CN114597272B - Sb 2 (S,Se) 3 Matrix heterojunction film, solar cell and cell preparation method thereof - Google Patents
Sb 2 (S,Se) 3 Matrix heterojunction film, solar cell and cell preparation method thereof Download PDFInfo
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- 229910052711 selenium Inorganic materials 0.000 title claims abstract description 83
- 238000002360 preparation method Methods 0.000 title claims abstract description 22
- 239000011159 matrix material Substances 0.000 title abstract description 9
- 239000010408 film Substances 0.000 claims abstract description 86
- 239000002073 nanorod Substances 0.000 claims abstract description 80
- 229910010413 TiO 2 Inorganic materials 0.000 claims abstract description 62
- 239000000463 material Substances 0.000 claims abstract description 35
- 239000002131 composite material Substances 0.000 claims abstract description 25
- 238000006243 chemical reaction Methods 0.000 claims abstract description 20
- 239000000758 substrate Substances 0.000 claims abstract description 19
- 239000010409 thin film Substances 0.000 claims abstract description 14
- 238000003491 array Methods 0.000 claims abstract description 12
- 239000011521 glass Substances 0.000 claims abstract description 12
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- 230000005525 hole transport Effects 0.000 claims abstract description 8
- 230000015572 biosynthetic process Effects 0.000 claims abstract description 4
- 238000013329 compounding Methods 0.000 claims abstract description 4
- 239000011669 selenium Substances 0.000 claims description 76
- OGIDPMRJRNCKJF-UHFFFAOYSA-N titanium oxide Inorganic materials [Ti]=O OGIDPMRJRNCKJF-UHFFFAOYSA-N 0.000 claims description 34
- GWEVSGVZZGPLCZ-UHFFFAOYSA-N Titan oxide Chemical compound O=[Ti]=O GWEVSGVZZGPLCZ-UHFFFAOYSA-N 0.000 claims description 15
- 238000001704 evaporation Methods 0.000 claims description 15
- 239000002105 nanoparticle Substances 0.000 claims description 14
- 230000008020 evaporation Effects 0.000 claims description 12
- 238000004528 spin coating Methods 0.000 claims description 12
- UMGDCJDMYOKAJW-UHFFFAOYSA-N thiourea Chemical compound NC(N)=S UMGDCJDMYOKAJW-UHFFFAOYSA-N 0.000 claims description 12
- VEXZGXHMUGYJMC-UHFFFAOYSA-N Hydrochloric acid Chemical compound Cl VEXZGXHMUGYJMC-UHFFFAOYSA-N 0.000 claims description 10
- 238000000151 deposition Methods 0.000 claims description 10
- ZMXDDKWLCZADIW-UHFFFAOYSA-N N,N-Dimethylformamide Chemical compound CN(C)C=O ZMXDDKWLCZADIW-UHFFFAOYSA-N 0.000 claims description 9
- 238000010438 heat treatment Methods 0.000 claims description 9
- 239000002243 precursor Substances 0.000 claims description 9
- 239000000203 mixture Substances 0.000 claims description 7
- 239000004408 titanium dioxide Substances 0.000 claims description 7
- XDXWNHPWWKGTKO-UHFFFAOYSA-N 207739-72-8 Chemical compound C1=CC(OC)=CC=C1N(C=1C=C2C3(C4=CC(=CC=C4C2=CC=1)N(C=1C=CC(OC)=CC=1)C=1C=CC(OC)=CC=1)C1=CC(=CC=C1C1=CC=C(C=C13)N(C=1C=CC(OC)=CC=1)C=1C=CC(OC)=CC=1)N(C=1C=CC(OC)=CC=1)C=1C=CC(OC)=CC=1)C1=CC=C(OC)C=C1 XDXWNHPWWKGTKO-UHFFFAOYSA-N 0.000 claims description 6
- XSQUKJJJFZCRTK-UHFFFAOYSA-N Urea Natural products NC(N)=O XSQUKJJJFZCRTK-UHFFFAOYSA-N 0.000 claims description 6
- 229910052737 gold Inorganic materials 0.000 claims description 6
- 238000002207 thermal evaporation Methods 0.000 claims description 6
- 229910021617 Indium monochloride Inorganic materials 0.000 claims description 5
- BUGBHKTXTAQXES-UHFFFAOYSA-N Selenium Chemical compound [Se] BUGBHKTXTAQXES-UHFFFAOYSA-N 0.000 claims description 5
- 230000008021 deposition Effects 0.000 claims description 5
- APHGZSBLRQFRCA-UHFFFAOYSA-M indium(1+);chloride Chemical compound [In]Cl APHGZSBLRQFRCA-UHFFFAOYSA-M 0.000 claims description 5
- 239000011261 inert gas Substances 0.000 claims description 5
- 238000002156 mixing Methods 0.000 claims description 5
- 239000000843 powder Substances 0.000 claims description 5
- HKJYVRJHDIPMQB-UHFFFAOYSA-N propan-1-olate;titanium(4+) Chemical compound CCCO[Ti](OCCC)(OCCC)OCCC HKJYVRJHDIPMQB-UHFFFAOYSA-N 0.000 claims description 5
- 239000011248 coating agent Substances 0.000 claims description 4
- 238000000576 coating method Methods 0.000 claims description 4
- 238000001816 cooling Methods 0.000 claims description 4
- -1 said Sb 2 (S Substances 0.000 claims description 4
- 229910052709 silver Inorganic materials 0.000 claims description 4
- 238000003756 stirring Methods 0.000 claims description 4
- XLYOFNOQVPJJNP-UHFFFAOYSA-N water Substances O XLYOFNOQVPJJNP-UHFFFAOYSA-N 0.000 claims description 4
- 229940007424 antimony trisulfide Drugs 0.000 claims description 3
- NVWBARWTDVQPJD-UHFFFAOYSA-N antimony(3+);trisulfide Chemical compound [S-2].[S-2].[S-2].[Sb+3].[Sb+3] NVWBARWTDVQPJD-UHFFFAOYSA-N 0.000 claims description 3
- 238000004140 cleaning Methods 0.000 claims description 3
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- DKAGJZJALZXOOV-UHFFFAOYSA-N hydrate;hydrochloride Chemical compound O.Cl DKAGJZJALZXOOV-UHFFFAOYSA-N 0.000 claims description 2
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- 238000007740 vapor deposition Methods 0.000 claims 1
- 238000013461 design Methods 0.000 abstract description 2
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- 238000002441 X-ray diffraction Methods 0.000 description 5
