ethanol, and isopropanol.

[0149] In the method for preparing the photoelectric device, the concentration of the inorganic metal cyanate in the perovskite precursor solution can be 0.002-20 mg / mL, for example, 0.005 mg / mL, 0.01 mg / mL, 0.05 mg / mL, 0.1 mg / mL, 0.5 mg / mL, 1 mg / mL, 2 mg / mL, 3 mg / mL, 5 mg / mL, 10 mg / mL, 15 mg / mL, or 20 mg / mL. Controlling the concentration of the inorganic metal cyanate in the perovskite precursor solution within the above range is conducive to the film crystallization quality of the perovskite thin film and further conducive to improving the efficiency and stability of the photoelectric device containing the perovskite thin film.

[0150] The present application provides a method for preparing a single-junction perovskite solar cell of the present application, which comprises the following steps:

[0151] (1) depositing a hole transport layer material on the surface of a transparent conductive glass to obtain a hole transport layer;

[0152] (2) depositing a perovskite precursor solution on the surface of the hole transport layer to obtain a perovskite thin film layer;

[0153] (3) depositing an electron transport layer material on the surface of the perovskite thin film layer to obtain an electron transport layer;

[0154] (4) depositing a back electrode material on the surface of the electron transport layer to obtain a back electrode and a trans single-junction perovskite solar cell at the same time; or

[0155] (1') depositing an electron transport layer material on the surface of the transparent conductive glass to obtain an electron transport layer;

[0156] (2') depositing a perovskite precursor solution on the surface of the electron transport layer to obtain a perovskite thin film layer;

[0157] (3') depositing a hole transport layer material on the surface of the perovskite thin film layer to obtain a hole transport layer;

[0158] (4') depositing a back electrode material on the surface of the hole transport layer to obtain a back electrode and a formal single-junction perovskite solar cell at the same time.

[0159] In the method for preparing a single-junction perovskite solar cell, the deposition method of the hole transport layer can be spin coating, blade coating, physical vapor deposition (PVD), atomic layer deposition (ALD), slot coating or immersion; preferably, the physical vapor deposition can be magnetron sputtering, reactive plasma deposition, electron beam evaporation or thermal evaporation.

[0160] In the method for preparing a single-junction perovskite solar cell, the deposition method of the perovskite thin film layer can be spin coating, blade coating, electron beam evaporation, thermal evaporation, printing, spraying, spray pyrolysis or slot coating.

[0161] In the method for preparing a single-junction perovskite solar cell, the deposition method of the electron transport layer can be spin coating, blade coating, physical vapor deposition, atomic layer deposition, slot coating or immersion; preferably, the physical vapor deposition can be magnetron sputtering, reactive plasma deposition, electron beam evaporation or thermal evaporation.

[0162] In the method for preparing a single-junction perovskite solar cell, the preparation method of the perovskite precursor solution can be: mixing raw materials of perovskite structure substances and inorganic metal cyanate in a solvent to prepare a perovskite precursor solution.

[0163] In the method for preparing a single-junction perovskite solar cell, the solvent in the perovskite precursor solution can be one or more selected from N, N-dimethylformamide, dimethyl sulfoxide, N-methyl pyrrolidone, acetonitrile, 2-methoxyethanol, ethanol and isopropanol.

[0164] In the method for preparing the single-layer perovskite solar cell, the concentration of the inorganic metal cyanate in the perovskite precursor solution can be 0.002-20 mg / mL, for example, 0.005 mg / mL, 0.01 mg / mL, 0.05 mg / mL, 0.1 mg / mL, 0.5 mg / mL, 1 mg / mL, 2 mg / mL, 3 mg / mL, 5 mg / mL, 10 mg / mL, 15 mg / mL, or 20 mg / mL. The concentration of the inorganic metal cyanate in the perovskite precursor solution is controlled in the above range, which is beneficial to the film forming and crystallization quality of the perovskite thin film, and further beneficial to improving the efficiency and stability of the single-layer perovskite solar cell containing the perovskite thin film.

[0165] In the method for preparing the single-junction perovskite solar cell, the deposition mode of the back electrode can be physical vapor deposition, printing, spraying, or electroplating; preferably, the physical vapor deposition can be magnetron sputtering, reactive plasma deposition, electron beam evaporation, or thermal evaporation.

