CN111162179A - High-reflection-film-coverage semitransparent perovskite solar cell and preparation method thereof - Google Patents

High-reflection-film-coverage semitransparent perovskite solar cell and preparation method thereof Download PDF

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CN111162179A
CN111162179A CN201911391505.4A CN201911391505A CN111162179A CN 111162179 A CN111162179 A CN 111162179A CN 201911391505 A CN201911391505 A CN 201911391505A CN 111162179 A CN111162179 A CN 111162179A
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perovskite
layer
solar cell
transport layer
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CN111162179B (en
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于军胜
吴梦鸽
杨根杰
侯思辉
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University of Electronic Science and Technology of China
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    • H—ELECTRICITY
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    • H10K30/00—Organic devices sensitive to infrared radiation, light, electromagnetic radiation of shorter wavelength or corpuscular radiation
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    • H10K30/87—Light-trapping means
    • H—ELECTRICITY
    • H10—SEMICONDUCTOR DEVICES; ELECTRIC SOLID-STATE DEVICES NOT OTHERWISE PROVIDED FOR
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    • H10—SEMICONDUCTOR DEVICES; ELECTRIC SOLID-STATE DEVICES NOT OTHERWISE PROVIDED FOR
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Abstract

The invention discloses a high-reflection film covered semitransparent perovskite solar cell and a preparation method thereof. This scheme is through introducing the high reflection stratum behind the ultra-thin negative pole of translucent perovskite solar cell, and the high reflection stratum can be with because the negative pole is too thin throws away the light inside the device of reflecting again, makes the perovskite layer carry out twice light absorption, and then increases photoproduction current, simultaneously, plays the effect of encapsulation through the high reflection stratum, and isolated water in the air, oxygen prevent that the metal electrode from being by oxidation to the erosion of perovskite layer, improve the operating stability and the storage stability of device.

Description

High-reflection-film-coverage semitransparent perovskite solar cell and preparation method thereof
Technical Field
The invention relates to the field of photovoltaic devices, in particular to a high-reflection film covered semitransparent perovskite solar cell and a preparation method thereof.
Background
Perovskite materials have been widely used in the field of optoelectronic devices such as light emitting diodes, solar cells, lasers, detectors, etc. because of their excellent optoelectronic properties, such as high absorption coefficient, adjustable forbidden band width, high electron mobility and hole mobility, low exciton binding energy, long carrier diffusion length, low material price, and solution compatible method.
Translucent batteries have attracted considerable attention because they can be used as glass for buildings. However, the conventional semitransparent device has a thin metal electrode, which causes a reduction in secondary absorption (light absorption due to incident light reflected by the metal electrode) of the device, and finally results in a significant reduction in device performance, which is not comparable to that of a non-semitransparent device. Meanwhile, water and oxygen in the air can cause perovskite crystals to be degraded, and the metal electrode is easy to oxidize in the air, so that the storage stability and the operation stability of the device are poor.
Disclosure of Invention
The invention aims to: the high-reflection film is formed by introducing a plurality of layers of high-refractive-index materials behind an ultrathin cathode, and is mainly used for solving the problems of light absorption reduction caused by the fact that the cathode is too thin in a semitransparent device and instability of the device.
The technical scheme adopted by the invention is as follows:
the high-reflection film covered semitransparent perovskite solar cell comprises a substrate, an anode, a hole transport layer, a perovskite photoactive layer, an electron transport layer, a cathode and a high-reflection film covering layer which are sequentially arranged, wherein the anode and the cathode are connected through an external power supply. Compare in traditional solar cell, this scheme can be with negative pole light-emitting reflection to perovskite active layer through the setting of perovskite active layer and high anti-mode overburden, makes it carry out twice light absorption to increase photoproduction electric current, improve the device performance, simultaneously, high anti-mode overburden can also completely cut off the inside and external world of battery, avoids water in the air, oxygen etc. to cause the influence to the inner structure of battery, improves the stability of device.
Preferably, the perovskite photoactive layer is made of organic and inorganic hybrid ABX3Mould standA cubic structure. Wherein A is an organic amine group (e.g. CH)3NH3 +1(MA+1)、CH(NH2)2 +1、Cs+1Etc. in a single or multiple combination); b is a metal of the fourth main group; x is a mono-halogen element or a combination of multi-halogen elements.
