CN108539023B - Perovskite type solar cell based on diboron compound modification and preparation method thereof - Google Patents

Perovskite type solar cell based on diboron compound modification and preparation method thereof Download PDF

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CN108539023B
CN108539023B CN201810318916.XA CN201810318916A CN108539023B CN 108539023 B CN108539023 B CN 108539023B CN 201810318916 A CN201810318916 A CN 201810318916A CN 108539023 B CN108539023 B CN 108539023B
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CN108539023A (en
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朱瑞
杨晓宇
涂用广
龚旗煌
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Peking University
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    • H10K30/15—Sensitised wide-bandgap semiconductor devices, e.g. dye-sensitised TiO2
    • H10K30/151—Sensitised wide-bandgap semiconductor devices, e.g. dye-sensitised TiO2 the wide bandgap semiconductor comprising titanium oxide, e.g. TiO2
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Abstract

The invention discloses a perovskite type solar cell based on diboron compound modification and a preparation method thereof, wherein the perovskite type solar cell comprises a planar type structure and a mesoporous type structure, wherein a metal oxide compact layer or a mesoporous layer serving as an electron transmission layer is modified by diboron compound, so that the valence state of metal ions on the surface of the metal oxide is changed, N-type doping on the surface is realized, and the concentration of current carriers is improved; meanwhile, the passivation effect is achieved, and the appearance of the metal oxide film is further improved. The perovskite solar cell with the electron transport layer modified by boronization has high photoelectric conversion efficiency and good light stability.

Description

Perovskite type solar cell based on diboron compound modification and preparation method thereof
Technical Field
The invention belongs to the technical field of photoelectric functional materials and devices, and particularly relates to a perovskite type solar cell modified based on a diboron compound and a preparation method thereof.
Background
The rapid development of economic society benefits from the widespread use of fossil fuels, however, the exhaustion crisis of fossil fuels and the continuous increase of environmental pollution have prompted us to actively search for renewable energy sources with low cost, cleanness and high efficiency. Solar power generation is a new renewable energy technology, but the cost of the silicon-based solar cell widely used at present is high and the preparation process is complicated, so that the discovery and preparation of the novel solar cell are not slow. Since 2009, metal halide perovskite-based solar cells have appeared due to their excellent photoelectric properties, a leap in photoelectric conversion efficiency from 3.8% to 22.7% has been realized in eight short years, and they are rapidly becoming research hotspots of novel photovoltaic technologies.
Metal oxides (e.g. TiO) 2、ZnO、SnO 2Etc.) are widely used in mesoporous and planar perovskite solar cells due to their good semiconductor properties and carrier transport characteristics. The first perovskite solar cell in the world and the perovskite solar cell with the highest efficiency certification at present use metal oxide as an electron transport layer, which proves irreplaceable importance in the development process of the perovskite solar cell. However, the interface contact problem between the metal oxide and the perovskite light absorption layer causes the resistance of the device to be increased and the recombination of carriers to be serious, so that the solar cell has the advantages of high efficiency, high yield and low costOpen circuit voltage (V) oc) And a decrease in Fill Factor (FF), which is a defect of metal oxides as electron transport layers for perovskite-type solar cells. Although many efforts have been reported to improve electron transport layers, for example, interfacial passivation by loading a buffer layer on the surface of a metal oxide electron transport layer; synthesizing metal oxide nanowires and nanotubes by using a morphology regulation and control mode to improve the transmission of current carriers; or rare earth elements, graphene and the like are doped in the conductive material to improve the conductivity. However, the above method has complicated process and high cost, and limits the development of perovskite-based solar cell technology. At present, the key problem is to optimize the metal oxide type electron transport layer by simple technical means, thereby improving the photoelectric conversion efficiency and stability of the cell.
Disclosure of Invention
The invention aims to provide a perovskite solar cell with a modified metal oxide type electron transport layer interface and a preparation method thereof.
The perovskite type solar cell comprises a transparent substrate, and a transparent electrode, a metal oxide electron transport layer, a perovskite light absorption layer, a hole transport layer and a top electrode which are sequentially stacked on the substrate, and is characterized in that the interface of the metal oxide electron transport layer in contact with the perovskite light absorption layer is modified by a boron-bonded compound.