[0166] The application provides a method for preparing the laminated perovskite solar cell, and the method comprises the following steps:

[0167] (1) depositing a back electrode material and a tunnel layer material on two surfaces of a bottom cell respectively to obtain a back electrode and an electron transport layer;

[0168] (2) depositing a hole transport layer material on the surface of the tunnel layer to obtain a hole transport layer;

[0169] (3) depositing a perovskite precursor solution on the surface of the hole transport layer to obtain a perovskite thin film layer;

[0170] (4) depositing an electron transport layer material on the surface of the perovskite thin film layer to obtain an electron transport layer;

[0171] (5) depositing a top electrode material on the surface of the electron transport layer to obtain a top electrode and a trans-laminated perovskite solar cell; or

[0172] (1') depositing a back electrode material and a tunnel layer material on two surfaces of a bottom cell respectively to obtain a back electrode and a hole transport layer;

[0173] (2') depositing an electron transport layer material on the surface of the tunnel layer to obtain an electron transport layer;

[0174] (3') depositing a perovskite precursor solution on the surface of the electron transport layer to obtain a perovskite thin film layer;

[0175] (4') depositing a hole transport layer material on the surface of the perovskite thin film layer to obtain a hole transport layer;

[0176] (5') Depositing a top electrode material on the surface of the hole transport layer to obtain a top electrode and a formal perovskite solar cell with a stack structure;

[0177] In the present application, the top electrode can comprise a transparent electrode layer; preferably, the top electrode can comprise a grid electrode and a transparent electrode layer in sequence from the light-receiving front surface to the light-receiving back surface, more preferably, the top electrode can comprise a grid electrode, an anti-reflection layer and a transparent electrode layer in sequence from the light-receiving front surface to the light-receiving back surface.

[0178] In the method for preparing the perovskite solar cell with a stack structure, the deposition of the back electrode can be physical vapor deposition, printing, spraying or electroplating; preferably, the physical vapor deposition can be magnetron sputtering, reactive plasma deposition, electron beam evaporation or thermal evaporation.

[0179] In the method for preparing the perovskite solar cell with a stack structure, the deposition of the tunneling layer can be physical vapor deposition, monolayer deposition, chemical vapor deposition, plasma-enhanced chemical vapor deposition or electron beam evaporation; preferably, the physical vapor deposition can be magnetron sputtering, reactive plasma deposition, electron beam evaporation or thermal evaporation.

[0180] In the method for preparing the perovskite solar cell with a stack structure, the deposition of the hole transport layer can be spin coating, blade coating, physical vapor deposition, atomic layer deposition, slot coating or soaking; preferably, the physical vapor deposition can be magnetron sputtering, reactive plasma deposition, electron beam evaporation or thermal evaporation.

[0181] In the method for preparing the perovskite solar cell with a stack structure, the method for preparing the perovskite precursor solution can be mixing raw materials of perovskite structure substances and inorganic metal cyanate in a solvent to prepare the perovskite precursor solution.

[0182] In the method for preparing the perovskite solar cell with a stack structure, the solvent in the perovskite precursor solution can be one or more selected from N,N-dimethylformamide, dimethyl sulfoxide, N-methyl pyrrolidone, acetonitrile, 2-methoxyethanol, ethanol and isopropanol.

[0183] In the method for preparing the perovskite solar cell with a stack structure, the concentration of the inorganic metal cyanate in the perovskite precursor solution can be 0.002-20 mg / mL, for example, 0.005 mg / mL, 0.01 mg / mL, 0.05 mg / mL, 0.1 mg / mL, 0.5 mg / mL, 1 mg / mL, 2 mg / mL, 3 mg / mL, 5 mg / mL, 10 mg / mL, 15 mg / mL or 20 mg / mL. Controlling the concentration of the inorganic metal cyanate in the perovskite precursor solution within the above range is conducive to the film forming and crystallization quality of the perovskite thin film, and further conducive to improving the efficiency and stability of the perovskite solar cell with a stack structure comprising the perovskite thin film.

[0184] In the method for preparing the laminated perovskite solar cell, the deposition method of the perovskite thin film layer can be spin coating, blade coating, electron beam evaporation, thermal evaporation, printing, spraying, spray pyrolysis or slot coating.

[0185] In the method for preparing the laminated perovskite solar cell, the deposition method of the electron transport layer can be spin coating, blade coating, physical vapor deposition, atomic layer deposition, slot coating or immersion; preferably, the physical vapor deposition can be magnetron sputtering, reactive plasma deposition, electron beam evaporation or thermal evaporation.

