CN112038420A - Broadband double-layer anti-reflection coating for improving efficiency of solar cell and preparation method thereof - Google Patents
Broadband double-layer anti-reflection coating for improving efficiency of solar cell and preparation method thereof Download PDFInfo
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- H—ELECTRICITY
- H01—ELECTRIC ELEMENTS
- H01L—SEMICONDUCTOR DEVICES NOT COVERED BY CLASS H10
- H01L31/00—Semiconductor devices sensitive to infrared radiation, light, electromagnetic radiation of shorter wavelength or corpuscular radiation and specially adapted either for the conversion of the energy of such radiation into electrical energy or for the control of electrical energy by such radiation; Processes or apparatus specially adapted for the manufacture or treatment thereof or of parts thereof; Details thereof
- H01L31/02—Details
- H01L31/0216—Coatings
- H01L31/02161—Coatings for devices characterised by at least one potential jump barrier or surface barrier
- H01L31/02167—Coatings for devices characterised by at least one potential jump barrier or surface barrier for solar cells
- H01L31/02168—Coatings for devices characterised by at least one potential jump barrier or surface barrier for solar cells the coatings being antireflective or having enhancing optical properties for the solar cells
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- H—ELECTRICITY
- H01—ELECTRIC ELEMENTS
- H01L—SEMICONDUCTOR DEVICES NOT COVERED BY CLASS H10
- H01L31/00—Semiconductor devices sensitive to infrared radiation, light, electromagnetic radiation of shorter wavelength or corpuscular radiation and specially adapted either for the conversion of the energy of such radiation into electrical energy or for the control of electrical energy by such radiation; Processes or apparatus specially adapted for the manufacture or treatment thereof or of parts thereof; Details thereof
- H01L31/18—Processes or apparatus specially adapted for the manufacture or treatment of these devices or of parts thereof
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- Y—GENERAL TAGGING OF NEW TECHNOLOGICAL DEVELOPMENTS; GENERAL TAGGING OF CROSS-SECTIONAL TECHNOLOGIES SPANNING OVER SEVERAL SECTIONS OF THE IPC; TECHNICAL SUBJECTS COVERED BY FORMER USPC CROSS-REFERENCE ART COLLECTIONS [XRACs] AND DIGESTS
- Y02—TECHNOLOGIES OR APPLICATIONS FOR MITIGATION OR ADAPTATION AGAINST CLIMATE CHANGE
- Y02E—REDUCTION OF GREENHOUSE GAS [GHG] EMISSIONS, RELATED TO ENERGY GENERATION, TRANSMISSION OR DISTRIBUTION
- Y02E10/00—Energy generation through renewable energy sources
- Y02E10/50—Photovoltaic [PV] energy
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Abstract
The invention discloses a broadband double-layer anti-reflection coating for improving the efficiency of a solar cell and a preparation method thereof. The broadband double-layer anti-reflection coating for improving the efficiency of the solar cell comprises a bottom layer anti-reflection coating and a top layer anti-reflection coating; the bottom layer anti-reflection coating is formed by curing bottom layer anti-reflection coating containing linear silicon dioxide polymer; the top anti-reflection coating is formed by curing a top anti-reflection coating formed by mixing modified mesoporous silica dispersion liquid and fluorinated silica polymer solution. The broadband double-layer anti-reflection coating for improving the efficiency of the solar cell can achieve a good anti-reflection effect in all visible light bands, is firmly bonded with a glass substrate, has good hydrophobicity and durability, and can effectively improve the efficiency of various solar cell devices; the preparation method of the broadband double-layer anti-reflection coating for improving the efficiency of the solar cell is simple and has good repeatability.
Description
Technical Field
The invention relates to the technical field of optical coating preparation, in particular to a broadband double-layer anti-reflection coating for improving the efficiency of a solar cell and a preparation method thereof.
Background
Solar cells are widely studied in the scientific research and industrial production fields as the most promising approach to the utilization of clean energy. In addition to the most commercialized silicon solar cells, organic cells and perovskite cells have attracted much attention due to their rapid development. The problem of how to improve the energy conversion efficiency of the solar cell is the first challenge for scientists.
On the one hand, scientists have looked for new active layer materials or employed interface modification to reduce defects or suppress energy loss in devices, starting from chemical molecular design. Although there have been some encouraging reports, the loss of light reflection at the outer surface of the solar cell has not been addressed accordingly, which is still a significant impediment to further improvements in solar cell efficiency. Therefore, a light management method is developed, and the light management method can improve the short-circuit current by reducing light reflection and improving light absorption of the solar cell, thereby improving the efficiency of the solar cell. However, the method is usually realized by preparing a plating layer by etching, evaporation, electron sputtering or other methods, so that the method is expensive, complicated to operate and difficult to prepare on a large scale.
The preparation of the mesoporous silica nanoparticle antireflection layer by a solution method is another efficient light management scheme. However, the single antireflection layer that has been widely used at present has the following disadvantages: firstly, the anti-reflection effect cannot meet the anti-reflection effect of the whole visible light wave band, so that the improvement on the efficiency of the solar cell is limited; secondly, the hydrophilicity of the mesoporous silicon dioxide causes the environmental stability of the mesoporous silicon dioxide to be weaker in the using process; thirdly, the coating has weak adhesion with the glass substrate, and the coating is easy to damage; all of the above problems result in limited efficiency of the coating, limiting its application to solar cells.
