CN111312904A - High-performance environment-friendly lead-based perovskite solar cell and preparation method thereof - Google Patents
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Abstract
The invention belongs to the field of solar cells, and discloses a high-performance environment-friendly lead-based perovskite solar cell and a preparation method thereof. In the preparation method, a certain amount of chelating agent disodium ethylene diamine tetraacetic acid or 2, 3-dimercaptosuccinic acid is introduced into the lead-based perovskite precursor liquid, so that the crystallinity and crystal orientation of the lead-based perovskite thin film layer can be effectively optimized, the grain boundary of the perovskite thin film is passivated, and the energy conversion efficiency of the perovskite thin film is improved. Meanwhile, when the device is decomposed, the chelating agent can be combined with lead ions in time to form a stable and soluble complex, and after being absorbed by a human body carelessly, the complex can be successfully metabolized by the human body and discharged along with urine, so that the harm to the human body is reduced remarkably finally. The invention is beneficial to the commercial development of perovskite solar cells, and particularly promotes the application of perovskite indoor photovoltaic as energy supply of intelligent household terminals in the time of Internet of things.
Description
Technical Field
The invention belongs to the field of solar cells, and particularly relates to a high-performance environment-friendly lead-based perovskite solar cell and a preparation method thereof.
Background
The energy problem is always the key research problem of the development of the human society, and the research and development of the solar photovoltaic device provides an effective solution for solving the energy shortage required by the development of the human. Among them, perovskite solar thin film cell devices have attracted extensive attention and have been developed rapidly due to their low cost and outstanding photoelectric properties. After a short period of development, the energy conversion efficiency can reach more than 20%. At present, the perovskite solar cell with high performance is mainly based on a lead-based perovskite thin film layer, but due to Pb2+The ions have a certain solubility in water, which has a serious influence on water and soil, and Pb2+The main symptoms of the existence of the traditional Chinese medicine are the harm to the systems of nerves, hematopoiesis, digestion, kidney, cardiovascular and endocrine and the like, and the main pathological change is Pb2+Influence on metal ions and enzyme systems in the human body. At present, non-lead-tin-based perovskites are considered to be ideal substitute materials for lead-based perovskites due to environmental friendliness, but the energy conversion efficiency is still low. Finding high photoelectric performance and environment-friendly photovoltaic materials becomes an application in the photovoltaic field, especially the indoor photovoltaic field.
The lead-based perovskite solar cell is a photovoltaic material which has the most potential to be commercially applied in a large scale at present, and is one of hot spots of research in the energy field at present. However, lead element contained in the lead-based perovskite is easily leaked into air in an ionic form, and harm to human health is caused. Reducing the lead ion content in the perovskite solar cell will in turn significantly affect the energy conversion efficiency of the photovoltaic device. Therefore, further development of a high-performance and environment-friendly lead-based perovskite solar cell has important significance for promoting development of the lead-based perovskite solar cell.
Disclosure of Invention
In order to solve the problems in the prior art, the invention aims to provide a high-performance environment-friendly lead-based perovskite solar cell and a preparation method thereof, a special processing technology is adopted, a certain amount of chelating agent disodium ethylene diamine tetraacetic acid or 2, 3-dimercaptosuccinic acid is introduced into a perovskite precursor solution, and the introduction of the two chelating agents can effectively passivate the crystal boundary of perovskite, enhance the charge transmission characteristic of the perovskite and obviously improve the energy conversion efficiency and stability of the device. Meanwhile, the perovskite decomposition and the lead leakage are caused by long-term use of the device, the chelating agent can be combined with lead ions in time to form a stable and soluble complex, and the complex can be successfully metabolized by a human body and discharged along with urine after being absorbed by the human body carelessly, so that the harm to the human body is remarkably reduced.
In order to achieve the purpose, the invention provides the following technical scheme:
the high-performance environment-friendly lead-based perovskite solar cell is characterized in that a chelating agent is added into the lead-based perovskite solar cell.
Further, the chelating agent is one or two of ethylene diamine tetraacetic acid or 2, 3-dimercaptosuccinic acid.
