CN112542550B - MXene-based high-efficiency perovskite solar cell and preparation method thereof - Google Patents
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Abstract
The invention relates to an MXene-based high-efficiency perovskite solar cell and a preparation method thereof, and belongs to the technical field of perovskite solar cells. The high-efficiency perovskite solar cell comprises a transparent conductive glass cathode, an electron transport layer, a perovskite layer, a hole transport layer and a metal anode from bottom to top in sequence; the electron transport layer being a low-level oxide of Ti3C2TxOr for high-degree oxidation of Ti3C2TxAnd original Ti3C2TxThe composite material of (1). The perovskite solar cell of the invention is a low-degree Ti oxide solar cell3C2TxOr for high-degree oxidation of Ti3C2TxAnd original Ti3C2TxThe composite material is used as a high-efficiency perovskite solar cell of an electron transport layer, and the photoelectric conversion efficiency of the perovskite solar cell can reach 18.29%. The preparation method of the high-efficiency perovskite solar cell provided by the invention has the advantages of simple and feasible synthesis process, low equipment requirement and good industrial application prospect.
Description
Technical Field
The invention belongs to the technical field of perovskite solar cells, and particularly relates to an MXene-based high-efficiency perovskite solar cell and a preparation method thereof.
Background
Solar energy has the advantages of environmental friendliness, abundant resources, renewability and the like, and is an important ring for solving the problems of energy shortage, environmental pollution and the like in the current society. The perovskite solar cell is a third-generation solar cell taking a perovskite type organic metal halide semiconductor material as a light absorption layer, and has the advantages of low cost, simple preparation process, good flexibility and good application prospect.
The perovskite type solar cell generally comprises five parts, namely transparent conductive glass, an electron transport layer, a perovskite absorption layer, a hole transport layer and a metal counter electrode. The electron transport layer has important significance in the perovskite solar cell, the high-efficiency electron transport layer can effectively transport electrons and block holes, the recombination rate of current carriers is reduced, and the accumulation of the current carriers in the device is avoided, so that the solar photoelectric conversion efficiency is improved, the service life of the device is prolonged, and the like.
Ti3C2TxThe (MXene) material is used as a two-dimensional layered material with high conductivity, flexibility and adjustable surface functional groups, and has wide application in the fields of energy storage, catalysis, medical treatment and the like. The material can be prepared at low temperature, is flexible, has high transmittance and the like, and has great application potential as an electron transport layer in perovskite solar cells.
Disclosure of Invention
The invention aims to provide an MXene-based high-efficiency perovskite solar cell and a preparation method thereof3C2TxOr a high degree of oxidation of Ti3C2TxAnd original Ti3C2TxThe perovskite solar cell with the composite material as the electron transport layer has the photoelectric conversion efficiency as high as 18.29 percent.
In order to achieve the above purpose, the technical scheme of the invention is as follows:
the invention provides an MXene-based high-efficiency perovskite solar cell which sequentially comprises a transparent conductive glass cathode, an electron transport layer, a perovskite layer, a hole transport layer and a metal anode from bottom to top;
the electron transport layer is low-degree oxidized Ti3C2TxOr for high-degree oxidation of Ti3C2TxAnd original Ti3C2TxThe composite of (a);
the low degree of oxidation of Ti3C2TxTo be Ti3C2TxThe colloidal solution was stirred on a 50 ℃ hot stand, and the solution after stirring for 48 hours was defined as a low-degree oxidized Ti3C2Tx;
The high degree of oxidation of Ti3C2TxTo be Ti3C2TxThe colloidal solution was stirred on a 50 ℃ hot plate, and the solution after stirring for 72 hours was defined as highly oxidized Ti3C2Tx;
The original Ti3C2TxIs untreated Ti3C2TxA colloidal solution.
In the above technical solution, the Ti 3C2TxThe concentration of the colloidal solution was 3.0 mg/mL.
In the technical scheme, the composite material has high-degree oxidized Ti3C2TxAnd original Ti3C2TxThe volume ratio of (A) to (B) is 1:1-10: 1.
In the technical scheme, the composite material has high-degree oxidized Ti3C2TxAnd original Ti3C2TxThe volume ratio of (A) to (B) is 1:1-5: 1.
In the technical scheme, the composite material has high-degree oxidized Ti3C2TxAnd original Ti3C2TxIs 5: 1.