Disclosure of Invention
The invention aims to overcome the technical defects, provides a broadband double-layer anti-reflection coating for improving the efficiency of a solar cell and a preparation method thereof, and solves the technical problem that a single-layer anti-reflection film in the prior art has poor anti-reflection effect in the whole visible light band.
In order to achieve the technical purpose, the invention provides a broadband double-layer anti-reflection coating for improving the efficiency of a solar cell, which comprises a bottom layer anti-reflection coating and a top layer anti-reflection coating; the bottom layer anti-reflection coating is formed by curing bottom layer anti-reflection coating containing linear silicon dioxide polymer; the top anti-reflection coating is formed by curing a top anti-reflection coating formed by mixing modified mesoporous silica dispersion liquid and fluorinated silica polymer solution.
The second aspect of the invention provides a preparation method of a broadband double-layer anti-reflection coating for improving the efficiency of a solar cell, which comprises the following steps:
coating the bottom anti-reflection coating on the surface of the substrate, and curing to form a bottom anti-reflection coating;
coating the top anti-reflection coating on the surface of the bottom anti-reflection coating, and curing to obtain a broadband double-layer anti-reflection coating for improving the efficiency of the solar cell;
the preparation method of the broadband double-layer anti-reflection coating for improving the efficiency of the solar cell provided by the second aspect of the invention is used for preparing the broadband double-layer anti-reflection coating for improving the efficiency of the solar cell provided by the first aspect of the invention.
Compared with the prior art, the invention has the beneficial effects that:
the broadband double-layer anti-reflection coating for improving the efficiency of the solar cell can achieve a good anti-reflection effect in all visible light bands, is firmly bonded with a glass substrate, has good hydrophobicity and durability, and can effectively improve the efficiency of various solar cell devices.
The preparation method of the broadband double-layer anti-reflection coating for improving the efficiency of the solar cell is simple and has good repeatability.
Drawings
FIG. 1 is a process flow diagram of an embodiment of a method for preparing a broadband double-layer anti-reflection coating for improving the efficiency of a solar cell provided by the invention;
in FIG. 2, a-c are AFM images of glass coated with only the bottom antireflective coating, glass coated with only the top antireflective coating, and glass coated with two antireflective coatings, corresponding to example 1, d-e are SEM images of glass coated with only the bottom antireflective coating and glass coated with two antireflective coatings, corresponding to example 1, and the inset in FIG. e is a static contact angle plot of a water droplet in the double antireflective coating coated glass obtained in example 1;
FIG. 3, a, is a graph of transmission for a blank glass, a glass coated with only a top antireflective coating, a glass coated with a dual layer antireflective coating, and a software-simulated dual layer antireflective coating corresponding to example 1; b is a reflectivity graph of the corresponding blank glass, the glass coated with only the top anti-reflection coating, the glass coated with the double anti-reflection coating and the software simulation double anti-reflection coating in the example 1; c is a transmittance graph of the dual anti-reflection coating obtained in example 1 before and after being placed in air for three months;
FIG. 4 shows a: J-V plot, b: EQE diagram, c: PCE bar graph, d: j. the design is a squareSCBar graph, e: FF bar graph and f: vOCBar graph;
FIG. 5 shows uncoated anti-reflective coating, top anti-reflective coating only, and a double anti-reflective coating (FAPBI) for example 13)x(MAPbBr3)1-xA of the device: J-V plot, b: EQE diagram, c: PCE bar graph, d: j. the design is a squareSCBar graph, e: FF bar graph and f: vOCBar graph.
Detailed Description
In order to make the objects, technical solutions and advantages of the present invention more apparent, the present invention is described in further detail below with reference to the accompanying drawings and embodiments. It should be understood that the specific embodiments described herein are merely illustrative of the invention and are not intended to limit the invention.
The invention provides a broadband double-layer anti-reflection coating for improving the efficiency of a solar cell, which comprises a bottom anti-reflection coating and a top anti-reflection coating, wherein the bottom anti-reflection coating is formed by curing a bottom anti-reflection coating containing a linear silicon dioxide polymer, and the top anti-reflection coating is formed by curing a top anti-reflection coating formed by mixing a modified mesoporous silicon dioxide dispersion solution and a fluorinated silicon dioxide polymer solution. In the invention, the bottom anti-reflection coating is prepared by the bottom anti-reflection coating containing the linear silicon dioxide polymer, so that the bonding strength between the bottom anti-reflection coating and the substrate and between the bottom anti-reflection coating and the top anti-reflection coating is improved, the coating is not easy to fall off, and the anti-reflection coating is matched with the top anti-reflection coating to improve the anti-reflection effect of the visible light in all wave bands; by adopting the top anti-reflection coating formed by mixing the modified mesoporous silica dispersion liquid and the fluorinated silica polymer solution, on one hand, the top anti-reflection coating can be matched with the bottom anti-reflection coating to improve the anti-reflection effect of the visible light in all bands, on the other hand, the formed broadband double-layer anti-reflection coating has low surface energy and higher hydrophobicity, can still maintain the anti-reflection effect of the coating after being placed in the air for a long time, and improves the stability; according to the invention, the refractive index of the top anti-reflection coating can be effectively regulated and controlled by controlling the addition of the modified mesoporous silica dispersion liquid and the fluorinated silica polymer solution, and the obtained top anti-reflection coating has better hydrophobicity.
