CN108321296B - Preparation method of trans-form low-dimensional perovskite solar cell based on photonic crystal heterojunction - Google Patents
Preparation method of trans-form low-dimensional perovskite solar cell based on photonic crystal heterojunction Download PDFInfo
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Abstract
The invention relates to the technical field of solar cells, and discloses a preparation method of a trans-form low-dimensional perovskite solar cell based on photonic crystal heterojunction. Compared with the prior art, the trans-form low-dimensional perovskite solar cell based on the photonic crystal heterojunction has the advantages of strong slow light effect, high incident light capturing efficiency, high carrier transport efficiency and good stability.
Description
Technical Field
The invention relates to the technical field of solar cells, in particular to a preparation method of a trans-form low-dimensional perovskite solar cell based on photonic crystal heterojunction.
Background
With the increasing global energy crisis, solar energy has become a research hotspot in the field of renewable clean energy due to the advantages of abundant resources, wide distribution, environmental protection and the like. Perovskite Solar Cells (PSCs) have the characteristics of high photoelectric conversion efficiency, low cost, simple process and the like, and are widely concerned as one of photovoltaic power generation technologies with the greatest development prospect.
Generally, PSCs have three typical structures, namely formal mesoporous structure (conductive glass (FTO)/electron transport layer/mesoporous layer/perovskite light absorption layer/hole transport layer/metal electrode), formal planar structure (FTO/electron transport layer/perovskite light absorption layer/hole transport layer/metal electrode), and trans-planar structure (FTO/hole transport layer/perovskite light absorption layer/electron transport layer/metal electrode). Researchers have made a lot of intensive research into the components of the device structure and their interfaces, such as: novel inorganic hole transport materials, perovskite light absorption layer materials, electron transport materials and metal electrode materials are developed, and the interfaces of the hole transport layer/light absorption layer and the electron transport layer/light absorption layer are optimized. In particular, the perovskite light absorption layer is used as the most key component in the device structure, and the crystal structure, the morphology and the optical performance of the perovskite light absorption layer play a crucial role in the device efficiency. In order to further improve the efficiency of the device, researchers use band gap engineering and interface engineering to explore the influence of the band gap of the perovskite light absorption layer and the interface matching property on the photoelectric performance of the device, and preliminarily expound the intrinsic action mechanism of the perovskite light absorption layer. Especially in trans PSCs, the adoption of band gap engineering is favorable for obtaining a highly-crystallized perovskite light absorption layer; by adopting the interface engineering, the battery device with more excellent photoelectric property can be effectively optimized. Therefore, the trans-planar structure is more beneficial to constructing the PSCs with high device efficiency, small hysteresis effect and good stability. However, the traditional three-dimensional perovskite material also has self defects, especially the stability of temperature, humidity, photo-thermal and the like, and the large-scale application of PSCs is seriously hindered. Meanwhile, the low-dimensional perovskite material has the characteristics of higher formation energy, lower self-doping effect, lower ion mobility and the like, so that the stability of the low-dimensional perovskite material is more excellent than that of a three-dimensional perovskite material. At present, the photoelectric conversion efficiency of the low-dimensional perovskite solar cell is improved from 4.37% to 13.7%. However, how to obtain low-dimensional PSCs with excellent photoelectric properties and low cost is still a difficult problem in the academic and industrial fields.
Disclosure of Invention
The purpose of the invention is as follows: aiming at the problems in the prior art, the invention provides a preparation method of a trans-form low-dimensional perovskite solar cell based on photonic crystal heterojunction, and the solar cell has the advantages of strong slow light effect, high incident light capturing efficiency, high carrier transport efficiency and good stability.
The technical scheme is as follows: the invention provides a trans-form low-dimensional perovskite solar cell based on photonic crystal heterojunction, which is characterized by comprising a transparent conductive substrate, a hole transmission layer, a low-dimensional perovskite light absorption layer based on silicon dioxide-titanium dioxide photonic crystal heterojunction, a hole blocking layer and a metal electrode, wherein the hole transmission layer, the low-dimensional perovskite light absorption layer, the hole blocking layer and the metal electrode are sequentially stacked on the transparent conductive substrate.
Further, the low-dimensional perovskite light absorption layer is a silica-titania photonic crystal heterojunction filled with a low-dimensional perovskite light absorption semiconductor material. The construction of the heterojunction is beneficial to improving the capture efficiency of the perovskite light absorption layer on incident light, and the perovskite solar cell with high efficiency can be optimized by regulating and controlling the interface and the thickness of the perovskite light absorption layer; the low-dimensional perovskite light absorption layer based on the silicon dioxide-titanium dioxide photonic crystal heterojunction improves the quantum efficiency of the device by utilizing the photonic band gap and slow light effect of the low-dimensional perovskite light absorption layer, and improves the transmission efficiency of carriers by utilizing a three-dimensional ordered macroporous structure, thereby improving the photoelectric conversion efficiency of the device.
Preferably, the low-dimensional perovskite light-absorbing semiconductor material is A ʹ2An-1BnX3n+1The semiconductor material with a crystal structure is characterized in that A ʹ is organic amine ions, A is cations, B is metal cations, X is halogen anions, and n is the number of layers of low-dimensional perovskite.
