KR101654470B1 - Method of forming uniform perovsktie light absorbing layer, and solar cell comprising uniform perovsktie light absorbing layer - Google Patents

Method of forming uniform perovsktie light absorbing layer, and solar cell comprising uniform perovsktie light absorbing layer Download PDF

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KR101654470B1
KR101654470B1 KR1020150070850A KR20150070850A KR101654470B1 KR 101654470 B1 KR101654470 B1 KR 101654470B1 KR 1020150070850 A KR1020150070850 A KR 1020150070850A KR 20150070850 A KR20150070850 A KR 20150070850A KR 101654470 B1 KR101654470 B1 KR 101654470B1
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light absorbing
absorbing layer
forming
uniform
layer
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KR1020150070850A
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정현석
권승리
김병조
이동건
진영운
한길상
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성균관대학교산학협력단
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    • H—ELECTRICITY
    • H01—ELECTRIC ELEMENTS
    • H01L—SEMICONDUCTOR DEVICES NOT COVERED BY CLASS H10
    • H01L31/00—Semiconductor devices sensitive to infrared radiation, light, electromagnetic radiation of shorter wavelength or corpuscular radiation and specially adapted either for the conversion of the energy of such radiation into electrical energy or for the control of electrical energy by such radiation; Processes or apparatus specially adapted for the manufacture or treatment thereof or of parts thereof; Details thereof
    • H01L31/02—Details
    • H01L31/0216—Coatings
    • H01L31/02161—Coatings for devices characterised by at least one potential jump barrier or surface barrier
    • H01L31/02167—Coatings for devices characterised by at least one potential jump barrier or surface barrier for solar cells
    • H01L31/02168—Coatings for devices characterised by at least one potential jump barrier or surface barrier for solar cells the coatings being antireflective or having enhancing optical properties for the solar cells
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    • C01—INORGANIC CHEMISTRY
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    • H—ELECTRICITY
    • H01—ELECTRIC ELEMENTS
    • H01L—SEMICONDUCTOR DEVICES NOT COVERED BY CLASS H10
    • H01L31/00—Semiconductor devices sensitive to infrared radiation, light, electromagnetic radiation of shorter wavelength or corpuscular radiation and specially adapted either for the conversion of the energy of such radiation into electrical energy or for the control of electrical energy by such radiation; Processes or apparatus specially adapted for the manufacture or treatment thereof or of parts thereof; Details thereof
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Abstract

The present invention relates to a method for fabricating a perovskite optical absorber using a MO sol-gel method. The present invention enables the production of a uniform perovskite optical absorption layer through the formation of MX 2 , a precursor of the perovskite optical absorber based on the MO sol-gel method. The perovskite solar cell produced by this technology provides excellent solar cell characteristics with a uniform perovskite thin film.

Description

TECHNICAL FIELD [0001] The present invention relates to a method of forming a uniform perovskite light absorbing layer and a solar cell including a uniform perovskite light absorbing layer,

The present invention relates to a method for forming a uniform perovskite light absorbing layer, and more particularly to a method for forming a uniform perovskite light absorbing layer using MO (M is a bivalent metal or rare earth metal) sol-gel method .

The term "solar cell" refers to a cell that generates a current-voltage using the photovoltaic effect of absorbing light energy from sunlight to generate electrons and holes.

In order to manufacture solar cells at a low cost, it is necessary to drastically reduce the cost of materials or manufacturing processes used as core materials for solar cells. As an alternative to inorganic semiconductor-based solar cells, dye-sensitized solar cells Cells and organic solar cells have been actively studied. In recent years, silicon-based, organic dye-based, and newly perovskite-based solar cells have been competing in the development of solar cells. Currently, perovskite- It is attracting attention as a promising solar technology.

Perovskite has a special crystal structure such as calcium titanium dioxide. The organic-inorganic composite light absorber having such a structure enables a high charge carrier mobility and a long diffusion distance in the solar cell, And as a result, electrons and holes can pass through thicker solar cells, absorbing more light.

The CH 3 NH 3 PbI 3 perovskite light absorber used as a light absorbing and activating material of the perovskite solar cell has a high possibility of developing an ultra-low-cost low-cost solar cell based on the high extinction coefficient characteristic.

