CN110299451B - Flexible perovskite-copper indium gallium selenide laminated solar cell and preparation method thereof - Google Patents
Flexible perovskite-copper indium gallium selenide laminated solar cell and preparation method thereof Download PDFInfo
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Abstract
The invention discloses a flexible perovskite-copper indium gallium selenide laminated solar cell which comprises a flexible copper indium gallium selenide cell serving as a bottom cell unit and a perovskite cell serving as a top cell unit, wherein the top cell unit and the bottom cell unit are connected through an ITO (indium tin oxide) middle layer. According to the laminated solar cell, two materials of CIGS and perovskite which are matched are selected as the light absorption layer, ITO with high conductivity and high light transmittance is selected as the middle layer tunnel junction, the two sub-cells are integrally combined, the total light reaching the bottom cell is increased, the series resistance is reduced, and the light absorption utilization rate is better than that of a single junction cell; the invention also selects a hole layer PTAA which is more matched with the ITO intermediate layer and has high conductivity and a PCBM electronic layer with hydrophobicity, thereby further improving the efficiency and stability of the laminated cell.
Description
Technical Field
The invention relates to a flexible perovskite-copper indium gallium selenide laminated solar cell and a preparation method thereof, belonging to the field of solar cell preparation processes and devices.
Background
In the present society, the problem of environmental pollution and the problem of consumption of non-renewable resources due to the massive use of fossil energy, such as coal, oil and natural gas, have become a big problem in human sustainable development. Therefore, the development and use of new energy sources which are novel, environment-friendly and renewable are great trends of social development, and the preparation and the use of solar cells have recognized advantages.
The perovskite light absorption layer is rich in material source and low in price, and in recent years, perovskite solar cells similar to dye sensitization structures are adopted to attract wide attention in the photovoltaic field. The photoelectric conversion efficiency of the perovskite solar cell is improved very rapidly, the conversion efficiency is only 3.8% at the beginning of 2009, the conversion efficiency is rapidly improved to 10.9% in 2012, and the efficiency of the perovskite solar cell is 23.7% nowadays.
However, the energy distribution in the spectrum of sunlight is wide, and any semiconductor material in the prior art can only absorb photons with energy higher than the energy gap value of the semiconductor material. Photons with smaller energy in the sunlight penetrate through the cell, are absorbed by the back electrode metal and are converted into heat energy; the excess energy of the high-energy photon exceeding the width of the energy gap is transferred to lattice atoms of the cell material through the energy thermolysis of the photon-generated carrier, so that the material is heated. None of this energy is transferred to the load by the photogenerated carriers and becomes effectively electrical energy. For a better and more complete absorption of light, tandem solar cells are thus produced. The solar spectrum can be divided into a plurality of continuous parts, the solar cells are made of materials with the energy band widths which are best matched with the parts, the solar cells are stacked from outside to inside according to the sequence of the energy gaps from large to small, light with the shortest wavelength is used by the outermost wide-gap material cell, light with longer wavelength can be transmitted into the solar cells with narrower energy gaps, the light energy can be converted into electric energy to the maximum extent, and the solar cells are stacked, so that the performance and the stability can be greatly improved.
The current matching of the top layer cell and the bottom layer cell in the tandem solar cell is a key factor influencing the performance of the tandem solar cell, so the principle of the structural design of the tandem solar cell is to make the absorption spectrum distribution of each single junction cell reasonable. The materials and the thicknesses of the top cell absorption layer and the bottom cell absorption layer are reasonably selected to solve the problem of current matching of the tandem solar cell, so that the tandem solar cell has better performance and important research significance.
Disclosure of Invention
Aiming at the key problem in the preparation of the laminated solar cell, the invention discloses a flexible perovskite-copper indium gallium selenide laminated solar cell and a preparation method thereof, aiming at solving the technical problem of adopting Cs 0.1 MA 0.9 PbI 2.9 Cl 0.1 The current matching of the top layer battery and the bottom layer battery is realized by two absorption layers of perovskite thin film and CIGS thin film with different band gaps and thicknesses, and the efficient and stable laminated solar battery is prepared by optimizing the energy level arrangement of each level.
