CN112993167B - Application of organic ammonium salt modified metal oxide nanoparticles in positive perovskite solar cell and preparation method of device - Google Patents
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Abstract
The invention relates to application of organic ammonium salt modified metal oxide nanoparticles in an upright perovskite solar cell and a preparation method of a device, and belongs to the technical field of solar cells. The organic ammonium salt modified metal oxide nano-particles are used for preparing an electron transport layer of the positive perovskite solar cell. Firstly, through modification of organic ammonium salt, agglomeration of nano particles can be inhibited, and the electrical property of the electron transport layer is improved. In addition, the organic ammonium salt modification can reduce the roughness of the electron transport layer, improve the film wettability, facilitate the growth of later perovskite crystals, increase the grain size of the perovskite film, and achieve better orientation, thereby facilitating the transport of current carriers. Finally, the organic ammonium salt can passivate the defects of the electron transport layer/perovskite layer interface and improve interface electrical contact. In a word, the organic ammonium salt modification can improve the carrier transport and collection efficiency, so that the bulk phase and interface carrier non-radiative recombination loss is inhibited, and finally the power conversion efficiency and stability of the device are improved.
Description
Technical Field
The invention belongs to the technical field of solar cells, and particularly relates to an application of organic ammonium salt modified metal oxide nanoparticles in an upright perovskite solar cell and a preparation method of a device.
Background
In recent years, organic-inorganic hybrid perovskite materials are widely applied to various photoelectric devices such as solar cells, light emitting diodes, lasers, photodetectors and the like due to the advantages of high molar extinction coefficient, adjustable band gap, low exciton binding energy, high defect tolerance, long carrier diffusion length, solution processability, low cost, flexible preparation and the like. Among them, application to solar cells has been greatly studied. To date, perovskite Solar Cells (PSCs) have achieved a documented certified Power Conversion Efficiency (PCE) of 25.5%. However, the poor operational stability of current PSCs severely hampers their large-scale commercial application. Numerous studies have shown that bulk and interfacial non-radiative recombination losses are the major cause of PCE and stability loss. Therefore, it is imperative to further improve PCE and stability by minimizing bulk and interfacial non-radiative recombination losses.
Patent CN 112201756 describes a perovskite solar cell with an interface modification layer. The method can only passivate the defects of the perovskite thin film. However, the loss in efficiency and stability of the device is not only due to the perovskite light absorbing layer, but the quality of other functional layers also affects the performance of the device. Therefore, this method still has a large limitation.
Disclosure of Invention
In view of the above, an object of the present invention is to provide an application of organic ammonium salt modified metal oxide nanoparticles in an orthosteric perovskite solar cell; the second purpose is to provide an upright perovskite solar cell; the third purpose is to provide a preparation method of the positive perovskite solar cell.
In order to achieve the purpose, the invention provides the following technical scheme:
1. the application of the organic ammonium salt modified metal oxide nanoparticles in the positive perovskite solar cell specifically comprises the following steps: the organic ammonium salt modified metal oxide nano-particles are used for preparing an electron transport layer of the positive perovskite solar cell.
Preferably, the organic ammonium salt has the following structural formula:
in the formula:
R 1 is-NH 2 -OH or-NH 2 ；
R 2 is-CH 2 -、-CH 2 CH 2 -or-CH 2 CH 2 CH 2 -；
R 3 Is composed of
or-NH 3 ；
X is Cl, br, I, BF 4 、PF 6 Or CF 3 SO 3 。
Preferably, the metal oxide nanoparticles are ZnO and TiO 2 、SnO 2 Or CeO 2 At least one of (1).
Preferably, the method for modifying metal oxide nanoparticles with an organic ammonium salt is as follows: and adding the organic ammonium salt aqueous solution into the metal oxide nanoparticle dispersion liquid, and oscillating to obtain the metal oxide nanoparticle dispersion liquid.
Preferably, the mass ratio of the organic ammonium salt to the metal oxide nanoparticles is 0.05-50.
2. The positive perovskite solar cell is formed by sequentially laminating a conductive substrate layer, an electron transmission layer, a perovskite light absorption layer, a hole transmission layer and a metal back electrode from bottom to top, wherein the electron transmission layer is prepared from organic ammonium salt modified metal oxide nanoparticles.