AMX 3 (A = organic compound, M = metal element, X = halogen element) material used as a light absorbing layer of a perovskite solar cell has a high possibility of developing a high efficiency solar cell based on its high extinction coefficient characteristic. At present, perovskite thin film formation method easily forms CH 3 NH 3 PbI 3 by direct application of PbI 2 solution and subsequent reaction with methlyamine iodide (MAI). However, direct application of the PbI 2 solution is not easy to penetrate into the porous particles of the electron collecting layer such as TiO 2, and it is difficult to form a uniform thin film on a flat substrate.

Due to these problems, the efficiency of the solar cell is greatly reduced, for example, pin holes are formed in the perovskite thin film when reacted with MAI. In particular, it is difficult to apply complicated nanostructures (nanorod, nanotube, nanowire), which limits its application.

In addition, in the case of the conventional method, there is a problem that it is difficult to control the thickness at a scale of several tens of nanometers in order to manufacture a uniform thin film, and a solution has been required.

The present invention aims at solving the problem that a conventional non-uniform MX 2 thin film is formed and a uniform perovskite light absorption layer can not be formed by a new method. According to the present invention, a uniform perovskite light absorbing layer is formed by forming a uniform MX 2 thin film through MO sol-gel coating.

A method of forming a uniform perovskite light absorbing layer according to an embodiment of the present invention includes: preparing a substrate; Forming a metal oxide electron collecting layer on the substrate; Forming a MO (M is a bivalent metal or rare earth metal) thin film layer on the metal oxide electron collecting layer; Replacing O in the MO thin film layer with a halogen atom to form MX 2 (X = halogen atom); And reacting MX 2 with a methylamine halide to form a perovskite light absorbing layer.

In this case, X is any one of I, Br and Cl, and M is any one of Pb, Sn, Cu, Cr, Mn, Pd, Cd and Eu.

The step of forming the MO thin film layer on the metal oxide electron collecting layer is formed using a MO sol-sel method. In this case, the MO sol-gel method comprises: preparing a precursor of M, putting it in a solvent capable of dissolving the M precursor, and spin-coating the solution obtained by stirring; And baking and heat treating the spin-coated solution.

In the step of replacing the O of the MO thin film layer with a halogen atom to form MX 2 (X = halogen atom), the substrate having the MO thin film layer formed thereon in the HX solution is dipped and heat treated by flowing the X 2 gas. The step of heat-treating the substrate with the X 2 gas is performed in an Ar atmosphere at a temperature of 150 to 350 ° C. The substrate having the MO thin film layer formed thereon is dipped and then heat-treated in an air atmosphere at 60 to 150 ° C. .

Forming a perovskite light absorbing layer is reacted with methylamine halide the MX 2 is methylamine halogen onto methylamine halogen substrate the MX 2 dipping the substrate is formed or provided that the MX 2 in the storage solution Cargo is spin coated and heat treated. The heat treatment is performed at a temperature of 100 to 150 캜.

According to the present invention, a uniform perovskite optical absorption layer can not be formed due to the formation of a non-uniform MX 2 thin film. The MO thin film is formed by the MO sol-gel coating method to form an oxygen atom (O) Substituted by a halogen atom. According to this method, a perovskite light absorbing layer without a pinhole can be formed, thereby realizing an excellent perovskite solar cell.

Further, according to the method of the present invention, it is possible to easily control the thickness of several tens nanoseconds in the production of a uniform thin film.

FIG. 1 shows a flowchart of a method of forming a uniform perovskite light absorbing layer using the MO sol-gel method according to an embodiment of the present invention.
2 is a cross-sectional schematic diagram of a perovskite solar cell structure according to an embodiment of the present invention.
3 is a schematic view illustrating a process of forming a perovskite thin film according to an embodiment of the present invention.
4 is a comparative photograph of PbI 2 prepared according to the present invention and PbI 2 prepared in the prior art.
FIG. 5 shows X-ray diffraction results to confirm that the PbO thin film was substituted with the PbI 2 thin film according to the present invention.
FIG. 6 is a graph showing a voltage-current density relationship between a solar cell manufactured according to the present invention and a conventional solar cell.
Various embodiments are now described with reference to the drawings, wherein like reference numerals are used throughout the drawings to refer to like elements. For purposes of explanation, various descriptions are set forth herein to provide an understanding of the present invention. It is evident, however, that such embodiments may be practiced without these specific details. In other instances, well-known structures and devices are shown in block diagram form in order to facilitate describing the embodiments.