Preferably, the organic amine ion is any one of: phenethylamine ion (PEA)+) N-butylamine ion (n-BA)+) Isobutylamine ion (iso-BA)+) Polyethyleneimine ion (PEI)+) (ii) a The cation is any one or the combination of the following: methylamine cation (MA)+，CH3NH3 + ) Formamidine cation (FA)+，CH(NH2)2 +) Cesium ion (Cs)+) (ii) a The metal cation is any one or combination of the following: pb2+ 、Sn2+(ii) a The halogen anion is any one or the combination of the following: i is-、Br-、Cl-(ii) a And n is a natural number which is more than 0 and less than or equal to 10.
Preferably, the hole transport layer is nickel oxide, copper oxide or cobalt oxide.
Preferably, the hole blocking layer is 2, 9-dimethyl-4, 7-biphenyl-1, 10-phenanthroline (BCP).
Preferably, the metal electrode is a silver electrode or a gold electrode.
Preferably, the transparent conductive substrate is fluorine-doped tin oxide conductive glass (FTO).
The invention also provides a preparation method of the trans-form low-dimensional perovskite solar cell based on the photonic crystal heterojunction, which comprises the following steps: s1: preparing a hole transport layer on a transparent conductive substrate; s2: preparing a silicon dioxide precursor solution and a titanium dioxide precursor solution; s3: taking polystyrene spheres as a construction element, preparing a combined solution A with the silicon dioxide precursor solution, taking the transparent conductive substrate as a substrate, and depositing polystyrene-silicon dioxide colloidal crystals on the hole transport layer by adopting a constant-temperature vertical deposition method; s4: preparing a component solution B by using polystyrene spheres as a construction element and the titanium dioxide precursor solution, and introducing titanium dioxide on the polystyrene-silicon dioxide colloidal crystal by using the transparent conductive substrate as a substrate and adopting a constant-temperature vertical deposition method to obtain a polystyrene-silicon dioxide-titanium dioxide colloidal crystal heterojunction; s5: removing polystyrene spheres in the polystyrene-silicon dioxide-titanium dioxide colloidal crystal heterojunction to obtain a three-dimensional ordered macroporous silicon dioxide-titanium dioxide photonic crystal heterojunction; s6: filling a low-dimensional perovskite light absorption semiconductor material in the three-dimensional ordered macroporous silicon dioxide-titanium dioxide photonic crystal heterojunction by using the transparent conductive substrate as a substrate and adopting a one-step method to obtain a low-dimensional perovskite light absorption layer based on the silicon dioxide-titanium dioxide photonic crystal heterojunction; s7: and sequentially vacuum evaporating a hole blocking layer and a metal electrode on the low-dimensional perovskite light absorption layer.
Further, in S6, the one-step method specifically includes the steps of: firstly, preparing a precursor solution: weighing a certain amount of organic amine ions, cations and metal cations, and dispersing the organic amine ions, the cations and the metal cations in an N, N-dimethyl formamide and dimethyl sulfoxide solvent, wherein the molar concentration of the metal cations is 0.6-1.2 mol/L, and the volume ratio of the N, N-dimethyl formamide to the dimethyl sulfoxide is 2:1 to 4: 1; secondly, spin-coating the precursor solution on the silicon dioxide-titanium dioxide photonic crystal heterojunction in sequence under an air environment: in an air environment, placing the silicon dioxide-titanium dioxide photonic crystal heterojunction substrate in a spin coater to carry out heat treatment at 75-95 ℃, and then spin-coating a precursor solution on the surface of the silicon dioxide-titanium dioxide photonic crystal heterojunction substrate at the temperature of 70-80 ℃; finally, obtaining the light absorption layer of the low-dimensional perovskite through heat treatment: covering the substrate by using a crystal dish attached with DMF, and keeping the temperature of 80-110 ℃ for 10-30 minutes to obtain the low-dimensional perovskite light absorption layer based on the silicon dioxide-titanium dioxide photonic crystal heterojunction.
Has the advantages that: the trans-form low-dimensional perovskite solar cell based on the photonic crystal heterojunction has the structure of conductive glass/a hole transmission layer/a low-dimensional perovskite light absorption layer/a hole barrier layer/a metal electrode based on the silicon dioxide-titanium dioxide photonic crystal heterojunction, and is characterized in that:
1) the photonic band gap of the light absorption layer of the low-dimensional perovskite based on the titanium dioxide photonic crystal is utilized to improve the quantum efficiency of the device in the range of 600-800nm of long wavelength;
2) the matching performance of the photonic band gap of the low-dimensional perovskite light absorption layer based on the silicon dioxide photonic crystal and the energy band gap of the perovskite material is utilized, the slow light effect is enhanced, and the capture efficiency of the device on incident light is improved;
3) the low-dimensional perovskite light absorption layer based on the silicon dioxide-titanium dioxide photonic crystal heterojunction has unique electrical properties: on one hand, the low-dimensional perovskite light absorption layer based on the silicon dioxide photonic crystal can separate the hole transmission layer from the low-dimensional perovskite light absorption layer based on the titanium dioxide photonic crystal, so that the electrons in the titanium dioxide are prevented from being compounded with the holes in the hole transmission layer; on the other hand, electrons can be transmitted to the hole blocking layer through titanium dioxide and then enter the metal electrode through the hole blocking layer, and meanwhile, the hole blocking layer can block holes from entering the metal electrode, so that the electrons and the holes are prevented from being compounded at the metal electrode; therefore, the unique electrical properties of the low-dimensional perovskite light absorption layer based on the silicon dioxide-titanium dioxide photonic crystal heterojunction are beneficial to improving the carrier transport efficiency;
4) the ordered macroporous structure of the low-dimensional perovskite light absorption layer based on the silicon dioxide-titanium dioxide photonic crystal heterojunction can effectively improve the transport efficiency of carriers;
5) the trans-form low-dimensional perovskite solar cell device based on the photonic crystal heterojunction shows a certain color, and the attractiveness is enhanced.