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- 229910052980 cadmium sulfide Inorganic materials 0.000 description 4
- 238000010586 diagram Methods 0.000 description 4
- MUYUEDVRJJRNOO-UHFFFAOYSA-N selanylidene(sulfanylidene)antimony Chemical compound S=[Sb]=[Se] MUYUEDVRJJRNOO-UHFFFAOYSA-N 0.000 description 4
- 239000011358 absorbing material Substances 0.000 description 3
- 230000007547 defect Effects 0.000 description 3
- 238000000034 method Methods 0.000 description 3
- WUPHOULIZUERAE-UHFFFAOYSA-N 3-(oxolan-2-yl)propanoic acid Chemical compound OC(=O)CCC1CCCO1 WUPHOULIZUERAE-UHFFFAOYSA-N 0.000 description 2
- QTBSBXVTEAMEQO-UHFFFAOYSA-N Acetic acid Chemical compound CC(O)=O QTBSBXVTEAMEQO-UHFFFAOYSA-N 0.000 description 2
- CSCPPACGZOOCGX-UHFFFAOYSA-N Acetone Chemical compound CC(C)=O CSCPPACGZOOCGX-UHFFFAOYSA-N 0.000 description 2
- KFZMGEQAYNKOFK-UHFFFAOYSA-N Isopropanol Chemical compound CC(C)O KFZMGEQAYNKOFK-UHFFFAOYSA-N 0.000 description 2
- NINIDFKCEFEMDL-UHFFFAOYSA-N Sulfur Chemical compound [S] NINIDFKCEFEMDL-UHFFFAOYSA-N 0.000 description 2
- 238000010549 co-Evaporation Methods 0.000 description 2
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- IYKVLICPFCEZOF-UHFFFAOYSA-N selenourea Chemical compound NC(N)=[Se] IYKVLICPFCEZOF-UHFFFAOYSA-N 0.000 description 2
- 238000005245 sintering Methods 0.000 description 2
- 238000004729 solvothermal method Methods 0.000 description 2
- 231100000331 toxic Toxicity 0.000 description 2
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- LFQSCWFLJHTTHZ-UHFFFAOYSA-N Ethanol Chemical compound CCO LFQSCWFLJHTTHZ-UHFFFAOYSA-N 0.000 description 1
- 229960000583 acetic acid Drugs 0.000 description 1
- 239000000956 alloy Substances 0.000 description 1
- 229910045601 alloy Inorganic materials 0.000 description 1
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- 239000008367 deionised water Substances 0.000 description 1
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- 238000000605 extraction Methods 0.000 description 1
- 239000012362 glacial acetic acid Substances 0.000 description 1
- PCHJSUWPFVWCPO-UHFFFAOYSA-N gold Chemical compound [Au] PCHJSUWPFVWCPO-UHFFFAOYSA-N 0.000 description 1
- 238000005286 illumination Methods 0.000 description 1
- 238000002190 incident photon conversion efficiency spectrum Methods 0.000 description 1
- 231100000053 low toxicity Toxicity 0.000 description 1
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- 125000004108 n-butyl group Chemical group [H]C([H])([H])C([H])([H])C([H])([H])C([H])([H])* 0.000 description 1
- 231100000956 nontoxicity Toxicity 0.000 description 1
- 238000010248 power generation Methods 0.000 description 1
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- 239000003440 toxic substance Substances 0.000 description 1
- 229910021642 ultra pure water Inorganic materials 0.000 description 1
- 239000012498 ultrapure water Substances 0.000 description 1
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Classifications
-
- H—ELECTRICITY
- H01—ELECTRIC ELEMENTS
- H01L—SEMICONDUCTOR DEVICES NOT COVERED BY CLASS H10
- H01L31/00—Semiconductor devices sensitive to infrared radiation, light, electromagnetic radiation of shorter wavelength or corpuscular radiation and specially adapted either for the conversion of the energy of such radiation into electrical energy or for the control of electrical energy by such radiation; Processes or apparatus specially adapted for the manufacture or treatment thereof or of parts thereof; Details thereof
- H01L31/0248—Semiconductor devices sensitive to infrared radiation, light, electromagnetic radiation of shorter wavelength or corpuscular radiation and specially adapted either for the conversion of the energy of such radiation into electrical energy or for the control of electrical energy by such radiation; Processes or apparatus specially adapted for the manufacture or treatment thereof or of parts thereof; Details thereof characterised by their semiconductor bodies
- H01L31/0256—Semiconductor devices sensitive to infrared radiation, light, electromagnetic radiation of shorter wavelength or corpuscular radiation and specially adapted either for the conversion of the energy of such radiation into electrical energy or for the control of electrical energy by such radiation; Processes or apparatus specially adapted for the manufacture or treatment thereof or of parts thereof; Details thereof characterised by their semiconductor bodies characterised by the material
- H01L31/0264—Inorganic materials
- H01L31/0328—Inorganic materials including, apart from doping materials or other impurities, semiconductor materials provided for in two or more of groups H01L31/0272 - H01L31/032
- H01L31/0336—Inorganic materials including, apart from doping materials or other impurities, semiconductor materials provided for in two or more of groups H01L31/0272 - H01L31/032 in different semiconductor regions, e.g. Cu2X/CdX hetero-junctions, X being an element of Group VI of the Periodic System
-
- B—PERFORMING OPERATIONS; TRANSPORTING
- B82—NANOTECHNOLOGY
- B82Y—SPECIFIC USES OR APPLICATIONS OF NANOSTRUCTURES; MEASUREMENT OR ANALYSIS OF NANOSTRUCTURES; MANUFACTURE OR TREATMENT OF NANOSTRUCTURES
- B82Y15/00—Nanotechnology for interacting, sensing or actuating, e.g. quantum dots as markers in protein assays or molecular motors
-
