CN109036851B - Graphene-based thin-film solar cell - Google Patents
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- OKTJSMMVPCPJKN-UHFFFAOYSA-N Carbon Chemical compound [C] OKTJSMMVPCPJKN-UHFFFAOYSA-N 0.000 title claims abstract description 135
- 229910021389 graphene Inorganic materials 0.000 title claims abstract description 135
- 239000010409 thin film Substances 0.000 title claims abstract description 18
- 239000010408 film Substances 0.000 claims abstract description 136
- XLYOFNOQVPJJNP-UHFFFAOYSA-N water Substances O XLYOFNOQVPJJNP-UHFFFAOYSA-N 0.000 claims abstract description 28
- 238000000034 method Methods 0.000 claims abstract description 20
- 238000000967 suction filtration Methods 0.000 claims description 11
- XUIMIQQOPSSXEZ-UHFFFAOYSA-N Silicon Chemical compound [Si] XUIMIQQOPSSXEZ-UHFFFAOYSA-N 0.000 claims description 10
- 238000001704 evaporation Methods 0.000 claims description 10
- 229910052710 silicon Inorganic materials 0.000 claims description 10
- 239000010703 silicon Substances 0.000 claims description 10
- 239000012528 membrane Substances 0.000 claims description 9
- 230000008020 evaporation Effects 0.000 claims description 5
- 238000004108 freeze drying Methods 0.000 claims description 5
- 239000000758 substrate Substances 0.000 claims description 5
- 238000006243 chemical reaction Methods 0.000 abstract description 11
- 230000007547 defect Effects 0.000 abstract description 4
- 229910001385 heavy metal Inorganic materials 0.000 abstract description 3
- 238000002834 transmittance Methods 0.000 abstract description 2
- 210000004379 membrane Anatomy 0.000 description 7
- 230000001276 controlling effect Effects 0.000 description 4
- 230000009286 beneficial effect Effects 0.000 description 3
- 238000000089 atomic force micrograph Methods 0.000 description 2
- 210000002469 basement membrane Anatomy 0.000 description 2
- 230000005540 biological transmission Effects 0.000 description 2
- 230000000052 comparative effect Effects 0.000 description 2
- 238000010586 diagram Methods 0.000 description 2
- 230000007613 environmental effect Effects 0.000 description 2
- 238000001914 filtration Methods 0.000 description 2
- TWNQGVIAIRXVLR-UHFFFAOYSA-N oxo(oxoalumanyloxy)alumane Chemical compound O=[Al]O[Al]=O TWNQGVIAIRXVLR-UHFFFAOYSA-N 0.000 description 2
- BASFCYQUMIYNBI-UHFFFAOYSA-N platinum Chemical compound [Pt] BASFCYQUMIYNBI-UHFFFAOYSA-N 0.000 description 2
- VYPSYNLAJGMNEJ-UHFFFAOYSA-N Silicium dioxide Chemical compound O=[Si]=O VYPSYNLAJGMNEJ-UHFFFAOYSA-N 0.000 description 1
- 238000004630 atomic force microscopy Methods 0.000 description 1
- 238000005452 bending Methods 0.000 description 1
- 230000006378 damage Effects 0.000 description 1
- 238000007599 discharging Methods 0.000 description 1
- 230000000694 effects Effects 0.000 description 1
- 230000005611 electricity Effects 0.000 description 1
- 239000007788 liquid Substances 0.000 description 1
- 239000002120 nanofilm Substances 0.000 description 1
- 229910052697 platinum Inorganic materials 0.000 description 1
- 230000001105 regulatory effect Effects 0.000 description 1
- 239000000126 substance Substances 0.000 description 1
- 230000037303 wrinkles Effects 0.000 description 1
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- H01G—CAPACITORS; CAPACITORS, RECTIFIERS, DETECTORS, SWITCHING DEVICES, LIGHT-SENSITIVE OR TEMPERATURE-SENSITIVE DEVICES OF THE ELECTROLYTIC TYPE
- H01G9/00—Electrolytic capacitors, rectifiers, detectors, switching devices, light-sensitive or temperature-sensitive devices; Processes of their manufacture
- H01G9/004—Details
- H01G9/04—Electrodes or formation of dielectric layers thereon
- H01G9/042—Electrodes or formation of dielectric layers thereon characterised by the material
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- B—PERFORMING OPERATIONS; TRANSPORTING
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- B82Y30/00—Nanotechnology for materials or surface science, e.g. nanocomposites
