CN113991026A - Perovskite photoelectric device interface modification method based on halogenated phenylalkylamine molecules - Google Patents

Perovskite photoelectric device interface modification method based on halogenated phenylalkylamine molecules Download PDF

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CN113991026A
CN113991026A CN202111161357.4A CN202111161357A CN113991026A CN 113991026 A CN113991026 A CN 113991026A CN 202111161357 A CN202111161357 A CN 202111161357A CN 113991026 A CN113991026 A CN 113991026A
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perovskite
hydroiodide
halogenated
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phenylalkylamine
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易陈谊
李明昊
周俊杰
谭理国
蒋超凡
李航
刘越
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Shenzhen Infinite Light Energy Technology Co ltd
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Tsinghua University
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Abstract

The application provides a perovskite photoelectric device interface modification method based on halogenated phenalkylamine molecules, after an interface modification layer based on halogenated phenalkylamine molecules is introduced between a perovskite light absorption layer and a hole transmission layer in a perovskite solar cell, because interface defects are effectively passivated, non-radiative recombination induced by defect states is weakened, radiative recombination is enhanced, the open-circuit voltage and the photoelectric conversion efficiency of the perovskite solar cell device are remarkably improved, and meanwhile, the stability of the device is also remarkably improved.

Description

Perovskite photoelectric device interface modification method based on halogenated phenylalkylamine molecules
Technical Field
The application relates to the technical field of perovskite photoelectric devices, in particular to a perovskite photoelectric device interface modification method based on halogenated phenylalkylamine molecules.
Background
Organic-inorganic metal halide perovskites are emerging semiconductor materials, have the advantages of high light absorption coefficient, high defect tolerance, adjustable band gap and the like, and perovskite photoelectric devices prepared on the basis of the semiconductor materials, such as Solar cells (Solar cells), Light Emitting Diodes (LEDs), photodetectors (photodetectors) and the like, are research hotspots of academics in recent years. The perovskite solar cell taking the perovskite thin film as the light absorption layer is facilitated, the perovskite solar cell is a solution with great prospect in the photovoltaic field, and the perovskite light emitting diode and the photoelectric detector also have wide application prospect in the fields of display, optical communication and flexible devices.
Perovskite optoelectronic devices are typically solution-fabricated multilayer thin-film device structures. Taking perovskite solar cells as an example, perovskite polycrystalline thin films prepared by a solution method are used as light absorption layers, and after absorbing light electrons, electron-hole pairs are generated and extracted through an electron transport layer and a hole transport layer and are conducted to electrodes and an external circuit. Through proper component regulation, morphology optimization and structure optimization, the certification record of the photoelectric conversion efficiency of the perovskite solar cell reaches 25.5%. However, the theory of photoelectric conversion efficiency is still a certain gap from the reality, and the stability of the photoelectric conversion efficiency is difficult to meet the life requirement of practical application.
Defect states at the surface/interface of the device have been a significant cause of affecting the performance of perovskite optoelectronic devices. The surface of the perovskite polycrystalline thin film prepared by the solution method has a plurality of defects, and the defects not only induce non-radiative recombination and are important sources for generating energy loss, but also induce the degradation of the perovskite thin film, thereby restricting the photoelectric property and stability of perovskite photoelectric devices. Therefore, effective defect passivation measures are needed to suppress defect states and energy loss at the surface interface in the perovskite photoelectric device, which is important for improving the performance and the service life of the perovskite photoelectric device.
Disclosure of Invention
The application aims to provide an interface modification means for perovskite photoelectric devices so as to effectively passivate defect states at interfaces in the perovskite photoelectric devices, and therefore photoelectric properties and stability of the devices are improved.
Therefore, in one aspect of the application, an embodiment provides a perovskite photoelectric device interface modification method based on halogenated phenalkylamine molecules, wherein an interface modification layer based on halogenated phenalkylamine molecules is introduced between a perovskite light absorption layer and a hole transport layer, namely a halogenated phenalkylamine molecular film is prepared on the surface of the perovskite light absorption layer, and a hole transport layer is prepared on the surface of the halogenated phenalkylamine molecular film.
