CN104218109A - High-efficiency perovskite thin film solar cell and preparation method thereof - Google Patents
High-efficiency perovskite thin film solar cell and preparation method thereof Download PDFInfo
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Abstract
The invention provides a high-efficiency perovskite thin film solar cell. The high-efficiency perovskite thin film solar cell is composed of a glass substrate, a front electrode, a compact layer, a porous TiO2 layer, a PVP modified perovskite thin film, a hole transport layer and a back electrode, and formed into a thin film laminated structure, wherein the front electrode is 350nm thick, the compact layer is 30-50nm thick, the porous TiO2 layer is 300-600nm, the PVP modified perovskite thin film is 300-600nm thick, the hole transport layer is 50-200nm thick and the back electrode is 50-200nm thick. The high-efficiency perovskite thin film solar cell has the advantages that the perovskite thin film is an intensively interconnected network formed by crystal grains relatively even in size and has a relatively smooth and continuous surface appearance, compared with a battery device with the perovskite thin film not doped with PVP and under the same conditions, the short circuit current, the open pressure and the fill factor of the high-efficiency perovskite thin film solar cell are all remarkably improved, and the battery efficiency is greatly improved, and therefore, a new preparation method is provided for the development of the low-cost high-efficiency perovskite thin film solar cells.
Description
Technical field
The present invention relates to technical field of solar cells, particularly relate to a kind of high efficiency perovskite thin film solar cell and preparation method thereof.
Background technology
Photovoltaic, as a developing direction of future source of energy, significantly must raise the efficiency, reduce costs the requirement that could meet real world applications.Ca-Ti ore type thin film solar cell is simple with its structure, preparation cost is cheap and the advantages such as easy production have attracted the great interest of numerous researcher.Organo-mineral complexing perovskite CH
3nH
3(X is halogen element I to PbX, Cl, Br or halogen compound) be direct gap semiconductor material, there is the advantages such as the absorption coefficient of light is large, carrier mobility is high, the life-span is long, in perovskite solar cell, illustrate huge application prospect as light trapping material.Its cell photoelectric transformation efficiency brought up to 19.3% rapidly from 3.8% in nearly 5 years, but also had the larger space promoted further, became a new direction of following theCourse of PV Industry.
The preparation method of Ca-Ti ore type thin film solar cell has two kinds usually: vacuum vapour deposition and solwution method.Compared with vapour deposition method, solwution method, due to without the need to vacuum equipment, is the better approach of preparation low cost, efficient solar battery.Perovskite thin film is as the light absorbing zone of perovskite solar cell, and its pattern and performance are the key factors affecting battery.Concerning solution spin-coating method prepares thin film solar cell, acquisition is even, the perovskite thin film of high coverage rate remains the severe challenge that this low-cost technologies faces at present.
Polyvinylpyrrolidone (PVP) is a kind of nontoxic water-soluble high-molecular compound, has good stability and film forming characteristics.It not only can be used as surface agent, can also be used as chelating agent, controls crystal growth by modifying interfacial energy, or is used as surface agent and chelating agent application simultaneously.The present invention proposes in perovskite precursor solution, to add PVP to improve the film forming characteristics of perovskite, improves its coverage rate on porous layer, and then promotes the photoelectric characteristic of perovskite thin film solar cell.
Summary of the invention
The object of the invention is for above-mentioned existing problems, a kind of high efficiency perovskite thin film solar cell and preparation method thereof is provided, perovskite thin film prepared by the method is the dense interconnection network formed by the crystal grain that size is relatively uniform, present surperficial relative smooth and continuous print pattern, adopt surface agent polyvinylpyrrolidone (PVP) to strengthen perovskite thin film surface coverage, and then improve perovskite efficiency of solar cell.
Technical scheme of the present invention:
A kind of high efficiency perovskite thin film solar cell, by glass substrate, front electrode, compacted zone, porous TiO
2the perovskite thin film that layer, PVP modulate, hole transmission layer and back electrode form and form pellicular cascade structure, and film thickness is respectively front electrode 350nm, compacted zone 30-50nm, porous TiO
2layer 300-600nm, perovskite thin film 300-600nm, hole transmission layer 50-200nm and back electrode 50-200nm.
