AU2020100802A4 - A fully-inorganic perovskite-type solar cell and its preparation method - Google Patents

A fully-inorganic perovskite-type solar cell and its preparation method Download PDF

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AU2020100802A4
AU2020100802A4 AU2020100802A AU2020100802A AU2020100802A4 AU 2020100802 A4 AU2020100802 A4 AU 2020100802A4 AU 2020100802 A AU2020100802 A AU 2020100802A AU 2020100802 A AU2020100802 A AU 2020100802A AU 2020100802 A4 AU2020100802 A4 AU 2020100802A4
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Jiandong FAN
Wenzhe Li
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Jinan University
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University of Jinan
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    • H—ELECTRICITY
    • H01—BASIC ELECTRIC ELEMENTS
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    • H01L31/00—Semiconductor devices sensitive to infra-red 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
    • H01L31/04—Semiconductor devices sensitive to infra-red 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 adapted as photovoltaic [PV] conversion devices
    • H01L31/06—Semiconductor devices sensitive to infra-red 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 adapted as photovoltaic [PV] conversion devices characterised by at least one potential-jump barrier or surface barrier
    • H01L31/072—Semiconductor devices sensitive to infra-red 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 adapted as photovoltaic [PV] conversion devices characterised by at least one potential-jump barrier or surface barrier the potential barriers being only of the PN heterojunction type
    • H—ELECTRICITY
    • H01—BASIC ELECTRIC ELEMENTS
    • H01L—SEMICONDUCTOR DEVICES; ELECTRIC SOLID STATE DEVICES NOT OTHERWISE PROVIDED FOR
    • H01L31/00—Semiconductor devices sensitive to infra-red 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
    • H01L31/18—Processes or apparatus specially adapted for the manufacture or treatment of these devices or of parts thereof
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    • Y02P70/00—Climate change mitigation technologies in the production process for final industrial or consumer products
    • Y02P70/50—Manufacturing or production processes characterised by the final manufactured product

Abstract

Abstract The invention discloses a fully-inorganic perovskite-type solar cell and its preparation method. The structure of this type of fully-inorganic perovskite-type solar cell includes: transparent conductive glass, inorganic hole-transporting layer, inorganic perovskite layer, cathode buffer layer, inorganic electron transport layer and metal electrode; among them, the material used for the electron transport layer is an n-type transition metal oxide, such as (tin oxide, titanium oxide, zinc oxide, etc.), and the preparation method is a sputtering method. The cathode buffer layer material is a wide-bandgap metal oxide, such as (tungsten oxide, vanadium pentoxide, molybdenum oxide, etc.), and its preparation method is an evaporation method. The invention can not only realize the preparation of a perovskite solar cell device with an fully-inorganic structure, but also realize the whole preparation process without the participation of chemical solvents, and fully realize the vacuum physical deposition process, which will effectively ensure that each film layer of the device achieves uniformity over a large area, and then promote the large-scale industrial production of the perovskite solar cell. Drawings Electr-ode Inorganic electr-on transport layer Inor-anlic chodsie rlaver Inorganic poervs rite ayer aet Transparen Figure - - - No cathode buffer layer Cathode buffer layer 0.0 0.2 0.4 0.6 0.8 1.0 Voltage (V) Figure 2

Description

Descriptions
2020100802 21 May 2020
A fully-inorganic perovskite-type solar cell and its preparation method
Technical Field
The invention belongs to the field of the perovskite solar cell, in particular to a fully-inorganic perovskite-type solar cell and its preparation method.
Background Technology
In recent years, the perovskite-type solar cell has become a hot newcomer in photovoltaic material in recent years due to their suitable direct bandgap semiconductor forbidden band width, high molar extinction coefficient, low exciton binding energy and excellent carrier transport characteristics. Among them, the photoelectric conversion efficiency of optoelectronic device based on organic-inorganic hybrid metal halide as the core absorbent material has been increased from the initial 3.8% to 25.2%% after a short period of ten years, which can be said to have reached or exceeded the achievable requirements needed to realize industrialization, in addition, compared with the current industrialized crystalline silicon batteries, the perovskite solar cells have the characteristics of abundant raw materials, low energy consumption and low cost, which enables such solar cell to have very broad development prospects.
