CN114388557A - Flexible antimony selenide/perovskite laminated solar cell and preparation method thereof - Google Patents

Flexible antimony selenide/perovskite laminated solar cell and preparation method thereof Download PDF

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CN114388557A
CN114388557A CN202111595120.7A CN202111595120A CN114388557A CN 114388557 A CN114388557 A CN 114388557A CN 202111595120 A CN202111595120 A CN 202111595120A CN 114388557 A CN114388557 A CN 114388557A
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layer
substrate
composite
perovskite
solar cell
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李梦洁
赵志国
赵东明
秦校军
丁坤
刘家梁
熊继光
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Huaneng Clean Energy Research Institute
Huaneng Renewables Corp Ltd
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Huaneng Renewables Corp Ltd
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Abstract

The invention provides a flexible antimony selenide/perovskite laminated solar cell, which comprises a substrate, a back electrode, an antimony selenide absorption layer, a buffer layer, a window layer, an intermediate composite layer, a hole transmission layer, a perovskite absorption layer, an electron transmission layer and a conductive electrode which are sequentially arranged; the material of the intermediate composite layer is selected from one or more of molybdenum oxide, indium tin oxide, zinc oxide, aluminum-doped zinc oxide, tin oxide and C60. Compared with the prior art, the light absorbers with different band gaps form the multi-junction solar cell, so that the utilization range of solar spectrum can be widened, the thermal relaxation loss of photon-generated carriers can be reduced, and the photoelectric conversion efficiency of the solar cell is improved.

Description

Flexible antimony selenide/perovskite laminated solar cell and preparation method thereof
Technical Field
The invention belongs to the technical field of solar cells, and particularly relates to a flexible antimony selenide/perovskite laminated solar cell and a preparation method thereof.
Background
Solar cells are receiving attention because they convert solar energy into electric energy through photoelectric conversion and are used directly by people. Solar cells can be classified into three types according to their development and the light absorbing layer materials used. The first type is a silicon-based solar cell, which comprises a monocrystalline silicon, a polycrystalline silicon solar cell, an amorphous silicon thin-film solar cell and a silicon laminated solar cell; the second type is a compound solar cell, including solar cells of Copper Indium Gallium Selenide (CIGS), cadmium telluride (CdTe), gallium arsenide (GaAs), perovskite, and the like; the third type is a novel solar cell including a dye-sensitized solar cell, an organic solar cell, a quantum dot solar cell, and the like.
Among them, perovskite solar cells (perovskite solar cells) are solar cells using perovskite organic metal halide semiconductors as light absorbing materials, and belong to the third generation solar cells, which are also called new concept solar cells.
Since 2009 perovskite solar cells have attracted much attention due to simple preparation methods, low production cost and excellent photoelectric properties, the perovskite solar cells rapidly increase the photoelectric conversion efficiency from 3.8% to 25.5%, which becomes the most rapidly developing photovoltaic technology and is a new photovoltaic technology that is attracting attention all over the world.
However, the existing single-junction perovskite material has a narrow light absorption range and can only absorb photons within a specific range, so that the single-junction perovskite material has a Shockley-Queisser efficiency limit, and further improvement of the photoelectric conversion efficiency of the single-junction perovskite material is limited.
Disclosure of Invention
In view of the above, the technical problem to be solved by the present invention is to provide a flexible antimony selenide/perovskite tandem solar cell with higher photoelectric conversion efficiency and a preparation method thereof.
The invention provides a flexible antimony selenide/perovskite laminated solar cell, which comprises a substrate, a back electrode, an antimony selenide absorption layer, a buffer layer, a window layer, an intermediate composite layer, a hole transmission layer, a perovskite absorption layer, an electron transmission layer and a conductive electrode which are sequentially arranged;
the substrate is a flexible substrate;
the material of the intermediate composite layer is selected from one or more of molybdenum oxide, indium tin oxide, zinc oxide, aluminum-doped zinc oxide, tin oxide and C60.
Preferably, the thickness of the antimony selenide absorption layer is 100-300 nm.
Preferably, the thickness of the buffer layer is 10-60 nm; the buffer layer is made of one or more materials selected from cadmium sulfide, zinc sulfide and indium sulfide.
Preferably, the thickness of the window layer is 80-1000 nm; the material of the window layer is selected from zinc oxide and/or aluminum-doped zinc oxide.
Preferably, the thickness of the intermediate composite layer is 10-120 nm.
Preferably, the thickness of the hole transport layer is 10-200 nm; the material of the hole transport layer is selected from PTAA, spiro-oMeTAD, PEDOT PSS, nickel oxide or CuSCN.
Preferably, the thickness of the perovskite absorption layer is 100-350 nm; the perovskite absorption layer is made of ABX3(ii) a Wherein A is one or more of MA, FA and PEA; MA is CH3NH3(ii) a FA is NH2CHNH2(ii) a PEA is C8H9NH3(ii) a B is Pb and/or Sn; x is one or more of Cl, Br and I.