In the invention, the refractive index of the bottom anti-reflection coating at 550nm is 1.41-1.43, and the refractive index of the top anti-reflection coating at 550nm is 1.20-1.22; the thickness of the bottom anti-reflection coating is 90-100 nm, and the thickness of the top anti-reflection coating is 110-120 nm. Within the above range, the refractive index of the two antireflection films satisfies
The optical thickness also meets lambda/4, and the formed double-layer anti-reflection coating can obtain the anti-reflection effect of wide wavelength.
In the embodiment, the bottom layer anti-reflection coating is prepared from isopropanol, hydrochloric acid with a molar concentration of 0.05-0.2 mol/L and tetraethoxysilane, and the volume ratio of the isopropanol to the hydrochloric acid to the tetraethoxysilane is 1: (0.02-0.03): (0.05-0.2). According to the raw material ratio, the concentration of the linear silicon dioxide polymer in the bottom layer anti-reflection coating is 2.3-4.6 wt%. Further, the hydrochloric acid concentration is 0.1mol/L, and the volume ratio of isopropanol, hydrochloric acid and ethyl orthosilicate is 1: 0.025: 0.1.
in the embodiment, in the top anti-reflection coating, the fluorinated silica polymer solution is prepared from isopropanol, fluorosilane and hydrochloric acid with a concentration of 0.05-0.2 mol/L, and the volume ratio of the isopropanol, fluorosilane and hydrochloric acid is 1: (0.05-0.07): (0.02-0.03), further, the concentration of hydrochloric acid is 0.1mol/L, and the volume ratio of isopropanol, fluorosilane and hydrochloric acid is 1: 0.06: 0.025; the modified mesoporous silica dispersion liquid is prepared by stirring and reacting isopropanol, concentrated hydrochloric acid, Hexamethyldisiloxane (HMDS) and mesoporous silica dispersion liquid with the mass fraction of 1-3 wt%, centrifuging and dispersing into isopropanol, wherein the concentration of the modified mesoporous silica dispersion liquid is 1-3 wt%. Specifically, the fluorosilane is one or two of 1H,1H,2H, 2H-perfluorooctyltriethoxysilane, 1H,2H, 2H-perfluorodecyltriethoxysilane and vinyl tris (2,2, 2-trifluoro) ethoxysilane, and the particle size of the modified mesoporous silica is 20-30 nm. In the experimental process, the inventor finds that if the modified mesoporous silica dispersion liquid and the linear silica polymer solution are directly mixed to prepare the top anti-reflection coating, the requirements on the refractive index and the hydrophobicity can not be simultaneously met, and the formed coating has poor durability. In the invention, the fluorosilane is adopted to replace TEOS, so that the hydrophobicity of the coating is not reduced on the premise of adjusting the refractive index of the mesoporous silica, thereby improving the durability of the coating in the air. Further, the volume ratio of the fluorinated silica polymer solution to the modified mesoporous silica dispersion is 1: (1-5), preferably 1: (2-4). Within the proportion range, the obtained broadband double-layer anti-reflection coating has a good anti-reflection effect on the whole visible light waveband. Further, in the preparation process of the modified mesoporous silica dispersion liquid, in the stirring reaction process, the volume ratio of isopropanol, concentrated hydrochloric acid, hexamethyldisiloxane and the mesoporous silica dispersion liquid with the mass fraction of 1-3 wt% is 1: (0.3-0.4): (0.85-0.9): (2.5-3). Furthermore, the mesoporous silica is obtained by mixing and reacting Cetyl Trimethyl Ammonium Bromide (CTAB), Triethanolamine (TEA), ethyl orthosilicate and water, removing a template, centrifuging and cleaning. In the step, the molar ratio of ethyl orthosilicate to hexadecyl trimethyl ammonium bromide to triethanolamine to water is 1: (0.1-0.3): (0.05-0.1): (100-200). Furthermore, the molar ratio of the ethyl orthosilicate to the hexadecyl trimethyl ammonium bromide to the triethanolamine to the water is 1: (0.15-0.25): (0.07 to 0.0.08): (150-160).
In the invention, the preparation process of the bottom layer anti-reflection coating specifically comprises the following steps: mixing isopropanol, hydrochloric acid with the molar concentration of 0.05-0.2 mol/L and ethyl orthosilicate, and stirring and reacting at room temperature for 1-3 hours to obtain the bottom anti-reflection layer coating. The preparation process of the top layer anti-reflection coating is as follows: and mixing the modified mesoporous silica dispersion liquid and the fluorinated silica polymer solution to obtain the top layer anti-reflection coating. In the process, the modified mesoporous silica dispersion is obtained by the following steps: stirring isopropanol, concentrated hydrochloric acid and hexamethyldisiloxane at 65-75 ℃ for reaction for 0.4-0.6 h, then adding 1-3 wt% of mesoporous silica dispersion, continuously stirring at 65-75 ℃ for reaction for 0.4-0.6 h, standing, centrifuging, and dispersing into isopropanol to obtain modified mesoporous silica dispersion; the fluorinated silica polymer solution is obtained by the following steps: mixing isopropanol, fluorosilane and hydrochloric acid with the concentration of 0.05-0.2 mol/L, and stirring and reacting for 1-3 h at room temperature to obtain the fluorinated silica polymer solution. Further, the mesoporous silica reaction solution is obtained by the following steps: uniformly mixing a CTAB solution and a TEA solution which are prepared in advance, heating to 65-75 ℃, adding TEOS, stirring and reacting for 0.5-1.5 h, cooling, adding 100-200 ml of dilute hydrochloric acid with the concentration of 0.1-0.2 mol/L, centrifuging, and washing to obtain the mesoporous silica. Wherein the mass concentration of the CTAB solution is 2-3 wt%, and the mass concentration of the TEA solution is 8-12 wt%.