The following description provides a simplified description of one or more embodiments in order to provide a basic understanding of embodiments of the invention. This section is not a comprehensive overview of all possible embodiments and is not intended to identify key elements or to cover the scope of all embodiments of all elements. Its sole purpose is to present the concept of one or more embodiments in a simplified form as a prelude to the more detailed description that is presented later.

The present invention relates to a method for fabricating a perovskite optical absorber using a MO sol-gel method. The present invention enables the production of a uniform perovskite optical absorption layer through the formation of MX 2 , a precursor of the perovskite optical absorber based on the MO sol-gel method. The perovskite solar cell produced by this technology provides excellent solar cell characteristics with a uniform perovskite thin film.

In the specification of the present invention, M means a bivalent metal or a rare earth metal. Specifically, M is any one of Pb, Sn, Cu, Cr, Mn, Pd, Cd and Eu.

FIG. 1 is a flowchart illustrating a method of forming a uniform perovskite light absorbing layer using the MO sol-gel method according to an embodiment of the present invention. FIG. 2 is a cross- Sectional structure of the solar cell structure. 3 is a schematic view illustrating a process of forming a perovskite thin film according to an embodiment of the present invention. In the embodiment of the present invention, P was used as M.

As shown in FIG. 2, a general structure of a perovskite solar cell includes a substrate; Conductive layer; An electron collection layer; A light absorbing layer; A hole transporting layer; It is obvious to a person skilled in the art that a hole blocking layer and the like may be included in addition to the electrode.

Referring to FIG. 1, a method of forming a uniform perovskite light absorbing layer according to an embodiment of the present invention includes: preparing a substrate (S 110); Forming a metal oxide electron collecting layer on the substrate (S 120); Forming a MO thin film layer on the metal oxide electron collecting layer (S 130); Replacing O in the MO thin film layer with a halogen atom to form MX 2 (X = halogen atom) (S 140); And reacting MX 2 with methylamine halide to form a perovskite light absorbing layer (S 150).

Step S 110 is a step of preparing a substrate. A transparent substrate is commonly used for the substrate. There is no particular limitation on the available substrate, and any substrate that can be used in manufacturing the solar cell is possible.

As the conductive layer (electrode layer) formed on the substrate, a transparent electrode layer is generally used, and typically ITO, FTO, or the like is used, but there is no particular limitation on this.

In steps S 120 to S 150, an electron collecting layer and a light absorbing layer are formed. A metal oxide electron collecting layer and a perovskite light absorbing layer material are disposed on the electron collecting layer and the light absorbing layer.

The electron collecting layer can be any structure that allows electrons generated when light is irradiated to reach the electrode layer. Materials commonly used as electron-collecting layer materials include TiO 2 , ZnO, and the like.

In the present invention, CH 3 NH 3 PbX 3 is used as the perovskite material. Wherein X is a halogen atom and the halogen atom used is Cl, Br, I.

The formation process of the electron collecting layer and the light absorbing layer will be described in detail as follows.

In step S 130, a MO thin film layer is formed on the metal oxide electron collecting layer formed in step S 120. The MO thin film layer is formed using the MO sol-gel method. The MO sol-gel method is a hydrophilic solvent capable of easily forming a thin film on a semiconductor oxide substrate or penetrating a complex nano-structured semiconductor oxide and forming a uniform film.

The MoO 2 sol-gel process comprises preparing a precursor material of M, putting the precursor material in a solvent capable of dissolving the M precursor, and spin-coating the solution obtained by stirring; And baking and heat treating the spin-coated solution.

After the solution is spin-coated on the metal oxide electron collecting layer, baking and heat treatment are performed. The baking is preferably performed at 100 ° C, and the heat treatment is preferably performed at 600 ° C in an air atmosphere.

In step S 140, O of the MO thin film layer formed on the electron collecting layer is replaced with a halogen atom to form MX 2 (X = halogen atom).

In order to replace an oxygen atom with a halogen atom, either of the following two methods can be used. First, there is a method of heat treatment by flowing X 2 gas. Secondly, there is a method of dipping a substrate on which a MO thin film layer is formed in HX solution and then performing a heat treatment.

Wherein X represents a halogen atom, and the substitutable halogen atom is any one of Br, Cl, and I.