Preferably, the thickness of the hole transport layer is 40-80nm, the thickness of the perovskite photoactive layer is 200-500nm, the thickness of the electron transport layer is 40-80nm, the thickness of the cathode is 5-20nm, and the thickness of the high-reflection film covering layer is 100-200 nm.
It should be noted that in this scheme, the anode is a metal film or a metal oxide film, the metal oxide film may be an ITO film or a zinc oxide film or a tin oxide film, and the metal film may be a metal film of gold, copper, silver, or the like. The invention preferably selects the ITO film as the anode, has strong enough conductivity, large enough work function and good chemical stability, and can inject holes into the electrode of the hole transport layer.
The hole transport layer is made of an organic polymer material having good chemical and stable hole transport properties, such as 4,4 '-cyclohexylidene bis [ N, N-di (p-tolyl) aniline ] (TAPC), poly [ (9, 9-di-N-octylfluorenyl-2, 7-diyl) -alt- (4,4' - (N- (4-N-butyl) phenyl) -diphenylamine) ] (TFB), poly [ bis (4-phenyl) (4-butylphenyl) amine ] (poly-TPD), poly [ bis (4-phenyl) (2,4, 6-trimethylphenyl) amine ] (PTAA), polyethylenedioxythiophene-poly (styrenesulfonate) (PEDOT: PSS), or any combination thereof. The hole transport material of the present invention is preferably 4,4' -cyclohexylidenebis [ N, N-di (p-tolyl) aniline ] (TAPC).
The electron transport layer is made of an electron transport material having good electron transport properties, low electron affinity, low film-forming properties and good chemical stability, such as metal oxide (ZnO, TiO)2，SnO2) Fullerene C60, C70, fullerene derivatives and the like [6,6 ]]-phenyl C61 butyric acid methyl ester (PC)61BM)，[6,6]-phenyl radical C71Butyric acid methyl ester (PC)71BM), the electron transport material of the present invention is preferably [6,6 ]]-phenyl radical C61Butyric acid methyl ester (PC)61BM)。
The cathode is an electrode with sufficient conductivity, small work function and good chemical stability, which can inject electrons into the electron transport layer, and is preferably a material with low work function, usually a metal oxide film (such as indium tin oxide ITO, zinc oxide, tin zinc oxide) or a metal film (an alloy of metals such as lithium, magnesium, calcium, strontium, aluminum, indium or copper, gold, silver, etc.), and the cathode material of the present invention is preferably Au.
The high-reflection film covering layer 7 is formed by overlapping high-refractive index and low-refractive index films for odd times by adopting a material with strong light transmittance and small extinction coefficient and stable physical and chemical properties, wherein the high-refractive index material is usually a metal oxide material such as MoO3、MgO、WO3The low refractive index material is LiF or CsF.
In addition, the invention also discloses a preparation method of the high-reflection film covered semitransparent perovskite solar cell, which comprises the following steps:
step 1: and cleaning the substrate by sequentially adopting a detergent, acetone, deionized water and an isopropanol solution.
Step 2: spin-coating a hole transport layer on the substrate after drying treatment, and then annealing at 120 ℃ for 20 minutes;
and step 3: putting the cooled substrate into a glove box, spin-coating a perovskite photoactive layer at a rotating speed of 3000 rpm, and then annealing at 120 ℃ for 10 minutes;
and 4, step 4: spin-coating an electron transport layer on the perovskite photoactive layer, and then annealing at 120 ℃ for 20 minutes;
and 5: and transferring the annealed substrate into a vacuum evaporation chamber, and sequentially evaporating an ultrathin metal cathode and a high-reflection film covering layer according to the structure of the diode device.
In summary, due to the adoption of the technical scheme, the invention has the beneficial effects that:
1. according to the invention, the high-reflection layer is introduced behind the ultrathin cathode of the semitransparent perovskite solar cell, and the high-reflection layer can reflect light projected out due to the ultrathin cathode back to the interior of the device, so that the perovskite layer can absorb light twice, and further the photoproduction current is increased.
2. In the invention, the introduced high-reflection film utilizes the difference of refractive indexes between adjacent film layers to enhance the reflection of incident light, and the light transmission of the semitransparent device is not damaged.