In order to realize the purpose of the invention, the following technical scheme is adopted:
a flexible perovskite-copper indium gallium selenide laminated solar cell is characterized in that: the flexible copper indium gallium selenide battery comprises a flexible copper indium gallium selenide battery serving as a bottom battery unit and a perovskite battery serving as a top battery unit, wherein the top battery unit is connected with the bottom battery unit through an ITO (indium tin oxide) middle layer;
the structure of the flexible copper indium gallium selenide battery sequentially comprises the following components: the device comprises a flexible stainless steel substrate, a Mo metal electrode layer, a CIGS light absorption layer film, a CdS buffer layer and an AZO film;
the perovskite battery structure from bottom to top does in proper order: PTAA hole transport layer, cs 0.1 MA 0.9 PbI 2.9 Cl 0.1 Perovskite light absorption layer thin film, PCBM electron transport layer, and C 60 An interface modification layer and an Ag top electrode.
Further: in the flexible copper indium gallium selenide battery, the thickness of the flexible stainless steel substrate is 20-40 mu m, and the Mo metal electrode layerThe thickness of the CIGS light absorption layer film is 400-600nm, the thickness of the CIGS light absorption layer film is 1-2 mu m, the thickness of the CdS buffer layer is 400-600nm, and the thickness of the AZO film is 200-300 nm; in the perovskite battery, the thickness of the PTAA hole transport layer is 100-120 nm, and the Cs is 0.1 MA 0.9 PbI 2.9 Cl 0.1 The thickness of the perovskite light absorption layer film is 500-600 nm, the thickness of the PCBM electron transmission layer is 30-40 nm, and C 60 The thickness of the interface modification layer is 10-20 nm, and the thickness of the Ag top electrode is 100-150 nm; the ITO intermediate layer is 30-50 nm.
The preparation method of the flexible perovskite-copper indium gallium selenide laminated solar cell comprises the following steps:
(1) Preparation of flexible copper indium gallium selenide battery serving as bottom battery unit
Firstly, sputtering a Mo metal electrode on a flexible stainless steel substrate, depositing a CIGS absorption layer film by using a multi-element co-evaporation method, preparing a CdS buffer layer by using a chemical water bath deposition method, and then sputtering an AZO film;
(2) Preparation of the intermediate layer
Sputtering an ITO intermediate layer on the AZO film of the flexible copper indium gallium selenide battery;
(3) Preparation of perovskite cells as top cell units
(31) Adhering the substrate to glass by using a double-sided adhesive tape; dissolving 6-10 mg of PTAA powder in 1mL of chlorobenzene, and then spin-coating the mixture on the ITO intermediate layer to form a PTAA hole transport layer;
(32) 0.645g of PbI 2 Dissolving the powder and 0.024g CsCl powder in 1mL of mixed solution consisting of DMF and DMSO according to the volume ratio of 7; spin-coating the precursor solution on the PTAA hole transport layer to form a film, transferring the substrate into a tube furnace, adding 3g of MAI powder into the tube furnace, and obtaining Cs by in-situ chemical vapor deposition 0.1 MA 0.9 PbI 2.9 Cl 0.1 A perovskite light absorption layer thin film;
(33) Dissolving 20-30 mg of PCBM powder in 1mL of chlorobenzene, and then spin-coating to the perovskite light absorption layer filmForming a PCBM electron transport layer; thermally evaporating a layer of C on the PCBM electron transport layer 60 As an interface modification layer; and finally, evaporating Ag to be used as a top electrode, and obtaining the flexible perovskite-copper indium gallium selenide laminated solar cell.
Further, the chemical water bath deposition method in the step (1) comprises the following steps: firstly, adding 100mL of deionized water into a beaker, weighing 0.0549g of cadmium chloride and 1.1418g of thiourea, adding 26mL of ammonia water with the mass concentration of 25-28%, and finally adding deionized water to a constant volume of 200mL to obtain a buffer layer precursor solution; and (3) heating the water bath to 60 ℃, soaking the substrate in the buffer layer precursor solution for 20min, taking out, washing the surface with deionized water, and drying with nitrogen to form the CdS buffer layer.
Further, in the step (31), the PTAA is spin-coated at 2500 to 3000rpm for 30 to 40 seconds, followed by annealing at 90 ℃ for 5min.
Further, in the step (32), the stirring temperature for forming the precursor solution is 70 to 90 ℃.
Further, in the step (32), the spin coating speed of the precursor solution is 4000-5000 rpm, the time is 30-40 s, and then annealing is performed at 100 ℃ for 30min.
Further, in the step (32), the conditions of the in-situ chemical vapor deposition are as follows: firstly, vacuumizing to 1-100 Pa, then heating to 140-150 ℃, preserving heat for reaction for 60min, finally naturally cooling to room temperature, and taking out.
Further, in step (33), the spin coating speed for forming the PCBM electron transport layer is 3000-4000 rpm for 30-40 s, and then the PCBM electron transport layer is annealed at 60 ℃ for 3min, so that the material used in the experiment can be scaled up or down according to the specific implementation.