The perovskite solar cell with the diboron compound modified metal oxide electron transport layer comprises two device structures, namely a mesoporous type device structure and a planar type device structure. For the mesoporous perovskite solar cell, the electron transmission layer comprises a metal oxide compact layer and a metal oxide mesoporous layer, wherein the interface of the metal oxide mesoporous layer in contact with the perovskite light absorption layer is modified by a boron compound. For the plane type perovskite solar cell, the electron transmission layer is a metal oxide dense layer, and the interface of the electron transmission layer, which is in contact with the perovskite light absorption layer, is modified by a diboron compound.
In the perovskite type solar cell, the transparent substrate can be made of transparent materials such as glass and flexible plastics. The transparent electrode material may be Indium Tin Oxide (ITO), fluorine doped tin oxide (FTO), aluminum doped zinc oxide (AZO), silver nanowires, graphene, or carbon nanotubes. One of ITO conductive glass, FTO conductive glass, AZO conductive glass, silver nanowire-modified conductive glass, graphene-modified conductive glass, and carbon nanotube layer-modified conductive glass is often used as a transparent substrate and a transparent electrode.
In the perovskite-type solar cell, the metal oxide dense layer as the electron transport layer may be selected from titanium oxide (TiO) 2) Zinc oxide (ZnO), tin oxide (SnO) 2) Nickel oxide, magnesium oxide, copper oxide, cuprous oxide, and tungsten oxide. For the mesoporous perovskite solar cell, the metal oxide mesoporous layer can be made of TiO 2And sintering the slurry to obtain the high-performance ceramic material.
The diboron compound used to treat the surface of the metal oxide dense or mesoporous layer may be selected from the following compounds containing a B-B bond: c 12H 24B 2O 4、C 10H 20B 2O 4、C 12H 8B 2O 4、B 2(OH) 4、C 8H 24B 2N 4And the like. The compound has the general formula B 2(XY) 4Wherein X may be N, O or an element of Si and Y may be hydrogen (H) pP is a positive integer) or a hydrocarbon group (C) mH nAnd m and n are positive integers).
In the perovskite type solar cell, the perovskite light absorption layer can be selected from the perovskite light absorption layer with the chemical general formula ABX 3Wherein A is CH 3NH 3 +(MA +)，NH 2＝CHNH 2 +(FA +)，C 4H 9NH 3 +，Cs +One or more of the components are mixed; b is Pb 2+，Sn 2+、Ge 2+、Sb 3+、Bi 3+、Ag +、Au 3+、Ti 4+At least one of; x is Cl -，Br -，I -In (1)One or more of the above components are mixed.
In the perovskite solar cell, the hole transport layer can be made of organic and inorganic materials, and the organic materials include but are not limited to: organic P-type semiconductor materials such as Spiro-OMeTAD, PEDOT, PSS, TPD, PTAA, P3HT, PCPDTBT and the like; inorganic materials include, but are not limited to: ni xO、V 2O 5、CuI、MoO 3、CuO、Cu 2And an inorganic P-type semiconductor material such as O. The organic hole transport layer is doped with an appropriate amount of lithium bis (trifluoromethane) sulfonimide and 4-tert-butylpyridine (4-tBP).
In the perovskite type solar cell, the top electrode can be made of metals such as Au, Ag and the like by a vacuum thermal evaporation method. In order to make reasonable use of the battery area and to facilitate the testing, different shapes of templates are often used to control the shape of the top electrode.
The invention also provides a preparation method of the perovskite solar cell with the diboron compound modified metal oxide electron transport layer, which comprises the following steps:
1) providing a transparent substrate and a transparent electrode;
2) preparing a metal oxide electron transport layer on the transparent electrode, and carrying out diboron modification on the metal oxide electron transport layer;
3) preparing a perovskite light absorption layer on the diboride-modified metal oxide electron transport layer;
4) preparing a hole transport layer on the perovskite light absorption layer;
5) a top electrode is prepared on the hole transport layer.
In the step 1), the transparent electrode is cleaned, dried and subjected to ultraviolet and/or ozone treatment.
