CN116490009A - Perovskite solar cell with reduced graphene oxide modified electron transport layer and preparation method thereof - Google Patents
Perovskite solar cell with reduced graphene oxide modified electron transport layer and preparation method thereof Download PDFInfo
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- CN116490009A CN116490009A CN202310420525.XA CN202310420525A CN116490009A CN 116490009 A CN116490009 A CN 116490009A CN 202310420525 A CN202310420525 A CN 202310420525A CN 116490009 A CN116490009 A CN 116490009A
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Abstract
The invention belongs to the technical field of perovskite solar cells, and provides a perovskite solar cell with a reduced graphene oxide modified electron transport layer, which comprises: a substrate; an electron transport layer disposed on the surface of the substrate; the reduced graphene oxide modification layer is arranged on the surface of the electron transport layer; the perovskite absorption layer is arranged on the surface of the reduced graphene oxide modification layer; a hole transport layer disposed on the surface of the perovskite absorption layer; and an electrode arranged on the surface of the hole transport layer. According to the invention, the electron transport layer materials such as titanium dioxide and the like are modified by utilizing the reduced graphene oxide, so that the transport of carriers at the interface between the perovskite light absorption layer and the electron transport layer can be effectively improved, and the photoelectric conversion efficiency of the solar cell is finally improved.
Description
Technical Field
The invention belongs to the technical field of perovskite solar cells, and particularly relates to a perovskite solar cell with a reduced graphene oxide modified electron transport layer and a preparation method thereof.
Background
Titanium dioxide and tin dioxide are electron transport layers commonly used in perovskite solar cells, but such inorganic oxide materials have lower electron mobility and tend to cause larger carrier loss, so that modification of such materials is required to improve the performance of the perovskite solar cells.
Disclosure of Invention
In view of the above, an object of the embodiments of the present invention is to provide a perovskite solar cell with a reduced graphene oxide modified electron transport layer and a method for preparing the same, where the perovskite solar cell provided by the present invention has a better photoelectric conversion efficiency.
The invention provides a perovskite solar cell of a reduced graphene oxide modified electron transport layer, which comprises the following components:
a substrate;
an electron transport layer disposed on the surface of the substrate;
the reduced graphene oxide layer is arranged on the surface of the electron transport layer;
the perovskite absorption layer is arranged on the surface of the reduced graphene oxide modification layer;
a hole transport layer disposed on the surface of the perovskite absorption layer;
and an electrode arranged on the surface of the hole transport layer.
Preferably, the material of the electron transport layer is selected from one or more of titanium dioxide, tin dioxide and zinc oxide.
Preferably, the thickness of the reduced graphene oxide layer is 1-10 nm.
Preferably, the perovskite absorbing layer is made of a material selected from halide perovskite.
Preferably, the hole transport layer is made of one or more materials selected from the group consisting of Spiro-OMeTAD and PTAA.
Preferably, the electrode is selected from at least one of a metal electrode, a conductive oxide electrode, and a carbon electrode.
Preferably, the thickness of the electron transport layer is 10-40 nm;
the thickness of the perovskite absorption layer is 300-800 nm;
the thickness of the hole transport layer is 100-300 nm;
the thickness of the electrode is 50-150 nm.
The invention provides a preparation method of a perovskite solar cell with a graphene modified electron transport layer, which comprises the following steps:
preparing an electron transport layer on the surface of a substrate;
preparing a reduced graphene oxide layer on the surface of the electron transport layer;
preparing a perovskite absorption layer on the surface of the reduced graphene oxide layer;
preparing a hole transport layer on the surface of the perovskite absorption layer;
and preparing an electrode on the surface of the hole transport layer.
Preferably, the method of preparing the reduced graphene oxide layer is preferably selected from electrochemical deposition methods; the electrochemical deposition method adopts a three-electrode system;
the electrolyte (electrolyte solution) in the electrochemical deposition process is graphene oxide dispersion;
the counter electrode in the electrochemical deposition process is a metal platinum electrode;
the reference electrode in the electrochemical deposition process is an Ag/AgCl electrode;
the working electrode in the electrochemical deposition process is a substrate with an electron transport layer.
Preferably, the deposition voltage in the electrochemical deposition process is-0.8 to-1.2V;
the deposition time in the electrochemical deposition process is 0.5-5 minutes.