A preparation method for described high efficiency perovskite thin film solar cell, step is as follows:
1) chemical bath method is adopted to prepare TiO on clean transparent conductive film FTO substrate
2compacted zone
Clean transparent conductive film FTO substrate is put into the TiCl that concentration is 0.04mol/L
4in the aqueous solution, be then placed in baking box and heat 30min at 70 DEG C, take out substrate and rinse well, anneal 45min at 500 DEG C, obtains the TiO that thickness is 30-50nm
2compacted zone, as electronic barrier layer;
2) spin-coating method is adopted to prepare porous TiO
2layer
By porous TiO
2with absolute ethyl alcohol according to weight ratio 1:4 dilution, the porous TiO that spin coating has been diluted on compacted zone
2solution, 5000 revs/min rotate 60 seconds, spin coating twice, and then 500oC annealing 45min, obtains the porous TiO that thickness is 300-600nm
2layer, as insulating barrier;
3) spin-coating method is adopted to prepare perovskite thin film
By methylpyridinium iodide ammonium (CH
3nH
3and lead chloride (PbCl I)
2) be dissolved in DMF and obtain mixed liquor, in mixed liquor, the mol ratio of methylpyridinium iodide ammonium and lead chloride is 3:1, and magnetic agitation is clarified to solution, in mixed liquor, add PVP, and PVP addition is CH
3nH
3i and PbCl
2the 0-5wt% of total weight, continue to stir, the mixed liquor containing PVP dropped in porous TiO
2on layer, 5000 revs/min rotate 60 seconds, and air anneal 50min at 100-160 DEG C, obtains the perovskite thin film that thickness is 300-600nm in an oven;
4) spin coating Spiro-OMeTAD{2,2,7,7-tetra-[N, N-bis-(4-methoxyphenyl) is amino]-9,9-spiral shell two fluorenes on perovskite thin film } hole transmission layer (HTM)
First two for 520mg trifluoromethanesulfonimide lithium (Li-TFSI) is dissolved in 1mL acetonitrile solution, then the acetonitrile solution of 17.5 μ L Li-TFSI and 80mg spiro-OMeTAD, 28.5 μ L 4-tert .-butylpyridine are dissolved in 1mL chlorobenzene altogether, obtain HTM solution, the HTM solution prepared is dropped on perovskite thin film, 5000 revs/min rotate 60 seconds, spin coating twice, obtained thickness is the hole transmission layer of 50-200nm;
5) thermal evaporation is adopted to prepare back electrode
On hole transmission layer, thermal evaporation layer of Au, Ag or Al metallic film are as back electrode, and thickness is 50-200nm, obtained perovskite thin film solar cell.
Working mechanism of the present invention:
The method can strengthen perovskite thin film surface coverage, and then improves perovskite efficiency of solar cell.Utilize PVP stable performance, there is good film forming characteristics, joined in the precursor solution of perovskite thin film, improve the affinity between precursor solution and multichip semiconductor aperture layer or insulating barrier, strengthen the coverage rate of perovskite thin film on its surface.The lifting of perovskite thin film surface coverage, can reduce on the one hand and do not lost by the light transmission that perovskite thin film absorbs, enhance light absorption; On the other hand by reducing the cavity of surface of insulating layer, reducing the part that hole transmission layer directly contacts with insulating barrier, reducing the recombination losses of charge carrier.Therefore make the short-circuit current density of perovskite solar cell, open pressure and fill factor, curve factor all gets a promotion, and then battery efficiency is greatly improved
Advantage of the present invention and good effect are:
The perovskite thin film adopting the present invention to prepare is the dense interconnection network formed by the crystal grain that size is relatively uniform, presents surperficial relative smooth and continuous print pattern; By the adjustment of surface agent addition, conveniently can control the key parameter such as coverage rate, surface topography of film, thus affect optical absorption intensity and photoelectric properties; With the perovskite thin film not adding surface agent as the same terms of absorbed layer battery device compared with, short circuit current, open pressure and fill factor, curve factor be all significantly increased, battery efficiency obtains and significantly promotes, for the development of low cost, efficient calcium titanium ore thin film solar cell provides a kind of new preparation method.
