CN112687803B - Application of diprophylline in inverted perovskite solar cell and preparation method of device - Google Patents
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- CN112687803B CN112687803B CN202011556532.5A CN202011556532A CN112687803B CN 112687803 B CN112687803 B CN 112687803B CN 202011556532 A CN202011556532 A CN 202011556532A CN 112687803 B CN112687803 B CN 112687803B
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Abstract
The invention relates to an application of diprophylline in an inverted perovskite solar cell and a preparation method of a device, belonging to the technical field of solar cells. According to the invention, diprophylline is doped with poly [3- (4-carboxybutyl) thiophene-2, 5-diyl ] -sodium and then is used for preparing a hole transport layer of the inverted perovskite solar cell, and the photoelectric conversion efficiency of the inverted perovskite solar cell with the hole transport layer reaches 20.87%, and the inverted perovskite solar cell has excellent long-term stability. Further, after the hole transport layer prepared by doping the diprophylline with the P3CT-Na is subjected to ultrasonic treatment for 10min, the layer still has an integral thin film and shows good durability, and the inverted perovskite solar cell prepared by the layer still maintains high efficiency of 18.77%.
Description
Technical Field
The invention belongs to the technical field of solar cells, and particularly relates to an application of diprophylline in an inverted perovskite solar cell and a preparation method of a device.
Background
Over the past decade, the power conversion efficiency of perovskite solar cells has breached 25%. Perovskite solar cells are considered promising photovoltaic technology, combining the excellent photovoltaic properties of perovskite materials, low cost, ease of fabrication and solution processability. Inverted perovskite solar cells have the potential for ease of fabrication, low temperature processing, negligible hysteresis effects, and large-scale production and flexible applications, making them highly competitive in future commercialization. The deposition of the hole transport layer on the surface of the indium tin oxide electrode in an inverted perovskite solar cell can modify the work function of the indium tin oxide and also affect the ohmic contact at the indium tin oxide/perovskite interface. Meanwhile, the hole transport layer is under the perovskite layer, and thus it affects the growth of perovskite crystals and the quality of the perovskite film. High quality perovskite thin films not only help to improve the power conversion efficiency of the cell, but also affect the stability of the device. Therefore, the hole transport layer is very important for improving the photovoltaic performance of the inverted perovskite solar cell. Poly [3- (4-carboxybutyl) thiophene-2, 5-diyl ] (P3 CT) is one of the commonly used polymer hole transport materials, but P3CT has some disadvantages, such as insufficient energy level matching with perovskite materials, strong aggregation and large surface energy, which makes the P3 CT-based device performance difficult to further improve. Therefore, it is necessary to improve the performance of P3CT hole transport materials by some strategies.
Disclosure of Invention
In view of the above, an object of the present invention is to provide an application of diprophylline in an inverted perovskite solar cell; the second purpose is to provide an inverted perovskite solar cell; the third purpose is to provide a preparation method of the inverted perovskite solar cell.
In order to achieve the purpose, the invention provides the following technical scheme:
1. the application of the diprophylline in the inverted perovskite solar cell specifically comprises the following steps: the diprophylline is doped with poly [3- (4-carboxyl butyl) thiophene-2, 5-diyl ] -sodium and then is used for preparing a hole transport layer of the inverted perovskite solar cell.
2. The inverted perovskite solar cell is formed by sequentially laminating a conductive substrate layer, a hole transport layer, a perovskite light absorption layer, an electron transport layer, a buffer layer and a metal back electrode from bottom to top, wherein the hole transport layer is prepared by dihydroxypropyl theophylline doped poly [3- (4-carboxybutyl) thiophene-2, 5-diyl ] -sodium.
Preferably, the conductive substrate layer is ITO; the perovskite light absorption layer is MAPbI 3-x Cl x A perovskite light-absorbing layer; the electron transport layer is C 60 An electron transport layer; the buffer layer is a BCP buffer layer; the metal back electrode is Ag.
