CN111628080A - Perovskite solar cell and preparation method of perovskite absorption layer - Google Patents
Perovskite solar cell and preparation method of perovskite absorption layer Download PDFInfo
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Abstract
The invention provides a perovskite solar cell and a preparation method of a perovskite absorption layer used in the perovskite solar cell. The perovskite solar cell comprises a substrate, a transparent electrode, an electron transport layer, a perovskite absorption layer, a hole transport layer and a back electrode, wherein the perovskite absorption layer is a 2D/3D composite perovskite absorption layer, and the 2D/3D composite perovskite absorption layer comprises a 2D perovskite material and a 3D perovskite material. The preparation method of the 2D/3D composite perovskite absorption layer comprises the step of reacting a solution of one or more lead halides with a solution of an organic cationic compound mixture, wherein the solution of the organic cationic compound mixture comprises one or more organic cationic compounds and one or more dopants, and the dopants are organic long-chain cationic compounds with longer ionic radius than that of the organic cationic compounds.
Description
Technical Field
The invention relates to a perovskite solar cell and a preparation method of a perovskite absorption layer.
Background
The perovskite solar cell is a thin-film solar cell taking an organic-inorganic hybrid perovskite material as a light absorption layer. The organic-inorganic hybrid perovskite material has the outstanding advantages of high photoelectric conversion efficiency, low cost, simple manufacture and the like, and becomes one of the most promising solar cells.
Perovskite materials are specifically different structures, such as 3D (three-dimensional) structure perovskite materials and 2D (two-dimensional) layered structure perovskite materials, and the like. The current research is mainly focused on 3D structure perovskite solar cells, and the conversion efficiency of the perovskite solar cells is about 23 percent. However, 3D-structured perovskite materials also have some disadvantages, such as poor stability. This severely restricts the commercial development of 3D-structured perovskite solar cells.
Compared with the perovskite material with the 3D structure, the perovskite material with the 2D structure has more excellent stability, and has two characteristics of adjustable photoelectric property and excellent environmental stability. However, the 2D perovskite material has problems of low absorption coefficient, poor charge transport capacity, large exciton binding capacity, and the like, resulting in poor photovoltaic performance and low battery efficiency.
Therefore, it is desirable in the art to produce a perovskite solar cell having both high conversion efficiency of 3D-structured perovskite materials and good stability of 2D-structured perovskite materials.
Disclosure of Invention
It is an object of the present invention to provide a perovskite solar cell with both high conversion efficiency and good stability, which has the advantages of high absorption coefficient, excellent charge transport and low exciton binding energy of 3D perovskite materials, while having easy film formation and good water tolerance of 2D perovskite layered structures.
In order to achieve the above object, the present invention provides a perovskite solar cell comprising a substrate, a transparent electrode, an electron transport layer, a perovskite absorption layer, a hole transport layer and a back electrode, wherein the perovskite absorption layer is a 2D/3D composite perovskite absorption layer, and the 2D/3D composite perovskite absorption layer comprises a 2D perovskite material and a 3D perovskite material.
The material of the substrate is selected from glass or transparent polymer.
The transparent electrode is a transparent conductive oxide thin film, including but not limited to fluorine-doped tin oxide (FTO), Indium Tin Oxide (ITO), and the like.
Such electron transport layers include, but are not limited to, titanium dioxide (TiO)2) Tin oxide (SnO)2) Wide bandgap semiconductors such as zinc oxide (ZnO), and organic materials such as fullerene derivatives (PCBM).
The above hole transport layer includes, but is not limited to, Spiro-OMeTAD (2,2 ', 7, 7' -tetrakis [ N, N-bis (4-methoxyphenyl) amino group)]-9, 9' -spirobifluorene), PTAA (poly [ bis (4-phenyl) (2,4, 6-trimethylphenyl) amine]) PEDOT, PASS (polyethylenedioxythiophene-poly (styrenesulfonate)) or CuSCN (cuprous thiocyanate), graphite, NiOx(nickel oxide), and the like.
The back electrode is a metal back electrode, and the metal back electrode is selected from Au, Ag or Al and the like. The metal back electrode can be formed by evaporating a layer of Au, Ag and Al thin film as an electrode by using a method such as evaporation.
The perovskite absorption layer is a 2D/3D composite perovskite absorption layer, and the 2D/3D composite perovskite absorption layer comprises a 2D perovskite material and a 3D perovskite material. The invention integrates the advantages of 2D and 3D perovskite materials, thereby improving the performance and stability of the perovskite solar cell.
