CN114335348B - PN heterojunction antimony selenide/perovskite solar cell and preparation method thereof - Google Patents
PN heterojunction antimony selenide/perovskite solar cell and preparation method thereof Download PDFInfo
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- OQRNKLRIQBVZHK-UHFFFAOYSA-N selanylideneantimony Chemical compound [Sb]=[Se] OQRNKLRIQBVZHK-UHFFFAOYSA-N 0.000 title claims abstract description 50
- 238000002360 preparation method Methods 0.000 title abstract description 31
- 239000000758 substrate Substances 0.000 claims abstract description 47
- 238000010521 absorption reaction Methods 0.000 claims abstract description 39
- 238000000034 method Methods 0.000 claims abstract description 37
- 229910052751 metal Inorganic materials 0.000 claims abstract description 36
- 239000002184 metal Substances 0.000 claims abstract description 36
- 239000000463 material Substances 0.000 claims description 41
- 238000001704 evaporation Methods 0.000 claims description 39
- 230000008020 evaporation Effects 0.000 claims description 30
- 239000002131 composite material Substances 0.000 claims description 24
- 238000000576 coating method Methods 0.000 claims description 18
- 239000011248 coating agent Substances 0.000 claims description 17
- 239000002243 precursor Substances 0.000 claims description 17
- 238000000137 annealing Methods 0.000 claims description 14
- 238000000151 deposition Methods 0.000 claims description 14
- 239000002994 raw material Substances 0.000 claims description 9
- 229910052787 antimony Inorganic materials 0.000 claims description 7
- 238000007738 vacuum evaporation Methods 0.000 claims description 7
- 238000007740 vapor deposition Methods 0.000 claims description 4
- ZOKXTWBITQBERF-UHFFFAOYSA-N Molybdenum Chemical group [Mo] ZOKXTWBITQBERF-UHFFFAOYSA-N 0.000 claims description 3
- 238000004519 manufacturing process Methods 0.000 claims description 2
- 229910052750 molybdenum Inorganic materials 0.000 claims description 2
- 239000011733 molybdenum Substances 0.000 claims description 2
- 230000005540 biological transmission Effects 0.000 abstract description 10
- 238000006243 chemical reaction Methods 0.000 abstract description 6
- 239000006096 absorbing agent Substances 0.000 abstract description 4
- 239000000969 carrier Substances 0.000 abstract description 4
- 238000001228 spectrum Methods 0.000 abstract description 4
- IAZDPXIOMUYVGZ-UHFFFAOYSA-N Dimethylsulphoxide Chemical compound CS(C)=O IAZDPXIOMUYVGZ-UHFFFAOYSA-N 0.000 description 24
- 239000000243 solution Substances 0.000 description 24
- LYQFWZFBNBDLEO-UHFFFAOYSA-M caesium bromide Chemical compound [Br-].[Cs+] LYQFWZFBNBDLEO-UHFFFAOYSA-M 0.000 description 14
- 239000000843 powder Substances 0.000 description 12
- 239000011888 foil Substances 0.000 description 11
- CSCPPACGZOOCGX-UHFFFAOYSA-N Acetone Chemical compound CC(C)=O CSCPPACGZOOCGX-UHFFFAOYSA-N 0.000 description 10
- WEVYAHXRMPXWCK-UHFFFAOYSA-N Acetonitrile Chemical compound CC#N WEVYAHXRMPXWCK-UHFFFAOYSA-N 0.000 description 9
- 229910001220 stainless steel Inorganic materials 0.000 description 9
- 239000010935 stainless steel Substances 0.000 description 9
- LFQSCWFLJHTTHZ-UHFFFAOYSA-N Ethanol Chemical compound CCO LFQSCWFLJHTTHZ-UHFFFAOYSA-N 0.000 description 8
- 238000010586 diagram Methods 0.000 description 7
- 239000002904 solvent Substances 0.000 description 7
- BAVYZALUXZFZLV-UHFFFAOYSA-N Methylamine Chemical compound NC BAVYZALUXZFZLV-UHFFFAOYSA-N 0.000 description 6
- 238000001755 magnetron sputter deposition Methods 0.000 description 6
- 239000008367 deionised water Substances 0.000 description 5
- 229910021641 deionized water Inorganic materials 0.000 description 5
- 238000001035 drying Methods 0.000 description 5
- 238000005498 polishing Methods 0.000 description 5
- 238000004506 ultrasonic cleaning Methods 0.000 description 5
- XLYOFNOQVPJJNP-UHFFFAOYSA-N water Chemical compound O XLYOFNOQVPJJNP-UHFFFAOYSA-N 0.000 description 5
- GWEVSGVZZGPLCZ-UHFFFAOYSA-N Titan oxide Chemical compound O=[Ti]=O GWEVSGVZZGPLCZ-UHFFFAOYSA-N 0.000 description 4
- XLOMVQKBTHCTTD-UHFFFAOYSA-N Zinc monoxide Chemical compound [Zn]=O XLOMVQKBTHCTTD-UHFFFAOYSA-N 0.000 description 4
- 239000002250 absorbent Substances 0.000 description 4
- 230000002745 absorbent Effects 0.000 description 4
- 230000008021 deposition Effects 0.000 description 4
- 239000010408 film Substances 0.000 description 4
- 238000002347 injection Methods 0.000 description 4
- 239000007924 injection Substances 0.000 description 4
- 238000004544 sputter deposition Methods 0.000 description 4
