CN108365105B - Perovskite solar cell and preparation method thereof - Google Patents
Perovskite solar cell and preparation method thereof Download PDFInfo
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- CN108365105B CN108365105B CN201810287497.8A CN201810287497A CN108365105B CN 108365105 B CN108365105 B CN 108365105B CN 201810287497 A CN201810287497 A CN 201810287497A CN 108365105 B CN108365105 B CN 108365105B
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Abstract
The invention discloses a perovskite solar cell and a preparation method thereof. The perovskite solar cell is characterized by comprising a substrate, a transparent conducting layer, a hole transport layer, a light absorption layer, an electron transport layer and a top electrode which are sequentially stacked; wherein, the substrate is made of glass or flexible plastic materials; the transparent conducting layer is a transparent electrode and is integrally arranged with the substrate; the hole transport layer is made of organic materials or inorganic materials and is used for transporting holes to the transparent electrode; the light absorption layer is made of a photovoltaic material with a perovskite structure and used for absorbing incident light; the electron transport layer is made of metal oxide, PCBM, C60And the like having an excellent electron conduction effect for transporting electrons and isolating the light absorbing layer from the top electrode; the top electrode is made of a material with a higher work function; the invention also provides a method for preparing the perovskite solar cell; the invention improves the short-circuit current and energy conversion efficiency of the perovskite solar cell.
Description
Technical Field
The invention relates to the field of perovskite solar cell preparation, in particular to a perovskite solar cell and a preparation method thereof.
Background
As the energy crisis is becoming more serious, the utilization of solar energy is receiving the attention of cleanness and high consumption of photovoltaic technology, and the high attention of people is attracted. Organometallic halide perovskite solar cells are widely studied due to the unique properties of perovskite materials, such as high absorption coefficient and large carrier diffusion length, low cost manufacturing processes and high power conversion efficiency. The energy conversion efficiency of PSCs (Perovskite Solar Cells) rose from the first reported 3.8% in 2009 to the last 22.1% in the near future. These advantages have led to the remarkable position of PSCs in numerous photovoltaic technologies.
In the case of perovskite thin film production, high quality thin films can be obtained by using thermal evaporation techniques. However, the solution method is low in preparation cost and compatible with flexible technology, so that the method is more promising in application. Compared with the two-step continuous solution deposition method, the one-step solution deposition method is simple in technology and time-saving, and therefore, is widely used for preparing perovskite thin films. However, perovskite thin films prepared by one-step method have small crystal grains and low coverage rate on a substrate. Physical processes such as generation and transmission of carriers, which are very important for the perovskite device, occur inside the perovskite thin film, and therefore, the morphology of the perovskite thin film greatly affects the performance of the PSC.
The ideal perovskite light absorption layer has the characteristics of uniform large grains, high coverage rate, smooth surface and the like. Much research has focused on improving the morphology of perovskite materials, for example, selecting high boiling point solvents to formulate perovskite precursor solutions, reducing the growth rate of perovskite grains by slowing down the evaporation of the solvents, improving the size and uniformity of the grains; the morphology of the perovskite layer is improved by optimizing the interface properties of the hole transport layer or the hole transport layer/the perovskite layer; the perovskite precursor solution at high temperature is coated on a hot substrate in a rotating way to obtain a large-grain perovskite thin film; and post-annealing the perovskite thin film by using solvent vapor, so that the healing of a grain boundary is facilitated, and the grain size is increased. Another widely used method is antisolvent cleaning (ASW) during spin coating of the perovskite precursor solution, which is simple in process and can effectively improve the perovskite morphology. Traditionally, the morphology of an ideal perovskite layer of a high-efficiency perovskite solar cell is considered to be realized, and the perovskite layer is visually represented as a dark brown film with a smooth surface.