In the first method, heat treatment is performed at a temperature of 150 to 350 ° C, preferably 250 ° C in an Ar atmosphere while flowing X 2 gas. This is a method of substituting in a gas atmosphere, and the second method is a method of substituting in a liquid atmosphere differently.

In the case of the second method, the substrate on which the PbO thin film layer is formed in the HX solution is dipped and then heat-treated. The heat treatment temperature is performed at a temperature of 60 to 150 DEG C, preferably at 70 DEG C in an air atmosphere.

In step S 140, the oxygen atom of MO is replaced with a halogen atom. In step S 150, MX 2 formed in step S 140 is reacted with methylamine halide to form a perovskite optical absorption layer.

This process is done By the heat treatment after the MX 2 is dipping the substrate formed or MX 2 is a spin coating methylamine halide on the substrate formed in the methylamine halide solution, in which case the heat treatment temperature is 100 to 150 ℃ and , And the heat treatment is performed in an air atmosphere.

After the electron collecting layer and the light absorbing layer of the perovskite solar cell are formed as described above, a hole transporting layer (hole transporting layer) and an upper electrode are sequentially formed thereon, thereby finally manufacturing a solar cell.

The hole transport layer preferably includes at least one of highly conductive polymer materials, and any structure can be used as long as holes generated when light is irradiated reach the hole transport layer. The metal electrode layer on the hole transport layer preferably includes one of the metal materials having a high work function.

As described above, in the present invention, the problem of the conventional non-uniform perovskite light absorbing layer can be solved by using the PbO sol-gel method to form a uniform film, The efficiency of the solar cell is improved, and the fill factor is improved. In addition, it is possible to suppress the occurrence of pinholes and the like caused by the formation of the non-uniform thin film mentioned in the prior art, and to easily apply a complicated nanostructure.

Hereinafter, the contents of the present invention will be further described with reference to specific embodiments.

[Example]

In this embodiment, Pb is used as M and I is used as X.

First, a transparent conductive substrate was prepared and cleaned. Thereafter, a TiO 2 metal oxide electron collecting layer for collecting electrons was dense and thinly formed.

As a process for forming a light absorbing layer, lead acetate trihydrate and monoethanolamine were added to 2-methoxy ethanol in a molar ratio of 1: 1 and then stirred at 60 ° C for 30 minutes. 2-methoxy ethanol was prepared in 10 ml of 0.8M, lead acetate trihydrate was 3.034 g, and monoethanolamine was 0.489 g.

The prepared solution was spin-coated on the electron-collecting layer using a spin coating machine, then baked at 100 ° C, and heat-treated at 600 ° C in an air atmosphere to finally coat the PbO.

The coated PbO substrate was heat treated at 250 ° C in an Ar atmosphere by placing a vapor I 2 chip in a 100 ml container. In this case, alternatively, the coated PbO substrate could be dipped in 0.5 M HI solution, washed, and heat treated in an air atmosphere at 70 ° C.

The substrate thus treated was dipped or spin-coated in a solution of 0.1 mg of CH 3 NH 3 I in 10 ml of 2-propanol and then heat-treated at 100 ° C. to 150 ° C. in an air atmosphere.

Next, a hole transporting solution prepared by mixing 80 mg of Spiro-MeOTAD, 8.4 μl of tBP and 51.6 μl of Li-TFSI 154 mg / ml in acetonitrile as a hole transport material was prepared and spin-coated on the substrate. Finally, The electrode was formed by depositing gold at 50 nm or more (10 -6 torr).

4 is a comparative photograph of PbI 2 prepared according to the present invention and PbI 2 prepared in the prior art. As shown in FIG. 4, in the case of the conventional PbI 2 thin film, the shape of the fine particle layer can be seen, which is TiO 2 particles and PbI 2 does not sufficiently surround the TiO 2 particles. In the case of the present invention, however, It was confirmed that PbI 2 surrounded the TiO 2 particles well.

FIG. 5 shows X-ray diffraction results to confirm that the PbO thin film was substituted with the PbI 2 thin film according to the present invention. As shown in FIG. 5, the PbO peak can be confirmed in the above diffraction graph, and the PbI 2 peak can be confirmed after the O of PbO is replaced with I as in the following diffraction graph. Therefore, it was confirmed that the substitution was well performed.

FIG. 6 is a graph showing a voltage-current density relationship between a solar cell manufactured according to the present invention and a conventional solar cell.