3. In the invention, the high-reflection film can play a role in packaging. The corrosion of water and oxygen in the air to the perovskite layer can be isolated, and more importantly, the metal electrode can be prevented from being oxidized, so that the operation stability and the storage stability of the device are improved.
Drawings
In order to more clearly illustrate the technical solutions of the embodiments of the present invention, the drawings needed to be used in the embodiments will be briefly described below, it should be understood that the following drawings only illustrate some embodiments of the present invention and therefore should not be considered as limiting the scope, and for those skilled in the art, other related drawings can be obtained according to the drawings without inventive efforts.
Fig. 1 is a schematic structural view of a semitransparent perovskite solar cell according to the present invention.
FIG. 2 is a graph showing a comparison of light transmittance in example 1 (control group) of the present invention, and in examples 2 and 3.
Fig. 3 is a graph showing a comparison of photoelectric conversion efficiencies between example 1 (control group) and examples 2 and 3 of the present invention.
FIG. 4 is a graph comparing the decay in performance of example 1 (control) and examples 2 and 3 of the present invention.
FIG. 5 is a graph showing a comparison of light transmittance in example 4 (control group) of the present invention, and in examples 5 and 6.
Fig. 6 is a graph showing a comparison of photoelectric conversion efficiencies of example 4 (control group) and examples 5 and 6 of the present invention.
FIG. 7 is a graph comparing the decay in performance of example 4 (control) and examples 5 and 6 of the present invention.
The labels in the figure are: 1-substrate, 2-anode, 3-hole transport layer, 4-perovskite photoactive layer, 5-electron transport layer, 6-cathode, 7-high-reflection film covering layer and 8-external power supply.
Detailed Description
In order to make the objects, technical solutions and advantages of the present invention more apparent, the present invention is described in further detail below with reference to the accompanying drawings and embodiments. It should be understood that the detailed description and specific examples, while indicating the preferred embodiment of the invention, are intended for purposes of illustration only and are not intended to limit the scope of the invention. The components of embodiments of the present invention generally described and illustrated in the figures herein may be arranged and designed in a wide variety of different configurations.
Thus, the following detailed description of the embodiments of the present invention, presented in the figures, is not intended to limit the scope of the invention, as claimed, but is merely representative of selected embodiments of the invention. All other embodiments, which can be derived by a person skilled in the art from the embodiments of the present invention without making any creative effort, shall fall within the protection scope of the present invention.
It is noted that relational terms such as "first" and "second," and the like, may be used solely to distinguish one entity or action from another entity or action without necessarily requiring or implying any actual such relationship or order between such entities or actions. Also, the terms "comprises," "comprising," or any other variation thereof, are intended to cover a non-exclusive inclusion, such that a process, method, article, or apparatus that comprises a list of elements does not include only those elements but may include other elements not expressly listed or inherent to such process, method, article, or apparatus. Without further limitation, an element defined by the phrase "comprising an … …" does not exclude the presence of other identical elements in a process, method, article, or apparatus that comprises the element.
As shown in figure 1, the high-reflection film covered semitransparent perovskite solar cell comprises a substrate, an anode, a hole transport layer 3, a perovskite photoactive layer 4, an electron transport layer 5, a cathode 6 and a high-reflection film covering layer 7 which are sequentially arranged, wherein the anode is connected with the cathode 6 through an external power supply 8.
In particular, as shown in FIG. 1The perovskite photoactive layer 4 is made of organic and inorganic hybrid ABX3A type cubic crystal system structure.
Specifically, as shown in FIG. 1, the thickness of the hole transport layer 3 is 40-80nm, the thickness of the perovskite photoactive layer 4 is 200-500nm, the thickness of the electron transport layer 5 is 40-80nm, the thickness of the cathode 6 is 5-20nm, and the thickness of the highly reflective coating 7 is 100-200 nm.