6) The trans-form low-dimensional perovskite solar cell based on photonic crystal heterojunction can effectively prepare a large-area cell device with excellent performance, and has the advantages of small hysteresis effect, good stability and the like compared with a three-dimensional perovskite solar cell.
Drawings
FIG. 1 is a schematic structural diagram of a trans-form low-dimensional perovskite solar cell based on photonic crystal heterojunction;
FIG. 2 is a flow chart of the preparation of a trans-form low-dimensional perovskite solar cell based on photonic crystal heterojunction;
FIG. 3 is a flow chart of the preparation of polystyrene-silica colloidal crystals;
FIG. 4 is a flow chart of the preparation of a three-dimensional ordered macroporous silica-titania photonic crystal heterojunction;
fig. 5 is a flow chart of the preparation of a low dimensional perovskite light absorption layer based on a silica-titania photonic crystal heterojunction.
The present invention will be described in detail with reference to the accompanying drawings.
Embodiment 1:
the embodiment provides a trans-form low-dimensional perovskite solar cell based on photonic crystal heterojunction, which has a structure shown in fig. 1 and consists of an FTO, a nickel oxide hole transport layer, a low-dimensional perovskite light absorption layer based on silicon dioxide-titanium dioxide photonic crystal heterojunction, a BCP hole blocking layer and a silver electrode, wherein the nickel oxide hole transport layer, the silicon dioxide-titanium dioxide photonic crystal heterojunction, the nickel oxide hole transport layer, the low-dimensional perovskite light absorption layer and the BCP hole blocking layer are sequentially stacked on the FTO. Wherein the light-absorbing layer of the low-dimensional perovskite is filled with (PEA)2(FA)8Sn9I28The three-dimensional ordered macroporous silicon dioxide-titanium dioxide photonic crystal heterojunction.
The preparation method of the trans-form low-dimensional perovskite solar cell based on the photonic crystal heterojunction comprises the following steps of:
s1: preparing a nickel oxide hole transport layer on the FTO by a spin coating method;
the specific process is as follows: preparing 0.5 mol/L nickel acetylacetonate solution by using absolute ethyl alcohol as a solvent, adding diethanol amine with the mole number equal to that of nickel ions, and stirring for 12 hours at 70 ℃; after the reaction is finished, evaporating the solution at 150 ℃ for 30 minutes to form a nickel oxide precursor; placing cleaned FTO conductive glass on a spin coater, dripping a nickel oxide precursor, and performing spin coating for 30 seconds at 3000 r/s; and (3) placing the FTO in a drying oven, and drying at 60 ℃ for 1 hour to obtain the nickel oxide hole transport layer.
S2: preparing a silicon dioxide precursor solution and a titanium dioxide precursor solution;
the specific process for preparing the silicon dioxide precursor solution comprises the following steps: firstly, at room temperature, 1mL tetraethyl orthosilicate and 1mL absolute ethyl alcohol are mixed and stirred uniformly; secondly, under the condition of stirring, slowly dripping 0.25mL of hydrochloric acid and 0.2mL of deionized water in turn to obtain a silicon dioxide precursor solution; and finally, storing the prepared silicon dioxide precursor solution at 4 ℃ for later use.
The specific process for preparing the titanium dioxide precursor solution comprises the following steps: firstly, at room temperature, 1mL of tetrabutyl titanate and 1mL of absolute ethyl alcohol are mixed and stirred uniformly; secondly, under the condition of stirring, slowly dripping 0.2mL of hydrochloric acid and 0.4mL of deionized water in turn to obtain a titanium dioxide precursor solution; and finally, storing the prepared titanium dioxide precursor solution at 4 ℃ for later use.
