CN111162179B - 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 PDFInfo
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Abstract
The invention discloses a high-reflective-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 semitransparent perovskite solar cell, and the high reflection stratum can be with because the negative pole is too thin throws the light that goes out and inside the device of reflection back again, makes the perovskite layer carry out twice light absorption, and then increases photoproduction electric current, simultaneously, plays the effect of encapsulation through the high reflection stratum, and isolated water in the air, oxygen are to the erosion of perovskite layer, prevent that metal electrode from being by oxidation, improve the operating stability and the storage stability of device.
Description
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 bandwidth, high electron mobility and hole mobility, low exciton binding energy, long carrier diffusion length, low material price, and solution compatible methods.
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 crystal degradation, 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 is connected with the cathode 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 battery inside with external, 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 ABX 3 A type cubic crystal system structure. Wherein A is an organic amine group (e.g. CH) 3 NH 3 +1 (MA +1 )、CH(NH2) 2 +1 、Cs +1 Etc. 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 100-200nm.
It should be noted that in this solution, the anode is a metal film or a metal oxide film, the metal oxide film may be an ITO film, 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 uses the ITO film as an 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 hole transport properties and good chemical stability, for example, one or more combinations of 4,4 '-cyclohexylidenebis [ 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), and the like. The hole transport material of the present invention is preferably 4,4' -cyclohexylidenebis [ N, N-di (p-tolyl) aniline ] (TAPC).
An electron transport layer 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 ，SnO 2 ) Fullerene C60, C70, fullerene derivatives, and the like [6,6 ]]-phenyl C61 butyric acid methyl ester (PC) 61 BM)，[6,6]-phenyl radical C 71 Butyric acid methyl ester (PC) 71 BM), the electron transport material of the present invention is preferably [6,6]-phenyl radical C 61 Butyric acid methyl ester (PC) 61 BM)。
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 MoO 3 、MgO、WO 3 The 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: placing the cooled substrate into a glove box, spin-coating the 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 (3) transferring the substrate after annealing treatment 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 cannot be damaged.
3. In the invention, the high-reflection film can play a role of packaging. The corrosion of water and oxygen in the air to a perovskite layer can be isolated, and more importantly, the metal electrode can be prevented from being oxidized, so that the running 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 translucent perovskite solar cell according to the present invention.
FIG. 2 is a graph showing a comparison between the light transmittance of example 1 (control group) and that of examples 2 and 3.
Fig. 3 is a graph comparing photoelectric conversion efficiencies of example 1 (control group) and examples 2 and 3 of the present invention.
FIG. 4 is a graph comparing the decay of the 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 comparing 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 further described in 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, as 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 phrases "comprising a," "8230," "8230," or "comprising" does not exclude the presence of additional like 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.
Specifically, as shown in fig. 1, the perovskite photoactive layer 4 is made of organic and inorganic hybrid ABX 3 A cubic crystal 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 high-reflection-film covering layer 7 is 100-200nm.
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;
and 2, step: spin-coating a hole transport layer 3TAPC (8 mg/ml, dissolved in chlorobenzene) on the dried ITO glass substrate 1, and then annealing;
and 3, step 3: putting the cooled substrate into a glove box, and spin-coating the substratePerovskite photoactive layer 4CH 3 NH 3 PbI 3 (MAPbI 3 1.2mol/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 4 61 BM,20 mg/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)/MAPbI 3 (300nm)/PC 61 BM(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.
And 2, step: TAPC (8 mg/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 3, step 3: the cooled substrate was placed in a glove box and the perovskite precursor was spin coated for 40 seconds (1.2 mol of MAPbI) at 3000 rpm 3 Dissolved in 700 μ L of dimethylformamide and 300 μ L of dimethylsulfoxide), the perovskite was rinsed 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 layer 61 BM (dissolved in chlorobenzene at a concentration of 20 mg/ml) and then annealed at 120 deg.C 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).
The second embodiment:
diode device structure from supreme being in proper order down:
ITO/TAPC(40nm)/MAPbI 3 (300nm)/PC 61 BM(40nm)/Au(10nm)/[LiF(80nm)/MoO 3 (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 (8 mg/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 3, step 3: the cooled substrate was placed in a glove box and the perovskite precursor was spin coated for 40 seconds (1.2 mol of MAPbI) at 3000 rpm 3 Dissolved 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 an electron transport layer PC on a perovskite photoactive layer 61 BM (dissolved in chlorobenzene at a concentration of 20 mg/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 (80 nm)/MoO according to the structure of the diode device 3 (40 nm)/LiF (80 nm) 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)/MAPbI 3 (300nm)/PC 61 BM(40nm)/Au(10nm)/[LiF(50nm)/MoO 3 (25nm)/LiF(50nm)/MoO 3 (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.