[0186] In the method for preparing the laminated perovskite solar cell, the deposition method of the transparent electrode layer can be physical vapor deposition; preferably, the physical vapor deposition can be magnetron sputtering, reactive plasma deposition, electron beam evaporation or thermal evaporation.

[0187] In the method for preparing the laminated perovskite solar cell, the deposition method of the anti-reflection layer can be physical vapor deposition; preferably, the physical vapor deposition can be magnetron sputtering, reactive plasma deposition, electron beam evaporation or thermal evaporation.

[0188] In the method for preparing the laminated perovskite solar cell, the deposition method of the grid electrode can be thermal evaporation, printing or electroplating.

[0189] Compared with the prior art, the present application has the following beneficial effects:

[0190] (1) By adding inorganic metal cyanate additives to the solution containing perovskite structure substances, the present application can significantly improve the film forming quality of the perovskite thin film, thereby improving the efficiency of the perovskite device;

[0191] (2) By doping specific inorganic metal ions into the perovskite crystal structure, the present application reduces lattice defects and forms a more stable crystal structure, thereby improving the stability of the device;

[0192] (3) The present application significantly improves the efficiency and stability of perovskite devices prepared by different components and different methods, and has significant advantages in single-junction and laminated cells.

[0193] The present application will be described below in the manner of specific examples. It should be understood that these examples are merely illustrative and are not intended to limit the scope of the present application. The methods, reagents and materials used in the examples are conventional in the art unless otherwise specified. The raw material compounds in the examples can be purchased through commercial channels.

[0194] Example 1

[0195] The perovskite film is prepared in the embodiment, and the specific steps are as shown below.

[0196] 88.3 mg of cesium iodide (Csl), 233.9 mg of formamidinium iodide (FAI), 187.2 mg of lead bromide (PbBr2), 548.6 mg of lead iodide (PbI2) and sodium cyanate are taken and dissolved in a mixed solvent of 900 μL of DMF and 100 μL of DMSO, and after being fully dissolved, a 250 μm oily filter head is used for filtration to obtain a perovskite precursor solution, and the perovskite precursor solution contains 1.7 mol / L of FA 0.8 Cs 0.2 Pb(I 0.8 Br 0.2 )3 and 1 mg / mL of sodium cyanate; a perovskite film layer is prepared on a clean glass substrate by using a slot coating method, and the specific operation is as follows: the height of the slot coating doctor blade from the glass substrate is 100 μm, the angle of the air knife is 45°, the air knife gas pressure is 0.5 MPa, the doctor blade moving speed is 5 mm / s, the air knife moving speed is 20 mm / s, the injection speed is 5 μL / s, and after the film is scraped, the film is transferred to a heating plate at 100 ℃ for annealing for 10 min to obtain a perovskite film layer, and the thickness of the perovskite film layer is 1500 nm.

[0197] Example 2

[0198] The other conditions in the embodiment are the same as those in example 1, and the only difference is that in the embodiment, the sodium cyanate in the perovskite precursor solution is replaced by potassium cyanate, and the concentration of the potassium cyanate is 0.5 mg / mL.

[0199] Example 3

[0200] The other conditions in the embodiment are the same as those in example 1, and the only difference is that in the embodiment, the sodium cyanate in the perovskite precursor solution is replaced by rubidium cyanate, and the concentration of the rubidium cyanate is 10 mg / mL.

[0201] Example 4

[0202] The other conditions in the embodiment are the same as those in example 1, and the only difference is that in the embodiment, the sodium cyanate in the perovskite precursor solution is replaced by cesium cyanate, and the concentration of the cesium cyanate is 20 mg / mL.

[0203] Example 5

[0204] The other conditions in the embodiment are the same as those in example 1, and the only difference is that in the embodiment, the sodium cyanate in the perovskite precursor solution is replaced by calcium cyanate, and the concentration of the calcium cyanate is 0.1 mg / mL.

[0205] Example 6

[0206] The other conditions of this example are the same as those of Example 1, except that in this example, sodium cyanate in the perovskite precursor solution is replaced by zinc cyanate, and the concentration of zinc cyanate is 0.2 mg / mL.

[0207] Example 7

[0208] The other conditions of this example are the same as those of Example 1, except that in this example, sodium cyanate in the perovskite precursor solution is replaced by cobalt cyanate, and the concentration of cobalt cyanate is 0.002 mg / mL.

[0209] Example 8

[0210] The other conditions of this example are the same as those of Example 1, except that in this example, sodium cyanate in the perovskite precursor solution is replaced by europium cyanate, and the concentration of europium cyanate is 5 mg / mL.

