CN113161488A - Homogeneous junction charge transmission film for perovskite solar cell - Google Patents
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- H—ELECTRICITY
- H10—SEMICONDUCTOR DEVICES; ELECTRIC SOLID-STATE DEVICES NOT OTHERWISE PROVIDED FOR
- H10K—ORGANIC ELECTRIC SOLID-STATE DEVICES
- H10K30/00—Organic devices sensitive to infrared radiation, light, electromagnetic radiation of shorter wavelength or corpuscular radiation
- H10K30/10—Organic devices sensitive to infrared radiation, light, electromagnetic radiation of shorter wavelength or corpuscular radiation comprising heterojunctions between organic semiconductors and inorganic semiconductors
- H10K30/15—Sensitised wide-bandgap semiconductor devices, e.g. dye-sensitised TiO2
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- H—ELECTRICITY
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- H10K—ORGANIC ELECTRIC SOLID-STATE DEVICES
- H10K71/00—Manufacture or treatment specially adapted for the organic devices covered by this subclass
- H10K71/10—Deposition of organic active material
- H10K71/12—Deposition of organic active material using liquid deposition, e.g. spin coating
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- Y—GENERAL TAGGING OF NEW TECHNOLOGICAL DEVELOPMENTS; GENERAL TAGGING OF CROSS-SECTIONAL TECHNOLOGIES SPANNING OVER SEVERAL SECTIONS OF THE IPC; TECHNICAL SUBJECTS COVERED BY FORMER USPC CROSS-REFERENCE ART COLLECTIONS [XRACs] AND DIGESTS
- Y02—TECHNOLOGIES OR APPLICATIONS FOR MITIGATION OR ADAPTATION AGAINST CLIMATE CHANGE
- Y02E—REDUCTION OF GREENHOUSE GAS [GHG] EMISSIONS, RELATED TO ENERGY GENERATION, TRANSMISSION OR DISTRIBUTION
- Y02E10/00—Energy generation through renewable energy sources
- Y02E10/50—Photovoltaic [PV] energy
- Y02E10/549—Organic PV cells
Abstract
The invention provides a homojunction charge transmission film for a perovskite solar cell, and the film is used for the perovskite solar cell, so that the photoelectric property of a device can be obviously improved. The charge transport materials with different impurity concentrations are deposited on the substrate layer by adopting a spin coating method, a spraying method or an atomic layer deposition method, and the like, and a built-in electric field which is favorable for transporting current carriers can be generated in the charge transport film through adjusting and controlling the impurity concentration, so that the separation and the transmission of the current carriers at the interface of the perovskite/charge transport film are accelerated, and the performance of the perovskite battery device is improved. Compared with the charge transmission film for the perovskite battery with the traditional structure, the film has the advantages that a built-in electric field beneficial to carrier transmission can be generated in the film, so that interface carrier recombination is reduced, and the battery performance is improved.
Description
Technical Field
The invention relates to a charge transmission film for a perovskite solar cell and a preparation method thereof.
Background
The photovoltaic plays an important role in promoting the green development and ecological civilization construction of China. At present, the photovoltaic industry starts to realize the internet surfing at a flat price. New high efficiency, low cost solar cell technologies are urgently needed in the market. Perovskite solar cells are hot candidates for their low fabrication cost and high efficiency. However, according to the Shockley-Queisser constraint theory, the performance of the perovskite solar cell still has a large improvement space, and the non-radiative recombination of carriers at the interface of the charge transport thin film and the perovskite active layer is an important constraint factor. Therefore, designing a new charge transport thin film to inhibit interface carrier recombination is one of the key issues that needs to be solved urgently in the development of current perovskite batteries. The inorganic charge transport material has the advantages of fast charge transport, good stability, simple preparation, low price and the like, so that the construction of the perovskite solar cell based on the inorganic charge transport material is an effective means for solving the stability of the cell and further reducing the cost of the cell.
Currently, the solution to the recombination of the interface carriers of the inorganic charge transport thin film and the perovskite active layer mainly depends on interface engineering, including interface energy level matching and interface passivation. In prior related patents and reports, there are several related patents relating to interfacial passivation of a perovskite battery charge transport thin film with a perovskite active layer. CN202010482213.8 discloses an interface modification method for perovskite solar cells, which is suitable for modifying the interface between a hole transport layer and a perovskite substrate. CN201810046177.3 also discloses a perovskite solar cell with an interface modification layer and a preparation method thereof, wherein a passivation layer optimizes the crystal structure of perovskite and inhibits ion migration in a perovskite active layer to a certain extent.