The structural general formula of the 2D perovskite material is as follows:
(RNH3)2An-1PbnX3n+1；
wherein:
r is a hydrocarbon group with the carbon number more than 1, preferably a linear chain or branched chain alkyl group with the carbon number of 3-5, including but not limited to CH3CH2CH2CH2-; cycloalkyl having 3 to 5 carbon atoms including, but not limited to, C3H5-; and aralkyl having 1 to 3 carbon atoms in the alkyl chain, including but not limited to C6H5CH2-、C6H5CH2CH2-。
A is CH3NH3 +(denoted as MA), HN ═ CHNH3 +(denoted as FA) and the like,
x is selected from I-、Br-、Cl-A halogen anion;
when n ═ 1, represents a pure 2D layered structure; when n is more than 1, representing a quasi-two-dimensional structure; n ═ infinity, and is a 3D structure.
Due to the introduction of organic cations (RNH)3 +) The radius does not satisfy the range required to satisfy the perovskite structure tolerance factor, and thus does not match that required by PbX6The octahedron cavity is formed by octahedron, the symmetry of the cuboids is broken, and the inorganic lead halide layer in the original 3D structure is separated along the octahedron cavity<001>Or<110>Oriented lamellar structures to accommodate such organic long chain cations.
Preferably, the 2D perovskite material of the invention is selected from (BA)2(MA)n-1PbnI3n+1(BA represents CH)3CH2CH2CH2NH3 +)、CA2(MA)n-1PbnI3n+1(CA represents C)3H5NH3 +)、(PMA)2(MA)n-1PbnI3n+1(PMA represents C6H5CH2NH3 +)、(PEA)2(MA)n-1PbnI3n+1(PEA represents C)6H5CH2CH2NH3 +)、(BA)2(FA)n-1PbnI3n+1、(BA)2(MAxFA1-x)n-1PbnI3n+1(x＝0～1)、CA2(FA)n-1PbnI3n+1、CA2(MAxFA1-x)n-1PbnI3n+1(x＝0～1)、(PEA)2(MA)n-1PbnI3n+1、(PEA)2(FA)n-1PbnI3n+1、(PEA)2(MAxFA1-x)n-1PbnI3n+1(x＝0～1)、(PEA)2(MAxFA1-x)n-1Pbn(I1- yBry)3n+1(x is 0 to 1, and y is 0 to 1), wherein n is an integer greater than or equal to 1.
The structural general formula of the 3D perovskite material is as follows:
ABX3；
wherein A is organic cation such as MA, FA, etc.;
b is Pb2+、Sn2+An isometalated cation;
x is I-、Br-、Cl-A halogen anion.
Preferably, the 3D perovskite material of the present invention is selected from MAPbI3、FAPbI3、MAPbI3-xBrx(x＝0-3)、MAPbI3-xClx(x＝0-3)、MAxFA1-xPbI3(x＝0-1)、MAxFA1-xPbI3-yBry(x＝0-1,y＝0-3)、MAxFA1- xPbI3-yCly(x＝0-1,y＝0-3)、FAPbI3/MAPbBr3。
Preferably, the 2D/3D composite perovskite absorber layer material is selected from the group consisting of:
(BA)2(MA)n-1PbnI3n+14/MAPbI3；
A2(MA)n-1PbnI3n+1/MAPbI3；
(PMA)2(MA)n-1PbnI3n+1/(FAPbI3)x(MAPbBr3)1-x(x is 0 to 1); or
(PEA)2(MA)n-1PbnI3n+1/FAPbClxI3-x(x＝0～3)；
N in the above formula is an integer of 1 or more.
In the 2D/3D composite perovskite absorption layer, the content of the 2D perovskite material is 0.01-10 mol%, preferably 0.5-5 mol%.
The 2D perovskite material is introduced into the 3D perovskite precursor through molecular engineering according to a certain molar ratio, and the 2D perovskite does not change the structure of the 3D perovskite, so that the advantages of high light absorption coefficient, excellent charge transmission and low exciton binding energy of the 3D perovskite are ensured, and the 2D perovskite layered structure has the advantages of easy film formation and good water tolerance.
The perovskite solar cell provided by the invention has the structure as shown in figure 1.
The perovskite solar cell shown in figure 1 sequentially comprises a substrate (1-1), a transparent electrode (1-2), an electron transport layer (1-3), a 2D/3D composite perovskite absorption layer (1-4), a hole transport layer (1-5) and a back electrode (1-6) from bottom to top.