- B—PERFORMING OPERATIONS; TRANSPORTING
- B82—NANOTECHNOLOGY
- B82Y—SPECIFIC USES OR APPLICATIONS OF NANOSTRUCTURES; MEASUREMENT OR ANALYSIS OF NANOSTRUCTURES; MANUFACTURE OR TREATMENT OF NANOSTRUCTURES
- B82Y30/00—Nanotechnology for materials or surface science, e.g. nanocomposites
-
- B—PERFORMING OPERATIONS; TRANSPORTING
- B82—NANOTECHNOLOGY
- B82Y—SPECIFIC USES OR APPLICATIONS OF NANOSTRUCTURES; MEASUREMENT OR ANALYSIS OF NANOSTRUCTURES; MANUFACTURE OR TREATMENT OF NANOSTRUCTURES
- B82Y40/00—Manufacture or treatment of nanostructures
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- H—ELECTRICITY
- H01—ELECTRIC ELEMENTS
- H01L—SEMICONDUCTOR DEVICES NOT COVERED BY CLASS H10
- H01L31/00—Semiconductor devices sensitive to infrared radiation, light, electromagnetic radiation of shorter wavelength or corpuscular radiation and specially adapted either for the conversion of the energy of such radiation into electrical energy or for the control of electrical energy by such radiation; Processes or apparatus specially adapted for the manufacture or treatment thereof or of parts thereof; Details thereof
- H01L31/02—Details
- H01L31/0224—Electrodes
- H01L31/022408—Electrodes for devices characterised by at least one potential jump barrier or surface barrier
- H01L31/022425—Electrodes for devices characterised by at least one potential jump barrier or surface barrier for solar cells
-
- H—ELECTRICITY
- H01—ELECTRIC ELEMENTS
- H01L—SEMICONDUCTOR DEVICES NOT COVERED BY CLASS H10
- H01L31/00—Semiconductor devices sensitive to infrared radiation, light, electromagnetic radiation of shorter wavelength or corpuscular radiation and specially adapted either for the conversion of the energy of such radiation into electrical energy or for the control of electrical energy by such radiation; Processes or apparatus specially adapted for the manufacture or treatment thereof or of parts thereof; Details thereof
- H01L31/04—Semiconductor devices sensitive to infrared radiation, light, electromagnetic radiation of shorter wavelength or corpuscular radiation and specially adapted either for the conversion of the energy of such radiation into electrical energy or for the control of electrical energy by such radiation; Processes or apparatus specially adapted for the manufacture or treatment thereof or of parts thereof; Details thereof adapted as photovoltaic [PV] conversion devices
- H01L31/06—Semiconductor devices sensitive to infrared radiation, light, electromagnetic radiation of shorter wavelength or corpuscular radiation and specially adapted either for the conversion of the energy of such radiation into electrical energy or for the control of electrical energy by such radiation; Processes or apparatus specially adapted for the manufacture or treatment thereof or of parts thereof; Details thereof adapted as photovoltaic [PV] conversion devices characterised by at least one potential-jump barrier or surface barrier
- H01L31/072—Semiconductor devices sensitive to infrared radiation, light, electromagnetic radiation of shorter wavelength or corpuscular radiation and specially adapted either for the conversion of the energy of such radiation into electrical energy or for the control of electrical energy by such radiation; Processes or apparatus specially adapted for the manufacture or treatment thereof or of parts thereof; Details thereof 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—ELECTRIC ELEMENTS
- H01L—SEMICONDUCTOR DEVICES NOT COVERED BY CLASS H10
- H01L31/00—Semiconductor devices sensitive to infrared radiation, light, electromagnetic radiation of shorter wavelength or corpuscular radiation and specially adapted either for the conversion of the energy of such radiation into electrical energy or for the control of electrical energy by such radiation; Processes or apparatus specially adapted for the manufacture or treatment thereof or of parts thereof; Details thereof
- H01L31/18—Processes or apparatus specially adapted for the manufacture or treatment of these devices or of parts thereof
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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
-
- 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 discloses Sb 2 (S,Se) 3 A matrix heterojunction film, a solar cell and a cell preparation method thereof relate to the technical field of solar cell material preparation and structural design. An anode, an electron transport layer and Sb are sequentially deposited on the glass substrate 2 (S,Se) 3 A substrate-type heterojunction thin film, an organic hole transport layer, and a cathode; sb (Sb) 2 (S,Se) 3 The substrate type heterojunction film is formed by TiO 2 Nanorod arrays, in 2 S 3 And Sb (Sb) 2 (S,Se) 3 Material layer constitution, tiO 2 Multiple TiO's in a nanorod array 2 Nanorods are vertically grown on the electron transport layer, in 2 S 3 A material layer deposited on the electron transport layer and wrapped on the TiO 2 TiO formation on nanorods 2 /In 2 S 3 Composite nanorod array, sb 2 (S,Se) 3 Material layer wrapping TiO 2 /In 2 S 3 And compounding the nano rod array and filling the middle gap to form the bulk heterojunction film. Sb in the present invention 2 (S,Se) 3 The substrate heterojunction solar cell is simple in preparation method, novel in structure and high in photoelectric conversion efficiency.