S3: preparing a first assembly solution with a silicon dioxide precursor solution prepared in S2 by taking polystyrene spheres as a construction element, and depositing polystyrene-silicon dioxide colloidal crystals on nickel oxide by adopting a constant-temperature vertical deposition method by taking FTO (fluorine-doped tin oxide) prepared in S1 as a substrate, wherein the FTO is spin-coated with a nickel oxide hole transport layer;
the specific process is as follows: adopting monodisperse polystyrene spheres prepared by a soap-free emulsion polymerization method as a construction element, dispersing 0.1mL of silicon dioxide precursor solution into 50mL of polystyrene sphere ethanol solution with the mass fraction of 0.05 percent to prepare an assembly solution A, and placing the assembly solution A in a vacuum drying oven at the temperature of 25 ℃; inserting the FTO substrate coated with nickel oxide into the assembly solution A, and obtaining polystyrene-silicon dioxide colloidal crystals after the solvent is volatilized; the preparation flow chart is shown in figure 3.
S4: preparing a component solution B by using polystyrene spheres as a construction element and a titanium dioxide precursor solution prepared in S2, and introducing titanium dioxide on polystyrene-silicon dioxide colloidal crystals by using a constant-temperature vertical deposition method by using FTO (fluorine-doped tin oxide) with polystyrene-silicon dioxide colloidal crystals deposited on nickel oxide as a substrate to obtain polystyrene-silicon dioxide-titanium dioxide colloidal crystals heterojunction;
the specific process is as follows: adopting monodisperse polystyrene spheres prepared by a soap-free emulsion polymerization method as a construction element, dispersing 0.1mL of titanium dioxide precursor solution into 50mL of polystyrene sphere ethanol solution with the mass fraction of 0.05 percent to prepare an assembly solution B, and placing the assembly solution B in a vacuum drying oven at the temperature of 25 ℃; inserting the FTO substrate with the polystyrene-silicon dioxide colloidal crystal deposited on the nickel oxide into the assembly solution B, and obtaining the polystyrene-silicon dioxide-titanium dioxide colloidal crystal heterojunction after the solvent is volatilized.
S5: removing polystyrene spheres in the polystyrene-silicon dioxide-titanium dioxide colloidal crystal heterojunction in the S4 to obtain a three-dimensional ordered macroporous silicon dioxide-titanium dioxide photonic crystal heterojunction;
the specific process is as follows: placing the polystyrene-silicon dioxide-titanium dioxide colloidal crystal heterojunction in a sintering furnace for heat treatment, wherein the heating rate is 2 ℃ per minute, and the temperature is kept at 500 ℃ for 1 hour, so that the three-dimensional ordered macroporous silicon dioxide-titanium dioxide photonic crystal heterojunction can be obtained; the preparation flow chart of the two steps of S4 and S5 is shown in FIG. 4.
S6: using FTO with three-dimensional ordered macroporous silicon dioxide-titanium dioxide photonic crystal heterojunction as substrate, and filling (PEA) in the three-dimensional ordered macroporous silicon dioxide-titanium dioxide photonic crystal heterojunction by one-step method2(FA)8Sn9I28Obtaining a low-dimensional perovskite light absorption layer based on silicon dioxide-titanium dioxide photonic crystal heterojunction;
first, a precursor solution is prepared. The specific process is as follows: 0.13mmol of phenethyl ammonium iodide (PEAI) and 0.60mmol of tin iodide (SnI) were weighed2) 0.53mmol of Formamidine Ammonium Iodide (FAI), and 0.06mmol of tin fluoride (SnF)2) Dispersing in 1mL of solvent (0.67mL of N, N-dimethylformamide and 0.33mL of dimethyl sulfoxide), and stirring at 70 ℃ for 3 hours to prepare a precursor solution;
and secondly, in an air environment, spin-coating the precursor solution on the silicon dioxide-titanium dioxide photonic crystal heterojunction in sequence. The specific process is as follows: in an air environment, placing an FTO substrate with a three-dimensional ordered macroporous silicon dioxide-titanium dioxide photonic crystal heterojunction into a spin coater, carrying out heat treatment for 15 minutes at 75 ℃, and then spin-coating a precursor solution with the temperature of 70 ℃ on the surface of the three-dimensional ordered macroporous silicon dioxide-titanium dioxide photonic crystal heterojunction, wherein the spin-coating condition is that spin-coating is carried out for 30 seconds at 5000 revolutions per second;
and finally, obtaining the low-dimensional perovskite light absorption layer through heat treatment. The specific process is as follows: covering the substrate by using a crystal dish attached with DMF, and continuously treating at the temperature of 80 ℃ for 30 minutes to obtain the low-dimensional perovskite light absorption layer based on the silicon dioxide-titanium dioxide photonic crystal heterojunction. The preparation process is shown in figure 5.
S7: and sequentially vacuum evaporating a hole blocking layer and a metal electrode on the low-dimensional perovskite light absorption layer to obtain the trans-form low-dimensional perovskite solar cell based on the photonic crystal heterojunction.
