CN104319349A - Perovskite type solar cell with sputtering ZnO as electron transfer layer and preparation - Google Patents
Perovskite type solar cell with sputtering ZnO as electron transfer layer and preparation Download PDFInfo
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- CN104319349A CN104319349A CN201410587279.8A CN201410587279A CN104319349A CN 104319349 A CN104319349 A CN 104319349A CN 201410587279 A CN201410587279 A CN 201410587279A CN 104319349 A CN104319349 A CN 104319349A
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Abstract
The invention provides a perovskite type solar cell with sputtering ZnO as an electron transfer layer and preparation and relates to solar cells. The perovskite type solar cell is provided with a transparent conducting glass substrate, the ZnO electron transfer layer, a perovskite type material layer, a hole transfer layer and a metal back electrode layer from bottom to top in sequence. The preparation comprises the steps that the transparent conducting glass substrate is preprocessed, a ZnO thin film is prepared on the transparent conducting glass substrate, and heating and annealing are conducted, in other words, the ZnO electron transfer layer is sputtered; a DMF solution of PbI2 is prepared, the ZnO electron transfer layer is coated with the DMF solution of the PbI2 in a spinning mode to prepare a PbI2 thin film, the PbI2 thin film is then steeped into an isopropanol solution of CH3NH3I, and thus the perovskite type material layer is obtained; 2,2',7,7'-Tetrakis[N,N-di(4-methoxyphenyl)amino]-9,9'-spirobifluorene, an acetonitrile solution of lithium bis(trifluoromethanesulphonyl)imide and 4-tert-butylpyridine are dissolved in a chlorobenzene solution, the perovskite type material layer is then coated with the solution in a spinning mode, the hole transfer layer is obtained, then the metal back electrode layer is obtained, and the perovskite type solar cell is obtained.
Description
Technical field
The present invention relates to solar cell, particularly relate to a kind of to sputter the Ca-Ti ore type solar cell and preparation method that ZnO is electron transfer layer.
Background technology
Along with the development of global economy, energy resource consumption gets more and more, and wherein fewer and feweri as petroleum resources, energy problem will become a significant problem from now on.Solar energy is renewable resource, and has inexhaustible feature, and therefore the development of solar cell has great importance.But solar cell now otherwise photoelectric conversion efficiency is low, otherwise cost is too high.At present, silicon solar cell has higher efficiency, but in preparation process, need high temperature, high vacuum, and cost is very high.Organic polymer solar cell has that cost is lower, nontoxic, preparation easily, can the feature such as large area flexible manufacture, but its photoelectric conversion efficiency is also lower.
Ca-Ti ore type solar cell is a newcomer of photovoltaic art, and its light absorbent is (modal for CH based on the perovskite structure of hybrid inorganic-organic
3nH
3pbI
3) semi-conducting material, light absorption range is wide, and self has high carrier mobility and longer carrier lifetime, and longer distance can be moved in light induced electron and hole, be conducive to it and collected formation electric current by external circuit, thus battery can obtain high photoelectric conversion efficiency.
At present, based on CH
3nH
3pbI
3ca-Ti ore type battery usually adopt TiO
2as electron transfer layer, and higher efficiency can be obtained.But this TiO
2electric transmission Rotating fields needs double-layer structure, and one deck is fine and close TiO
2layer, one deck is the TiO of meso-hole structure
2layer, and all need up to the preparation of 500 DEG C of temperature sintering, more than two layers of thickness 300nm, technique is comparatively complicated.
And adopt ZnO Thin Films Sputtered as electron transfer layer, only need more than 20nm, only need one deck simultaneously, preparation technology is comparatively simple, and has higher efficiency.
Chinese patent CN104091888A discloses a kind of Ca-Ti ore type solar cell and preparation method thereof.Described Ca-Ti ore type solar cell is by FTO substrate of glass, sandwich structure TiO
2/ ZnO/TiO
2compacted zone, TiO
2mesoporous/perovskite structural material active light-absorption layer, spiro-OMeTAD hole transmission layer and gold electrode form.
