WO2023109071A1 - Cellule solaire en pérovskite contenant une structure de micro-cavité optique - Google Patents

Cellule solaire en pérovskite contenant une structure de micro-cavité optique Download PDF

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WO2023109071A1
WO2023109071A1 PCT/CN2022/100716 CN2022100716W WO2023109071A1 WO 2023109071 A1 WO2023109071 A1 WO 2023109071A1 CN 2022100716 W CN2022100716 W CN 2022100716W WO 2023109071 A1 WO2023109071 A1 WO 2023109071A1
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solar cell
perovskite solar
layer
film layer
preparation
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PCT/CN2022/100716
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Chinese (zh)
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张赟
赵志国
赵东明
李新连
夏渊
李梦洁
刘家梁
董超
王百月
王森
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中国华能集团清洁能源技术研究院有限公司
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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
    • 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
    • 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
    • H10K30/80—Constructional details
    • H10K30/81—Electrodes
    • 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
    • H10K30/80—Constructional details
    • H10K30/87—Light-trapping means
    • H—ELECTRICITY
    • H10—SEMICONDUCTOR DEVICES; ELECTRIC SOLID-STATE DEVICES NOT OTHERWISE PROVIDED FOR
    • H10K—ORGANIC ELECTRIC SOLID-STATE DEVICES
    • H10K71/00—Manufacture or treatment specially adapted for the organic devices covered by this subclass
    • H10K71/60—Forming conductive regions or layers, e.g. electrodes
    • 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