The specific process is as follows: placing the FTO substrate with the low-dimensional perovskite light absorption layer in a high vacuum coating instrument, and sequentially evaporating BCP and silver electrodes to construct a trans-form low-dimensional perovskite solar cell based on photonic crystal heterojunction, wherein the area of the device is controlled to be 0.1cm through a mask plate2。
Embodiment 2:
the embodiment provides a trans-form low-dimensional perovskite solar cell based on photonic crystal heterojunction, which has a structure shown in fig. 1 and consists of an FTO, a copper oxide hole transport layer, a low-dimensional perovskite light absorption layer based on silicon dioxide-titanium dioxide photonic crystal heterojunction, a BCP hole blocking layer and a gold electrode, wherein the copper oxide hole transport layer, the silicon dioxide-titanium dioxide photonic crystal heterojunction, the copper oxide hole transport layer, the low-dimensional perovskite light absorption layer and the BCP hole blocking layer are sequentially stacked on the FTO. Wherein the light absorption layer of the low-dimensional perovskite is filled with (BA)2(MA)3Pb4I13The three-dimensional ordered macroporous silicon dioxide-titanium dioxide photonic crystal heterojunction,
the preparation method of the trans-form low-dimensional perovskite solar cell based on the photonic crystal heterojunction comprises the following steps of:
s1: preparing a copper oxide hole transport layer on the FTO by a spin coating method;
the specific process is as follows: preparing 0.5 mol/L copper sulfate pentahydrate solution by using ethylene glycol as a solvent, and adding a certain amount of 1, 2-ethylenediamine dihydrochloride (the concentration is 1.0 mol/L); forming a copper oxide precursor after the reaction is finished; placing cleaned FTO conductive glass on a spin coater, dripping a copper oxide precursor, and spin-coating for 50 seconds at 6000 rpm; and placing the FTO in a tube furnace, and carrying out heat treatment for 2 hours at 300 ℃ in an argon atmosphere to obtain the copper oxide hole transport layer.
S2: preparing a silicon dioxide precursor solution and a titanium dioxide precursor solution;
the specific process for preparing the silicon dioxide precursor solution comprises the following steps: firstly, at room temperature, 1mL tetraethyl orthosilicate and 1mL absolute ethyl alcohol are mixed and stirred uniformly; secondly, under the condition of stirring, slowly dripping 0.25mL of hydrochloric acid and 0.2mL of deionized water in turn to obtain a silicon dioxide precursor solution; and finally, storing the prepared silicon dioxide precursor solution at 4 ℃ for later use.
The specific process for preparing the titanium dioxide precursor solution comprises the following steps: firstly, at room temperature, 1mL of tetrabutyl titanate and 1mL of absolute ethyl alcohol are mixed and stirred uniformly; secondly, under the condition of stirring, slowly dripping 0.2mL of hydrochloric acid and 0.4mL of deionized water in turn to obtain a titanium dioxide precursor solution; and finally, storing the prepared titanium dioxide precursor solution at 4 ℃ for later use.
S3: preparing a first assembly solution with a silicon dioxide precursor solution prepared in S2 by taking polystyrene spheres as a construction element, and depositing polystyrene-silicon dioxide colloidal crystals on copper oxide by adopting a constant-temperature vertical deposition method by taking FTO (fluorine-doped tin oxide) prepared in S1 as a substrate, wherein the FTO is spin-coated with a copper oxide hole transport layer;
the specific process is as follows: adopting monodisperse polystyrene spheres prepared by a soap-free emulsion polymerization method as a construction element, dispersing 0.1mL of silicon dioxide precursor solution into 50mL of polystyrene sphere ethanol solution with the mass fraction of 0.05 percent to prepare an assembly solution A, and placing the assembly solution A in a vacuum drying oven at the temperature of 25 ℃; inserting the FTO substrate coated with the copper oxide into the assembly solution A, and obtaining a polystyrene-silicon dioxide colloidal crystal after the solvent is volatilized; the preparation flow chart is shown in figure 3.
S4: preparing a component solution B by using polystyrene spheres as a construction element and a titanium dioxide precursor solution prepared in S2, and introducing titanium dioxide on a polystyrene-silicon dioxide colloidal crystal by using a constant-temperature vertical deposition method by using FTO (fluorine-doped tin oxide) with the polystyrene-silicon dioxide colloidal crystal deposited on copper oxide as a substrate to obtain a polystyrene-silicon dioxide-titanium dioxide colloidal crystal heterojunction;
the specific process is as follows: adopting monodisperse polystyrene spheres prepared by a soap-free emulsion polymerization method as a construction element, dispersing 0.1mL of titanium dioxide precursor solution into 50mL of polystyrene sphere ethanol solution with the mass fraction of 0.05 percent to prepare an assembly solution B, and placing the assembly solution B in a vacuum drying oven at the temperature of 25 ℃; inserting the FTO substrate with the polystyrene-silicon dioxide colloidal crystal deposited on the copper oxide into the assembly solution B, and obtaining the polystyrene-silicon dioxide-titanium dioxide colloidal crystal heterojunction after the solvent is volatilized.
S5: removing polystyrene spheres in the polystyrene-silicon dioxide-titanium dioxide colloidal crystal heterojunction in the S4 to obtain a three-dimensional ordered macroporous silicon dioxide-titanium dioxide photonic crystal heterojunction;
the specific process is as follows: placing the polystyrene-silicon dioxide-titanium dioxide colloidal crystal heterojunction in a sintering furnace for heat treatment, wherein the heating rate is 2 ℃ per minute, and the temperature is kept at 450 ℃ for 1 hour, so that the three-dimensional ordered macroporous silicon dioxide-titanium dioxide photonic crystal heterojunction can be obtained; the preparation flow chart of the two steps of S4 and S5 is shown in FIG. 4.