- XOLBLPGZBRYERU-UHFFFAOYSA-N tin dioxide Chemical compound O=[Sn]=O XOLBLPGZBRYERU-UHFFFAOYSA-N 0.000 description 4
- 229910001887 tin oxide Inorganic materials 0.000 description 4
- XUIMIQQOPSSXEZ-UHFFFAOYSA-N Silicon Chemical group [Si] XUIMIQQOPSSXEZ-UHFFFAOYSA-N 0.000 description 3
- GUVUOGQBMYCBQP-UHFFFAOYSA-N dmpu Chemical compound CN1CCCN(C)C1=O GUVUOGQBMYCBQP-UHFFFAOYSA-N 0.000 description 3
- 235000019441 ethanol Nutrition 0.000 description 3
- 229910052710 silicon Inorganic materials 0.000 description 3
- 239000010703 silicon Substances 0.000 description 3
- MARUHZGHZWCEQU-UHFFFAOYSA-N 5-phenyl-2h-tetrazole Chemical compound C1=CC=CC=C1C1=NNN=N1 MARUHZGHZWCEQU-UHFFFAOYSA-N 0.000 description 2
- KTSFMFGEAAANTF-UHFFFAOYSA-N [Cu].[Se].[Se].[In] Chemical compound [Cu].[Se].[Se].[In] KTSFMFGEAAANTF-UHFFFAOYSA-N 0.000 description 2
- 229910001507 metal halide Inorganic materials 0.000 description 2
- 150000005309 metal halides Chemical class 0.000 description 2
- 238000013082 photovoltaic technology Methods 0.000 description 2
- 238000012360 testing method Methods 0.000 description 2
- 239000004408 titanium dioxide Substances 0.000 description 2
- 239000011787 zinc oxide Substances 0.000 description 2
- JBRZTFJDHDCESZ-UHFFFAOYSA-N AsGa Chemical compound [As]#[Ga] JBRZTFJDHDCESZ-UHFFFAOYSA-N 0.000 description 1
- 229910010413 TiO 2 Inorganic materials 0.000 description 1
- 229910000611 Zinc aluminium Inorganic materials 0.000 description 1
- 239000011358 absorbing material Substances 0.000 description 1
- 238000000862 absorption spectrum Methods 0.000 description 1
- 229910021417 amorphous silicon Inorganic materials 0.000 description 1
- 239000003153 chemical reaction reagent Substances 0.000 description 1
- 150000001875 compounds Chemical class 0.000 description 1
- HVMJUDPAXRRVQO-UHFFFAOYSA-N copper indium Chemical compound [Cu].[In] HVMJUDPAXRRVQO-UHFFFAOYSA-N 0.000 description 1
- 239000013078 crystal Substances 0.000 description 1
- 229910021419 crystalline silicon Inorganic materials 0.000 description 1
- 238000013461 design Methods 0.000 description 1
- 238000001514 detection method Methods 0.000 description 1
- 238000011161 development Methods 0.000 description 1
- ZZEMEJKDTZOXOI-UHFFFAOYSA-N digallium;selenium(2-) Chemical compound [Ga+3].[Ga+3].[Se-2].[Se-2].[Se-2] ZZEMEJKDTZOXOI-UHFFFAOYSA-N 0.000 description 1
- 238000002474 experimental method Methods 0.000 description 1
- 239000011521 glass Substances 0.000 description 1
- 238000000227 grinding Methods 0.000 description 1
- 230000005525 hole transport Effects 0.000 description 1
- 150000002500 ions Chemical class 0.000 description 1
- 230000031700 light absorption Effects 0.000 description 1
- 229910021645 metal ion Inorganic materials 0.000 description 1
- 229910021421 monocrystalline silicon Inorganic materials 0.000 description 1
- 229910021420 polycrystalline silicon Inorganic materials 0.000 description 1
- 239000002096 quantum dot Substances 0.000 description 1
- 239000004065 semiconductor Substances 0.000 description 1
- 238000004528 spin coating Methods 0.000 description 1
- 238000005507 spraying Methods 0.000 description 1
- 239000010409 thin film Substances 0.000 description 1
- 230000005641 tunneling Effects 0.000 description 1
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- H01L—SEMICONDUCTOR DEVICES NOT COVERED BY CLASS H10
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- 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 potential barriers
- 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 potential barriers the potential barriers being only of the PN heterojunction type
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Abstract
The invention provides a PN heterojunction antimony selenide/perovskite solar cell which comprises a substrate, a metal back electrode, a P-type antimony selenide layer, an N-type perovskite absorption layer and a conductive electrode which are sequentially arranged. Compared with the prior art, the multi-junction solar cell is formed by a plurality of light absorbers with different band gaps, so that the utilization range of solar spectrum can be widened, the thermal relaxation loss of photo-generated carriers can be reduced, and the photoelectric conversion efficiency can be improved; and the invention passes through PN heterojunction Sb 2 Se 3 And the perovskite absorption layer does not need an electron transmission layer, a hole transmission layer and the like, reduces the process preparation steps and the cost, and improves the stability of the battery.