The invention provides a preparation method of a high-reflection film covered semitransparent perovskite solar cell, which comprises the following steps:
step 1: cleaning the ITO glass substrate 1 by using a detergent, deionized water, acetone and isopropanol, and then drying;
step 2: spin-coating a hole transport layer 3TAPC (8mg/ml, dissolved in chlorobenzene) on the dried ITO glass substrate 1, and then carrying out annealing treatment;
and step 3: placing the cooled substrate into a glove box, and spin-coating perovskite photoactive layer 4CH on the substrate3NH3PbI3(MAPbI31.2mol/ml, dissolved in a mixed solvent of dimethylformamide and dimethyl sulfoxide), and then annealing treatment is carried out;
and 4, step 4: an electron transport layer 5 (PC) was spin coated over the perovskite photoactive layer 461BM, 20mg/ml), and then annealing;
and 5: and transferring the annealed substrate into a vacuum evaporation chamber, and sequentially evaporating an ultrathin metal cathode 6 and a high-reflection film covering layer 7 according to the structure of the diode device.
The first embodiment is as follows: (as a control for example 2 and example 3)
Diode device structure from supreme being in proper order down:
ITO/TAPC(40nm)/MAPbI3(300nm)/PC61BM(40nm)/Au(10nm)
the preparation method comprises the following steps:
step 1: and sequentially adopting a detergent, acetone, deionized water and an isopropanol solution to carry out ultrasonic cleaning on the flexible substrate.
Step 2: TAPC (8mg/ml dissolved in chlorobenzene) is coated on the dried ITO glass substrate in a spinning mode to serve as a hole transport layer, and then annealing treatment is carried out for 20 minutes at 120 ℃;
and step 3: the cooled substrate was placed in a glove box and the perovskite precursor was spin coated for 40 seconds (1.2mol of MAPbI) at 3000 rpm3Dissolved in 700 μ L of dimethylformamide and 300 μ L of dimethylsulfoxide), the perovskite was washed with 200 μ L of chlorobenzene as an anti-solvent during spin coating. Then annealing for 10 minutes at 120 ℃;
and 4, step 4: spin coating of an electron transport layer PC on a perovskite photoactive layer61BM (dissolved in chlorobenzene at a concentration of 20mg/ml) and then annealed at 120 ℃ for 20 minutes;
and 5: and (3) transferring the annealed substrate into a vacuum evaporation chamber, and sequentially evaporating 10nm of Au as a cathode according to the structure of the diode device.
Example 1 prepared was Device 1(Device 1).
Example two:
diode device structure from supreme being in proper order down:
ITO/TAPC(40nm)/MAPbI3(300nm)/PC61BM(40nm)/Au(10nm)/[LiF(80nm)/MoO3(40nm)/LiF(80nm)]
the preparation method comprises the following steps:
step 1: and sequentially adopting a detergent, acetone, deionized water and an isopropanol solution to carry out ultrasonic cleaning on the flexible substrate.
Step 2: TAPC (8mg/ml dissolved in chlorobenzene) is coated on the dried ITO glass substrate in a spinning mode to serve as a hole transport layer, and then annealing treatment is carried out for 20 minutes at 120 ℃;
and step 3: the cooled substrate was placed in a glove box and the perovskite precursor was spin coated for 40 seconds (1.2mol of MAPbI) at 3000 rpm3Dissolved in 700 μ L of dimethylformamide and 300 μ L of dimethylsulfoxide), the perovskite was washed with 200 μ L of chlorobenzene as an anti-solvent during spin coating. Then annealing for 10 minutes at 120 ℃;
and 4, step 4: spin coating of an electron transport layer PC on a perovskite photoactive layer61BM (at 20 m)g/ml of the solution is dissolved in chlorobenzene), and then annealing treatment is carried out for 20 minutes at 120 ℃;
and 5: transferring the annealed substrate into a vacuum evaporation chamber, and sequentially evaporating 10nm Au as a cathode and LiF (80nm)/MoO according to the structure of the diode device3(40nm)/LiF (80nm) as a high-reflectivity coating.
Example 2 prepared was Device 2(Device 2).
Example 3:
diode device structure from supreme being in proper order down:
ITO/TAPC(40nm)/MAPbI3(300nm)/PC61BM(40nm)/Au(10nm)/[LiF(50nm)/MoO3(25nm)/LiF(50nm)/MoO3(25nm)/LiF(50nm)]
the preparation method comprises the following steps:
step 1: and sequentially adopting a detergent, acetone, deionized water and an isopropanol solution to carry out ultrasonic cleaning on the flexible substrate.
