Modified intermediate layer of perovskite laminated cell, preparation method of modified intermediate layer and perovskite laminated cell

Abstract

The invention provides a modified intermediate layer of a perovskite laminated cell, a preparation method of the modified intermediate layer and the perovskite laminated cell, and belongs to the field of solar cells. The modified middle layer is a composite layer doped with a down-conversion material, and the composite layer is located between the top cell and the bottom cell; or, the modified intermediate layer is a first charge transport layer doped with a down-conversion material, and the first charge transport layer is located between the tunnel junction layer and the perovskite light absorption layer. By introducing the down-conversion material into the intermediate layer of the perovskite laminated cell, part of high-energy photons can be converted into a plurality of low-energy photons, so that the cell can effectively utilize each wave band in a spectrum, the response range of the cell to the spectrum is widened, the energy band structure of the intermediate layer can be improved, and the photons can be efficiently converted. Therefore, the conversion efficiency of the cell can be improved, the light loss and the heat loss of the cell can be reduced, the stability of the cell is improved, the service life of the cell is prolonged, and the applicability of the cell in practical application is improved.

Description

Technical Field

[0001] This invention belongs to the field of solar cells, specifically relating to a modified intermediate layer of a perovskite tandem solar cell, its preparation method, and the perovskite tandem solar cell. Background Art

[0002] Perovskite tandem solar cells, as a novel and highly efficient solar energy conversion technology, have made significant research progress in the solar energy field in recent years. Although they possess characteristics such as high efficiency, low manufacturing cost, and good stability, they still face some shortcomings and deficiencies. 1) Light loss: In perovskite tandem solar cells, some high-energy photons cannot be effectively utilized due to the limitations of the band structure, resulting in light loss. This limits the photoelectric conversion efficiency of the cell and affects its performance under low light intensity conditions; 2) Heat loss: The absorption of high-energy photons generates additional heat, which may lead to an increase in cell temperature, reduce cell efficiency, and potentially shorten its lifespan; 3) Market maturity: Although perovskite tandem solar cells exhibit good performance in laboratory environments, they still face challenges related to market maturity in practical applications. Issues such as the stability of manufacturing processes, mass production costs, and stability and reliability in large-scale applications still need further resolution; 4) Large-scale manufacturing: The large-scale manufacturing of perovskite tandem solar cells remains a challenge. Large-scale production needs to meet the requirements of high quality, high efficiency, and low cost, while ensuring the stability and consistency of cell performance.

[0003] Therefore, overcoming the current technical challenges of light loss, heat loss, and large-scale manufacturing in perovskite tandem solar cells, and thus effectively improving the light utilization efficiency of the cells, is a key research direction at present. Summary of the Invention

[0004] To address the shortcomings of existing technologies, the present invention aims to provide a modified intermediate layer for perovskite tandem solar cells, its preparation method, and the perovskite tandem solar cell itself. By introducing downconversion materials into the perovskite tandem solar cell, the present invention can convert some high-energy photons into low-energy photons, enabling the cell to utilize various wavelengths in the spectrum more effectively, broadening the cell's spectral response range. Simultaneously, it can improve the band structure of the intermediate layer, ensuring efficient photon conversion. Therefore, the present invention not only increases the light utilization rate and conversion efficiency of the cell but also reduces light and heat losses, improves the cell's stability and lifespan, and increases its applicability in practical applications. Furthermore, the present invention can promote the development and market maturity of solar tandem solar cell technology, enabling larger-scale clean energy generation and utilization.

[0005] To achieve this objective, the present invention adopts the following technical solution:

[0006] In a first aspect, the present invention provides a modified intermediate layer for a perovskite tandem solar cell, wherein the modified intermediate layer is a composite layer doped with a downconversion material, and the composite layer is located between the top cell and the bottom cell.

[0007] Alternatively, the modified intermediate layer may be a first charge transport layer doped with downconversion material, which is located between the tunneling junction layer and the perovskite light-absorbing layer.

[0008] This invention introduces downconversion materials into perovskite tandem solar cells, converting some high-energy photons into low-energy photons. This allows the cells to utilize various wavelengths of the spectrum more effectively, broadening the cell's spectral response range. This reduces light loss and improves photoelectric conversion efficiency, especially under low light intensity conditions. Simultaneously, it reduces the additional heat generated by high-energy photon absorption, lowering the risk of temperature rise and improving the band structure of the intermediate layer, ensuring efficient photon conversion. Therefore, this invention not only increases the cell's light utilization and conversion efficiency but also reduces light and heat loss, improving stability and lifespan, and increasing its applicability in practical applications. Furthermore, this invention can promote the development and market maturity of solar tandem cell technology, enabling larger-scale clean energy generation and utilization.

[0009] This invention solves a series of problems faced by perovskite tandem solar cells, such as light loss, heat loss, spectral spread, and stability, by introducing downconversion materials into the perovskite tandem layer. This improves the light utilization efficiency, stability, and practical application performance of the cells, and promotes the development and market maturity of solar cell technology.

[0010] As a preferred technical solution of the present invention, the emission wavelength of the downconversion material is 400-700nm, for example, it can be 450nm, 550nm or 570nm.

[0011] In this invention, the downconversion material emits light at a wavelength of 400-700 nm. After absorbing a high-energy photon of ultraviolet light, it can emit two or more low-energy photons, thereby reducing the thermal relaxation of the battery and improving the light utilization efficiency.

[0012] Preferably, the doping amount of the downconversion material in the composite layer or the first charge transport layer is independently 0-50%, excluding 0, for example, it can be 5%, 10% / 20%, 30% / 40% or 50%, etc., preferably 0-30%, excluding 0, and more preferably 0-5%, excluding 0.

[0013] In this invention, if the downconversion material is doped too much in the composite layer or the first charge transport layer, the conductivity and light transmittance will be reduced, thereby reducing the device efficiency.

[0014] As a preferred embodiment of the present invention, the composite layer comprises a transparent conductive oxide.

[0015] Preferably, the transparent conductive oxide includes any one of indium tin oxide (ITO), indium zinc oxide (IZO), indium tungsten oxide (IWO), indium titanium oxide (ITIO), fluorine-doped tin oxide (FTO), or aluminum-doped zinc oxide (AZO).

[0016] Preferably, the first charge transport layer includes a hole transport layer.

[0017] Preferably, the hole transport layer comprises a nickel oxide layer.

[0018] As a preferred embodiment of the present invention, the downconversion material includes a first compound doped with rare earth ions, a composite oxide, or a material doped with Bi. 3+ Any one or a combination of at least two of the second compounds.