In the technical scheme, the cathode of the transparent conductive glass is Indium Tin Oxide (ITO), and the perovskite layer is CH3NH3PbI3The hole transport layer is Spiro-OMeTAD ((2,2',7,7' -tetra [ N, N-di (4-methoxyphenyl) amino)]-9,9' -spirobifluorene)), the metal anode being Ag.
In the above technical solution, the thickness of the electron transport layer is 15-25nm, the thickness of the perovskite layer is 290-310nm, the thickness of the hole transport layer is 120-140nm, and the thickness of the metal anode is 50-70 nm.
The invention also provides a preparation method of the MXene-based high-efficiency perovskite solar cell, which comprises the following steps:
1) carrying out ultraviolet ozone pretreatment on a transparent conductive glass cathode;
2) spin-coating an electron transport layer on transparent conductive glass;
3) spin coating a perovskite layer on the electron transport layer;
4) Spin coating a hole transport layer on the perovskite layer;
5) evaporating a metal anode on the hole transport layer;
the method is characterized in that the step 2) specifically comprises the following steps:
placing the transparent conductive glass pretreated by ultraviolet ozone in the step 1) on a spin coater, and spin-coating low-degree Ti oxide3C2TxOr high degree of oxidation of Ti3C2TxAnd original Ti3C2TxAfter the spin coating is finished, the composite material is subjected to annealing treatment and ultraviolet ozone treatment.
In the technical scheme, the rotation speed of the spin coating of the electron transport layer in the step 2) is 2500rpm/min and 30 seconds of rotation, the annealing treatment is 100 ℃ annealing for 30min, and the ultraviolet ozone treatment is 30 minutes.
In the technical scheme, one specific implementation manner of the preparation method of the MXene-based high-efficiency perovskite solar cell is as follows:
1) and (3) treating a transparent conductive glass cathode:
carrying out ultraviolet ozone pretreatment on the cleaned transparent conductive glass for 30 minutes;
2) preparing and processing an electron transport layer:
placing the transparent conductive glass pretreated by ultraviolet ozone in the step 1) on a spin coater, and spin-coating low-degree Ti oxide3C2TxOr high degree of oxidation of Ti3C2TxAnd original Ti3C2TxThe composite material rotates at the speed of 2500rpm/min for 30s, and after the spin coating is finished, annealing treatment is carried out Annealing at 100 deg.C for 30min, and performing ultraviolet ozone treatment for 30 min;
3) preparation of perovskite layer:
placing the device in the step 2) in a glove box filled with argon, spin-coating a perovskite precursor solution on an electron transport layer, wherein the spin-coating process is 5000rpm/min for 30 seconds, dropwise adding 350 microliters of chlorobenzene in 25 seconds, and after the spin-coating process is finished, placing the device on a hot bench for annealing at the annealing temperature and the annealing time of 100 ℃ for 10 minutes;
4) preparation of hole transport layer:
spin coating a hole transport layer on the perovskite layer at 4000rpm/min for 30 seconds, and then placing the perovskite layer in a drying oven to oxidize the perovskite layer for 1 night;
5) preparing a metal anode:
using vacuum evaporation coating machine to make pressure less than 6 x 10-4Evaporating metal anode on the hole transport layer at Pa with the evaporation rate of
The invention has the beneficial effects that:
the perovskite solar cell of the invention is a low-degree Ti oxide solar cell3C2TxOr for high-degree oxidation of Ti3C2TxAnd original Ti3C2TxThe composite material is used as a high-efficiency perovskite solar cell of an electron transport layer, and the photoelectric conversion efficiency of the perovskite solar cell can reach 18.29%.
The preparation method of the high-efficiency perovskite solar cell provided by the invention has the advantages of simple and feasible synthesis process, low equipment requirement and good industrial application prospect.
Drawings
The present invention will be described in further detail with reference to the accompanying drawings and specific embodiments.
FIG. 1 is a graph based on low degree of oxidation of Ti in accordance with the present invention3C2TxOr for high-degree oxidation of Ti3C2TxAnd original Ti3C2TxThe structural diagram of the high-efficiency perovskite solar cell device using the composite material as an electron transport layer is shown.
FIG. 2 shows that the present invention is based on Ti3C2TxLow degree of oxidation of Ti3C2TxHigh degree of oxidation of Ti3C2TxAnd high degree of oxidation of Ti3C2TxAnd original Ti3C2TxPhotograph of the solution of the composite.
FIG. 3 is a Ti-based alloy prepared according to the present invention3C2TxLow degree of oxidation of Ti3C2TxHigh degree of oxidation of Ti3C2TxAnd high degree of oxidation of Ti3C2TxAnd original Ti3C2TxJ-V curve diagram of high efficiency perovskite solar cell device with composite material as electron transport layer.