Preferably, the thickness of the electron transmission layer is 10-100 nm; the material of the electron transport layer is selected from one or more of tin oxide, C60, titanium oxide, PCBM, zinc oxide and cadmium sulfide.
The invention also provides a preparation method of the flexible antimony selenide/perovskite laminated solar cell, which comprises the following steps:
s1) depositing a back electrode on the substrate to obtain a substrate of a composite back electrode;
s2) evaporating an antimony selenide absorption layer on the substrate of the composite back electrode to obtain the substrate of the composite antimony selenide absorption layer;
s3) depositing a buffer layer on the substrate of the composite antimony selenide absorption layer to obtain the substrate of the composite buffer layer;
s4) depositing a window layer on the substrate of the composite buffer layer to obtain the substrate of the composite window layer;
s5) depositing an intermediate composite layer on the substrate of the composite window layer to obtain a substrate of a composite intermediate composite layer;
s6) preparing a hole transport layer on the substrate of the composite intermediate composite layer to obtain a substrate of the composite hole transport layer;
s7) preparing a perovskite absorption layer on the substrate of the composite hole transport layer to obtain the substrate of the composite perovskite absorption layer;
s8) evaporating an electron transport layer on the substrate of the composite perovskite absorption layer to obtain the substrate of the composite electron transport layer;
s9) depositing a conductive electrode on the substrate of the composite electron transport layer to obtain the flexible antimony selenide/perovskite laminated solar cell.
The invention provides a flexible antimony selenide/perovskite laminated solar cell, which comprises a substrate, a back electrode, an antimony selenide absorption layer, a buffer layer, a window layer, an intermediate composite layer, a hole transmission layer, a perovskite absorption layer, an electron transmission layer and a conductive electrode, wherein the substrate, the back electrode, the antimony selenide absorption layer, the buffer layer, the window layer, the intermediate composite layer, the hole transmission layer, the perovskite absorption layer, the electron transmission layer and the conductive electrode are sequentially arranged; the material of the intermediate composite layer is selected from one or more of molybdenum oxide, indium tin oxide, zinc oxide, aluminum-doped zinc oxide, tin oxide and C60. Compared with the prior art, the light absorbers with different band gaps form the multi-junction solar cell, so that the utilization range of solar spectrum can be widened, the thermal relaxation loss of photon-generated carriers can be reduced, and the photoelectric conversion efficiency of the solar cell is improved.
Experiments show that the flexible antimony selenide/perovskite laminated solar cell prepared by the invention widens the spectral absorption range of the perovskite cell, and the absorption range is widened from 350-750 nm to 350-1050 nm; the photoelectric conversion efficiency is improved, and is improved from 16% to 18.5%.
Drawings
Fig. 1 is a schematic structural diagram of a flexible antimony selenide/perovskite tandem solar cell provided by the present invention;
fig. 2 is an EQE spectrum of a flexible antimony selenide/perovskite tandem solar cell prepared in sample 3 of example 4 of the present invention.
Detailed Description
The technical solutions in the embodiments of the present invention will be clearly and completely described below with reference to the embodiments of the present invention, and it is obvious that the described embodiments are only a part of the embodiments of the present invention, and not all of the embodiments. All other embodiments, which can be derived by a person skilled in the art from the embodiments given herein without making any creative effort, shall fall within the protection scope of the present invention.
The invention provides a flexible antimony selenide/perovskite laminated solar cell, which comprises a substrate, a back electrode, an antimony selenide absorption layer, a buffer layer, a window layer, an intermediate composite layer, a hole transmission layer, a perovskite absorption layer, an electron transmission layer and a conductive electrode which are sequentially arranged; the substrate is a flexible substrate; the material of the intermediate composite layer is selected from one or more of molybdenum oxide, indium tin oxide, zinc oxide, aluminum-doped zinc oxide, tin oxide and C60.
Referring to fig. 1, fig. 1 is a schematic structural diagram of a flexible antimony selenide/perovskite tandem solar cell provided by the present invention; wherein 1 is the substrate, 2 is the back electrode, 3 is the antimony selenide absorbed layer, 4 is the buffer layer, 5 is the window layer, 6 is middle composite bed, 7 is the hole transport layer, 8 is the perovskite absorbed layer, 9 is the electron transport layer, 10 is the conductive electrode.
Wherein, the substrate is a flexible substrate well known to those skilled in the art, and is not particularly limited, and in the present invention, a metal foil is preferred, and a stainless steel foil is more preferred; the thickness of the substrate is preferably 0.1-0.3 mm.