[0019] It is important to note that selecting a suitable downconversion material is crucial. The material's absorption characteristics must be considered to ensure its ability to effectively convert high-energy photons into low-energy photons, thereby improving the solar cell's light utilization efficiency. Furthermore, the band structure of the downconversion material must match the band structure of the perovskite layer to ensure efficient electron and hole transport and avoid losses caused by band shift. In addition, the photostability and durability of the conversion material should also be considered to prevent degradation or deterioration under long-term illumination, which could affect solar cell performance.

[0020] Preferably, the rare earth ions include Ce. 3+ Pr 3+ Yb 3+ 、Sm 3+ Eu 3+ or Tb 3+ Any one or at least two of them.

[0021] Preferably, the first compound and the second compound independently comprise any one of metal oxides, phosphates, sulfur oxides, fluorides, yttrium aluminum garnet, molybdates, or vanadates.

[0022] Preferably, the metal oxide includes any one of titanium oxide, gadolinium oxide, or tin oxide.

[0023] Preferably, the sulfur oxide includes lanthanum sulfide.

[0024] Preferably, the fluoride comprises sodium yttrium tetrafluoride.

[0025] Preferably, the phosphate comprises yttrium phosphate.

[0026] Preferably, the molybdate includes yttrium molybdate.

[0027] Preferably, the vanadate includes yttrium vanadate.

[0028] Preferably, the composite oxide comprises any one or a combination of at least two of nickel trioxide, copper oxide, antimony trioxide, or tin oxide.

[0029] As a preferred technical solution of the present invention, the thickness of the composite layer doped with the downconversion material is 20-40nm, for example, it can be 20nm, 25nm, 30nm or 35nm, etc.

[0030] Preferably, the thickness of the first charge transport layer doped with the downconversion material is 15-25 nm, for example, it can be 15 nm, 20 nm or 25 nm.

[0031] In a second aspect, the present invention provides a method for preparing a modified intermediate layer of a perovskite tandem solar cell as described in the first aspect, the method comprising the following steps:

[0032] Using the raw materials for preparing the composite layer or the raw materials for preparing the first charge transport layer as the first sputtering target and the subconversion material as the second sputtering target, dual-source magnetron sputtering is performed using the first sputtering target and the second sputtering target to obtain the modified intermediate layer.

[0033] The process provided by this invention is simple and does not require upgrading existing equipment. This process effectively reduces light loss and improves light utilization efficiency, thereby improving battery efficiency, while also reducing heat loss and improving stability.

[0034] As a preferred technical solution of the present invention, a working gas is introduced before performing the dual-source magnetron sputtering.

[0035] Preferably, the working gas includes an inert gas and oxygen, and the volume ratio of the inert gas to oxygen is 10:(0.8-1.5), for example, it can be 10:0.8, 10:1, 10:1.3 or 10:1.5, etc.

[0036] Preferably, the inert gas includes argon.

[0037] Preferably, during the dual-source magnetron sputtering process, the pressure inside the sputtering chamber is 0.3-0.8 Pa, for example, it can be 0.3 Pa, 0.4 Pa, 0.5 Pa, 0.6 Pa, 0.7 Pa or 0.8 Pa.

[0038] Preferably, the sputtering time of the dual-source magnetron sputtering is 5-60 min, for example, it can be 5 min, 10 min, 20 min, 30 min, 40 min, 50 min or 60 min.

[0039] As a preferred technical solution of the present invention, the sputtering power of the first sputtering target is 170-250W, for example, it can be 170W, 190W, 200W, 210W or 230W.

[0040] Preferably, the sputtering power of the second sputtering target is 5-15W, for example, it can be 5W, 8W, 10W, 13W or 15W.

[0041] Preferably, the deposition rate ratio of the first sputtering target to the second sputtering target is (0.15-0.25):(0.004-0.0125), wherein the selection range of the first sputtering target "0.15-0.25" can be, for example, 0.15, 0.2, 0.2375 or 0.25, etc., and the selection range of the first sputtering target "0.004-0.0125" can be, for example, 0.004, 0.008, 0.01 or 0.0125, etc.

[0042] In this invention, if the deposition rate ratio between the first sputtering target and the second sputtering target is too large, that is, if the deposition rate of the second sputtering target is too small, the doping amount will be too low and the downconversion purpose cannot be achieved; if the deposition rate ratio between the first sputtering target and the second sputtering target is too small, that is, if the deposition rate of the second sputtering target is too large, the doping amount will be too high, which will reduce the conductivity and light transmittance of the doped layer, thereby reducing the device efficiency.

[0043] Preferably, the raw material mass ratio of the first sputtering target and the second sputtering target is (95-99):(1-5), wherein the raw material mass selection range of the first sputtering target "95-99" can be, for example, 95, 96, 97, 98 or 99, etc., and the selection range of the first sputtering target "1-5" can be, for example, 1, 2, 3, 4 or 5, etc.

[0044] As a preferred technical solution of the present invention, the preparation method includes the following steps:

[0045] (1) Using the raw materials for preparing the composite layer or the raw materials for preparing the first charge transport layer as the first sputtering target, and the subconversion material as the second sputtering target, the sputtering chamber is evacuated to a vacuum level ≤ 5 × 10⁻⁶. -4 Pa;

[0046] (2) Introduce working gas with a flow rate of 20-60 sccm, perform pre-sputtering for 10-30 min, and then perform dual-source magnetron sputtering for 5-60 min at a pressure of 0.3-0.8 Pa. After the process, the modified intermediate layer is obtained.

[0047] The working gas includes an inert gas and oxygen in a volume ratio of 10:(0.8-1.5), the sputtering power of the first sputtering target is 170-250W, the sputtering power of the second sputtering target is 5-15W, the deposition rate ratio of the first sputtering target and the second sputtering target is (0.15-0.25):(0.004-0.0125), and the raw material mass ratio of the first sputtering target and the second sputtering target is (95-99):(1-5).

[0048] In this invention, the purpose of pre-sputtering for 10-30 minutes is to remove the aged layer on the surface and to make the sputtered film gradually stabilize.

[0049] Thirdly, the present invention provides a perovskite tandem solar cell, the perovskite tandem solar cell comprising the modified intermediate layer as described in the first aspect.

[0050] It should be noted that this invention applies to all perovskite tandem solar cells, including perovskite / perovskite tandem, crystalline silicon / perovskite tandem, and other thin-film solar cells (such as cadmium telluride, copper indium gallium selenide, etc.) / perovskite tandem, etc.