Description
Technical Field
The invention belongs to the technical field of solar cells, and particularly relates to a PN heterojunction antimony selenide/perovskite solar cell and a preparation method thereof.
Background
Solar cells, which can convert solar energy into electric energy through photoelectric conversion, are being directly used by people to pay attention. Solar cells can be classified into three types according to the development of solar cells and the light absorbing layer materials used. The first category is silicon-based solar cells, including single crystal silicon, polycrystalline silicon solar cells, amorphous silicon thin film solar cells, and stacked solar cells of silicon; the second category is compound solar cells, including Copper Indium Gallium Selenide (CIGS), cadmium telluride (CdTe), gallium arsenide (GaAs), and perovskite; the third category is novel solar cells, including dye sensitized solar cells, organic solar cells, quantum dot solar cells, and the like.
Among them, the perovskite type solar cell (perovskite solar cells) is a solar cell using a perovskite type organic metal halide semiconductor as a light absorbing material, and belongs to the third generation solar cell, and is also called a new concept solar cell.
Perovskite solar cells, which use organic-inorganic hybrid metal halides having a perovskite crystal structure as light-absorbing layers, have been attracting attention since 2009 because of their simple preparation method, low production cost and excellent photoelectric properties, and the photoelectric conversion efficiency has rapidly increased from 3.8% to 25%, and have become the photovoltaic technology currently developing fastest, and have been the emerging photovoltaic technology in the world.
Single junction solar cells have a schottky-Queisser (Shockley-Queisser) efficiency limit because they can only absorb photons within a specific range. The multi-junction solar cell is composed of a plurality of light absorbers with different band gaps, so that the utilization range of solar spectrum can be widened, and meanwhile, the thermal relaxation loss of photo-generated carriers can be reduced. At present, perovskite is mainly overlapped with crystalline silicon, copper indium gallium diselenide, perovskite and the like to form a double-junction or multi-junction battery device. However, the double-junction perovskite laminated cell is prepared by the procedures of an electron transmission layer, a wide-bandgap absorption layer, a hole transmission layer, a middle tunneling layer, a hole transmission layer, a narrow-bandgap absorption layer, an electron transmission layer and the like, and has a complex structure, for example, chinese patent publication No. CN111244220A discloses an all-inorganic P/N heterojunction antimony selenide/perovskite solar cell and a preparation method thereof, and the double-junction perovskite laminated cell comprisesThe structure of the solar cell is an FTO conductive glass substrate and titanium dioxide (TiO) 2 ) Layer, inorganic CsPbBri 2 Perovskite layer, selenized Sb 2 Se 3 The layer and the metal counter electrode layer, in which the inorganic perovskite layer is not N-type treated, still require an electron transport layer of TiO 2 Is prepared by the following steps.
Disclosure of Invention
In view of the above, the technical problem to be solved by the invention is to provide a PN heterojunction antimony selenide/perovskite solar cell with a wider absorption spectrum and a simple structure and a preparation method thereof.
The invention provides a PN heterojunction antimony selenide/perovskite solar cell which comprises a substrate, a metal back electrode, a P-type antimony selenide layer, an N-type perovskite absorption layer and a conductive electrode which are sequentially arranged.
Preferably, the substrate is a flexible metal substrate; the thickness of the substrate is 0.1-0.3 mm.
Preferably, the material of the metal back electrode is molybdenum; the thickness of the metal back electrode is 800-1000 mm.
Preferably, the thickness of the P-type antimony selenide layer is 50-300 nm.
Preferably, the thickness of the N-type perovskite absorption layer is 100-200 mm.
Preferably, the material of the N-type perovskite absorption layer is ABX doped with N-type material 3 The method comprises the steps of carrying out a first treatment on the surface of the Wherein A is one or more of MA, FA, cs and PEA; MA is CH 3 NH 3 The method comprises the steps of carrying out a first treatment on the surface of the FA is NH 2 CHNH 2 The method comprises the steps of carrying out a first treatment on the surface of the PEA is C 8 H 9 NH 3 The method comprises the steps of carrying out a first treatment on the surface of the B is Pb and/or Sn; x is one or more of Cl, br and I; the N-type material comprises Bi 3+ 、Sb 3+ 、Fe 3+ With Al 3+ One or more of the following.