A back electrode is arranged on the substrate; the back electrode is a back electrode known to the skilled person, and is not particularly limited, and in the present invention, molybdenum is preferred; the thickness of the back electrode is preferably 600-1000 nm; in the embodiment provided by the invention, the thickness of the back electrode is specifically 600nm, 700nm, 800nm, 900nm, 910nm, 920nm, 950nm or 1000 nm.
An antimony selenide absorption layer is arranged on the back electrode; the thickness of the antimony selenide absorption layer is preferably 100-300 nm.
A buffer layer is arranged on the antimony selenide absorption layer; the buffer layer is preferably made of one or more of cadmium sulfide, zinc sulfide and indium sulfide; the thickness of the buffer layer is preferably 10-60 nm, more preferably 20-50 nm, and further preferably 20-40 nm; in the embodiments provided by the present invention, the thickness of the buffer layer is specifically 40nm, 25nm, 23nm, 35nm, 37nm, or 20 nm.
A window layer is arranged on the buffer layer; the material of the window layer is preferably zinc oxide and/or aluminum-doped zinc oxide; the thickness of the window layer is preferably 80-1000 nm, more preferably 100-1000 nm, further preferably 200-800 nm, and most preferably 400-600 nm; in the present invention, the window layer preferably comprises a zinc oxide layer and an aluminum-doped zinc oxide layer; the thickness of the zinc oxide layer is preferably 50-200 nm, and more preferably 100-150 nm; the thickness of the aluminum-doped zinc oxide layer is preferably 100-800 nm, more preferably 200-600 nm, still more preferably 400-600 nm, and most preferably 500 nm.
An intermediate composite layer is arranged on the window layer; the material of the intermediate composite layer is preferably one or more of molybdenum oxide, indium tin oxide, zinc oxide, aluminum-doped zinc oxide, tin oxide and C60; the thickness of the intermediate composite layer is preferably 10-120 nm, more preferably 20-100 nm, still more preferably 20-80 nm, and most preferably 30-50 nm.
A hole transport layer is arranged on the intermediate composite layer; the material of the hole transport layer is preferably PTAA, spiro-oMeTAD, PEDOT PSS, nickel oxide or CuSCN; the thickness of the hole transport layer is preferably 10-200 nm, more preferably 15-150 nm, still more preferably 15-100 nm, still more preferably 15-80 nm, and most preferably 15-40 nm; in the embodiments provided herein, the thickness of the hole transport layer is specifically 10nm, 15nm, 25nm, 30nm, 28nm, 18nm, or 40 nm.
A perovskite absorption layer is arranged on the hole transport layer; the material of the perovskite absorption layer is preferably ABX3(ii) a Wherein A is one or more of MA, FA and PEA, and more preferably MA, FA and PEA; the preferable molar ratio of MA, FA and PEA is (0.5-1.5): (0.5-1.5): (0.5 to 1.5), more preferably (0.8 to 1.2): (0.8-1.2): (0.8 to 1.2), and more preferably 1:1: 1; MA is CH3NH3(ii) a FA is NH2CHNH2(ii) a PEA is C8H9NH3(ii) a B is Pb and/or Sn; x is one or more of Cl, Br and I, and Br and I are more preferable; the molar ratio of Br to I is preferably 1: (4-10); the thickness of the perovskite absorption layer is preferably 100-350 nm, more preferably 100-250 nm, and most preferably 150-250 nm; in embodiments provided herein, the thickness of the perovskite absorption layer is specifically 150nm, 200nm, or 250 nm.
An electron transport layer is arranged on the perovskite absorption layer; the material of the electron transport layer is preferably one or more of tin oxide, C60, titanium oxide, PCBM, zinc oxide and cadmium sulfide; the thickness of the electron transport layer is preferably 10-100 nm, more preferably 30-100nm, still more preferably 50-100 nm, and most preferably 80-100 nm.
A conductive electrode is arranged on the electron transmission layer; the conductive electrode is preferably one or more of indium tin oxide, zinc oxide and aluminum-doped zinc oxide; the thickness of the conductive electrode is preferably 100-1000 nm, more preferably 200-800 nm, still more preferably 400-600 nm, and most preferably 500 nm.
The light absorbers with different band gaps form the multi-junction solar cell, so that the utilization range of solar spectrum can be widened, the thermal relaxation loss of photon-generated carriers can be reduced, and the photoelectric conversion efficiency of the solar cell is improved.