However, to achieve the final industrialization, three basic conditions need to be met at the same time: high efficiency, low cost and stability. After continuous breakthroughs in efficiency and continuous improvement in cost processes, the most urgent problem facing researchers is stability. The stability problems mainly include: the perovskite solar cell, which shows relatively poor stability at higher humidity and temperature. The source of the thermal stability problem is that the organic charge transport materials in cell devices are synthesized with lower binding energy, which inevitably leads to the decomposition of the generated materials at higher energy. The source of humidity stability problems are the water absorption of organic charge transport layer materials and the water absorption of perovskite materials itself. Inorganic materials usually require a higher energy for synthesis during the synthesis process, and their stability exhibits more excellent performance compared to organic matter. To achieve industrialization of a type of cell, it must withstand
Descriptions
2020100802 21 May 2020 long-term testing in the working environment. However, more and more high-efficiency reports are based on organic materials. Because, compared with some inorganic materials, the synthesis of organic materials often requires lower synthesis energy, but it shows better transmission characteristics. In addition, the semiconductor's valence band and conduction band position play a decisive role in the energy band matching of cell film materials, and a large number of new organic semiconductor materials are synthesized, so they have an advantage in energy level matching. Inorganic materials are more complex both in doping and in material synthesis, so relatively little attention is paid to the research of inorganic materials. In addition, as an important part of the traditional organic-inorganic hybrid perovskite material, the introduction of MA+ and FA+ organic groups is a perovskite with its own poor temperature resistance and strong hygroscopicity. The foreshadowing of the instability of the material itself. If you want to solve this problem fundamentally, you can only replace it with other inorganic metal ions with similar atomic radii.
In summary, there have been some reports that inorganic materials are used to replace organic materials, which is intended to improve the stability of the perovskite solar cell while maintaining high efficiency. Scholars such as Alex K.-Y. Jen used the sol-gel method to prepare Cu-doped NiOx, which not only formed a more perfect energy level match with the perovskite material, but also enhanced its conductivity by doping engineering. Compared with PEDOT: PSS based on organic materials, the perovskite solar cell shows better stability and better photovoltaic performance. Scholars such as Yangyang introduced an inorganic ZnO nanoparticle to replace the organic material PCBM, which also showed more excellent stability. Recently, scholars such as snaith used inorganic metal CS+ instead of organic MA+ and FA+ to prepare inorganic perovskite thin films, and showed outstanding thermal stability. However, the above work is to apply inorganic materials to a certain film layer in the cell device. That is to say, other film layers in the cell device still use organic materials, which causes the thermal stability of the entire cell device to be limited. Therefore, the thermal stability of the perovskite solar cell cannot be fundamentally solved.
The sputtering method is used to deposit an electron transport layer on the surface of the perovskite film, which is beneficial to the extraction of electrons. However, the sputtering of high-energy particles will cause certain damage to the perovskite thin film, which makes a large number of defect states formed between the perovskite layer and the
Descriptions
2020100802 21 May 2020 electron transport layer, and introduces the electron recombination centers, which eventually causes the transmission interruption of the charge.
Invention Summary
The purpose of the present invention is to provide a fully-inorganic perovskite-type solar cell; another purpose of the present invention is a method for preparing such a solar cell.
In order to achieve the above purpose of the invention, the technical solution is as follows:
A fully-inorganic perovskite-type solar cell, including from bottom to top; transparent conductive glass, inorganic hole-transporting layer, inorganic perovskite layer, inorganic electron transport layer, metal electrode;
The perovskite solar cell inserts an inorganic cathode buffer layer between the inorganic perovskite layer and the inorganic electron transport layer. The material of the inorganic cathode buffer layer is selected from any one of tungsten oxide, vanadium pentoxide, molybdenum oxide, chromium oxide, aluminum trioxide, manganese oxide, zirconia, silicon oxide.
The material of the inorganic electron transport layer is selected from any one of zinc oxide, tin oxide, and titanium oxide.