Preferably, the molar ratio of the N-type material to B in the N-type perovskite absorption layer is (0.01 to 0.05): (0.95-0.99).
The invention also provides a preparation method of the PN heterojunction antimony selenide/perovskite solar cell, which comprises the following steps:
s1) depositing a metal back electrode on a substrate to obtain a substrate of a composite metal back electrode;
s2) evaporating a P-type antimony selenide layer on the substrate of the composite metal back electrode to obtain a substrate of the composite P-type antimony selenide layer;
s3) coating the N-type perovskite precursor solution on the surface of the substrate of the composite P-type antimony selenide layer, and annealing to obtain the substrate of the composite N-type perovskite absorption layer;
s4) depositing a conductive electrode on the substrate of the composite N-type perovskite absorption layer to obtain the PN heterojunction antimony selenide/perovskite solar cell.
Preferably, the evaporation in the step S2) is vacuum evaporation; the vacuum degree of the evaporation is less than 4 multiplied by 10 -4 Pa; the evaporation temperature is 300-600 ℃; the vapor deposition rate is 0.3 to 1.5 angstrom/second; the evaporation raw materials are Se and Sb 2 Se 3 。
Preferably, the N-type perovskite precursor solution comprises AX, BX 2 And an N-type doping material; a is one or more of MA, FA, cs and PEA; MA is CH 3 NH 3 The method comprises the steps of carrying out a first treatment on the surface of the FA is NH 2 CHNH 2 The method comprises the steps of carrying out a first treatment on the surface of the PEA is C 8 H 9 NH 3 The method comprises the steps of carrying out a first treatment on the surface of the B is Pb and/or Sn; x is one or more of Cl, br and I; the N-type doping material comprises Bi 3+ 、Sb 3+ 、Fe 3+ With Al 3+ One or more of the following; the annealing temperature is 70-150 ℃; the annealing time is 10-60 min.
The invention provides a PN heterojunction antimony selenide/perovskite solar cell which comprises a substrate, a metal back electrode, a P-type antimony selenide layer, an N-type perovskite absorption layer and a conductive electrode which are sequentially arranged. Compared with the prior art, the multi-junction solar cell is formed by a plurality of light absorbers with different band gaps, so that the utilization range of solar spectrum can be widened, the thermal relaxation loss of photo-generated carriers can be reduced, and the photoelectric conversion efficiency can be improved; and the invention passes through PN heterojunction Sb 2 Se 3 The perovskite absorption layer does not need an electron transport layer, a hole transport layer and the like, reduces the process preparation steps and the cost, and improves the stability of the battery.
Compared with a double-junction perovskite laminated battery, the preparation of an electron and/or hole transmission layer and an intermediate composite layer is not needed, the 1.4-2.0 eV wide-bandgap N-type perovskite battery doped with metal ions is directly prepared on the 1.1-1.3 eV narrow-bandgap P-type antimony selenide layer by blade coating, PN heterojunction structures with different bandgaps can be formed, meanwhile, the preparation of an electron transmission layer and/or an electron transmission layer is not needed through the doping of the perovskite layer strong N-type ions, and the preparation method has the advantages of simple working procedure, low cost, wide light absorption range and the like, and the technical difficulty of battery design and preparation is reduced.
Experiments show that the photoelectric conversion efficiency of the PN heterojunction antimony selenide/perovskite solar cell prepared by the method can reach 17.5%.
Drawings
Fig. 1 is a schematic structural diagram of a PN heterojunction antimony selenide/perovskite solar cell provided by the invention;
FIG. 2 is a schematic diagram showing the structure of an apparatus for evaporating antimony selenide used in the embodiment of the invention.
Detailed Description
The technical solutions of the embodiments of the present invention will be clearly and completely described below in conjunction with the embodiments of the present invention, and it is apparent that the described embodiments are only some embodiments of the present invention, 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.
The invention provides a PN heterojunction antimony selenide/perovskite solar cell which comprises a substrate, a metal back electrode, a P-type antimony selenide layer, an N-type perovskite absorption layer and a conductive electrode which are sequentially arranged.
Referring to fig. 1, fig. 1 is a schematic structural diagram of a PN heterojunction antimony selenide/perovskite solar cell provided by the invention; wherein 1 is a substrate, 2 is a metal back electrode, 3 is a P-type antimony selenide layer, 4 is an N-type perovskite absorption layer, and 5 is a conductive electrode.
The substrate is not particularly limited, and is preferably a metal foil, more preferably a stainless steel foil; the thickness of the substrate is preferably 0.1 to 0.3mm.
A metal back electrode is arranged on the substrate; the metal back electrode is a metal back electrode well known to the skilled person, and is not particularly limited, and is preferably molybdenum metal in the present invention; the thickness of the back electrode is preferably 800-1000 nm.