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- H—ELECTRICITY
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- H01G—CAPACITORS; CAPACITORS, RECTIFIERS, DETECTORS, SWITCHING DEVICES, LIGHT-SENSITIVE OR TEMPERATURE-SENSITIVE DEVICES OF THE ELECTROLYTIC TYPE
- H01G9/00—Electrolytic capacitors, rectifiers, detectors, switching devices, light-sensitive or temperature-sensitive devices; Processes of their manufacture
- H01G9/004—Details
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- H01G9/048—Electrodes or formation of dielectric layers thereon characterised by their structure
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- H01—ELECTRIC ELEMENTS
- H01G—CAPACITORS; CAPACITORS, RECTIFIERS, DETECTORS, SWITCHING DEVICES, LIGHT-SENSITIVE OR TEMPERATURE-SENSITIVE DEVICES OF THE ELECTROLYTIC TYPE
- H01G9/00—Electrolytic capacitors, rectifiers, detectors, switching devices, light-sensitive or temperature-sensitive devices; Processes of their manufacture
- H01G9/20—Light-sensitive devices
- H01G9/2059—Light-sensitive devices comprising an organic dye as the active light absorbing material, e.g. adsorbed on an electrode or dissolved in solution
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- 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
- Y02E10/542—Dye sensitized solar cells
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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
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Abstract
The invention discloses a graphene-based thin-film solar cell, which comprises a transparent electrode, wherein the transparent electrode is a graphene thin film, and the thickness of the transparent electrode is not more than 20 nm; the thickness of the graphene film is controlled at a nanometer level by adopting a water transfer method, so that the light transmittance of the film is improved; in the transfer process, micro-folds are introduced, so that the contact area of the film and the photosensitive layer is increased; after high-temperature treatment, the graphene has few defects, the film has high strength, and the flexible electrode can endure stress change in the repeated folding process. The whole process is simple, green and easy to operate. The film is used as a photo-anode, a counter electrode and the like; in comparison, the graphene has higher electron mobility, and the problem of heavy metal pollution does not exist, so that the cost is reduced, and the light conversion efficiency is improved.
Description
Technical Field
The invention relates to a solar cell, in particular to a graphene-based thin-film solar cell.
Background
With the increasing severity of environmental issues, environmental issues arising from the unregulated use of fossil energy sources are attracting increasing attention. People hope to find renewable and pollution-free new energy to replace heavily polluted fossil energy. Solar energy has been a concern of people as a source of the earth statement. Among them is the use of flexible solar cells, which are the photogenerated electronic effect of photosensitive substances, converting light into electricity. However, the conventional solar flexible cell uses ITO as a transparent conductive electrode, and has several problems, one of which is that ITO has a heavy metal pollution problem; secondly, ITO has poor conductivity and low electron mobility, which is not beneficial to the transmission of photoelectrons; and thirdly, the ITO has poor flexibility and is not suitable for being used as a flexible electrode.
Therefore, a graphene film with high strength, high conductivity and high transparency is designed to overcome the above problems of the ITO.
Disclosure of Invention
The invention aims to overcome the defects of the prior art and provides a graphene-based thin-film solar cell.