The invention also provides a preparation method of the flexible antimony selenide/perovskite laminated solar cell, which comprises the following steps: s1) depositing a back electrode on the substrate to obtain a substrate of a composite back electrode; s2) evaporating an antimony selenide absorption layer on the substrate of the composite back electrode to obtain the substrate of the composite antimony selenide absorption layer; s3) depositing a buffer layer on the substrate of the composite antimony selenide absorption layer to obtain the substrate of the composite buffer layer; s4) depositing a window layer on the substrate of the composite buffer layer to obtain the substrate of the composite window layer; s5) depositing an intermediate composite layer on the substrate of the composite window layer to obtain a substrate of a composite intermediate composite layer; s6) preparing a hole transport layer on the substrate of the composite intermediate composite layer to obtain a substrate of the composite hole transport layer; s7) preparing a perovskite absorption layer on the substrate of the composite hole transport layer to obtain the substrate of the composite perovskite absorption layer; s8) evaporating an electron transport layer on the substrate of the composite perovskite absorption layer to obtain the substrate of the composite electron transport layer; s9) depositing a conductive electrode on the substrate of the composite electron transport layer to obtain the flexible antimony selenide/perovskite laminated solar cell.
Wherein, the sources of all raw materials are not specially limited and can be sold in the market; the substrate, the back electrode, the antimony selenide absorption layer, the buffer layer, the window layer, the intermediate composite layer, the hole transport layer, the perovskite absorption layer, the electron transport layer and the conductive electrode are the same as above, and are not described again.
In the present invention, it is preferable that the substrate is pretreated first; because the substrate is preferably a metal foil, the pretreatment preferably comprises grinding and polishing, and then ultrasonic cleaning and drying are sequentially carried out by using deionized water, absolute ethyl alcohol and acetone.
Depositing a back electrode on the pretreated substrate to obtain a substrate of a composite back electrode; the method for depositing the 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; the parameters during magnetron sputtering are preferably as follows: sputtering power120W, sputtering pressure of 0.4-1.2 Pa, sputtering time of 15-30 min, equipment vacuum degree of 2.0 multiplied by 10-4Pa, the target base distance is 50mm, the substrate temperature is 50-250 ℃, and the Ar flow is 20-80 sccm.
Evaporating an antimony selenide absorption layer on the substrate of the composite back electrode to obtain the substrate of the composite antimony selenide absorption layer; the method of evaporation is preferably a method well known to those skilled in the art, and is not particularly limited, and vacuum evaporation is preferred in the present invention; the vapor deposition is preferably performed in a vacuum degree of less than 1X 10-4Under the conditions of (a); the evaporation temperature is preferably 300-600 ℃, more preferably 400-600 ℃, and further preferably 500 ℃; the evaporation rate during evaporation is preferably 0.5 to 1 angstrom per second, more preferably 0.6 to 0.9 angstrom per second, and still more preferably 0.7 to 0.8 angstrom per second.
Depositing a buffer layer on the composite antimony selenide absorption layer to obtain a substrate of the composite buffer layer; the buffer layer may be deposited by a method known to those skilled in the art, and is not particularly limited, and chemical bath deposition is preferred in the present invention. The solution used in the chemical bath deposition comprises metal salt, thiourea and a complexing agent; the metal salt is preferably a cadmium salt, a zinc salt or an indium salt; the complexing agent is preferably ammonia water; the ratio of the volume of the ammonia water to the volume of the water in the solution is preferably 1: (100-200); the concentration of the metal salt in the solution is preferably 0.2-0.7 mol/L; the temperature of the chemical bath deposition is preferably 55-90 ℃; the time of the chemical bath deposition is preferably 350 to 500 s.
Depositing a window layer on the substrate of the composite buffer layer to obtain a substrate of the composite window layer; the method for depositing the window layer is known to those skilled in the art, and is not particularly limited, and magnetron sputtering is preferred in the present invention.
Depositing an intermediate composite layer on the substrate of the composite window layer to obtain a substrate of the composite intermediate composite layer; the method for depositing the intermediate composite layer is vacuum evaporation, and the intermediate composite layer can be obtained by directly utilizing corresponding commercially available materials through vacuum evaporation without special limitation.
Compounding a hole transport layer on the substrate of the composite intermediate composite layer to obtain a substrate of the composite hole transport layer; the method for recombining the hole transport layer is a method well known to those skilled in the art, and is not particularly limited, and when the hole transport layer is organic, it is preferably prepared by knife coating; when the material of the hole transport layer is nickel oxide, a spray pyrolysis method is preferably adopted, namely a nickel salt solution is sprayed on the intermediate composite layer and sintered to obtain the substrate of the composite hole transport layer; the nickel salt is preferably nickel nitrate; the concentration of the nickel salt solution is preferably 0.05-0.3 mol/L, more preferably 0.1-0.3 mol/L, still more preferably 0.2-0.3 mol/L, and most preferably 0.25 mol/L; the sintering temperature is preferably 300-450 ℃, and more preferably 350-400 ℃; the sintering time is preferably 20-60 min, and more preferably 30-40 min.
