CN112635675A - Perovskite solar cell based on 3-thiophene acetic acid interface modification layer and preparation method thereof - Google Patents
Perovskite solar cell based on 3-thiophene acetic acid interface modification layer and preparation method thereof Download PDFInfo
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- RCNOGGGBSSVMAS-UHFFFAOYSA-N 2-thiophen-3-ylacetic acid Chemical compound OC(=O)CC=1C=CSC=1 RCNOGGGBSSVMAS-UHFFFAOYSA-N 0.000 title claims abstract description 102
- 230000004048 modification Effects 0.000 title claims abstract description 101
- 238000012986 modification Methods 0.000 title claims abstract description 101
- 238000002360 preparation method Methods 0.000 title claims abstract description 29
- 238000004528 spin coating Methods 0.000 claims abstract description 57
- 230000031700 light absorption Effects 0.000 claims abstract description 40
- XOLBLPGZBRYERU-UHFFFAOYSA-N tin dioxide Chemical compound O=[Sn]=O XOLBLPGZBRYERU-UHFFFAOYSA-N 0.000 claims abstract description 40
- 230000005525 hole transport Effects 0.000 claims abstract description 31
- 239000000758 substrate Substances 0.000 claims abstract description 27
- 229910001887 tin oxide Inorganic materials 0.000 claims abstract description 22
- 238000000034 method Methods 0.000 claims abstract description 16
- 238000001704 evaporation Methods 0.000 claims abstract description 8
- 239000000243 solution Substances 0.000 claims description 53
- 238000000137 annealing Methods 0.000 claims description 40
- MVPPADPHJFYWMZ-UHFFFAOYSA-N chlorobenzene Chemical compound ClC1=CC=CC=C1 MVPPADPHJFYWMZ-UHFFFAOYSA-N 0.000 claims description 38
- 239000002243 precursor Substances 0.000 claims description 38
- IAZDPXIOMUYVGZ-UHFFFAOYSA-N Dimethylsulphoxide Chemical compound CS(C)=O IAZDPXIOMUYVGZ-UHFFFAOYSA-N 0.000 claims description 36
- WEVYAHXRMPXWCK-UHFFFAOYSA-N Acetonitrile Chemical compound CC#N WEVYAHXRMPXWCK-UHFFFAOYSA-N 0.000 claims description 30
- 238000004381 surface treatment Methods 0.000 claims description 18
- CSCPPACGZOOCGX-UHFFFAOYSA-N Acetone Chemical compound CC(C)=O CSCPPACGZOOCGX-UHFFFAOYSA-N 0.000 claims description 16
- KFZMGEQAYNKOFK-UHFFFAOYSA-N Isopropanol Chemical compound CC(C)O KFZMGEQAYNKOFK-UHFFFAOYSA-N 0.000 claims description 16
- YSHMQTRICHYLGF-UHFFFAOYSA-N 4-tert-butylpyridine Chemical compound CC(C)(C)C1=CC=NC=C1 YSHMQTRICHYLGF-UHFFFAOYSA-N 0.000 claims description 14
- XMBWDFGMSWQBCA-UHFFFAOYSA-N hydrogen iodide Chemical compound I XMBWDFGMSWQBCA-UHFFFAOYSA-N 0.000 claims description 14
- LLWRXQXPJMPHLR-UHFFFAOYSA-N methylazanium;iodide Chemical compound [I-].[NH3+]C LLWRXQXPJMPHLR-UHFFFAOYSA-N 0.000 claims description 14
- 229910052709 silver Inorganic materials 0.000 claims description 13
- 239000004332 silver Substances 0.000 claims description 13
- 238000003756 stirring Methods 0.000 claims description 13
- XDXWNHPWWKGTKO-UHFFFAOYSA-N 207739-72-8 Chemical compound C1=CC(OC)=CC=C1N(C=1C=C2C3(C4=CC(=CC=C4C2=CC=1)N(C=1C=CC(OC)=CC=1)C=1C=CC(OC)=CC=1)C1=CC(=CC=C1C1=CC=C(C=C13)N(C=1C=CC(OC)=CC=1)C=1C=CC(OC)=CC=1)N(C=1C=CC(OC)=CC=1)C=1C=CC(OC)=CC=1)C1=CC=C(OC)C=C1 XDXWNHPWWKGTKO-UHFFFAOYSA-N 0.000 claims description 12
- 239000007788 liquid Substances 0.000 claims description 11
- WHXSMMKQMYFTQS-UHFFFAOYSA-N Lithium Chemical compound [Li] WHXSMMKQMYFTQS-UHFFFAOYSA-N 0.000 claims description 10
- 229910052744 lithium Inorganic materials 0.000 claims description 10
- VRGUHZVPXCABAX-UHFFFAOYSA-N methyllead Chemical compound [Pb]C VRGUHZVPXCABAX-UHFFFAOYSA-N 0.000 claims description 9
- OFULWSFBIJPJLM-UHFFFAOYSA-N COC1=CC=C(C=C1)N(C1=CC=C(C=C1)OC)C1(C=C2C3(C4=CC(C=CC4=C2C=C1)(N(C1=CC=C(C=C1)OC)C1=CC=C(C=C1)OC)N(C1=CC=C(C=C1)OC)C1=CC=C(C=C1)OC)C1=CC=CC=C1C=1C=CC=CC=13)N(C1=CC=C(C=C1)OC)C1=CC=C(C=C1)OC Chemical compound COC1=CC=C(C=C1)N(C1=CC=C(C=C1)OC)C1(C=C2C3(C4=CC(C=CC4=C2C=C1)(N(C1=CC=C(C=C1)OC)C1=CC=C(C=C1)OC)N(C1=CC=C(C=C1)OC)C1=CC=C(C=C1)OC)C1=CC=CC=C1C=1C=CC=CC=13)N(C1=CC=C(C=C1)OC)C1=CC=C(C=C1)OC OFULWSFBIJPJLM-UHFFFAOYSA-N 0.000 claims description 8
- LFQSCWFLJHTTHZ-UHFFFAOYSA-N Ethanol Chemical compound CCO LFQSCWFLJHTTHZ-UHFFFAOYSA-N 0.000 claims description 8
- 239000007864 aqueous solution Substances 0.000 claims description 8
- 239000008367 deionised water Substances 0.000 claims description 8
- 229910021641 deionized water Inorganic materials 0.000 claims description 8
- 239000003599 detergent Substances 0.000 claims description 8
- XLYOFNOQVPJJNP-UHFFFAOYSA-N water Chemical compound O XLYOFNOQVPJJNP-UHFFFAOYSA-N 0.000 claims description 8
- 238000001035 drying Methods 0.000 claims description 7
- 238000001291 vacuum drying Methods 0.000 claims description 6
- 238000004140 cleaning Methods 0.000 claims description 5
- 239000000075 oxide glass Substances 0.000 claims description 5
- RTAQQCXQSZGOHL-UHFFFAOYSA-N Titanium Chemical compound [Ti] RTAQQCXQSZGOHL-UHFFFAOYSA-N 0.000 claims description 4
- 229910052719 titanium Inorganic materials 0.000 claims description 4
- 239000010936 titanium Substances 0.000 claims description 4
- AMGQUBHHOARCQH-UHFFFAOYSA-N indium;oxotin Chemical group [In].[Sn]=O AMGQUBHHOARCQH-UHFFFAOYSA-N 0.000 claims description 3
- 239000000463 material Substances 0.000 claims description 2
- 239000012046 mixed solvent Substances 0.000 claims description 2
- 238000002156 mixing Methods 0.000 claims description 2
- YDZQQRWRVYGNER-UHFFFAOYSA-N iron;titanium;trihydrate Chemical compound O.O.O.[Ti].[Fe] YDZQQRWRVYGNER-UHFFFAOYSA-N 0.000 claims 1
- 230000007547 defect Effects 0.000 abstract description 8
- 230000000694 effects Effects 0.000 abstract description 4
