CN112071985A - Interface engineering method for improving full-spectrum stability of perovskite solar cell - Google Patents
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Abstract
The invention discloses a method for improving the full spectrum light stability of a perovskite solar cell through interface engineering, which is characterized in that a related device structure comprises transparent conductive glass, an electron transmission layer, an interface layer, a perovskite active layer, a hole transmission layer and a metal electrode layer from bottom to top respectively, the interface layer is introduced between the electron transmission layer and the perovskite active layer, the interface layer is formed by mixing fullerene or fullerene derivatives and phenanthroline derivatives, and the mass ratio of the phenanthroline derivatives to the fullerene or fullerene derivatives is 1: 5-15. The interface layer prevents the electron transport layer from catalytically decomposing the perovskite active layer under illumination, and simultaneously enhances the stability of the interface layer, thereby greatly improving the full spectrum light stability of the perovskite solar cell, and due to the effect of passivating the surface defects of the perovskite, the energy conversion efficiency of the cell is also improved, and the hysteresis phenomenon is slowed down. The method greatly promotes the commercialization of the perovskite solar cell.
Description
Technical Field
The invention belongs to the field of perovskite photovoltaics, and particularly relates to an interface engineering method for improving the full-spectrum stability of a perovskite solar cell.
Background
Organic-inorganic metal halide perovskites have received much attention as solution processed and low cost photovoltaic materials due to their excellent properties of strong light absorption, high carrier mobility, long intrinsic carrier lifetime, low temperature processability, etc. However, the stability of perovskite solar cells has not yet reached industry standards.
At present, metal oxides such as TiO are often adopted in the device structure of the perovskite solar cell with high efficiency2And SnO2As an electron transport layer, however, the perovskite is extremely easy to decompose due to the photocatalysis effect of the electron transport layer under illumination (the ultraviolet part is particularly remarkable), and the degradation occurs at the interface between the electron transport layer and the perovskite, so that the illumination stability of the electron transport layer is greatly influenced. In order to weaken the destructive effect, the invention introduces an interface engineering method for the full spectrum stability of the high perovskite solar cell, and an organic interface layer is prepared between an electron transmission layer and a perovskite active layer, so that the interface recombination is relieved to a great extent, the hysteresis phenomenon is reduced, and more importantly, the full spectrum light stability of the cell is obviously improved. The invention provides a basic approach for improving the full-spectrum light stability of the perovskite solar cell, and has important significance for promoting the commercialization of the perovskite solar cell with low cost and good light stability.
Disclosure of Invention
The invention aims to disclose a method for improving the full-spectrum light stability of a perovskite solar cell, which relieves the interface recombination to a great extent, reduces the hysteresis phenomenon and obviously improves the full-spectrum light stability of the cell.
In order to achieve the purpose, the technical scheme adopted by the invention is as follows:
a method for improving the full spectrum light stability of a perovskite solar cell is provided, the device structure of the perovskite solar cell is as follows from bottom to top: transparent conductive glass, an electron transport layer, a perovskite active layer, a hole transport layer and a metal electrode layer. An 8-15 nm interface layer is inserted between the electron transport layer and the perovskite active layer, the interface layer is formed by mixing fullerene or fullerene derivatives and phenanthroline derivatives, and the mass ratio of the phenanthroline derivatives to the fullerene or fullerene derivatives is 1: 5-15.
Furthermore, the transparent conductive glass is ITO or FTO transparent conductive glass,
furthermore, the square resistance of the ITO or FTO transparent conductive glass is 8-15 omega, the light transmittance is 85-90%, the thickness of the glass is 1-2 mm, and the thickness of the ITO or FTO is 150-300 nm.
Furthermore, the electron transport layer is a tin oxide or titanium oxide nanocrystalline film with a thickness of 30-50 nm.
Further, the fullerene or fullerene derivative is C60PCBM, etc. The phenanthroline derivatives are BCP, Bphen and the like.
Further, the perovskite active layer is MAPbI3Or (FAPBI)3)0.95(MAPbBr3)0.05The thickness of the film is 500-1000 nm.
Further, the hole transport layer material is spiro-OMeTAD, and the thickness is 100-200 nm.
Furthermore, the metal electrode layer is made of gold or silver, and the thickness of the metal electrode layer is 80-140 nm.
The invention also provides a full-spectrum light-stable perovskite solar cell prepared by the method for improving the full-spectrum light stability of the perovskite solar cell.