S6: the FTO with three-dimensional ordered macroporous silicon dioxide-titanium dioxide photonic crystal heterojunction is used as a substrate, and the three-dimensional ordered macroporous silicon dioxide-titanium dioxide photonic crystal heterojunction is filled with the FTO by adopting a one-step methodCharger (BA)2(MA)3Pb4I13Obtaining a low-dimensional perovskite light absorption layer based on silicon dioxide-titanium dioxide photonic crystal heterojunction;
first, a precursor solution is prepared. The specific process is as follows: 0.45mmol of Butyl Amine Iodide (BAI), 0.675mmol of Methyl Amine Iodide (MAI) and 0.90mmol of lead iodide (PbI) were weighed out2) Dispersing in 1mL of solvent (0.75mL of N, N-dimethylformamide and 0.25mL of dimethyl sulfoxide), and stirring at 70 ℃ for 3 hours to prepare a precursor solution;
and secondly, sequentially spin-coating a precursor solution on the silicon dioxide-titanium dioxide photonic crystal heterojunction in an air environment. The specific process is as follows: in an air environment, placing an FTO substrate with a three-dimensional ordered macroporous silicon dioxide-titanium dioxide photonic crystal heterojunction into a spin coater, carrying out heat treatment for 15 minutes at 85 ℃, and then spin-coating a precursor solution with the temperature of 75 ℃ on the surface of the three-dimensional ordered macroporous silicon dioxide-titanium dioxide photonic crystal heterojunction, wherein the spin-coating condition is that spin-coating is carried out for 20 seconds at 5000 revolutions per second;
and finally, obtaining the low-dimensional perovskite light absorption layer through heat treatment. The specific process is as follows: covering the substrate with a crystallization vessel attached with DMF, and continuously processing at the temperature of 95 ℃ for 20 minutes to obtain the low-dimensional perovskite light absorption layer based on the silicon dioxide-titanium dioxide photonic crystal heterojunction. The preparation process is shown in figure 5.
S7: and sequentially vacuum evaporating a hole blocking layer and a metal electrode on the low-dimensional perovskite light absorption layer to obtain the trans-form low-dimensional perovskite solar cell based on the photonic crystal heterojunction.
The specific process is as follows: placing the FTO substrate with the low-dimensional perovskite light absorption layer in a high vacuum coating instrument, and sequentially evaporating BCP and gold electrodes to construct a trans-form low-dimensional perovskite solar cell based on photonic crystal heterojunction, wherein the area of the device is controlled to be 0.1cm through a mask plate2。
Embodiment 3:
the embodiment provides a trans-form low-dimensional perovskite solar cell based on photonic crystal heterojunction, which has a structure as shown in figure 1 and is formed by sequentially laminating FTO (fluorine-doped tin oxide) on a substrateThe structure comprises a cobalt oxide hole transport layer on the FTO, a low-dimensional perovskite light absorption layer based on silicon dioxide-titanium dioxide photonic crystal heterojunction, a BCP hole blocking layer and a gold electrode. Wherein the light absorbing layer of the low-dimensional perovskite is filled with (PEI)2(MA)2Sn3I10The three-dimensional ordered macroporous silicon dioxide-titanium dioxide photonic crystal heterojunction,
the preparation method of the trans-form low-dimensional perovskite solar cell based on the photonic crystal heterojunction comprises the following steps of:
s1: preparing a cobalt oxide hole transport layer on the FTO by a spin coating method;
the specific process is as follows: preparing 0.5 mol/L cobalt acetate tetrahydrate solution by using ethylene glycol as a solvent, and adding a certain amount of 1, 2-ethylenediamine dihydrochloride (the concentration is 1.0 mol/L); forming a cobalt oxide precursor after the reaction is finished; placing cleaned FTO conductive glass on a spin coater, dripping a cobalt oxide precursor, and spin-coating for 50 seconds at 6000 rpm; and (3) placing the FTO in a tube furnace, and carrying out heat treatment for 2 hours at 300 ℃ in an argon atmosphere to obtain the cobalt oxide hole transport layer.
S2: preparing a silicon dioxide precursor solution and a titanium dioxide precursor solution;
the specific process for preparing the silicon dioxide precursor solution comprises the following steps: firstly, at room temperature, 1mL tetraethyl orthosilicate and 1mL absolute ethyl alcohol are mixed and stirred uniformly; secondly, under the condition of stirring, slowly dripping 0.25mL of hydrochloric acid and 0.2mL of deionized water in turn to obtain a silicon dioxide precursor solution; and finally, storing the prepared silicon dioxide precursor solution at 4 ℃ for later use.
The specific process for preparing the titanium dioxide precursor solution comprises the following steps: firstly, at room temperature, 1mL of tetrabutyl titanate and 1mL of absolute ethyl alcohol are mixed and stirred uniformly; secondly, under the condition of stirring, slowly dripping 0.2mL of hydrochloric acid and 0.4mL of deionized water in turn to obtain a titanium dioxide precursor solution; and finally, storing the prepared titanium dioxide precursor solution at 4 ℃ for later use.