Preferably, the mass ratio of the diprophylline to the poly [3- (4-carboxybutyl) thiophene-2, 5-diyl ] -sodium is 0.1-1.
3. The preparation method of the inverted perovskite solar cell comprises the following steps:
(1) Pretreating the conductive substrate;
(2) Spin-coating on the conductive substrate treated in the step (1) to prepare a hole transport layer;
(3) Spin-coating the hollow hole transmission layer in the step (2) to prepare a perovskite light absorption layer;
(4) And (4) sequentially evaporating an electron transmission layer, a buffer layer and a metal back electrode on the perovskite light absorption layer in the step (3).
Preferably, in the step (1), the conductive substrate is pretreated as follows: conducting ultrasonic treatment on the conductive substrate ITO by using a glass cleaning agent, deionized water and absolute ethyl alcohol in sequence, drying by using nitrogen, and then treating by using oxygen plasma.
Preferably, in the step (2), the method for preparing the hole transport layer by spin coating comprises the following steps: adding diprophylline into poly [3- (4-carboxyl butyl) thiophene-2, 5-diyl ] -sodium solution, uniformly mixing to obtain a precursor solution, dripping the precursor solution onto a conductive substrate, spin-coating for 50-60s at the speed of 3000-5000rpm, and finally annealing at 120-150 ℃ for 20-30min.
Preferably, the poly [3- (4-carboxybutyl) thiophene-2, 5-diyl ] -sodium solution is prepared as follows: adding poly [3- (4-carboxybutyl) thiophene-2, 5-diyl ] and sodium hydroxide into water according to the mass ratio of 1-10, and stirring at room temperature for 1-3d to obtain the compound.
Preferably, in the step (3), the method for preparing the perovskite light absorption layer by spin coating comprises the following steps: MAPbI is added 3-x Cl x Dropping perovskite precursor on the hole transport layer, spin-coating at 300-500rpm for 3-5s, spin-coating at 3000-5000rpm for 30-50s, annealing at 40-60 deg.C for 1-3min, and annealing at 80-100 deg.C for 20-30min, wherein MAPbI is added in the hole transport layer 3-x Cl x When the precursor solution starts to spin for 10-12s, 100-200 μ L of the anti-solvent is dropped within 3-5 s.
Preferably, the antisolvent is one of chlorobenzene, toluene or anisole.
Preferably, in the step (4), the degree of vacuum at the time of vapor deposition is 10 -4 ～10 -3 Pa。
The invention has the beneficial effects that: the invention provides an application of diprophylline in an inverted perovskite solar cell and a preparation method of a device, wherein the photoelectric conversion efficiency of the inverted perovskite solar cell using diprophylline doped poly [3- (4-carboxybutyl) thiophene-2, 5-diyl ] -sodium (P3 CT-Na) as a hole transport layer reaches 20.87%, and the inverted perovskite solar cell has excellent long-term stability. Further, after the hole transport layer prepared by doping the diprophylline with the P3CT-Na is subjected to ultrasonic treatment for 10min, the layer still has an integral thin film and shows good durability, and the inverted perovskite solar cell prepared by the layer still maintains high efficiency of 18.77%.
In the present invention, diprophylline changes its work function by self-assembly onto the surface of an ITO conductive substrate because diprophylline can self-assemble onto the ITO conductive substrate through hydroxyl groups, introducing a dipole moment at the interface, which can increase the work function of ITO by bending the vacuum level. Meanwhile, the durability of the hole transport layer prepared from P3CT-Na can be improved by doping diprophylline, because P3CT-Na is firmly fixed on the ITO conductive substrate through the hydrogen bond interaction (action 1) of diprophylline and P3CT-Na and the self-assembly bond (action 2) formed by diprophylline and ITO, thereby finally improving the durability of the hole transport layer (see figure 1). In addition, the interaction between P3CT-Na and diprophylline induces the ordered arrangement of polymer molecules P3CT-Na, thereby reducing the light scattering inside the P3CT-Na film and improving the light transmittance of the hole transport layer. Furthermore, in the preparation of perovskite film by spin coating, dihydroxypropyltheophylline doped in P3CT-Na is partially dissolved in the perovskite as the upper layer, and from the viewpoint of molecular structure, carbonyl group may react with Pb in perovskite due to the presence of carbonyl functional group on heterocyclic ring part of dihydroxypropyltheophylline 2+ Strong interactions are generated which increase the activation energy of perovskite nucleation and slow down the nucleation process of perovskite crystals thereby improving the crystallinity of the perovskite thin film.