The material of the inorganic perovskite layer is CsPb(i-x)SnxI(3-y)Bry, 0<x<l, 0<y<3.
The material of the inorganic hole-transporting layer is selected from any one of nickel oxide, cuprous oxide, cuprous iodide, and tricobalt tetroxide.
The thickness of the inorganic cathode buffer layer is 1 -10 nm.
The preparation method of the cell includes the following steps:
1) Inorganic hole-transporting layer: the inorganic hole-transporting layer is prepared on the upper surface of FTO glass by reactive sputtering method or evaporation method;
2) Inorganic perovskite layer: Co-evaporation method is used to prepare inorganic perovskite layer on the surface of the inorganic hole-transporting layer in step 1);
Descriptions
2020100802 21 May 2020
3) Inorganic cathode buffer layer: the inorganic cathode buffer layer is prepared on the surface of the inorganic perovskite layer in step 2) by evaporation or atomic layer deposition;
4) Inorganic electron transport layer: an inorganic electron transport layer is prepared on the surface of the inorganic cathode buffer layer in step 3) by radio frequency sputtering;
5) Electrode: An electrode is prepared on the surface of the inorganic electron transport layer in step 4) by metal evaporation method.
Step 3) When the evaporation method is used, the material used is any one of tungsten oxide, vanadium pentoxide, molybdenum oxide, and chromium oxide.
Step 3) When using the atomic layer deposition method, the material used is any one of aluminum oxide, manganese oxide, zirconium oxide, and silicon oxide.
The thickness of the FTO is about 450 nm, the inorganic hole-transporting layer 10 -50 nm, the inorganic perovskite layer 300 -400 nm, the inorganic cathode buffer layer 0-10 nm, the inorganic electron transport layer 50 -100 nm, and the metal electrode 80 -150 nm.
Compared with the prior art, the advantages and beneficial effects of the present invention are as follows:
(1) The present invention proposes a new structure of a fully-inorganic perovskite solar cell, which can effectively improve the thermal stability of the cell device, and the heat-resistant temperature of the cell device reaches above 200 °C.
(2) The present invention can realize the entire preparation process without chemical solvent participation, and can fully realize the vacuum physical deposition process, and the sputtered inorganic electron transport layer has a dense structure, which will effectively ensure that each film layer of the device achieves uniformity over a large area, and then promote the large-scale industrial production of the perovskite solar cell.
(3) The function of the inorganic cathode buffer layer material added in the present invention can effectively block the bombardment of perovskite
Descriptions
2020100802 21 May 2020 crystals by high-energy particles and reduce the damage of the surface of the perovskite film;
(4) The inorganic cathode buffer layer material added in the present invention can increase the wettability of the surface of the perovskite film, which is beneficial to the contact between the perovskite film and the electron transport layer.
(5) The materials of the inorganic cathode buffer layer deposited in the present invention are all wide band gap inorganic metal oxide materials, and the deposited thickness is only 0-10 nm, so that electrons can easily tunnel through the film layer, and then be extracted by the electron transport layer.
(6) The cathode buffer layer material added in the present invention can effectively improve the photovoltaic performance of the cell device.
Description with Drawings
Figure 1 is a structural diagram of a cell in the present invention.
Figure 2 is a J-V curve of the device before and after modification of the inorganic cathode buffer layer in Embodiment 1.
Figure 3 is an EQE curve of the device before and after modification of the inorganic cathode buffer layer in Embodiment 1.
Figure 4 is a J-V curve of the device before and after modification of the inorganic cathode buffer layer in Embodiment 2.
Figure 5 is an EQE curve of the device before and after modification of the inorganic cathode buffer layer in Embodiment 2.
Figure 6 is the efficiency change of the fully-inorganic perovskite solar cell device prepared in Embodiment 1 at 200 °C for 48 hours.
Descriptions
2020100802 21 May 2020
Detailed Description of the Presently Preferred Embodiments
The present invention is further described below in conjunction with specific embodiments, but the present invention is not limited to the following embodiments. The methods are conventional methods unless otherwise specified. The raw materials can be obtained from open commercial channels unless otherwise specified.