However, the introduction of new species at the interface may also result in reduced photogenerated carrier injection efficiency, increased cell series resistance, and even instability factors for perovskite cells. The invention provides a novel charge transmission film, which achieves the purposes of accelerating the carrier transmission and reducing the recombination of interface carriers of the charge transmission film and a perovskite active layer by constructing a built-in electric field with a certain direction in the film.
Disclosure of Invention
The invention aims to provide a homojunction charge transport film for a perovskite cell, which solves the problem of the recombination of interface carriers of the charge transport film and a perovskite active layer of the existing perovskite solar cell and improves the efficiency of a device.
The object of the present invention is achieved by constructing a charge transport film having a homogeneous structure.
The charge transport film containing the homogeneous structure is formed by depositing two or more charge transport films with different impurity concentrations layer by layer, and the impurity concentration is from high to low from the substrate to the top.
The charge transport film may be an electron transport film or a hole transport film.
The film main body material can be a hole transmission material such as nickel oxide, vanadium oxide, cobalt oxide, cuprous thiocyanate, ferrous sulfide, copper indium tin sulfide and the like, and can also be an electron transmission material such as titanium dioxide, zinc oxide, tin oxide and the like.
The impurity can be Cu, Li, Co, La, Sr and other elements for the hole transport material; the electron transport material may be an element such as Nb, Ta, Li, V, Y, or Sb.
The preparation method of the charge transmission film can be a film preparation method such as a solution spin coating method, a spraying method, a spray pyrolysis method, an atomic layer deposition method, a magnetron sputtering method, an electrochemical deposition method, a chemical vapor deposition method, a liquid phase epitaxial growth method, a molecular beam epitaxy method and the like, and has wide applicability.
The perovskite battery can be of a formal structure, namely, a homojunction electron transmission film, a perovskite active film, a hole transmission film and a metal back electrode are sequentially deposited on a conductive substrate; or a trans-structure, namely a hole transmission film containing a homojunction, a perovskite active film, an electron transmission film and a metal back electrode are sequentially deposited on the conductive substrate.
The preparation method of the homojunction-containing charge transport film provided by the invention has various forms, takes the preparation of the homojunction charge transport film by a solution spin coating method as an example, and comprises the following specific preparation process steps:
(1) and ultrasonic cleaning the conductive substrate by deionized water, ethanol, acetone, isopropanol and the like in sequence.
(2) A precursor solution was prepared by dissolving 5mmol of metal nitrate (e.g., nickel nitrate if a NiO hole transport film was prepared) in 5mL of ethylene glycol followed by the addition of 0.3g of ethylenediamine.
(3) And adding a certain amount of impurity precursors (if a Cu-doped NiO hole transport film is prepared, adding copper nitrate), and controlling the impurity concentration in the charge transport film through the addition amount of the impurity precursors to obtain a doped precursor solution.
(4) Firstly, dripping the high-concentration doping precursor solution to a conductive substrate, and rotating for 40s at the rotating speed of 5000 rpm. The obtained film is naturally cooled after being heated (100-200 ℃).
(5) And dripping low-concentration or undoped precursor solution on the basis of the thin film. At 5000rpm, the rotation was carried out for 40 seconds.
(6) And circulating the film deposition process to obtain the multilayer or double-layer charge transmission film with different impurity concentrations. After high-temperature annealing treatment (400-500 ℃), homojunctions are generated in the film, and a built-in electric field beneficial to carrier transport is formed.
By adopting other film deposition methods, a similar process can be followed to realize the charge transport film with the multilayer or double-layer homogeneous structure with different impurity concentrations.
The invention has the beneficial effects that the charge transmission film is composed of double-layer or multi-layer films with homogeneous structures, an electric field is built in the film, the carrier transport in the film can be effectively accelerated, the injection acceleration of the charge transmission film/perovskite film interface carrier is caused, the interface carrier recombination is reduced, and the efficiency of the perovskite solar cell device is further improved.
The problem of the interface carrier recombination of the charge transport layer/the perovskite active layer of the existing perovskite solar cell is solved, and the purpose of the invention is achieved.
The advantages are that: the film provided by the invention has simple preparation process and strong technical adaptability, can be realized by using various film deposition technologies, and can realize uniform preparation of large-area films through process selection; the film can effectively solve the problem of compounding of the interface carriers of the perovskite battery device, and avoids the loss of photoelectric properties or working stability of the device caused by the traditional passivation process.