- YTPLMLYBLZKORZ-UHFFFAOYSA-N Thiophene Chemical group C=1C=CSC=1 YTPLMLYBLZKORZ-UHFFFAOYSA-N 0.000 abstract description 2
- 238000005886 esterification reaction Methods 0.000 abstract description 2
- 125000002887 hydroxy group Chemical group [H]O* 0.000 abstract description 2
- 150000002500 ions Chemical class 0.000 abstract description 2
- 125000003178 carboxy group Chemical group [H]OC(*)=O 0.000 abstract 1
- 230000005540 biological transmission Effects 0.000 description 14
- BQCADISMDOOEFD-UHFFFAOYSA-N Silver Chemical compound [Ag] BQCADISMDOOEFD-UHFFFAOYSA-N 0.000 description 12
- 239000000203 mixture Substances 0.000 description 11
- 230000000052 comparative effect Effects 0.000 description 8
- 238000006243 chemical reaction Methods 0.000 description 6
- CBENFWSGALASAD-UHFFFAOYSA-N Ozone Chemical compound [O-][O+]=O CBENFWSGALASAD-UHFFFAOYSA-N 0.000 description 5
- QVGXLLKOCUKJST-UHFFFAOYSA-N atomic oxygen Chemical compound [O] QVGXLLKOCUKJST-UHFFFAOYSA-N 0.000 description 5
- 239000010408 film Substances 0.000 description 5
- 230000001590 oxidative effect Effects 0.000 description 5
- 229910052760 oxygen Inorganic materials 0.000 description 5
- 239000001301 oxygen Substances 0.000 description 5
- 238000004506 ultrasonic cleaning Methods 0.000 description 5
- 239000013078 crystal Substances 0.000 description 4
- 239000011259 mixed solution Substances 0.000 description 4
- 239000010409 thin film Substances 0.000 description 4
- 230000009286 beneficial effect Effects 0.000 description 3
- 239000011521 glass Substances 0.000 description 3
- 238000011049 filling Methods 0.000 description 2
- 230000006911 nucleation Effects 0.000 description 2
- 238000010899 nucleation Methods 0.000 description 2
- 238000009832 plasma treatment Methods 0.000 description 2
- 239000002994 raw material Substances 0.000 description 2
- 238000000926 separation method Methods 0.000 description 2
- 230000004075 alteration Effects 0.000 description 1
- 125000002843 carboxylic acid group Chemical group 0.000 description 1
- 239000003153 chemical reaction reagent Substances 0.000 description 1
- 238000010586 diagram Methods 0.000 description 1
- 238000010438 heat treatment Methods 0.000 description 1
- 238000001000 micrograph Methods 0.000 description 1
- 238000002715 modification method Methods 0.000 description 1
- 230000002035 prolonged effect Effects 0.000 description 1
- 238000011160 research Methods 0.000 description 1
- 238000007789 sealing Methods 0.000 description 1
- 238000001228 spectrum Methods 0.000 description 1
- 238000006467 substitution reaction Methods 0.000 description 1
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- H10—SEMICONDUCTOR DEVICES; ELECTRIC SOLID-STATE DEVICES NOT OTHERWISE PROVIDED FOR
- H10K—ORGANIC ELECTRIC SOLID-STATE DEVICES
- H10K30/00—Organic devices sensitive to infrared radiation, light, electromagnetic radiation of shorter wavelength or corpuscular radiation
- H10K30/10—Organic devices sensitive to infrared radiation, light, electromagnetic radiation of shorter wavelength or corpuscular radiation comprising heterojunctions between organic semiconductors and inorganic semiconductors
- H10K30/15—Sensitised wide-bandgap semiconductor devices, e.g. dye-sensitised TiO2
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- H10K—ORGANIC ELECTRIC SOLID-STATE DEVICES
- H10K71/00—Manufacture or treatment specially adapted for the organic devices covered by this subclass
- H10K71/10—Deposition of organic active material
- H10K71/12—Deposition of organic active material using liquid deposition, e.g. spin coating
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- H10K—ORGANIC ELECTRIC SOLID-STATE DEVICES
- H10K85/00—Organic materials used in the body or electrodes of devices covered by this subclass
- H10K85/60—Organic compounds having low molecular weight
- H10K85/649—Aromatic compounds comprising a hetero atom
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- Y02E—REDUCTION OF GREENHOUSE GAS [GHG] EMISSIONS, RELATED TO ENERGY GENERATION, TRANSMISSION OR DISTRIBUTION
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Abstract
The invention discloses a perovskite solar cell based on a 3-thiophene acetic acid interface modification layer and a preparation method thereof. The battery comprises a cathode substrate, an electron transport layer, an interface modification layer, a perovskite light absorption layer, a hole transport layer and an anode electrode. The method comprises the following steps: and spin-coating a tin oxide electron transport layer, an interface modification layer, a perovskite light absorption layer and a hole transport layer on the cathode substrate in sequence, and evaporating an anode electrode to obtain the solar cell. Carboxyl in the 3-thiopheneacetic acid can be subjected to esterification reaction with hydroxyl on the surface of tin oxide to form bonding effect, and S element in the thiophene ring is subjected to bonding effect with Pb ions in the perovskite. The addition of the 3-thiophene acetic acid interface modification layer reduces the work function of the surface of the tin oxide electron transport layer, so that the energy levels of the tin oxide electron transport layer and the perovskite light absorption layer are more matched, and the high-efficiency collection of photo-generated electrons is facilitated. After the 3-thiophene acetic acid interface modification layer is added, the crystallinity of the perovskite is improved, and the internal defects of the perovskite are inhibited.