According to the invention, the reduced graphene oxide has good conductivity, and the reduced graphene oxide is utilized to modify electron transport layer materials such as titanium dioxide, so that the transport of carriers at the interface between the perovskite light absorption layer and the electron transport layer can be effectively improved, and the photoelectric conversion efficiency of the solar cell is finally improved.
According to the invention, the reduced graphene oxide modified inorganic oxide electron transport layer with high carrier mobility is adopted, so that the interface carrier transport efficiency can be effectively improved, and the device performance can be improved. In addition, by adopting an electrochemical modification method, the rapid and efficient deposition can be realized, the thickness is controllable, and the electron transport layer is not damaged.
Drawings
Fig. 1 is a graph showing the results of performance test of the solar cell prepared in example 1;
fig. 2 is a graph showing the results of performance test of the solar cell prepared in example 2;
fig. 3 is a performance test result of the solar cell prepared in comparative example 1.
Detailed Description
The following description of the technical solutions in the embodiments of the present invention will be clear and complete, and it is obvious that the described embodiments are only some embodiments of the present invention, but not all embodiments. All other embodiments, which can be made by those skilled in the art based on the embodiments of the invention without making any inventive effort, are intended to be within the scope of the invention.
The invention provides a perovskite solar cell of a reduced graphene oxide modified electron transport layer, which comprises the following components:
a substrate;
an electron transport layer disposed on the surface of the substrate;
the reduced graphene oxide layer is arranged on the surface of the electron transport layer;
the perovskite absorption layer is arranged on the surface of the reduced graphene oxide modification layer;
a hole transport layer disposed on the surface of the perovskite absorption layer;
and an electrode arranged on the surface of the hole transport layer.
In the present invention, the substrate is preferably made of FTO (transparent conductive glass) and/or ITO (transparent conductive glass).
In an embodiment of the present invention, the material of the electron transport layer may be one or more selected from titanium dioxide, tin dioxide, and zinc oxide; the thickness of the electron transport layer may be selected from 10 to 40nm, such as 20nm, 30nm.
In embodiments of the present invention, the reduced graphene oxide layer may have a thickness selected from 1 to 10nm, such as 2nm, 3nm, 4nm, 5nm, 6nm, 7nm, 8nm, 9nm.
In an embodiment of the present invention, the perovskite absorbing layer may be made of perovskite or halide perovskite, and the perovskite may have a crystal structure of ABX 3 A can be at least one of organic cations or inorganic cations, and can be at least one of formamidine ions (FA), methylamine ions (MA) and cesium ions (Cs); b may be a divalent metal ion, and may be at least one selected from lead ion (Pb) and stannous ion (Sn); x may be a halogen ion, and may be at least one selected from iodide (I), bromide (Br) and chloride (Cl).
In embodiments of the invention, the thickness of the perovskite absorber layer may be selected from 300 to 800nm, such as 400nm, 500nm, 600nm, 700nm.
In an embodiment of the present invention, the electrode may be selected from at least one of a metal electrode, a conductive oxide transparent electrode, a carbon electrode, and a graphite electrode.
In embodiments of the invention, the thickness of the electrode may be selected from 50 to 150nm, such as 80nm, 100nm, 120nm.
The invention provides a preparation method of a perovskite solar cell with a reduced graphene oxide modified electron transport layer, which comprises the following steps:
preparing an electron transport layer on the surface of a substrate;
preparing a reduced graphene oxide layer on the surface of the electron transport layer;
preparing a perovskite absorption layer on the surface of the reduced graphene oxide layer;
preparing a hole transport layer on the surface of the perovskite absorption layer;
and preparing an electrode on the surface of the hole transport layer.
In the embodiment of the invention, the substrate can be cleaned and then treated; the cleaning can be sequentially performed by adopting acetone, isopropanol and deionized water; drying, such as blow drying, and processing; the treatment may be an ultraviolet-ozone treatment; the treatment time may be 10 to 30 minutes, such as 20 minutes.
In the embodiment of the invention, an electron transport layer is prepared on a substrate, a reduced graphene oxide modification layer can be deposited on the electron transport layer by an electrochemical method, a perovskite absorption layer is prepared on the reduced graphene oxide modification layer, a hole transport layer is prepared on the perovskite absorption layer, and finally an electrode is prepared.