Detailed Description
The invention provides a Ti-based material with reference to FIG. 13C2Tx(TxRepresents a surface functional group, typically x has the value 2, comprising-F, -OH and ═ O functional groups. ) The high-efficiency perovskite solar cell comprises a transparent conductive glass cathode, an electron transport layer, a perovskite layer, a hole transport layer and a metal anode from bottom to top in sequence; characterized in that the electron transport layer is a low-degree oxidized Ti3C2TxOr for high-degree oxidation of Ti3C2TxAnd original Ti3C2TxThe composite of (a); the low degree of oxidation of Ti 3C2TxTo be Ti3C2TxThe colloidal solution was stirred on a 50 ℃ hot stand, and the solution after stirring for 48 hours was defined as a low-degree oxidized Ti3C2Tx(ii) a The high degree of oxidation of Ti3C2TxTo be Ti3C2TxThe colloidal solution was stirred on a 50 ℃ hot plate, and the solution after stirring for 72 hours was defined as highly oxidized Ti3C2Tx(ii) a The original Ti3C2TxIs untreated Ti3C2TxA colloidal solution. It is preferable that the Ti is3C2TxThe concentration of the colloidal solution is 3.0mg/mL, and the Ti oxide with high degree is in the composite material3C2TxAnd original Ti3C2TxIs 1:1 to 10:1, and further preferably high degree of oxidation of Ti in the composite material3C2TxAnd original Ti3C2TxIn a volume ratio of 1:1 to 5:1, most preferably high degree of oxidation of Ti in the composite material3C2TxAnd original Ti3C2TxIs 5: 1.
The cathode of the transparent conductive glass is Indium Tin Oxide (ITO), and the perovskite layer is CH3NH3PbI3The hole transport layer is Spiro-OMeTAD ((2,2',7,7' -tetra [ N, N-di (4-methoxyphenyl) amino)]-9,9' -spirobifluorene)), the metal anode being Ag.
The thickness of the electron transport layer is 15-25nm, the thickness of the perovskite layer is 290-310nm, the thickness of the hole transport layer is 120-140nm, and the thickness of the metal anode is 50-70 nm.
The invention also provides a preparation method of the MXene-based high-efficiency perovskite solar cell, which comprises the following steps:
1) And (3) treating a transparent conductive glass cathode:
carrying out ultraviolet ozone pretreatment on the cleaned transparent conductive glass for 30 minutes;
2) preparing and processing an electron transport layer:
placing the transparent conductive glass pretreated by ultraviolet ozone in the step 1) on a spin coater, and spin-coating low-degree Ti oxide3C2TxOr high degree of oxidation of Ti3C2TxAnd original Ti3C2TxThe composite material rotates at the rotating speed of 2500rpm/min for 30s, annealing treatment is carried out after the spin coating is finished, the annealing temperature and the annealing time are 100 ℃, the annealing treatment is carried out for 30min, and then ultraviolet ozone treatment is carried out for 30 min;
3) preparation of perovskite layer:
placing the device in the step 2) in a glove box filled with argon, spin-coating a perovskite precursor solution on an electron transport layer, wherein the spin-coating process is 5000rpm/min for 30 seconds, dropwise adding 350 microliters of chlorobenzene in 25 seconds, and after the spin-coating process is finished, placing the device on a hot bench for annealing at the annealing temperature and the annealing time of 100 ℃ for 10 minutes;
4) preparation of hole transport layer:
spin coating a hole transport layer on the perovskite layer at 4000rpm/min for 30 seconds, and then placing the perovskite layer in a drying oven to oxidize the perovskite layer for 1 night;
5) preparing a metal anode:
using vacuum evaporation coating machine to make pressure less than 6 x 10 -4Evaporating metal anode on the hole transport layer at Pa with the evaporation rate of
Ti used in the invention3C2TxColloidal solution, low degree of oxidation Ti3C2TxHigh degree of oxidation of Ti3C2TxHigh degree of oxidation of Ti3C2TxAnd original Ti3C2TxThe preparation process of the composite material is as follows:
step 1, Ti3C2TxPreparation of colloidal solution:
adding 0.8g LiF into 10mL of 9mol/L hydrochloric acid, stirring, and stirring to fully dissolve 0.5g Ti3AlC2Slowly adding the mixture into the solution, and continuously etching the solution for 24 hours under an oil bath at the temperature of 35 ℃; then, centrifuging the etched material for 5 minutes at 8000 rpm for multiple times, pouring out the clear liquid after centrifugation, and adding deionized water for cleaning until the pH value is adjusted>5; then, under the protection of argon, performing ice-bath ultrasonic treatment for 30 minutes, performing centrifugal treatment for 1 hour at the rotating speed of 3500 revolutions, and obtaining a clear liquid which is Ti after the centrifugation is finished3C2TxA colloidal solution;