Further, the preparation of the perovskite solar cell comprises the following steps:
the method comprises the following steps: and cleaning the transparent conductive glass.
Step two: and preparing an electron transport layer. And spin-coating the tin dichloride or titanium dioxide nanocrystal aqueous solution with the mass fraction of 2-4% on the transparent conductive glass at the rotating speed of 3000-5000 rpm for 20-40 s. Then, annealing the sample at 80-200 ℃ for 20-60 min, cooling, and then placing the sample into ultraviolet ozone for treatment for 10-20 min;
step three: and preparing an interface layer. Dissolving 10-15 mg of fullerene or a derivative thereof in 1mL of chlorobenzene, adding 100-200 mu L of 10mg/mL of chlorobenzene solution of phenanthroline derivative, uniformly mixing, then spin-coating the mixed solution on an electron transport layer at 3000-4000 rpm, and heating for 1min at 100-120 ℃;
step four: preparation of MAPbI3Or (FAPBI)3)0.95(MAPbBr3)0.05A perovskite active layer. Wherein MAPbI3The preparation of (a) was as follows: will PbI2、CH3NH3I and DMSO are dissolved in DMF according to the molar ratio of 1:1:1 and are uniformly mixed to prepare a perovskite precursor solution, wherein the volume ratio of the DMSO to the DMF is 1: 8-9; and spin-coating the perovskite precursor solution on the electron transport layer, wherein the rotation speed of the perovskite precursor solution is 1000rpm for the first 10s, the rotation speed of the perovskite precursor solution is 5000rpm for the second 20s, and 0.6-1 mL of diethyl ether is dripped in the electron transport layer at the 15 th s. Then, the sample is thermally treated on a heating table at 80-110 ℃ for 10min to prepare MAPbI3；
(FAPbI3)0.95(MAPbBr3)0.05The preparation of (a) was as follows: 1.33mol of FAPBI3And 0.07mol of MAPbBr3Dissolving the perovskite precursor solution in 800 mu L of DMF and 200 mu L of DMSO to prepare a perovskite precursor solution, then spin-coating the perovskite precursor solution on an electron transport layer, wherein the rotation speed of the electron transport layer is 1000rpm for the first 10s, the rotation speed of the electron transport layer is 5000rpm for the second 20s, and 0.6-1 mL of diethyl ether is dripped in the electron transport layer at the 15 th s. Then, the sample is thermally treated for 10-20 min at 140-180 ℃ on a heating table
Step five: a hole transport layer is prepared. Dripping 0.05-0.06 mol/L spiro-OMeTAD solution on the surface of the perovskite active layer, and spin-coating for 30-40 s at 3000-5000 rpm.
Step six: and preparing a metal electrode layer. And evaporating gold or silver onto the hole transport layer to form a metal electrode layer.
Further, in the fifth step, the spiro-OMeTAD solution further comprises 4-tert-butylpyridine TBP and lithium bistrifluoromethanesulfonylimide (LiTFSI), wherein the ratio of spiro-MeOTAD: and (3) LiTFSI: the molar ratio of TBP is 1: 0.13-0.4: 0.8 to 1.2.
Compared with the prior art, the invention has the following beneficial technical effects:
by introducing the fullerene or fullerene derivative interface layer modified by the phenanthroline derivative between the electron transport layer and the perovskite active layer, the electron transport layer is prevented from being catalytically decomposed by the interface layer under illumination, the phenanthroline derivative pins functional groups or free radicals primarily decomposed by the fullerene and the fullerene derivative, so that the fullerene and the fullerene derivative are prevented from being polymerized or further decomposed under illumination, the molecular structure of the fullerene or the fullerene derivative is stabilized, the stability of an interface layer is enhanced, and the interface layer can passivate the surface defects of perovskite, therefore, interface recombination is relieved to a great extent, hysteresis is reduced, the light stability of the device is obviously enhanced, a basic way is provided for improving the full spectrum light stability of the perovskite solar cell, and the commercialization of the perovskite solar cell with low cost and good light stability is promoted.