Preparing a perovskite absorption layer on the substrate of the composite hole transport layer to obtain the substrate of the composite perovskite absorption layer; in the present invention, the perovskite absorption layer is preferably prepared according to the following steps: when A is MA and/or PEA, AX and BX are firstly2After mixing in an organic solvent, spraying the mixture to the surface of the hole transport layer, and annealing to obtain a perovskite absorption layer; when A also comprises FA, performing evaporation deposition of FAX on the surface of the sprayed layer after spraying, and performing annealing treatment to obtain a perovskite absorption layer; the temperature of the annealing treatment is preferably 100-150 ℃; the time of the annealing treatment is preferably 10-60 min; the temperature of the evaporation deposition is preferably 70-90 ℃, and more preferably 80 ℃; the evaporation deposition rate is preferably 0.1-0.5 angstrom per second.
Evaporating an electron transmission layer on the substrate of the composite perovskite absorption layer to obtain the substrate of the composite electron transmission layer; the method for evaporating the electron transport layer is not particularly limited, and is preferably vacuum evaporation.
Depositing a conductive electrode on the substrate of the composite electron transmission layer to obtain a flexible antimony selenide/perovskite laminated solar cell; the method for depositing the conductive electrode is not particularly limited as long as it is a method known to those skilled in the art, and vacuum evaporation or magnetron sputtering is preferable in the present invention.
To further illustrate the present invention, the following describes a flexible antimony selenide/perovskite tandem solar cell and a method for manufacturing the same in detail with reference to the examples.
The reagents used in the following examples are all commercially available.
Example 1
1) Selecting a stainless steel foil (1) with the thickness of 0.3mm, grinding and polishing, then respectively adopting deionized water, absolute ethyl alcohol and acetone to carry out ultrasonic cleaning for 30min, and then N2Drying;
2) preparation of the metal back electrode (2): mo is deposited on the stainless steel foil (1) as Sb by adopting magnetron sputtering2Se3The parameters of the back electrode of the battery are as follows: the sputtering power is 120W, the sputtering pressure is 0.4-1.2 Pa, the sputtering time is 15-30 min, and the equipment vacuum degree is 2.0 multiplied by 10-4Pa, the target base distance is 50mm, the substrate temperature is 50-250 ℃, the Ar flow is 20-80 sccm, and the thickness of the prepared back electrode is 600-1000 nm (see table 1 specifically);
3)Sb2Se3preparation of the absorbing layer (3): under vacuum degree less than 1 x 10-4Evaporating a layer of Sb with the thickness of 300nm at the evaporation rate of 0.8 angstrom per second under Pa at 500 ℃ by adopting a vacuum evaporation method2Se3Layer(s)
4) Preparation of the buffer layer (4): by chemical bath on Sb2Se3A CdS buffer layer with the thickness of 25nm is deposited on the absorption layer (3); the parameters are as follows: wherein solutes in the precursor solution deposited by the CdS chemical bath are as follows: cadmium salt (3 CdSO)4·8H2O), thiourea (SC (NH)2)2) Complexing agent ammonia (NH)3·H2O). The solvent is deionized water. Dissolving cadmium salt and thiourea in a mixed solution of ammonia water and deionized water in a volume ratio of 1:150 according to a molar ratio of 1:2, wherein the mass ratio concentration of the ammonia water is 35% w/w; the concentration of cadmium salt in the mixed solution is 0.2 mol/L. The deposition temperature is 90 ℃, and the reaction time is 375 s;
5) preparation of the window layer (5): depositing a 100nm intrinsic zinc oxide layer on the CdS buffer layer (4) by magnetron sputtering, and then sputtering and depositing a 500nm aluminum-doped zinc oxide layer;
6) preparation of the intermediate composite layer (6): preparing a layer of 30nm SnO on the window layer (5) by atomic force deposition2；
7) Preparation of hole transport layer (7): adopting a spray pyrolysis process to mix 0.25mol.L-1NiNO of3Spraying the precursor solution on the intermediate composite layer (6), and sintering at 350 ℃ for 30min to obtain a NiOx hole transport layer with the thickness of 15 nm;
8) preparation of perovskite phase absorption layer (8): firstly, methyl amine bromide (MABr) and lead bromide (PbBr)2) And lead iodide (PbI)2) Dissolving in N-N Dimethylformamide (DMF) solvent at a molar ratio of 1:1:4, spraying onto the NiOx hole transport layer (7) to a thickness of 150nm, and evaporating 1M dimethyl ether iodide (FAI) at 80 deg.C at an evaporation rate of 0.1 Angstrom per second (depositing onto the hole transport layer with MABr, PbBr2、PbI2Reacting to generate perovskite, and annealing at 150 ℃ for 10min to form a perovskite phase absorption layer with the thickness of 200 nm;
9) preparation of the electron transport layer (9): evaporating and plating a layer of 80nm C60 on the perovskite phase absorption layer (8) by adopting a vacuum evaporation method to obtain an electron transmission layer;
10) preparation of the counter electrode (10): and carrying out magnetron sputtering on a layer of indium-doped tin oxide with the thickness of 500nm on the electron transmission layer (9).