The preparation method of the lead-based perovskite solar cell comprises the following steps:
(1) processing tin oxide or titanium oxide solution on a substrate base in a mode of a spin coating method, chemical deposition, ink-jet printing or roll-to-roll processing method to form a uniform electron transport layer film;
(2) dissolving lead iodide in a mixed solution of dimethyl sulfoxide and dimethylformamide to form a first solution, and dissolving methyl ether ammonium iodide (FAI), methyl ammonium bromide (MABr), methyl ammonium chloride (MACl) and a chelating agent in isopropanol to form a second solution; carrying out spin coating, ink-jet printing or roll-to-roll processing on the first solution on the electron transmission layer, further depositing a second solution after annealing treatment, and obtaining a lead-based perovskite thin film layer through annealing treatment;
(3) 2,2',7,7' -tetra [ N, N-di (4-methoxyphenyl) amino ] -9,9' -spirobifluorene film is processed on the perovskite film by spin coating, ink-jet printing or roll-to-roll processing, and a uniform hole transport layer is obtained without annealing;
(5) processing the molybdenum trioxide modification layer on the hole transport layer by adopting an ink-jet printing or evaporation method;
(6) and processing the anode electrode on the molybdenum trioxide modification layer by adopting an ink-jet printing or evaporation method.
Further, the substrate base in the step (1) is ITO, FTO transparent glass or a flexible plastic conductive film substrate.
Further, the thickness of the electron transport layer in the step (1) is 40-50 nm.
Further, the annealing temperature after the first solution is spin-coated in the step (2) is 70 ℃, and the time is 1 min; the annealing temperature of the second solution in air is 150 ℃ and the time is 10 min.
Further, the thickness of the lead-based perovskite thin film layer in the step (2) is 300-400 nm.
Further, the thickness of the hole transport layer in the step (4) is 250-350 nm.
Further, the thickness of the molybdenum trioxide modification layer in the step (5) is 8-10 nm.
Further, in the step (6), the anode electrode is Ag, Cu or Au, and the thickness of the electrode is 60-100 nm.
Has the advantages that: compared with the prior art, the invention effectively passivates the crystal boundary of the perovskite, optimizes the crystallization performance, enhances the charge transmission characteristic of the perovskite and obviously improves the energy conversion efficiency and the stability of the lead-based perovskite photovoltaic device by introducing a certain amount of chelating agent disodium ethylene diamine tetraacetate or 2, 3-dimercaptosuccinic acid into the perovskite precursor solution. Meanwhile, perovskite decomposition and lead leakage are caused by long-term use of the device, most lead ions in the device prepared by the method can form stable and soluble complexes, the biotoxicity of the lead ions is reduced, the lead ions can be effectively metabolized after human body contact, and finally the harm to the human body is remarkably reduced. The lead-based perovskite prepared by the method effectively promotes the commercial development of perovskite solar cells, and particularly promotes the application of perovskite indoor photovoltaics of smart home terminals in the era of the Internet of things.
Drawings
Fig. 1 is a schematic structural diagram of a perovskite type solar cell manufactured by the preparation method of the invention.
FIG. 2 is a scanning electron microscope image of different types of perovskite thin films.
Fig. 3 is a diagram of pathological changes of zebra fish after treatment of the zebra fish by different types of perovskite aqueous solutions.
In the figure, 1 is a transparent substrate, 2 is a cathode electrode, 3 is an electron transport layer, 4 is a perovskite thin film, 5 and 6 are hole transport layers, and 7 is an anode electrode.