Drawings
FIG. 1 is an SEM surface view of a bilayer (Cu: NiO/NiO) hole transport film prepared in example 1.
FIG. 2 is a SEM structural diagram of a cross section of a perovskite solar cell based on a double-layer (Cu: NiO/NiO) hole transport film prepared in example 1.
Fig. 3 is a J-V plot of the perovskite solar cell prepared in example 1 and comparative examples 1 and 2.
FIG. 4 is a positive-reverse sweep J-V plot of the perovskite solar cell prepared in example 1.
Fig. 5 is a graph of the operational stability of the perovskite solar cell prepared in example 1.
Table 1 is a table of photovoltaic performance parameters for the perovskite solar cells prepared in example 1 and comparative examples 1, 2.
Detailed Description
The invention includes a homojunction charge transport film for perovskite solar cells. The substantial features and the remarkable effects of the present invention can be shown from the following examples, which are not intended to limit the present invention in any way. The apparatus and reagents used in the present invention are commercially available general-purpose products unless otherwise specified.
Example 1
(1) Specific process for preparing double-layer NiO hole transport film with homojunction structure by solution spin coating method
Cutting and etching the conductive substrate, and then sequentially cleaning the conductive substrate by using deionized water, ethanol, acetone, isopropanol and other ultrasonic waves.
② dissolving 5mmol nickel nitrate in 5mL ethylene glycol, and then adding 0.3g ethylenediamine to prepare precursor solution.
And thirdly, adding 0.025mol of copper nitrate into the precursor solution, and stirring for dissolving. The solution was dropped onto a conductive substrate and spun at 5000rpm for 40 seconds. The obtained film is naturally cooled after being heated at 200 ℃.
And fourthly, dropwise adding the undoped nickel oxide precursor solution again on the basis of the film. At 5000rpm, the rotation was carried out for 40 seconds. And fifthly, annealing the obtained film at 450 ℃ to finish the preparation of the double-layer NiO hole transport film containing the homojunction structure.
FIG. 1 shows SEM surface images of the prepared bilayer (Cu: NiO/NiO) hole transport films, which were uniformly dense.
(2) Perovskite solar cell preparation process based on NiO hole transport film containing homojunction structure
Firstly, preparing a perovskite solution: 1mmol of FAI, 0.2mmol of MABr and 0.2mmol of PbBr2And 1.1mmol of PbI2Added to a mixed solution of 800uL DMF and 200uL DMSO and stirred for 2 h. Then, 41.6uL of 1.5mol/L CsI DMSO solution was added, and filtered for use.
Preparing a perovskite active layer: coating the perovskite solution on a NiO hole transmission film containing a homojunction structure, rotating at 1000rpm for 10s, rotating at 5000rpm for 30s, and dropwise adding a filtered ethyl acetate anti-solvent after rotating at 5000rpm for 8 s. Heating the film at 70 ℃ for 3min, and then heating at 100 ℃ for 12min to obtain the mixed perovskite film.
Preparing an electron transmission film: PCBM is deposited on the cooled perovskite thin film to be used as an electron transport layer of the perovskite battery, the PCBM is dissolved in chlorobenzene, the concentration of the PCBM is 20g/L, and the PCBM is used after being filtered. The spin coating was carried out at 3000rpm for 30 s. In order to ensure the film to be compact and solve the back contact problem of the device, a layer of BCP film (ethanol is used as a solvent, the concentration is 0.5g/L, the rotating speed is 3000rpm, and the time is 30s) is deposited after PCBM deposition.
Metal back electrode: putting the device into a vacuum evaporator, and evaporating a silver electrode with the thickness of 50-70 nm.
FIG. 2 shows a cross-sectional SEM structural diagram of a prepared perovskite solar cell based on a double-layer (Cu: NiO/NiO) hole transport film. The perovskite battery has clear and visible components and comprises a double-layer hole transport layer (Cu: NiO/NiO), a perovskite active layer, an electron transport layer (PCBM) and an Ag electrode, wherein the thicknesses of the double-layer hole transport layer, the perovskite active layer, the electron transport layer and the Ag electrode are 30 nm, 550nm, 80nm and 60nm in sequence.
(3) Perovskite solar cell testing method
Perovskite solar cell performance was tested under standard simulated sunlight (light intensity 100mW/cm 2). Connecting the anode and the cathode of the battery to an electrochemical workstation, and performing forward and reverse linear scanning between 1.2V and 0V to obtain an I-V curve of the battery. The delay time is set to 40 ms.