In another embodiment, the substrate (1-1) and the transparent electrode (1-2) can be replaced by a transparent conductive substrate.
The invention also provides a method of preparing a 2D/3D composite perovskite absorber layer, the method comprising the step of reacting a solution of one or more lead halides with a solution of a mixture of organic cationic compounds comprising one or more organic cationic compounds and one or more dopants which are organic long-chain cationic compounds having a longer ionic radius than the ionic radius of the organic cationic compounds.
In a preferred embodiment, the present invention provides a method of preparing a 2D/3D composite perovskite absorber layer comprising the sequential steps of:
a: dissolving one or more lead halides in a first solvent to obtain a lead halide solution;
b: depositing the lead halide solution on a substrate, and heating to obtain a lead halide layer;
c: dissolving one or more organic cationic compounds and one or more doping agents in a second solvent to obtain an organic cationic compound mixed solution; the dopant is an organic long-chain cationic compound, and the ionic radius of the dopant is larger than that of the organic cationic compound;
d: and dripping the organic cationic compound mixed solution onto the lead halide layer, and heating after spin coating to obtain the 2D/3D composite perovskite absorption layer.
The deposition in step b) may be carried out by conventional methods in the art, including but not limited to spin coating and the like.
The lead halide is selected from PbI2、PbCl2And PbBr2One or more of (a).
The first solvent is selected from one of N, N-Dimethylformamide (DMF) and dimethyl sulfoxide (DMSO) or a mixture thereof.
The second solvent is isopropanol.
The organic cation compound is selected from one or more of FAI, MAI, MABr, MACl, FACL and FABr.
The dopant of the present invention is an organic long-chain cationic compound having an ionic radius longer than that of the organic cationic compound, and is selected from one or more of BAI, BABr, CAI, PMAI, PMABr, PEAI and PEABr. Organic Long-chain cationic Compounds due to the introduction of organic cations (RNH)3 +) The radius does not satisfy the range required to satisfy the perovskite structure tolerance factor, and thus does not match that required by PbX6The octahedron cavity is formed by octahedron, the symmetry of the cuboids is broken, and the inorganic lead halide layer in the original 3D structure is separated along the octahedron cavity<001>Or<110>Oriented lamellar structures to accommodate such organic long chain cations.
In the conventional perovskite absorption layer preparation method, usually, organic cation compounds such as FAI or MAI and the like cannot be reacted with PbI2The layers are fully reacted to form a 3D perovskite film containing excess PbI2. The invention introduces a certain amount of organic long-chain cationic compound and organic long-chain amino cation RNH into organic cation isopropanol solution such as FAI, MAI and the like3 +And PbI 22D or quasi-2D perovskite is generated through reaction, the 2D/3D perovskite solar cell is prepared, and the conversion efficiency and stability of the perovskite solar cell are improved.
Drawings
Fig. 1 is a schematic structural diagram of a perovskite solar cell.
Fig. 2 is a schematic structural diagram of a perovskite solar cell of the present invention.
Fig. 3 is a performance test chart of 2D/3D and 3D perovskite solar cells according to an example of the present invention, and the results (a) are a current-voltage graph and (b) are a conversion efficiency distribution chart.
FIG. 4 is a stability analysis of a 2D/3D perovskite solar cell of an embodiment of the invention.
Detailed Description
In order to make the objects, technical solutions and advantages of the present invention more apparent, the present invention will be described in further detail with reference to the accompanying drawings in conjunction with the following detailed description. It should be understood that the description is intended to be exemplary only, and is not intended to limit the scope of the present invention.
Structure of perovskite solar cell:
the present embodiment provides a perovskite solar cell, and the cell structure is shown in fig. 2. The perovskite solar cell sequentially comprises a transparent conductive substrate (101), an electron transport layer (102), a 2D/3D perovskite absorption layer (103), a hole transport layer (104) and a back electrode (105) from bottom to top.