Description
Technical Field
The invention belongs to the technical field of solar cell material preparation and structural design, and particularly relates to Sb 2 (S,Se) 3 A matrix heterojunction film, a solar cell and a cell preparation method thereof are provided.
Background
Solar energy is a green sustainable energy source, and increasing the proportion of solar energy in energy supply is one of the main ways of solving environmental pollution and energy crisis. Solar energy is converted into electric energy through a solar cell, photovoltaic power generation is achieved, and the solar energy is an important mode for utilizing the solar energy. The exploration of new material systems, improving cell efficiency and stability, and reducing cell cost has become a major challenge in solar cell research and photovoltaic industry development.
Sb 2 (S,Se) 3 The (selenium antimony sulfide) has the advantages of large earth reserves of contained elements, no toxicity, low price and the like, and the defect and the electronic performance of the material can be regulated and controlled by regulating the content of selenium, so that the selenium antimony sulfide is a potential solar cell light absorbing material. The solar cell with the bulk heterojunction structure formed by the one-dimensional inorganic nano rod or wire array and the light absorbing material has a plurality of advantages, namely the inorganic nano rod or wire array can be used as an electron transmission channel, so that photo-generated electrons can be directly transported to a collector along the nano array grown in an oriented way, and the recombination of charges is reduced; secondly, in the bulk heterojunction structure, a larger charge separation interface area can be obtained, the defect of short effective diffusion length of photo-generated carriers can be overcome, the utilization efficiency of the cell on incident light is improved, and the bulk heterojunction structure has become an important research object in low-price solar cells in recent years.
In the prior art, tang et al (Nat. Energy 2020,5,587-595) prepared Sb on cadmium sulfide films by solvothermal methods using selenourea as a selenium source 2 (S,Se) 3 Film, prepared V oc ＝0.63V、J sc ＝23.70mA/cm 2 And η=10.10% CdS/Sb 2 (S,Se) 3 A flat heterojunction solar cell; however, selenourea is a toxic substance, especially highly toxic to organic substances in water. YIN et al (adv. Mater.2021,33,2006689) prepared Sb on cadmium sulfide film by double source co-evaporation of sulfur powder and a selenizing ladder 2 (S,Se) 3 Thin film, prepared CdS/Sb 2 (S,Se) 3 V of flat heterojunction solar cell oc 、J sc FF and eta respectively reach 0.46V, 30.20mA/cm 2 57.9% and 8.0%; however, the equipment required by the multi-source co-evaporation technology is expensive and the control conditions are severe. In addition, the two battery structures are both flat plates, the extraction of photo-generated charges is limited, and toxic sulfur is used in the batteryCadmium-melting materials.
Disclosure of Invention
Aiming at the defects existing in the prior art, the invention provides Sb 2 (S,Se) 3 In the invention, a solvothermal method and a precursor solution spin-coating method are respectively used for preparing TiO (titanium dioxide) on the basis of a matrix heterojunction film, a solar cell and a cell preparation method of the solar cell 2 Preparation of TiO on nanoparticle films 2 /In 2 S 3 Composite nanorod arrays and then deposited on TiO by vapor deposition process 2 /In 2 S 3 Intermediate gap deposition of Sb in composite nanorod arrays 2 (S,Se) 3 A material layer for forming TiO 2 /In 2 S 3 /Sb 2 (S,Se) 3 Bulk heterojunction film, tiO 2 /In 2 S 3 /Sb 2 (S,Se) 3 The bulk heterojunction film is compounded with the organic hole transport material to establish a structure based on Sb 2 (S,Se) 3 Solar cell of bulk heterojunction thin film (abbreviated as Sb 2 (S,Se) 3 Matrix heterojunction solar cell) and a preparation method thereof, the efficiency of the solar cell reaches eta=10.78%.
The invention is realized by the following technical scheme:
Sb 2 (S,Se) 3 matrix heterojunction film, sb 2 (S,Se) 3 Filling TiO with material layer 2 /In 2 S 3 And compounding the nano rod array and wrapping the nano rod array to form the bulk heterojunction film. TiO (titanium dioxide) 2 /In 2 S 3 The composite nano rod array forms an electron transmission channel, sb 2 (S,Se) 3 The material layer is a light absorption layer. TiO (titanium dioxide) 2 The thickness of the nano rod array is 200-500nm, the diameter of the nano rod is 20-80nm, and the TiO is the same as that of the nano rod array 2 The number density of the nano rods is 50-200/mu m 2 ，In 2 S 3 The thickness of the film layer is 10-100nm, sb 2 (S,Se) 3 The thickness of the film layer is 100-300nm, and the TiO 2 /In 2 S 3 /Sb 2 (S,Se) 3 The thickness of the bulk heterojunction film is 250-550nm.