taking a certain volume of Ti3C2TxVacuum filtering the dispersion liquid to obtain Ti3C2TxThe membrane was completely dried and weighed to calculate its concentration;
step 3, oxidizing Ti3C2TxPreparation of colloidal solution
Mixing Ti3C2TxThe colloidal solution was stirred on a 50 ℃ hot stand, and the solution after stirring for 48 hours was defined as a low-degree oxidized Ti 3C2Tx(ii) a The solution after stirring for 72 hours is defined as highly oxidized Ti3C2Tx;
Step 4, oxidizing Ti to a high degree3C2TxAnd original Ti3C2TxPreparation of composite materials
Oxidizing Ti to a high degree in terms of volume ratio3C2TxWith the original Ti3C2TxMixing the solutions of the materials to obtain high-degree oxidized Ti3C2TxAnd original Ti3C2TxA composite material.
According to the high-efficiency perovskite solar cell, when the perovskite layer is CH3NH3PbI3The preparation process of the precursor solution is as follows:
in an argon glove box, 1.3Mol of PbI2(242mg) and 1.3Mol of CH3NH3I (83mg) was dissolved in 408. mu.L of a 4:1 by volume DMF/DMSO solution and stirred at ambient temperature for 1 hour.
The hole transport layer is Spiro-OMeTAD, and the preparation process of the solution is as follows:
in an argon glove box, Spiro-OMeTAD was dissolved in chlorobenzene and stirred at room temperature to dissolve, resulting in a solution of Spiro-OMeTAD at a concentration of 80mg/mL, followed by addition of 10.5. mu.L/mL of TBP solution and 15.5. mu.L/mL of Li-TFSI solution at a concentration of 510mg/mL as additives.
The present invention will be described in detail with reference to the accompanying drawings.
In order to further understand the present invention, the following technical solutions are clearly and completely described with reference to the following embodiments, but the embodiments of the present invention are only for explaining the present invention and do not limit the present invention, and all other embodiments obtained by those skilled in the art without creative efforts belong to the protection scope of the present invention.
The starting materials used in the following examples are all commercially available products.
Examples
1) Sequentially carrying out ultrasonic treatment on the etched ITO by using an ITO cleaning agent, deionized water, acetone, alcohol and isopropanol for 30 minutes;
2) taking etched Ti3C2TxThe solution concentration of the colloidal solution was adjusted to 3.0mg/mL, and Ti was added3C2TxThe colloidal solution is placed on a 50 ℃ hot bench to be stirred, and the solution after stirring for 48 hours is low-degree oxidized Ti3C2Tx(ii) a The solution after stirring for 72 hours is high-degree oxidized Ti3C2Tx(ii) a Oxidizing Ti to a high degree3C2TxWith the original Ti3C2TxMaterial (Ti)3C2TxColloidal solution) are mixed with solutions with the volume ratios of 1:1, 5:1 and 10:1 respectively to obtain high-degree Ti oxide compounded with different volume ratios3C2TxAnd original Ti3C2TxA composite material.
3) Pretreating ITO with ultraviolet ozone for 30 minutes, placing on a spin coater, and respectively spin-coating Ti at 2500rpm/min for 30s3C2TxLow degree of oxidation of Ti3C2TxHigh degree of oxidation of Ti3C2TxAnd high-degree oxidized Ti compounded in different volume ratios3C2TxAnd original Ti3C2TxComposite material, subsequently UV-deodorizing the substrates separatelyOxygen treatment for 30 minutes.
4) Preparing CH in an argon glove box3NH3PbI3Precursor solution, 1.3Mol of PbI2(242mg) and 1.3Mol of CH3NH3I (83mg) was dissolved in 408. mu.L of a 4:1 by volume DMF/DMSO solution and stirred at ambient temperature for 1 hour. The substrate is put into a glove box, the perovskite precursor solution is spin-coated on the electron transport layer, the rotation speed is 5000rpm/min, the time is 30 seconds, 350 microliters of chlorobenzene is dropwise added in 25 seconds, after the spin-coating is finished, the substrate is placed on a hot bench to be annealed, and the annealing temperature and the annealing time are 100 ℃ for 10 minutes.