Embodiment 1 Preparation of a fully-inorganic perovskite solar cell with tungsten oxide as the cathode buffer layer material
1) Preparation of nickel oxide hole-transporting layer:
The specific steps are as follows: nickel oxide films are deposited on FTO glass by a reactive nickel sputtering method with a thickness of 50 nm.
2) Preparation of CsPbIBr2 perovskite layer:
The excess lead bromide and cesium iodide powder are placed in two quartz crucibles respectively, and the temperature of two quartz crucibles are controlled by co-evaporation technology, so that they can reach the same evaporation rate. Finally, lead bromide and cesium iodide are deposited on the nickel oxide film at the same time, resulting in a film in which lead bromide and cesium iodide are stacked on top of each other. After annealing at 200 °C for 1 hour in nitrogen, a CsPblBn perovskite film is formed with a thickness of 350 nm.
3) Preparation of tungsten oxide cathode buffer layer:
Excessive tungsten oxide powder is taken and placed in a metal evaporation boat, thermal evaporation technique is used to control the deposition rate of the film. A layer of tungsten oxide film is deposited on the surface of the perovskite film, the thickness of the film is 2 nm. After the deposition is completed, it needs to be heated and annealed at 160 °C for 10 min in a nitrogen atmosphere.
4) Preparation of zinc oxide electron transport layer:
The surface of zinc oxide ceramic target is bombarded by radio frequency sputtering method, and zinc oxide film is deposited on the surface of tungsten oxide film, and the thickness of the film is 70 nm.
Descriptions
2020100802 21 May 2020
5) Evaporated silver electrode
The metal silver electrode is deposited on the zinc oxide surface by a metal silver evaporation method with a thickness of 120 nm.
The J-V performance curve of the cell is tested by solar simulator under AM 1.5, lOOmW / cm2 illumination. As shown in a curve of Figure 1, the blank condition obtained the short-circuit current density of the cell is 1.48 mA/cm2, the open circuit voltage is 0.51 V. and the fill factor is 0.11 and the photoelectric conversion efficiency is 0.08%. The short-circuit current density modified by adding the cathode buffer layer is 8.78mA / cm2, the open circuit voltage is 0.95 V, the fill factor is 0.44, and the photoelectric conversion efficiency is 3.6%. Before and after the cathode buffer layer is added, the external quantum efficiency of the battery device is shown in Figure 2, and the external quantum efficiency is significantly improved after the cathode buffer layer is added. Figure 6 is the efficiency change of the fully-inorganic perovskite solar cell device prepared in Embodiment 1 at 200 °C for 48 hours.
Comparative Example 1
The remaining steps are the same as in Embodiment 1, but the cathode buffer layer is not prepared.
Embodiment 2 Preparation of the fully-inorganic perovskite solar cell with molybdenum oxide as the cathode buffer layer material
Following the procedure of Embodiment 1, only the tungsten oxide powder used in step 3 ) is replaced with molybdenum oxide powder.
The JV performance curve of the cell is tested by solar simulator under AM 1.5, lOOmW / cm2 illumination. As shown in Figure 3, the blank condition obtained the short-circuit current density of the cell is 1.48 mA/ cm2, the open circuit voltage is 0.51 V. and the fill factor is 0.11 and the photoelectric conversion efficiency is 0.08%. The short-circuit current density modified by adding the cathode buffer layer is 8.9 mA/ cm2, the open circuit voltage is 0.97 V, the fill factor is 0.3, and the photoelectric conversion efficiency is 2.6%. Before and after the cathode buffer layer is added, the external quantum efficiency of the battery device shown in Figure 4, and the external quantum efficiency is
Descriptions
2020100802 21 May 2020 significantly improved after the cathode buffer layer is added.
Embodiment 3 Preparation of the fully-inorganic perovskite solar cell with vanadium pentoxide as the cathode buffer layer material
Following the procedure of Embodiment 1, only the tungsten oxide powder used in step 3 ) is replaced with vanadium pentoxide powder.
The JV performance curve of the cell is tested by solar simulator under AM 1.5, 1 OOmW / cm2 illumination. The short-circuit current density modified by adding the cathode buffer layer is 7.6mA/ cm2, the open circuit voltage is 1 V, the fill factor is 0.43, and the photoelectric conversion efficiency is 3.4%.