Preparation of perovskite solar cell：
The preparation method of the perovskite solar cell shown in FIG. 2 comprises the following steps:
1) cleaning and ultraviolet ozone treatment of a transparent conductive substrate (101): selecting FTO glass as a transparent conductive substrate 101, ultrasonically cleaning the FTO glass with deionized water, ethanol, acetone and deionized water for 15 to 30 minutes in sequence, then blow-drying the FTO glass with nitrogen, and placing the FTO glass into an ultraviolet ozone machine for treatment for 15 to 30 minutes;
2) preparation of the electron transport layer (102): diluting SnO with deionized water2Colloid of nanocrystalline aqueous solution (15% mass concentration) to SnO with concentration of 2.67%2Depositing SnO on the FTO substrate treated in the step 1) by adopting a spin coating method2An electron transport layer (102) with a spin coating speed of 3000 r/min for 30 s, and after the spin coating is finished, the substrate is placed on a heating table at 180 ℃ for annealing for 20 min to form SnO2An electron transport layer (102);
3) preparation of 2D/3D perovskite absorption layer (103): firstly, PbI is added2Dissolving in mixed solvent of DMF and DMSO (volume ratio of DMF to DMSO is 0.95/0.05) to obtain 600mg/ml solution, and preparing SnO in step 2)2The electron transport layer (102) is spin-coated with PbI2Solution, the spin coating speed is 1500 r/min, the time is 30 seconds, and after the spin coating is finished, the substrate is placed on a heating table at 70 ℃ for annealing for 30min to form PbI2A layer; then, FAI, MABr, MACl were dissolved in 1ml of isopropanol at a ratio of 60mg:6mg:6mg, while PMAI was added thereto at a molar concentration of 2% (PMAI/FAI molar ratio 2: 98); dripping the mixed solution of FAI, MABr, MACl and PMAI into PbI2Spin coating on the layer to prepare 2D/3D perovskite absorption layer at 1500 rpm for 30 s, and annealing the substrate on a heating table at 150 deg.C for 15min to obtain 2D/3D perovskite absorption layer with structure of (PMA)2(MA)n-1PbnI3n+1/(FAPbI3)0.97(MAPbBr3)0.03. The preparation method of the 3D perovskite absorption layer is the same as that of the 2D/3D perovskite absorption layer except that the PMAI is not added into the organic cation mixed solution.
4) Preparation of the hole transport layer (104): to 1ml of chlorobenzene was added 72.3mg of spiro-OMeTAD (2,2 ', 7,7 ' -tetrakis [ N, N-bis (4-methoxyphenyl) amino ] -9,9 ' -spirobifluorene), 28.8. mu.l of TBP (tert-butylpyridine), 17.5. mu.l of Li-TFSI solution (lithium bis (trifluoromethylsulfonyl) amide salt, 520mg of Li-TFSI in 1ml of acetonitrile). The hole transport layer (104) was prepared by spin-coating a spiro-OMeTAD solution on the perovskite absorption layer (103) at a spin speed of 3000 rpm for a period of 30 seconds.
5) Preparation of the back electrode (105): depositing Au electrode on the hole transport layer (104) by evaporation at a thickness of 100nm and a deposition rate of
Performance testing
Under standard test conditions (AM1.5, 25 ℃, 1000W/m)2) The IV performance of the cells was tested and the short circuit current density (J) was measured separatelysc) Open circuit voltage (V)oc) Conversion Efficiency (PCE) and fill factor: (PCE)FF), the results of the specific cell performance parameter tests are shown in figure 3 and table 1.
TABLE 1 Performance parameters of perovskite solar cells
According to table 1 and fig. 3, compared with the 3D perovskite solar cell without doping PMAI, the 2D/3D perovskite solar cell prepared by doping 2% PMAI has a significant increase in short circuit current density and fill factor, and the cell efficiency is improved from 18.34% to 18.88%. This is because the 2D perovskite formed by small amount of PMAI doping can passivate the defects at the perovskite grain boundaries, reducing carrier recombination.
Stability analysis
The stability of the cells was tested in the unpackaged condition (as shown in fig. 4). The test result shows that the 2D/3D perovskite solar cell still maintains 82% of initial efficiency after being stored for 21 days under the condition of no encapsulation, and has good stability compared with the 3D perovskite solar cell.
It is to be understood that the above-described embodiments of the present invention are merely illustrative of or explaining the principles of the invention and are not to be construed as limiting the invention. Therefore, any modification, equivalent replacement, improvement and the like made without departing from the spirit and scope of the present invention should be included in the protection scope of the present invention.
Claims (13)
1. A perovskite solar cell comprising a substrate, a transparent electrode, an electron transport layer, a perovskite absorber layer, a hole transport layer and a back electrode, characterised in that the perovskite absorber layer is a 2D/3D composite perovskite absorber layer, the 2D/3D composite perovskite absorber layer comprising a 2D perovskite material and a 3D perovskite material.