[0211] Example 9

[0212] The other conditions of this example are the same as those of Example 1, except that in this example, sodium cyanate in the perovskite precursor solution is replaced by cerium cyanate, and the concentration of cerium cyanate is 3 mg / mL.

[0213] Comparative Example 1

[0214] The other conditions of this comparative example are the same as those of Example 1, except that in this comparative example, the perovskite precursor solution does not contain inorganic metal cyanate.

[0215] Example 10

[0216] This example prepares a single-junction perovskite solar cell with a structure as shown in FIG. 1, and the specific steps are as follows:

[0217] 1. Dissolve [2-(3,6-dimethoxy-9H-carbazol-9-yl)ethyl] phosphonic acid (MeO-2PACZ) in ethanol to prepare a MeO-2PACZ solution with a concentration of 1 mmol / mL. Take 130 μL of the MeO-2PACZ solution and drop it on a clean ITO glass with a size of 2.5 cm*2.5 cm, then spin coat at a speed of 4000 rpm for 15 s. After spin coating, transfer it to a heating plate at 100°C for annealing for 10 min, then take it off to obtain a hole transport layer with a thickness of 2 nm.

[0218] 2. Dissolve 19.5 mg of cesium iodide (CsI), 232.2 mg of formamidinium iodide (FAI), 11.9 mg of methylammonium iodide (MAI), 691.5 mg of lead iodide (PbI2), and sodium cyanate in 800 μL of a mixed solvent of DMF and 200 μL of DMSO. After complete dissolution, filter using a 250 μm oil filter to obtain a perovskite precursor solution. The perovskite precursor solution contains 1.5 mol / L of FA0.9 MA 0.05 Cs 0.05 PbI3(FAMACs) and 1 mg / mL of sodium cyanate; the perovskite thin film layer was prepared by spin coating as follows: the perovskite precursor solution was placed in a glove box for spin coating, 100 μL of the perovskite precursor solution was first added dropwise on the surface of the hole transport layer, spin coating was performed according to a process of 2000 rpm for 10 s and 6000 rpm for 30 s for a total of 40 s, 300 μL of anisole solution (anti-solvent) was taken up by a 1 μL pipette gun head, and the anisole solution was added dropwise when the perovskite solution was spin coated for 30 s, after spin coating was stopped, the thin film was taken off the spin coater, and heated on a hot plate at 100 °C for 10 min to obtain the perovskite thin film layer, the thickness of the perovskite thin film layer was 600 nm;

[0219] 3. Fullerene (C60) was deposited on the surface of the perovskite thin film layer by thermal evaporation to obtain a fullerene layer, the thickness of the fullerene layer was 25 nm; tin dioxide (SnO2) was deposited on the surface of the fullerene layer by atomic layer deposition to obtain a tin dioxide layer, the thickness of the tin dioxide layer was 20 nm, the fullerene layer and the tin dioxide layer together constituted an electron transport layer, during the thermal evaporation process, the temperature of the evaporation source was 450 °C, and the evaporation rate was 0.1 A / s;

[0220] 4. Metal copper was deposited on the surface of the electron transport layer by thermal evaporation to obtain a back electrode, and at the same time to obtain a single-junction perovskite solar cell, the thickness of the back electrode was 200 nm.

[0221] Example 11

[0222] The other conditions of this example were the same as those of Example 10, except that in this example, sodium cyanate in the perovskite precursor solution was replaced by potassium cyanate, and the concentration of potassium cyanate was 0.2 mg / mL.

[0223] Example 12

[0224] The other conditions of this example were the same as those of Example 10, except that in this example, sodium cyanate in the perovskite precursor solution was replaced by rubidium cyanate, and the concentration of rubidium cyanate was 0.5 mg / mL.

[0225] Example 13

[0226] The other conditions of this example were the same as those of Example 10, except that in this example, sodium cyanate in the perovskite precursor solution was replaced by cesium cyanate, and the concentration of cesium cyanate was 10 mg / mL.

[0227] Comparative Example 2

[0228] The other conditions of this comparative example were the same as those of Example 10, except that in this comparative example, the solute in the perovskite precursor solution was only FAMACs, and did not contain sodium cyanate.