In the step 2), for the planar perovskite solar cell, the metal oxide electron transmission layer is a metal oxide compact layer, and is subjected to diboration modification; for the mesoporous perovskite solar cell, the metal oxide electron transmission layer comprises a metal oxide compact layer and a metal oxide mesoporous layer, and the metal oxide mesoporous layer is subjected to diboration modification. The method for carrying out diboration modification on the metal oxide compact layer or the mesoporous layer comprises the following specific steps: in an oxygen-free atmosphereSoaking the prepared metal oxide compact layer or mesoporous layer substrate in a diboron compound solution for 18-36 h to load a diboron compound containing a B-B bond on the surface of the metal oxide; then washing to remove redundant diboron compounds on the surface, transferring to a heating table for annealing treatment at 50-100 ℃ to obtain low-valence metal cations (such as TiO) 2/Ti 3+、ZnO/Zn +) The metal oxide dense layer or the mesoporous layer of (a).
In the above method, the solvent used for dissolving the diboron compound is water, alcohols, ketones, or hydrocarbon non-oxidizing solvents, and may be selected from: non-oxidizing solvents such as isopropanol, methanol, ethanol, acetone, n-hexane, acetone, acetonitrile, water, etc. The concentration of the diboron compound solution is preferably 0.5-20 mg/mL, and more preferably 10 mg/mL. The oxygen-free atmosphere is generally chosen to be N 2And Ar or the like. Often by using N 20.5-20 mg/mL of isopropanol solution of diboron compound under protective atmosphere.
The step 5) can adopt a vacuum thermal evaporation method to prepare the metal top electrode. In order to make reasonable use of the battery area and to facilitate the testing, different shapes of templates are often used to control the shape of the top electrode.
Compared with the existing method for modifying the electron transmission layer of the perovskite solar cell, the method adopts simple methods of solution soaking and heating annealing to modify the surface of the metal oxide type electron transmission layer, realizes surface N-type doping through low-valence metal ions, improves the carrier concentration, passivates the interface of the metal oxide and the perovskite light absorption layer, reduces interface recombination and is more beneficial to the transmission of carriers.
The diboron compound is utilized to modify the surface of the metal oxide electron transport layer, and the method belongs to the research field of perovskite solar cells for the first time. The electron transport layer modified by the method can effectively improve the property of the electron transport layer, and the device prepared based on the method obtains higher photoelectric conversion efficiency (18 percent, see figure 1), and the preparation method is simple and convenient, has shorter production period and also has good stability.
Drawings
FIG. 1 is a J-V curve for the perovskite solar cell device prepared in example 1.
FIG. 2 is a Scanning Electron Microscope (SEM) observation of a modified metal oxide (TiO) modified with a diboron compound of example 1 2) And (6) surface topography.
Fig. 3 is a schematic structural diagram of the diboron compound modified planar and mesoporous perovskite solar cells prepared in examples 1 and 2, wherein (a) is a planar perovskite solar cell structure, and (b) is a mesoporous perovskite solar cell structure.
Fig. 4 is an SEM cross-sectional view of the diboron compound modified planar perovskite solar cell prepared in example 1.
Detailed Description
The following examples are provided to further illustrate the principles and procedures of the present invention, but the present invention is not limited to the following examples.
Example 1
Firstly, ultrasonic cleaning an FTO glass substrate (15 omega/□) by using deionized water, acetone, an optical glass cleaner, deionized water and isopropanol in sequence, drying for 4 hours at 60 ℃ in an oven, and then spin-coating TiO with the concentration of 5mg/mL on the surface of the FTO 2The solvent used in the colloidal quantum dots is a mixed solvent of methanol and chloroform, wherein the volume ratio of the mixed solvent to the chloroform is 1: 1. The spin speed was 4000rpm, the spin time was 20s, and the acceleration was 2000 rpm/s. The substrate was then annealed at 150 ℃ for 30 minutes.
Second, TiO is added 2Film substrate transfer to N 2Atmosphere glove box, and dipping into prepared C with concentration of 10mg/mL 12H 24B 2O 4Soaking in isopropanol solution at room temperature for 24h to sufficiently adsorb C 12H 24B 2O 4On TiO 2Washing the film surface with isopropanol solvent to remove excess C 12H 24B 2O 4. Transferring the film substrate to a hot table at 80 ℃, and heating for 30 minutes to obtain the film substrate with Ti-rich surface 3+Of TiO 2 2A film. Modified TiO 2The topography of the film is shown in figure 2,the surface after treatment is compact and has no obvious defects and holes.