In some embodiments, the haloalkylalkylamine molecule has the formula:
Figure BDA0003290337360000021
wherein: substituent group R1、R2、R3、R4、R5Is any one of hydrogen, alkyl, cyano, trifluoromethyl, iodine, bromine and chlorine, at least one of which is a halogen atom, and the substitution positions are combined randomly; x-Is an anion.
In some embodiments, alkylamine CnH2n-NH3 +Is any one of methylamine, ethylamine, propylamine and butylamine.
In some embodiments, the anion X-Including but not limited to iodide, bromide, chloride, sulfate, tetrafluoroborate, thiocyanate, formate, acetate, triflate, or trifluoroacetate.
In some embodiments, the substituent group R1、R2、R3、R4、R5Of which up to three are halogen atoms of the same or different species.
In some embodiments, the haloalkylamine compounds do not include 2-trifluoromethylphenethylamine hydroiodide, 3-trifluoromethylphenethylamine hydroiodide, 4-trifluoromethylphenethylamine hydroiodide, or 3-chlorobenzylamine hydroiodide.
In some embodiments, the haloalkylalkylamine solution required for the interface modification layer is prepared using a solution process.
In some embodiments, the interface modification layer is prepared by: the prepared halogenated phenylalkylamine solution is attached to the surface of the perovskite light absorption layer by a method including but not limited to a spin coating method, a blade coating method or an evaporation method.
In some embodiments, the halophenylalkylamine is 2-bromophenylethylamine hydroiodide prepared by: dissolving 2-bromophenylethylamine hydroiodide in isopropanol to obtain a 2-bromophenylethylamine hydroiodide solution, and spin-coating the 2-bromophenylethylamine hydroiodide solution on the surface of the perovskite light absorption layer film to obtain the 2-bromophenylethylamine hydroiodide interface modification layer film.
Another embodiment of the present application proposes the use of the above modification method in the fabrication of perovskite optoelectronic devices, including but not limited to perovskite solar cells, light emitting diodes or photodetectors.
Compared with the prior art, the invention has the following characteristics: after an interface modification layer based on halogenated phenethylamine molecules is introduced between a perovskite light absorption layer and a hole transmission layer in the perovskite solar cell, because the interface defects are effectively passivated, the non-radiative recombination induced by the defect state is weakened, and the radiative recombination is enhanced, the open-circuit voltage and the photoelectric conversion efficiency of the perovskite solar cell device are obviously improved. Meanwhile, the stability of the device is obviously improved.
Additional aspects and advantages of the present application will be set forth in part in the description which follows and, in part, will be obvious from the description, or may be learned by practice of the present application.
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The above and/or additional aspects and advantages of the present application will become apparent and readily appreciated from the following description of the embodiments taken in conjunction with the accompanying drawings,
wherein:
FIG. 1 is a schematic structural diagram of a basic device of a perovskite solar cell without an interface modification layer;
fig. 2 is a schematic structural diagram of a basic device of a perovskite solar cell after an interface modification layer is introduced in an embodiment of the application;
FIG. 3 is a graph comparing the J-V curves of the best performing perovskite solar cells of example 1 and comparative example 1;
FIG. 4 is a plot of maximum power point output tracking comparison of perovskite solar cells of example 1 and comparative example 1;
FIG. 5 is a graph comparing the photoluminescence spectra (PL) of the perovskite light absorbing layer thin films of example 1 and comparative example 1;
Detailed Description
Reference will now be made in detail to embodiments of the present application, examples of which are illustrated in the accompanying drawings. The embodiments described below with reference to the drawings are exemplary and intended to be used for explaining the present application and should not be construed as limiting the present application.
An exemplary method for modifying the interface of a perovskite optoelectronic device based on haloalkylalkylamine molecules is described below with reference to fig. 1-5.
The embodiment of the application provides a perovskite photoelectric device interface modification method based on halogenated phenylalkylamine molecules, wherein an interface modification layer based on halogenated phenylalkylamine molecules is introduced between a perovskite light absorption layer and a hole transport layer, namely a halogenated phenylalkylamine molecular film is prepared on the surface of the perovskite light absorption layer, and a hole transport layer is prepared on the surface of the halogenated phenylalkylamine molecular film, as shown in figures 1-2.