[0229] Example 14

[0230] The other conditions of this example are the same as those of Example 1, except that in this example, step (2) is as follows: 77.9 mg of cesium iodide (Csl), 206.4 mg of formamidinium iodide (FAI), 691.5 mg of lead iodide (Pbl2), and calcium cyanate are dissolved in a mixed solvent of 800 μL of DMF and 200 μL of DMSO, and after being dissolved sufficiently, a 250 μm oil filter is used for filtration to obtain a perovskite precursor solution, which contains 1.5 mol / L of FA 0.8 Cs 0.2 Pbl3(FAcs) and 2 mg / mL of calcium cyanate; a perovskite thin film layer is prepared by a slot coating method, and the specific operation is as follows: the height of the slot coating doctor blade from the glass substrate is 100 μm, the angle of the air knife is 45°, the air knife gas pressure is 1 MPa, the doctor blade moving speed is 15 mm / s, the air knife moving speed is 10 mm / s, the injection speed is 7.5 μL / s, and after the thin film is scraped, the thin film is transferred to a hot plate at 100°C for annealing for 10 min to obtain a perovskite thin film layer, and the thickness of the perovskite thin film layer is 2000 nm.

[0231] Example 15

[0232] The other conditions of this example are the same as those of Example 14, except that in this example, calcium cyanate in the perovskite precursor solution is replaced by zinc cyanate, and the concentration of the zinc cyanate is 0.5 mg / mL.

[0233] Example 16

[0234] The other conditions of this example are the same as those of Example 14, except that in this example, calcium cyanate in the perovskite precursor solution is replaced by europium cyanate, and the concentration of the europium cyanate is 0.2 mg / mL.

[0235] Example 17

[0236] The other conditions of this example are the same as those of Example 14, except that in this example, calcium cyanate in the perovskite precursor solution is replaced by cerium cyanate, and the concentration of the cerium cyanate is 1 mg / mL.

[0237] Comparative Example 3

[0238] The other conditions of this comparative example are the same as those of Example 14, except that in this comparative example, the solute in the perovskite precursor solution is only FACs, and does not contain calcium cyanate.

[0239] Example 18

[0240] The structure of the crystalline silicon / perovskite stacked solar cell of this example is shown in FIG. 3, and the preparation process is as follows:

[0241] 1. Preparation of the bottom cell: using a plasma enhanced chemical vapor deposition (PECVD) process, depositing intrinsic amorphous silicon layers (a-Si(i)) on both sides of the intrinsic silicon layer (c-Si(n)) at 200°C to obtain a passivation layer, then depositing n-type microcrystalline silicon layers and p-type microcrystalline silicon layers on both sides of the passivation layer to obtain an electron transport layer (nc-Si(p)) and a hole transport layer (nc-Si(p)) respectively, and then obtaining a bottom cell, the thickness of the bottom cell is 300 μm;

[0242] 2. Preparation of the back electrode and the tunneling layer: depositing ITO on the surface of the p-type microcrystalline silicon layer by magnetron sputtering to obtain a transparent electrode layer with a thickness of 80 nm, printing silver on the surface of the transparent electrode layer by printing to obtain a silver grid line electrode with a height of 20 μm and a width of 30 μm, and the transparent electrode layer and the silver grid line electrode constitute the back electrode; depositing ITO on the surface of the n-type microcrystalline silicon layer by magnetron sputtering to obtain a tunneling layer with a thickness of 20 nm;

[0243] 3. Dissolve [2-(3,6-dimethoxy-9H-carbazol-9-yl)ethyl] phosphonic acid (MeO-2PACZ) in ethanol to prepare a MeO-2PACZ solution with a concentration of 1 mmol / mL, take 130 μL of the MeO-2PACZ solution and drop it on the surface of the tunneling layer ITO, then spin-coat at a speed of 4000 rpm for 15 s, after spin-coating, transfer it to a heating plate at 100°C for annealing for 10 min, then take it off to obtain a hole transport layer, the thickness of the hole transport layer is 2 nm;

[0244] 4. Dissolve 88.3 mg of cesium iodide (CsI), 233.9 mg of formamidinium iodide (FAI), 187.2 mg of lead bromide (PbBr2), 548.6 mg of lead iodide (PbI2), and calcium cyanate in 800 μL of a mixed solvent of DMF and 200 μL of DMSO, filter with a 250 μm oil filter after fully dissolving to obtain a perovskite precursor solution, the perovskite precursor solution contains 1.7 mol / L of FA 0.8 Cs 0.2 Pb(I 0.8 Br 0.2 )3 and 2 mg / mL of copper cyanide; prepare a perovskite film layer by doctor blade method; the specific operation is as follows: take 10 μL of the perovskite precursor solution and drop it on the doctor blade tip, the moving speed of the doctor blade is 5-30 mm / s, the doctor blade height is 50-150 um, after scraping, use N2 gas knife to blow, the air pressure is 0.5-1.5 Mpa, the moving speed is 5-30 mm / s, after blowing, transfer the perovskite film to a heating plate at 100°C for annealing for 10 min to obtain a perovskite film layer, the thickness of the perovskite film layer is 1500 nm;