Detailed Description
Example 1
(1) Providing a fluorine-doped tin oxide (FTO) transparent conductive substrate, and performing standardized cleaning;
(2) 599 mg of lead iodide was dissolved in 1 mL of a mixed solution (volume ratio 5: 95) of dimethyl sulfoxide and dimethylformamide while 70 mg of FAI, 7 mg of MABr, 7 mg of MACl and 1 mg of disodium ethylenediaminetetraacetate were dissolved in 1 mL of isopropanol;
(3) treating FTO with ozone for 30 min, then dropwise adding a tin oxide solution, rotating at the rotation speed of 4000 rpm for 40 s, then annealing at the temperature of 180 ℃ for 30 min to obtain a solidified electron transport layer;
(4) the lead-based perovskite thin film layer is prepared by a two-step method, the lead iodide solution rotates for 30 s at the rotating speed of 1500 rpm, the annealing temperature is 70 ℃, and the time is 1 min. Then adding an isopropanol solution of an ammonium salt of ethylene diamine tetraacetic acid, rotating at the rotating speed of 1700rpm for 30 s, and annealing in the air at the temperature of 150 ℃ for 10 min to obtain a lead-based perovskite thin film layer;
(5) processing the hole transport layer 2,2',7,7' -tetra [ N, N-di (4-methoxyphenyl) amino ] -9,9' -spirobifluorene on the perovskite thin film by a spin coating method, and rotating at the rotating speed of 5000 rpm for 40 s to obtain a uniform hole transport layer thin film;
(6) preparing a hole transport layer molybdenum trioxide with the thickness of 10 nm by adopting an evaporation method;
(7) the cathode electrode Ag is prepared by adopting an evaporation method, and the thickness of the cathode electrode Ag is 100 nm.
Example 2
(1) Providing a fluorine-doped tin oxide (FTO) transparent conductive substrate, and performing standardized cleaning;
(2) 599 mg of lead iodide was dissolved in 1 mL of a mixed solution (volume ratio 5: 95) of dimethyl sulfoxide and dimethylformamide, while 70 mg of FAI, 7 mg of MABr, 7 mg of MACl and 1 mg of 2, 3-dimercaptosuccinic acid were dissolved in 1 mL of isopropanol;
(3) treating FTO with ozone for 30 min, then dropwise adding a tin oxide solution, rotating at the rotation speed of 4000 rpm for 40 s, then annealing at the temperature of 180 ℃ for 30 min to obtain a solidified electron transport layer;
(4) the lead-based perovskite thin film layer is prepared by a two-step method, the lead iodide solution rotates for 30 s at the rotating speed of 1500 rpm, the annealing temperature is 70 ℃, and the time is 1 min. Then adding an isopropanol solution of ammonium salt of 2, 3-dimercaptosuccinic acid, rotating at the rotating speed of 1700rpm for 30 s, and annealing in the air at the temperature of 150 ℃ for 10 min to obtain a lead-based perovskite thin film layer;
(5) processing the hole transport layer 2,2',7,7' -tetra [ N, N-di (4-methoxyphenyl) amino ] -9,9' -spirobifluorene on the perovskite thin film by a spin coating method, and rotating at the rotating speed of 5000 rpm for 40 s to obtain a uniform hole transport layer thin film;
(6) preparing a hole transport layer molybdenum trioxide with the thickness of 10 nm by adopting an evaporation method;
(7) the cathode electrode Ag is prepared by adopting an evaporation method, and the thickness of the cathode electrode Ag is 100 nm.
Example 3
(1) Providing a fluorine-doped tin oxide (FTO) transparent conductive substrate, and performing standardized cleaning;
(2) 599 mg of lead iodide was dissolved in 1 mL of a mixed solution of dimethyl sulfoxide and dimethylformamide (volume ratio 5: 95), while 70 mg of FAI, 7 mg of MABr, 7 mg of MACl, and 10 mg of disodium ethylenediaminetetraacetate were dissolved in 1 mL of isopropanol;
(3) treating FTO with ozone for 30 min, then dropwise adding a tin oxide solution, rotating at the rotation speed of 4000 rpm for 40 s, then annealing at the temperature of 180 ℃ for 30 min to obtain a solidified electron transport layer;
(4) the lead-based perovskite thin film layer is prepared by a two-step method, the lead iodide solution rotates for 30 s at the rotating speed of 1500 rpm, the annealing temperature is 70 ℃, and the time is 1 min. Then adding an isopropanol solution of an ammonium salt of ethylene diamine tetraacetic acid, rotating at the rotating speed of 1700rpm for 30 s, and annealing in the air at the temperature of 150 ℃ for 10 min to obtain a lead-based perovskite thin film layer;
(5) processing the hole transport layer 2,2',7,7' -tetra [ N, N-di (4-methoxyphenyl) amino ] -9,9' -spirobifluorene on the perovskite thin film by a spin coating method, and rotating at the rotating speed of 5000 rpm for 40 s to obtain a uniform hole transport layer thin film;
(6) preparing a hole transport layer molybdenum trioxide with the thickness of 10 nm by adopting an evaporation method;
(7) the cathode electrode Ag is prepared by adopting an evaporation method, and the thickness of the cathode electrode Ag is 100 nm.