Definitions

  • the invention relates to the technical field of batteries, in particular to a perovskite solar battery including an optical microcavity structure.
  • An optical microcavity is an optical resonant cavity that can confine the light field in the micron or even nanometer range. It uses reflection, scattering or diffraction at material interfaces with discontinuous dielectric constants to confine light energy to oscillate back and forth in a small area, thereby increasing photon lifetime.
  • the optical microcavity structure can increase the optical path of incident light through reflection and scattering at the interface, which greatly improves the absorption of incident light by the photoactive layer in the cell structure, thereby improving the photoelectric conversion efficiency of the cell. (PCE).
  • the vacuum deposition thin film process usually includes three processes: 1) the evaporation material changes from the condensed phase to the gas phase to form evaporated particles; 2) the movement of the evaporated particles between the evaporation source and the substrate; 3) the condensation of the evaporated particles after reaching the substrate, Nucleation, growth, and film formation.
  • the deposition sequence of the film on the substrate under high vacuum conditions has a clear stage (as shown in the schematic diagram 1 of each stage of film growth): 1) firstly form a three-dimensional nucleus with disordered distribution, the formation of the nucleus is disordered and isotropic, Then the evaporated particles on the surface of the substrate quickly reach the saturation density, and the three-dimensional nucleus grows slowly to form a three-dimensional island-like microstructure.
  • the shape of the island is determined by the interface energy and deposition conditions, and the entire growth process is controlled by diffusion; With further deposition, the size of the islands gradually increases, and the islands approach each other and merge into large islands, and the density of the islands decreases monotonously at a rate determined by the deposition conditions; 3) when the distribution of the islands reaches a certain critical state, the islands and islands rapidly Merge to form a Unicom network structure (the network contains a large number of empty tunnels); 4) The final stage is to evaporate particles to fill the network and tunnels between the islands and generate a continuous dense film layer.
  • the technical problem solved by the present invention is to provide a perovskite solar cell including an optical microcavity structure, which can increase the collection efficiency of incident light without affecting other performances of the cell, and finally improve the photoelectric conversion efficiency of the cell.
  • the application provides a perovskite solar cell comprising an optical microcavity structure, including a substrate, a discontinuous metallic silver thin film layer, a hole transport layer, a perovskite active layer, an electron transport layer and dense metallic silver thin film layer.
  • the thickness of the discontinuous metallic silver thin film layer is 2-10 nm, and the thickness of the dense metallic silver thin film layer is 50-200 nm.
  • the substrate is selected from a hard substrate or a flexible substrate;
  • the hole transport layer is selected from NiO x , PEDOT:PSS or poly[bis(4-phenyl)(2,4,6-trimethyl phenyl)amine];
  • the electron transport layer is selected from one or more of TiO 2 , SnO 2 , PCBM, C 60 and BCP.
  • the preparation method of the perovskite solar cell comprises the following steps: A) substrate cleaning; B) preparation of a hole transport layer; C) preparation of a discontinuous metal silver film layer; D) preparation of a perovskite active layer; E) Preparation of electron transport layer; F) Preparation of dense metallic silver thin film layer.
  • the discontinuous metal silver film layer is prepared by vacuum evaporation method, the vacuum degree of the vacuum evaporation method is less than 4*10 -4 Pascal, the coating speed is 0.05nm/s ⁇ 0.5nm/s, and the film thickness is 2 ⁇ 10nm.
  • the coating speed is 0.02nm/s ⁇ 0.08nm/s.
  • the dense metal silver film layer is prepared by vacuum evaporation method, the vacuum degree of the vacuum evaporation method is less than 4*10 -4 Pascal, the coating speed is 0.5nm/s ⁇ 5nm/s, and the film thickness is 50 ⁇ 200nm.
  • the application provides a perovskite solar cell comprising an optical microcavity structure, wherein a discontinuous silver thin film layer and a dense silver thin film layer are introduced as an optical microcavity, under this structure, the incident sunlight passes through calcium After being absorbed by the titanium active layer, the transmitted light is irradiated on the dense silver film, and most of the light is reflected and enters the interior of the perovskite solar cell again to be absorbed by the perovskite active layer.
  • the discontinuous silver thin film does not affect the incidence of light, while the dense silver film layer can reflect most of the incident light. Therefore, the application of the microcavity structure can greatly increase the absorption efficiency of perovskite solar cells for incident sunlight, thereby improving the photoelectric conversion efficiency of the cells.
  • Fig. 1 is the schematic diagram of each stage of the growth of vacuum deposited film in the background technology of the present invention
  • Fig. 2 is the microphotograph of discontinuous silver film layer of the present invention
  • Fig. 3 is the microphotograph of dense silver film layer of the present invention.
  • Fig. 4 is the basic structure schematic diagram of perovskite solar cell of the present invention.
  • FIG. 5 is a schematic diagram of the working principle of the microcavity structure of the perovskite solar cell of the present invention.
  • Fig. 6 is the current-voltage characteristic curve of the embodiment of the present invention and the comparative example.
  • the present invention adds an optical microcavity inside the perovskite solar cell that can improve the light collection efficiency of the perovskite solar cell.
  • This structure is organically combined with the classic perovskite solar cell (including p-i-n and n-i-p structures), increasing the The collection efficiency of incident light does not affect other characteristics of the battery, which improves the photoelectric conversion efficiency of the battery.
  • the embodiment of the present application discloses a perovskite solar cell containing an optical microcavity structure, including a substrate, a discontinuous silver metal film layer, a hole transport layer, a perovskite active layer, an electronic Transport layer and dense metallic silver film layer.