[0245] 5. Fullerene (C60) is deposited on the surface of the perovskite thin film layer by thermal evaporation to obtain a fullerene layer, the thickness of the fullerene layer being 12 nm; tin dioxide (SnO2) is deposited on the surface of the fullerene layer by atomic layer deposition to obtain a tin dioxide layer, the thickness of the tin dioxide layer being 20 nm, the fullerene layer and the tin dioxide layer together forming an electron transport layer, in the thermal evaporation process, the temperature of the evaporation source being 450°C, and the evaporation rate being 0.1 A / s;

[0246] 6. IZO is deposited on the surface of the electron transport layer by magnetron sputtering to obtain a transparent conductive layer, the thickness of the transparent conductive layer being 70 nm; MgF2 is deposited on the surface of the transparent conductive layer by thermal evaporation to obtain an anti-reflection layer, the thickness of the anti-reflection layer being 120 nm; finally, silver is deposited on the surface of the anti-reflection layer by thermal evaporation to obtain a silver grid line electrode with a thickness of 800 nm, the transparent conductive layer, the anti-reflection layer and the silver grid line electrode together forming a top electrode, and a crystalline silicon / perovskite laminated solar cell is obtained.

[0247] Example 19

[0248] The other conditions of this example are the same as those of Example 18, except that in this example, copper cyanate in the perovskite precursor solution is replaced by cobalt cyanate, and the concentration of the cobalt cyanate is 1 mg / mL.

[0249] Comparative Example 4

[0250] The other conditions of this comparative example are the same as those of Example 18, except that in this comparative example, the solute in the perovskite precursor solution is only FA 0.8 Cs 0.2 Pb(I 0.8 Br 0.2 )3, and does not contain copper cyanate.

[0251] Test Example

[0252] Crystallization test of the perovskite thin film layer: the perovskite thin films prepared in Examples 1-3, Example 6, Examples 8-9 and Comparative Example 1 are subjected to X-ray diffraction, the X-ray diffractometer being a D2X X-ray diffractometer of Bruker, the energy of the X-ray being 8 keV, the angle range for testing being 5° to 30°, and the step speed for testing being 0.02° / s, and the test results are shown in FIG. 4; the perovskite thin films prepared in Examples 1-9 and Comparative Example 1 are subjected to fluorescence test, the excitation light wavelength of the fluorescence being 450 nm, the test camera being a CCD camera, the pixel size being 20 μm, and the integral time for testing being 2 s, and the test results are shown in FIG. 5.

[0253] Initial performance test of perovskite solar device: the current output of the perovskite solar cells prepared from Examples 10-19 and Comparative Examples 2-4 under different voltages was tested using a solar simulator with the voltage range set to 2 V to -0.5 V at 25 °C under AM1.5G standard solar spectrum, and the corresponding current-voltage (I-V) characteristic curves were plotted, wherein the cell surface area was 1.1664 cm 2 and the incident light power (Pin) was 100 mW / cm 2 At this time, the characteristic curve is the initial performance characteristic curve, and the initial performance (initial open-circuit voltage, initial short-circuit current density, initial fill factor and initial photoelectric conversion efficiency) of the perovskite solar cells prepared from Examples 10-19 and Comparative Examples 2-4 is obtained according to the initial performance characteristic curve.

[0254] (1) Open-circuit voltage (Voc): the voltage value corresponding to the current equal to zero.

[0255] (2) Short-circuit current density (Jsc): the current value when the voltage is zero is the short-circuit current (Isc), and the current size on the unit cell surface area is the short-circuit current density.

[0256] (3) Fill factor (FF): the ratio of the maximum output power (Pmax) of the cell to the product of the open-circuit voltage and the short-circuit current, the calculation formula is (Pmax / Voc*Isc), wherein the maximum power point is the point at which the cell output power reaches the maximum value.

[0257] (4) Photoelectric conversion efficiency (PCE): the photoelectric conversion efficiency refers to the ratio of the maximum output power to the incident light power (Pin), and the calculation formula is (Pmax / Pin)*100%.