5) Then, a solution of Spiro-OMeTAD was prepared in an argon glove box, dissolved in chlorobenzene, and stirred at room temperature to dissolve, to obtain a solution of Spiro-OMeTAD having a concentration of 80mg/mL, followed by addition of 10.5. mu.L/mL of TBP solution and 15.5. mu.L/mL of Li-TFSI solution having a concentration of 510mg/mL as additives and stirring for 5 minutes. Subsequently spin-coating the Spiro-OMeTAD solution on CH at 4000rpm/min for 60s3NH3PbI3A Spiro-OMeTAD film was formed on the layer.
6) Finally, the substrate is sent into an organic evaporation evaporator, and when the pressure in the cavity is lower than 6 x 10-4Pa time evaporation of anode silver, its evaporation rateThe silver film thickness was 60 nm. Thereby obtaining a Ti based oxide3C2TxAnd oxidized Ti3C2TxAnd original Ti3C2TxThe composite material is used as a high-efficiency perovskite solar cell of an electron transport layer. The device structure is shown in fig. 1. The thickness of the electron transport layer in this example was 20nm, the thickness of the perovskite layer was 300nm, the thickness of the hole transport layer was 130nm and the thickness of the metal anode was 60 nm. The thickness of the layers may be virtually any value within the aforementioned limits, only preferred thickness values being given here.
Table 1 shows Ti-based compositions prepared according to the invention3C2TxLow degree of oxidation of Ti3C2TxHigh degree of oxidationTi3C2TxAnd high-degree oxidized Ti compounded in different volume ratios 3C2TxAnd original Ti3C2TxThe composite material is respectively used as each photovoltaic parameter of the high-efficiency perovskite solar cell device of the electron transport layer. The most suitable mixing volume ratio is 5:1, under which the photoelectric conversion efficiency of the device is as high as 18.29%.
TABLE 1
FIG. 1 is a graph based on low degree of oxidation of Ti in accordance with the present invention3C2TxOr for high-degree oxidation of Ti3C2TxAnd original Ti3C2TxThe structural diagram of the high-efficiency perovskite solar cell device using the composite material as an electron transport layer is shown.
FIG. 2 shows that the present invention is based on Ti3C2TxLow degree of oxidation of Ti3C2TxHigh degree of oxidation of Ti3C2TxAnd high degree of oxidation of Ti3C2TxAnd original Ti3C2TxPhotograph of the solution of the composite.
FIG. 3 is a Ti-based alloy prepared according to the present invention3C2TxLow degree of oxidation of Ti3C2TxHigh degree of oxidation of Ti3C2TxAnd high degree of oxidation of Ti3C2TxAnd original Ti3C2TxThe J-V curves for the high efficiency perovskite solar cell devices with the composite materials as electron transport layers, respectively, correspond to table 1. The low-degree oxidized Ti prepared by the invention3C2Tx(MXene) and high degree of oxidation of Ti3C2TxAnd original Ti3C2TxCompared with original Ti, the high-efficiency perovskite solar cell with the composite material as the electron transport layer3C2TxThe perovskite solar cell with (MXene) as the electron transport layer has remarkable improvement on the aspect of photoelectric conversion efficiency and high-degree oxidation of Ti 3C2TxAnd original Ti3C2TxUnder the condition that the composite proportion is 5:1, the photoelectric conversion efficiency of the perovskite solar cell can reach 18.29%.
It should be understood that the above examples are only for clarity of illustration and are not intended to limit the embodiments. Other variations and modifications will be apparent to persons skilled in the art in light of the above description. And are neither required nor exhaustive of all embodiments. And obvious variations or modifications therefrom are within the scope of the invention.
Claims (10)
1. An MXene-based high-efficiency perovskite solar cell sequentially comprises a transparent conductive glass cathode, an electron transport layer, a perovskite layer, a hole transport layer and a metal anode from bottom to top;
characterized in that the electron transport layer is a low-degree oxidized Ti3C2TxOr for high-degree oxidation of Ti3C2TxAnd original Ti3C2TxThe composite of (a);
the low degree of oxidation of Ti3C2TxTo be Ti3C2TxThe colloidal solution was stirred on a 50 ℃ hot stand, and the solution after stirring for 48 hours was defined as a low-degree oxidized Ti3C2Tx;
The high degree of oxidation of Ti3C2TxTo be Ti3C2TxThe colloidal solution was stirred on a 50 ℃ hot plate, and the solution after stirring for 72 hours was defined as highly oxidized Ti 3C2Tx;
The original Ti3C2TxIs untreated Ti3C2TxA colloidal solution;
wherein, Ti3C2TxMiddle TxRepresents a surface functional group, x has the value 2 and comprises-F, -OH and ═ O functional groups.