[0051] The numerical range described in this invention includes not only the point values ​​listed above, but also any point values ​​within the numerical ranges not listed above. Due to space limitations and for the sake of brevity, this invention will not exhaustively list all the specific point values ​​included in the range.

[0052] Compared with the prior art, the present invention has the following beneficial effects:

[0053] (1) By introducing downconversion materials into perovskite tandem solar cells, this invention can convert some high-energy photons into low-energy photons, enabling the cells to utilize various bands in the spectrum more effectively. This will reduce light loss, improve photoelectric conversion efficiency, and enable solar cells to generate electricity more effectively under different lighting conditions, thereby improving the performance of the cells in practical applications, especially under low light intensity conditions.

[0054] (2) By introducing downconversion materials into perovskite tandem solar cells, this invention can reduce the extra heat generated by high-energy photon absorption, reduce the risk of temperature rise in the battery, and thus improve the working stability and long-term reliability of the battery.

[0055] (3) By introducing a downconversion material into the perovskite tandem solar cell, this invention can broaden the spectral response range of the cell, enabling it to absorb more high-energy photons that traditional cells cannot utilize or have relatively low utilization rates. At the same time, by improving the band structure of the intermediate layer, the downconversion material is matched with the band structure of the perovskite layer, ensuring efficient photon conversion and increasing its applicability in practical applications.

[0056] (4) By combining downconversion materials with traditional solar cell materials, this invention can achieve stable and efficient application of downconversion materials, promote the large-scale production of perovskite tandem solar cells, increase the market share of perovskite tandem solar cells, accelerate the maturity and promotion of the technology, and thus realize the generation and utilization of clean energy on a larger scale. Attached Figure Description

[0057] Figure 1 This is a schematic diagram of the sputtering equipment structure used in a specific embodiment of the present invention.

[0058] Figure 2 A schematic diagram of the structure of the perovskite / silicon heterostructure tandem solar cell prepared in Example 1 of this invention is shown.

[0059] Figure 3 The stability comparison curves are for the stacked batteries prepared in Application Example 2 and Comparative Example 1 of this invention.

[0060] Wherein, 1-substrate; 2-first sputtering target; 3-second sputtering target; 4-first baffle; 5-second baffle; 6-sputtering chamber; 11-silver grid line; 12-reverse IZO layer; 13-P-type hydrogenated polycrystalline silicon layer; 14-reverse intrinsic hydrogenated polycrystalline silicon layer; 15-N-type single crystal silicon layer; 16-front intrinsic hydrogenated polycrystalline silicon layer; 17-N-type hydrogenated polycrystalline silicon layer; 18-modified intermediate layer; 19-nickel oxide hole transport layer; 20-wide bandgap perovskite absorber layer; 21-lithium fluoride layer; 22-C 60 Layer; 23-Tin dioxide layer; 24-Front IZO layer; 25-Magnesium fluoride layer; 26-Ag electrode. Detailed Implementation

[0061] The technical solution of the present invention will be further illustrated below through specific embodiments. Those skilled in the art should understand that the embodiments described are merely illustrative of the present invention and should not be construed as limiting the invention in any way.

[0062] It should be noted that the following embodiments and comparative examples all adopt the following... Figure 1 The sputtering apparatus shown includes a sputtering chamber 6, which comprises:

[0063] The substrate 1 is located at the top inside the sputtering chamber 6;

[0064] The first sputtering target 2 and the second sputtering target 3 are located on both sides of the bottom end inside the sputtering chamber 6, respectively.

[0065] A first baffle 4 and a second baffle 5 are located above the first sputtering target 2 and above the second sputtering target 3.

[0066] The following are the specific implementation methods.

[0067] Example 1

[0068] This embodiment provides a modified intermediate layer for a perovskite / silicon heterostructure tandem solar cell. The modified intermediate layer is a composite layer doped with downconversion material and is located between the perovskite solar cell and the silicon heterostructure solar cell.

[0069] The downconversion material is Ce. 3+ The doped titanium oxide material has an emission wavelength of 565 nm and a doping amount of 5% in the composite layer.

[0070] The composite layer is an ITO layer, and the thickness of the downconversion material-doped composite layer is 30 nm.

[0071] This embodiment also provides a method for preparing the modified intermediate layer of the above-mentioned perovskite / silicon heterostructure solar cell, the preparation method comprising the following steps:

[0072] (1) Using ITO as the first sputtering target and Ce 3+ The doped titanium oxide material was used as the second sputtering target, and the sputtering chamber was evacuated to a vacuum level of 6 × 10⁻⁶. -4 Pa;

[0073] (2) Introduce an argon-oxygen mixture (volume ratio Ar:O2 = 10:1) with a gas flow rate of 40 sccm and perform a 10-minute pre-sputtering. At this time, close the first and second baffles and then perform a 20-minute dual-source magnetron sputtering under a vacuum pressure of 0.3 Pa. After the sputtering is completed, a modified intermediate layer is obtained on the substrate.

[0074] The first sputtering target has a sputtering power of 250W, the second sputtering target has a sputtering power of 15W, the deposition rate ratio of the first sputtering target to the second sputtering target is 0.2375:0.0125, and the raw material mass ratio of the first sputtering target to the second sputtering target is 95:5.

[0075] Example 2

[0076] This embodiment provides a modified intermediate layer for a perovskite / silicon heterostructure tandem solar cell. The modified intermediate layer is a composite layer doped with downconversion material and is located between the perovskite solar cell and the silicon heterostructure solar cell.

[0077] The downconversion material is Ce. 3+ The doped titanium oxide material has an emission wavelength of 545 nm and a doping amount of 2% in the composite layer;

[0078] The composite layer is an ITO layer, and the thickness of the downconversion material-doped composite layer is 30 nm.

[0079] This embodiment also provides a method for preparing the modified intermediate layer of the above-mentioned perovskite / silicon heterostructure solar cell, the preparation method comprising the following steps:

[0080] (1) Using ITO as the first sputtering target and Ce 3+ The doped titanium oxide material was used as the second sputtering target, and the sputtering chamber was evacuated to a vacuum level of 6 × 10⁻⁶. -4 Pa;

[0081] (2) Introduce an argon-oxygen mixture (volume ratio Ar:O2 = 10:1) with a gas flow rate of 40 sccm and perform a 10-minute pre-sputtering. At this time, close the first and second baffles and then perform a 20-minute dual-source magnetron sputtering under a vacuum pressure of 0.3 Pa. After the sputtering is completed, a modified intermediate layer is obtained on the substrate.