Drawings
FIG. 1 is a device structure of a perovskite solar cell in an embodiment of the invention;
FIG. 2 is a schematic illustration of an AFM of an electron transport layer according to an embodiment of the present invention;
FIG. 3 is a scanning electron microscope image of an interfacial layer in an embodiment of the invention;
FIG. 4 is a graph of the infrared spectrum of the interface layer before and after aging in this example;
FIG. 5 is a stability test chart of the perovskite solar cell in the present embodiment under pure ultraviolet light;
FIG. 6 is a test chart of the maximum output power stability of the perovskite solar cell in the present embodiment under simulated sunlight;
FIG. 7 is a test chart of the maximum output power stability of the perovskite solar cell in the present embodiment under simulated sunlight;
fig. 8 is a stability test chart of the perovskite solar cell in the present embodiment under pure ultraviolet light.
Detailed Description
The present invention will be described in further detail with reference to specific examples, which are illustrative of the present invention but not limiting thereto. In this embodiment, the tin dioxide nanocrystal solution (tin dioxide aqueous colloidal dispersion) and the titanium dioxide nanocrystal solution used are obtained from Alfa Aesar and Avantama, respectively, but are not limited thereto.
Example 1
As shown in fig. 1, the device structure of the perovskite solar cell is from bottom to top: the ITO transparent conductive glass comprises a glass substrate and an ITO transparent conductive electrode, an electron transport layer, an interface layer, a perovskite active layer, a hole transport layer and a metal electrode layer. The preparation method comprises the following steps:
firstly, cleaning ITO conductive glass. Selecting ITO conductive glass with the square resistance of 8-15 omega, the light transmittance of 85-90% and the thickness of 2mm, carrying out ultrasonic cleaning in deionized water, acetone, ethanol and isopropanol solutions for 5min in sequence, then blowing the ITO conductive glass with nitrogen for drying, and then treating for 20min by adopting an ultraviolet ozone cleaning machine;
secondly, spin coating an electron transport layer. SnO with the mass fraction of 2.3 percent is prepared2And (3) a nanocrystalline precursor solution. And (3) spin-coating 30uL of tin dioxide precursor solution on the ITO conductive glass at the rotating speed of 3000rpm for 30 s. Then, the sample coated with the electron transport layer by the spin coating is preheated for 30min at 150 ℃ by using a heating table, and is naturally cooled to obtain compact SnO2As shown in figure 2, after cooling, putting into ultraviolet ozone for treatment for 10 min;
and thirdly, spin coating an interface layer. Mixing 10mg of C60Dissolved in 1mL of chlorobenzene, and then 100. mu.L of 10mg/mL BCP solution in chlorobenzene was added for further use. 30 μ L of the precursor solution was spin coated onto the electron transport layer at 3000rpm and heated at 100 ℃ for 1min to obtain a smooth and uniform film as shown in FIG. 3. FIG. 4 is C with/without BCP modification60The infrared spectra of the film after one week of ultraviolet irradiation are compared before and after, and the result can be seen from the figure that C is modified by BCP60The film is 700cm after one week of ultraviolet irradiation-1、741cm-1The C-H peak of (A) shows almost no attenuation, indicating that the functional group or radical decomposed primarily by fullerene and its derivatives is pinned by phenanthroline derivatives (Segura et al [60 ]]Fullerene dimers, chemical Society Reviews,2000,29:13, Yoo et al, tuning the electronic band structure of PCBM by electronic irradiation nanoscales Letters 2011,6:545) to prevent them from polymerizing or further decomposing under light irradiation, and to stabilize the molecular structure of Fullerene or Fullerene derivative, thereby effectively improving the Fullerene or Fullerene derivativeStability of the derivatives in light.
Fourthly, coating the perovskite active layer in a spinning mode. In the prepared perovskite precursor solution, PbI2MAI DMSO 461mg 150mg 78mg 600mg DMF. Spin coating 30uL of perovskite precursor solution on the electron transport layer, wherein the rotation speed of the first 10s is 1000rpm, the rotation speed of the second 20s is 5000rpm, and at the 15 th s, 1mL of diethyl ether is dripped. Then, the sample coated with the perovskite active layer by the spin coating is thermally treated for 10min at 100 ℃ on a heating table to obtain MAPbI3A layer;
and fourthly, spin coating the hole transport layer. A mixed solution of spiro-OMeTAD was prepared by adding 72.3mg of spiro-OMeTAD, 17.5uL of a solution of lithium bistrifluoromethanesulfonylimide in acetonitrile at a concentration of 520mg/mL, and 28.8uL of TBP to 1mL of chlorobenzene solvent. 40uL of spiro-OMeTAD mixed solution is dripped on the surface of the perovskite active layer and is spin-coated for 35s at the rotating speed of 3000 rpm.