[0258] Aging performance test of perovskite solar device: the perovskite solar cells prepared from Examples 10-19 and Comparative Examples 2-4 were aged for 100 h at 85 °C under open-circuit AM1.5G, and the current output of the perovskite solar cells prepared from Examples 10-19 and Comparative Examples 2-4 under different voltages was tested using a solar simulator with the voltage range set to 2 V to -0.5 V, and the corresponding current-voltage (I-V) characteristic curves were plotted, wherein the cell surface area was 1.1664 cm 2 and the incident light power (Pin) was 100 mW / cm 2 At this time, the characteristic curve is the aging performance characteristic curve, and the aging performance (aged open-circuit voltage, aged short-circuit current density, aged fill factor and aged photoelectric conversion efficiency) of the perovskite solar cells prepared from Examples 10-19 and Comparative Examples 2-4 is obtained according to the aging performance characteristic curve.

[0259] Efficiency ratio of perovskite solar device: efficiency ratio = initial photoelectric conversion efficiency / aged photoelectric conversion efficiency x 100%.

[0260] The test results of initial performance, aging performance and efficiency ratio of the single-junction perovskite solar cells prepared in Examples 10-17 and Comparative Examples 2-3 are shown in Table 1; the test results of initial performance, aging performance and efficiency ratio of the tandem perovskite solar cells prepared in Examples 18-19 and Comparative Example 4 are shown in Table 2.

[0261] Table 1: initial performance, aging performance and efficiency ratio of the single-junction perovskite solar cells prepared in Examples 10-17 and Comparative Examples 2-3

[0262] Table 2: initial performance, aging performance and efficiency ratio of the tandem perovskite solar cells prepared in Examples 18-19 and Comparative Example 4

[0263] Figure 4 is the X-ray diffraction pattern of the perovskite thin films prepared in Examples 1-3, Example 6, Examples 8-9 and Comparative Example 1, from which it can be seen that the peak at 14.2° represents the peak of perovskite, and the stronger the peak, the higher the crystallinity of perovskite. The inorganic metal cyanate additives of the present application can significantly improve the crystalline quality of perovskite.

[0264] Figure 4 is the fluorescence pattern of the perovskite thin films prepared in Examples 1-9 and Comparative Example 1. The improvement of perovskite film crystalline quality will ultimately manifest in the reduction of non-radiative recombination of the thin film, which can be distinguished by the fluorescence intensity. The stronger the fluorescence, the lower the non-radiative recombination. As can be seen from Figure 5, although the perovskite thin films with inorganic metal cyanate additives have different degrees of improvement in fluorescence intensity, they all bring different degrees of improvement to the perovskite thin film, among which potassium cyanate, cesium cyanate, calcium cyanate, europium cyanate and cerium cyanate can significantly improve the fluorescence intensity.

[0265] As can be seen from Table 1, compared with Comparative Example 2 in which no additive is added to the perovskite thin film, the efficiency and stability of Examples 10-13 in which inorganic metal cyanate additives are added to the perovskite thin film are higher. Compared with Comparative Example 3 in which no additive is added to the perovskite thin film, the efficiency and stability of Examples 14-17 in which inorganic metal cyanate additives are added to the perovskite thin film are higher. It can be seen that the inorganic metal cyanate additives of the present application can improve the efficiency and stability of perovskite devices. Further, the preparation method of the perovskite thin film of Examples 10-13 and Comparative Example 2 is spin coating, and the components contain MA; the preparation method of the perovskite thin film of Examples 14-17 and Comparative Example 3 is slot coating, and the components do not contain MA. It can be seen that the present application has significantly improved the efficiency and stability of perovskite devices prepared by different components and different methods.

[0266] As can be seen from Table 2, compared with the comparative example 4 without the inorganic metal cyanate additive in the perovskite film, the efficiency and stability of the examples 18-19 with the inorganic metal cyanate additive in the perovskite film are higher. The perovskite films of the examples 10-17 and the comparative examples 2-3 are located in the single-junction perovskite solar cells, and the perovskite films of the examples 18-19 and the comparative example 4 are located in the tandem perovskite solar cells, thus it can be known that the single-junction perovskite solar cells and the tandem perovskite solar cells of the present application have significant improvement in the efficiency and stability.

[0267] In summary, the inorganic metal cyanate improves the crystallization quality of the perovskite, thereby reducing the non-radiative recombination in the perovskite film, and finally improving the performance of the perovskite device.

Claims

1. A perovskite thin film, characterized in that, The perovskite film comprises a perovskite structural material and an inorganic metal cyanate, wherein the metal in the inorganic metal cyanate is selected from one or more of alkali metals, alkaline earth metals, transition metals, and rare earth metals.