The perovskite photoelectric device serving as the application main body of the invention is exemplified by a perovskite solar cell. The structure of the thin film deposition device sequentially comprises a transparent conductive substrate, an electron transmission layer, a perovskite light absorption layer, an interface modification layer, a hole transmission layer and a counter electrode from bottom to top according to the thin film deposition sequence. The basic preparation process is as follows:
step 1, etching and cleaning a conductive substrate.
Step 2, preparing an electron transport layer: preparation of SnO on surface of conductive substrate2And (4) carrying out annealing treatment on the electron transport layer.
Step (ii) of3. Preparing a perovskite light absorption layer: preparation on the Electron transport layer (FA)xMA1-x)PbI3And carrying out annealing treatment.
Step 4, preparing an interface modification layer: preparing a halogenated phenethylamine molecular film on the surface of the perovskite light absorption layer.
Step 5, preparing a hole transport layer: preparing the spiro-OMeTAD film on the interface modification layer.
Step 6, preparing a counter electrode: and depositing a counter electrode material on the hole transport layer by methods such as vacuum evaporation, magnetron sputtering and the like.
In some embodiments, the haloalkylalkylamine molecule has the formula:
Figure BDA0003290337360000031
wherein:
1. alkylamines C substituted on the benzene ringnH2n-NH3 +Is any one of methylamine, ethylamine, propylamine and butylamine.
2. Substituent group R on benzene ring1、R2、R3、R4、R5Is hydrogen (H), alkyl (C)nH2n+1) Cyano (CN), trifluoromethyl (CF)3) At least one of iodine (I), bromine (Br) and chlorine (Cl) is halogen atom I, Br and Cl, and the halogen substitution on the benzene ring can be at most three halogen atoms with the same or different types. Any combination of 5 substitution positions;
3. anion X-Can be various types of anions, including but not limited to iodide (I)-) Bromine ion (Br)-) Chloride ion (Cl)-) Sulfate ion (SO)4 2-) Tetrafluoroborate ion (BF)4 -) Thiocyanate ion (SCN)-) Formate ion (HCOO)-) Acetate ion (CH)3COO-) Triflate ion (CF)3SO3 -) Or trifluoroacetate ion (CF)3COO-) And the like.
4. 2-Trifluoromethylphenylethylamine hydroiodide (2-CF)3PEAI), 3-trifluoromethylphenethylamine hydroiodide (3-CF)3PEAI), 4-trifluoromethylphenethylamine hydroiodide (4-CF)3PEAI), 3-chlorobenzeneamine hydroiodide (3-ClPBAI) is not included.
In some embodiments, the haloalkylalkylamine solution required for the interface modification layer is prepared using a solution process.
In some embodiments, the interface modification layer is prepared by: the prepared halogenated phenylalkylamine solution is attached to the surface of the perovskite light absorption layer by a method including but not limited to a spin coating method, a blade coating method or an evaporation method.
In some embodiments, the halophenylalkylamine is 2-bromophenylethylamine hydroiodide prepared by: dissolving 2-bromophenylethylamine hydroiodide in isopropanol to obtain a 2-bromophenylethylamine hydroiodide solution, and spin-coating the 2-bromophenylethylamine hydroiodide solution on the surface of the perovskite light absorption layer film to obtain the 2-bromophenylethylamine hydroiodide interface modification layer film.
Another embodiment of the present application proposes the use of the above modification method in the fabrication of perovskite optoelectronic devices, including but not limited to perovskite solar cells, light emitting diodes or photodetectors.
The present disclosure is described in detail below by specific examples:
example 1
Step 1, etching and cleaning a conductive substrate.
An ITO conductive glass substrate was used. Firstly, etching a pre-designed pattern on a conductive surface of conductive glass by laser etching to distinguish the anode and the cathode of a solar cell; cleaning the conductive glass, namely soaking the conductive glass in solvents such as a detergent, deionized water, ethanol, isopropanol and the like in sequence, and ultrasonically cleaning; and finally, treating the surface of the ITO conductive glass by ultraviolet ozone.
And 2, preparing an electron transport layer.
Preparation of tin oxide (SnO) by solution method2) An electron transport layer film. Firstly, deionized water is usedSnO with dilution mass fraction of 15%2The volume ratio of the colloid aqueous solution is 3-6: 1. Then diluting SnO2The colloid aqueous solution is coated on the transparent electrode layer of the ITO conductive glass in a spinning way; finally, putting the sample subjected to spin coating on a hot table for annealing treatment to obtain SnO2The film acts as an electron transport layer.
And 3, preparing the perovskite light absorption layer.
Two-step solution preparation (FA)xMA1-x)PbI3Perovskite light absorption layer film.
Firstly, preparing a two-step precursor solution. Mixing lead iodide (PbI)2) Dissolving the powder in a mixed solution of N, N Dimethylformamide (DMF) and dimethyl sulfoxide (DMSO) (the volume ratio is 4-9: 1) to obtain a lead iodide precursor solution with the concentration of 1.5M; mixing iodoformamidine (CH (NH)2)2I) Iodomethylamine (CH)3NH3I) Chloromethane (CH)3NH3Cl) powder was dissolved in Isopropanol (IPA) to give a 0.7M solution of the amine salt precursor.