Third step, passing through C 12H 24B 2O 4After modification, in TiO 2And (3) coating perovskite precursor liquid on the film in a spinning way. Wherein the precursor solution is prepared from equal mass of PbI 2And CH 3NH 3The compound I is prepared by dissolving the components in a mixed solvent of DMF and DMSO, wherein the volume ratio of the components is 4: 1. The spin speed was 6000rpm, the spin time was 30s, and the acceleration was 2000 rpm/s. After the completion of the spin coating, the substrate was transferred to a hot stage and heated at 100 ℃ for 30 minutes to form a film, and after cooling, an 80mg/mL solution of Spiro-OMeTAD in chlorobenzene containing 17.5. mu.L of lithium salt per mL (520mg/mL in acetonitrile) and 28.8. mu.L of 4-tBP was spin-coated. The spin speed was 2000rpm and the spin time was 25 s. After the film formation, gold was deposited to a thickness of 80nm as a metal top electrode. The photoelectric conversion efficiency of the cell can reach 18 percent (see figure 1). And the basic structure of the device is schematically shown in FIG. 3(a), the SEM cross-section is shown in FIG. 4, and the treated TiO 2The film thickness is uniform, and the perovskite film deposited on the film thickness is uniform and compact.
Example 2
In the second step, TiO is added 2Film substrate transfer to N 2Atmosphere glove box, and dipping into prepared C with concentration of 10mg/mL 10H 20B 2O 4Soaking in isopropanol solution at room temperature for 24h to sufficiently adsorb C 10H 20B 2O 4On TiO 2Washing the film surface with isopropanol solvent to remove excess C 10H 20B 2O 4. Transferring the film substrate to a hot table at 80 ℃, and heating for 30 minutes to obtain the film substrate with Ti-rich surface 3+Of TiO 2 2A film. The preparation method of the product is the same as that of example 1 in the other steps. The photoelectric conversion efficiency of the perovskite solar cell can reach 17 percent.
Example 3
In the second step, TiO is added 2Film substrate transfer to N 2Atmosphere glove box, and dipping into prepared B with concentration of 10mg/mL 2(OH) 4Soaking in isopropanol solution at room temperature for 24h to sufficiently adsorb B 2(OH) 4On TiO 2Washing the film surface with isopropanol solvent to remove excess B 2(OH) 4. Transferring the film substrate to a hot table at 80 ℃, and heating for 30 minutes to obtain the film substrate with Ti-rich surface 3+Of TiO 2 2A film. The preparation method of the product is the same as that of example 1 in the other steps. The photoelectric conversion efficiency of the perovskite solar cell can reach 17 percent.
Example 4
In the first step, an FTO glass substrate (15 omega/□) is ultrasonically cleaned by sequentially using deionized water, acetone, an optical glass cleaning agent, deionized water and isopropanol, and is dried for 4 hours at 60 ℃ in an oven, and then a layer of TiO with the thickness of 30nm is prepared on the surface of the FTO by adopting a spray pyrolysis method 2A dense layer. Spin-coating a layer of TiO on the substrate 2Colloid, wherein, TiO 2The colloid is commercially available TiO 2The mass ratio of the slurry to the absolute ethyl alcohol is 1: 6. The spin speed was 5000rpm, the spin time was 10s, and the acceleration was 2000 rpm/s. Then transferring the mixture to a heating table to sinter the mixture for 30min at a high temperature of 500 ℃ to prepare TiO 2A mesoporous layer. The preparation method of the product is the same as that of example 1 in the other steps. The photoelectric conversion efficiency of the perovskite solar cell can reach 18 percent. The basic structure of the device is schematically shown in fig. 3 (b).
Example 5
Firstly, an ITO glass substrate (15 omega/□) is ultrasonically cleaned by deionized water, acetone, an optical glass cleaner, deionized water and isopropanol in sequence, and after drying for 4 hours at 60 ℃ in an oven, ZnO colloidal solution with the concentration of 5mg/mL is spin-coated on the surface of the ITO, wherein the used solvent is methanol. The spin speed was 4000rpm, the spin time was 20s, and the acceleration was 2000 rpm/s. The spin-coated substrate was then placed on a hot stage and heated to 150 ℃ for 30 minutes to form a film.