Additional advantages, objects, and features of the invention will be set forth in part in the description which follows and in part will become apparent to those having ordinary skill in the art upon examination of the following or may be learned from practice of the invention. The objectives and other advantages of the invention may be realized and attained by the means of the instrumentalities and combinations particularly pointed out hereinafter.
Drawings
For the purposes of promoting a better understanding of the objects, aspects and advantages of the invention, reference will now be made to the following detailed description taken in conjunction with the accompanying drawings in which:
FIG. 1 is a schematic view showing the action of diprophylline with P3CT-Na and ITO, respectively;
FIG. 2 is a graph of the infrared test results of diprophylline, P3CT-Na and a mixture of the two;
fig. 3 is a graph showing the results of light transmittance tests of the hole transport layers prepared in example 1, example 2 and comparative example;
fig. 4 is a current-voltage graph of inverted perovskite solar cells prepared in example 1, example 2 and comparative example;
fig. 5 is a graph showing results of external quantum efficiency tests of inverted perovskite solar cells prepared in example 1, example 2 and comparative example;
fig. 6 is a graph showing the results of long-term stability tests of the inverted perovskite solar cells prepared in example 1 and comparative example;
fig. 7 is a graph showing the results of photoelectric property tests of devices prepared on the basis of the hole transport layers of example 1 and comparative examples after being subjected to ultrasonic cleaning treatment for 10 min.
Detailed Description
The embodiments of the present invention are described below with reference to specific embodiments, and other advantages and effects of the present invention will be easily understood by those skilled in the art from the disclosure of the present specification. The invention is capable of other and different embodiments and of being practiced or of being carried out in various ways, and its several details are capable of modification in various respects, all without departing from the spirit and scope of the present invention.
Example 1
Preparing an inverted perovskite solar cell, wherein the cell sequentially comprises an ITO conductive substrate layer, a hole transport layer prepared by doping P3CT-Na with diprophylline, and MAPbI from bottom to top 3-x Cl x Perovskite light-absorbing layer, C 60 The electron transport layer, the BCP buffer layer and the Ag electrode are laminated, and the preparation method comprises the following steps:
(1) Adding P3CT and sodium hydroxide into water according to the mass ratio of 1;
(2) Carrying out ultrasonic treatment on an ITO conductive substrate sequentially through a glass cleaning agent, deionized water and absolute ethyl alcohol, then drying the ITO conductive substrate through nitrogen, and then carrying out oxygen plasma treatment for 180s for later use;
(3) Adding diprophylline into the P3CT-Na solution prepared in the step (1), uniformly mixing to obtain a precursor solution, dripping the precursor solution onto the ITO conductive substrate treated in the step (2), spin-coating at the speed of 4000rpm for 60s, and finally annealing at 140 ℃ for 30min to prepare a hole transport layer, wherein the concentration of diprophylline in the precursor solution is 0.5mg/mL, and the concentration of P3CT-Na in the precursor solution is 1 mg/mL;
(4) MAPbI is added 3-x Cl x Dropwise adding the perovskite precursor on the hole transport layer prepared in the step (3), spin-coating at the speed of 400rpm for 3s, then spin-coating at the speed of 4000rpm for 30s, finally annealing at 50 ℃ for 2min, and then annealing at 85 ℃ for 25min, wherein MAPbI is added on the hole transport layer 3-x Cl x At 11s after the precursor liquid starts to spin, 170 mu L chlorobenzene is dripped in 4s to prepare MAPbI 3-x Cl x A perovskite light-absorbing layer;
(5) Under high vacuum (10) -4 Pa), MAPbI produced in step (4) by thermal evaporation 3-x Cl x Sequentially evaporating C with the thickness of 40nm on the perovskite light absorption layer 60 The electron transport layer, the BCP buffer layer with the thickness of 6nm and the Ag electrode with the thickness of 100 nm.