Disclosure of Invention
The invention aims to provide a perovskite solar cell and a preparation method thereof aiming at the technical problems in the prior art, and the specific technical scheme is as follows:
on one hand, the perovskite solar cell comprises a substrate, a transparent conducting layer, a hole transport layer, a light absorption layer, an electron transport layer and a top electrode which are sequentially stacked;
wherein the substrate is made of glass or flexible plastic materials; the transparent conducting layer is a transparent electrode, and the transparent conducting layer and the substrate are integratedSetting; the hole transport layer is made of an organic material or an inorganic material and is used for transporting holes to the transparent electrode; the light absorption layer is a photovoltaic material with a perovskite structure and is used for absorbing incident light; the electron transport layer is made of metal oxide, PCBM, C60A material having an excellent electron conduction effect for transporting electrons and isolating the light absorbing layer and the top electrode; the top electrode is a material having a higher work function.
Further, the transparent electrode is Indium Tin Oxide (ITO), Fluorine Tin Oxide (FTO), or Aluminum Zinc Oxide (AZO).
Further, the thickness of the hole transport layer is 50 nm-300 nm; the inorganic material is metal oxide, and the organic material is PEDOT, PSS, Spiro-MeOTAD, PTAA, P3HT, NPB and the like.
Furthermore, the thickness of the light absorption layer is 200 nm-400 nm and the light absorption layer is composed of compact crystal grains of perovskite materials.
Furthermore, the thickness of the electron transmission layer is 10 nm-100 nm.
Further, the top electrode may be a metal such as gold, silver, copper, aluminum, or a conductive carbon material.
In another aspect, there is provided a method of fabricating a perovskite solar cell, for fabricating the perovskite solar cell described above, the method comprising the steps of:
sequentially carrying out ultrasonic cleaning on the substrate for a preset time in deionized water, acetone and ethanol, drying and cleaning for a preset time through ozone plasma;
preparing a hole transport layer film on a substrate by using a spin coating mode, and carrying out high-temperature annealing operation on the formed film at 100 ℃ to form a hole transport layer with a preset thickness;
spin-coating a precursor solution on the hole transport layer, and dripping a quantitative anti-solvent through a dropper in the spin-coating process for washing to form a light absorption layer;
forming an electron transmission layer on the light absorption layer in a spin coating mode, and placing the electron transmission layer on a 70 ℃ hot table for annealing treatment;
and (3) placing the substrate sequentially laminated with the hole transport layer, the light absorption layer and the electron transport layer in a vacuum plating cavity with set vacuum degree to deposit the top electrode through thermal evaporation.
Further, the substrate is subjected to ultrasonic cleaning in the deionized water, acetone and ethanol for 10min to 20min respectively, and is cleaned in the ozone plasma for 3min to 5 min.
Further, the preparation of the light absorbing layer comprises a first stage: carrying out spin coating operation on the precursor solution at the speed of 900-1100 rpm, and carrying out a second stage: and dropwise adding the anti-solvent at the speed of 4000-6000 rpm.
Further, the angle between the dropper and the substrate is kept between 40 degrees and 50 degrees.
In the invention, a light absorption layer in the perovskite solar cell is prepared by using a photovoltaic material with a perovskite structure, and in the preparation of the light absorption layer, a spin coating mode is used, and a white mirror thin film layer different from a traditional brown thin film layer, namely the light absorption layer, is finally obtained by an anti-solvent cleaning process in the spin coating process; compared with the prior art, the invention has the beneficial effects that: the white mirror surface thin film layer formed in the invention has a multilayer laminated structure and has fewer horizontal crystal boundaries; the method is beneficial to the transmission of current carriers, and achieves the effects of improving the short-circuit current and the energy conversion efficiency of the perovskite solar cell.
Drawings
FIG. 1 is a schematic diagram of the structural composition of a perovskite solar cell of the present invention;
FIG. 2 is a block diagram of a perovskite solar cell fabrication process of the present invention;
FIG. 3 is a schematic comparison of a light-absorbing layer film preparation process of the present invention and a conventional light-absorbing layer film preparation process;
FIG. 4 is a schematic representation of a comparison of a photograph of a perovskite thin film in a light absorbing layer of the present invention with a photograph of a perovskite thin film in a conventional light absorbing layer;
FIG. 5 is a schematic SEM topography comparing perovskite thin film in light absorbing layer of the present invention with perovskite thin film in conventional light absorbing layer
Fig. 6 is a schematic voltage-current density test curve of the perovskite solar cell of the present invention and a conventional perovskite solar cell.