Description
Technical Field
The invention relates to the field of perovskite solar cells, in particular to a perovskite solar cell based on a 3-thiophene acetic acid interface modification layer and a preparation method thereof.
Background
Perovskite solar cells are widely concerned in the field of solar cells due to the characteristics of long exciton life, wide light absorption range, low preparation cost and high photoelectric conversion efficiency. The working principle of the perovskite solar cell is as follows: sunlight is transmitted through the ITO transparent electrode and the electron transmission layer and then enters the perovskite light absorption layer to be absorbed, and excitons are generated. The excitons are then separated in the perovskite light-absorbing layer to form electrons and holes which are injected into the electron transport layer and the hole transport layer respectively, and finally collected by the cathode and the anode respectively, and a photocurrent and a photovoltage are generated.
Researches show that the large energy level difference between an electron transport layer and a perovskite light absorption layer in the perovskite solar cell and the poor crystallinity of the perovskite are important factors influencing the efficiency of the perovskite solar cell. The Energy level difference between the perovskite light absorption layer and the carrier transmission layer can be reduced by an interface modification method, and the transmission of charges at the interface is effectively promoted, so that the open-circuit voltage and the short-circuit current density of the perovskite solar cell are improved (ACS appl. mater. interfaces 2020,12(1), 771-779; Nano Energy 2019,56, 733-740). In addition, the introduction of the interface modification layer can improve the hydrophobicity of the substrate, thereby reducing the nucleation density of the perovskite, increasing the crystal grain size of the perovskite crystal, reducing the defect state density of the perovskite thin film and being beneficial to improving the photoelectric conversion performance and stability of the device (Nanoscale 2018,10(12), 5617-.
The energy level difference between the perovskite and the tin oxide electron transmission layer can be effectively improved by introducing a proper interface modification layer into the perovskite solar cell, the film forming property of the perovskite film is improved, the crystallinity of the perovskite film is improved, the crystal boundary and the defects in the perovskite film are reduced, and the perovskite solar cell has important significance for improving the performance and the stability of the perovskite solar cell.
Disclosure of Invention
In order to overcome the defects in the prior art, the invention aims to provide a perovskite solar cell based on a 3-thiophene acetic acid interface modification layer and a preparation method thereof.
According to the invention, the perovskite solar cell with high photoelectric conversion efficiency and high stability is prepared by adding a 3-thiophene acetic acid interface modification layer between the electron transmission layer and the perovskite light absorption layer.
The purpose of the invention is realized by at least one of the following technical solutions.
The perovskite solar cell based on the 3-thiophene acetic acid interface modification layer provided by the invention sequentially comprises the following components from bottom to top: the cathode comprises a cathode substrate, an electron transport layer, an interface modification layer, a perovskite light absorption layer, a hole transport layer and an anode electrode; the material used by the interface modification layer is 3-thiopheneacetic acid.
Further, the cathode substrate is indium tin oxide glass (ITO glass) or fluorine-doped tin oxide glass (FTO glass); the electron transport layer is SnO2(tin oxide), the perovskite light-absorbing layer being MAPbI3The hole transport layer is made of Spiro-OMeTAD, the anode electrode is made of silver, and the thickness of the anode electrode is 80-100 nm.
Further, the interface modification layer precursor solution is a chlorobenzene solution with a concentration of 0.01-1 mg/ml of 3-thiopheneacetic acid.
The invention provides a method for preparing the titanium ore solar cell based on the 3-thiophene acetic acid interface modification layer, which comprises the following steps:
(1) cleaning a cathode substrate, and then carrying out surface treatment on the cathode substrate to obtain a cathode surface after surface treatment;
(2) spin-coating an electron transport layer, an interface modification layer, a perovskite light absorption layer and a hole transport layer on the surface of the cathode subjected to the surface treatment in the step (1) in sequence;
(3) and (3) evaporating an anode electrode on the surface of the hole transport layer in the step (2) to obtain the perovskite solar cell based on the 3-thiophene acetic acid interface modification layer.
Further, the surface treatment of step (1) comprises: sequentially ultrasonically cleaning the cathode substrate by using liquid detergent, deionized water, acetone, absolute ethyl alcohol and isopropanol for 15-20 minutes; then drying in a vacuum drying oven at 70-80 ℃; and finally, carrying out plasma surface treatment on the surface of the cleaned and dried cathode substrate for 10-15 minutes.
Preferably, the surface treatment of step (1) comprises: sequentially ultrasonically cleaning the mixture for 20 minutes by using liquid detergent, deionized water, acetone, absolute ethyl alcohol and isopropanol respectively; then drying in a vacuum drying oven at 80 ℃; and finally, carrying out plasma surface treatment on the surface of the cleaned and dried cathode substrate for 10 minutes.
Further, the preparation of the electron transport layer in the step (2) comprises: SnO2Spin-coating the aqueous solution on the surface of the cathode substrate after surface treatment, and then carrying out annealing treatment to obtain the electron transport layer; wherein the spin coating speed is 2000-5000 r/min, and the spin coating time is 20-60 seconds; the temperature of the annealing treatment is 120-180 ℃, and the time of the annealing treatment is 30-60 minutes; the SnO2The mass fraction of the aqueous solution is 1-4%.
Preferably, the preparation of the electron transport layer in the step (2) comprises: SnO2Spin-coating the solution on the surface of the cathode substrate after surface treatment, and then carrying out annealing treatment to obtain the electron transport layer; wherein the rotating speed of the spin coating is 3500 rpm, and the time of the spin coating is 30 seconds; the temperature of the annealing treatment was 150 ℃ and the time of the annealing treatment was 60 minutes.