Accompanying drawing explanation
Fig. 1 is atomic force microscope (AFM) shape appearance figure of the perovskite thin film of preparation.
Fig. 2 is the structure chart of this perovskite thin film solar cell.
Fig. 3 is the I-V performance diagram of this perovskite thin film solar cell.
Fig. 4 is the light absorption spectrogram of the perovskite thin film of preparation
Fig. 5 is the quantum efficiency curve chart with Fig. 4 solar cell corresponding to the perovskite thin film prepared.
Embodiment
Below in conjunction with the drawings and specific embodiments, technical solutions according to the invention are described in detail.
embodiment 1:
A kind of high efficiency perovskite thin film solar cell, by glass substrate, front electrode, compacted zone, porous TiO
2the perovskite thin film that layer, PVP modulate, hole transmission layer and back electrode form and form pellicular cascade structure, as shown in Figure 1, the preparation method of described high efficiency perovskite thin film solar cell, step is as follows:
1) chemical bath method is adopted to prepare TiO on clean transparent conductive film FTO substrate
2compacted zone
Be that the transparent conductive film FTO substrate of 350nm puts into the TiCl that concentration is 0.04mol/L by clean thickness
4in the aqueous solution, be then placed in baking box and heat 30min at 70 DEG C, take out substrate and rinse well, anneal 45min at 500 DEG C, obtains the TiO that thickness is about 30nm
2compacted zone, as electronic barrier layer;
2) spin-coating method is adopted to prepare porous TiO
2layer
By porous TiO
2with absolute ethyl alcohol according to weight ratio 1:4 dilution, the porous TiO that spin coating has been diluted on compacted zone
2solution, 5000 revs/min rotate 60 seconds, spin coating twice, and then 500oC annealing 45min, obtains the porous TiO that thickness is 400nm
2layer, as insulating barrier;
3) spin-coating method is adopted to prepare perovskite thin film
By methylpyridinium iodide ammonium (CH
3nH
3and lead chloride (PbCl I)
2) be dissolved in DMF and obtain mixed liquor, in mixed liquor, the mol ratio of methylpyridinium iodide ammonium and lead chloride is 3:1, and magnetic agitation 12h clarifies to solution.Mixed liquor is dropped in porous TiO
2on layer, 5000 revs/min rotate 60 seconds, and air anneal 50min at 140 DEG C, obtains the perovskite thin film that thickness is about 400nm in an oven, and Fig. 1 is atomic force microscope (AFM) shape appearance figure of the perovskite thin film of preparation;
4) spin coating Spiro-OMeTAD{2,2,7,7-tetra-[N, N-bis-(4-methoxyphenyl) is amino]-9,9-spiral shell two fluorenes on perovskite thin film } hole transmission layer (HTM)
First two for 520mg trifluoromethanesulfonimide lithium (Li-TFSI) is dissolved in 1mL acetonitrile solution, then the acetonitrile solution of 17.5 μ L Li-TFSI and 80mg spiro-OMeTAD, 28.5 μ L 4-tert .-butylpyridine are dissolved in 1mL chlorobenzene altogether, obtain HTM solution, the HTM solution prepared is dropped on perovskite thin film, 5000 revs/min rotate 60 seconds, spin coating twice, obtained thickness is about the hole transmission layer of 150nm;
5) thermal evaporation is adopted to prepare back electrode
On hole transmission layer, thermal evaporation one deck Ag metallic film is as back electrode, and thickness is about 150nm, obtained perovskite thin film solar cell.