[0082] The first sputtering target has a sputtering power of 250W, the second sputtering target has a sputtering power of 10W, the deposition rate ratio of the first sputtering target to the second sputtering target is 0.2375:0.008, and the raw material mass ratio of the first sputtering target to the second sputtering target is 98:2.

[0083] Example 3

[0084] This embodiment provides a modified intermediate layer for a perovskite / silicon heterostructure tandem solar cell. The modified intermediate layer is a composite layer doped with downconversion material and is located between the perovskite solar cell and the silicon heterostructure solar cell.

[0085] The downconversion material is Ce. 3+ The doped titanium oxide material has an emission wavelength of 525 nm and the doping amount of the downconversion material in the composite layer is 1%.

[0086] The composite layer is an ITO layer, and the thickness of the downconversion material-doped composite layer is 30 nm.

[0087] This embodiment also provides a method for preparing the modified intermediate layer of the above-mentioned perovskite / silicon heterostructure solar cell, the preparation method comprising the following steps:

[0088] (1) Using ITO as the first sputtering target and Ce 3+ The doped titanium oxide material was used as the second sputtering target, and the sputtering chamber was evacuated to a vacuum level of 6 × 10⁻⁶. -4 Pa;

[0089] (2) Introduce an argon-oxygen mixture (volume ratio Ar:O2 = 10:1) with a gas flow rate of 40 sccm and perform a 10-minute pre-sputtering. At this time, close the first and second baffles and then perform a 20-minute dual-source magnetron sputtering under a vacuum pressure of 0.3 Pa. After the sputtering is completed, a modified intermediate layer is obtained on the substrate.

[0090] The first sputtering target has a sputtering power of 250W, the second sputtering target has a sputtering power of 7W, the deposition rate ratio of the first sputtering target to the second sputtering target is 0.2375:0.0056, and the raw material mass ratio of the first sputtering target to the second sputtering target is 99:1.

[0091] Example 4

[0092] The difference between this embodiment and Embodiment 2 is that the composite layer is an IZO layer.

[0093] The remaining preparation methods and parameters are consistent with those in Example 2.

[0094] Example 5

[0095] The difference between this embodiment and Embodiment 2 is that the composite layer is an IWO layer.

[0096] The remaining preparation methods and parameters are consistent with those in Example 2.

[0097] Example 6

[0098] The difference between this embodiment and Embodiment 2 is that the composite layer is an ITIO layer.

[0099] The remaining preparation methods and parameters are consistent with those in Example 2.

[0100] Example 7

[0101] The difference between this embodiment and Embodiment 2 is that the composite layer is an FTO layer.

[0102] The remaining preparation methods and parameters are consistent with those in Example 2.

[0103] Example 8

[0104] The difference between this embodiment and Embodiment 2 is that the composite layer is an AZO layer.

[0105] The remaining preparation methods and parameters are consistent with those in Example 2.

[0106] Example 9

[0107] The difference between this embodiment and Embodiment 2 is that the downconversion material is Sm. 3+ Doped yttrium phosphate materials.

[0108] The remaining preparation methods and parameters are consistent with those in Example 2.

[0109] Example 10

[0110] The difference between this embodiment and Embodiment 2 is that the downconversion material is Eu. 3+ Doped lanthanum oxide materials.

[0111] The remaining preparation methods and parameters are consistent with those in Example 2.

[0112] Example 11

[0113] The difference between this embodiment and Embodiment 2 is that the downconversion material is Eu. 3+ Doped gadolinium oxide materials.

[0114] The remaining preparation methods and parameters are consistent with those in Example 2.

[0115] Example 12

[0116] The difference between this embodiment and Embodiment 2 is that the downconversion material is Tb. 3+ and Yb 3+ Co-doped sodium yttrium tetrafluoride material.

[0117] The remaining preparation methods and parameters are consistent with those in Example 2.

[0118] Example 13

[0119] The difference between this embodiment and Embodiment 2 is that the downconversion material is tin oxide material co-doped with nickel trioxide, copper oxide, and antimony trioxide.

[0120] The remaining preparation methods and parameters are consistent with those in Example 2.

[0121] Example 14

[0122] The difference between this embodiment and Embodiment 2 is that the downconversion material is Pr. 3+ and Yb 3+ Co-doped yttrium phosphate materials.

[0123] The remaining preparation methods and parameters are consistent with those in Example 2.

[0124] Example 15

[0125] The difference between this embodiment and Embodiment 2 is that the downconversion material is Ce. 3+ 、Tb 3+ and Yb 3+ Co-doped yttrium aluminum garnet materials.

[0126] The remaining preparation methods and parameters are consistent with those in Example 2.

[0127] Example 16

[0128] The difference between this embodiment and Embodiment 2 is that the downconversion material is Yb. 3+ Doped yttrium molybdate material.

[0129] The remaining preparation methods and parameters are consistent with those in Example 2.

[0130] Example 17

[0131] The difference between this embodiment and Embodiment 2 is that the downconversion material is Eu. 3+ Doped yttrium vanadate materials.

[0132] The remaining preparation methods and parameters are consistent with those in Example 2.

[0133] Example 18

[0134] The difference between this embodiment and Embodiment 2 is that the downconversion material is Bi. 3+ and Eu 3+ Doped yttrium vanadate materials.

[0135] The remaining preparation methods and parameters are consistent with those in Example 2.

[0136] Example 19

[0137] The difference between this embodiment and Embodiment 2 is that the doping amount of the downconversion material in the composite layer is 55%.

[0138] The remaining preparation methods and parameters are consistent with those in Example 2.

[0139] Example 20

[0140] The difference between this embodiment and embodiment 2 is that the deposition rate ratio of the first sputtering target and the second sputtering target in step (2) is 0.14:0.013.

[0141] The remaining preparation methods and parameters are consistent with those in Example 2.

[0142] Example 21

[0143] The difference between this embodiment and embodiment 2 is that the deposition rate ratio of the first sputtering target and the second sputtering target in step (2) is 0.3:0.003.

[0144] The remaining preparation methods and parameters are consistent with those in Example 2.

[0145] Example 22

[0146] This embodiment provides a modified intermediate layer for a perovskite / silicon heterostructured solar cell. The modified intermediate layer is a hole transport layer doped with downconversion material, and the hole transport layer is located between the tunneling junction layer and the perovskite light-absorbing layer.