Comparative example 1
(1) Providing a fluorine-doped tin oxide (FTO) transparent conductive substrate, and performing standardized cleaning;
(2) 599 mg of lead iodide was dissolved in 1 mL of a mixed solution (volume ratio 5: 95) of dimethyl sulfoxide and dimethylformamide, while 70 mg of methyl ether amine iodide (FAI), 7 mg of methyl ammonium bromide (MABr) and 7 mg of methyl ammonium chloride (MACl) were dissolved in 1 mL of isopropanol;
(3) treating FTO with ozone for 30 min, then dropwise adding a tin oxide solution, rotating at the rotation speed of 4000 rpm for 40 s, then annealing at the temperature of 180 ℃ for 30 min to obtain a solidified electron transport layer;
(4) the lead-based perovskite thin film layer is prepared by a two-step method, the lead iodide solution rotates for 30 s at the rotating speed of 1500 rpm, the annealing temperature is 70 ℃, and the time is 1 min. Then, the isopropanol solution of ammonium salt is rotated for 30 s at the rotating speed of 1700rpm, the annealing temperature in the air is 150 ℃, and the time is 10 min, so that the lead-based perovskite thin film layer is obtained;
(5) processing the hole transport layer 2,2',7,7' -tetra [ N, N-di (4-methoxyphenyl) amino ] -9,9' -spirobifluorene on the perovskite thin film by a spin coating method, and rotating at the rotating speed of 5000 rpm for 40 s to obtain a uniform hole transport layer thin film;
(6) preparing a hole transport layer molybdenum trioxide with the thickness of 10 nm by adopting an evaporation method;
(7) the cathode electrode Ag is prepared by adopting an evaporation method, and the thickness of the cathode electrode Ag is 100 nm.
The performance of the outdoor and indoor solar cells of the above examples is shown in table 1 below:
TABLE 1
By comparing examples 1, 2 and 3, it can be seen that the addition of appropriate concentration (1 mg/mL) of disodium EDTA or 2, 3-dimercaptosuccinic acid can provide better photovoltaic properties, and the excessive concentration (10 mg/mL) will reduce the photovoltaic properties of the device. Meanwhile, the energy conversion efficiency of the low-concentration (1 mg/mL) doped disodium ethylene diamine tetraacetate or 2, 3-dimercaptosuccinic acid is obviously improved compared with that of an undoped device. For both outdoor energy conversion efficiency and indoor conversion efficiency, the device performance of the lead-based perovskite battery is better optimized by the introduction of disodium ethylene diamine tetraacetate or 2, 3-dimercaptosuccinic acid than undoped lead-based perovskite battery.
The perovskite thin film crystal optimization of the above example is shown in fig. 2, and fig. 2 is the scanning electron microscope morphology of different types of perovskite thin films, (a) the crystal morphology of a pure perovskite of comparative example 1, (b) the crystal morphology of a perovskite of example 2 added with 1 mg/mL of 2, 3-dimercaptosuccinic acid, (c) the crystal morphology of a perovskite of example 1 added with 1 mg/mL of disodium ethylenediaminetetraacetate, and (d) the crystal morphology of a perovskite of example 3 added with 10 mg/mL of disodium ethylenediaminetetraacetate. It can be seen from the scanning electron microscope of the comparative example that the growth of the crystal morphology can be promoted no matter the disodium ethylene diamine tetraacetate or the 2, 3-dimercaptosuccinic acid is added, and finally the crystal with better crystallization property is obtained. Meanwhile, if the doping proportion of the disodium ethylene diamine tetraacetate is increased, when the concentration is 10 mg/mL, the appearance of crystals is reduced relative to the appearance of crystals with low concentration of 1 mg/mL. The addition of the chelating agent disodium ethylene diamine tetraacetate or 2, 3-dimercaptosuccinic acid with proper concentration can effectively promote the growth of the crystal film.