Referring to fig. 1, a second aspect of the present invention provides a method for preparing a broadband double-layer anti-reflection coating for improving efficiency of a solar cell, including the following steps:
s1: coating the bottom anti-reflection coating on the surface of the substrate, and curing to form a bottom anti-reflection coating;
s2: and coating the top anti-reflection coating on the surface of the bottom anti-reflection coating, and curing to obtain the broadband double-layer anti-reflection coating for improving the efficiency of the solar cell.
In the embodiment, the curing temperature is 40-60 ℃, preferably 45-55 ℃; the curing time is 30-60 s, preferably 30-40 s.
In the method, the substrate used is glass, silicon wafer, optical device and the like.
The preparation method of the broadband double-layer anti-reflection coating for improving the efficiency of the solar cell provided by the second aspect of the invention is used for obtaining the broadband double-layer anti-reflection coating for improving the efficiency of the solar cell provided by the first aspect of the invention.
In the invention, unless otherwise specified, all raw materials are purchased and used directly, for example, concentrated hydrochloric acid is directly purchased and has a mass fraction of 36-38%.
Example 1
Synthesizing a bottom layer anti-reflection coating: 2mL of isopropanol and 50 mu L of hydrochloric acid with the molar concentration of 0.1mol/L are taken, 200 mu L of TEOS is added, and stirring is carried out for 2 hours at room temperature, so as to obtain the bottom layer anti-reflection coating. In the process, the concentration of the linear silicon dioxide polymer in the bottom layer anti-reflection coating is 4.6 wt%.
Synthesizing a bottom layer anti-reflection coating: mixing the modified mesoporous silica dispersion liquid and the fluorinated silica polymer solution according to the volume ratio of 2:1 to obtain a bottom layer anti-reflection coating; wherein the content of the first and second substances,
the modified mesoporous silica dispersion is obtained by the following steps: 15g of CTAB solution with a concentration of 2.5 wt.% and 600. mu.L of TEA solution with a concentration of 10 wt.% were added to a 30mL round-bottomed flask, mixed by magnetic stirring while the oil bath was heated to 70 ℃ and 1.2mL of TEOS was added, the reaction was stirred at 70 ℃ for 1H, then stirring was stopped and the temperature was reduced to room temperature (during this process, TEOS, CTAB, TEA and H were added2The molar ratio of O is 1:0.2:0.074:156), then pouring the reaction liquid into a centrifuge tube, adding 100-200 ml of hydrochloric acid with the concentration of 0.1mol/L to generate white floccule, centrifuging and cleaning to obtain mesoporous silica, and then dispersing the obtained mesoporous silica into isopropanol to prepare mesoporous silica dispersion liquid with the concentration of 2 wt%; taking 26.75mL of isopropanol, 9.3mL of concentrated hydrochloric acid and 23.76mL of hexamethyldisiloxane, heating the mixed solution to 70 ℃ under violent magnetic stirring, maintaining the temperature for half an hour, adding 80mL of the mesoporous silica dispersion, stirring for half an hour at 70 ℃, stopping stirring after the reaction is finished, standing for layering, taking the supernatant in a centrifuge tube, and centrifuging to obtain the modified mesoporous disiloxaneSilicon oxide, and finally dispersing the obtained modified mesoporous silicon dioxide into isopropanol to prepare a modified mesoporous silicon dioxide dispersion liquid with the concentration of 2.5 wt%;
the fluorinated silica polymer solution is obtained by the following steps: 2mL of isopropanol, 120 mu L of 1H,1H,2H, 2H-perfluorooctyltriethoxysilane and 50 mu L of hydrochloric acid with the mass concentration of 0.1mol/L are mixed, stirred for 2 hours at room temperature and finally sealed in a reagent bottle; in this step, the concentration of the resulting fluorinated silica polymer solution was 6.76 wt%.
Preparing a broadband double-layer anti-reflection coating: spin-coating 40 μ L of the bottom layer anti-reflection coating on the glass surface at the rotating speed of 3000rpm for 30s, and then heating (about 50 ℃) for 30s to obtain a bottom layer anti-reflection coating; and spin-coating 30 mu L of the top anti-reflection coating on the bottom anti-reflection coating at the rotating speed of 3000rpm for 30s, and then heating (about 50 ℃) for 30s to obtain the double-layer anti-reflection coating. In the step, the refractive index of the obtained bottom anti-reflection coating (ACR1) is 1.41, and the thickness is 95 nm; the resulting top antireflective coating (ACR2) had a refractive index of 1.21 and a thickness of 115 nm.
Example 2
Synthesizing a bottom layer anti-reflection coating: 2mL of isopropanol and 40 mu L of hydrochloric acid with the molar concentration of 0.1mol/L are taken, then 100 mu L of TEOS is added, and stirring is carried out for 1 hour at room temperature, so as to obtain the bottom layer anti-reflection coating. In the process, the concentration of the linear silicon dioxide polymer in the bottom layer anti-reflection coating is 2.3 wt%.