Sb 2 (S,Se) 3 A substrate-type heterojunction solar cell comprising the aboveSb 2 (S,Se) 3 The matrix heterojunction film is characterized in that: sb (Sb) 2 (S,Se) 3 A substrate type heterojunction film is deposited on the electron transport layer, tiO 2 Multiple TiO's in a nanorod array 2 Nanorods are vertically grown on the electron transport layer, in 2 S 3 A material layer deposited on the electron transport layer and wrapped on the TiO 2 TiO formation on nanorods 2 /In 2 S 3 Composite nanorod array, sb 2 (S,Se) 3 Material layer wrapping TiO 2 /In 2 S 3 Composite nanorod arrays and filling the intermediate gaps to form TiO 2 /In 2 S 3 /Sb 2 (S,Se) 3 An inorganic bulk heterojunction thin film.
Sb 2 (S,Se) 3 The preparation method of the substrate type heterojunction solar cell comprises the following steps:
(1) Etching ITO or FTO layer on conductive glass into desired shape with concentrated hydrochloric acid and Zn powder, cleaning, drying, and depositing 50-100nm thick TiO thereon 2 A nanoparticle film;
(2) Uniformly mixing water and concentrated hydrochloric acid according to the volume ratio of 0.5-1.5:1, then adding tetrapropyl titanate, and fully and uniformly stirring, wherein the volume ratio of the tetrapropyl titanate to the hydrochloric acid-water mixture is 1-2:100; pouring the prepared reaction solution into an autoclave, and depositing TiO 2 The conductive glass of the film is suspended in the reaction solution face down, the reaction kettle is sealed and then placed at the temperature of 150-190 ℃ for reaction for 1-3 hours, finally the film is put in TiO 2 Growth of TiO on nanoparticle films 2 A nanorod array;
(3) InCl at room temperature 3 ·4H 2 O is dissolved in N, N-dimethylformamide, inCl 3 ·4H 2 O concentration is 0.3-0.5mol/L, thiourea is added, and the mixture is stirred at room temperature for 1-3 hours to obtain In 2 S 3 Reacting the precursor solution, wherein InCl 3 ·4H 2 The molar ratio of O to thiourea is 1:2-4; in is to 2 S 3 Drop of reaction precursor solution in TiO obtained in step (2) 2 Coating the nanorod array film with spin coating, repeating spin coating for 1-3 times, and protecting with inert gasHeat treating at 240-300 deg.c for 5-15 min; after the heat treatment is finished, naturally cooling the sample to room temperature to obtain TiO 2 /In 2 S 3 A composite nanorod array film;
(4) Fully mixing selenium powder and antimony trisulfide powder according to a molar ratio of 0-2:1, placing the mixed powder serving as an evaporation source material into an evaporation boat of an evaporation coating instrument, and obtaining TiO (titanium dioxide) in the step (3) 2 /In 2 S 3 The composite nano rod array film sample is placed above an evaporation boat, and the film sample is heated to 200-300 ℃ under the protection of certain vacuum or inert gas, and simultaneously the Sb is obtained by thermal evaporation 2 (S,Se) 3 Deposition of a Material layer onto TiO 2 /In 2 S 3 Forming TiO by filling the intermediate gap on the composite nano-rod array 2 /In 2 S 3 /Sb 2 (S,Se) 3 A bulk heterojunction thin film.
(5) Spin-coating a layer of SpiroOMeTAD, liTFSI and TBP mixture solution with the concentration of 30-80mg/mL on the bulk heterojunction film obtained in the step (4), and carrying out heat treatment for 5-15 minutes at the temperature of 50-150 ℃ in air to obtain a Spiro-OMeTAD hole transport layer film; evaporating Au or Ag film by thermal evaporation to obtain Sb-based alloy 2 (S,Se) 3 A solar cell of a matrix heterojunction film.
The invention has the following beneficial effects:
the invention comprises the following steps:
(1) In terms of core materials, compared with the prior art (Nat. Energy 2020,5,587-595; adv. Mater.2021,33, 2006689), low-toxicity TiO is used 2 /In 2 S 3 As electron acceptor/buffer layer material, and critical Sb 2 (S,Se) 3 The preparation methods of the layers are obviously different, and the preparation method of the invention is easier to realize low-cost and large-area preparation;
(2) In terms of battery structure and performance, the battery adopts a bulk heterojunction structure composed of an inorganic nano rod (or wire) array and a light absorbing material, and has higher photogenerated carrier transmission efficiency and higher photoelectric conversion efficiency. The invention has great application value in the fields of photovoltaic materials, low-price solar cell devices and the like.
Of course, it is not necessary for any one product to practice the invention to achieve all of the advantages set forth above at the same time.
Drawings
In order to more clearly illustrate the technical solutions of the embodiments of the present invention, the drawings that are needed for the description of the embodiments will be briefly described below, and it is obvious that the drawings in the following description are only some embodiments of the present invention, and that other drawings may be obtained according to these drawings without inventive effort for a person skilled in the art.
FIG. 1 is a schematic view of a solar cell structure;
FIG. 2 is a diagram of TiO 2 Nanoparticle films and TiO 2 XRD characterization results of the nanorod array films;
FIG. 3 is a diagram of TiO 2 Nanoparticle films and TiO 2 SEM characterization results of the nanorod array film;
FIG. 4 is a diagram of TiO 2 /In 2 S 3 Composite nanorod array and TiO 2 /In 2 S 3 /Sb 2 (S,Se) 3 XRD characterization results of bulk heterojunction thin films;
FIG. 5 is a diagram of TiO 2 /In 2 S 3 Composite nanorod array and TiO 2 /In 2 S 3 /Sb 2 (S,Se) 3 SEM characterization results of bulk heterojunction thin films;
FIG. 6 is a graph showing the current-voltage (J-V) characteristic characterization of a solar cell;
FIG. 7 is a graph showing the results of characterization of incident photon-electron conversion efficiency (IPCE) of a solar cell;
in the drawings, the list of components represented by the various numbers is as follows:
1-glass substrate, 2-FTO electrode, 3-TiO 2 Nanoparticle films, 4-TiO 2 Nanorods, 5-In 2 S 3 Shell layer, 6-Sb 2 (S,Se) 3 A light absorbing layer, a 7-Spiro-OMeTAD film, and an 8-gold electrode.