Preferably, the conductive substrate layer is one of ITO or FTO; the perovskite light absorption layer is ABX 3 Perovskite light-absorbing layer, wherein A is CH 3 NH 3 + 、CH(NH 2 ) 2 + 、Cs + Or Rb + B is Pb 2+ 、Sn 2+ Or Ge 2+ At least one of (1), X is Cl - 、Br - Or I - At least one of; the hole transport material is 2,2', 7' -tetra [ N, N-di (4-methoxyphenyl) amino]-9,9' -spirobifluorene, poly [ bis (4-phenyl) (2, 4, 6-trimethylphenyl) amine]At least one of poly (3-hexylthiophene-2, 5-diyl), cuprous thiocyanate, cuprous iodide or nickel oxide; the metal back electrode is one of Au, cu or Ag.
3. The preparation method of the positive perovskite solar cell comprises the following steps:
(1) Pretreating the conductive substrate;
(2) Adding an organic ammonium salt aqueous solution into the metal oxide nanoparticle dispersion liquid, after oscillation, spin-coating on the conductive substrate treated in the step (1) to prepare an electron transport layer, and then carrying out ultraviolet ozone irradiation treatment on the electron transport layer;
(3) Spin-coating the electron transport layer in the step (2) to prepare a perovskite light absorption layer;
(4) Spin-coating the perovskite light absorption layer in the step (3) to prepare a hole transport layer;
(5) And (5) evaporating a metal back electrode on the hollow transmission layer in the step (4).
Preferably, in the step (2), the time of the ultraviolet ozone irradiation treatment is 10-40min.
The invention has the beneficial effects that: the invention provides application of organic ammonium salt modified metal oxide nanoparticles in an upright perovskite solar cell and a preparation method of a device, and an electronic transmission layer of the upright perovskite solar cell is prepared from the organic ammonium salt modified metal oxide nanoparticles. Firstly, through modification of organic ammonium salt, agglomeration of nano particles can be inhibited, and the electrical property of the electron transport layer is improved. In addition, the organic ammonium salt modification can reduce the roughness of the electron transport layer, improve the film wettability, facilitate the growth of later perovskite crystals, increase the grain size of the perovskite film, and achieve better orientation, thereby facilitating the transport of current carriers. Finally, the organic ammonium salt can passivate the defects of the electron transport layer/perovskite layer interface and improve interface electrical contact. In a word, the organic ammonium salt modification can improve the carrier transport and collection efficiency, so that the bulk phase and interface carrier non-radiative recombination loss is inhibited, and finally the power conversion efficiency and stability of the device are improved. And the organic ammonium salt modification reduces the J-V retardation of the battery. The method has simple process and good repeatability when the organic ammonium salt modified metal oxide nano particles are used for preparing the electron transport layer, and has very important significance in promoting the industrialization process of the perovskite solar cell.
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 current-voltage plot for perovskite solar cells in comparative example and example 1;
FIG. 2 is a statistical plot of the hysteresis factor of the perovskite solar cells of comparative example and example 1;
fig. 3 is a statistical graph of low humidity stability and thermal stability of the perovskite solar cell in comparative example and example 1 (fig. 3 (a) is a statistical graph of low humidity stability of the perovskite solar cell in comparative example and example 1, and fig. 3 (b) is a statistical graph of thermal stability of the perovskite solar cell in comparative example and example 1);
FIG. 4 is a current density-voltage plot of the perovskite solar cell of example 2;
FIG. 5 is a current density-voltage plot of the perovskite solar cell of example 3;
FIG. 6 is a current density-voltage plot for the perovskite solar cell of example 4;
FIG. 7 is a current density-voltage plot for the perovskite solar cell of example 5;
FIG. 8 is a current density-voltage plot of the perovskite solar cell of example 6;
fig. 9 is a current density-voltage plot of the perovskite solar cell of example 7.
Detailed Description
The following embodiments of the present invention are provided by way of specific examples, and other advantages and effects of the present invention will be readily apparent to those skilled in the art from the disclosure herein. 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.