Compared with the prior art, the invention has the beneficial effects that:
1. according to the laminated solar cell, two materials of CIGS and perovskite which are matched are selected as the light absorption layer, ITO with high conductivity and high light transmittance is selected as the middle layer tunnel junction, the two sub-cells are integrally combined, the total light reaching the bottom cell is increased, the series resistance is reduced, and the light absorption utilization rate is better than that of a single junction cell. The invention also selects a hole layer PTAA which is more matched with the ITO intermediate layer and has high conductivity and a PCBM electronic layer with hydrophobicity, thereby further improving the efficiency and stability of the laminated cell.
2. The laminated solar cell adopts the flexible substrate, has light weight, thin thickness, good flexibility, moderate bending, excellent performance and wide application, and is greatly convenient for the application of outdoor solar charging.
3. The laminated solar cell is simple in preparation process, free of expensive equipment application and complex glove box operation, capable of being prepared in the atmosphere and strong in processability.
4. The laminated solar cell is easy to amplify due to the laminated design, and can be properly expanded to the preparation of laminated cells such as perovskite-perovskite and perovskite-silicon.
Drawings
Fig. 1 is a schematic structural view of a flexible copper indium gallium selenide solar cell in comparative example 1;
fig. 2 is a current density-voltage (J-V) characteristic curve of the flexible copper indium gallium selenide solar cell in comparative example 1;
fig. 3 is a schematic structural diagram of a flexible perovskite-copper indium gallium selenide laminated solar cell in example 1;
FIG. 4 is a scanning electron microscope photograph of an ITO intermediate layer in example 1;
FIG. 5 shows Cs in example 1 0.1 MA 0.9 PbI 2.9 Cl 0.1 Scanning electron micrographs of the perovskite light absorbing layer thin film;
fig. 6 is a current density-voltage (J-V) characteristic curve of the flexible perovskite-copper indium gallium selenide tandem solar cell in example 1.
Detailed Description
In order to make the aforementioned objects, features and advantages of the present invention more comprehensible, specific embodiments thereof will be described in detail with reference to the following examples. The following is merely exemplary and illustrative of the inventive concept and various modifications, additions and substitutions of similar embodiments may be made to the described embodiments by those skilled in the art without departing from the inventive concept or exceeding the scope of the claims defined thereby.
Comparative example 1
In this embodiment, the flexible copper indium gallium selenide battery is used as a comparison, as shown in fig. 1, the structure thereof is from bottom to top: the flexible thin film solar cell comprises a flexible stainless steel substrate with the thickness of 30 mu m, a Mo metal electrode layer with the thickness of 500nm, a CIGS light absorption layer thin film with the thickness of 1 mu m, a CdS buffer layer with the thickness of 60nm, an AZO thin film with the thickness of 300nm and an Ag top electrode with the thickness of 100 nm.
The preparation method of the flexible copper indium gallium selenide battery comprises the following steps:
firstly, a layer of Mo metal electrode is sputtered on a flexible stainless steel substrate.
And then depositing a CIGS absorption layer film by using a multi-stage co-evaporation method, wherein the specific method can be referred to as the following documents: prog.Photoroll: res.appl.2008;16:235-239.
And preparing the CdS buffer layer by using a chemical water bath deposition method: firstly, adding 100mL of deionized water into a beaker, weighing 0.0549g of cadmium chloride and 1.1418g of thiourea, adding 26mL of ammonia water with the mass concentration of 25-28%, and finally adding deionized water to a constant volume of 200mL to obtain a buffer layer precursor solution; and (3) heating the water bath to 60 ℃, soaking the substrate in the buffer layer precursor solution for 20min, taking out, washing the surface with deionized water, and blow-drying with nitrogen to form the CdS buffer layer.
Sputtering a layer of AZO film; and finally, thermally evaporating Ag on the AZO film to be used as an electrode, thereby obtaining the flexible copper indium gallium selenide solar cell.
Fig. 2 is a current density-voltage (J-V) characteristic curve of the flexible copper indium gallium selenide solar cell obtained in the comparative example, and the test conditions are as follows: room temperature, atmospheric environment, spectral distribution AM1.5, light irradiation intensity 100mW/cm 2 。
Example 1
As shown in fig. 2, the flexible perovskite-copper indium gallium selenide stacked solar cell of the embodiment includes a flexible copper indium gallium selenide cell as a bottom cell unit and a perovskite cell as a top cell unit, and the top cell unit and the bottom cell unit are connected through an ITO intermediate layer. Wherein:
the structure of the flexible copper indium gallium selenide battery sequentially comprises the following components: the flexible thin film solar cell comprises a flexible stainless steel substrate with the thickness of 30 mu m, a Mo metal electrode layer with the thickness of 500nm, a CIGS light absorption layer thin film with the thickness of 1 mu m, a CdS buffer layer with the thickness of 60nm, an AZO thin film with the thickness of 300nm and an Ag top electrode with the thickness of 100 nm.