2. The perovskite thin film as described in claim 1, characterized in that, The perovskite thin film has one or more of the following characteristics: The inorganic metal cyanate is selected from one or more of lithium cyanate, sodium cyanate, potassium cyanate, rubidium cyanate, cesium cyanate, magnesium cyanate, calcium cyanate, barium cyanate, zinc cyanate, cobalt cyanate, copper cyanate, europium cyanate, cerium cyanate, and lanthanum cyanate. The chemical formula of the perovskite structure is ABX3, wherein A is a monovalent cation, including one or more of cesium, rubidium, methylamino and formamidinyl; B is a divalent cation, including one or more of lead, copper, zinc, gallium, tin and calcium; and X is a monovalent anion, including one or more of iodine, bromine, chloride, fluorine, thiocyanate, tetrafluoroborate, hexafluorophosphate, formate and acetate. The mass ratio of the inorganic metal cyanate to the perovskite structure material is ≤5.5%; The thickness of the perovskite thin film is 200–10000 nm.

3. A method for preparing perovskite thin films, characterized in that, The method includes the following steps: mixing the raw materials of the perovskite structure material and the inorganic metal cyanate in a solvent to prepare a perovskite precursor solution, depositing the perovskite precursor solution to obtain a perovskite thin film.

4. The method as described in claim 3, characterized in that, The method has one or more of the following characteristics: The solvent is selected from one or more of N,N-dimethylformamide, dimethyl sulfoxide, N-methylpyrrolidone, acetonitrile, 2-methoxyethanol, ethanol and isopropanol; The method for depositing the perovskite precursor solution is spin coating, blade coating, electron beam evaporation, thermal evaporation, printing, spraying, spray pyrolysis, or slot coating. The concentration of the inorganic metal cyanate in the perovskite precursor solution is 0.002-20 mg / mL.

5. An optoelectronic device, characterized in that, The optoelectronic device comprises a perovskite thin film, which contains a perovskite structural material and an inorganic metal cyanate.

6. The optoelectronic device as described in claim 5, characterized in that, The perovskite solar devices include single-junction perovskite solar cells and / or tandem perovskite solar cells.

7. The optoelectronic device as described in claim 5, characterized in that, In the single-junction perovskite solar cell or the tandem perovskite solar cell, the thickness of the perovskite thin film is 200-3000 nm.

8. A method for preparing the optoelectronic device according to any one of claims 5-7, characterized in that, The method includes the following steps: (1) Deposit a hole transport layer or an electron transport layer on the surface of a transparent conductive glass; (2) Deposit a perovskite thin film on the surface of the hole transport layer or electron transport layer; (3) Deposit an electron transport layer or a hole transport layer on the surface of the perovskite thin film; (4) Deposit a back electrode on the surface of the electron transport layer or hole transport layer to obtain a single-junction perovskite solar cell; or (1') Deposit back electrode material and tunneling layer on the two surfaces of the bottom cell, respectively; (2') Deposit a hole transport layer or an electron transport layer on the surface of the tunneling layer. (3') Deposit a perovskite thin film on the surface of the hole transport layer or electron transport layer; (4') Deposit an electron transport layer or a hole transport layer on the surface of the perovskite thin film; (5') A top electrode is deposited on the surface of the electron transport layer or hole transport layer to obtain a stacked perovskite solar cell.

9. The method as described in claim 8, characterized in that, The method has one or more of the following characteristics: In step (2) or step (3'), a perovskite precursor solution is deposited on the surface of the hole transport layer or electron transport layer to obtain a perovskite thin film layer. The perovskite precursor solution includes raw materials of perovskite structural material, inorganic metal cyanate and solvent.

10. The method as described in claim 7, characterized in that, The method has one or more of the following characteristics: The perovskite precursor solution is prepared by mixing the raw materials of the perovskite structure and inorganic metal cyanate in a solvent to obtain the perovskite precursor solution. The solvent is selected from one or more of N,N-dimethylformamide, dimethyl sulfoxide, N-methylpyrrolidone, acetonitrile, 2-methoxyethanol, ethanol and isopropanol; The concentration of the inorganic metal cyanate in the perovskite precursor solution is 0.002-20 mg / mL; The deposition method of the perovskite thin film layer is spin coating, blade coating, electron beam evaporation, thermal evaporation, printing, spraying, spray pyrolysis, or slot coating.

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