The metal back electrode is provided with a P-type antimony selenide layer; the thickness of the P-type antimony selenide layer is preferably 50-300 nm.
An N-type perovskite absorption layer is arranged on the P-type antimony selenide layer; the thickness of the N-type perovskite absorption layer is preferably 100-200 mm, more preferably 120-150 nm, still more preferably 130-150 nm, and most preferably 150mm; the material of the N-type perovskite absorption layer is preferably ABX doped with N-type material 3 The method comprises the steps of carrying out a first treatment on the surface of the Wherein A is one or more of MA, FA, cs and PEA; MA is CH 3 NH 3 The method comprises the steps of carrying out a first treatment on the surface of the FA is NH 2 CHNH 2 The method comprises the steps of carrying out a first treatment on the surface of the PEA is C 8 H 9 NH 3 The method comprises the steps of carrying out a first treatment on the surface of the B is Pb and/or Sn; x is one or more of Cl, br and I; in the embodiment provided by the invention, A is MA and/or Cs and FA; the molar ratio of MA and/or Cs to FA is preferably (0.1-0.2): (0.8 to 0.9), more preferably 0.15:0.85; the N-type material comprises Bi 3+ 、Sb 3+ 、Fe 3+ With Al 3+ One or more of the following; the molar ratio of the N-type material to B in the N-type perovskite absorption layer is preferably (0.01-0.05): (0.95 to 0.99), more preferably (0.03 to 0.05): (0.95-0.97).
A conductive electrode is arranged on the N-type perovskite absorption layer; the conductive electrode is preferably a transparent electrode, more preferably one or more of ITO, zinc oxide and aluminum-doped zinc oxide; the thickness of the conductive electrode is preferably 100-1000 nm.
The multi-junction solar cell is formed by a plurality of light absorbers with different band gaps, so that the utilization range of solar spectrum can be widened, the thermal relaxation loss of photo-generated carriers can be reduced, and the photoelectric conversion efficiency is improved; and the invention passes through PN heterojunction Sb 2 Se 3 Perovskite absorption layer, no electron transport layer and no holes are neededAnd a transmission layer, etc., reduces the process preparation steps and cost, and improves the stability of the battery.
The invention also provides a preparation method of the PN heterojunction antimony selenide/perovskite solar cell, which comprises the following steps: s1) depositing a metal back electrode on a substrate to obtain a substrate of a composite metal back electrode; s2) evaporating a P-type antimony selenide layer on the substrate of the composite metal back electrode to obtain a substrate of the composite P-type antimony selenide layer; s3) coating the N-type perovskite precursor solution on the surface of the substrate of the composite P-type antimony selenide layer, and annealing to obtain the substrate of the composite N-type perovskite absorption layer; s4) depositing a conductive electrode on the substrate of the composite N-type perovskite absorption layer to obtain the PN heterojunction antimony selenide/perovskite solar cell.
The sources of all raw materials are not particularly limited, and the raw materials are commercially available; the substrate, the metal back electrode, the P-type antimony selenide layer, the N-type perovskite absorption layer and the conductive electrode are all as described above, and are not described here again.
In the present invention, the substrate is preferably pretreated first; since the substrate is preferably a metal foil in the present invention, the pretreatment preferably includes grinding and polishing, and then sequentially ultrasonic cleaning with deionized water, absolute ethyl alcohol and acetone, and drying.
Depositing a metal back electrode on the pretreated substrate to obtain a substrate of a composite metal back electrode; the method for depositing the metal back electrode is a method well known to those skilled in the art, and is not particularly limited, and magnetron sputtering is preferably used in the present invention.
Evaporating a P-type antimony selenide layer on the substrate of the composite back electrode to obtain a substrate of the P-type antimony selenide layer; the method of vapor deposition is preferably a method well known to those skilled in the art, and is not particularly limited, but vacuum vapor deposition is preferred in the present invention; the evaporation is preferably performed under vacuum degree of less than 4×10 -4 Is carried out under the condition of (2); the temperature of the evaporation is preferably 300-600 ℃; the evaporation rate is preferably 0.1 to 1.5 angstrom/second; the evaporation raw materials are preferably Se and Sb 2 Se 3 The method comprises the steps of carrying out a first treatment on the surface of the The Se and the Sb 2 Se 3 Is a vapor rate of (2)The ratio is 1: (10 to 15), more preferably 1: (10-12).