  • FIG. 4 The schematic diagram of the basic structure of the perovskite solar cell described in this application is shown in Figure 4, wherein the basic structure of the p-i-n perovskite solar cell is: 1-substrate (containing a transparent electrode layer); 2-microcavity structure layer; 3-hole transport layer; 4-perovskite active layer; 5-electron transport layer; 6-microcavity structure layer; n-i-p type perovskite solar cell basic structure is: 1-substrate (including transparent electrode layer); 2-microcavity structure layer; 3-electron transport layer; 4-perovskite active layer; 5-hole transport layer; 6-microcavity structure layer.
  • the discontinuous metallic silver thin film layer and the dense metallic silver thin film layer in the present application are used as an optical microcavity, and its working principle is specifically shown in Figure 5, and 1 in Figure 5 -substrate; 2-discontinuous silver film layer; 3-carrier transport layer (hole and electron transport layer) and perovskite active layer; 4-continuous or dense silver film layer; 5-metal electrode; 6- Reflected light; 7-reflected light; 8-incident light.
  • the described substrate (containing transparent electrode) of the perovskite solar cell described in the application is usually hard substrates such as commercial high-transmission FTO glass and ITO glass, or the flexible substrate material (PET, PEN, PI, PC film that covers ITO) wait).
  • hard substrates such as commercial high-transmission FTO glass and ITO glass
  • flexible substrate material PET, PEN, PI, PC film that covers ITO
  • the material of the hole transport layer is usually NiO x , PEDOT:PSS, poly[bis(4-phenyl)(2,4,6-trimethylphenyl)amine](PTAA) and the like.
  • the NiO x layer is usually prepared by a magnetron sputtering method, and the thickness of the NiO x layer is 20-30 nm, preferably 25 nm.
  • the silver film layer (discontinuous layer and dense layer) is prepared by vacuum evaporation, and the thickness and microstructure of the film are prepared by adjusting the evaporation rate and evaporation time, wherein the dense layer can be used as a metal electrode at the same time.
  • the silver thin film thickness of transparent electrode side is 2 ⁇ 10nm, and the microscopic structure of silver thin film layer here is discontinuous island shape, as shown in Figure 2, the translucency performance of described discontinuous silver thin film layer is good, to light The reflection is diffuse reflection; the thickness of the silver film on the metal electrode side is 50-200nm, where the silver film layer is a dense continuous film layer, as shown in Figure 3; the light transmission of the dense silver film layer is poor, and there are mirror surfaces. Excellent reflective and conductive properties.
  • the discontinuous metallic silver thin film layer and the dense metallic silver electrode layer described in this application together constitute a microcavity structure, and the dense metallic silver thin film layer can also serve as a conductive electrode layer.
  • the material of the perovskite active layer is an ABX type 3 compound, wherein A is selected from K + , Rb + , Cs + , CH 3 NH 3 + or CH(NH 2 ) 2 + , B is Pb 2+ , and X is Cl - , Br - , I - or SCN - , the thickness of the perovskite active layer is 100-1000nm.
  • the perovskite active layer material is prepared by a solution processing film forming process from a precursor solution.
  • the electron transport layer is selected from one or more of TiO 2 , SnO 2 , PCBM, C 60 and BCP; preferably, the electron transport layer is a composite film of PCBM or C 60 and BCP.
  • the PCBM film is deposited on the perovskite active layer film by the solution film forming process, and the film thickness is 10-50nm;
  • the C 60 film is deposited on the perovskite active layer film layer by the vacuum thermal evaporation process, and the film thickness is 5-25nm ;
  • the BCP film is also deposited on the PCBM or C 60 film layer by vacuum thermal evaporation process, with a thickness of 5-10nm.
  • the PCBM thin film is prepared by a spin-coating method, and the spin-coating speed is 3000-5000 rpm/min.
  • the vapor deposition rate of the C 60 and BCP is 0.01-0.2 angstroms per second.
  • the metal electrodes are selected from one or more of gold, copper, silver, aluminum and conductive carbon material electrodes.
  • the preparation method of the perovskite solar cell according to the present invention is prepared according to methods well known to those skilled in the art, and can be divided into the following steps carried out in sequence: (1) cleaning of the substrate; (2) preparation of the hole transport layer; (3) Preparation of discontinuous metallic silver thin film layer; (4) Preparation of perovskite active layer precursor solution; (5) Preparation of perovskite active layer: (6) Preparation of electron transport layer; (7) Dense metallic silver thin film layer That is, the metal electrode layer is prepared.
  • the substrate cleaning refers to the substrate material covered with transparent conductive electrodes and flexible substrates such as glass, PET, PC, and PI, which are ultrasonically cleaned twice with surfactant, deionized water, acetone, and isopropanol in sequence, each time for 10 to 15 minutes. Minutes, then dried or blown dry with nitrogen, surface treated with ultraviolet ozone (UVO) or plasma for 10 to 20 minutes before use.
  • transparent conductive electrodes and flexible substrates such as glass, PET, PC, and PI
  • the preparation process of the discontinuous silver thin film is as follows: the degree of vacuum is less than 4*10 -4 Pascals, the coating speed is 0.02nm/s-0.5nm/s, the film thickness is 2-10nm, and the microstructure of the obtained film is discontinuous island-like Crystallization; wherein, the preferred coating speed is 0.02nm/s-0.08nm/s.
  • the preparation process of the continuous and dense silver thin film is as follows: the degree of vacuum is less than 4*10 -4 Pascal, the coating speed is 0.5nm/s-5nm/s, and the film thickness is 50-200nm, to obtain a dense and dense silver film that completely covers the carrier transport layer. Continuous silver film layer.
  • the preparation of the perovskite active layer includes two parts: precursor solution preparation and thin film deposition: the precursor solution is prepared by dissolving methyl ammonium iodide (MAI) and lead iodide (PbI 2 ) in a mixed solvent at a molar ratio of 1:1 Medium; thin film deposition chooses any one of conventional solution film-forming methods such as spin coating method, wire bar coating method, doctor blade coating method, slit extrusion coating method, screen printing, gravure printing, letterpress printing, etc. kind.