2. The MXene-based high efficiency perovskite solar cell of claim 1, wherein the Ti is3C2TxThe concentration of the colloidal solution was 3.0 mg/mL.
3. The MXene-based high efficiency perovskite solar cell of claim 2, wherein the composite material has a high degree of oxidation of Ti3C2TxAnd original Ti3C2TxThe volume ratio of (A) to (B) is 1:1-10: 1.
4. The MXene-based high efficiency perovskite solar cell of claim 2, wherein the composite material has a high degree of oxidation of Ti3C2TxAnd original Ti3C2TxThe volume ratio of (A) to (B) is 1:1-5: 1.
5. The MXene-based high efficiency perovskite solar cell of claim 2, wherein the composite material has a high degree of oxidation of Ti3C2TxAnd original Ti3C2TxIs 5: 1.
6. The MXene-based high efficiency perovskite solar cell of claim 1, wherein the transparent conductive glass cathode is Indium Tin Oxide (ITO) and the perovskite layer is CH3NH3PbI3The hole transport layer is Spiro-OMeTAD ((2,2',7,7' -tetra [ N, N-di (4-methoxyphenyl) amino) ]-9,9' -spirobifluorene)), the metal anode being Ag.
7. The MXene-based high-efficiency perovskite solar cell according to claim 1, wherein the thickness of the electron transport layer is 15-25nm, the thickness of the perovskite layer is 290-310nm, the thickness of the hole transport layer is 120-140nm, and the thickness of the metal anode is 50-70 nm.
8. A method of fabricating an MXene-based high-efficiency perovskite solar cell as in any one of claims 1-7, comprising the steps of:
1) carrying out ultraviolet ozone pretreatment on the cathode of the transparent conductive glass;
2) spin coating an electron transport layer on transparent conductive glass;
3) spin coating a perovskite layer on the electron transport layer;
4) spin coating a hole transport layer on the perovskite layer;
5) evaporating a metal anode on the hole transport layer;
the method is characterized in that the step 2) specifically comprises the following steps:
placing the transparent conductive glass pretreated by ultraviolet ozone in the step 1) on a spin coater, and spin-coating low-degree Ti oxide3C2TxOr high degree of oxidation of Ti3C2TxAnd original Ti3C2TxAfter the spin coating is finished, the composite material is subjected to annealing treatment and ultraviolet ozone treatment.
9. The method for preparing the MXene-based perovskite solar cell according to claim 8, wherein the spin coating of the electron transport layer in step 2) is performed at a rotation speed of 2500rpm/min for 30s, the annealing treatment is 100 ℃ annealing for 30min, and the UV ozone treatment is 30 min.
10. The method of claim 8, wherein one embodiment is as follows:
1) and (3) processing a transparent conductive glass cathode:
carrying out ultraviolet ozone pretreatment on the cleaned transparent conductive glass for 30 minutes;
2) preparing and processing an electron transport layer:
placing the transparent conductive glass pretreated by ultraviolet ozone in the step 1) on a spin coater, and spin-coating low-degree Ti oxide3C2TxOr high degree of oxidation of Ti3C2TxAnd original Ti3C2TxThe composite material rotates at the rotating speed of 2500rpm/min for 30s, annealing treatment is carried out after the spin coating is finished, the annealing temperature and the annealing time are 100 ℃, the annealing treatment is carried out for 30min, and then ultraviolet ozone treatment is carried out for 30 min;
3) preparation of perovskite layer:
placing the device in the step 2) in a glove box filled with argon, spin-coating a perovskite precursor solution on an electron transport layer, wherein the spin-coating process is 5000rpm/min for 30 seconds, dropwise adding 350 microliters of chlorobenzene in 25 seconds, and after the spin-coating process is finished, placing the device on a hot bench for annealing at the annealing temperature and the annealing time of 100 ℃ for 10 minutes;
4) preparation of hole transport layer:
spin coating a hole transport layer on the perovskite layer at 4000rpm/min for 30 seconds, and then placing the perovskite layer in a drying oven to oxidize the perovskite layer for 1 night;
5) Preparation of the metal anode:
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