Step 2: TAPC (8mg/ml dissolved in chlorobenzene) is coated on the dried ITO glass substrate in a spinning mode to serve as a hole transport layer, and then annealing treatment is carried out for 20 minutes at 120 ℃;
and step 3: the cooled substrate was placed in a glove box and the perovskite precursor was spin coated for 40 seconds (1.2mol of MAPbI) at 3000 rpm3Dissolved in 700L of dimethylformamide and 300L of dimethylsulfoxide), the perovskite was washed with 200 μ L of chlorobenzene as an anti-solvent during spin coating. Then annealing for 10 minutes at 120 ℃;
and 4, step 4: spin coating of an electron transport layer PC on a perovskite photoactive layer61BM (dissolved in chlorobenzene at a concentration of 20mg/ml) and then annealed at 120 ℃ for 20 minutes;
and 5: transferring the annealed substrate into a vacuum evaporation chamber, and sequentially evaporating 10nm Au as a cathode and LiF (50nm)/MoO according to the structure of the diode device3(25nm)/LiF(50nm)/MoO3(25nm)/LiF (50nm) as a high-reflectivity coating.
Example 3 prepared was Device 3(Device 3).
Example 4: (as a control in examples 5 and 6)
Diode device structure from supreme being in proper order down:
ITO/TAPC(40nm)/Cs0.1FA0.8MA0.1PbI3(300nm)/PC61BM(40nm)/Au(10nm)
the preparation method comprises the following steps:
step 1: and sequentially adopting a detergent, acetone, deionized water and an isopropanol solution to carry out ultrasonic cleaning on the flexible substrate.
Step 2: TAPC (8mg/ml dissolved in chlorobenzene) is coated on the dried ITO glass substrate in a spinning mode to serve as a hole transport layer, and then annealing treatment is carried out for 20 minutes at 120 ℃;
and step 3: the cooled substrate was placed in a glove box and the perovskite precursor was spin coated at 3000 rpm for 40 seconds (1.58mol Cs0.1FA0.8MA0.1PbI3 dissolved in 0.7ml dimethylformamide and 0.3ml dimethylsulfoxide) with 200. mu.l chlorobenzene as the anti-solvent rinsing the perovskite during the spin coating process. Then annealing for 10 minutes at 120 ℃;
and 4, step 4: spin coating of an electron transport layer PC on a perovskite photoactive layer61BM (dissolved in chlorobenzene at a concentration of 20mg/ml) and then annealed at 120 ℃ for 20 minutes;
and 5: and (3) transferring the annealed substrate into a vacuum evaporation chamber, and sequentially evaporating 10nm of Au as a cathode according to the structure of the diode device.
Example 4 prepared was Device 4(Device 4).
Example 5:
diode device structure from supreme being in proper order down:
ITO/TAPC(40nm)/Cs0.1FA0.8MA0.1PbI3(300nm)/PC61BM(40nm)/Au(10nm)/LiF(80nm)/WO3(40nm)/LiF(80nm)
the preparation method comprises the following steps:
step 1: and sequentially adopting a detergent, acetone, deionized water and an isopropanol solution to carry out ultrasonic cleaning on the flexible substrate.
Step 2: TAPC (8mg/ml dissolved in chlorobenzene) is coated on the dried ITO glass substrate in a spinning mode to serve as a hole transport layer, and then annealing treatment is carried out for 20 minutes at 120 ℃;
and step 3: the cooled substrate was placed in a glove box and the perovskite precursor was spin coated at 3000 rpm for 40 seconds (1.58mol Cs)0.1FA0.8MA0.1PbI3Dissolved in 0.7ml of dimethylformamide and 0.3ml of dimethylsulfoxide), the perovskite was washed with 200. mu.l of chlorobenzene as an anti-solvent during spin-coating. Then annealing for 10 minutes at 120 ℃;
and 4, step 4: spin coating of an electron transport layer PC on a perovskite photoactive layer61BM (dissolved in chlorobenzene at a concentration of 20mg/ml) and then annealed at 120 ℃ for 20 minutes;
and 5: transferring the annealed substrate into a vacuum evaporation chamber, and sequentially evaporating 10nm Au as a cathode and LiF (80nm)/WO (tungsten) according to the structure of the diode device3(40nm)/LiF (80nm) as a high-reflectivity coating.
Example 5 prepared was Device 5(Device 5).