[0147] The downconversion material is Ce. 3+ The doped titanium oxide material has an emission wavelength of 565 nm and a doping amount of 5% in the composite layer.

[0148] The hole transport layer is a nickel oxide layer, and the thickness of the hole transport layer doped with the downconversion material is 20 nm.

[0149] This embodiment also provides a method for preparing the modified intermediate layer of the above-mentioned perovskite / silicon heterostructure solar cell, the preparation method comprising the following steps:

[0150] (1) Using ITO as the first sputtering target and Ce 3+ The doped titanium oxide material was used as the second sputtering target, and the sputtering chamber was evacuated to a vacuum level of 6 × 10⁻⁶. -4 Pa;

[0151] (2) Introduce an argon-oxygen mixture (volume ratio Ar:O2 = 10:1) with a gas flow rate of 40 sccm and perform a 10-minute pre-sputtering. At this time, close the first and second baffles and then perform a 13-minute dual-source magnetron sputtering under a vacuum pressure of 0.3 Pa. After the sputtering is completed, a modified intermediate layer is obtained on the substrate.

[0152] The first sputtering target has a sputtering power of 210W, the second sputtering target has a sputtering power of 15W, the deposition rate ratio of the first sputtering target to the second sputtering target is 0.1995:0.0125, and the raw material mass ratio of the first sputtering target to the second sputtering target is 95:5.

[0153] Example 23

[0154] This embodiment provides a modified intermediate layer for a perovskite / silicon heterostructured solar cell. The modified intermediate layer is a hole transport layer doped with downconversion material, and the hole transport layer is located between the tunneling junction layer and the perovskite light-absorbing layer.

[0155] The downconversion material is Ce. 3+ The doped titanium oxide material has an emission wavelength of 545 nm and a doping amount of 2% in the composite layer;

[0156] The hole transport layer is a nickel oxide layer, and the thickness of the hole transport layer doped with the downconversion material is 20 nm.

[0157] This embodiment also provides a method for preparing the modified intermediate layer of the above-mentioned perovskite / silicon heterostructure solar cell, the preparation method comprising the following steps:

[0158] (1) Using ITO as the first sputtering target and Ce 3+ The doped titanium oxide material was used as the second sputtering target, and the sputtering chamber was evacuated to a vacuum level of 6 × 10⁻⁶. -4 Pa;

[0159] (2) Introduce an argon-oxygen mixture (volume ratio Ar:O2 = 10:1) with a gas flow rate of 40 sccm and perform a 10-minute pre-sputtering. At this time, close the first and second baffles and then perform a 13-minute dual-source magnetron sputtering under a vacuum pressure of 0.3 Pa. After the sputtering is completed, a modified intermediate layer is obtained on the substrate.

[0160] The first sputtering target has a sputtering power of 210W, the second sputtering target has a sputtering power of 10W, the deposition rate ratio of the first sputtering target to the second sputtering target is 0.1995:0.008, and the raw material mass ratio of the first sputtering target to the second sputtering target is 98:2.

[0161] Example 24

[0162] This embodiment provides a modified intermediate layer for a perovskite / silicon heterostructured solar cell. The modified intermediate layer is a hole transport layer doped with downconversion material, and the hole transport layer is located between the tunneling junction layer and the perovskite light-absorbing layer.

[0163] The downconversion material is Ce. 3+ The doped titanium oxide material has an emission wavelength of 525 nm and the doping amount of the downconversion material in the composite layer is 1%.

[0164] The hole transport layer is a nickel oxide layer, and the thickness of the hole transport layer doped with the downconversion material is 20 nm.

[0165] This embodiment also provides a method for preparing the modified intermediate layer of the above-mentioned perovskite / silicon heterostructure solar cell, the preparation method comprising the following steps:

[0166] (1) Using ITO as the first sputtering target and Ce 3+ The doped titanium oxide material was used as the second sputtering target, and the sputtering chamber was evacuated to a vacuum level of 6 × 10⁻⁶. -4 Pa;

[0167] (2) Introduce an argon-oxygen mixture (volume ratio Ar:O2 = 10:1) with a gas flow rate of 40 sccm and perform a 10-minute pre-sputtering. At this time, close the first and second baffles and then perform a 13-minute dual-source magnetron sputtering under a vacuum pressure of 0.3 Pa. After the sputtering is completed, a modified intermediate layer is obtained on the substrate.

[0168] The first sputtering target has a sputtering power of 210W, the second sputtering target has a sputtering power of 7W, the deposition rate ratio of the first sputtering target to the second sputtering target is 0.1995:0.006, and the raw material mass ratio of the first sputtering target to the second sputtering target is 99:1.

[0169] Example 25

[0170] The difference between this embodiment and Embodiment 22 is that the downconversion material is Sm. 3+ Doped yttrium phosphate materials.

[0171] The remaining preparation methods and parameters are consistent with those in Example 22.

[0172] Example 26

[0173] The difference between this embodiment and embodiment 22 is that the downconversion material is Eu. 3+ Doped lanthanum oxide materials.

[0174] The remaining preparation methods and parameters are consistent with those in Example 22.

[0175] Example 27

[0176] The difference between this embodiment and embodiment 22 is that the downconversion material is Eu. 3+ Doped gadolinium oxide materials.

[0177] The remaining preparation methods and parameters are consistent with those in Example 22.

[0178] Example 28

[0179] The difference between this embodiment and embodiment 22 is that the downconversion material is Tb. 3+ and Yb 3+ Co-doped sodium yttrium tetrafluoride material.

[0180] The remaining preparation methods and parameters are consistent with those in Example 22.

[0181] Example 29

[0182] The difference between this embodiment and Embodiment 22 is that the downconversion material is tin oxide material co-doped with nickel oxide, copper oxide, and antimony oxide.

[0183] The remaining preparation methods and parameters are consistent with those in Example 22.

[0184] Example 30

[0185] The difference between this embodiment and embodiment 22 is that the downconversion material is Pr. 3+ and Yb 3+ Co-doped yttrium phosphate materials.

[0186] The remaining preparation methods and parameters are consistent with those in Example 22.

[0187] Example 31

[0188] The difference between this embodiment and embodiment 22 is that the downconversion material is Ce. 3+ 、Tb 3+ and Yb 3+ Co-doped yttrium aluminum garnet materials.

[0189] The remaining preparation methods and parameters are consistent with those in Example 22.