Detailed Description
The following description of the embodiments of the present invention will be made clearly and completely with reference to the accompanying drawings, in which it is apparent that the embodiments described are only some embodiments of the present invention, but not all embodiments. All other embodiments, which can be made by those skilled in the art based on the embodiments of the invention without making any inventive effort, are intended to be within the scope of the invention.
Sb 2 (S,Se) 3 The preparation method of the substrate type heterojunction solar cell comprises the following steps:
1、TiO 2 preparation of films and nanorod arrays.
(1-2)TiO 2 Nanoparticle film 3 preparation:
etched FTO conductive glass (size 2.5x2.5 cm 2 15 Ω/≡), respectively ultrasonically cleaning with acetone, isopropanol and ultrapure water for 5 minutes, and drying for later use. Absolute ethyl alcohol, n-butyl titanate and glacial acetic acid are mixed according to the volume ratio of 4:1:0.1 to prepare uniform colorless TiO 2 Sol precursor liquid. 150. Mu.L of TiO 2 Spin-coating sol precursor liquid drops on etched ITO conductive glass (2000 rpm, 30 seconds), and continuously spin-coating twice to obtain TiO 2 A sol film; tiO was added at room temperature 2 After the sol film was stored in a humidifier having a relative humidity of 52% for 12 hours, it was placed in a muffle furnace in an air atmosphere, the temperature of the muffle furnace was raised to 550℃at a heating rate of 1℃per minute, and the temperature was kept for 30 minutes to perform TiO 2 Sintering a sol film; after sintering, cooling the muffle furnace to room temperature at a speed of 1 ℃/min to obtain TiO 2 Nanoparticle film 3.TiO (titanium dioxide) 2 The thickness of the nanoparticle film 3 is controlled by the number of spin-coating times.
(1-2)TiO 2 Preparation of nanorod 4 arrays:
adding 20ml of deionized water into 20ml of concentrated hydrochloric acid, uniformly stirring, and then adding 0.7ml of tetrapropyl titanate, and fully and uniformly stirring; pouring the prepared reaction solution into an autoclave, and then depositing TiO 2 The conductive glass of the film is suspended in the reaction solution face down, the reaction kettle is sealed and then placed at 170 ℃ for reactionFor 2 hours, finally at TiO 2 Growth of TiO on nanoparticle film 3 2 An array of nanorods 4;
characterization of the product of (1-3):
TiO 2 the arrays of nanorods 4 are characterized in FIGS. 2 and 3. X-ray diffraction (XRD) tests showed that TiO 2 The nano rod 4 has a rutile phase structure (JCPLDS 86-0147); scanning Electron Microscope (SEM) pictures showed that the resulting TiO 2 The nanorods 4 were grown perpendicular to the FTO substrate, and had a length of about 350nm, a diameter of about 50nm, and a number density of about 100 nanorods/μm 2 。
2、TiO 2 /In 2 S 3 /Sb 2 (S,Se) 3 And (3) preparing the bulk heterojunction film.
(2-1)TiO 2 Preparation of nanorod 4 arrays: as in example 1.
(2-2) InCl 3 ·4H 2 O is dissolved in N, N-dimethylformamide, inCl 3 ·4H 2 O concentration is 0.4mol/L, thiourea is then added and stirred at room temperature for 2 hours to obtain In 2 S 3 Reacting the precursor solution, wherein InCl 3 ·4H 2 The molar ratio of O to thiourea is 1:3; in is to 2 S 3 Drop of reaction precursor solution in TiO 2 The nanorod 4 array film is coated with a film in a spin mode, the spin coating is repeated for 2 times, and then the film is subjected to heat treatment for 10 minutes at 270 ℃ under the protection of inert gas; after the heat treatment is finished, naturally cooling the sample to room temperature to obtain TiO 2 /In 2 S 3 A composite nanorod array film; fully mixing selenium powder and antimony trisulfide powder according to a molar ratio of 1:1, placing the mixed powder serving as an evaporation source material into an evaporation boat of an evaporation coating instrument, and placing TiO 2 /In 2 S 3 The composite nano rod array film sample is placed above an evaporation boat, and the film sample is heated to 250 ℃ under the protection of certain vacuum or inert gas, and simultaneously, the Sb is obtained by thermal evaporation 2 (S,Se) 3 Deposition of a Material layer on TiO 2 /In 2 S 3 Forming TiO by filling the intermediate gap on the composite nano-rod array 2 /In 2 S 3 /Sb 2 (S,Se) 3 Bulk heterojunction thin film。
(2-3) characterization of the product:
TiO 2 /In 2 S 3 characterization of the composite nanorod arrays is shown In fig. 4 and 5a, and X-ray diffraction (XRD) test shows that In is prepared 2 S 3 Is a cubic phase structure; characterization by scanning electron microscope showed In 2 S 3 The material is tightly packed in TiO 2 Deposition of a certain thickness, in, is formed on the nanorods 4 and at the bottom 2 S 3 The shell layer 5 has a thickness of about 50nm. TiO (titanium dioxide) 2 /In 2 S 3 /Sb 2 (S,Se) 3 Characterization of bulk heterojunction films is shown in fig. 4 and 5b, and it can be seen from X-ray diffraction (XRD) patterns that diffraction peaks are very consistent with that of antimony selenide sulfide (00-052-1649), indicating successful obtainment of antimony selenide sulfide material; characterization of scanning electron microscope showed Sb 2 (S,Se) 3 Tightly wrap on TiO 2 /In 2 S 3 On the composite nano rod, the thickness is 200nm, and TiO is formed 2 /In 2 S 3 /Sb 2 (S,Se) 3 A bulk heterojunction thin film.