Chinese patent CN104051629A discloses a kind of method preparing Ca-Ti ore type solar cell based on spraying coating process, prepares specifically by spraying hole transmission layer, perovskite active layer, electron transfer layer and top electrode in electrically conducting transparent substrate successively.By changing the different parameters of spraying coating process, the regulation and control to device quality and performance can be realized.
Summary of the invention
The object of the present invention is to provide a kind of to sputter Ca-Ti ore type solar cell that ZnO is electron transfer layer and preparation method thereof.
Describedly be provided with transparent conducting glass substrate, ZnO electron transfer layer, perovskite-type material layer, hole transmission layer and metallic back electrode layer to sputter the Ca-Ti ore type solar cell that ZnO is electron transfer layer, transparent conducting glass substrate, ZnO electron transfer layer, perovskite-type material layer, hole transmission layer and metallic back electrode layer lamination successively from bottom to up;
Described perovskite-type material layer is CH
3nH
3pbI
3layer, described hole transmission layer is 2,2', 7,7'-tetra-[N, N-bis-(4-methoxyphenyl) is amino]-9,9'-spiral shell two fluorenes (spiro-MeOTAD) hole transmission layers; Described metallic back electrode layer is Au dorsum electrode layer or Ag dorsum electrode layer.
Described transparent conducting glass substrate can adopt the Conducting Glass that indium tin oxide (ITO) is conductive layer, and the thickness of described transparent conducting glass substrate can be 100 ~ 150nm.
The thickness of described ZnO electron transfer layer can be 20 ~ 120nm.
The thickness of described perovskite-type material layer can be 20 ~ 120nm.
The thickness of described hole transmission layer can be 40 ~ 60nm.
The thickness of described metallic back electrode layer can be 60 ~ 150nm.
Described with the preparation method sputtering the Ca-Ti ore type solar cell that ZnO is electron transfer layer, comprise the following steps:
1) transparent conducting glass substrate is removed grease and organic substance, then supersound washing, nitrogen dries up, and obtains pretreated transparent conducting glass substrate;
2) in step 1) making ZnO film on the pretreated transparent conducting glass substrate of gained, then heat, annealing, namely sputter ZnO electron transfer layer;
3) PbI is prepared
2dMF solution, then by PbI
2dMF solution be spin-coated on ZnO electron transfer layer, obtained yellow PbI
2film, by PbI after drying
2film immerses CH
3nH
3the aqueous isopropanol of I, then uses isopropyl alcohol, and nitrogen dries up, and obtains brown CH
3nH
3pbI
3layer;
4) by 2,2', 7,7'-tetra-[N, N-bis-(4-methoxyphenyl) is amino]-9,9'-spiral shell two fluorenes (spiro-MeOTAD), the acetonitrile solution of two (trifluoromethane sulfonic acid acyl) imine lithium (Li-TFSI), 4-tert .-butylpyridine (TBP) are dissolved in chlorobenzene solution, then are spin-coated on CH
3nH
3pbI
3on layer, obtained hole transmission layer;
5) on hole transmission layer, metallic back electrode layer is prepared, i.e. obtained Ca-Ti ore type solar cell.
In step 1) in, the size of described transparent conducting glass substrate can be 25mm × 25mm; Described removal grease and organic substance can adopt liquid detergent and deionized water washing 15min; Described supersound washing can use acetone, ethanol, deionized water supersound washing 10min successively.
In step 2) in, the method for described making ZnO film can adopt magnetron sputtering method to obtain the ZnO film of desired thickness; The condition of described heating can heat 10min at 150 DEG C.
In step 3) in, described preparation PbI
2the temperature of DMF solution can at 70 DEG C; Described PbI
2the molar concentration of DMF solution can be 1mol/L; Described spin coating can adopt sol evenning machine spin coating; The time of described drying can be 5min; Described CH
3nH
3the mass concentration of the aqueous isopropanol of I can be 10mg/mL.