  • the mixed solvent is a mixed solvent of DMF and DMSO, the concentration of the solution is 0.5-5 mol/ml, and the volume ratio of the two solvents of DMF and DMSO is (0.2-5):1.
  • the preparation of the perovskite active layer is prepared by uniform coating method, and the high-efficiency perovskite light-absorbing layer is prepared by anti-solvent method, which can be divided into three steps: (I) the precursor liquid is added dropwise to the hole The surface of the transport layer; (II) start to spin-coat to prepare a thin film, and anti-solvent is added dropwise during the spin-coating process to obtain a high-efficiency perovskite active layer; (III) annealing.
  • the solution processing film-forming process of the perovskite active layer is preferably a film preparation process of uniform glue spin coating, doctor blade coating and slit extrusion coating.
  • the spin-coating method adopts a table-top coating machine to spin the film, and the preferred film coating speed is 1000-6000 rpm/min (rev/min).
  • the blade coating method adopts a flat coater to coat the film, the coating speed is 0.02-1 m/min (meter/min), and the coating width is 0.2-5 cm.
  • the solution supply speed is 5-500 microliters/minute
  • the coating speed is 0.2-2m/min
  • the substrate temperature is 25-100°C during coating
  • the coating width is 0.2-5 cm
  • the preparation of the active layer by spin coating is divided into two stages, the first stage is a slow stage, the preferred spin coating speed is 1000 ⁇ 4000rpm/min, and the spin coating time is 1 ⁇ 3 seconds; the second stage is a high speed stage, preferably The spin-coating speed is 4000-5000 rpm/min, and the spin-coating time is 30-50 seconds.
  • the anti-solvent is chlorobenzene
  • the volume of the solvent is 100-200 ⁇ l
  • the anti-solvent is added dropwise 20 seconds before the spin coating stops.
  • the anti-solvent is added within 2 seconds.
  • the perovskite solar cell with optical microcavity structure provided by the present invention is more excellent in photoelectric conversion performance, especially output current.
  • the patterned FTO glass is cleaned by the method described above, and then treated with UVO for 15 minutes for later use;
  • step (3) Spin-coat the perovskite precursor solution described in step (4) on the NiO x hole-transport layer obtained in step (3): the whole spin-coating process is divided into three steps, first with 4000rpm/min spin-coating 3 second; then spin-coat at 5000rpm/min for 30 seconds; finally add 200 ⁇ l of chlorobenzene (anti-solvent) dropwise when 5000rpm/min high-speed spin-coat for 11 seconds. The requirement is that all anti-solvents are added dropwise within 2 seconds.
  • the thickness of the light-absorbing layer is controlled at about 500nm;
  • step (5) The sheet obtained in step (5) is annealed at 130° C. for 20 minutes in an oven and taken out after being cooled;
  • step (6) The sheet obtained in step (6) is moved into a vacuum evaporation chamber, and after vacuuming until the vacuum degree is lower than 4*10 -4 Pa, the thermal evaporation deposition method is started to prepare the electron transport layer; the evaporation rate of C 60 is less than 0.05 angstrom/s, film thickness 20nm; BCP evaporation rate less than 0.1 angstrom/s, film thickness 9nm;
  • the sheet prepared in step (7) is also prepared by the thermal evaporation deposition method to prepare silver electrodes, the vacuum degree is controlled to be lower than 4*10 -4 Pa, the initial evaporation rate is 0.8nm/s, and the online film thickness testing equipment is passed Monitor the real-time film thickness. When the film thickness is greater than 10nm, adjust the evaporation rate to 1.5nm/s. After the film thickness is greater than 20nm, adjust the evaporation rate to 4nm/s. The final thickness of the silver electrode is 100nm, and the perovskite solar cell device is prepared. .
  • Example 1 Preparation of perovskite solar cells based on microcavity structure
  • the substrate after magnetron sputtering NiO x and annealing was moved into the vacuum evaporation chamber, and after vacuuming until the vacuum degree was lower than 4*10 -4 Pa, a discontinuous silver film layer was evaporated, and the evaporation rate was 0.02nm/second, the silver film thickness is controlled to 5nm; the subsequent perovskite active layer, electron transport layer and silver metal electrode layer are the same as those described in Comparative Example 1.
  • Example 1 The evaporation rate of the discontinuous silver thin film layer in Example 1 was changed to 0.08nm/second, the film thickness was 5nm, and the other steps remained unchanged.
  • Example 1 The evaporation rate of the discontinuous silver thin film layer in Example 1 was changed to 0.1 nm/sec, the film thickness was 5 nm, and the other steps remained unchanged.
  • Example 1 The evaporation rate of the discontinuous silver thin film layer in Example 1 was changed to 0.2nm/second, the film thickness was 5nm, and other steps remained unchanged.
  • Example 1 The evaporation rate of the discontinuous silver thin film layer in Example 1 was changed to 0.5nm/second, the film thickness was 5nm, and the other steps remained unchanged.
  • Example 1 The evaporation rate of the discontinuous silver thin film layer in Example 1 was changed to 0.08nm/second, the film thickness was 2nm, and the other steps remained unchanged.
  • Example 8 Preparation of perovskite solar cells based on microcavity structure
  • Example 1 The evaporation rate of the discontinuous silver thin film layer in Example 1 was changed to 0.08nm/second, the film thickness was 8nm, and the other steps remained unchanged.
  • the perovskite solar cell prepared by the above-mentioned embodiment is tested under a standard sunlight intensity (AM1.5G, 100mW/cm 2 ) using a solar simulator (xenon lamp as a light source), and the solar simulation
  • the detectors were calibrated at the National Renewable Energy Laboratory using silicon diodes (with KG9 visible filters). The corresponding test results are shown in Table 1 and Figure 6.
  • the perovskite solar cell based on the microcavity structure of the present invention can adjust the output current value of the battery by regulating the thickness and evaporation rate of the discontinuous silver film, and then can realize the same Traditional structure perovskite solar cells have comparable or higher photoelectric conversion efficiency.