3、Sb 2 (S,Se) 3 Preparation of bulk heterojunction solar cells:
(3-1)TiO 2 preparation of nanorod 4 arrays: as in example 1;
(3-2)TiO 2 /In 2 S 3 /Sb 2 (S,Se) 3 preparing a bulk heterojunction film: same as in example 2;
(3-3)Sb 2 (S,Se) 3 and preparing the substrate type heterojunction solar cell.
Spin-coating a layer of SpiroOMeTAD, liTFSI and TBP mixture solution with a concentration of 30-80mg/mL on the bulk heterojunction film obtained in implementation example 2, and performing heat treatment in air at 50-150 ℃ for 5-15 minutes to obtain a Spiro-OMeTAD hole transport layer; evaporating Au film on the hole transport layer by thermal evaporation method to obtain Sb 2 (S,Se) 3 The substrate type heterojunction thin-film solar cell (see figure 1) comprises a glass substrate 1, an FTO electrode 2 and TiO from bottom to top 2 Nanoparticle thin film 3, tiO 2 Nanorods 4, in 2 S 3 Shell layer 5, sb 2 (S,Se) 3 A light absorbing layer 6, a Spiro-OMeTAD film 7 and a gold electrode 8.
(3-4) characterization of the cell:
solar cell performance was characterized by current-voltage (J-V) characteristics and IPCE spectra, see FIGS. 6 and 7. The current-voltage (J-V) curve of the cell was obtained by simulating sunlight (light intensity P) using AM 1.5 in ＝100mW/cm 2 ) Testing was performed. In the J-V test process, the illumination area of the battery is controlled to be below the Au electrode by the shielding window and is consistent with the size of the Au electrode, so that only the area of the photoactive layer of the battery, which is consistent with the size of the Au electrode, is illuminated, and the area is the effective area of the battery; table 1 shows the battery performance parameters obtained by the test, V of the battery oc 、J sc The FF and the energy conversion efficiency (. Eta.) respectively reach 0.67V, 26.29mA/cm 2 61.37% and 10.78%, indicating the prepared Sb 2 (S,Se) 3 The bulk heterojunction battery has good photovoltaic performance. The IPCE spectrum shows that the battery has stronger photon-electron conversion efficiency in the spectral range of 300-1000 nm.
Manufacturing Sb included in the above-described method of manufacturing a battery 2 (S,Se) 3 In the substrate type heterojunction film, sb 2 (S,Se) 3 Filling TiO with material layer 2 /In 2 S 3 Compounding the nano rod array and wrapping the nano rod array to form a bulk heterojunction film, and additionally, tiO 2 /In 2 S 3 The composite nano rod array forms an electron transmission channel, sb 2 (S,Se) 3 The material layer is a light absorption layer, tiO 2 The thickness of the nano rod array is 200-500nm, the diameter of the nano rod is 20-80nm, and the TiO is the same as that of the nano rod array 2 The number density of the nano rods is 50-200/mu m 2 ，In 2 S 3 The thickness of the film layer is 10-100nm, sb 2 (S,Se) 3 The thickness of the film layer is 100-300nm, and the TiO 2 /In 2 S 3 /Sb 2 (S,Se) 3 The thickness of the bulk heterojunction film is250-550nm。
Sb 2 (S,Se) 3 Substrate type heterojunction solar cell, sb described above 2 (S,Se) 3 A substrate type heterojunction film is deposited on the electron transport layer, tiO 2 Multiple TiO's in a nanorod array 2 Nanorods are vertically grown on the electron transport layer, in 2 S 3 A material layer deposited on the electron transport layer and wrapped on the TiO 2 TiO formation on nanorods 2 /In 2 S 3 Composite nanorod array, sb 2 (S,Se) 3 Material layer wrapping TiO 2 /In 2 S 3 Composite nanorod arrays and filling the intermediate gaps to form TiO 2 /In 2 S 3 /Sb 2 (S,Se) 3 An inorganic bulk heterojunction thin film.
The glass substrate is sequentially deposited with an anode, an electron transport layer and Sb 2 (S,Se) 3 The anode of the solar cell is an FTO or ITO layer, and the electron transport layer is TiO 2 The nanometer particle film, the organic hole transport layer is a Spiro-OMeTAD film, and the solar cell cathode is an Au or Ag film.
In the description of the present specification, the descriptions of the terms "one embodiment," "example," "specific example," and the like, mean that a particular feature, structure, material, or characteristic described in connection with the embodiment or example is included in at least one embodiment or example of the present invention. In this specification, schematic representations of the above terms do not necessarily refer to the same embodiments or examples. Furthermore, the particular features, structures, materials, or characteristics described may be combined in any suitable manner in any one or more embodiments or examples.
The preferred embodiments of the invention disclosed above are intended only to assist in the explanation of the invention. The preferred embodiments are not exhaustive or to limit the invention to the precise form disclosed. Obviously, many modifications and variations are possible in light of the above teaching. The embodiments were chosen and described in order to best explain the principles of the invention and the practical application, to thereby enable others skilled in the art to best understand and utilize the invention. The invention is limited only by the claims and the full scope and equivalents thereof.