In an embodiment of the present invention, the electron transport layer may be prepared by a method selected from a chemical bath deposition method, an atomic layer deposition method, and a spin coating method, such as a chemical bath deposition method. In an embodiment of the present invention, a method for preparing an electron transport layer may include:
and immersing the substrate in the electron transport layer precursor solution for heating, and then taking out, washing and annealing to obtain the electron transport layer.
In an embodiment of the present invention, the electron transport layer precursor may be titanium tetrachloride; the solvent in the electron transport layer precursor solution may be water. In an embodiment of the present invention, the electron transport layer precursor solution may be a titanium tetrachloride solution; the preparation method of the titanium tetrachloride solution can comprise the following steps:
dropwise adding titanium tetrachloride into ice water, and uniformly mixing to obtain titanium tetrachloride solution.
In an embodiment of the present invention, the volume ratio of titanium tetrachloride to water may be (2 to 5): 200 may be (3 to 4): 200.
in embodiments of the invention, heating may be performed in an oven; the heating temperature can be 65-75 ℃ or 70 ℃; the heating time may be 60 to 120 minutes, 80 to 100 minutes, or 90 minutes. In the embodiment of the invention, the washing can be performed by adopting water and ethanol, the water can be deionized water, and the ethanol can be absolute ethanol. In the embodiment of the invention, the annealing temperature can be 170-190 ℃ or 180 ℃; the annealing time may be 30 to 60 minutes or 40 to 50 minutes.
In an embodiment of the present invention, the preparation method of the reduced graphene oxide (modified) layer may be selected from electrochemical deposition methods; a three-electrode system can be adopted in the electrochemical deposition process; the electrolyte in the electrochemical deposition process can be graphene oxide dispersion liquid, and the solvent in the graphene oxide dispersion liquid can be water, such as deionized water; the concentration of the graphite oxide dispersion liquid can be 0.5-2 mg/mL, 1-1.5 mg/mL, or 1.2-1.3 mg/mL; the counter electrode in the electrochemical deposition process can be metallic platinum; the reference electrode in the electrochemical deposition process can be Ag/AgCl; the working electrode in the electrochemical deposition process can be a substrate with an electron transport layer (i.e., a product obtained after preparing the electron transport layer on the surface of the substrate); the deposition voltage in the electrochemical deposition process can be-0.8 to-1.2V, can be-0.9 to-1.1V, and can be-1V; the deposition time in the electrochemical deposition process may be 0.5 to 5 minutes, may be 1 to 4 minutes, or may be 2 to 3 minutes.
In the present invention, the preparation method of the graphene oxide dispersion liquid may include:
graphene oxide is dispersed in water.
In the embodiment of the invention, the preparation method of the perovskite absorption layer can be selected from one or more of spin coating, knife coating and slit coating. In an embodiment of the present invention, a method of preparing a perovskite absorber layer may include:
and spin-coating the perovskite solution on the surface of the reduced graphene oxide layer, and then annealing.
In an embodiment of the present invention, the solute in the perovskite solution may be selected from formamidine iodide, cesium iodide, lead iodide, methylamine chloride, lead bromide, and the like; the solvent in the perovskite solution can be selected from one or more of DMF (N, N-dimethylformamide) and DMSO (dimethyl sulfoxide); the molar concentration of the perovskite solution may be 0.7 to 1.5mol/L or 1.2 to 1.3mol/L.
In an embodiment of the invention, the perovskite solution can be spin-coated on the surface of the reduced graphene oxide; the rotating speed in the spin coating process can be 2500-3500 rpm, 2800-3200 rpm or 3000rpm; the spin coating time can be 30-50 s, can be 35-45 s, can be 50s; the anti-solvent may be added dropwise at 10s during spin coating, and the anti-solvent may be diethyl ether, such as anhydrous diethyl ether.
In the embodiment of the invention, the annealing temperature can be 130-170 ℃, 140-160 ℃ or 150 ℃; the annealing time may be 20 to 40 minutes, 25 to 35 minutes, or 30 minutes.