Then preparing the perovskite light absorption layer film. Firstly, lead iodide precursor solution is coated on SnO in a spinning way2And annealing at 70 ℃ after the spin coating is finished on the substrate of the electron transport layer to obtain the lead iodide thin film. And then, spin-coating an amine salt precursor solution on the lead iodide thin film, and annealing after the spin-coating is finished to obtain the perovskite light absorption layer thin film.
And 4, preparing an interface modification layer.
The solution method is used for preparing the 2-bromophenylethylamine hydroiodide (2-BrPEAI) interface modification layer. The 2-BrPEAI is dissolved in Isopropanol (IPA) to give a 2-BrPEAI solution. And spin-coating the 2-BrPEAI solution on the surface of the perovskite light absorption layer film to obtain the 2-BrPEAI interface modification layer film.
Wherein, the molecular structure of the 2-bromophenethylamine hydroiodide (2-BrPEAI) is as follows:
Figure BDA0003290337360000051
and 5, preparing a hole transport layer.
The solution method is used for preparing the spiro-OMeTAD hole transport layer. The hole transport material, spiro-OMeTAD powder, was dissolved in Chlorobenzene (CB) to give a hole transport layer solution. The solution was spin-coated on a 2-BrPEAI film to obtain a spiro-OMeTAD hole transport layer film.
And 6, preparing a counter electrode.
The silver (Ag) electrode is prepared by an evaporation method. Sequentially evaporating molybdenum oxide (MoO) on the spiro-OMeTAD hole transport layer film3) And (3) a film and a silver (Ag) electrode to obtain a complete perovskite solar cell device.
Comparative example 1:
compared with the above embodiment, the step of preparing the interface modification layer in step 4 is omitted, and the step 5 and the step 6 are directly performed after the step 3, that is, the hole transport layer is directly prepared on the perovskite light absorption layer.
Comparison of example 1 with comparative example 1:
in example 1, after the interface modification layer based on the halogenated phenethylamine molecules is introduced between the perovskite light absorption layer and the hole transport layer in the perovskite solar cell, because the interface defects are effectively passivated, the non-radiative recombination induced by the defect states is weakened, and the radiative recombination is enhanced (as shown in fig. 5), so that the open-circuit voltage and the photoelectric conversion efficiency of the perovskite solar cell device are remarkably improved (as shown in fig. 3). And meanwhile, the stability of the device is also remarkably improved (as shown in figure 4).
In addition, the preparation process of the interface modification layer based on the substance, such as the preparation method (spin coating method, blade coating method, evaporation method, etc.), the process parameters (concentration, rotation speed, annealing condition, duration, etc.), etc., can be any feasible way of substitution and combination. The specific steps and parameters other than those described in the examples can be substituted by other equivalent or similar means to achieve the interface modification layer based on halophenylethylamine molecules of the present invention.
The perovskite solar cell applied to the main body of the invention has the advantages that the device structure (formal trans form, the action position of the interface modification layer), the material selection (different electron transport materials, perovskite components, hole transport materials and the like), the preparation method (a solution method, an evaporation method and the like), the process parameters (concentration, rotating speed, annealing conditions, duration and the like), and the like can be replaced and combined in any feasible way. Other equivalent or similar objects, in addition to the specific steps, parameters described in the examples, may be substituted to achieve a perovskite solar cell device to which the present invention may be applied.
The application of the interface modification scheme is not limited to the perovskite solar cell in the embodiment, and can also be applied to other photoelectric devices based on perovskite materials, such as Light Emitting Diodes (LEDs), photodetectors (photodetectors) and the like.
In the present disclosure, the terms "one embodiment," "some embodiments," "an example," "a specific example," or "some examples" and the like mean that a specific feature, structure, material, or characteristic described in connection with the embodiment or example is included in at least one embodiment or example of the present disclosure. In this specification, the schematic representations of the terms used above are not necessarily intended to refer to the same embodiment or example. Furthermore, the particular features, structures, materials, or characteristics described may be combined in any suitable manner in any one or more embodiments or examples. Furthermore, various embodiments or examples and features of different embodiments or examples described in this specification can be combined and combined by one skilled in the art without contradiction.
Although embodiments of the present invention have been shown and described above, it is understood that the above embodiments are exemplary and should not be construed as limiting the present invention, and that variations, modifications, substitutions and alterations can be made to the above embodiments by those of ordinary skill in the art within the scope of the present invention.