Coating the N-type perovskite precursor solution on the surface of the substrate of the composite P-type antimony selenide layer, and annealing to obtain the substrate of the composite N-type perovskite absorption layer; the N-type perovskite precursor solution preferably comprises AX and BX 2 And N-type material; a is one or more of MA, FA, cs and PEA, more preferably one or two of Cs and MA and FA; the molar ratio of one or two of Cs and MA to FA is preferably (0.05-0.5): (0.7 to 0.95), more preferably (0.1 to 0.5): (0.7 to 0.9), more preferably (0.15 to 0.5): 0.85; MA is CH 3 NH 3 The method comprises the steps of carrying out a first treatment on the surface of the FA is NH 2 CHNH 2 The method comprises the steps of carrying out a first treatment on the surface of the PEA is C 8 H 9 NH 3 The method comprises the steps of carrying out a first treatment on the surface of the B is Pb and/or Sn; x is one or more of Cl, br and I; the N-type material preferably comprises Bi 3+ 、Sb 3+ 、Fe 3+ With Al 3+ One or more of the following; the solvent of the N-type perovskite precursor solution is preferably one or more of DMF, NMP, 2ME, DMSO, DMPU, acetonitrile and methylamine alcohol, more preferably one or more of NMP, 2ME, DMSO, DMPU, acetonitrile and methylamine alcohol and DMF; the volume ratio of one or more of NMP, 2ME, DMSO, DMPU, acetonitrile and methylamine alcohol to DMF is preferably (2-4): (6-8); in the embodiment provided by the invention, the solvent of the N-type perovskite precursor solution is specifically a solvent with a volume ratio of 6:4, the volume ratio of the DMF to the DMSO is 6:2:2 with DMSO and 2ME, the volume ratio of 7:3:0.25 DMF and 2ME and NMP in a ratio of 8:2:0.25 of DMF and 2ME and NMP; ABX in the N-type perovskite precursor solution 3 The concentration of (C) is preferably 0.1 to 1.5mol/mL; wet forming the N-type perovskite precursor solution into a film by coating, wherein the coating method may be coating, spraying, spin coating, or the like, and is not particularly limited; the annealing temperature is preferably 70-150 ℃; the annealing time is preferably 10 to 60 minutes.
Depositing a conductive electrode on the substrate of the composite N-type perovskite absorption layer to obtain a PN heterojunction antimony selenide/perovskite solar cell; the method for depositing the conductive electrode is a method well known to those skilled in the art, and is not particularly limited, and vacuum evaporation or magnetron sputtering is preferred in the present invention.
To further illustrate the present invention, the following examples are provided to illustrate a PN heterojunction antimony selenide/perovskite solar cell and a method for preparing the same.
The reagents used in the examples below are all commercially available.
Example 1
1) Selecting a stainless steel foil (1) with the thickness of 0.2mm, polishing, respectively adopting deionized water, absolute ethyl alcohol and acetone to carry out ultrasonic cleaning for 30min, and then drying;
2) Preparation of a metal back electrode (2): mo is deposited on the stainless steel foil (1) by magnetron sputtering to be used as a back electrode of the battery, and the deposition thickness is 800nm;
3)Sb 2 Se 3 preparation of the absorbent layer (3): at a vacuum level of less than 4 x 10 -4 Evaporating a layer of Sb with thickness of 300nm by vacuum evaporation at 350 ℃ under Pa 2 Se 3 A layer. Wherein the evaporation raw materials are Se and Sb 2 Se 3 Powder, se powder with evaporation rate of 0.1 angstrom/second, sb 2 Se 3 The evaporation rate of the powder was 1.2 angstrom/sec. The structure schematic diagram of the evaporation equipment is shown in fig. 2; wherein 2-1 is a heat insulating layer, 2-2 is a Se evaporation source, 2-3 is a bottom heater, and 2-4 is Sb 2 Se 3 2-5 parts of evaporation source are top heaters, and 2-6 parts of distributor.
4) Preparation of an N-type perovskite absorption layer (4): preparing N-type perovskite material solution, wherein solute is PbI 2 MAI, FAI, wherein the molar ratio of MAI to FAI is 0.15:0.85.PbI 2 The molar ratio to (MAI+FAI) was 1:1. bi is selected in the present embodiment 3+ As N-type doping material, wherein BiI 3 With PbI 2 Molar ratio of 0.05:0.95, the solvent is DMF and DMSO, wherein the volume ratio of DMF to DMSO is 6:4, forming perovskite precursor solution doped with N-type material, wherein the concentration of the perovskite precursor solution is 1 mol/mL; then the N-type perovskite material solution is coated with wet film forming, wherein the coating speed is 12mm/s, the coating injection amount is 170uL, and then annealing treatment is carried out for 20min at 120 ℃ to formAn N-type perovskite material layer having a thickness of about 120nm;
5) Preparation of the counter electrode (5): and (3) magnetically sputtering a layer of indium-doped tin oxide with a thickness of 200nm on the N-type perovskite absorption layer (4).