And (3) testing results:
the measured I-V curves are shown in FIG. 3, and the obtained photovoltaic parameters are shown in Table 1. Under reverse-sweeping conditionAt this time, the short-circuit current was 20.07mA/cm2The open circuit voltage was 1.04V, the fill factor was 0.805, and the photoelectric conversion efficiency was 16.84%. Under the normal scanning condition, the short-circuit current is 20.21mA/cm2The open circuit voltage was 1.03V, the fill factor was 0.802, and the photoelectric conversion efficiency was 16.81%. Under the positive and negative scanning condition, the perovskite solar cell based on the hole transport film with the homogeneous structure has small performance difference and unobvious I-V hysteresis effect, as shown in figure 4. The perovskite cell operating stability results are shown in fig. 5, and 80% of the initial efficiency was maintained over 350 hours of operation.
Comparative example 1: the hole transport film was an undoped NiO film, which was otherwise the same as in example 1. The corresponding cell performance is shown in fig. 3 and table 1. Under the reverse-scanning condition, the short-circuit current of the battery is 18.24mA/cm2The open circuit voltage was 1.00V, the fill factor was 0.660, and the photoelectric conversion efficiency was 12.15%. Under the normal scanning condition, the short-circuit current is 18.59mA/cm2The open circuit voltage was 0.96V, the fill factor was 0.697, and the photoelectric conversion efficiency was 12.51%. The efficiency of the solar cell is not as high as that of a perovskite solar cell based on a NiO hole transport film with a homogeneous structure.
Table 1:
comparative example 2: the hole transport film was a NiO film treated with Cu doping, and the other steps were the same as in example 1. The corresponding cell performance is shown in fig. 3 and table 1. Under the reverse-scanning condition, the short-circuit current of the battery is 19.07mA/cm2The open circuit voltage was 1.00V, the fill factor was 0.772, and the photoelectric conversion efficiency was 14.83%. Under the normal scan condition, the short-circuit current is 19.37mA/cm2The open circuit voltage was 0.93V, the fill factor was 0.781, and the photoelectric conversion efficiency was 14.21%. The efficiency is not as good as that of a perovskite solar cell based on a NiO hole transport film with a homogeneous structure.
Claims (6)
1. A homogeneous junction charge transport film for perovskite solar cells is characterized in that: the method comprises the steps of firstly depositing a charge transport film with high impurity concentration and then depositing a charge transport film with low impurity concentration or without impurity, wherein the charge transport film is an electron transport film or a hole transport film.
2. The homojunction charge transport film for perovskite solar cells as claimed in claim 1, wherein: the film host material includes but is not limited to a hole transport material selected from nickel oxide, vanadium oxide, cobalt oxide, cuprous thiocyanate, ferrous sulfide, copper indium tin sulfide, or an electron transport material selected from but not limited to titanium dioxide, zinc oxide, and tin oxide.
3. The homojunction charge transport film for perovskite solar cells as claimed in claim 1, wherein: in the construction of the homojunction, for the hole transport material, one or more of Cu, Li, Co, La and Sr are used as doping elements; for the electron transport material, one or more of Nb, Ta, Li, V, Y, Sb are used as the doping element, but not limited thereto.
4. The homojunction charge transport film for perovskite solar cells as claimed in claim 1, wherein: the film is a double-layer film with different doping concentrations or a multi-layer film with gradient change of doping concentrations.
5. The homojunction charge transport film for perovskite solar cells as claimed in claim 1, wherein: the film is prepared by any film preparation method of a solution spin coating method, a spraying method, a spray pyrolysis method, an atomic layer deposition method, a magnetron sputtering method, an electrochemical deposition method, a chemical vapor deposition method, a liquid phase epitaxial growth method and a molecular beam epitaxial method.
6. A perovskite solar cell preparation method is characterized by comprising the following steps: the charge transport film containing homojunction, the perovskite active film, the charge transport film and the metal back electrode are deposited on the conductive substrate in sequence, and the charge transport film containing homojunction meets the requirements of claims 1 to 5.
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| CN113745410A (en) * | 2021-08-24 | 2021-12-03 | 上海工程技术大学 | Based on P type CuNiO2Preparation method of thin film perovskite solar cell |
Citations (6)
| Publication number | Priority date | Publication date | Assignee | Title |
|---|---|---|---|---|
| CN105070834A (en) * | 2015-07-28 | 2015-11-18 | 华中科技大学 | Perovskite solar cell based on doped NiO hole transport layer and preparation method thereof |
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