Synthesizing a bottom layer anti-reflection coating: mixing the modified mesoporous silica dispersion liquid and the fluorinated silica polymer solution according to the volume ratio of 4:1 to obtain a bottom layer anti-reflection coating; wherein the content of the first and second substances,
the modified mesoporous silica dispersion is obtained by the following steps: adding 8g of CTAB solution with the mass concentration of 2.5 wt% and 400 mu L of TEA solution with the mass concentration of 10 wt% into a 30mL round-bottom flask, magnetically stirring and mixing, heating the mixture to 65 ℃ through an oil bath, adding 1.2mL TEOS, stirring and reacting at 65 ℃ for 1h, stopping stirring, cooling to room temperature, pouring the reaction liquid into a centrifuge tube, adding 100-200 mL of hydrochloric acid with the concentration of 0.1mol/L to generate white floccule, centrifuging and cleaning to obtain mesoporous silica, dispersing the obtained mesoporous silica into isopropanol, and preparing mesoporous silica dispersion with the concentration of 2 wt%; taking 26.75mL of isopropanol, 8mL of concentrated hydrochloric acid and 22.74mL of hexamethyldisiloxane, heating the mixed solution to 70 ℃ under violent magnetic stirring, maintaining the temperature for half an hour, adding 67mL of the mesoporous silica dispersion, stirring for half an hour at 70 ℃, stopping stirring after the reaction is finished, standing for layering, taking supernatant liquid in a centrifuge tube, centrifuging to obtain modified mesoporous silica, and finally dispersing the obtained modified mesoporous silica into the isopropanol to prepare the modified mesoporous silica dispersion with the concentration of 1 wt%;
the fluorinated silica polymer solution is obtained by the following steps: 2mL of isopropanol, 100 mu L of 1H,1H,2H, 2H-perfluorodecyl triethoxysilane and 40 mu L of hydrochloric acid with the mass concentration of 0.1mol/L are mixed, stirred for 1H at room temperature and finally sealed in a reagent bottle; in this step, the concentration of the resulting fluorinated silica polymer solution was 5.43 wt%.
Preparing a broadband double-layer anti-reflection coating: spin-coating 50 μ L of the bottom layer anti-reflection coating on the glass surface at a rotating speed of 3000rpm for 30s, and then heating (about 50 ℃) for 30s to obtain a bottom layer anti-reflection coating; and spin-coating 40 mu L of the top anti-reflection coating on the bottom anti-reflection coating at the rotating speed of 3000rpm for 30s, and then heating (about 50 ℃) for 30s to obtain the double-layer anti-reflection coating. In the step, the refractive index of the obtained bottom anti-reflection coating is 1.42, and the thickness is 100 nm; the refractive index of the top anti-reflection coating layer was 1.20, and the thickness was 120 nm.
Example 3
Synthesizing a bottom layer anti-reflection coating: 2mL of isopropanol and 60 mu L of hydrochloric acid with the molar concentration of 0.1mol/L are taken, then 150 mu L of TEOS is added, and stirring is carried out for 3 hours at room temperature, so as to obtain the bottom layer anti-reflection coating. In the process, the concentration of the linear silicon dioxide polymer in the bottom layer anti-reflection coating is 3.45 wt%.
Synthesizing a bottom layer anti-reflection coating: mixing the modified mesoporous silica dispersion liquid and the fluorinated silica polymer solution according to the volume ratio of 3:1 to obtain a bottom layer anti-reflection coating; wherein the content of the first and second substances,
the modified mesoporous silica dispersion is obtained by the following steps: adding 23g of CTAB solution with the mass concentration of 2.5 wt% and 800 mu L of TEA solution with the mass concentration of 10 wt% into a 30mL round-bottom flask, magnetically stirring and mixing, heating the mixture to 75 ℃ through an oil bath, adding 1.2mL of TEOS, stirring and reacting at 75 ℃ for 1h, stopping stirring, cooling to room temperature, pouring the reaction liquid into a centrifuge tube, adding 100-200 mL of hydrochloric acid with the concentration of 0.1mol/L to generate white floccule, centrifuging and cleaning to obtain mesoporous silica, dispersing the obtained mesoporous silica into isopropanol, and preparing mesoporous silica dispersion with the concentration of 2 wt%; taking 26.75mL of isopropanol, 10.7mL of concentrated hydrochloric acid and 24.1mL of hexamethyldisiloxane, heating the mixed solution to 70 ℃ under violent magnetic stirring, maintaining the temperature for half an hour, adding 72mL of the mesoporous silica dispersion, stirring for half an hour at 70 ℃, stopping stirring after the reaction is finished, standing for layering, taking supernatant into a centrifuge tube, centrifuging to obtain modified mesoporous silica, and finally dispersing the obtained modified mesoporous silica into the isopropanol to prepare the modified mesoporous silica dispersion with the concentration of 3 wt%;
the fluorinated silica polymer solution is obtained by the following steps: 2mL of isopropanol, 140 mu L of vinyl tri (2,2, 2-trifluoro) ethoxysilane and 60 mu L of hydrochloric acid with the mass concentration of 0.1mol/L are mixed, stirred for 3h at room temperature and finally sealed in a reagent bottle; in this step, the concentration of the resulting fluorinated silica polymer solution was 7.21 wt%.
Preparing a broadband double-layer anti-reflection coating: spin-coating 40 μ L of the bottom layer anti-reflection coating on the glass surface at the rotating speed of 3000rpm for 30s, and then heating (about 50 ℃) for 30s to obtain a bottom layer anti-reflection coating; and spin-coating 30 mu L of the top anti-reflection coating on the bottom anti-reflection coating at the rotating speed of 3000rpm for 30s, and then heating (about 50 ℃) for 30s to obtain the double-layer anti-reflection coating. In the step, the refractive index of the obtained bottom anti-reflection coating is 1.43, and the thickness is 90 nm; the resulting top antireflective coating had a refractive index of 1.22 and a thickness of 110 nm.