Fifthly, metal electrode layers are thermally evaporated. Adopting a thermal evaporation coating machine at-1.0 multiplied by 10-3And thermally evaporating 100nm of gold onto the hole transport layer under Pa vacuum to form a metal electrode layer.
The performance parameters of the perovskite solar cell obtained in this example are shown in table 1, and it is understood that the energy conversion efficiency of the cell is high and the hysteresis is small. According to the ultraviolet irradiation stability test shown in fig. 5, it can be seen that the efficiency of the cell is still maintained above 70% after 1000h of ultraviolet irradiation, which indicates that the stability of the cell against ultraviolet light is strong. The stability of the interface layer is enhanced while the interface layer material is introduced to prevent the electron transport layer from catalytically decomposing the perovskite active layer under illumination, so that the full spectrum light stability of the perovskite solar cell is greatly improved. The method of the present invention greatly facilitates the commercialization of low-cost and photostable perovskite solar cells.
TABLE 1 Performance parameters of perovskite solar cells
Example 2
In this example, the procedure was the same as in example 1 except for the preparation of the electron transport layer. The electron transport layer in this example was prepared as follows: preparing a titanium dioxide nanocrystalline precursor solution with the mass fraction of 1.5%, and dripping the titanium dioxide nanocrystalline precursor solution on FTO at 5000rpm for 20 s. Subsequently, the sample is annealed at 200 ℃ for 20min, and after cooling, the sample is placed in ultraviolet ozone for treatment for 20 min. According to the test of simulating the stable output of the sunlight for 1000 hours in the figure 6, the full spectrum light stability of the cell is stronger.
Example 3
In this example, the procedure was the same as in example 1 except that the preparation of the interface layer was different. The preparation process of the interface layer in the embodiment is as follows: 12.5mg of PCBM was dissolved in 1mL of chlorobenzene, 200. mu.L of a 10mg/mL Bphen solution in chlorobenzene was added, the interface layer was prepared by spin coating at 4000rpm and heated at 120 ℃ for 1 min. According to the aging test of 1000 hours of pure ultraviolet light in FIG. 7, the efficiency is almost not attenuated, and the battery has stronger ultraviolet light resistance.
Example 4
In this example, the procedure was the same as in example 1 except that the perovskite active layer used was prepared differently. The perovskite active layer in the embodiment is prepared as follows: configuring 891mg FAPBI3、33mg MAPbBr3222mg of DMSO and 762mg of DMF. And spin-coating the perovskite precursor solution on the electron transport layer at the rotation speed of 1000rpm for the first 10s and 5000rpm for the last 20s, and dripping 0.6mL of diethyl ether at the 15 th s. Subsequently, the sample is subjected to heat treatment on a heating table at 140-180 ℃ for 20 min. The metal electrode was a 140nm silver electrode. According to the graph 8, the efficiency is almost not attenuated when the test is carried out for simulating the stable output of the sunlight for 1000 hours, and the full spectrum light stability of the cell is stronger.
The above description is only a non-limiting embodiment of the present invention, and it will be apparent to those skilled in the art that various changes and modifications may be made without departing from the inventive concept and without inventive step, and these changes and modifications are all within the scope of the present invention.
Claims (11)
1. An interface engineering method for improving the full spectrum light stability of a perovskite solar cell is characterized in that the device structure of the perovskite solar cell is as follows from bottom to top: transparent conductive glass, an electron transport layer, a perovskite active layer, a hole transport layer and a metal electrode layer. The perovskite-type organic electroluminescent device is characterized in that an 8-15 nm interface layer is inserted between an electron transport layer and a perovskite active layer, the interface layer is formed by mixing fullerene or fullerene derivatives and phenanthroline derivatives, and the mass ratio of the phenanthroline derivatives to the fullerene or fullerene derivatives is 1: 5-15.
2. The interface engineering method for improving the full spectrum light stability of the perovskite solar cell according to claim 1, is characterized in that: the transparent conductive glass is ITO or FTO transparent conductive glass.
3. The interface engineering method for improving the full spectrum light stability of the perovskite solar cell according to claim 2, characterized in that: the square resistance of the ITO or FTO transparent conductive glass is 8-15 omega, the light transmittance is 85-90%, the thickness of the glass is 1-2 mm, and the thickness of the ITO or FTO is 150-300 nm.
4. The interface engineering method for improving the full spectrum light stability of the perovskite solar cell according to claim 1, is characterized in that: the electron transmission layer is a tin oxide or titanium oxide nanocrystalline film with the thickness of 30-50 nm.