Detailed Description
In order to make the technical solutions of the present invention better understood, the technical solutions in the embodiments of the present invention will be clearly and completely described below with reference to the drawings in the embodiments of the present invention. It is to be understood that the described embodiments are merely illustrative of some, but not all, of the embodiments of the invention, and that the preferred embodiments of the invention are shown in the drawings. This invention may be embodied in many different forms and should not be construed as limited to the embodiments set forth herein, but rather should be construed as broadly as the present disclosure is set forth in order to provide a more thorough understanding thereof. 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.
Referring to fig. 1, in an embodiment of the present invention, in one aspect, there is provided a perovskite solar cell, the cell including a substrate 1, a transparent conductive layer 2, a hole transport layer 3, a light absorbing layer 4, an electron transport layer 5, and a top electrode 6, which are sequentially stacked; wherein, the substrate 1 is made of glass or flexible plastic material; the transparent conducting layer 2 is a transparent electrode, the transparent electrode is Indium Tin Oxide (ITO), Fluorine Tin Oxide (FTO) or Aluminum Zinc Oxide (AZO), and the transparent conducting layer 2 and the substrate 1 are integrally arranged; the hole transport layer 3 is made of organic material or inorganic material and is used for transporting holes to the transparent electrode, specifically, the thickness of the hole transport layer 3 is 50 nm-300 nm, and the inorganic material is metal oxide such as CuO and NiO2CuO, etc., organic materials PEDOT, PSS, Spiro-MeOTAD, PTAA, P3HT, NPB, etc.; the light absorption layer 4 is a photovoltaic material with a perovskite structure and used for absorbing incident light, the thickness of the light absorption layer 4 is 200 nm-400 nm, and the light absorption layer is composed of compact crystal grains of the perovskite material, specifically methyl lead triiodide perovskite CH3NH3PbI3（MAPbI3) The surface is a white mirror surface; the electron transport layer 5 is metal oxide, PCBM, C60Etc. having an excellent electron transfer effect for transferring electrons and isolating the light absorbing layer 4 and the top electrode 6,the thickness of the electron transmission layer 5 is 10 nm-100 nm; the top electrode 6 is made of a material having a high work function, and may be made of a metal such as gold, silver, copper, or aluminum, or a conductive carbon material.
Referring to fig. 6, a voltage-current density comparison curve of the perovskite solar cell of the present invention and the perovskite solar cell of the prior art is schematically shown, from which it is clear that the perovskite solar cell provided by the present invention has higher short circuit current and energy conversion efficiency compared to the perovskite solar cell of the prior art.
On the other hand, referring to fig. 2, an embodiment of the present invention provides a method for manufacturing a perovskite solar cell, for manufacturing the perovskite solar cell, the method including the steps of:
s1: sequentially carrying out ultrasonic cleaning on the substrate for a preset time in deionized water, acetone and ethanol, drying and cleaning by ozone plasma;
in the embodiment of the invention, in order to ensure that the prepared perovskite solar cell has good performance, the substrate needs to be cleaned before preparation, and specifically, the substrate 1 is also provided with a layer of transparent electrode; putting the substrate 1 laminated with the transparent electrode into deionized water, acetone and ethanol for ultrasonic cleaning in sequence, wherein each cleaning agent needs to be cleaned for 10-20 min and can be selected according to actual conditions; in this embodiment, the cleaning time is preferably 20 min; after cleaning, putting the mixture into a vacuum environment for drying treatment to remove the detergent; and finally, cleaning for 3-5 min by using ozone plasma to remove organic impurities on the surface, and drying and treating by using ozone plasma to facilitate subsequent preparation of the hole transport layer 3.
Preferably, in the present embodiment, the thickness of the transparent conductive layer 2 is 150nm to 200 nm.
S2: preparing a hole transport layer film on a substrate by using a spin coating mode, and carrying out high-temperature annealing operation on the formed film at 100 ℃ to form a hole transport layer with a preset thickness;
specifically, after ultrasonic cleaning, drying and ozone plasma cleaning are carried out on the substrate 1, a hole transport layer 3 is prepared on the transparent conducting layer 2 in a spin coating mode; in this example, the spin-coating of PEDOT: the PSS solution is exemplified, wherein the spin coating speed is 2000rpm, by which the ratio of PEDOT: the PSS solution uniformly forms a thin film layer on the transparent conductive layer 2; then, the film is put into a vacuum environment, the temperature is controlled at 100 ℃, and high-temperature annealing treatment is carried out for 20min, so that the hole transport film layer with the thickness of 20nm, which is preferred by the invention, is finally formed.