The solar cell obtained in example 1 was tested for conversion efficiency and the results are shown in table 1.
TABLE 1 Effect of different Metal Back electrodes on solar cell Performance
Figure BDA0003430289300000091
Example 2
1) Selecting a stainless steel foil (1) with the thickness of 0.3mm, grinding and polishing, then respectively adopting deionized water, absolute ethyl alcohol and acetone to carry out ultrasonic cleaning for 30min, and then N2Drying;
2) preparation of the metal back electrode (2): mo is deposited on the stainless steel foil (1) as Sb by adopting magnetron sputtering2Se3The parameters of the back electrode of the battery are as follows: sputtering power of 120W, sputtering pressure of 1Pa, sputtering time of 15min, equipment vacuum degree of 2.0 × 10- 4Pa, the target base distance is 50mm, the substrate temperature is 150 ℃, the Ar flow is 40sccm, and the thickness of the prepared back electrode is 910 nm;
3)Sb2Se3preparation of the absorbing layer (3): under vacuum degree less than 1 x 10-4Evaporating a layer of Sb with the thickness of 300nm at the evaporation rate of 0.8 angstrom per second under Pa at 500 ℃ by adopting a vacuum evaporation method2Se3And (3) a layer.
4) Preparation of the buffer layer (4): by chemical bath on Sb2Se3A CdS buffer layer with the thickness of 25nm is deposited on the absorption layer (3), and the parameters are as follows: wherein solutes in the precursor solution deposited by the CdS chemical bath are as follows: cadmium salt (3 CdSO)4·8H2O), thiourea (SC (NH)2)2) Complexing agent ammonia (NH)3·H2O). The solvent is deionized water. Dissolving cadmium salt and thiourea in a mixed solution of ammonia water and deionized water in a volume ratio of 1: 100-200 according to a molar ratio of 1:2, wherein the mass ratio concentration of the ammonia water is 35% w/w. The deposition temperature is 55-90 ℃, and the reaction time is 350-500 s;
5) preparation of the window layer (5): depositing a 100nm intrinsic zinc oxide layer on the CdS buffer layer (4) by magnetron sputtering, and then sputtering and depositing a 500nm aluminum-doped zinc oxide layer;
6) preparation of the intermediate composite layer (6): preparing a layer of 30nm SnO on the window layer (5) by atomic force deposition2；
7) Preparation of hole transport layer (7): adopting a spray pyrolysis process to mix 0.25 mol.L-1NiNO of3Spraying the precursor solution on the intermediate composite layer (6), and sintering at 350 ℃ for 30min to obtain a NiOx hole transport layer with the thickness of 15 nm;
8) preparation of perovskite phase absorption layer (8): firstly, methyl amine bromide (MABr) and lead bromide (PbBr)2) And lead iodide (PbI)2) Dissolving in N-N Dimethylformamide (DMF) solvent at a molar ratio of 1:1:4, spraying onto NiOx hole transport layer (7) to a thickness of 200nm, and adding 1M methyl ether iodine (DMF)FAI) at 80 deg.C, by evaporation rate of 0.1 angstroms per second (depositing it onto the hole transport layer with MABr, PbBr2、PbI2Reacting to generate perovskite, and annealing at 150 ℃ for 10min to form a perovskite phase absorption layer with the thickness of 200 nm;
9) preparation of the electron transport layer (9): evaporating and plating a layer of 80nm C60 on the perovskite phase absorption layer (8) by adopting a vacuum evaporation method to obtain an electron transmission layer;
10) preparation of the counter electrode (10): and carrying out magnetron sputtering on the electron transmission layer (9) to form a layer of indium-doped tin oxide or aluminum-doped zinc oxide with the thickness of 500 nm.
TABLE 2 influence of different CdS Process parameters on solar cell Performance
Figure BDA0003430289300000101
Example 3
1) Selecting a stainless steel foil (1) with the thickness of 0.1mm, grinding and polishing, then respectively adopting deionized water, absolute ethyl alcohol and acetone to carry out ultrasonic cleaning for 30min, and then N2Drying;
2) preparation of the metal back electrode (2): mo is deposited on the stainless steel foil (1) as Sb by adopting magnetron sputtering2Se3The parameters of the back electrode of the battery are as follows: sputtering power of 120W, sputtering pressure of 1Pa, sputtering time of 15min, equipment vacuum degree of 2.0 × 10- 4Pa, the target base distance is 50mm, the substrate temperature is 150 ℃, the Ar flow is 40sccm, and the thickness of the prepared back electrode is 910 nm;
3)Sb2Se3preparation of the absorbing layer (3): under vacuum degree less than 1 x 10-4Evaporating a layer of Sb with the thickness of 300nm at the evaporation rate of 0.8 angstrom per second under Pa at 500 ℃ by adopting a vacuum evaporation method2Se3And (3) a layer.