The thickness of the ITO intermediate layer was 40nm.
The structure of the perovskite battery is as follows from up in proper order: PTAA hole transport layer 100nm thick, cs 500nm thick 0.1 MA 0.9 PbI 2.9 Cl 0.1 Perovskite light absorption layer film, PCBM electron transmission layer with thickness of 30nm, and C with thickness of 20nm 60 An interface modification layer and an Ag top electrode with the thickness of 100 nm.
The preparation method of the flexible perovskite-copper indium gallium selenide laminated solar cell comprises the following steps:
(1) Preparation of flexible copper indium gallium selenide battery serving as bottom battery unit
Reference is made to comparative example 1, except that the Ag top electrode is not evaporated.
(2) Preparation of the intermediate layer
Sputtering an ITO intermediate layer on an AZO film of the flexible copper indium gallium selenide battery, and FIG. 4 is a scanning electron microscope image of the ITO intermediate layer.
(3) Preparation of perovskite cells as top cell units
(31) Adhering the substrate to the glass by using a double-sided adhesive tape; the PTAA hole transport layer was formed by adding 8mg PTAA powder to 1mL chlorobenzene, stirring at 60 ℃ for 2h, and spin-coating onto the ITO interlayer (spin-coating speed 2500rpm for 30s, followed by annealing on a heated platform at 90 ℃ for 5 min).
(32) 0.645g of PbI 2 Dissolving the powder and 0.024g CsCl powder in 1mL of mixed solution consisting of DMF and DMSO according to a volume ratio of 7; dripping two drops of DMF solution on the PTAA hole transport layer for spin coating to improve wettability, spin coating the precursor solution on the PTAA hole transport layer to form a film (the spin coating speed is 4000rpm, the time is 30s, then annealing is carried out for 30min at 100 ℃), transferring the substrate into a tube furnace, and putting 3g of MAI powder (the MAI powder is put into the tube furnacePlacing the boat with the substrate facing downwards above the burning boat), and performing in-situ chemical vapor deposition (first vacuumizing, then heating to 140 deg.C, reacting for 60min, naturally cooling to room temperature, taking out, and cleaning the surface with isopropanol) to obtain Cs 0.1 MA 0.9 PbI 2.9 Cl 0.1 A perovskite light absorption layer thin film. FIG. 5 shows Cs 0.1 MA 0.9 PbI 2.9 Cl 0.1 Scanning electron micrographs of the perovskite light absorbing layer thin film revealed that the resulting thin film was uniformly dense.
(33) 20mg of PCBM powder was added to 1mL of chlorobenzene, stirred at 60 ℃ for 1h, and then spin-coated (at a spin-coating speed of 3000rpm for 30s, followed by annealing at 60 ℃ for 30 min) onto the perovskite light-absorbing layer film to form a PCBM electron transport layer. Taking 40mg of C 60 Placing the powder in a tungsten boat, fixing the substrate thereon, and thermally evaporating C under high vacuum 60 As an interface modification layer. And then thermally evaporating Ag particles to be used as a top electrode, thus obtaining the flexible perovskite-copper indium gallium selenide laminated solar cell.
Fig. 6 is a current density-voltage (J-V) characteristic curve of the flexible perovskite-copper indium gallium selenide laminated solar cell obtained in the embodiment, and the test conditions are as follows: room temperature, atmospheric environment, spectral distribution AM1.5, light irradiation intensity 100mW/cm 2 。
Comparing this example with the comparative example, it can be seen that the addition of the perovskite roof cell greatly increases the short-circuit current density value, thereby improving the cell efficiency.
The present invention is not limited to the above exemplary embodiments, and any modifications, equivalent replacements, and improvements made within the spirit and principle of the present invention should be included in the protection scope of the present invention.