Testing result is as in Figure 3-5: J
sc, V
oc13.12 mA/cm are respectively with FF
2, 0.787 V, 43.7; Photoelectric conversion efficiency η is 4.51%.
embodiment 2:
A kind of high efficiency perovskite thin film solar cell, by glass substrate, front electrode, compacted zone, porous TiO
2the perovskite thin film that layer, PVP modulate, hole transmission layer and back electrode form and form pellicular cascade structure, as shown in Figure 1, the preparation method of described high efficiency perovskite thin film solar cell, step 1), 2), 4) with 5) identical with embodiment 1, difference is that step 3) is:
3) by CH
3nH
3i and PbCl
2be dissolved in DMF and obtain mixed liquor, in mixed liquor, the mol ratio of methylpyridinium iodide ammonium and lead chloride is 3:1, and magnetic agitation 12h clarifies to solution, in mixed liquor, add PVP, and PVP addition is CH
3nH
3i and PbCl
2the 1.6wt% of total weight, continue to stir, the mixed liquor containing PVP dropped in porous TiO
2on layer, 5000 revs/min rotate 60 seconds, and air anneal 50min at 140 DEG C, obtains the perovskite thin film that thickness is about 400nm in an oven.
Testing result is as in Figure 3-5: J
sc, V
oc14.96 mA/cm are respectively with FF
2, 0.823 V, 48.5.Photoelectric conversion efficiency η is 5.97%.
embodiment 3:
A kind of high efficiency perovskite thin film solar cell, by glass substrate, front electrode, compacted zone, porous TiO
2the perovskite thin film that layer, PVP modulate, hole transmission layer and back electrode form and form pellicular cascade structure, as shown in Figure 1, the preparation method of described high efficiency perovskite thin film solar cell, step 1), 2), 4) with 5) identical with embodiment 1, difference is that step 3) is:
3) by CH
3nH
3i and PbCl
2be dissolved in DMF and obtain mixed liquor, in mixed liquor, the mol ratio of methylpyridinium iodide ammonium and lead chloride is 3:1, and magnetic agitation 12h clarifies to solution, adds the PVP of 3.3wt% in mixed liquor, continues to stir, and the mixed liquor containing PVP is dropped in porous TiO
2on layer, 5000 revs/min rotate 60 seconds, and air anneal 50min at 140 DEG C, obtains the perovskite thin film that thickness is about 400nm in an oven.
Testing result is as in Figure 3-5: J
sc, V
oc17.54 mA/cm are respectively with FF
2, 0.848 V, 58.8.Photoelectric conversion efficiency η is 8.74%.
embodiment 4:
A kind of high efficiency perovskite thin film solar cell, by glass substrate, front electrode, compacted zone, porous TiO
2the perovskite thin film that layer, PVP modulate, hole transmission layer and back electrode form and form pellicular cascade structure, as shown in Figure 1, the preparation method of described high efficiency perovskite thin film solar cell, step 1), 2), 4) with 5) identical with embodiment 1, difference is that step 3) is:
3) by CH
3nH
3i and PbCl
2be dissolved in DMF and obtain mixed liquor, in mixed liquor, the mol ratio of methylpyridinium iodide ammonium and lead chloride is 3:1, and magnetic agitation 12h clarifies to solution, adds the PVP of 5wt% in mixed liquor, continues to stir, and the mixed liquor containing PVP is dropped in porous TiO
2on layer, 5000 revs/min rotate 60 seconds, and air anneal 50min at 140 DEG C, obtains the perovskite thin film that thickness is about 400nm in an oven.
Testing result is as in Figure 3-5: J
sc, V
oc16.56 mA/cm are respectively with FF
2, 0.837 V, 36.8.Photoelectric conversion efficiency η is 5.10%.
?
The detailed performance parameter of solar cell prepared by embodiment of the present invention 1-4 is in table 1.
Table 1 adds and does not add the detailed performance parameter of PVP battery device
| Samples | J sc (mA/cm 2) | V oc (V) | FF | η(%) |
| 0% | 13.12 | 0.787 | 43.7 | 4.51 |
| 1.6% | 14.96 | 0.823 | 48.5 | 5.97 |
| 3.3% | 17.54 | 0.848 | 58.8 | 8.74 |
| 5% | 16.56 | 0.837 | 36.8 | 5.10 |
Because the emphasis of the present invention is providing high coverage rate, the perovskite thin film of high photoelectric properties for efficient, low cost perovskite thin film solar cell.The device efficiency of battery can be promoted to 8.74% from 4.51%, means that the present invention can make the photoelectric properties of battery be improved significantly.