The purpose of the invention is realized by the following technical scheme: the graphene-based thin-film solar cell comprises a transparent electrode, wherein the transparent electrode is a graphene thin film, the thickness of the transparent electrode is not more than 20nm, and the graphene-based thin-film solar cell is prepared by the following method:
(1) carrying out suction filtration on the AAO base membrane to obtain a graphene oxide membrane;
(2) placing the AAO base film with the graphene film attached to the surface on the water surface with the surface of the graphene oxide film facing upwards; pressing the AAO basement membrane to make the AAO basement membrane sink, the graphene oxide membrane floats on the water surface.
(3) Fishing up the graphene oxide film floating on the water surface from bottom to top by using a silicon wafer, so that the graphene film is laid on the surface of the substrate;
(4) evaporating water in the graphene oxide film at room temperature to enable the water content of the graphene oxide film to be more than 50 wt%; and (4) freeze-drying the graphene oxide film subjected to evaporation treatment, and separating the graphene oxide film from the surface of the silicon wafer.
(5) And reducing the graphene oxide film at 2000-3000 ℃ to ensure that the conductivity of the graphene oxide film is more than 0.5 MS/m.
Further, in the step 2, the pressing position is an edge of the AAO base film.
Further, the thickness of the graphene in the step 1 is 4 nm.
Further, the porosity of the surface of the AAO base film is not less than 40%.
The invention has the beneficial effects that: the film is prepared by a suction filtration method, so that the uniformity of the film and the stability of a device are ensured; the thickness of the graphene film is controlled at a nanometer level by adopting a water transfer method, so that the light transmittance of the film is improved; in the transfer process, micro-folds are introduced, so that the contact area of the film and the photosensitive layer is increased; after high-temperature treatment, the graphene film has extremely low defect content and high conductivity and electron mobility, and is beneficial to photoelectron transmission of the organic solar cell; after high-temperature treatment, the graphene has few defects, the film has high strength, and the flexible electrode can endure stress change in the repeated folding process. The whole process is simple, green and easy to operate. The transparent film ensures the transparency, ensures the great electric conductivity and mechanical bearing performance, and can bear the tension action of the battery in the discharging process and the flexible bending process of the battery. When in use, the film is used as a photo-anode, a counter electrode and the like; in comparison, the graphene has higher electron mobility, and the problem of heavy metal pollution does not exist, so that the cost is reduced, and the light conversion efficiency is improved.
Drawings
Fig. 1 is a schematic flow chart of peeling a graphene film from an AAO base film.
Fig. 2 is a graph showing an experimental process of peeling a graphene film from an AAO base film of example 1.
Fig. 3 is an atomic force microscope image of the graphene film obtained in example 1.
Fig. 4 is a scanned image of the graphene film prepared in example 1.
Fig. 5 is an atomic force microscope image of the graphene film obtained in example 2.
Fig. 6 is a graph showing an experimental process of peeling a graphene film from an MCE base film of comparative example 1.
Fig. 7 is a schematic structural diagram of a graphene-based dye-sensitized transparent solar cell, in which a graphene film serves as a photo-anode.
Fig. 8 is a schematic structural diagram of a graphene-based dye-sensitized transparent solar cell, in which a graphene film is used as a positive electrode.
In the figure, quartz glass 1, graphene film 2, positive electrode 3, and ITO4 are shown.
Detailed Description
Example 1:
as shown in fig. 1, by controlling the concentration of the graphene solution, an ultra-thin graphene oxide film is obtained by suction filtration on an AAO base film by a suction filtration method; placing an AAO base film (with a porosity of 40%) with a graphene oxide film attached to the surface on a water surface with the graphene film facing upward, as shown in fig. 1a and 2 a; pressing the AAO base membrane as in fig. 2b, the AAO base membrane starts to sink as in fig. 2c, and finally, the AAO base membrane sinks to the bottom of the cup, and the graphene membrane (inside the dashed circle) floats on the water surface as in fig. 1b and 2 d.