[0190] Example 32

[0191] The difference between this embodiment and embodiment 22 is that the downconversion material is Yb. 3+ Doped yttrium molybdate material.

[0192] The remaining preparation methods and parameters are consistent with those in Example 22.

[0193] Example 33

[0194] The difference between this embodiment and embodiment 22 is that the downconversion material is Eu. 3+ Doped yttrium vanadate materials.

[0195] The remaining preparation methods and parameters are consistent with those in Example 22.

[0196] Example 34

[0197] The difference between this embodiment and embodiment 22 is that the downconversion material is Bi. 3+ and Eu 3+ Doped yttrium vanadate materials.

[0198] The remaining preparation methods and parameters are consistent with those in Example 22.

[0199] Example 35

[0200] The difference between this embodiment and embodiment 22 is that the doping amount of the downconversion material in the hole transport layer is 55%.

[0201] The remaining preparation methods and parameters are consistent with those in Example 22.

[0202] Comparative Example 1

[0203] The difference between this comparative example and Example 2 is that this comparative example does not dope the composite layer with downconversion material; that is, this comparative example provides a pure ITO layer.

[0204] The remaining preparation methods and parameters are consistent with those in Example 2.

[0205] Application Example 1

[0206] This application example provides a perovskite / silicon heterostructure tandem solar cell, the schematic diagram of which is shown below. Figure 2 As shown, the perovskite / silicon heterostructured solar cell includes, in sequence, a silver grid line 11, a reverse IZO layer 12, a P-type hydrogenated polycrystalline silicon layer 13, a reverse intrinsic hydrogenated polycrystalline silicon layer 14, an N-type monocrystalline silicon layer 15, a front intrinsic hydrogenated polycrystalline silicon layer 16, an N-type hydrogenated polycrystalline silicon layer 17, a modified intermediate layer 18, a nickel oxide hole transport layer 19, a wide-bandgap perovskite absorber layer 20, a lithium fluoride layer 21, and a C-type silicon layer 22. 60 Layer 22, tin dioxide layer 23, front IZO layer 24, magnesium fluoride layer 25 and Ag electrode 26.

[0207] This application example also provides a method for fabricating the above-mentioned perovskite / silicon heterostructure tandem solar cell, the method comprising the following steps:

[0208] (a) A 150 μm thick N-type monocrystalline silicon layer 15 is formed by sequentially pre-cleaning with ozone and deionized water, post-cleaning with a mixture of ozone and hydrofluoric acid, and finally cleaning and etching with a mixture of hydrofluoric acid and nitric acid.

[0209] (b) A 2 nm intrinsic hydrogenated polysilicon passivation layer (including an intrinsic hydrogenated polysilicon layer 16 on the front side and an intrinsic hydrogenated polysilicon layer 14 on the back side) is deposited on both sides of the N-type monocrystalline silicon layer 15 by PECVD. Then, a 9 nm P-type hydrogenated polysilicon layer 13 and a 6 nm N-type hydrogenated polysilicon layer 17 are deposited on both sides respectively.

[0210] (c) Using the modified preparation method as described in Example 1, a modified intermediate layer 18 is sputtered and deposited on the N-type hydrogenated polycrystalline silicon layer 17;

[0211] (d) A 15 nm nickel oxide hole transport layer 19 and a 400 nm wide-bandgap perovskite light-absorbing layer 20 (CH(NH2)2PbI3) are sequentially deposited on the surface of the modified intermediate layer 18. 0.83 Cs 0.17 Pb(I 0.82 Br 0.18 3. A 1nm lithium fluoride layer; 21. A 12nm C layer 60Layer 22 and 9nm tin dioxide layer 23;

[0212] (e) Deposit 110 nm IZO layers (including front IZO layer 24 and back IZO layer 12) on the front and back sides of the battery respectively, and then deposit a 90 nm magnesium fluoride layer 25 on the front IZO layer 24.

[0213] (f) A 180nm Ag electrode 26 and a 180nm silver grid line 11 are screen-printed on the front and back sides of the battery, respectively, and the perovskite / silicon heterostructure tandem battery is obtained after sintering and solidification.

[0214] Application Example 2-21

[0215] The difference between Application Example 2-21 and Application Example 1 is that the preparation method of the modified intermediate layer in step (c) is provided by Example 2-21.

[0216] The remaining preparation methods and parameters are consistent with those in Application Example 1.

[0217] Application Example 22

[0218] This application example provides a perovskite / silicon heterostructure tandem solar cell, the schematic diagram of which is shown below. Figure 2 As shown, the perovskite / silicon heterostructure tandem solar cell includes, in sequence, a silver grid line, a reverse IZO layer, a P-type hydrogenated polycrystalline silicon layer, a reverse intrinsic hydrogenated polycrystalline silicon layer, an N-type monocrystalline silicon layer, a front intrinsic hydrogenated polycrystalline silicon layer, an N-type hydrogenated polycrystalline silicon layer, a modified intermediate layer, a nickel oxide hole transport layer, a wide-bandgap perovskite absorber layer, a lithium fluoride layer, and a C-type monocrystalline silicon layer. 60 The structure consists of a tin dioxide layer, a front-side IZO layer, a magnesium fluoride layer, and an Ag electrode.

[0219] This application example also provides a method for fabricating the above-mentioned perovskite / silicon heterostructure tandem solar cell, the method comprising the following steps:

[0220] (a) A 150 μm thick N-type monocrystalline silicon layer is sequentially pre-cleaned with ozone and deionized water, post-cleaned with a mixture of ozone and hydrofluoric acid, and finally cleaned and etched with a mixture of hydrofluoric acid and nitric acid to form an N-type monocrystalline silicon layer with double-sided textured surface.

[0221] (b) A 2 nm intrinsic hydrogenated polysilicon passivation layer (including an intrinsic hydrogenated polysilicon layer on the front side and an intrinsic hydrogenated polysilicon layer on the back side) is deposited on both sides of the N-type single crystal silicon layer using the PECVD method. Then, a 9 nm P-type hydrogenated polysilicon layer and a 6 nm N-type hydrogenated polysilicon layer are deposited on both sides respectively.

[0222] (c) A 30 nm ITO layer is sputtered onto the N-type hydrogenated polycrystalline silicon.

[0223] (d) A modified intermediate layer (prepared by the preparation method provided in Example 22) and a 400 nm perovskite light-absorbing layer (CH(NH2)2PbI3) are sequentially deposited on the surface of the ITO layer. 0.83 Cs 0.17 Pb(I 0.82 Br 0.18 3. 1nm lithium fluoride, 12nm C 60 A layer and a 9nm tin dioxide layer;

[0224] (e) Deposit 110 nm IZO layers (including front IZO layer and back IZO layer) on the front and back sides of the battery respectively, and then deposit a 90 nm magnesium fluoride layer on the front IZO layer.