4) Preparation of the buffer layer (4): by chemical bath on Sb2Se3And a 35nm CdS buffer layer is deposited on the absorption layer (3), wherein the mass ratio concentration of ammonia water is 35% w/w. The deposition temperature is 70 ℃, and the reaction time is 420 s;
5) preparation of the window layer (5): depositing a 100nm intrinsic zinc oxide layer on the CdS buffer layer (4) by magnetron sputtering, and then sputtering and depositing a 500nm aluminum-doped zinc oxide layer;
6) preparation of the intermediate composite layer (6): preparing a layer of 30nm SnO on the window layer (5) by atomic force deposition2；
7) Preparation of hole transport layer (7): adopting a spray pyrolysis process to mix 0.05-0.3 molar concentration of NiNO3Spraying the precursor solution for 10-35 circles, and sintering at 350-500 ℃ for 30min to obtain NiO with the thickness of 10-40 nmxA hole transport layer;
8) preparation of perovskite phase absorption layer (8): firstly, methyl amine bromide (MABr) and lead bromide (PbBr)2) And lead iodide (PbI)2) Dissolving in N-N Dimethylformamide (DMF) solvent at a molar ratio of 1:1:4, spraying onto the NiOx hole transport layer (7) to a thickness of 200nm, and evaporating 1M dimethyl ether iodide (FAI) at 80 deg.C at an evaporation rate of 0.1 Angstrom per second (depositing onto the hole transport layer with MABr, PbBr2、PbI2Reacting to generate perovskite, and annealing at 150 ℃ for 10min to form a perovskite phase absorption layer with the thickness of 200 nm;
9) preparation of the electron transport layer (9): evaporating a layer of C60 with the thickness of 30-100nm on the perovskite phase absorption layer (8) by adopting a vacuum evaporation method to obtain an electron transmission layer;
10) preparation of the counter electrode (10): and carrying out magnetron sputtering on the electron transmission layer (9) to form a layer of indium-doped tin oxide or aluminum-doped zinc oxide with the thickness of 500 nm.
TABLE 3 Effect of different hole transport layers on solar cell Performance
Figure BDA0003430289300000121
Example 4
1) Selecting a stainless steel foil (1) with the thickness of 0.1mm, grinding and polishing, then respectively adopting deionized water, absolute ethyl alcohol and acetone to carry out ultrasonic cleaning for 30min, and then N2Drying;
2) preparation of the metal back electrode (2): mo is deposited on the stainless steel foil (1) as Sb by adopting magnetron sputtering2Se3The parameters of the back electrode of the battery are as follows: sputtering power of 120W, sputtering pressure of 1Pa, sputtering time of 15min, equipment vacuum degree of 2.0 × 10- 4Pa, the target base distance is 50mm, the substrate temperature is 150 ℃, the Ar flow is 40sccm, and the thickness of the prepared back electrode is 910 nm;
3)Sb2Se3preparation of the absorbing layer (3): under vacuum degree less than 1 x 10-4Evaporating a layer of Sb with the thickness of 300nm at the evaporation rate of 0.8 angstrom per second under Pa at 500 ℃ by adopting a vacuum evaporation method2Se3And (3) a layer.
4) Preparation of the buffer layer (4): by chemical bath on Sb2Se3And a 35nm CdS buffer layer is deposited on the absorption layer (3), wherein the mass ratio concentration of ammonia water is 35% w/w. The deposition temperature is 70 ℃, and the reaction time is 420 s;
5) preparation of the window layer (5): depositing a 100nm intrinsic zinc oxide layer on the CdS buffer layer (4) by magnetron sputtering, and then sputtering and depositing a 500nm aluminum-doped zinc oxide layer;
6) preparation of the intermediate composite layer (6): preparing a layer of 30nm SnO on the window layer (5) by atomic force deposition2；
7) Preparation of hole transport layer (7): adopting spray pyrolysis process to add NiNO with 0.3 molar concentration3Spraying the precursor solution for 24 circles, and sintering at 350 ℃ for 30min to obtain a NiOx hole transport layer with the thickness of 30 nm;
8) preparation of perovskite phase absorption layer (8): firstly, methyl amine bromide (MABr) and lead bromide (PbBr)2) And lead iodide (PbI)2) Dissolving the NiO-containing composite material into N-N Dimethylformamide (DMF) solvent according to the ratio of 1:1:4, spraying the NiO-containing composite material onto a NiO hole transport layer (7), and depositing 1M methyl ether iodine (FAI) onto the hole transport layer together with MABr and PbBr by evaporation at the temperature of 100-250 DEG C2、PbI2Reacting to generate perovskite, heating at 100 ℃ for 10-60 min to obtain an organic-inorganic hybrid perovskite phase absorption layer with the thickness of 100-250 nm;
9) preparation of the electron transport layer (9): evaporating and plating a layer of 80nm C60 on the perovskite phase absorption layer (8) by adopting a vacuum evaporation method to obtain an electron transmission layer;
10) preparation of the counter electrode (10): and carrying out magnetron sputtering on the electron transmission layer (9) to form a layer of indium-doped tin oxide or aluminum-doped zinc oxide with the thickness of 500 nm.