S3: preparing a first assembly solution with a silicon dioxide precursor solution prepared in S2 by taking polystyrene spheres as a construction element, and depositing a polystyrene-silicon dioxide colloidal crystal on cobalt oxide by adopting a constant-temperature vertical deposition method by taking FTO (fluorine-doped tin oxide) prepared in S1 as a substrate, wherein the FTO is spin-coated with a cobalt oxide hole transport layer;
the specific process is as follows: adopting monodisperse polystyrene spheres prepared by a soap-free emulsion polymerization method as a construction element, dispersing 0.1mL of silicon dioxide precursor solution into 50mL of polystyrene sphere ethanol solution with the mass fraction of 0.05 percent to prepare an assembly solution A, and placing the assembly solution A in a vacuum drying oven at the temperature of 25 ℃; inserting the FTO substrate coated with the cobalt oxide into the assembly solution A, and obtaining a polystyrene-silicon dioxide colloidal crystal after the solvent is volatilized; the preparation flow chart is shown in figure 3.
S4: preparing a component solution B by using polystyrene spheres as a construction element and a titanium dioxide precursor solution prepared in S2, and introducing titanium dioxide on polystyrene-silicon dioxide colloidal crystals by using a constant-temperature vertical deposition method by using FTO (fluorine-doped tin oxide) with the polystyrene-silicon dioxide colloidal crystals as a substrate to obtain polystyrene-silicon dioxide-titanium dioxide colloidal crystals heterojunction;
the specific process is as follows: adopting monodisperse polystyrene spheres prepared by a soap-free emulsion polymerization method as a construction element, dispersing 0.1mL of titanium dioxide precursor solution into 50mL of polystyrene sphere ethanol solution with the mass fraction of 0.05 percent to prepare an assembly solution B, and placing the assembly solution B in a vacuum drying oven at the temperature of 25 ℃; inserting the FTO substrate with the polystyrene-silicon dioxide colloidal crystal deposited on the cobalt oxide into the assembly solution B, and obtaining the polystyrene-silicon dioxide-titanium dioxide colloidal crystal heterojunction after the solvent is volatilized.
S5: removing polystyrene spheres in the polystyrene-silicon dioxide-titanium dioxide colloidal crystal heterojunction in the S4 to obtain a three-dimensional ordered macroporous silicon dioxide-titanium dioxide photonic crystal heterojunction;
the specific process is as follows: placing the polystyrene-silicon dioxide-titanium dioxide colloidal crystal heterojunction in a sintering furnace for heat treatment, wherein the heating rate is 2 ℃ per minute, and the temperature is kept at 450 ℃ for 1 hour, so that the three-dimensional ordered macroporous silicon dioxide-titanium dioxide photonic crystal heterojunction can be obtained; the preparation flow chart of the two steps of S4 and S5 is shown in FIG. 4.
S6: the FTO with three-dimensional ordered macroporous silica-titanium dioxide photonic crystal heterojunction is used as a substrate, and the three-dimensional ordered macroporous silica-titanium dioxide photonic crystal heterojunction is filled with (PEI) by adopting a two-step method2(MA)2 Sn 3I10Obtaining a low-dimensional perovskite light absorption layer based on silicon dioxide-titanium dioxide photonic crystal heterojunction;
first, a precursor solution is prepared. The specific process is as follows: 0.80mmol of polyethyleneimine hydroiodide (PEI. HI), 0.80mmol of Methyl Amine Iodide (MAI) and 1.20mmol of lead iodide (PbI) were weighed2) Dispersing in 1mL of solvent (0.8mL of N, N-dimethylformamide and 0.2mL of dimethyl sulfoxide), and stirring at 70 ℃ for 3 hours to prepare a precursor solution;
and secondly, sequentially spin-coating a precursor solution on the silicon dioxide-titanium dioxide photonic crystal heterojunction in an air environment. The specific process is as follows: in an air environment, placing an FTO substrate with a three-dimensional ordered macroporous silicon dioxide-titanium dioxide photonic crystal heterojunction into a spin coater, carrying out heat treatment for 15 minutes at 95 ℃, and then spin-coating a precursor solution with the temperature of 80 ℃ on the surface of the three-dimensional ordered macroporous silicon dioxide-titanium dioxide photonic crystal heterojunction, wherein the spin-coating condition is that the spin-coating is carried out for 30 seconds at 3000 revolutions per second;
and finally, obtaining the low-dimensional perovskite light absorption layer through heat treatment. The specific process is as follows: covering the substrate with a crystallization vessel attached with DMF, and continuously processing at the temperature of 110 ℃ for 10 minutes to obtain the low-dimensional perovskite light absorption layer based on the silicon dioxide-titanium dioxide photonic crystal heterojunction. The preparation process is shown in figure 5.
S7: and sequentially vacuum evaporating a hole blocking layer and a metal electrode on the three-dimensional perovskite light absorption layer to obtain the trans-form three-dimensional perovskite solar cell based on the photonic crystal heterojunction.