As shown in FIG. 6, it was confirmed that FF (fill factor) was superior to the conventional solar cell in the case of the present invention. This is because PbI 2 surrounds the TiO 2 particles well as shown in FIG. That is, in the case of the solar cell of the present invention, the FF was improved and it was confirmed that the voltage-current density graph approximated to a rectangular shape.

The description of the disclosed embodiments is provided to enable any person skilled in the art to make or use the present invention. Various modifications to these embodiments will be readily apparent to those skilled in the art, and the generic principles defined herein may be applied to other embodiments without departing from the scope of the invention. Thus, the present invention is not intended to be limited to the embodiments shown herein but is to be accorded the widest scope consistent with the principles and novel features presented herein.

Claims (11)

Preparing a substrate;
Forming a metal oxide electron collecting layer on the substrate;
Forming a uniform MO (M is a bivalent metal or rare earth metal) thin film layer on the metal oxide electron collecting layer using a sol-sel method;
Replacing O in the MO thin film layer with a halogen atom to form a homogeneous MX 2 (X = halogen atom); And
And reacting MX 2 with a methylamine halide to form a uniform perovskite light absorbing layer.
A method for forming a uniform perovskite light absorbing layer.
delete The method according to claim 1,
In the MO sol-gel method,
Preparing a precursor of M, putting it in a solvent capable of dissolving M precursor, and spin coating the solution obtained by stirring; And
Baking and heat treating the spin-coated solution.
A method for forming a uniform perovskite light absorbing layer.
The method according to claim 1,
The step of replacing O in the MO thin film layer with a halogen atom to form MX 2 (X = a halogen atom)
X 2 gas, or by dipping a substrate on which a MO thin film layer is formed in an HX solution, and then heat-
A method for forming a uniform perovskite light absorbing layer.
5. The method of claim 4,
The step of heat-treating the X 2 gas while flowing the X 2 gas may include heat treatment at 150 to 350 ° C in an Ar atmosphere,
A method for forming a uniform perovskite light absorbing layer.
5. The method of claim 4,
The step of dipping the substrate on which the MO thin film layer is formed in the HX solution and performing the heat treatment may be performed by heat treatment in an air atmosphere at 60 to 150 ° C,
A method for forming a uniform perovskite light absorbing layer.
The method according to claim 1,
The step of reacting MX 2 with a methylamine halide to form a perovskite light-
Dipping the substrate having MX 2 formed thereon in a methylamine halide solution or spin-coating a methylamine halide on the substrate having MX 2 formed thereon,
A method for forming a uniform perovskite light absorbing layer.
8. The method of claim 7,
Wherein the heat treatment is performed at a temperature of 100 to < RTI ID = 0.0 > 150 C. &
A method for forming a uniform perovskite light absorbing layer.
9. The method according to any one of claims 1 to 8,
Wherein X is any one of I, Br, and Cl,
A method for forming a uniform perovskite light absorbing layer.
9. The method according to any one of claims 1 to 8,
Wherein M is at least one of Pb, Sn, Cu, Cr, Mn, Pd, Cd,
A method for forming a uniform perovskite light absorbing layer.
9. A perovskite solar cell comprising a uniform perovskite light absorbing layer formed according to the method of any one of claims 1 to 8.
KR1020150070850A 2015-05-21 2015-05-21 Method of forming uniform perovsktie light absorbing layer, and solar cell comprising uniform perovsktie light absorbing layer KR101654470B1 (en)

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Citations (1)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
JPH09171715A (en) * 1995-12-20 1997-06-30 Oki Electric Ind Co Ltd Ferroelectric film, application liquid for formation of film, manufacture of application liquid, usage of application liquid

Patent Citations (1)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
JPH09171715A (en) * 1995-12-20 1997-06-30 Oki Electric Ind Co Ltd Ferroelectric film, application liquid for formation of film, manufacture of application liquid, usage of application liquid

Non-Patent Citations (2)

* Cited by examiner, † Cited by third party
Title
X. K. DING ET. AL. / OPTICAL AND ELECTRICAL PROPERTIES OF CH3NH3PBI3 PEROVSKITE THIN FILMS TRANSFORMED FROM PBO-PBI2 HYBRID FILMS *
X.-P. CUI ET. AL. / ELECTRODEPOSITION OF PBO AND ITS IN SITU CONVERSION TO CH3NH3PBI3 FOR MESOSCOPIC PEROVSKITE SOLAR CELLS *

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