Claims (5)
1.Sb 2 (S,Se) 3 A substrate-type heterojunction solar cell, characterized in that: comprises Sb 2 (S,Se) 3 A base heterojunction film, said Sb 2 (S,Se) 3 The substrate type heterojunction film is formed by Sb 2 (S,Se) 3 Filling TiO with material layer 2 /In 2 S 3 Compounding the nano rod array and wrapping the nano rod array to form the nano rod array;
Sb 2 (S,Se) 3 a substrate type heterojunction film is deposited on the electron transport layer, tiO 2 Multiple TiO's in a nanorod array 2 Nanorods are vertically grown on the electron transport layer, in 2 S 3 A material layer deposited on the electron transport layer and wrapped on the TiO 2 TiO formation on nanorods 2 /In 2 S 3 Composite nanorod array, sb 2 (S,Se) 3 Material layer wrapping TiO 2 /In 2 S 3 Composite nanorod arrays and filling the intermediate gaps to form TiO 2 /In 2 S 3 /Sb 2 (S,Se) 3 An inorganic bulk heterojunction thin film;
the Sb is as follows 2 (S,Se) 3 The preparation method of the substrate type heterojunction solar cell comprises the following steps:
etching ITO or FTO layer on conductive glass into required shape with concentrated hydrochloric acid and Zn powder, cleaning and drying, and depositing 50-100nm thick TiO thereon 2 A nanoparticle film;
uniformly mixing water and concentrated hydrochloric acid according to the volume ratio of 0.5-1.5:1, then adding tetrapropyl titanate, and fully and uniformly stirring, wherein the volume ratio of the tetrapropyl titanate to the hydrochloric acid-water mixture is 1-2:100; pouring the prepared reaction solution into an autoclave, and depositing TiO 2 The conductive glass surface of the nanoparticle film is suspended downwards and placed in the reaction solution, the reaction kettle is sealed and placed at the temperature of 150-190 ℃ for reaction for 1-3 hours, and finally the reaction kettle is used for TiO 2 Growth of TiO on nanoparticle films 2 A nanorod array;
step three, inCl is added at room temperature 3 ·4H 2 O is dissolved in N, N-dimethylformamide, inCl 3 ·4H 2 O concentration is 0.3-0.5mol/L, thiourea is added, and the mixture is stirred at room temperature for 1-3 hours to obtain In 2 S 3 Reacting the precursor solution, wherein InCl 3 ·4H 2 The molar ratio of O to thiourea is 1:2-4; in is to 2 S 3 Reaction precursor solution drops the TiO obtained in the step two 2 Spin-coating the nanorod array film, repeating spin-coating for 1-3 times, and then performing heat treatment at 240-300 ℃ for 5-15 minutes under the protection of inert gas; after the heat treatment is finished, naturally cooling the sample to room temperature to obtain TiO 2 /In 2 S 3 A composite nanorod array film;
step four, fully mixing selenium powder and antimony trisulfide powder according to a molar ratio of 0-2:1, placing the mixed powder serving as an evaporation source material into an evaporation boat of an evaporation coating instrument, and obtaining TiO (titanium dioxide) in the step three 2 /In 2 S 3 The composite nano rod array film sample is placed above an evaporation boat, and the film sample is heated to 200-300 ℃ under the protection of vacuum or inert gas, and simultaneously, the Sb is obtained by thermal evaporation 2 (S,Se) 3 Deposition of a Material layer onto TiO 2 /In 2 S 3 Forming TiO by filling the intermediate gap on the composite nano-rod array 2 /In 2 S 3 /Sb 2 (S,Se) 3 A bulk heterojunction thin film;
spin-coating a layer of SpiroOMeTAD, liTFSI and TBP mixture solution with the concentration of 30-80mg/mL on the bulk heterojunction film obtained in the step four, and performing heat treatment in air at the temperature of 50-150 ℃ for 5-15 minutes to obtain a Spiro-OMeTAD hole transport layer film; evaporating Au or Ag film by thermal evaporation to obtain Sb 2 (S,Se) 3 A substrate-type heterojunction solar cell.
2. Sb according to claim 1 2 (S,Se) 3 A substrate-type heterojunction solar cell characterized by comprising TiO 2 /In 2 S 3 Composite nano rod array forming electronTransmission channel, sb 2 (S,Se) 3 The material layer is a light absorption layer.
3. Sb according to claim 2 2 (S,Se) 3 A substrate-type heterojunction solar cell characterized by comprising TiO 2 The thickness of the nano rod array is 200-500nm, the diameter of the nano rod is 20-80nm, and the TiO is the same as that of the nano rod array 2 The number density of the nano rods is 50-200/mu m 2 ，In 2 S 3 The thickness of the film layer is 10-100nm, sb 2 (S,Se) 3 The thickness of the film layer is 100-300nm, and the TiO 2 /In 2 S 3 /Sb 2 (S,Se) 3 The thickness of the bulk heterojunction film is 250-550nm.
4. Sb according to claim 1 2 (S,Se) 3 A substrate-type heterojunction solar cell, characterized in that: the glass substrate is sequentially deposited with an anode, an electron transport layer and Sb 2 (S,Se) 3 The anode of the solar cell is an FTO or ITO layer, and the electron transport layer is TiO 2 The nanometer particle film, the organic hole transport layer is a Spiro-OMeTAD film, and the solar cell cathode is an Au or Ag film.
5. Sb according to claim 1 2 (S,Se) 3 A substrate-type heterojunction solar cell, characterized in that: sb in step four 2 (S,Se) 3 The vapor deposition operation of the material layer is performed in a tube furnace or a box furnace.
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