S3: spin-coating a precursor solution on the hole transport layer, and dripping a quantitative anti-solvent through a dropper in the spin-coating process for washing to form a light absorption layer;
in this embodiment, the hole transport layer 4 is prepared by combining a precursor solution and an anti-solvent, and is specifically prepared by: firstly, a preset amount of precursor solution is taken, and MAPbI is preferably selected3As the precursor solution in the embodiment of the invention, the prepared precursor solution is spin-coated on the hole transport layer 3 at the speed of 900 rpm-1100 rpm, after 15s, the spin-coating speed is adjusted to 4000 rpm-6000 rpm, and MAPbI is added3Dripping an antisolvent toluene into the precursor solution through a dropper for washing, specifically: the dropping amount of the toluene is 600 mu l, the dropping time is ensured to be 0.4 s-0.6 s in the dropping process, the angle between a dropper and the substrate 1 is kept in the range of 40-50 degrees, and after 25s, the spin coating operation is stopped to form a light absorption layer; similarly, a drying operation is finally performed to remove the solution remaining after spin coating.
In the present invention, the anti-solvent may be toluene, chlorobenzene, diethyl ether, etc., which is not limited and fixed in the present invention, and may be selected according to actual circumstances.
Referring to fig. 3, the angle between the substrate 1 and the dip tube when the antisolvent is dropped in the preparation of the light absorbing layer 4 according to the present invention is compared with the angle between the substrate 1 and the dip tube in the prior art, from which it can be seen that the angle between the substrate 1 and the dip tube in the prior art is 90 °, the antisolvent is dropped in the manner that the dip tube makes an angle of 45 ° with the substrate 1 according to the present invention; as can be seen from a comparison between fig. 4 and fig. 5, the light absorbing layer 4 prepared by the present invention has a multi-layered structure with fewer horizontal grain boundaries, and is a white mirror film.
S4: forming an electron transmission layer on the light absorption layer in a spin coating mode, and placing the electron transmission layer on a 70 ℃ hot table for annealing treatment;
in the present embodiment, PC is selected61BM is used as a preparation material of the electron transport layer 5, and a thin film layer is formed by spin coating, specifically, PC is spin-coated at 3000rpm6120s BM material, adjusting the speed to 6000rpm, spin-coating for 20s, and annealing at 70 deg.C for 60min on a hot stage for the purpose of removing the residual PC61BM is removed, so that the dryness is ensured, on one hand, the subsequent preparation of the top electrode 6 is facilitated, and on the other hand, the performance of the final perovskite solar cell finished product can be improved.
S5: and (3) placing the substrate sequentially laminated with the hole transport layer, the light absorption layer and the electron transport layer in a vacuum plating cavity with set vacuum degree to deposit the top electrode through thermal evaporation.
After the hole transmission layer, the light absorption layer and the electron transmission layer are sequentially prepared, the top electrode 6 is finally prepared, and the top electrode 6 is required to be placed at 3 x 10-4Sequentially thermally evaporating BCP with the thickness of 10nm and Ag with the thickness of 150nm in a vacuum environment of Pa to form an effective area of 0.096cm2A top electrode 6 of size.
The light absorption layer of the perovskite solar cell formed finally by the perovskite solar cell preparation method provided by the invention is a white mirror film, and the crystal grains of the white mirror film are of a multilayer laminated structure, so that the perovskite solar cell preparation method is beneficial to carrier transmission and can improve the energy conversion efficiency of the cell.
In the invention, a photovoltaic material with a perovskite structure is used for preparing a light absorption layer in a perovskite solar cell; in the preparation of the light absorption layer, a spin coating mode is used, and a white mirror surface thin film layer different from the traditional brown thin film layer, namely the light absorption layer, is finally obtained through an anti-solvent cleaning process in the spin coating process; compared with the prior art, the invention has the beneficial effects that: the white mirror surface thin film layer formed in the invention has a multilayer laminated structure and has fewer horizontal crystal boundaries; the method is beneficial to the transmission of current carriers, and achieves the effects of improving the short-circuit current and the energy conversion efficiency of the perovskite solar cell.