AFM, SEM characterization, contact angle test, transmittance, reflectance and stability test were performed on the glass coated with the bottom anti-reflection coating only, the glass coated with the top anti-reflection coating only, and the glass coated with the dual anti-reflection coating in example 1, which were formed by respectively coating the bottom anti-reflection coating and the top anti-reflection coating obtained in example 1 on the surface of the glass, and the results are shown in fig. 2 and fig. 3.
Referring to FIG. 2, a-c in FIG. 2 are AFM images of glass coated with only the bottom antireflective coating, glass coated with only the top antireflective coating, and glass coated with two antireflective coatings for example 1, d-e are SEM images of glass coated with only the bottom antireflective coating and glass coated with two antireflective coatings for example 1, and the inset in FIG. e is a static contact angle image of a water droplet in glass coated with two antireflective coatings for example 1. As can be seen from FIG. 2a, the bottom anti-reflection coating is densely and uniformly coated on the surface of the glass substrate, the roughness of the bottom anti-reflection coating is only 0.3nm, and the coating of the top anti-reflection coating is not influenced; meanwhile, as can be seen from fig. 2e, the HMDS-MSNs spherical nanoparticles are more continuously distributed on the bottom anti-reflection coating, and although the compactness is poor and there are many cavities, the cavities have extremely small sizes which are far lower than the incident wavelength, so that the scattering loss of light is not caused, and the inset at the upper right end shows that the obtained double-layer anti-reflection coating has better hydrophobicity, the water contact angle can reach 132.82 degrees, which indicates that the obtained double-layer anti-reflection coating has better durability. As can be seen in fig. 2b and 2c, the RMS values for both the glass coated with top antireflective coating alone and the glass coated with dual antireflective coatings were about 25nm, indicating that the roughness does not differ significantly between the top antireflective coating applied to the bottom antireflective coating surface and the glass substrate surface directly.
Referring to fig. 3, a in fig. 3 is a graph showing the transmittance of a blank glass, a glass coated with only a top anti-reflection coating, a glass coated with a double anti-reflection coating, and a software simulation double anti-reflection film corresponding to example 1; b is a reflectivity graph of the corresponding blank glass, the glass coated with only the top anti-reflection coating, the glass coated with the double anti-reflection coating and the software simulation double anti-reflection coating in the example 1; and c is a graph of the transmission of the dual layer antireflective coating obtained in example 1 before and after exposure to air for three months. As can be seen from fig. 3a, compared with the blank glass, the glass coated with only the top anti-reflection coating and the glass coated with the double anti-reflection coating both have a transmittance peak value of more than 95% at a wavelength of about 550nm, and the glass coated with the double anti-reflection coating can realize anti-reflection in a wider wavelength range than the glass coated with only the top anti-reflection coating. This is also confirmed by the reflectivity test results in fig. 3 b. 3c, the measured transmittance curve and initial transmittance curve of the glass coated with the double anti-reflection coating after being placed in the air for three months show that the anti-reflection effect of the coating is not influenced although the glass is exposed in the air for a long time, which shows that the obtained double anti-reflection coating has better stability in the air.
The bottom anti-reflection coating obtained in example 1 is spin-coated on the light-receiving surface of the substrate of the organic solar cell, a bottom anti-reflection coating is formed after curing, then a top anti-reflection coating is spin-coated on the surface of the bottom anti-reflection coating, and a double-layer anti-reflection coating is obtained after curing, and the results are shown in table 1 and fig. 4.
The specific flow of the organic solar cell used in this example is as follows:
cleaning the ITO glass: sequentially performing ultrasonic treatment on the ITO glass in deionized water, ethanol and isopropanol for 10min, then blowing the isopropanol on the ITO glass by using nitrogen, drying the ITO glass on a heating table at 100 ℃, and treating the dried ITO glass in an ultraviolet ozone treatment instrument for 15 min;
preparing an electron transport layer: spin-coating a ZnO precursor (prepared by stirring 200mg of zinc acetate dihydrate, 2mL of ethylene glycol monomethyl ether and 56 μ L of ethanolamine for 6 hours) on ITO glass at the rotation speed of 4000rpm-30s, and then annealing at 200 ℃ for 30min to finally obtain a zinc oxide layer with the thickness of about 30 nm;
preparation of the active layer: preparing a chlorobenzene solution (containing 0.5 vol% of DIO) with the concentration of 14mg/mL by PBDB-T: ITIC according to the mass ratio of 1:1 in a glove box, and coating an active layer with the thickness of about 100nm at the rotating speed of 1000 rpm;
preparation of hole transport layer and positive electrode: at 10nm MoO3And 100nm Ag as hole transport layer and anode, respectively, and adding the specific pattern by vacuum evaporation in a vacuum evaporatorPreparing a mask plate;
each ITO glass comprises eight battery sites, and each battery has an area of 2.12mm2Finally, each device must be encapsulated with uv curing agents and a cover slip.