Fishing up the graphene film floating on the water surface from bottom to top by using a silicon wafer, paving the graphene film on the surface of a substrate, evaporating water in the graphene oxide film for 30 minutes at room temperature, and measuring that the water content of the graphene oxide film is 54 wt%; carrying out freeze drying on the graphene oxide film subjected to evaporation treatment, and separating the graphene oxide film from the surface of the silicon wafer; as shown in fig. 4, the surface has a large number of wrinkles; the thickness was 4nm as measured by atomic force microscopy, as shown in FIG. 3.
The graphene oxide film is thermally reduced at 2000 ℃, the electric conductivity of the graphene oxide film is 0.5MS/m after the graphene oxide film is reduced for 1h, and the strength of the graphene film is 10 GPa.
As shown in fig. 7, the organic thin film solar cell ① assembled with the graphene film as the photo-anode has a photoelectric conversion efficiency improved by 91% compared to the dye-sensitized transparent solar cell ② assembled with ITO as the photo-anode, and has a photoelectric conversion efficiency improved by 37% compared to the dye-sensitized transparent solar cell ③ assembled with a conventional graphene film (spin-coated on ITO) as the photo-anode, whereas when the conventional graphene film (spin-coated on ITO) is used as the photo-anode, the conductivity of the graphene film may be reduced to 48% due to the destruction of the microstructure after 2400h, and the photoelectric conversion efficiency of the solar cell ③ is reduced to 44%, whereas the conductivity of the graphene film of the present application is maintained to 95% or more after 3600h, and the photoelectric conversion efficiency of the solar cell ① is maintained to 97% or more.
Example 2:
by controlling the concentration of the graphene solution, carrying out suction filtration on an AAO (anodic aluminum oxide) base film by a suction filtration method to obtain an ultrathin reduced graphene oxide film; placing the AAO base film (with the porosity of 60%) with the graphene oxide film attached to the surface on the water surface with the surface of the graphene film facing upwards, pressing the edge of the AAO base film to enable the AAO base film to start sinking, finally enabling the AAO base film to sink to the cup bottom, enabling the graphene film to float on the water surface, and successfully stripping the graphene film.
Fishing up the graphene film floating on the water surface from bottom to top by using a silicon wafer, paving the graphene film on the surface of a substrate, evaporating water in the graphene oxide film for 30 minutes at room temperature, and measuring that the water content of the graphene oxide film is 67 wt%; and (3) freeze-drying the graphene oxide film subjected to the evaporation treatment, separating the graphene oxide film from the surface of the silicon wafer to obtain a graphene film with a wrinkled surface, and testing the thickness of the graphene film to be 14nm by using an atomic force microscope, as shown in fig. 5.
The graphene oxide film is thermally reduced at 2000 ℃, the electric conductivity of the graphene oxide film is 0.6MS/m after the graphene oxide film is reduced for 1h, and the strength of the graphene film is 7 GPa.
The dye-sensitized thin-film solar cell ① assembled by using the graphene film as the photo-anode has a photoelectric conversion efficiency improved by 87% compared with the dye-sensitized transparent solar cell ② assembled by using ITO as the photo-anode, and has a photoelectric conversion efficiency improved by 29% compared with the dye-sensitized transparent solar cell ③ assembled by using a conventional graphene film (spin-coated on ITO) as the photo-anode, after 3600h, the electric conductivity is 95% and the photoelectric conversion efficiency of the solar cell ① is 96% of the original electric conductivity.
Example 3:
by controlling the concentration of the graphene solution, carrying out suction filtration on an AAO (anodic aluminum oxide) base film by a suction filtration method to obtain an ultrathin reduced graphene oxide film; placing the AAO base film (with the porosity of 60%) with the graphene oxide film attached to the surface on the water surface with the surface of the graphene film facing upwards, pressing the edge of the AAO base film to enable the AAO base film to start sinking, finally enabling the AAO base film to sink to the cup bottom, enabling the graphene film to float on the water surface, and successfully stripping the graphene film.