To sum up, the invention provides the preparation method being strengthened perovskite thin film surface coverage and then lifting efficiency of solar cell by surface agent, the method is simple, by the adjustment of surface agent addition, conveniently can control the key parameter such as coverage rate, surface topography of film, thus affect its photoelectric properties, and then significantly promote the photoelectric conversion efficiency of solar cell.For the development of low cost, efficient calcium titanium ore thin film solar cell provides condition, make this novel solar cell be practical to become possibility.
The above; be only the present invention's preferably embodiment, but protection scope of the present invention is not limited thereto, is anyly familiar with those skilled in the art in the technical scope that the present invention discloses; the change that can expect easily or replacement, all should be encompassed within protection scope of the present invention.Therefore, protection scope of the present invention should be as the criterion with the protection range of claim.
Claims (2)
1. a high efficiency perovskite thin film solar cell, is characterized in that: by glass substrate, front electrode, compacted zone, porous TiO
2the perovskite thin film that layer, PVP modulate, hole transmission layer and back electrode form and form pellicular cascade structure, and film thickness is respectively front electrode 350nm, compacted zone 30-50nm, porous TiO
2layer 300-600nm, perovskite thin film 300-600nm, hole transmission layer 50-200nm and back electrode 50-200nm.
2. a preparation method for high efficiency perovskite thin film solar cell as claimed in claim 1, is characterized in that step is as follows:
1) chemical bath method is adopted to prepare TiO on clean transparent conductive film FTO substrate
2compacted zone
Clean transparent conductive film FTO substrate is put into the TiCl that concentration is 0.04mol/L
4in the aqueous solution, be then placed in baking box and heat 30min at 70 DEG C, take out substrate and rinse well, anneal 45min at 500 DEG C, obtains the TiO that thickness is 30-50nm
2compacted zone, as electronic barrier layer;
2) spin-coating method is adopted to prepare porous TiO
2layer
By porous TiO
2with absolute ethyl alcohol according to weight ratio 1:4 dilution, the porous TiO that spin coating has been diluted on compacted zone
2solution, 5000 revs/min rotate 60 seconds, spin coating twice, and then 500oC annealing 45min, obtains the porous TiO that thickness is 300-600nm
2layer, as insulating barrier;
3) spin-coating method is adopted to prepare perovskite thin film
By methylpyridinium iodide ammonium (CH
3nH
3and lead chloride (PbCl I)
2) be dissolved in DMF and obtain mixed liquor, in mixed liquor, the mol ratio of methylpyridinium iodide ammonium and lead chloride is 3:1, and magnetic agitation is clarified to solution, in mixed liquor, add PVP, and PVP addition is CH
3nH
3i and PbCl
2the 0-5wt% of total weight, continue to stir, the mixed liquor containing PVP dropped in porous TiO
2on layer, 5000 revs/min rotate 60 seconds, and air anneal 50min at 100-160 DEG C, obtains the perovskite thin film that thickness is 300-600nm in an oven;
4) spin coating Spiro-OMeTAD{2,2,7,7-tetra-[N, N-bis-(4-methoxyphenyl) is amino]-9,9-spiral shell two fluorenes on perovskite thin film } hole transmission layer (HTM)
First two for 520mg trifluoromethanesulfonimide lithium (Li-TFSI) is dissolved in 1mL acetonitrile solution, then the acetonitrile solution of 17.5 μ L Li-TFSI and 80mg spiro-OMeTAD, 28.5 μ L 4-tert .-butylpyridine are dissolved in 1mL chlorobenzene altogether, obtain HTM solution, the HTM solution prepared is dropped on perovskite thin film, 5000 revs/min rotate 60 seconds, spin coating twice, obtained thickness is the hole transmission layer of 50-200nm;
5) thermal evaporation is adopted to prepare back electrode
On hole transmission layer, thermal evaporation layer of Au, Ag or Al metallic film are as back electrode, and thickness is 50-200nm, obtained perovskite thin film solar cell.
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| CN110176546A (en) * | 2019-04-28 | 2019-08-27 | 华南师范大学 | A kind of light emitting diode and preparation method thereof based on multiple addition calcium titanium material layer |
| CN111403607A (en) * | 2020-03-25 | 2020-07-10 | 华东理工大学 | Chelated perovskite material, film, device and preparation method and application thereof |
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