Further, the preparation of the interface modification layer in the step (2) comprises: spin-coating a 3-thiopheneacetic acid precursor solution on the surface of the electron transport layer, and then carrying out annealing treatment to obtain the interface modification layer; wherein the spin coating speed is 1000-; the annealing temperature is 60-150 ℃, and the annealing time is 5-20 minutes; the 3-thiopheneacetic acid precursor solution is chlorobenzene solution with the concentration of 0.01-1 mg/ml.
Preferably, the preparation of the interface modification layer in the step (2) comprises: spin-coating a 3-thiopheneacetic acid precursor solution on the surface of the electron transport layer, and then carrying out annealing treatment to obtain the interface modification layer; wherein the rotating speed of the spin coating is 3500 rpm, and the time of the spin coating is 30 seconds; the annealing temperature is 100 ℃, and the annealing time is 10 minutes; the 3-thiopheneacetic acid precursor solution is a chlorobenzene solution with the concentration of 0.1 mg/ml.
Further, the preparation of the perovskite light absorption layer in the step (2) comprises the following steps: adding methyl ammonium iodide and lead iodide into a mixed solvent of DMF and DMSO, and uniformly stirring to form a perovskite precursor solution; and spin-coating the perovskite precursor solution on the interface modification layer, and then annealing to obtain the perovskite light absorption layer.
Preferably, the concentrations of both methyl ammonium iodide and lead iodide in the perovskite precursor liquid are 1.3 mol/l.
Preferably, the spin coating speed is 3500 rpm, the spin coating time is 40 seconds, the annealing temperature is 100 ℃, and the annealing time is 20 minutes.
Preferably, the stirring is uniform, and the stirring can be carried out at 60 ℃, so that the methyl ammonium iodide and the lead iodide are completely dissolved.
Preferably, the volume ratio of DMF to DMSO is 3: 1-5: 1; in the perovskite precursor liquid, the concentrations of methyl ammonium iodide and lead iodide are both 1-1.5 mol/L.
Preferably, the speed of the spin coating is 2000-; the temperature of the annealing treatment is 60-120 ℃, and the time of the annealing treatment is 10-20 minutes.
Further, the preparation of the hole transport layer in the step (2) comprises the following steps: adding an acetonitrile solution of 2,2,7, 7-tetra [ N, N-di (4-methoxyphenyl) amino ] -9, 9-spirobifluorene and lithium trifluoromethanesulfonylimide and 4-tert-butylpyridine into chlorobenzene, uniformly mixing, and then spin-coating on the perovskite light absorption layer to obtain the hole transport layer; the mass volume ratio of the 2,2,7, 7-tetra [ N, N-di (4-methoxyphenyl) amino ] -9, 9-spirobifluorene to chlorobenzene is 60: 1-80: 1 mg/ml; the concentration of the acetonitrile solution of the lithium trifluoromethanesulfonylimide is 400-600 mg/ml; the volume ratio of the acetonitrile solution of the lithium trifluoromethanesulfonylimide to the 4-tert-butylpyridine is 1: 1-1: 3; the volume ratio of the 4-tert-butylpyridine to the chlorobenzene is 20: 1-40: 1.
according to the perovskite solar cell based on the 3-thiophene acetic acid interface modification layer, carboxylic acid groups on the 3-thiophene acetic acid and hydroxyl groups on the surface of tin oxide can be subjected to esterification reaction to form a bonding effect, and meanwhile, S elements in thiophene rings can be subjected to the bonding effect with Pb ions in perovskite. The addition of the 3-thiophene acetic acid interface modification layer reduces the work function of the surface of the tin oxide electron transport layer, so that the electron energy levels of the tin oxide electron transport layer and the perovskite light absorption layer are more matched, and the efficient collection of photo-generated electrons is facilitated. Meanwhile, after the 3-thiophene acetic acid interface modification layer is added, the hydrophobicity of the substrate is improved, the nucleation density of the perovskite is reduced, the crystallinity of the perovskite is improved, and the internal defects of the perovskite are effectively inhibited. Finally, the 3-thiophene acetic acid interface modification layer effectively improves the photoelectric conversion efficiency of the perovskite solar cell.
Compared with the prior art, the invention has the following advantages and beneficial effects:
(1) according to the preparation method of the perovskite solar cell based on the 3-thiophene acetic acid interface modification layer, the 3-thiophene acetic acid interface modification layer is added between the electron transmission layer and the perovskite light absorption layer, so that SnO is reduced2The surface work function of the electron transport layer (refer to figure 3) reduces the energy level difference between the electron transport layer and the perovskite light absorption layer, and is more beneficial to the collection of photo-generated electrons. Meanwhile, the crystallinity of the perovskite thin film is improved due to the addition of the interface modification layer, and the crystal grains of the perovskite are obviously enlarged (refer to the attached figure 4), so that the internal defects of the perovskite are reduced, and the service life of a photon-generated carrier in the light absorption layer is prolonged; a new method is provided for preparing a high-performance perovskite solar cell;
(2) compared with the perovskite solar cell without the 3-thiophene acetic acid interface modification layer, the perovskite solar cell based on the 3-thiophene acetic acid interface modification layer provided by the invention has the advantages that the current density, the open-circuit voltage and the filling factor of the cell are obviously improved, and the stability is also improved.
Drawings
Fig. 1 is a schematic structural diagram of a perovskite solar cell based on a 3-thiophene acetic acid interface modification layer according to an embodiment of the invention;
FIG. 2 is a flow chart of a preparation method of a perovskite solar cell device based on a 3-thiophene acetic acid interface modification layer according to an embodiment of the invention;
FIG. 3 is a surface ultraviolet electron energy spectrum of tin oxide and modified with 3-thiopheneacetic acid;
FIG. 4 is an SEM representation of perovskite thin films before and after 3-thiopheneacetic acid modification;
fig. 5 is a graph of current density versus voltage for the solar devices of examples 1-4 and the comparative solar device.
Detailed Description
The following examples are presented to further illustrate the practice of the invention, but the practice and protection of the invention is not limited thereto. It is noted that the processes described below, if not specifically described in detail, are all realizable or understandable by those skilled in the art with reference to the prior art. The reagents or apparatus used are not indicated to the manufacturer, and are considered to be conventional products available by commercial purchase.