Fishing up the graphene film floating on the water surface from bottom to top by using a silicon wafer, paving the graphene film on the surface of a substrate, evaporating water in the graphene oxide film for 30 minutes at room temperature, and measuring that the water content of the graphene oxide film is 75 wt%; and (3) freeze-drying the graphene oxide film subjected to the evaporation treatment, separating the graphene oxide film from the surface of the silicon wafer to obtain a graphene film with a wrinkled surface, and testing the thickness of the graphene film to be 20nm by using an atomic force microscope.
And carrying out thermal reduction on the graphene oxide film at 3000 ℃, and measuring the conductivity of the graphene oxide film after the graphene oxide film is reduced for 0.2h to be 0.8 MS/m. The graphene film strength was 9 GPa.
As shown in fig. 8, when the organic thin-film solar cell ① was assembled using the graphene film as the positive electrode and ITO as the photo-anode, the photoelectric conversion efficiency was improved by 66% compared to the dye-sensitized transparent solar cell ② assembled using a platinum electrode as the positive electrode, and 13% compared to the dye-sensitized transparent solar cell ③ assembled using a conventional graphene film (spin-coated on ITO) as the positive electrode, and after 3600h use, the electric conductivity was 96% and the photoelectric conversion efficiency of the solar cell ① was 97% compared to the original one.
Comparative example 1
According to the suction filtration method as in example 2, a reduced graphene oxide film with a thickness of 14nm was obtained by suction filtration on an MCE base film, and then the MCE base film (porosity: 60%) with the reduced graphene oxide film attached to the surface thereof was placed on a water surface with the surface on which the graphene film was placed facing upward, and as shown in fig. 6a, the MCE base film was not sunk by pressing the edge of the MCE base film, and as shown in fig. 6b, the graphene film failed to be peeled off.
The filtration method is the most uniform method for preparing graphene films, and can control the thickness of a graphene film by regulating and controlling the concentration under a certain amount of filtration liquid, the thickness can be the lowest graphene, the newly added graphene gradually fills the gap of the first graphene layer under the action of pressure along with the increase of the concentration of the graphene, so that the first graphene layer is gradually and completely filled, and then the first graphene layer is developed into a second graphene layer, and the steps are continuously repeated, so that the graphene nano film with the thickness of 2 to ten thousand graphene layers can be prepared. Therefore, the graphene film with the thickness of 4nm can be obtained by simple experimental parameter adjustment by the skilled person.
Claims (4)
1. The graphene-based thin film solar cell is characterized by comprising a transparent electrode, wherein the transparent electrode is a graphene thin film, the thickness of the transparent electrode is not more than 20nm, and the graphene-based thin film solar cell is prepared by the following method:
(1) carrying out suction filtration on the AAO base membrane to obtain a graphene oxide membrane;
(2) placing the AAO base film with the graphene oxide film attached to the surface on the water surface with the surface of the graphene oxide film facing upwards; pressing the AAO base film to enable the AAO base film to sink, and enabling the graphene oxide film to float on the water surface;
(3) fishing up the graphene oxide film floating on the water surface from bottom to top by using a silicon wafer, so that the graphene film is laid on the surface of the substrate;
(4) evaporating water in the graphene oxide film at room temperature to enable the water content of the graphene oxide film to be more than 50 wt%; carrying out freeze drying on the graphene oxide film subjected to evaporation treatment, and separating the graphene oxide film from the surface of the silicon wafer;
(5) and reducing the graphene oxide film at 2000-3000 ℃ to ensure that the conductivity of the graphene oxide film is more than 0.5 MS/m.
2. The graphene-based thin film solar cell according to claim 1, wherein in the step (2), the pressing position is an edge of the AAO base film.
3. The graphene-based thin film solar cell according to claim 1, wherein the graphene oxide film in step (1) has a thickness of 4 nm.
4. The graphene-based thin film solar cell according to claim 1, wherein the AAO base film surface has a porosity of not less than 40%.
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