Claims (8)
1. A flexible perovskite-copper indium gallium selenide laminated solar cell is characterized in that: the flexible copper indium gallium selenide battery comprises a flexible copper indium gallium selenide battery as a bottom battery unit and a perovskite battery as a top battery unit, wherein the top battery unit is connected with the bottom battery unit through an ITO (indium tin oxide) middle layer;
the structure of the flexible copper indium gallium selenide battery sequentially comprises the following components: a flexible stainless steel substrate with the thickness of 20-40 mu m, a Mo metal electrode layer with the thickness of 400-600nm, a CIGS light absorption layer film with the thickness of 1-2 mu m, a CdS buffer layer with the thickness of 400-600nm and an AZO film with the thickness of 200-300 nm;
the perovskite battery structure from bottom to top does in proper order: a PTAA hole transport layer with the thickness of 100-120 nm and Cs with the thickness of 500-600 nm 0.1 MA 0.9 PbI 2.9 Cl 0.1 Perovskite light absorption layer film, PCBM electron transmission layer with thickness of 30-40 nm, and C with thickness of 10-20 nm 60 An interface modification layer, an Ag top electrode with the thickness of 100-150 nm;
the ITO intermediate layer is 30-50 nm.
2. A method for preparing the flexible perovskite-copper indium gallium selenide laminated solar cell as claimed in claim 1, which is characterized by comprising the following steps:
(1) Preparation of flexible copper indium gallium selenide battery serving as bottom battery unit
Firstly, sputtering a Mo metal electrode on a flexible stainless steel substrate, depositing a CIGS absorption layer film by using a multi-element co-evaporation method, preparing a CdS buffer layer by using a chemical water bath deposition method, and then sputtering an AZO film;
(2) Preparation of the intermediate layer
Sputtering an ITO intermediate layer on the AZO film of the flexible copper indium gallium selenide battery;
(3) Preparation of perovskite cells as top cell units
(31) Adhering the substrate to glass by using a double-sided adhesive tape; dissolving 6-10 mg of PTAA powder in 1mL of chlorobenzene, and then spin-coating the solution on the ITO intermediate layer to form a PTAA hole transport layer;
(32) 0.645g of PbI 2 Dissolving the powder and 0.024g CsCl powder in 1mL of mixed solution consisting of DMF and DMSO according to the volume ratio of 7; spin-coating the precursor solution on the PTAA hole transport layer to form a film, transferring the substrate into a tube furnace, adding 3g of MAI powder into the tube furnace, and obtaining Cs by in-situ chemical vapor deposition 0.1 MA 0.9 PbI 2.9 Cl 0.1 A perovskite light absorption layer thin film;
(33) Dissolving 20-30 mg of PCBM powder in 1mL of chlorobenzene, and then spin-coating the solution on the perovskite light absorption layer film to form a PCBM electron transmission layer; thermally evaporating a layer C on the PCBM electron transport layer 60 As an interface modification layer; and finally, evaporating Ag to be used as a top electrode, and obtaining the flexible perovskite-copper indium gallium selenide laminated solar cell.
3. The method for preparing the nano-particles according to claim 2, wherein the step of the chemical water bath deposition method in the step (1) comprises the following steps:
firstly, adding 100mL of deionized water into a beaker, weighing 0.0549g of cadmium chloride and 1.1418g of thiourea, adding 26mL of ammonia water with the mass concentration of 25-28%, and finally adding deionized water to a constant volume of 200mL to obtain a buffer layer precursor solution; and (3) heating the water bath to 60 ℃, soaking the substrate in the buffer layer precursor solution for 20min, taking out, washing the surface with deionized water, and drying with nitrogen to form the CdS buffer layer.
4. The production method according to claim 2, characterized in that: in the step (31), the PTAA is spin-coated at 2500-3000 rpm for 30-40 s, and then annealed at 90 ℃ for 5min.
5. The method of claim 2, wherein: in the step (32), the stirring temperature for forming the precursor solution is 70-90 ℃.
6. The method of claim 2, wherein: in the step (32), the spin coating speed of the precursor solution is 4000-5000 rpm, the time is 30-40 s, and then annealing is carried out for 30min at 100 ℃.
7. The method of claim 2, wherein: in step (32), the conditions of the in-situ chemical vapor deposition are as follows: firstly, vacuumizing to 1-100 Pa, then heating to 140-150 ℃, preserving heat for reaction for 60min, finally naturally cooling to room temperature, and taking out.
8. The method of claim 2, wherein: in the step (33), the spin coating speed for forming the PCBM electron transport layer is 3000-4000 rpm and the time is 30-40 s, and then annealing is carried out for 3min at 60 ℃.
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| CN112436068A (en) * | 2020-08-25 | 2021-03-02 | 宣城开盛新能源科技有限公司 | CIGS and perovskite laminated solar cell and preparation method thereof |
| CN113193002A (en) * | 2021-04-08 | 2021-07-30 | 电子科技大学 | Perovskite/silicon laminated solar cell and preparation method thereof |
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