The embodiment of the invention provides a perovskite solar cell based on a 3-thiophene acetic acid interface modification layer, which comprises a cathode substrate, an electron transport layer, an interface modification layer, a perovskite light absorption layer, a hole transport layer and an anode electrode from bottom to top as shown in figure 1.
The cathode substrate is indium tin oxide glass (ITO glass).
The electron transport layer is tin oxide (SnO)2)。
The interface modification layer is 3-thiopheneacetic acid.
The perovskite light absorption layer is MAPbI3。
The hole transport layer is a Spiro-oMeTAD.
The anode electrode is silver, and the thickness of the anode electrode is 80-100 nm.
The preparation process of the perovskite solar cell based on the 3-thiophene acetic acid interface modification layer is shown in figure 2 and comprises the following steps:
step 1, ultrasonic cleaning is sequentially carried out on the raw materials by using liquid detergent, deionized water, acetone, absolute ethyl alcohol and isopropanol for 15-20 minutes respectively; then drying in a drying oven at 70-80 ℃.
And 2, performing surface plasma treatment on the cleaned and dried cathode substrate (ITO) for 10-15 minutes, wherein the treatment method utilizes the strong oxidizing property of ozone generated under microwave to clean residual organic matters and the like on the surface of the ITO, and simultaneously can improve the oxygen vacancy on the surface of the ITO and improve the work function of the surface of the ITO.
Step 3, carrying out spin coating on the ITO surface treated in the step 2 to obtain SnO2The solution has the rotation speed of 2000-5000 r/min and the time of 20-60 seconds, and is annealed at the temperature of 120-180 ℃ for 30-60 minutes to form the electron transport layer.
Step 4, spin-coating a 3-thiophene acetic acid precursor solution on the surface of the electron transport layer; the preparation process of the 3-thiophene acetic acid interface modification layer comprises the following steps: dissolving 3-thiopheneacetic acid into chlorobenzene solution to form precursor solution with the concentration of 0.01-1 mg/ml, fully stirring and dissolving, then spin-coating the 3-thiopheneacetic acid precursor solution on a tin oxide electron transmission layer at the rotation speed of 1000-6000 r/min for 20-50 seconds, and then annealing at the temperature of 60-150 ℃ for 5-20 minutes to form a 3-thiopheneacetic acid interface modification layer.
And 5, spin-coating the perovskite precursor solution on the surface of the 3-thiophene acetic acid interface modification layer at the rotation speed of 2000-5000 rpm for 30-60 seconds, and then annealing at the temperature of 60-120 ℃ for 10-20 minutes on a heating table to form the perovskite light absorption layer.
And 6, spin coating a hole transport layer on the surface of the perovskite light absorption layer.
And 7, evaporating anode electrode silver (Ag) on the surface of the hole transport layer, wherein the thickness of the anode electrode silver (Ag) is 80-100 nm.
And obtaining the perovskite solar cell based on the 3-thiophene acetic acid interface modification layer after the steps are finished.
The following describes in detail embodiments of the present invention with reference to the accompanying drawings.
Example 1
Perovskite phase based on 3-thiophene acetic acid interface modification layer in example 1Solar cell device structure: ITO/SnO23-Thiopheneacetic acid/MAPbI3/Spiro-OMeTAD/Ag。
The preparation process flow of the perovskite solar cell is as follows:
step 1, ultrasonic cleaning is sequentially carried out for 20 minutes by using liquid detergent, deionized water, acetone, absolute ethyl alcohol and isopropanol respectively; then drying in a drying oven at 80 ℃;
step 2, performing surface plasma treatment on the surface of the cleaned and dried cathode substrate (ITO) for 10 minutes, wherein the treatment method utilizes the strong oxidizing property of ozone generated under microwave to clean residual organic matters and the like on the surface of the ITO, and simultaneously can improve oxygen vacancies on the surface of the ITO and improve the work function of the surface of the ITO;
step 3, carrying out spin coating on the ITO surface treated in the step 2 to obtain SnO2Aqueous solution (SnO)2The mass fraction is 2.67%), the rotating speed is 3500 rpm, the time is 40 seconds, and the electron transmission layer is formed after annealing treatment for 60 minutes under the condition of 150 ℃;
step 4, spin-coating a 3-thiophene acetic acid precursor solution on the surface of the electron transport layer; the preparation process of the 3-thiophene acetic acid interface modification layer comprises the following steps: dissolving 3-thiopheneacetic acid into chlorobenzene solution to form precursor solution with the concentration of 0.1 mg/ml, fully stirring and dissolving, then spin-coating the 3-thiopheneacetic acid precursor solution on a tin oxide electron transport layer at the rotation speed of 3500 rpm for 30 seconds, and then annealing at 100 ℃ for 10 minutes to form a 3-thiopheneacetic acid interface modification layer.
And 5, spin-coating the perovskite precursor solution on the surface of the interface modification layer. The perovskite light absorption layer preparation process comprises the following steps: dissolving methyl ammonium iodide and lead iodide into a mixed solution of DMF and DMSO (the volume ratio of DMF to DMSO is 4: 1) according to the molar ratio of 1:1 to form a perovskite precursor solution, stirring the mixture at 60 ℃ until the methyl ammonium iodide and the lead iodide are completely dissolved, then spin-coating the mixture on an interface modification layer at the rotation speed of 3500 revolutions per minute for 40 seconds, and annealing the mixture for 20 minutes at 100 ℃ to form a perovskite light absorption layer.
And 6, spin-coating a hole transport layer on the surface of the perovskite light absorption layer at the rotating speed of 4000 revolutions per minute for 40 seconds. The hole transport layer was a mixture of 72 mg of 2,2,7, 7-tetrakis [ N, N-bis (4-methoxyphenyl) amino ] -9, 9-spirobifluorene (Spiro-OMeTAD), 17.5. mu.l of lithium trifluoromethanesulfonylimide (Li-TFSI) in acetonitrile (520 mg/mL) and 28.5. mu.l of 4-tert-butylpyridine (tBP) co-dissolved in 1mL of chlorobenzene.
And 7, evaporating anode electrode silver on the surface of the hole transport layer, wherein the thickness of the anode electrode silver is 100 nm.