In step 4) in, described 2, 2', 7, 7'-tetra-[N, N-bis-(4-methoxyphenyl) is amino]-9, 9'-spiral shell two fluorenes (spiro-MeOTAD), the acetonitrile solution of two (trifluoromethane sulfonic acid acyl) imine lithium (Li-TFSI), the proportioning of 4-tert .-butylpyridine (TBP) can be 80mg: 17.5 μ L: 28.5 μ L, wherein, 2, 2', 7, 7'-tetra-[N, N-bis-(4-methoxyphenyl) is amino]-9, 9'-spiral shell two fluorenes (spiro-MeOTAD) is calculated in mass, acetonitrile solution and the 4-tert .-butylpyridine (TBP) of two (trifluoromethane sulfonic acid acyl) imine lithium (Li-TFSI) are calculated by volume, the mass concentration of the acetonitrile solution of described two (trifluoromethane sulfonic acid acyl) imine lithium (Li-TFSI) can be 520mg/ml, described spin coating is by the method for solution spin coating.
In step 5) in, the described method preparing metallic back electrode layer on hole transmission layer can be: 4 × 10
-4hot vapour deposition method is adopted to prepare metallic back electrode layer under vacuum condition on hole transmission layer.
Advantage of the present invention and good effect are:
1, in Ca-Ti ore type solar cell, sputtering ZnO is adopted to be electron transfer layer, this ZnO Thin Films Sputtered has preferred c-axis orientation and low defect density, there is higher electron transport ability, the electronics that separation of charge goes out more efficiently can be collected by external circuit and form electric current, and photoelectric conversion efficiency is higher.
2, the present invention is to sputter the Ca-Ti ore type solar cell that ZnO is electron transfer layer, simple for production, only needs one deck, and thickness lower (below 120nm), do not need two-layer.
3, the present invention is high with the photoelectric conversion efficiency sputtering the Ca-Ti ore type solar cell that ZnO is electron transfer layer.
Accompanying drawing explanation
Fig. 1 is the structural representation of Ca-Ti ore type solar cell embodiment of the present invention.
Embodiment
Embodiment 1:
A kind of to sputter the Ca-Ti ore type solar cell that ZnO is electron transfer layer, as shown in Figure 1, formed by transparent conducting glass substrate 1, electron transfer layer 2, perovskite-type material layer 3, hole transmission layer 4 and Au/Ag metallic back electrode layer 5 and formed laminated construction successively, described transparent conducting glass substrate 1 is ITO electro-conductive glass; Electron transfer layer 2 is ZnO Thin Films Sputtered, and thickness is 40nm; Perovskite-type material layer 3 is CH
3nH
3pbI
3layer, thickness is 300nm; Hole transmission layer 4 is 2,2', 7,7'-tetra-[N, N-bis-(4-methoxyphenyl) is amino]-9,9'-spiral shell two fluorenes (spiro-MeOTAD) layers, and thickness is 40nm; Metallic back electrode layer 5 is Ag, and thickness is 100nm.
Embodiment 2:
A kind of to sputter the Ca-Ti ore type solar cell that ZnO is electron transfer layer, be made up of transparent conducting glass substrate, electron transfer layer, perovskite-type material layer, hole transmission layer and Au/Ag metallic back electrode layer and form laminated construction successively, described transparent conducting glass substrate is ITO electro-conductive glass; Electron transfer layer is ZnO Thin Films Sputtered, and thickness is 20nm; Perovskite-type material layer is CH
3nH
3pbI
3layer, thickness is 300nm; Hole transmission layer is 2,2', 7,7'-tetra-[N, N-bis-(4-methoxyphenyl) is amino]-9,9'-spiral shell two fluorenes (spiro-MeOTAD) layers, and thickness is 40nm; Metallic back electrode layer is Ag, and thickness is 60nm.