5. The interface engineering method for improving the full spectrum light stability of the perovskite solar cell according to claim 1, is characterized in that: the fullerene or fullerene derivative is C60PCBM, etc. The phenanthroline derivatives are BCP, Bphen and the like.
6. The interface engineering method for improving the full spectrum light stability of the perovskite solar cell according to claim 1, is characterized in that: the perovskite active layer is MAPbI3Or (FAPBI)3)0.95(MAPbBr3)0.05The thickness of the film is 500 to 1000nm。
7. The interface engineering method for improving the full spectrum light stability of the perovskite solar cell according to claim 1, is characterized in that: the hole transport layer is made of spirol-OMeTAD and has the thickness of 100-200 nm.
8. The interface engineering method for improving the full spectrum light stability of the perovskite solar cell according to claim 1, is characterized in that: the metal electrode layer is made of gold or silver, and the thickness of the metal electrode layer is 80-140 nm.
9. An interface engineering method for improving the full-spectrum light stability of a perovskite solar cell according to any one of claims 1 to 7.
10. The all-spectral, light-stable perovskite solar cell of claim 8, wherein the preparation of the perovskite solar cell comprises the steps of:
the method comprises the following steps: and cleaning the transparent conductive glass.
Step two: and preparing an electron transport layer. And spin-coating the tin dichloride or titanium dioxide nanocrystal aqueous solution with the mass fraction of 2-4% on the transparent conductive glass at the rotating speed of 3000-5000 rpm for 20-40 s. Then, annealing the sample at 80-200 ℃ for 20-60 min, cooling, and then placing the sample into ultraviolet ozone for treatment for 10-20 min;
step three: and preparing an interface layer. Dissolving 10-15 mg of fullerene or a derivative thereof in 1mL of chlorobenzene, adding 100-200 mu L of 10mg/mL of chlorobenzene solution of phenanthroline derivative, uniformly mixing, then spin-coating the mixed solution on an electron transport layer at 3000-4000 rpm, and heating for 1min at 100-120 ℃;
step four: preparation of MAPbI3Or (FAPBI)3)0.95(MAPbBr3)0.05A perovskite active layer. Wherein MAPbI3The preparation of (a) was as follows: will PbI2、CH3NH3I and DMSO in a ratio of 1:1:1Dissolving the mixture in DMF in a molar ratio, and uniformly mixing to obtain a perovskite precursor solution, wherein the volume ratio of DMSO to DMF is 1: 8-9; and spin-coating the perovskite precursor solution on the electron transport layer, wherein the rotation speed of the perovskite precursor solution is 1000rpm for the first 10s, the rotation speed of the perovskite precursor solution is 5000rpm for the second 20s, and 0.6-1 mL of diethyl ether is dripped in the electron transport layer at the 15 th s. Then, the sample is thermally treated on a heating table at 80-110 ℃ for 10min to prepare MAPbI3；
(FAPbI3)0.95(MAPbBr3)0.05The preparation of (a) was as follows: 1.33mol of FAPBI3And 0.07mol of MAPbBr3Dissolving the perovskite precursor solution in 800 mu L of DMF and 200 mu L of DMSO to prepare a perovskite precursor solution, then spin-coating the perovskite precursor solution on an electron transport layer, wherein the rotation speed of the electron transport layer is 1000rpm for the first 10s, the rotation speed of the electron transport layer is 5000rpm for the second 20s, and 0.6-1 mL of diethyl ether is dripped in the electron transport layer at the 15 th s. Then, the sample is thermally treated for 10-20 min at 140-180 ℃ on a heating table
Step five: a hole transport layer is prepared. Dripping 0.05-0.06 mol/L spiro-OMeTAD solution on the surface of the perovskite active layer, and spin-coating for 30-40 s at 3000-5000 rpm.
Step six: and preparing a metal electrode layer. And evaporating gold or silver onto the hole transport layer to form a metal electrode layer.
11. The all-spectral, photostable perovskite solar cell of claim 9, characterized in that: in the fifth step, the spiro-OMeTAD solution further comprises 4-tert-butylpyridine TBP and lithium bistrifluoromethanesulfonylimide (LiTFSI), wherein the spiro-MeOTAD: and (3) LiTFSI: the molar ratio of TBP is 1: 0.13-0.4: 0.8 to 1.2.
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