[0225] (f) A 180nm Ag electrode and a 180nm silver grid line are screen-printed on the front and back sides of the battery, respectively, and the perovskite / silicon heterostructure tandem battery is obtained after sintering and solidification.

[0226] Application Examples 23-35

[0227] The difference between Application Examples 23-35 and Application Example 22 is that the preparation method of the modified intermediate layer in step (d) is provided by Examples 23-35.

[0228] The remaining preparation methods and parameters are consistent with those in Application Example 22.

[0229] Application Example 36

[0230] This application example provides a perovskite / perovskite tandem solar cell, comprising a glass substrate, a thin metal layer, a PEDOT:PSS layer, and a narrow bandgap perovskite light-absorbing layer FA stacked sequentially. 0.7 MA 0.3 Pb 0.5 Sn 0.5 I3, C 60 Dense layer, modified intermediate layer, PTAA, wide-bandgap perovskite light-absorbing layer FA 0.8 Cs 0.2 Pb(I 0.62 Br 0.38 3. C 60 The structure consists of a buffer layer, a transparent conductive layer, and a top gate electrode.

[0231] This application example also provides a method for preparing the above-mentioned perovskite / perovskite tandem solar cell, the method comprising the following steps:

[0232] (a) A 20 nm copper layer is deposited on a clean glass substrate by thermal evaporation as a bottom metal layer, and then an ITO layer with a thickness of 10 nm is deposited on the metal layer by magnetron sputtering as a non-metallic conductive layer.

[0233] (c) Using poly(3,4-ethylenedioxythiophene):polystyrene sulfonate (PEDOT:PSS) as the hole transport layer, the annealing temperature is 100℃; a narrow bandgap perovskite light-absorbing layer FA is deposited on the PEDOT:PSS layer. 0.7 MA 0.3 Pb 0.5 Sn 0.5 I3, annealed at 100℃, with a thickness of 1100nm; a layer of C was prepared by thermal evaporation. 60 As an electron transport layer, it has a thickness of 30 nm; atomic layer deposition is used on C 60 A SnO2 layer is grown on top as a dense layer, the chamber temperature is 75℃, and the thickness is 10nm;

[0234] (d) Using ITO as the primary sputtering target and Ce 3+ The doped titanium oxide material was used as the second sputtering target, and the sputtering chamber was evacuated to a vacuum level of 6 × 10⁻⁶. -4 Pa; an argon-oxygen mixture (volume ratio Ar:O2 = 10:1) with a flow rate of 40 sccm was introduced, and pre-sputtering was performed for 10 min. At this time, the first and second baffles were closed, and then dual-source magnetron sputtering was performed for 20 min under a vacuum pressure of 0.3 Pa. After the process, a modified intermediate layer with a thickness of 20 nm was obtained.

[0235] The first sputtering target has a sputtering power of 170W, the second sputtering target has a sputtering power of 5W, and Ce 3+ The doping amount of the titanium oxide material in the modified intermediate layer is 2%;

[0236] (e) Prepare a 20 nm layer of poly[bis(4-phenyl)(2,4,6-trimethylphenyl)amine] (PTAA) as a hole transport layer; deposit a wide-bandgap perovskite light-absorbing layer FA on the hole transport layer. 0.8 Cs 0.2 Pb(I 0.62 Br 0.38 3. Annealing temperature is 85℃, thickness is 400nm; a layer of C is prepared by thermal evaporation. 60 As an electron transport layer, it has a thickness of 15 nm; a SnO2 layer with a thickness of 10 nm is grown using atomic layer deposition.

[0237] (f) An IZO layer with a thickness of 60 nm was grown on the buffer layer by magnetron sputtering as a transparent conductive layer; a Cu layer with a thickness of 150 nm was deposited by thermal evaporation as the top gate electrode.

[0238] Application Example 37

[0239] This application example provides a copper indium gallium selenide (CIGS) / perovskite tandem solar cell, which includes a CIGS multilayer film structure layer, an electron transport layer, a perovskite absorber layer, a hole transport layer, an ITO layer, and a metal conductor layer stacked sequentially.

[0240] This application example also provides a method for fabricating the above-mentioned copper indium gallium selenide / perovskite tandem solar cell, the method comprising the following steps:

[0241] (a) A Mo metal back electrode layer with a thickness of 300 nm was physically sputtered on a glass substrate, followed by a CIGS absorber layer with a thickness of 2 μm was physically vacuum evaporated, and finally a double buffer layer (the first buffer layer is a CdS buffer layer and the second buffer layer is a MgZnO buffer layer with a thickness of 30 nm each) and a second transparent conductive layer were fabricated sequentially using a physical vacuum sputtering equipment.

[0242] (b) Using ITO as the primary sputtering target and Ce 3+ The doped titanium oxide material was used as the second sputtering target, and the sputtering chamber was evacuated to a vacuum level of 6 × 10⁻⁶. -4 Pa; an argon-oxygen mixture (volume ratio Ar:O2 = 10:1) with a flow rate of 40 sccm was introduced, and pre-sputtering was performed for 10 min. At this time, the first and second baffles were closed, and then dual-source magnetron sputtering was performed for 20 min under a vacuum pressure of 0.3 Pa. After the process, a modified intermediate layer with a thickness of 20 nm was obtained.

[0243] The first sputtering target has a sputtering power of 170W, the second sputtering target has a sputtering power of 5W, and Ce 3+ The doping amount of the titanium oxide material in the modified intermediate layer is 2%;

[0244] (c) An electron transport layer of SnO2 with a thickness of 15 nm was grown on the modified intermediate layer using atomic layer deposition; a wide-bandgap perovskite light-absorbing layer FA was also deposited. 0.8 Cs 0.2 Pb(I 0.62 Br 0.38 3. Annealing temperature is 85℃, thickness is 400nm; a hole transport layer with a thickness of 15nm is formed by plasma reaction deposition of nickel oxide;

[0245] (d) An ITO layer with a thickness of 80 nm was formed by magnetron sputtering; silver metal lines were screen printed to obtain a metal conductor layer with a thickness of 15 μm.

[0246] Application Comparative Example 1

[0247] The difference between Comparative Example 1 and Application Example 1 is that the method for preparing the modified intermediate layer in step (c) is provided by Comparative Example 1.