And 2, step: TAPC (8 mg/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 3, step 3: the cooled substrate was placed in a glove box and the perovskite precursor was spin coated for 40 seconds (1.2 mol of MAPbI) at 3000 rpm 3 Dissolved 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 layer 61 BM (dissolved in chlorobenzene at a concentration of 20 mg/ml) and then annealed at 120 deg.C for 20 minutes;
and 5: transferring the annealed substrate into a vacuum evaporation chamber, and sequentially evaporating 10nm Au as a cathode and LiF (50 nm)/MoO according to the structure of the diode device 3 (25nm)/LiF(50nm)/MoO 3 (25 nm)/LiF (50 nm) as a high-reflective film covering layer.
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)/Cs 0.1 FA 0.8 MA 0.1 PbI 3 (300nm)/PC 61 BM(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 (8 mg/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 (1.58 mol Cs0.1FA0.8MA0.1PbI3 dissolved in 0.7ml dimethylformamide and 0.3ml dimethylsulfoxide) with 200 microliters of chlorobenzene as the anti-solvent 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 layer 61 BM (dissolved in chlorobenzene at a concentration of 20 mg/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)/Cs 0.1 FA 0.8 MA 0.1 PbI 3 (300nm)/PC 61 BM(40nm)/Au(10nm)/LiF(80nm)/WO 3 (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 (8 mg/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 3, step 3: the cooled substrate was placed in a glove box and the perovskite precursor was spin-coated at 3000 rpm for 40 seconds (1.58 mol Cs) 0.1 FA 0.8 MA 0.1 PbI 3 Dissolved 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 layer 61 BM (dissolved in chlorobenzene at a concentration of 20 mg/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 (80 nm)/WO (tungsten) according to the structure of the diode device 3 (40 nm)/LiF (80 nm) asAnd a high-reflection film covering layer.
Example 5 prepared was Device 5 (Device 5).
Example 6:
diode device structure from supreme being in proper order down:
ITO/TAPC(40nm)/Cs 0.1 FA 0.8 MA 0.1 PbI 3 (300nm)/PC 61 BM(40nm)/Au(10nm)/LiF(50nm)/WO 3 (25nm)/LiF(50nm)/WO 3 (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.
And 2, step: TAPC (8 mg/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 3, step 3: the cooled substrate was placed in a glove box and the perovskite precursor was spin coated at 3000 rpm for 40 seconds (1.58 mol of MAPbI) 3 Dissolved in 0.7ml of dimethylformamide and 0.3ml of dimethylsulfoxide), the perovskite was washed with 200 microliters 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 layer 61 BM (dissolved in chlorobenzene at a concentration of 20 mg/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 (50 nm)/WO (tungsten) according to the structure of the diode device 3 (25nm)/LiF(50nm)/WO 3 (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 (3)
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;
the preparation method of the semitransparent perovskite solar cell covered by the high-reflection film comprises the following steps:
step 1: 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 3, 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-reflective-film covering layer (7) according to the structure of the diode device.
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 ABX 3 A type cubic crystal system structure.
3. The highly reflective film covered semitransparent perovskite solar cell according to claim 1, wherein the hole transport layer (3) has a thickness of 40-80nm, the perovskite photoactive layer (4) has a thickness of 200-500nm, the electron transport layer (5) has a thickness of 40-80nm, the cathode (6) has a thickness of 5-20nm, and the highly reflective film covering layer (7) has a thickness of 100-200nm.
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| CN109037397A (en) * | 2018-06-29 | 2018-12-18 | 南开大学 | A kind of preparation method and stacked solar cell, cascade solar cell of antireflective coating |
| CN109148688A (en) * | 2018-07-11 | 2019-01-04 | 复旦大学 | A kind of efficient perovskite solar battery and preparation method thereof |
| CN109471285B (en) * | 2018-11-26 | 2020-09-01 | 惠州市华星光电技术有限公司 | Flexible substrate, flexible display panel and display device |
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