And obtaining the perovskite solar cell based on the 3-thiophene acetic acid interface modification layer after the steps are finished.
Comparative example
The comparative example, which was substantially the same as example 1 except for the absence of step 4 and the remaining parameters were the same as example 1, produced a perovskite solar cell without the 3-thienylacetic acid interface modification.
FIG. 3 is a graph of current density versus voltage for the perovskite solar cell based on the 3-thienylacetic acid interface modification layer of example 1 and the perovskite solar cell without the 3-thienylacetic acid interface modification layer of the comparative example; wherein the tin oxide curve in FIG. 3 is a perovskite solar cell (structure: ITO/SnO) without 3-thiophene acetic acid interface modification layer in the comparative example2/MAPbI3Current density versus voltage curve of/Spiro-OMeTAD/Ag), tin oxide/3-thiopheneacetic acid curve is a curve based on 3-thiopheneacetic acid interface modification layer perovskite solar cell of example 1 (structure: ITO/SnO23-Thiopheneacetic acid/MAPbI3Current density versus voltage curve of/Spiro-OMeTAD/Ag); as can be seen from FIG. 3, the open circuit voltage (V) of the perovskite solar cell without the 3-thienylacetic acid interface modification layer in the comparative exampleoc) 1.07V, short-circuit current density (J)sc) Is 22.26mA/cm2Fill Factor (FF) 73.53%; open circuit voltage (V) of 3-thienylacetic acid interface modification layer-based perovskite solar cell of example 1oc) 1.12V, short-circuit current density (J)sc) Is 23.03mA/cm2The Fill Factor (FF) was 80.12%. Therefore, after the 3-thiophene acetic acid interface modification layer is added, the short-circuit current density, the open-circuit voltage and the filling factor of the perovskite solar cell device are obviously improved, and the 3-thiophene acetic acid interface modification is provedThe addition of the layer can reduce the energy level difference between the tin oxide electron transmission layer and the perovskite light absorption layer, promote the transmission of electrons at the tin oxide/perovskite interface, effectively improve the perovskite film forming property, improve the carrier separation and transmission efficiency and reduce the defect state density in the perovskite.
FIG. 4 is a scanning electron microscope image of the perovskite thin film surface before and after 3-thiopheneacetic acid modification. As can be seen, the crystallinity of the surface of the perovskite is obviously improved after the modification of 3-thiopheneacetic acid, and the grain size is larger, so that the performance and the stability of the solar cell device are improved.
TABLE 1
From Table 1, it can be found that the short-circuit current density (J) of example 1sc) From 22.26mA/cm2The temperature is increased to 23.03mA/cm2The Fill Factor (FF) is increased from 73.53% to 80.12%, the open circuit voltage (V)oc) The voltage is increased from 1.07V to 1.12V, which shows that the separation and transmission efficiency of the current carrier of the perovskite solar cell after the 3-thiophene acetic acid interface modification layer is added is improved, and the internal defects are effectively inhibited. The photoelectric conversion efficiency is improved from 17.54% to 20.61%, and is improved by 14.9%. Meanwhile, the photoelectric conversion efficiency of the devices of examples 2 to 4 were improved to various degrees as compared with the comparative examples.
Example 2
The perovskite solar cell device based on the 3-thiophene acetic acid interface modification layer in the embodiment 2 has the following structure: ITO/SnO23-Thiopheneacetic acid/MAPbI3/Spiro-OMeTAD/Ag。
The preparation process flow of the perovskite solar cell based on the 3-thiophene acetic acid interface modification layer is as follows:
step 1, ultrasonic cleaning is sequentially carried out on the raw materials by using liquid detergent, deionized water, acetone, absolute ethyl alcohol and isopropanol for 15 minutes respectively; and then dried in a vacuum drying oven at 70 ℃.
And 2, carrying out plasma surface treatment on the surface of the cleaned and dried cathode substrate (ITO) for 12 minutes, wherein the treatment method utilizes the strong oxidizing property of ozone generated under microwave to clean residual organic matters and the like on the surface of the ITO, and simultaneously can improve the oxygen vacancy on the surface of the ITO and improve the work function of the surface of the ITO.
Step 3, carrying out spin coating on the ITO surface treated in the step 2 to obtain SnO2Aqueous solution (SnO)2The mass fraction is 2.67 percent), the rotating speed is 2000 r/min, the time is 20 seconds, and the electron transmission layer is formed after annealing treatment for 30 minutes at the temperature of 120 ℃;
step 4, spin-coating a 3-thiophene acetic acid precursor solution on the surface of the electron transport layer; the preparation process of the 3-thiophene acetic acid interface modification layer comprises the following steps: dissolving 3-thiopheneacetic acid into chlorobenzene solution to form precursor solution with the concentration of 0.01 mg/ml, fully stirring and dissolving, then spin-coating the precursor solution on a tin oxide electron transport layer at the rotating speed of 1000 revolutions per minute for 20 seconds, and then annealing at 60 ℃ for 5 minutes to form a 3-thiopheneacetic acid interface modification layer.
And 5, spin-coating the perovskite precursor solution on the surface of the interface modification layer. The perovskite light absorption layer preparation process comprises the following steps: dissolving methyl ammonium iodide and lead iodide into a mixed solution of DMF and DMSO (the volume ratio of DMF to DMSO is 4: 1) according to the molar ratio of 1:1 to form a perovskite precursor solution, stirring at 60 ℃ until the methyl ammonium iodide and the lead iodide are completely dissolved, then spin-coating on an interface modification layer at the rotation speed of 2000 r/min for 30 s, and annealing at 60 ℃ for 15 min to form a perovskite light absorption layer.
And 6, spin-coating a hole transport layer on the surface of the perovskite light absorption layer at the rotating speed of 4000 revolutions per minute for 40 seconds. The hole transport layer was a mixture of 72 mg of 2,2,7, 7-tetrakis [ N, N-bis (4-methoxyphenyl) amino ] -9, 9-spirobifluorene (Spiro-OMeTAD), 17.5. mu.l of lithium trifluoromethanesulfonylimide (Li-TFSI) in acetonitrile (520 mg/mL) and 28.5. mu.l of 4-tert-butylpyridine (tBP) co-dissolved in 1mL of chlorobenzene.
And 7, evaporating anode electrode silver on the surface of the hole transport layer, wherein the thickness of the anode electrode silver is 80 nm.