The specific process is as follows: placing the FTO substrate with the three-dimensional perovskite light absorption layer in a high vacuum coating instrument, sequentially evaporating BCP and gold electrodes to construct a trans-form three-dimensional perovskite solar cell based on photonic crystal heterojunction, and passing through a maskThe area of the plate control device is 0.1cm2。
The above embodiments are merely illustrative of the technical concepts and features of the present invention, and the purpose of the embodiments is to enable those skilled in the art to understand the contents of the present invention and implement the present invention, and not to limit the protection scope of the present invention. All equivalent changes and modifications made according to the spirit of the present invention should be covered within the protection scope of the present invention.
Claims (9)
1. A preparation method of a trans-form low-dimensional perovskite solar cell based on photonic crystal heterojunction is characterized by comprising the following steps:
s1: preparing a hole transport layer on a transparent conductive substrate;
s2: preparing a silicon dioxide precursor solution and a titanium dioxide precursor solution;
s3: taking polystyrene spheres as a construction element, preparing a combined solution A with the silicon dioxide precursor solution, taking the transparent conductive substrate as a substrate, and depositing polystyrene-silicon dioxide colloidal crystals on the hole transport layer by adopting a constant-temperature vertical deposition method;
s4: preparing a component solution B by using polystyrene spheres as a construction element and the titanium dioxide precursor solution, and introducing titanium dioxide on the polystyrene-silicon dioxide colloidal crystal by using the transparent conductive substrate as a substrate and adopting a constant-temperature vertical deposition method to obtain a polystyrene-silicon dioxide-titanium dioxide colloidal crystal heterojunction;
s5: removing polystyrene spheres in the polystyrene-silicon dioxide-titanium dioxide colloidal crystal heterojunction to obtain a three-dimensional ordered macroporous silicon dioxide-titanium dioxide photonic crystal heterojunction;
s6: filling a low-dimensional perovskite light absorption semiconductor material in the three-dimensional ordered macroporous silicon dioxide-titanium dioxide photonic crystal heterojunction by using the transparent conductive substrate as a substrate and adopting a one-step method to obtain a low-dimensional perovskite light absorption layer based on the silicon dioxide-titanium dioxide photonic crystal heterojunction;
s7: and sequentially vacuum evaporating a hole blocking layer and a metal electrode on the low-dimensional perovskite light absorption layer to obtain the trans-form low-dimensional perovskite solar cell based on the photonic crystal heterojunction.
2. The method for preparing the trans-form low-dimensional perovskite solar cell based on the photonic crystal heterojunction as claimed in claim 1, wherein the trans-form low-dimensional perovskite solar cell based on the photonic crystal heterojunction comprises a transparent conductive substrate, and a hole transport layer, a low-dimensional perovskite light absorption layer based on the silicon dioxide-titanium dioxide photonic crystal heterojunction, a hole blocking layer and a metal electrode which are sequentially stacked on the transparent conductive substrate.
3. The method for preparing the trans-form low-dimensional perovskite solar cell based on the photonic crystal heterojunction as claimed in claim 2, wherein the low-dimensional perovskite light absorption layer is a silica-titania photonic crystal heterojunction filled with a low-dimensional perovskite light absorption semiconductor material.
4. The method for preparing the photonic crystal heterojunction-based trans-form low-dimensional perovskite solar cell according to claim 3, wherein the low-dimensional perovskite light-absorbing semiconductor material is A ʹ -containing material2An-1BnX3n+1The semiconductor material with a crystal structure is characterized in that A ʹ is organic amine ions, A is cations, B is metal cations, X is halogen anions, and n is the number of layers of low-dimensional perovskite.
5. The method for preparing the trans-form low-dimensional perovskite solar cell based on the photonic crystal heterojunction as claimed in claim 4,
the organic amine ion is any one of the following ions: phenethylamine ion (PEA)+) N-butylamine ion (n-BA)+) Isobutylamine ion (iso-BA)+) Polyethyleneimine ion (PEI)+)；
The cation is any one or the combination of the following: methylamine cation, formamidine cation, cesium ion;
the metal cation is any one or combination of the following: pb2+ 、Sn2+；
The halogen anion is any one or the combination of the following: i is-、Br-、Cl-；
And n is a natural number which is more than 0 and less than or equal to 10.
6. The method for preparing the photonic crystal heterojunction-based trans-form low-dimensional perovskite solar cell according to any one of claims 1 to 5, wherein the hole transport layer is nickel oxide, copper oxide or cobalt oxide.
7. The method for preparing the photonic crystal heterojunction-based trans-form low-dimensional perovskite solar cell according to any one of claims 1 to 5, wherein the hole blocking layer is 2, 9-dimethyl-4, 7-biphenyl-1, 10-phenanthroline.
8. The method for preparing the photonic crystal heterojunction-based trans-low dimensional perovskite solar cell according to any one of claims 1 to 5, wherein the metal electrode is a silver electrode or a gold electrode.
9. The method for preparing the photonic crystal heterojunction-based trans-form low-dimensional perovskite solar cell according to any one of claims 1 to 5, wherein the transparent conductive substrate is fluorine-doped tin oxide conductive glass.
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