[0248] The remaining preparation methods and parameters are consistent with those in Application Example 1.

[0249] Performance testing

[0250] The photoelectric performance of the tandem solar cells prepared in the above application examples and comparative examples was tested under standard test conditions (1.5 AM), with a test area of ​​1 cm². 2 The test results are shown in Table 1.

[0251] Table 1

[0252]

[0253]

[0254] Stability Test: In this invention, the stacked batteries prepared in Application Example 2 and Comparative Example 1 were placed under sunlight for 500 hours, and the battery efficiency was tested. Figure 3 As shown in the figure, the efficiency of the stacked battery prepared in Application Example 2 can still be maintained at over 80%, which is significantly higher than that of Application Comparative Example 1.

[0255] analyze:

[0256] As shown in the table above, the modified intermediate layer provided by this invention can effectively reduce light loss and improve light utilization efficiency, thus significantly improving the efficiency of the tandem solar cell. Furthermore, the stability of the cell is also improved to some extent.

[0257] The data results from Application Example 2 and Application Example 19 show that if the downconversion material is doped too much in the composite layer, the electrical conductivity and light transmittance will be reduced, thereby reducing the device efficiency.

[0258] The data results from Application Example 2 and Application Examples 20-21 show that if the deposition rate ratio of the first sputtering target to the second sputtering target is too small, that is, the deposition rate of the second sputtering target is too large, the doping amount will be too high, which will reduce the conductivity and light transmittance of the doped layer, thereby reducing the device efficiency; if the deposition rate ratio of the first sputtering target to the second sputtering target is too large, that is, the deposition rate of the second sputtering target is too small, the doping amount will be too low, and the down-conversion purpose cannot be achieved.

[0259] The data results from Application Examples 22 and 35 show that if the downconversion material is doped too much in the hole transport layer, the performance of the device will be severely reduced.

[0260] As can be seen from the data results of Application Example 1 and Application Comparative Example 1, by introducing downconversion materials into the perovskite tandem solar cell, the present invention can not only increase the light utilization rate and improve the conversion efficiency of the cell, but also reduce the light loss and heat loss of the cell, improve the stability and lifespan of the cell, and increase its applicability in practical applications.

[0261] The applicant declares that the present invention is illustrated by the above embodiments, but the present invention is not limited to the above process steps, that is, it does not mean that the present invention must rely on the above process steps to be implemented. Those skilled in the art should understand that any improvements to the present invention, equivalent substitutions of the raw materials used in the present invention, addition of auxiliary components, selection of specific methods, etc., all fall within the protection scope and disclosure scope of the present invention.

Claims

1. A modified intermediate layer for a perovskite tandem solar cell, characterized in that, The modified intermediate layer is a composite layer doped with downconversion material, and the composite layer is located between the top cell and the bottom cell; or, The modified intermediate layer is a first charge transport layer doped with downconversion material, and the first charge transport layer is located between the tunneling junction layer and the perovskite light-absorbing layer.

2. The modified intermediate layer according to claim 1, characterized in that, The downconversion material has an emission wavelength of 400-700 nm; The doping amount of the downconversion material in the composite layer or the first charge transport layer is independently 0-50%, excluding 0%.

3. The modified intermediate layer according to claim 1, characterized in that, The composite layer comprises a transparent conductive oxide; The first charge transport layer includes a hole transport layer.

4. The modified intermediate layer according to any one of claims 1-3, characterized in that, The downconversion material includes a first compound doped with rare earth ions, a composite oxide, or a material doped with Bi. 3+ Any one or at least two of the second compounds; The rare earth ions include Ce. 3+ Pr 3+ Yb 3+ 、Sm 3+ Eu 3+ or Tb 3+ Any one or at least two of them; The first and second compounds independently comprise any one of metal oxides, phosphates, sulfur oxides, fluorides, yttrium aluminum garnet, molybdates, or vanadates.

5. The modified intermediate layer according to claim 1, characterized in that, The thickness of the composite layer doped with the downconversion material is 20-40 nm; The thickness of the first charge transport layer doped with the downconversion material is 15-25 nm.

6. A method for preparing a modified intermediate layer of a perovskite tandem solar cell as described in any one of claims 1-5, characterized in that, The preparation method includes the following steps: Using the raw materials for preparing the composite layer or the raw materials for preparing the first charge transport layer as the first sputtering target and the subconversion material as the second sputtering target, dual-source magnetron sputtering is performed using the first sputtering target and the second sputtering target to obtain the modified intermediate layer.

7. The preparation method according to claim 6, characterized in that, Before performing the dual-source magnetron sputtering, a working gas is first introduced; The working gas includes an inert gas and oxygen, and the volume ratio of the inert gas to oxygen is 10:(0.8-1.5). During the dual-source magnetron sputtering process, the pressure inside the sputtering chamber is 0.3-0.8 Pa; The sputtering time for the dual-source magnetron sputtering is 5-60 minutes.

8. The preparation method according to claim 6, characterized in that, The sputtering power of the first sputtering target is 170-250W; The sputtering power of the second sputtering target is 5-15W; The deposition rate ratio of the first sputtering target to the second sputtering target is (0.15-0.25):(0.004-0.0125); The mass ratio of the raw materials of the first sputtering target and the second sputtering target is (95-99):(1-5).

9. The preparation method according to claim 6, characterized in that, The preparation method includes the following steps: (1) Using the raw materials for preparing the composite layer or the raw materials for preparing the first charge transport layer as the first sputtering target, and the subconversion material as the second sputtering target, the sputtering chamber is evacuated to a vacuum level ≤ 5 × 10⁻⁶. -4 Pa; (2) Introduce working gas with a flow rate of 20-60 sccm, perform pre-sputtering for 10-30 min, and then perform dual-source magnetron sputtering for 5-60 min at a pressure of 0.3-0.8 Pa. After the process, the modified intermediate layer is obtained. The working gas includes an inert gas and oxygen in a volume ratio of 10:(0.8-1.5), the sputtering power of the first sputtering target is 170-250W, the sputtering power of the second sputtering target is 5-15W, the deposition rate ratio of the first sputtering target and the second sputtering target is (0.15-0.25):(0.004-0.0125), and the raw material mass ratio of the first sputtering target and the second sputtering target is (95-99):(1-5).

10. A perovskite tandem solar cell, characterized in that, The perovskite tandem solar cell includes a modified intermediate layer as described in any one of claims 1-5.

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