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  • Physics & Mathematics (AREA)
  • Electromagnetism (AREA)
  • Chemical & Material Sciences (AREA)
  • Inorganic Chemistry (AREA)
  • Engineering & Computer Science (AREA)
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Abstract

La présente invention concerne une cellule solaire en pérovskite comprenant une structure de micro-cavité optique. La cellule solaire en pérovskite comprend un substrat, une couche de film mince d'argent métallique discontinue, une couche de transport de trous, une couche active de pérovskite, une couche de transport d'électrons et une couche de film mince d'argent métallique compacte, qui sont empilées séquentiellement ensemble. Par comparaison avec une cellule solaire en pérovskite ayant une structure classique, la cellule solaire en pérovskite ayant une structure de micro-cavité optique selon la présente invention présente de meilleures performances en termes de performances de conversion photoélectrique, en particulier en termes de courant de sortie.
PCT/CN2022/100716 2021-12-15 2022-06-23 Cellule solaire en pérovskite contenant une structure de micro-cavité optique WO2023109071A1 (fr)

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CN106981571A (zh) * 2016-01-15 2017-07-25 深圳清华大学研究院 增强光吸收型钙钛矿薄膜太阳能电池及制备方法
CN107591483A (zh) * 2017-08-22 2018-01-16 电子科技大学 一种混合陷光结构的钙钛矿太阳能电池及其制备方法

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CN108281552A (zh) * 2018-03-06 2018-07-13 电子科技大学 一种具有能带梯度的钙钛矿太阳能电池及其制备方法
CN113258005A (zh) * 2021-04-16 2021-08-13 杭州电子科技大学 一种复合电极构成的有机太阳能电池及制备方法
CN114203916A (zh) * 2021-12-15 2022-03-18 华能新能源股份有限公司 一种包含光学微腔结构的钙钛矿太阳能电池

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