The morphology of the treated zebra fish after dissolution of the device in the above examples in an aqueous solution is shown in fig. 3, and fig. 3 shows the lesion morphology of the zebra fish after the treatment of the zebra fish with different types of perovskite aqueous solutions, (a) the morphology of the zebra fish after the treatment of a comparative pure perovskite, (b) the morphology of the zebra fish after the perovskite treatment with 1 mg/mL of 2, 3-dimercaptosuccinic acid added in example 2, (c) the morphology of the zebra fish after the perovskite treatment with 1 mg/mL of disodium ethylenediaminetetraacetate added in example 1, and (d) the morphology of the zebra fish after the perovskite treatment with 10 mg/mL of disodium ethylenediaminetetraacetate added in example 3. The biotoxicological analysis of the perovskite aqueous solution of the comparative example on the zebra fish can show that the zebra fish treated by the original perovskite solution has serious morbidity, curved spine and serious pericardial cyst. And the phenomenon can be effectively relieved by adding the disodium ethylene diamine tetraacetate or the 2, 3-dimercaptosuccinic acid, and finally the zebra fish with lighter morbidity is obtained. When the concentration of the disodium ethylene diamine tetraacetate is increased, the relative disease state of the zebra fish is further relieved. The fact shows that the harm of the perovskite film to the biological toxicity of the environment can be effectively relieved by adding a certain amount of disodium ethylene diamine tetraacetate or 2, 3-dimercaptosuccinic acid.
Claims (10)
1. The high-performance environment-friendly lead-based perovskite solar cell is characterized in that a chelating agent is added into the lead-based perovskite solar cell.
2. The high-performance environment-friendly lead-based perovskite solar cell as claimed in claim 1, wherein the chelating agent is one or a combination of disodium ethylene diamine tetraacetate or 2, 3-dimercaptosuccinic acid.
3. The method for producing a lead-based perovskite solar cell as defined in claim 1 or 2, comprising the steps of:
(1) processing tin oxide or titanium oxide solution on a substrate base in a mode of a spin coating method, chemical deposition, ink-jet printing or roll-to-roll processing method to form a uniform electron transport layer film;
(2) dissolving lead iodide in a mixed solution of dimethyl sulfoxide and dimethylformamide to form a first solution, and dissolving methyl ether ammonium iodide, methyl ammonium bromide, methyl ammonium chloride and a chelating agent in isopropanol to form a second solution; carrying out spin coating, ink-jet printing or roll-to-roll processing on the first solution on the electron transmission layer, further depositing a second solution after annealing treatment, and obtaining a lead-based perovskite thin film layer through annealing treatment;
(3) 2,2',7,7' -tetra [ N, N-di (4-methoxyphenyl) amino ] -9,9' -spirobifluorene film is processed on the perovskite film by spin coating, ink-jet printing or roll-to-roll processing, and a uniform hole transport layer is obtained without annealing;
(5) processing the molybdenum trioxide modification layer on the hole transport layer by adopting an ink-jet printing or evaporation method;
(6) and processing the anode electrode on the molybdenum trioxide modification layer by adopting an ink-jet printing or evaporation method.
4. The preparation method according to claim 3, wherein the substrate base in the step (1) is ITO, FTO transparent glass or a flexible plastic conductive film substrate.
5. The method according to claim 3, wherein the thickness of the electron transport layer in the step (1) is 40 to 50 nm.
6. The method according to claim 3, wherein the annealing temperature after the spin-coating of the first solution in the step (2) is 70 ℃ for 1 min; the annealing temperature of the second solution in air is 150 ℃ and the time is 10 min.
7. The method according to claim 3, wherein the thickness of the lead-based perovskite thin film layer in the step (2) is 300-400 nm.
8. The method as set forth in claim 3, wherein the hole transport layer in step (4) has a thickness of 250-350 nm.
9. The preparation method according to claim 3, wherein the thickness of the molybdenum trioxide modification layer in the step (5) is 8-10 nm.
10. The method according to claim 3, wherein the anode electrode in step (6) is Ag, Cu or Au, and the thickness of the electrode is 60-100 nm.
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CN115117247B (en) * | 2022-06-23 | 2024-04-16 | 中国科学技术大学 | Perovskite solar cell and preparation method thereof |
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