Example 2
1) Selecting a stainless steel foil (1) with the thickness of 0.2mm, polishing, respectively adopting deionized water, absolute ethyl alcohol and acetone to carry out ultrasonic cleaning for 30min, and then drying;
2) Preparation of a metal back electrode (2): mo is deposited on the stainless steel foil (1) by magnetron sputtering to be used as a back electrode of the battery, and the deposition thickness is 1000nm;
3)Sb 2 Se 3 preparation of the absorbent layer (3): at a vacuum level of less than 4 x 10 -4 Evaporating a layer of Sb with thickness of 300nm by vacuum evaporation at 350 ℃ under Pa 2 Se 3 A layer. Wherein the evaporation raw materials are Se and Sb 2 Se 3 Powder, se powder with evaporation rate of 0.1 angstrom/second, sb 2 Se 3 The evaporation rate of the powder was 1 angstrom/sec. A schematic diagram of the evaporation apparatus is shown in fig. 2.
4) Preparation of an N-type perovskite absorption layer (4): preparing N-type perovskite material solution, wherein solute is PbI 2 CsBr, FAI, wherein the molar ratio of CsBr to FAI is 0.15:0.85.PbI 2 The molar ratio to (csbr+fai) was 1:1. in this example, sb is selected 3+ As N-type doping material, wherein SbI 3 With PbI 2 The molar ratio of (2) is 0.03:0.97 of DMF, DMSO and 2ME, wherein the volume ratio of the solvent is 6:2:2, forming perovskite precursor solution doped with N-type material, wherein the concentration of the perovskite precursor solution is 1 mol/ml; then coating the N-type perovskite material solution into a film by a wet method, wherein the coating speed is 11mm/s, the coating injection amount is 170uL, and then annealing at 120 ℃ for 20min to form an N-type perovskite material layer, and the thickness is about 110nm;
5) Preparation of the counter electrode (5): and (3) magnetically sputtering a layer of indium-doped tin oxide with a thickness of 300nm on the N-type perovskite absorption layer (4).
Example 3
1) Selecting a stainless steel foil (1) with the thickness of 0.2mm, polishing, respectively adopting deionized water, absolute ethyl alcohol and acetone to carry out ultrasonic cleaning for 30min, and then drying;
2) Preparation of a metal back electrode (2): mo is deposited on the stainless steel foil (1) by magnetron sputtering to be used as a back electrode of the battery, and the deposition thickness is 800nm;
3)Sb 2 Se 3 preparation of the absorbent layer (3): at a vacuum level of less than 4 x 10 -4 Evaporating a layer of Sb with thickness of 300nm by vacuum evaporation at 350 ℃ under Pa 2 Se 3 A layer. Wherein the evaporation raw materials are Se and Sb 2 Se 3 Powder, se powder with evaporation rate of 0.1 angstrom/second, sb 2 Se 3 The evaporation rate of the powder was 1.2 angstrom/sec. A schematic diagram of the evaporation apparatus is shown in fig. 2.
4) Preparation of an N-type perovskite absorption layer (4): preparing N-type perovskite material solution, wherein solute is PbI 2 CsBr, FAI, MACl, wherein the molar ratio CsBr to FAI is 0.15:0.85.PbI 2 The molar ratio to (csbr+fai) was 1:1, molar ratio of MACl to (CsBr+FAI) 0.35:1. bi is selected in the present embodiment 3+ As N-type doping material, wherein BiI 3 With PbI 2 The molar ratio of (2) is 0.03:0.97 of DMF, 2ME and NMP in a volume ratio of 7:3:0.25, forming a perovskite precursor solution doped with an N-type material at a concentration of 1 mol/ml; then, the N-type perovskite material solution is coated and wet-formed, wherein the coating speed is 15mm/s, the coating injection amount is 170uL, and then the N-type perovskite material layer is formed by annealing at 130 ℃ for 20min, and the thickness is about 150nm.
5) Preparation of the counter electrode (5): and (3) magnetically sputtering a layer of indium-doped tin oxide with a thickness of 300nm on the N-type perovskite absorption layer (4).
Example 4
1) Selecting a stainless steel foil (1) with the thickness of 0.2mm, polishing, respectively adopting deionized water, absolute ethyl alcohol and acetone to carry out ultrasonic cleaning for 30min, and then drying;
2) Preparation of a metal back electrode (2): mo is deposited on the stainless steel foil (1) by magnetron sputtering to be used as a back electrode of the battery, and the deposition thickness is 1000nm;
3)Sb 2 Se 3 preparation of the absorbent layer (3): at a vacuum level of less than 4 x 10 -4 Evaporating a layer of Sb with thickness of 300nm by vacuum evaporation at 350 ℃ under Pa 2 Se 3 A layer. Wherein the evaporation raw materials are Se and Sb 2 Se 3 Powder, se powder with evaporation rate of 0.1 angstrom/second, sb 2 Se 3 The evaporation rate of the powder was 1.2 angstrom/sec. A schematic diagram of the evaporation apparatus is shown in fig. 2.