Embodiment 4 Preparation of the fully-inorganic perovskite solar cell with aluminum oxide as the cathode buffer layer material
Following the steps of Embodiment 1, only the tungsten oxide film prepared by evaporation in step 3) is replaced with atomic layer deposition of aluminum oxide film.
The JV performance curve of the cell is tested by solar simulator under AM 1.5, 100mW/cm2 illumination. The short-circuit current density modified by adding the cathode buffer layer is 6.4 mA/cm2, the open circuit voltage is 1 V, the fill factor is 0.47, and the photoelectric conversion efficiency is 3.1 %.
Table 1. J-V parameters of perovskite solar cells and modified devices of Embodiments 1 to 4
Jsc/mA cm'2 Voc/V PCE FF
Comparative 1 1.48 0.51 0.08% 0.11
Embodiment 1 8.78 0.95 3.6% 0.44
Embodiment 2 8.9 0.97 2.6% 0.3
Embodiment 3 7.6 1 3.3% 0.43
Embodiment 4 6.4 1 3.0% 0.47
Obtained from Embodiments 1-4, the short-circuit current, fill factor and open-circuit voltage of the device are generally improved after treatment with modifiers, mainly because 8
Descriptions
2020100802 21 May 2020 the cathode buffer layer blocks the damage of sputtered high-energy particles to the perovskite film, reduces the interface defects between the perovskite layer and the electron transport layer, and improves the extraction efficiency of electrons.

Claims (8)

Claims 2020100802 21 May 2020
1) Inorganic hole-transporting layer: the inorganic hole-transporting layer is prepared on the upper surface of FTO glass by reactive sputtering method or evaporation method;
1. A fully-inorganic perovskite-type solar cell, including from bottom to top; transparent conductive glass, inorganic hole-transporting layer, inorganic perovskite layer, inorganic electron transport layer, metal electrode;
It is characterized in that the perovskite-type solar cell inserts an inorganic cathode buffer layer between the inorganic perovskite layer and the inorganic electron transport layer. The material of the inorganic cathode buffer layer is selected from any one of tungsten oxide, vanadium pentoxide, molybdenum oxide, chromium oxide, aluminum trioxide, manganese oxide, zirconia, silicon oxide.
2) Inorganic perovskite layer: Co-evaporation method is used to prepare inorganic perovskite layer on the surface of the inorganic hole-transporting layer in step 1);
2. The cell according to claim 1 is characterized in that the material of the inorganic electron transport layer is selected from any one of zinc oxide, tin oxide, and titanium oxide.
3) Inorganic cathode buffer layer: the inorganic cathode buffer layer is prepared on the surface of the inorganic perovskite layer in step 2) by evaporation or atomic layer deposition;
3. The cell according to claim 1 is characterized in that the material of the inorganic perovskite layer is CsPb(i-x)SnxI(3-y)Bry, 0<x<l, 0<y<3.
4) Inorganic electron transport layer: an inorganic electron transport layer is prepared
Claims
2020100802 21 May 2020 on the surface of the inorganic cathode buffer layer in step 3) by radio frequency sputtering;
4. The cell according to claim 1 is characterized in that the material of the inorganic hole-transporting layer is selected from any one of nickel oxide, cuprous oxide, cuprous iodide, and tricobalt tetroxide.
5) Electrode: An electrode is prepared on the surface of the inorganic electron transport layer in step 4) by metal evaporation method.
5. The cell according to claim 1 is characterized in that the thickness of the inorganic cathode buffer layer is 1 -10 nm.
6. The method for preparing a cell according to any one of claims 1 to 5, characterized in that it includes the following steps:
7. According to the method described in claim 6, it is characterized in that the material used is either of tungsten oxide, vanadium pentoxide, molybdenum oxide, chromium oxide when the evaporation method is used in step 3).
8. According to the method described in claim 6, it is characterized in that the material used is any one of aluminum oxide, manganese oxide, zirconium oxide, and silicon oxide when atomic layer deposition is used in step 3).
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