Although the present invention has been described in detail with reference to the foregoing embodiments, it will be apparent to those skilled in the art that modifications may be made to the embodiments described in the foregoing detailed description, or equivalent changes may be made in some of the features of the embodiments described above. All equivalent structures made by using the contents of the specification and the attached drawings of the invention can be directly or indirectly applied to other related technical fields, and are also within the protection scope of the patent of the invention.
Claims (8)
1. A method of fabricating a perovskite solar cell, for fabricating a perovskite solar cell, the method comprising the steps of:
sequentially carrying out ultrasonic cleaning on the substrate for a preset time in deionized water, acetone and ethanol, drying and cleaning for a preset time through ozone plasma;
preparing a hole transport layer film on a substrate by using a spin coating mode, and carrying out high-temperature annealing operation on the formed film at 100 ℃ to form a hole transport layer with a preset thickness;
spin-coating a precursor solution on the hole transport layer, and dripping a quantitative anti-solvent through a dropper in the spin-coating process for washing to form a light absorption layer, wherein the dripping time is ensured to be 0.4 s-0.6 s in the dripping process, and the angle between the dropper and the substrate is kept at 40-50 degrees;
forming an electron transmission layer on the light absorption layer in a spin coating mode, and placing the electron transmission layer on a 70 ℃ hot table for annealing treatment;
a substrate which is sequentially laminated with a hole transmission layer, a light absorption layer and an electron transmission layer is placed in a vacuum plating cavity with set vacuum degree, and a top electrode is deposited through thermal evaporation;
the perovskite solar cell comprises a substrate, a transparent conducting layer, a hole transport layer, a light absorption layer and electrons which are sequentially stackedA transmission layer and a top electrode; wherein the substrate is made of glass or flexible plastic material; the transparent conducting layer is a transparent electrode and is integrally arranged with the substrate; the hole transport layer is made of an organic material or an inorganic material and is used for transporting holes to the transparent electrode; the light absorption layer is a photovoltaic material with a perovskite structure and is used for absorbing incident light; the electron transport layer is made of metal oxide, PCBM, C60Any one of materials having an excellent electron-conducting effect for transporting electrons and isolating the light-absorbing layer and the top electrode; the top electrode is made of a material with a higher work function; the light absorption layer is a white mirror perovskite film and has a multilayer laminated compact grain structure.
2. The method for preparing a perovskite solar cell according to claim 1, wherein the substrate is subjected to ultrasonic cleaning in deionized water, acetone and ethanol for 10-20 min and ozone plasma cleaning for 3-5 min.
3. The method of claim 1, wherein the step of forming the light absorbing layer comprises a first stage of: carrying out spin coating operation on the precursor solution at the speed of 900-1100 rpm, and carrying out a second stage: and dropwise adding the anti-solvent at the speed of 4000-6000 rpm.
4. The method of claim 1, wherein the transparent electrode is Indium Tin Oxide (ITO), Fluorine Tin Oxide (FTO), or Aluminum Zinc Oxide (AZO).
5. The method for preparing a perovskite solar cell according to claim 1, wherein the thickness of the hole transport layer is 50nm to 300 nm; the inorganic material is metal oxide, and the organic material is PEDOT: PSS, Spiro-MeOTAD, PTAA, P3HT, NPB.
6. The method for manufacturing a perovskite solar cell as claimed in claim 1, wherein the light absorbing layer has a thickness of 200nm to 400nm and is composed of dense crystal grains of perovskite material.
7. The method for preparing a perovskite solar cell according to claim 1, wherein the thickness of the electron transport layer is 10nm to 100 nm.
8. The method of claim 1, wherein the top electrode is made of a conductive carbon material or any one of gold, silver, copper, and aluminum.
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| CN116914031A (en) * | 2023-09-11 | 2023-10-20 | 西安电子科技大学 | Preparation method of semitransparent and trans-type all-inorganic perovskite solar cell |
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