4) Preparation of an N-type perovskite absorption layer (4): preparing N-type perovskite material solution, wherein solute is PbI 2 MAI, FAI, csBr, wherein the molar ratio of MAI, FAI to CsBr is 0.10:0.85:0.05.PbI 2 The molar ratio to (MAI+FAI+CsBr) is 1:1. bi is selected in the present embodiment 3+ As N-type doping material, wherein BiI 3 With PbI 2 The molar ratio of (2) is 0.03:0.97, wherein the solvent is DMF, NMP and 2ME, and the volume ratio of DMF, 2ME and NMP is 8:2:0.25, forming a perovskite precursor solution doped with an N-type material at a concentration of 1.03 mol/ml; then coating the N-type perovskite material solution into a film by a wet method, wherein the coating speed is 13mm/s, the coating injection amount is 170uL, and then annealing at 130 ℃ for 20min to form an N-type perovskite material layer, and the thickness is about 130nm;
5) Preparation of the counter electrode (5): and (3) magnetically sputtering a layer of indium-doped tin oxide with a thickness of 300nm on the N-type perovskite absorption layer (4).
The performance of the PN heterojunction antimony selenide/perovskite solar cell obtained in examples 1 to 4 was examined, and the results are shown in table 1. The detection method is as follows.
I-V efficiency test: the test I-V curves and steady state Jsc were recorded by a solar simulator (7 SS1503A, beijing simulating am1.5g sunlight with an intensity of 100mW/cm2 using digital source table 2400Keithley Instruments Inc). The incident light intensity was calibrated with NREL calibrated silicon solar cells (Newport Stratford Inc 91150V). The scan rate was 50mV/s and the delay time was 0.1s. The reverse scan is from 1.2V to 0.05V, while the forward scan is from 0.05V to 1.2V.
TABLE 1 influence of different N-type doping and solvent ratios on cell performance
Claims (4)
1. The PN heterojunction antimony selenide/perovskite solar cell is characterized by comprising a substrate, a metal back electrode, a P-type antimony selenide layer, an N-type perovskite absorption layer and a conductive electrode which are sequentially arranged;
the thickness of the P-type antimony selenide layer is 50-300 nm;
the thickness of the N-type perovskite absorption layer is 100-200 mm;
the material of the N-type perovskite absorption layer is ABX doped with N-type material 3 The method comprises the steps of carrying out a first treatment on the surface of the Wherein A is one or more of MA, FA, cs and PEA; MA is CH 3 NH 3 The method comprises the steps of carrying out a first treatment on the surface of the FA is NH 2 CHNH 2 The method comprises the steps of carrying out a first treatment on the surface of the PEA is C 8 H 9 NH 3 The method comprises the steps of carrying out a first treatment on the surface of the B is Pb and/or Sn; x is one or more of Cl, br and I; the N-type material comprises Bi 3+ 、Sb 3+ 、Fe 3+ With Al 3+ One or more of the following;
the molar ratio of the N-type material to the B in the N-type perovskite absorption layer is (0.01-0.05): (0.95-0.99).
2. The PN heterojunction antimony selenide/perovskite solar cell of claim 1, wherein the substrate is a flexible metal substrate; the thickness of the substrate is 0.1-0.3 mm.
3. The PN heterojunction antimony selenide/perovskite solar cell of claim 1, wherein the material of the metal back electrode is molybdenum; the thickness of the metal back electrode is 800-1000 mm.
4. A method of making a PN heterojunction antimony selenide/perovskite solar cell as claimed in claim 1, comprising:
s1) depositing a metal back electrode on a substrate to obtain a substrate of a composite metal back electrode;
s2) evaporating a P-type antimony selenide layer on the substrate of the composite metal back electrode to obtain a substrate of the composite P-type antimony selenide layer;
s3) coating the N-type perovskite precursor solution on the surface of the substrate of the composite P-type antimony selenide layer, and annealing to obtain the substrate of the composite N-type perovskite absorption layer;
s4) depositing a conductive electrode on the substrate of the composite N-type perovskite absorption layer to obtain a PN heterojunction antimony selenide/perovskite solar cell;
the evaporation in the step S2) is vacuum evaporation; the vacuum degree of the evaporation is less than 4 multiplied by 10 -4 Pa; the evaporation temperature is 300-600 ℃; the vapor deposition rate is 0.3 to 1.5 angstrom/second; the evaporation raw materials are Se and Sb 2 Se 3 ；
The N-type perovskite precursor solution comprises AX and BX 2 And an N-type doping material; a is one or more of MA, FA, cs and PEA; MA is CH 3 NH 3 The method comprises the steps of carrying out a first treatment on the surface of the FA is NH 2 CHNH 2 The method comprises the steps of carrying out a first treatment on the surface of the PEA is C 8 H 9 NH 3 The method comprises the steps of carrying out a first treatment on the surface of the B is Pb and/or Sn; x is one or more of Cl, br and I; the N-type doping material comprises Bi 3+ 、Sb 3+ 、Fe 3+ With Al 3+ One or more of the following; the annealing temperature is 70-150 ℃; the annealing time is 10-60 min.
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