Second, transferring the ZnO film substrate to N 2Atmosphere glove box, and dipping into prepared C with concentration of 10mg/mL 12H 24B 2O 4Soaking in isopropanol solution at room temperature for 24h to sufficiently adsorb C 12H 24B 2O 4Washing the ZnO film surface with isopropanol solvent to remove excessive C 12H 24B 2O 4. Transferring the film substrate to a hot table at 80 ℃, and heating for 30 minutes to obtainTo the surface rich in Zn +The ZnO thin film of (1).
The third step of the preparation method is the same as that of the embodiment 1, and the photoelectric conversion of the perovskite solar cell can reach 18 percent.

Claims (10)

1. A perovskite solar cell comprises a transparent substrate, and a transparent electrode, a metal oxide electron transmission layer, a perovskite light absorption layer, a hole transmission layer and a top electrode which are sequentially stacked on the substrate 2(XY) 4Wherein X is N, O or Si, Y represents H pOr C mH nAnd m, n and p are positive integers.
2. The perovskite solar cell according to claim 1, wherein the perovskite solar cell is a mesoporous perovskite solar cell, and the metal oxide electron transport layer comprises a metal oxide dense layer and a metal oxide mesoporous layer, wherein an interface where the metal oxide mesoporous layer contacts the perovskite light absorbing layer is modified by a diboron compound.
3. The perovskite solar cell of claim 2, wherein the metal oxide dense layer is selected from any one of titanium oxide, zinc oxide, tin oxide, nickel oxide, magnesium oxide, copper oxide, cuprous oxide, and tungsten oxide; the metal oxide mesoporous layer is made of TiO 2And sintering the slurry to obtain the high-performance ceramic material.
4. The perovskite solar cell according to claim 1, wherein the perovskite solar cell is a planar perovskite solar cell, and the metal oxide compound electron transport layer is a metal oxide dense layer, the interface of which in contact with the perovskite light absorbing layer is modified by a diboron compound.
5. The perovskite solar cell of claim 4, wherein the metal oxide dense layer is selected from any one of titanium oxide, zinc oxide, tin oxide, nickel oxide, magnesium oxide, copper oxide, cuprous oxide, and tungsten oxide.
6. The perovskite solar cell of claim 1, wherein the diboron compound is selected from one or more of the following compounds containing a B-B bond: c 12H 24B 2O 4、C 10H 20B 2O 4、C 12H 8B 2O 4、B 2(OH) 4And C 8H 24B 2N 4。
7. A method of manufacturing a perovskite solar cell as claimed in any one of claims 1 to 6, comprising the steps of:
1) providing a transparent substrate and a transparent electrode;
2) preparing a metal oxide electron transport layer on the transparent electrode, and modifying the metal oxide electron transport layer by a diboron compound;
3) preparing a perovskite light absorption layer on the diboron compound modified metal oxide electron transport layer;
4) preparing a hole transport layer on the perovskite light absorption layer;
5) a top electrode is prepared on the hole transport layer.
8. The production method according to claim 7, wherein, for the planar perovskite solar cell, the metal oxide dense layer is produced in step 2) and modified with a diboron compound; for the mesoporous perovskite solar cell, the metal oxide compact layer and the metal oxide mesoporous layer are sequentially prepared in the step 2), and boron compound modification is carried out on the metal oxide mesoporous layer.
9. The preparation method according to claim 8, wherein the method for modifying the metal oxide dense layer or the mesoporous layer by the diboron compound in the step 2) is specifically as follows: soaking the substrate with the prepared metal oxide compact layer or mesoporous layer in diboron compound solution for 18-36 h in an oxygen-free atmosphere to enable the diboron compound containing B-B bonds to be loaded on the surface of the metal oxide; and then, washing to remove redundant diboron compounds on the surface, transferring to a heating table for annealing treatment at 50-100 ℃, and obtaining a metal oxide compact layer or mesoporous layer with the surface rich in low-valence metal cations.
10. The method according to claim 9, wherein the diboron compound solution is prepared by dissolving a diboron compound in a non-oxidizing solvent selected from the group consisting of water, alcohols, ketones, and hydrocarbons, wherein the diboron compound is present in a concentration of from 0.5 to 20 mg/mL.
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