And obtaining the perovskite solar cell based on the 3-thiophene acetic acid interface modification layer after the steps are finished.
Example 3
The perovskite solar cell device based on the 3-thiophene acetic acid interface modification layer in the embodiment 3 has the following structure: ITO/SnO23-Thiopheneacetic acid/MAPbI3/Spiro-OMeTAD/Ag。
The preparation process flow of the perovskite solar cell based on the 3-thiophene acetic acid interface modification layer is as follows:
step 1, ultrasonic cleaning is sequentially carried out for 20 minutes by using liquid detergent, deionized water, acetone, absolute ethyl alcohol and isopropanol respectively; and then dried in a vacuum drying oven at 80 ℃.
And 2, carrying out plasma surface treatment on the surface of the cleaned and dried cathode substrate (ITO) for 13 minutes, wherein the treatment method utilizes the strong oxidizing property of ozone generated under microwave to clean residual organic matters and the like on the surface of the ITO, and simultaneously can improve the oxygen vacancy on the surface of the ITO and improve the work function of the surface of the ITO.
Step 3, carrying out spin coating on the ITO surface treated in the step 2 to obtain SnO2Aqueous solution (SnO)2The mass fraction is 2.67 percent), the rotating speed is 2500 rpm, the time is 30 seconds, and the electron transport layer is formed after annealing treatment for 40 minutes at the temperature of 150 ℃;
step 4, spin-coating a 3-thiophene acetic acid precursor solution on the surface of the electron transport layer; the preparation process of the 3-thiophene acetic acid interface modification layer comprises the following steps: dissolving 3-thiopheneacetic acid into chlorobenzene solution to form precursor solution with the concentration of 0.5 mg/ml, fully stirring and dissolving, then spin-coating the precursor solution on a tin oxide electron transport layer at the rotating speed of 2500 rpm for 40 seconds, and then annealing at the temperature of 80 ℃ for 12 minutes to form a 3-thiopheneacetic acid interface modification layer.
And 5, spin-coating the perovskite precursor solution on the surface of the interface modification layer. The perovskite light absorption layer preparation process comprises the following steps: dissolving methyl ammonium iodide and lead iodide into a mixed solution of DMF and DMSO (the volume ratio of DMF to DMSO is 4: 1) according to the molar ratio of 1:1 to form a perovskite precursor solution, stirring the mixture at the temperature of 60 ℃ until the methyl ammonium iodide and the lead iodide are completely dissolved, then spin-coating the mixture on an interface modification layer at the rotation speed of 4000 revolutions per minute for 50 seconds, and annealing the mixture at the temperature of 110 ℃ for 10 minutes to form a perovskite light absorption layer.
And 6, spin-coating a hole transport layer on the surface of the perovskite light absorption layer at the rotating speed of 4000 revolutions per minute for 40 seconds. The hole transport layer was a mixture of 72 mg of 2,2,7, 7-tetrakis [ N, N-bis (4-methoxyphenyl) amino ] -9, 9-spirobifluorene (Spiro-OMeTAD), 17.5. mu.l of lithium trifluoromethanesulfonylimide (Li-TFSI) in acetonitrile (520 mg/mL) and 28.5. mu.l of 4-tert-butylpyridine (tBP) co-dissolved in 1mL of chlorobenzene.
And 7, evaporating anode electrode silver on the surface of the hole transport layer, wherein the thickness of the anode electrode silver is 90 nm.
And obtaining the perovskite solar cell based on the 3-thiophene acetic acid interface modification layer after the steps are finished.
Example 4
The perovskite solar cell device based on the 3-thiophene acetic acid interface modification layer in the embodiment 4 has the following structure: ITO/SnO23-Thiopheneacetic acid/MAPbI3/Spiro-OMeTAD/Ag。
The preparation process flow of the perovskite solar cell based on the 3-thiophene acetic acid interface modification layer is as follows:
step 1, ultrasonic cleaning is sequentially carried out for 20 minutes by using liquid detergent, deionized water, acetone, absolute ethyl alcohol and isopropanol respectively; and then dried in a vacuum drying oven at 80 ℃.
And 2, carrying out plasma surface treatment on the surface of the cleaned and dried cathode substrate (ITO) for 15 minutes, wherein the treatment method utilizes the strong oxidizing property of ozone generated under microwave to clean residual organic matters and the like on the surface of the ITO, and simultaneously can improve the oxygen vacancy on the surface of the ITO and improve the work function of the surface of the ITO.
Step 3, carrying out spin coating on the ITO surface treated in the step 2 to obtain SnO2Aqueous solution (SnO)2The mass fraction is 2.67 percent), the rotating speed is 5000 r/min, the time is 60 seconds, and the electron transmission layer is formed after annealing treatment for 45 minutes at the temperature of 180 ℃;
step 4, spin-coating a 3-thiophene acetic acid precursor solution on the surface of the electron transport layer; the preparation process of the 3-thiophene acetic acid interface modification layer comprises the following steps: dissolving 3-thiopheneacetic acid into chlorobenzene solution to form precursor solution with the concentration of 1 mg/ml, fully stirring and dissolving, then spin-coating the precursor solution on a tin oxide electron transport layer at the rotating speed of 6000 revolutions per minute for 50 seconds, and then annealing at 150 ℃ for 20 minutes to form a 3-thiopheneacetic acid interface modification layer.
And 5, spin-coating the perovskite precursor solution on the surface of the interface modification layer. The perovskite light absorption layer preparation process comprises the following steps: dissolving methyl ammonium iodide and lead iodide into a mixed solution of DMF and DMSO (the volume ratio of DMF to DMSO is 4: 1) according to the molar ratio of 1:1 to form a perovskite precursor solution, stirring at 60 ℃ until the methyl ammonium iodide and the lead iodide are completely dissolved, then spin-coating on an interface modification layer at the rotation speed of 5000 r/min for 60 seconds, and annealing at 120 ℃ for 15 minutes to form a perovskite light absorption layer.
And 6, spin-coating a hole transport layer on the surface of the perovskite light absorption layer at the rotating speed of 4000 revolutions per minute for 40 seconds. The hole transport layer was a mixture of 72 mg of 2,2,7, 7-tetrakis [ N, N-bis (4-methoxyphenyl) amino ] -9, 9-spirobifluorene (Spiro-OMeTAD), 17.5. mu.l of lithium trifluoromethanesulfonylimide (Li-TFSI) in acetonitrile (520 mg/mL) and 28.5. mu.l of 4-tert-butylpyridine (tBP) co-dissolved in 1mL of chlorobenzene.