Example 2
The difference from example 1 is that in step (3), the concentration of diprophylline in the precursor solution is 1mg/mL.
Comparative examples
The difference from example 1 is that, in step (3), the hole transport layer was prepared by spin coating directly with a P3CT-Na solution without adding diprophylline.
The results of infrared tests on diprophylline, P3CT-Na and the mixture of the two are shown in figure 2, and as can be seen from figure 2, the hydroxyl peak in the mixture of diprophylline and P3CT-Na has obvious change compared with diprophylline, thus proving the interaction between diprophylline and P3 CT-Na.
The light transmittances of the hole transport layers prepared in example 1, example 2 and comparative example were respectively tested, and as can be seen from fig. 3, all three had higher transmittances, wherein the hole transport layer in example 1 had higher transmittances in the visible light range, which is attributed to the fact that the interaction between P3CT-Na and dyphylline induces the ordered arrangement of P3CT-Na molecules, and light scattering inside the hole transport layer can be reduced.
Under simulated AM 1.5G sunlight (light intensity of 100 mW/cm) 2 ) The inverted perovskite solar cells prepared in example 1, example 2 and comparative example were tested for current-voltage curves, respectively, with a forward scan of-0.2V → 1.2V and a scan rate of 50mV/S, with the results shown in table 1 and fig. 4.
TABLE 1 optoelectronic Property parameters of the devices
| Test sample | Open circuit voltage (V) | Short circuit current (mA/cm) 2 ) | Filling factor (%) | Efficiency (%) |
| Comparative examples | 1.094 | 20.62 | 80.24 | 18.10(17.22±0.43) |
| Example 1 | 1.120 | 22.19 | 83.98 | 20.87(20.43±0.30) |
| Example 2 | 1.115 | 21.61 | 82.87 | 19.97(19.32±0.37) |
As can be seen from FIG. 4 and Table 1, the photoelectric performance parameters of the devices of examples 1 and 2 are superior to those of the devices of the comparative example, wherein the photoelectric efficiency of the devices prepared in example 1 is as high as 20.87%, the open-circuit voltage is 1.120V, and the short-circuit current is 22.19mA/cm 2 The filling factor is as high as 83.98 percent.
The external quantum efficiencies of the inverted perovskite solar cells prepared in example 1, example 2 and comparative example were respectively tested at different wavelengths using a lock-in amplifier (SR-830), and the results are shown in fig. 5, and it can be seen from fig. 5 that the highest optical response was observed in the wavelength range of 300nm to 800nm for the device prepared in example 1.
Using equipment in a glove box at room temperature under N 2 The long-term stability of the inverted perovskite solar cells prepared in example 1 and comparative example was tested in the environment for a duration of 50 days, and the results are shown in fig. 6. As can be seen from fig. 6, the devices prepared in example 1 maintained 92% of the initial photovoltaic efficiency value after 50 days, while the devices prepared in comparative example decreased to about 83% of the initial photovoltaic efficiency value after 50 days.
Respectively carrying out ultrasonic cleaning treatment for 10min on the hole transport layers prepared in the embodiment 1 and the comparative embodiment 1, preparing perovskite by spin coating, and evaporating C 60 The electron transport layer, the BCP buffer layer and the Ag electrode are prepared into two devices, the photoelectric properties of the two devices are respectively tested, the result is shown in figure 7, and as can be seen from figure 7, after the hole transport layer prepared by doping the diprophylline with the P3CT-Na is subjected to ultrasonic treatment for 10min, the layer still has a complete film and shows good durability, so that the hole transport layer prepared by the method has good durability and can be used for manufacturing the semiconductor deviceThe device still maintains a high efficiency of 18.77%.