Comparative examples
Preparation of perovskite solar cell
(1) Carrying out ultrasonic cleaning on the ITO conductive substrate for 20min by sequentially using a detergent, deionized water and absolute ethyl alcohol, then drying the ITO conductive substrate by using nitrogen, then carrying out ultraviolet ozone treatment for 20min, and cooling the ITO conductive substrate for later use;
(2) SnO with mass fraction of 15% 2 Deionized water (V) was added to the nanoparticle dispersion SnO2 :V H2O = 1);
(3) FAI (232.8 mg), MABr (8.0 mg), rbI (15.9 mg), MACl (36.0 mg), pbI 2 (656.9 mg) and PbBr 2 (27.5 mg) was dissolved in a mixed solvent of DMF and DMSO (V) DMF :V DMSO = 8), shaking for 10min to obtain a perovskite solution with the concentration of 1.5mol/L, dropwise adding the perovskite solution onto the electron transport layer prepared in the step (2), carrying out spin coating at the rotating speed of 4000rpm for 30s, dropwise adding 80 mu L of chlorobenzene at the 14 th s before the end of the spin coating, and then annealing at 155 ℃ for 23min to obtain a perovskite light absorption layer;
(4) Dissolving 72.3mg of 2,2', 7' -tetra [ N, N-di (4-methoxyphenyl) amino ] -9,9' -spirobifluorene (Spiro-OMeTAD) in L mL of chlorobenzene, adding 29 mu L of TBP and 18 mu L of Li-TFSI (the concentration is 520mg/mL, the solvent is anhydrous acetonitrile), uniformly mixing, dropwise adding the mixture to the perovskite light absorption layer prepared in the step (3), and carrying out spin coating at the rotating speed of 3000rpm for 30s to prepare a hole transport layer;
(5) Under high vacuum (10) -4 Pa), and evaporating an Au electrode with the thickness of 80nm on the hole transport layer prepared in the step (4) by thermal evaporation.
Example 1
Preparation of perovskite solar cell
The difference from the comparative example is that the step (2) is specifically:
SnO with mass fraction of 15% 2 Adding 0.5mg/mL aqueous solution (V) of organic ammonium salt A into the nanoparticle dispersion SnO2 :V Modifier A = 1) 2 And (2) shaking the nano particles for 5min, dripping the nano particles onto the ITO conductive substrate treated in the step (1), spin-coating the ITO conductive substrate at the rotating speed of 4000rpm for 30s, annealing the ITO conductive substrate at 150 ℃ for 30min to prepare an electron transport layer, and then carrying out ultraviolet ozone irradiation treatment on the electron transport layer for 10min.
Organic ammonium salts A
Fig. 1 is a current density-voltage curve diagram of the perovskite solar cell in the comparative example and the perovskite solar cell in the example 1, and various photovoltaic parameters of the two cells are obtained according to the curve, and the result is shown in table 1, and the efficiency of the perovskite solar cell in the example 1 is obviously improved according to the graph 1 and the table 1.
TABLE 1
Fig. 2 is a statistical graph of the hysteresis factors of the perovskite solar cells in the comparative example and the example 1, and it can be seen that the hysteresis factor of the perovskite solar cell in the example 1 is significantly reduced.
Fig. 3 is a statistical graph of low humidity stability and thermal stability of the perovskite solar cell in comparative example and example 1, wherein (a) in fig. 3 is a statistical graph of low humidity stability of the perovskite solar cell in comparative example and example 1, and (b) in fig. 3 is a statistical graph of thermal stability of the perovskite solar cell in comparative example and example 1, and it is known that the perovskite solar cell in example 1 exhibits excellent stability in an environment of low humidity (5% to 10%) or 60 ℃.
Example 2
The difference from example 1 is that the concentration of the perovskite solution in step (3) is 1.55mol/L.
Fig. 4 is a current density-voltage plot of the perovskite solar cell of example 2, which has an efficiency of 20.88%, and the device efficiency is significantly improved compared to the efficiency of the cell of the comparative example (19.77%).
Example 3
The difference from example 1 is that the concentration of the perovskite solution in step (3) is 1.6mol/L.
Fig. 5 is a current density-voltage plot of the perovskite solar cell of example 3, which has an efficiency of 21.08%, and a significant improvement in device efficiency compared to the efficiency of the cell of the comparative example (19.77%).
Example 4
The difference from example 1 is that the aqueous solution of the organic ammonium salt A having a concentration of 0.5mg/mL in step (2) is replaced by an aqueous solution of the organic ammonium salt B having a concentration of 5mg/mL
Reacting organic ammonium salt B with SnO 2 The mass ratio of the nanoparticles is 25.
Organic ammonium salts B
Fig. 6 is a current density-voltage graph of the perovskite solar cell of example 4, which has an efficiency of 20.72% and a significant improvement in device efficiency compared to the efficiency of the cell of the comparative example (19.77%).
Example 5
The difference from example 1 is that the aqueous solution of the organic ammonium salt A having a concentration of 0.5mg/mL in step (2) is replaced with an aqueous solution of the organic ammonium salt C having a concentration of 1mg/mL (V) SnO2 :V Modifier B = 1) 2 The mass ratio of the nanoparticles is 5.