And 7, evaporating anode electrode silver on the surface of the hole transport layer, wherein the thickness of the anode electrode silver is 100 nm.
And obtaining the perovskite solar cell based on the 3-thiophene acetic acid interface modification layer after the steps are finished.
The current density versus voltage plots for the comparative and example solar devices are shown in fig. 5. The test was conducted in a 100 milliwatt/square centimeter solar simulator, voltage was applied across the device, voltage current data was recorded and plotted as figure 5. As can be seen from FIG. 5, the open-circuit voltage of the device is significantly improved after the modification by 3-thiopheneacetic acid, and the short-circuit current density is correspondingly improved.
The above examples are only preferred embodiments of the present invention, which are intended to be illustrative and not limiting, and those skilled in the art should understand that they can make various changes, substitutions and alterations without departing from the spirit and scope of the invention.
Claims (10)
1. The perovskite solar cell based on the 3-thiophene acetic acid interface modification layer is characterized by sequentially comprising the following components from bottom to top: the cathode comprises a cathode substrate, an electron transport layer, an interface modification layer, a perovskite light absorption layer, a hole transport layer and an anode electrode; the material used by the interface modification layer is 3-thiopheneacetic acid.
2. The 3-thiophene acetic acid interface modification layer-based ilmenite solar cell of claim 1, wherein the cathode substrate is indium tin oxide glass or fluorine-doped tin oxide glass; the electron transport layer is SnO2The perovskite light absorption layer is MAPbI3The hole transport layer is made of Spiro-OMeTAD, the anode electrode is made of silver, and the thickness of the anode electrode is 80-100 nm.
3. A method for preparing a 3-thienylacetic acid interface modification layer-based titanium ore solar cell according to any one of claims 1 to 2, comprising the steps of:
(1) cleaning a cathode substrate, and then carrying out surface treatment on the cathode substrate to obtain a cathode surface after surface treatment;
(2) spin-coating an electron transport layer, an interface modification layer, a perovskite light absorption layer and a hole transport layer on the surface of the cathode subjected to the surface treatment in the step (1) in sequence;
(3) and (3) evaporating an anode electrode on the surface of the hole transport layer in the step (2) to obtain the perovskite solar cell based on the 3-thiophene acetic acid interface modification layer.
4. The method for preparing the 3-thiophene acetic acid interface modification layer-based titanium ore solar cell according to claim 3, wherein the surface treatment in the step (1) comprises: sequentially ultrasonically cleaning the cathode substrate by using liquid detergent, deionized water, acetone, absolute ethyl alcohol and isopropanol for 15-20 minutes; then drying in a vacuum drying oven at 70-80 ℃; and finally, carrying out plasma surface treatment on the surface of the cleaned and dried cathode substrate for 10-15 minutes.
5. The method for preparing the 3-thienylacetic acid interface modification layer-based titanium ore solar cell according to claim 3, wherein the step (2) of preparing the electron transport layer comprises: SnO2Spin-coating the aqueous solution on the surface of the cathode substrate after surface treatment, and then carrying out annealing treatment to obtain the electron transport layer; wherein the spin coating speed is 2000-5000 r/min, and the spin coating time is 20-60 seconds; the temperature of the annealing treatment is 120-180 ℃, and the time of the annealing treatment is 30-60 minutes; the SnO2The mass fraction of the aqueous solution is 1-4%.
6. The method for preparing a perovskite solar cell based on a 3-thiopheneacetic acid interface modification layer according to claim 3, wherein the step (2) of preparing the interface modification layer comprises: spin-coating a 3-thiopheneacetic acid precursor solution on the surface of the electron transport layer, and then carrying out annealing treatment to obtain the interface modification layer; wherein the spin coating speed is 1000-; the annealing temperature is 60-150 ℃, and the annealing time is 5-20 minutes; the 3-thiopheneacetic acid precursor solution is chlorobenzene solution with the concentration of 0.01-1 mg/ml.
7. The method for preparing a perovskite solar cell based on a 3-thiopheneacetic acid interface modification layer according to claim 3, wherein the step (2) of preparing the perovskite light absorption layer comprises: adding methyl ammonium iodide and lead iodide into a mixed solvent of DMF and DMSO, and uniformly stirring to form a perovskite precursor solution; and spin-coating the perovskite precursor solution on the interface modification layer, and then annealing to obtain the perovskite light absorption layer.
8. The method for preparing a perovskite solar cell based on a 3-thiopheneacetic acid interface modification layer according to claim 7, wherein the volume ratio of DMF to DMSO is 3: 1-5: 1; in the perovskite precursor liquid, the concentrations of methyl ammonium iodide and lead iodide are both 1-1.5 mol/L.
9. The method for preparing a perovskite solar cell based on a 3-thienylacetic acid interface modification layer as claimed in claim 7, wherein the spin coating rate is 2000-5000 rpm, and the spin coating time is 30-60 seconds; the temperature of the annealing treatment is 60-120 ℃, and the time of the annealing treatment is 10-20 minutes.
10. The preparation method of the perovskite solar cell based on the 3-thiopheneacetic acid interface modification layer according to the claim 3, wherein the step (2) of preparing the hole transport layer comprises the following steps: adding an acetonitrile solution of 2,2,7, 7-tetra [ N, N-di (4-methoxyphenyl) amino ] -9, 9-spirobifluorene and lithium trifluoromethanesulfonylimide and 4-tert-butylpyridine into chlorobenzene, uniformly mixing, and then spin-coating on the perovskite light absorption layer to obtain the hole transport layer; the mass volume ratio of the 2,2,7, 7-tetra [ N, N-di (4-methoxyphenyl) amino ] -9, 9-spirobifluorene to chlorobenzene is 60: 1-80: 1 mg/ml; the concentration of the acetonitrile solution of the lithium trifluoromethanesulfonylimide is 400-600 mg/ml; the volume ratio of the acetonitrile solution of the lithium trifluoromethanesulfonylimide to the 4-tert-butylpyridine is 1: 1-1: 3; the volume ratio of the 4-tert-butylpyridine to the chlorobenzene is 20: 1-40: 1.
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