2. The perovskite solar cell according to claim 1, characterized in that the content of the 2D perovskite material in the 2D/3D composite perovskite absorption layer is 0.01-10 mol%.
3. The perovskite solar cell according to claim 2, characterized in that the content of the 2D perovskite material in the 2D/3D composite perovskite absorption layer is 0.5-5 mol%.
4. The perovskite solar cell according to any one of claims 1 to 3, characterized in that in the 2D/3D composite perovskite absorption layer the 2D perovskite material is selected from (BA)2(MA)n-1PbnI3n+1、CA2(MA)n-1PbnI3n+1、(PMA)2(MA)n-1PbnI3n+1、(PEA)2(MA)n-1PbnI3n+1、(BA)2(FA)n-1PbnI3n+1、(BA)2(MAxFA1-x)n-1PbnI3n+1(x＝0～1)、CA2(FA)n-1PbnI3n+1、CA2(MAxFA1-x)n-1PbnI3n+1(x＝0～1)、(PEA)2(MA)n-1PbnI3n+1、(PEA)2(FA)n-1PbnI3n+1、(PEA)2(MAxFA1-x)n-1PbnI3n+1(x＝0～1)、(PEA)2(MAxFA1-x)n-1Pbn(I1-yBry)3n+1(x is 0 to 1, and y is 0 to 1), wherein n is an integer greater than or equal to 1.
5. The perovskite solar cell according to any one of claims 1 to 3, characterized in that in the 2D/3D composite perovskite absorption layer the 3D perovskite material is selected from MAPbI3、FAPbI3、MAPbI3-xBrx(x＝0-3)、MAPbI3-xClx(x＝0-3)、MAxFA1-xPbI3(x＝0-1)、MAxFA1-xPbI3-yBry(x＝0-1,y＝0-3)、MAxFA1-xPbI3-yCly(x＝0-1,y＝0-3)、FAPbI3/MAPbBr3。
6. Perovskite solar cell according to any of claims 1 to 3, characterized in that the 2D/3D composite perovskite absorber layer material is selected from (BA)2(MA)n-1PbnI3n+14/MAPbI3(n＝1-∞)、CA2(MA)n-1PbnI3n+1/MAPbI3(n＝1-∞)、(PMA)2(MA)n-1PbnI3n+1/(FAPbI3)x(MAPbBr3)1-x(x＝0～1)、(PEA)2(MA)n-1PbnI3n+1/FAPbClxI3-x(x＝0～3)。
7. A process for the preparation of a 2D/3D composite perovskite absorption layer as claimed in any one of claims 1 to 6, characterized in that the process comprises the step of reacting a solution of one or more lead halides with a solution of a mixture of organic cationic compounds comprising one or more organic cationic compounds and one or more dopants, said dopants being organic long-chain cationic compounds having a longer ionic radius than the ionic radius of the organic cationic compounds.
8. The method according to claim 7, characterized in that the lead halide is selected from PbI2、PbCl2And PbBr2One or more of (a).
9. The method according to claim 7, characterized in that the organic cationic compound is selected from one or more of the group consisting of FAI, MAI, MABr, MACl, FACI, FABr.
10. The method according to claim 7, characterized in that the organic long-chain cationic compound is selected from one or more of BAI, BABr, CAI, PMAI, PMABr, PEAI and PEABr.
11. Method according to any of claims 7-10, characterized in that it comprises the following sequence of steps:
a: dissolving one or more lead halides in a first solvent to obtain a lead halide solution;
b: depositing the lead halide solution on a substrate, and heating to obtain a lead halide layer;
c: dissolving one or more organic cationic compounds and one or more doping agents in a second solvent to obtain an organic cationic compound mixed solution;
d: and dripping the organic cation compound mixed solution onto the lead halide layer, and heating to obtain the 2D/3D composite perovskite absorption layer.
12. The method according to claim 11, wherein the first solvent is selected from one of N, N-dimethylformamide and dimethylsulfoxide, or a mixture thereof.
13. The method according to claim 12, characterized in that the second solvent is isopropanol.
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| CN114107960B (en) * | 2021-10-22 | 2024-04-26 | 信阳师范学院 | SnO preparation by using stannous oxalate as raw material2Method for forming electron transport layer film |
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| CN115377291A (en) * | 2022-10-21 | 2022-11-22 | 重庆大学 | Bottom-up 2D/3D perovskite heterojunction, preparation method thereof and application thereof in perovskite solar cell |
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