Embodiment 3:
A kind of to sputter the Ca-Ti ore type solar cell that ZnO is electron transfer layer, be made up of transparent conducting glass substrate, electron transfer layer, perovskite-type material layer, hole transmission layer and Au/Ag metallic back electrode layer and form laminated construction successively, described transparent conducting glass substrate is ITO electro-conductive glass; Electron transfer layer is ZnO Thin Films Sputtered, and thickness is 120nm; Perovskite-type material layer is CH
3nH
3pbI
3layer, thickness is 300nm; Hole transmission layer is 2,2', 7,7'-tetra-[N, N-bis-(4-methoxyphenyl) is amino]-9,9'-spiral shell two fluorenes (spiro-MeOTAD) layers, and thickness is 40nm; Metallic back electrode layer is Au, and thickness is 60nm.
Embodiment 4:
A kind of to sputter the Ca-Ti ore type solar cell that ZnO is electron transfer layer, as shown in Figure 1, be made up of transparent conducting glass substrate, electron transfer layer, perovskite-type material layer, hole transmission layer and Au/Ag metallic back electrode layer and form laminated construction successively, described transparent conducting glass substrate is ITO electro-conductive glass; Electron transfer layer is ZnO Thin Films Sputtered, and thickness is 40nm; Perovskite-type material layer is CH
3nH
3pbI
3layer, thickness is 300nm; Hole transmission layer is 2,2', 7,7'-tetra-[N, N-bis-(4-methoxyphenyl) is amino]-9,9'-spiral shell two fluorenes (spiro-MeOTAD) layers, and thickness is 40nm; Metallic back electrode layer is Au, and thickness is 150nm.
Below provide test result: after prepared by Ca-Ti ore type solar cell, by Au (Ag) negative electrode one termination ammeter positive pole, ito anode one termination ammeter negative pole.Test data is in table 1.
Table 1
| Embodiment | Jsc/mA | Voc/V | FF | PCE(％) |
| 1 | 13.46 | 0.98 | 0.42 | 6.78 |
| 2 | 13.72 | 0.92 | 0.44 | 6.21 |
| 3 | 14.56 | 0.98 | 0.43 | 6.57 |
| 4 | 12.08 | 0.92 | 0.45 | 5.73 |
Result shows: at AM 1.5G (100mW/cm
2) under illumination, Jsc, Voc, FF, PCE are respectively at least at 12mA/cm
2, 0.92V, 0.42, more than 5.73%, most high-photoelectric transformation efficiency reaches 6.78%.
Claims (10)
1. to sputter the Ca-Ti ore type solar cell that ZnO is electron transfer layer, it is characterized in that being provided with transparent conducting glass substrate, ZnO electron transfer layer, perovskite-type material layer, hole transmission layer and metallic back electrode layer, transparent conducting glass substrate, ZnO electron transfer layer, perovskite-type material layer, hole transmission layer and metallic back electrode layer lamination successively from bottom to up;
Described perovskite-type material layer is CH
3nH
3pbI
3layer, described hole transmission layer is 2,2', 7,7'-tetra-[N, N-bis-(4-methoxyphenyl) is amino]-9,9'-spiral shell two fluorenes (spiro-MeOTAD) hole transmission layers; Described metallic back electrode layer is Au dorsum electrode layer or Ag dorsum electrode layer.
2., as claimed in claim 1 to sputter the Ca-Ti ore type solar cell that ZnO is electron transfer layer, it is characterized in that described transparent conducting glass substrate adopts indium tin oxide to be the Conducting Glass of conductive layer.
3. as claimed in claim 1 to sputter the Ca-Ti ore type solar cell that ZnO is electron transfer layer, it is characterized in that the thickness of described transparent conducting glass substrate is 100 ~ 150nm, the thickness of described ZnO electron transfer layer is 20 ~ 120nm, the thickness of described perovskite-type material layer is 20 ~ 120nm, the thickness of described hole transmission layer is 40 ~ 60nm, and the thickness of described metallic back electrode layer is 60 ~ 150nm.