Claims (10)

1. The interface modification method of the perovskite photoelectric device based on the halogenated phenylalkylamine molecules is characterized in that an interface modification layer based on the halogenated phenylalkylamine molecules is introduced between a perovskite light absorption layer and a hole transport layer, namely a halogenated phenylalkylamine molecular film is prepared on the surface of the perovskite light absorption layer, and a hole transport layer is prepared on the surface of the halogenated phenylalkylamine molecular film.
2. The modification method according to claim 1, wherein the haloalkylamine compound has the formula:
Figure FDA0003290337350000011
wherein: substituent group R1、R2、R3、R4、R5Is any one of hydrogen, alkyl, cyano, trifluoromethyl, iodine, bromine and chlorine, at least one of which is a halogen atom, and the substitution positions are combined randomly; x-Is an anion.
3. The modification method according to claim 2, wherein alkylamine CnH2n-NH3 +Is any one of methylamine, ethylamine, propylamine and butylamine.
4. The modification method according to claim 2, wherein the anion X is an anion-Including but not limited to iodide, bromide, chloride, sulfate, tetrafluoroborate, thiocyanate, formate, acetate, triflate, or trifluoroacetate.
5. The modification method according to claim 2, wherein the substituent group R is1、R2、R3、R4、R5Of which up to three are halogen atoms of the same or different species.
6. The modification method according to claim 2, wherein the haloalkylamine compound does not include 2-trifluoromethylphenethylamine hydroiodide, 3-trifluoromethylphenethylamine hydroiodide, 4-trifluoromethylphenethylamine hydroiodide or 3-chlorobenzylamine hydroiodide.
7. The modification method according to claim 1, wherein the solution of haloalkenylalkylamine required for the interface modification layer is prepared by a solution method.
8. The modification method according to claim 7, wherein the interface modification layer is prepared by: the prepared halogenated phenylalkylamine solution is attached to the surface of the perovskite light absorption layer by a method including but not limited to a spin coating method, a blade coating method or an evaporation method.
9. The modification method according to claim 2, wherein the halophenylalkylamine is 2-bromophenylethylamine hydroiodide, which is prepared by: dissolving 2-bromophenylethylamine hydroiodide in isopropanol to obtain a 2-bromophenylethylamine hydroiodide solution, and spin-coating the 2-bromophenylethylamine hydroiodide solution on the surface of the perovskite light absorption layer film to obtain the 2-bromophenylethylamine hydroiodide interface modification layer film.
10. Use of a modification process as claimed in any one of claims 1 to 9 in the manufacture of perovskite optoelectronic devices including but not limited to perovskite solar cells, light emitting diodes or photodetectors.
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Cited By (1)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
CN115260027A (en) * 2022-06-27 2022-11-01 清华大学 Stress sustained-release agent and preparation method and application thereof

Cited By (2)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
CN115260027A (en) * 2022-06-27 2022-11-01 清华大学 Stress sustained-release agent and preparation method and application thereof
CN115260027B (en) * 2022-06-27 2023-08-25 清华大学 Stress sustained release agent and preparation method and application thereof

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