TABLE 1 parameters of PBDB-T ITIC device before and after coating single and double antireflection films
As can be seen from Table 1, the efficiency of the PBDB-T/ITIC device coated with only the top anti-reflection coating can be 10.8%, and the efficiency of the PBDB-T/ITIC device coated with the double anti-reflection coating is increased to 11.1% compared with the PBDB-T/ITIC device not coated with the anti-reflection coating. Referring to FIG. 4, FIG. 4 shows a: J-V plot, b: EQE diagram, c: PCE bar graph, d: JSC bar graph, e: FF bar graph and f: VOC bar graph. As can be seen from FIG. 4a, the current of the device coated with the double anti-reflection coating is slightly larger than that of the device coated with the single anti-reflection coating, as can be seen from FIG. 4b, the response wavelength range of the PBDB-T: ITIC solar cell is 300nm to 800nm, after the film is coated, the photon response of the PBDB-T: ITIC solar cell in the wavelength range of 390nm to 745nm is enhanced, and the double anti-reflection coating has a better effect of increasing the photon response of the solar cell than the single anti-reflection coating (ACR 2). Meanwhile, fig. 4c-4f show bar graphs of photovoltaic parameters of 8 active sites on the same ITO sheet, and it can be seen that the improvement of PCE is JSCCaused by lift, FF and VOCThe coating layer is basically kept unchanged, so that the antireflection coating can uniformly cover the surface of the device and uniformly improve 8 active sites.
The bottom anti-reflection coating obtained in example 1 is spin-coated on the light receiving surface of the substrate of the perovskite solar cell, a bottom anti-reflection coating is formed after curing, then a top anti-reflection coating is spin-coated on the surface of the bottom anti-reflection coating, and a double-layer anti-reflection coating is obtained after curing, and the results are shown in table 2 and fig. 5.
The perovskite solar cell used in the present example is (FAPBI)3)x(MAPbBr3)1-xThe solar cell sequentially comprises the following components from bottom to top: battery cathode (ITO), electron transport layer (SnO)2) The organic light emitting diode comprises an active layer ((FAPBI3) x (MAPBR 3)1-x), a hole transport layer (Spiro-OMeTAD) and an anode (Ag). The specific process of battery preparation is as follows:
cleaning the ITO glass: sequentially performing ultrasonic treatment on the ITO glass in deionized water, ethanol and isopropanol for 10min, then blowing the isopropanol on the ITO glass by using nitrogen, drying the ITO glass on a heating table at 100 ℃, and treating the dried ITO glass in an ultraviolet ozone treatment instrument for 15 min;
preparation of an electron transport layer: under the condition of normal temperature and air, 1015mg of SnCl2·2H2O and 335mg CH4N2S is added into an open container filled with 30mL of deionized water to form milky turbid liquid, and after 1-2 days of uninterrupted magnetic stirring, yellow clear quantum dots SnO are formed2A solution; taking 30 mu L of the quantum dots SnO2The solution is coated on the surface of an ITO substrate in a rotating way at the speed of 3000rpm-30s, the film is placed on a hot bench at the temperature of 200 ℃ for treatment for 60min, and the SnO with a smooth and compact surface is obtained by ultraviolet-ozone treatment for 10min2A film;
preparation of the active layer: coating SnO with NMBF-Cl dimer (fullerene dimer) as a modification layer2On the film; 642.6mg of PbI were weighed in a glove box under nitrogen atmosphere2Dissolving the mixture in a mixed solvent of 940 mu L of DMF and 60 mu L of DMSO, and then placing the mixture on a hot bench at 60 ℃ to be fully stirred and dissolved; formamidine iodide (FAI), methylamine bromide (MABr) and methylamine chloride (MACl) (the mass ratio is 80:5:9) are dissolved in isopropanol solution to prepare mixed solution with the mass concentration of 94 mg/L. The perovskite thin film is prepared by adopting a two-step method, and 30 mu L of PbI is firstly spin-coated at the speed of 2000rpm-30s2And (3) carrying out thermal annealing on the solution on a 70 ℃ hot table for 1min, after the temperature is reduced to room temperature, spin-coating 50 mu L of FAI, MABr and MACl mixed solution at the speed of 2200rpm-15s, transferring the film into air with the humidity of 40% and carrying out heat treatment at the temperature of 150 ℃ for 15min to form the smooth and flat black perovskite film.
Preparation of hole transport layer: preparing a 520mg/mL Li-TFSI acetonitrile solution, dissolving 80mg of Spiro-OMeTAD in 1mL of chlorobenzene, fully dissolving, adding 17.5 mu L of the prepared Li-TFSI acetonitrile solution, and adding 28.5 mu L of 4-tert-butylpyridine (TBP) as a doping agent; coating the uniformly mixed solution on a perovskite film in a spinning mode at the speed of 4000rpm-30s, placing the film after the spinning mode in a glass drier for oxidation for 16h, and scraping redundant parts by a blade after the film is fully oxidized to expose partial ITO electrodes;
preparing an anode: placing ITO glass in a patterned mask plate, placing the patterned mask plate into a film coating machine, and pumping to a vacuum degree of 2 x 10-6Above torr, metal counter electrode is evaporated.