Organic ammonium salt C
Fig. 7 is a current density-voltage graph of the perovskite solar cell of example 5, which has an efficiency of 20.68% and a significant improvement in device efficiency compared to the efficiency of the cell of the comparative example (19.77%).
Example 6
The difference from example 1 is that in step (2), 15% by mass of SnO is added 2 And replacing the nano-particle dispersion liquid with 15 mass percent of ZnO nano-particle dispersion liquid.
Fig. 8 is a current density-voltage graph of the perovskite solar cell of example 6, which has an efficiency of 20.55%, which is a significant improvement in device efficiency compared to the efficiency of the cell of the comparative example (19.77%).
Example 7
The difference from example 2 is that in step (2), the organic ammonium salt A is replaced by an organic ammonium salt D.
Organic ammonium salts D
Fig. 9 is a current density-voltage graph of the perovskite solar cell of example 7, which has an efficiency of 21.15%, which is a significant improvement in device efficiency compared to the efficiency of the cell of the comparative example (19.77%).
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 (8)
1. The application of the organic ammonium salt modified metal oxide nanoparticles in the positive perovskite solar cell is characterized by comprising the following specific steps: the organic ammonium salt modified metal oxide nano particles are used for preparing an electron transport layer of the positive perovskite solar cell;
the structural formula of the organic ammonium salt is as follows:
in the formula:
R 1 is-NH 2 -OH or-NH 2 ；
R 2 is-CH 2 -、-CH 2 CH 2 -or-CH 2 CH 2 CH 2 -；
R 3 Is composed of
or-NH 3 ；
X is Cl, br, I, BF 4 、PF 6 Or CF 3 SO 3 。
2. The use of claim 1, wherein the metal oxide nanoparticles are ZnO, tiO 2 、SnO 2 Or CeO 2 At least one of (a).
3. The use according to claim 1, wherein the method for modifying metal oxide nanoparticles with an organic ammonium salt is as follows: and adding the organic ammonium salt aqueous solution into the metal oxide nanoparticle dispersion liquid, and oscillating.
4. The use according to claim 3, wherein the mass ratio of the organic ammonium salt to the metal oxide nanoparticles is 0.05 to 50.
5. The positive perovskite solar cell is formed by stacking a conductive substrate layer, an electron transport layer, a perovskite light absorption layer, a hole transport layer and a metal back electrode from bottom to top in sequence, and is characterized in that the electron transport layer is prepared from organic ammonium salt modified metal oxide nanoparticles;
the structural formula of the organic ammonium salt is as follows:
in the formula:
R 1 is-NH 2 -OH or-NH 2 ；
R 2 is-CH 2 -、-CH 2 CH 2 -or-CH 2 CH 2 CH 2 -；
R 3 Is composed of
or-NH 3 ；
X is Cl, br, I, BF 4 、PF 6 Or CF 3 SO 3 。
6. The orthoperovskite solar cell of claim 5, wherein the conductive substrate layer is one of ITO or FTO; the perovskite light absorption layer is ABX 3 Perovskite light-absorbing layer, wherein A is CH 3 NH 3 + 、CH(NH 2 ) 2 + 、Cs + Or Rb + B is Pb 2+ 、Sn 2+ Or Ge 2+ At least one of (1), X is Cl - 、Br - Or I - At least one of; the hole transport layer is 2,2', 7' -tetra [ N, N-di (4-methoxyphenyl) amino]-9,9' -spirobifluorene, poly [ bis (4-phenyl) (2, 4, 6-trimethylphenyl) amine]At least one of poly (3-hexylthiophene-2, 5-diyl), cuprous thiocyanate, cuprous iodide or nickel oxide; the metal back electrode is one of Au, cu or Ag.
7. The method of manufacturing an orthoperovskite solar cell as defined in claim 5, wherein the method comprises:
(1) Pretreating the conductive substrate;
(2) Adding an organic ammonium salt aqueous solution into the metal oxide nanoparticle dispersion liquid, after oscillation, spin-coating on the conductive substrate treated in the step (1) to prepare an electron transport layer, and then carrying out ultraviolet ozone irradiation treatment on the electron transport layer;
(3) Spin-coating the electron transport layer in the step (2) to prepare a perovskite light absorption layer;
(4) Spin-coating the perovskite light absorption layer in the step (3) to prepare a hole transport layer;
(5) And (4) evaporating a metal back electrode on the hole transmission layer in the step (4).
8. The method according to claim 7, wherein in the step (2), the ultraviolet ozone irradiation treatment time is 10 to 40min.
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