Example 6:
diode device structure from supreme being in proper order down:
ITO/TAPC(40nm)/Cs0.1FA0.8MA0.1PbI3(300nm)/PC61BM(40nm)/Au(10nm)/LiF(50nm)/WO3(25nm)/LiF(50nm)/WO3(25nm)/LiF(50nm)
the preparation method comprises the following steps:
step 1: and sequentially adopting a detergent, acetone, deionized water and an isopropanol solution to carry out ultrasonic cleaning on the flexible substrate.
Step 2: TAPC (8mg/ml dissolved in chlorobenzene) is coated on the dried ITO glass substrate in a spinning mode to serve as a hole transport layer, and then annealing treatment is carried out for 20 minutes at 120 ℃;
and step 3: the cooled substrate was placed in a glove box and the perovskite precursor was spin coated for 40 seconds (1.58mol of MAPbI) at 3000 rpm3Dissolved in 0.7ml of dimethylformamide and 0.3ml of dimethylsulfoxide), spin-coated200 microliters of chlorobenzene was used as an anti-solvent to flush the perovskite during the process. Then annealing for 10 minutes at 120 ℃;
and 4, step 4: spin coating of an electron transport layer PC on a perovskite photoactive layer61BM (dissolved in chlorobenzene at a concentration of 20mg/ml) and then annealed at 120 ℃ for 20 minutes;
and 5: transferring the annealed substrate into a vacuum evaporation chamber, and sequentially evaporating 10nm Au as a cathode and LiF (50nm)/WO (tungsten) according to the structure of the diode device3(25nm)/LiF(50nm)/WO3(25nm)/LiF(50nm)。
Example 6 prepared was Device 6(Device 6).
As can be seen from the above embodiments and the corresponding drawings, compared with the conventional solar cell, the light transmittance and the photoelectric conversion efficiency of the solar cell can be significantly improved, and meanwhile, the performance attenuation can be reduced, so that the solar cell has strong practicability.
The above description is only for the purpose of illustrating the preferred embodiments of the present invention and is not to be construed as limiting the invention, and any modifications, equivalents and improvements made within the spirit and principle of the present invention are intended to be included within the scope of the present invention.

Claims (4)

1. A semitransparent perovskite solar cell covered by a high-reflection film is characterized by comprising a substrate (1), an anode (2), a hole transport layer (3), a perovskite photoactive layer (4), an electron transport layer (5), a cathode (6) and a high-reflection film covering layer (7) which are arranged in sequence, wherein:
the anode and the cathode (6) are connected through an external power supply (8);
the high-reflection-film covering layer (7) comprises a high-refractive-index material and a low-refractive-index material which are overlapped for odd times.
2. The highly reflective film covered semitransparent perovskite solar cell according to claim 1, wherein the material of the perovskite photoactive layer (4) is organic and inorganic hybrid ABX3A type cubic crystal system structure.
3. The highly reflective film covered semitransparent perovskite solar cell as claimed in claim 1, wherein the thickness of the hole transport layer (3) is 40-80nm, the thickness of the perovskite photoactive layer (4) is 200-500nm, the thickness of the electron transport layer (5) is 40-80nm, the thickness of the cathode (6) is 5-20nm, and the thickness of the highly reflective film covering layer (7) is 100-200 nm.
4. A preparation method of a high-reflection film covered semitransparent perovskite solar cell is characterized by comprising the following steps:
step 1: and cleaning the substrate (1) by sequentially adopting a detergent, acetone, deionized water and an isopropanol solution.
Step 2: spin-coating a hole transport layer (3) on the substrate after drying treatment, and then annealing at 120 ℃ for 20 minutes;
and step 3: putting the cooled substrate into a glove box, spin-coating the perovskite light active layer (4) at the rotating speed of 3000 rpm, and then annealing for 10 minutes at 120 ℃;
and 4, step 4: spin-coating an electron transport layer (5) on the perovskite photoactive layer, and then annealing at 120 ℃ for 20 minutes;
and 5: and (3) transferring the annealed substrate into a vacuum evaporation chamber, and sequentially evaporating an ultrathin metal cathode (6) and a high-reflection film covering layer (7) according to the structure of the diode device.
CN201911391505.4A 2019-12-30 2019-12-30 High-reflection-film-coverage semitransparent perovskite solar cell and preparation method thereof Active CN111162179B (en)

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