TABLE 2 before and after coating with double layers of antireflection coating (FAPBI)3)x(MAPbBr3)1-xDevice parameters
As can be seen from Table 2, the coating is compatible with uncoated anti-reflection coating (FAPBI)3)x(MAPbBr3)1-xDevices coated with a dual anti-reflective coating (FAPBI)3)x(MAPbBr3)1-xThe efficiency of the device may be 23.9%. Referring to FIG. 5, FIG. 5 shows uncoated anti-reflective coating, top anti-reflective coating only, and double anti-reflective coating (FAPBI) for example 13)x(MAPbBr3)1-xA of the device: J-V plot, b: EQE diagram, c: PCE bar graph, d: JSC bar graph, e: FF bar graph and f: VOC bar graph. It can be seen from fig. 5a that the current for the device with the double anti-reflective coating is significantly increased compared to the device without the anti-reflective coating, and it can be seen from fig. 5b that after coating, (FAPbI) the device with the anti-reflective coating is coated3)x(MAPbBr3)1-xThe photon response of the solar cell is enhanced in the wavelength range of 320nm to 790 nm. Meanwhile, fig. 5c-5f show bar graphs of photovoltaic parameters of 8 active sites on the same ITO sheet, and it can be seen that the improvement of PCE is JSCCaused by lift, FF and VOCRemain substantially unchanged, indicating that the anti-reflection coating can be uniformThe coating covers the surface of the device and uniformly increases 8 active sites.
Compared with the prior art, the invention has the beneficial effects that:
the broadband double-layer anti-reflection coating for improving the efficiency of the solar cell can realize a better anti-reflection effect in all visible light bands, and can effectively improve the light absorption and device conversion efficiency of various solar cells through light management; meanwhile, the mechanical cohesiveness of the coating and the substrate is improved by the glass transition temperature differential design of the double-layer anti-reflection layer material; the water resistance of the coating is improved by the surface low-surface-energy material, and the stability of the coating is good.
The preparation method of the broadband double-layer anti-reflection coating for improving the efficiency of the solar cell is simple and has good repeatability.
The above description is only for the purpose of illustrating the preferred embodiments of the present invention and is not to be construed as limiting the invention, and any modifications, equivalents, improvements and the like that fall within the spirit and principle of the present invention are intended to be included therein.
Claims (10)
1. A broadband double-layer anti-reflection coating for improving the efficiency of a solar cell is characterized by comprising a bottom layer anti-reflection coating and a top layer anti-reflection coating; wherein the content of the first and second substances,
the bottom layer anti-reflection coating is formed by curing bottom layer anti-reflection coating containing linear silicon dioxide polymer;
the top anti-reflection coating is formed by curing a top anti-reflection coating formed by mixing modified mesoporous silica dispersion liquid and fluorinated silica polymer solution.
2. The broadband double-layer anti-reflection coating for improving the efficiency of the solar cell according to claim 1, wherein the bottom anti-reflection coating is prepared from isopropanol, hydrochloric acid with a molar concentration of 0.05-0.2 mol/L and tetraethoxysilane, and the volume ratio of the isopropanol to the hydrochloric acid to the tetraethoxysilane is 1: (0.02-0.03): (0.05-0.2).
3. The broadband double-layer antireflection coating for improving the efficiency of the solar cell according to claim 1, wherein the fluorinated silica polymer solution is prepared from isopropanol, fluorosilane and hydrochloric acid with a concentration of 0.05-0.2 mol/L, and the volume ratio of the isopropanol, fluorosilane and hydrochloric acid is 1: (0.05-0.07): (0.02-0.03).
4. The broadband double-layer antireflection coating for improving the efficiency of the solar cell according to claim 1, wherein the modified mesoporous silica dispersion is prepared by stirring and reacting isopropanol, concentrated hydrochloric acid, hexamethyldisiloxane and a mesoporous silica dispersion with the mass fraction of 1-3 wt%, centrifuging and dispersing into isopropanol.
5. The broadband double-layer antireflection coating for improving the efficiency of the solar cell according to claim 4, wherein in the preparation process of the modified mesoporous silica dispersion, during a stirring reaction, the volume ratio of isopropanol, concentrated hydrochloric acid, hexamethyldisiloxane and the mesoporous silica dispersion with the mass fraction of 1-3 wt% is 1: (0.3-0.4): (0.85-0.9): (2.5-3).
6. The broadband double-layer anti-reflection coating for improving the efficiency of the solar cell according to claim 4, wherein the mesoporous silica is prepared by carrying out mixed reaction on hexadecyl trimethyl ammonium bromide, triethanolamine, ethyl orthosilicate and water, then removing a template, centrifuging and cleaning; the molar ratio of the ethyl orthosilicate to the hexadecyl trimethyl ammonium bromide to the triethanolamine to the water is 1: (0.1-0.3): (0.05-0.1): (100-200).
7. The broadband dual-layer antireflective coating for improving solar cell efficiency according to claim 1, wherein the volume ratio of the fluorinated silica polymer solution to the modified mesoporous silica dispersion is 1: (1-5).
8. The broadband double-layer anti-reflection coating for improving the efficiency of the solar cell according to claim 1, wherein the refractive index of the bottom anti-reflection coating at 550nm is 1.41-1.43, and the refractive index of the top anti-reflection coating at 550nm is 1.20-1.22;
the thickness of the bottom anti-reflection coating is 90-100 nm, and the thickness of the top anti-reflection coating is 110-120 nm.
9. A preparation method of the broadband double-layer antireflection coating for improving the efficiency of the solar cell according to any one of claims 1 to 8, comprising the following steps:
coating the bottom anti-reflection coating on the surface of the substrate, and curing to form a bottom anti-reflection coating;
and coating the top anti-reflection coating on the surface of the bottom anti-reflection coating, and curing to obtain the broadband double-layer anti-reflection coating for improving the efficiency of the solar cell.
10. The method for preparing the broadband double-layer anti-reflection coating for improving the efficiency of the solar cell according to claim 9, wherein the curing temperature is 40-60 ℃ and the curing time is 30-60 s.
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