4., to sputter the preparation method of the Ca-Ti ore type solar cell that ZnO is electron transfer layer as described in as arbitrary in claims 1 to 3, it is characterized in that comprising the following steps:
1) transparent conducting glass substrate is removed grease and organic substance, then supersound washing, nitrogen dries up, and obtains pretreated transparent conducting glass substrate;
2) in step 1) making ZnO film on the pretreated transparent conducting glass substrate of gained, then heat, annealing, namely sputter ZnO electron transfer layer;
3) PbI is prepared
2dMF solution, then by PbI
2dMF solution be spin-coated on ZnO electron transfer layer, obtained yellow PbI
2film, by PbI after drying
2film immerses CH
3nH
3the aqueous isopropanol of I, then uses isopropyl alcohol, and nitrogen dries up, and obtains brown CH
3nH
3pbI
3layer;
4) by 2,2', 7,7'-tetra-[N, N-bis-(4-methoxyphenyl) is amino]-9,9'-spiral shell two fluorenes, the acetonitrile solution of two (trifluoromethane sulfonic acid acyl) imine lithium, 4-tert .-butylpyridine are dissolved in chlorobenzene solution, then are spin-coated on CH
3nH
3pbI
3on layer, obtained hole transmission layer;
5) on hole transmission layer, metallic back electrode layer is prepared, i.e. obtained Ca-Ti ore type solar cell.
5., as claimed in claim 4 to sputter the preparation method of the Ca-Ti ore type solar cell that ZnO is electron transfer layer, it is characterized in that in step 1) in, described removal grease and organic substance adopt liquid detergent and deionized water washing 15min; Described supersound washing can use acetone, ethanol, deionized water supersound washing 10min successively.
6., as claimed in claim 4 to sputter the preparation method of the Ca-Ti ore type solar cell that ZnO is electron transfer layer, it is characterized in that in step 2) in, the method for described making ZnO film adopts magnetron sputtering method to obtain the ZnO film of desired thickness.
7., as claimed in claim 4 to sputter the preparation method of the Ca-Ti ore type solar cell that ZnO is electron transfer layer, it is characterized in that in step 2) in, the condition of described heating heats 10min at 150 DEG C.
8., as claimed in claim 4 to sputter the preparation method of the Ca-Ti ore type solar cell that ZnO is electron transfer layer, it is characterized in that in step 3) in, described preparation PbI
2the temperature of DMF solution be at 70 DEG C; Described PbI
2the molar concentration of DMF solution can be 1mol/L; Described spin coating can adopt sol evenning machine spin coating; The time of described drying can be 5min; Described CH
3nH
3the mass concentration of the aqueous isopropanol of I can be 10mg/mL.
9. as claimed in claim 4 to sputter the preparation method of the Ca-Ti ore type solar cell that ZnO is electron transfer layer, it is characterized in that in step 4) in, described 2, 2', 7, 7'-tetra-[N, N-bis-(4-methoxyphenyl) is amino]-9, 9'-spiral shell two fluorenes (spiro-MeOTAD), the acetonitrile solution of two (trifluoromethane sulfonic acid acyl) imine lithium (Li-TFSI), the proportioning of 4-tert .-butylpyridine (TBP) is 80mg: 17.5 μ L: 28.5 μ L, wherein, 2, 2', 7, 7'-tetra-[N, N-bis-(4-methoxyphenyl) is amino]-9, 9'-spiral shell two fluorenes (spiro-MeOTAD) is calculated in mass, acetonitrile solution and the 4-tert .-butylpyridine (TBP) of two (trifluoromethane sulfonic acid acyl) imine lithium (Li-TFSI) are calculated by volume, the mass concentration of the acetonitrile solution of described two (trifluoromethane sulfonic acid acyl) imine lithium (Li-TFSI) can be 520mg/ml, described spin coating is by the method for solution spin coating.
10., as claimed in claim 4 to sputter the preparation method of the Ca-Ti ore type solar cell that ZnO is electron transfer layer, it is characterized in that in step 5) in, the described method preparing metallic back electrode layer on hole transmission layer is: 4 × 10
-4hot vapour deposition method is adopted to prepare metallic back electrode layer under vacuum condition on hole transmission layer.
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