TABLE 4 influence of different perovskite phase light-absorbing layer preparation processes on solar cell performance
Figure BDA0003430289300000131
The I-V efficiency test of the batteries prepared in examples 1-4 was carried out as follows: the I-V curves and steady-state Jsc were tested by passing sunlight through a solar simulator (7SS1503A, Beijing simulating AM1.5G sunlight with a light intensity of 100mW/cm2Data was recorded using a digital source table 2400 keithley instruments Inc); calibrating the incident light intensity with NREL calibrated silicon solar cell (Newport Stratford Inc 91150V) F; the scanning speed is 50mV/s, and the delay time is 0.1 s; the reverse scan is from 1.2V to 0.05V, and the forward scan is from 0.05V to 1.2V.
The external quantum efficiency of the solar energy prepared by sample 3 in example 4 was examined to obtain its EQE spectrum, as shown in fig. 2.

Claims (9)

1. A flexible antimony selenide/perovskite laminated solar cell is characterized by comprising a substrate, a back electrode, an antimony selenide absorption layer, a buffer layer, a window layer, an intermediate composite layer, a hole transmission layer, a perovskite absorption layer, an electron transmission layer and a conductive electrode which are sequentially arranged;
the substrate is a flexible substrate;
the material of the intermediate composite layer is selected from one or more of molybdenum oxide, indium tin oxide, zinc oxide, aluminum-doped zinc oxide, tin oxide and C60.
2. The flexible antimony selenide/perovskite tandem solar cell according to claim 1, wherein the thickness of the antimony selenide absorbing layer is 100-300 nm.
3. The flexible antimony selenide/perovskite tandem solar cell according to claim 1, wherein the buffer layer has a thickness of 10-60 nm; the buffer layer is made of one or more materials selected from cadmium sulfide, zinc sulfide and indium sulfide.
4. The flexible antimony selenide/perovskite tandem solar cell according to claim 1, wherein the thickness of the window layer is 80-1000 nm; the material of the window layer is selected from zinc oxide and/or aluminum-doped zinc oxide.
5. The flexible antimony selenide/perovskite tandem solar cell according to claim 1, wherein the thickness of the intermediate composite layer is 10-120 nm.
6. The flexible antimony selenide/perovskite tandem solar cell according to claim 1, wherein the thickness of the hole transport layer is 10-200 nm; the material of the hole transport layer is selected from PTAA, spiro-oMeTAD, PEDOT PSS, nickel oxide or CuSCN.
7. The flexible antimony selenide/perovskite tandem solar cell according to claim 1, wherein the thickness of the perovskite absorption layer is 100-350 nm; the perovskite absorption layer is made of ABX3(ii) a Wherein A is one or more of MA, FA and PEA; MA is CH3NH3(ii) a FA is NH2CHNH2(ii) a PEA is C8H9NH3(ii) a B is Pb and/or Sn; x is one or more of Cl, Br and I.
8. The flexible antimony selenide/perovskite tandem solar cell according to claim 1, wherein the thickness of the electron transport layer is 10-100 nm; the material of the electron transport layer is selected from one or more of tin oxide, C60, titanium oxide, PCBM, zinc oxide and cadmium sulfide.
9. A method of fabricating a flexible antimony selenide/perovskite tandem solar cell according to claim 1, comprising:
s1) depositing a back electrode on the substrate to obtain a substrate of a composite back electrode;
s2) evaporating an antimony selenide absorption layer on the substrate of the composite back electrode to obtain the substrate of the composite antimony selenide absorption layer;
s3) depositing a buffer layer on the substrate of the composite antimony selenide absorption layer to obtain the substrate of the composite buffer layer;
s4) depositing a window layer on the substrate of the composite buffer layer to obtain the substrate of the composite window layer;
s5) depositing an intermediate composite layer on the substrate of the composite window layer to obtain a substrate of a composite intermediate composite layer;
s6) preparing a hole transport layer on the substrate of the composite intermediate composite layer to obtain a substrate of the composite hole transport layer;
s7) preparing a perovskite absorption layer on the substrate of the composite hole transport layer to obtain the substrate of the composite perovskite absorption layer;
s8) evaporating an electron transport layer on the substrate of the composite perovskite absorption layer to obtain the substrate of the composite electron transport layer;
s9) depositing a conductive electrode on the substrate of the composite electron transport layer to obtain the flexible antimony selenide/perovskite laminated solar cell.
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