Finally, the above embodiments are only intended to illustrate the technical solutions of the present invention and not to limit the present invention, and although the present invention has been described in detail with reference to the preferred embodiments, it will be understood by those skilled in the art that modifications or equivalent substitutions may be made on the technical solutions of the present invention without departing from the spirit and scope of the technical solutions, and all of them should be covered by the claims of the present invention.
Claims (10)
1. The application of the diprophylline in the inverted perovskite solar cell is characterized by comprising the following specific steps: the diprophylline is doped with poly [3- (4-carboxyl butyl) thiophene-2, 5-diyl ] -sodium and then is used for preparing a hole transport layer of the inverted perovskite solar cell;
the conductive substrate layer of the inverted perovskite solar cell is ITO.
2. An inverted perovskite solar cell is formed by stacking a conductive substrate layer, a hole transport layer, a perovskite light absorption layer, an electron transport layer, a buffer layer and a metal back electrode from bottom to top in sequence, and is characterized in that the hole transport layer is prepared by dihydroxypropyl theophylline doped poly [3- (4-carboxybutyl) thiophene-2, 5-diyl ] -sodium;
the conductive substrate layer is ITO.
3. The inverted perovskite solar cell of claim 2, wherein the perovskite light absorbing layer is MAPbI 3-x Cl x A perovskite light-absorbing layer; the electron transport layer is C 60 An electron transport layer; the buffer layer is a BCP buffer layer; the metal back electrode is Ag.
4. The inverted perovskite solar cell of claim 3, wherein the mass ratio of the dihypophylline to the poly [3- (4-carboxybutyl) thiophene-2, 5-diyl ] -sodium is 0.1-1.
5. A method of fabricating an inverted perovskite solar cell as claimed in any one of claims 2 to 4, wherein the method comprises:
(1) Pretreating the conductive substrate;
(2) Spin-coating on the conductive substrate treated in the step (1) to prepare a hole transport layer;
(3) Spin-coating the hollow hole transmission layer in the step (2) to prepare a perovskite light absorption layer;
(4) And (4) sequentially evaporating an electron transmission layer, a buffer layer and a metal back electrode on the perovskite light absorption layer in the step (3).
6. The method of claim 5, wherein in step (1), the conductive substrate is pretreated as follows: the ITO conductive substrate is subjected to ultrasonic treatment by a glass cleaning agent, deionized water and absolute ethyl alcohol in sequence, then is dried by nitrogen, and then is subjected to oxygen plasma treatment.
7. The method of claim 5, wherein in step (2), the spin coating is performed to form the hole transport layer by: adding diprophylline into poly [3- (4-carboxybutyl) thiophene-2, 5-diyl ] -sodium solution, uniformly mixing to obtain a precursor solution, dripping the precursor solution onto a conductive substrate, spin-coating at the speed of 3000-5000rpm for 50-60s, and finally annealing at 120-150 ℃ for 20-30min.
8. The method of claim 7, wherein the solution of poly [3- (4-carboxybutyl) thiophene-2, 5-diyl ] -sodium is prepared by: adding poly [3- (4-carboxyl butyl) thiophene-2, 5-diyl ] and sodium hydroxide into water according to the mass ratio of 1-10, and stirring and reacting at room temperature for 1-3 d.
9. The method of claim 5, wherein in step (3), the spin coating process for preparing the perovskite light absorbing layer comprises: MAPbI is added 3-x Cl x The perovskite precursor is dripped on the hole transport layer, spin-coated for 3-5s at the speed of 300-500rpm, and then coated at 3000-5000rpSpin coating at speed of m for 30-50s, annealing at 40-60 deg.C for 1-3min, and annealing at 80-100 deg.C for 20-30min, wherein the MAPbI is coated on the substrate 3-x Cl x When the precursor solution starts to spin for 10-12s, 100-200 μ L of the anti-solvent is dropped within 3-5 s.
10. The method according to claim 5, wherein in the step (4), the degree of vacuum in the evaporation is 10 -4 ～10 -3 Pa。
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