In an embodiment of the present invention, the preparation method of the hole transport layer may be selected from spin coating methods, and may include:
and spin-coating the hole transport layer precursor solution on the perovskite absorption layer to obtain the hole transport layer.
In an embodiment of the present invention, the solute in the hole transport layer precursor solution may be selected from the group consisting of Spiro-OMeTAD, 4-t-butylpyridine, lithium bistrifluoromethane sulfonimide solution (520 mg mL) -1 Dissolved in acetonitrile); the solvent in the hole transport layer precursor solution may be selected from chlorobenzene; the mass concentration of the hole transport layer precursor solution may be Spiro-ome: 50-100 mg mL -1 May be 60-90 mg mL -1 May also be 70-80 mg mL -1 The method comprises the steps of carrying out a first treatment on the surface of the 4-tert-butylpyridine: 30-50 mu L mL -1 Can be 35 to 45 mu L mL -1 May be 40. Mu.L/mL -1 The method comprises the steps of carrying out a first treatment on the surface of the Lithium bis (trifluoromethanesulfonyl) imide solution: 20-30 mu L mL -1 Can be 22-26 mu L mL -1 May be 23. Mu.L/mL -1 . In the embodiment of the invention, the rotating speed of spin coating can be 2500-3500 rpm, 2800-3200 rpm or 3000rpm; the spin coating time may be 20 to 40 seconds, 25 to 35 seconds, or 30 seconds.
In an embodiment of the present invention, the electrode may be prepared by a method selected from a vacuum evaporation method and a sputtering method; the vacuum degree in the vacuum evaporation process can be lower than 10 -4 Pa, deposition rate may beCan also be +.>Can also be +.>
According to the invention, the reduced graphene oxide modified inorganic oxide electron transport layer with high carrier mobility is adopted, so that the interface carrier transport efficiency can be effectively improved, and the device performance can be improved. In addition, by adopting an electrochemical modification method, the rapid and efficient deposition can be realized, the thickness is controllable, and the electron transport layer is not damaged.
Example 1
The FTO glass substrate is cleaned by acetone, isopropanol and deionized water in sequence, and is treated by ultraviolet-ozone for 20 minutes after being dried. Dropwise adding 4.5mL of titanium tetrachloride into 200mL of ice water, uniformly mixing to prepare a titanium tetrachloride solution, placing FTO glass into the titanium tetrachloride solution, placing the titanium tetrachloride solution into a 70 ℃ oven for 60 minutes, taking out, washing the titanium tetrachloride solution with deionized water and absolute ethyl alcohol, and annealing the titanium tetrachloride solution at 180 ℃ for 30 minutes to obtain a titanium dioxide layer.
And depositing a 2nm reduced graphene oxide layer on the titanium dioxide layer by adopting an electrochemical deposition method, wherein the concentration of graphene oxide dispersion liquid is 1.5mg/mL, the titanium dioxide layer is a working electrode, an Ag/AgCl electrode is a reference electrode, a platinum electrode is a counter electrode, the deposition voltage is-1.2V, and the deposition time is 2 minutes.
Preparation of perovskite precursor solutions in a nitrogen glove box (solutes in the perovskite precursor solution are FAI, pbI 2 And MACl, pbI 2 Molar ratio to FAI is 1:1, MACl and PbI 2 The molar ratio of (2) is 0.35: 1) The concentration is 1.4mol/L, and the volume ratio of the solvent is 9: 1) 50 microliters of a perovskite precursor solution was dropped on the reduced graphene oxide layer, spin-coated at 5000rpm for 15s, 150 microliters of anhydrous diethyl ether was added dropwise at 10s, and annealing was performed at 150 ℃ for 20 minutes, to obtain a perovskite layer.
72mg of Spiro-OMeTAD and 39. Mu.l of 4-t-butylpyridine were dissolved in 1mL of chlorobenzene, and 23. Mu.l of 520mg mL were added -1 And (3) uniformly mixing the acetonitrile solution of the lithium bis (trifluoromethanesulfonyl) imide, and spin-coating the mixture at 3000rpm for 30s on a perovskite layer to obtain a hole transport layer.
Silver electrode is prepared on the hole transport layer by vacuum evaporation, and the vacuum degree is lower than 10 -4 Pa, deposition rateAnd obtaining the perovskite solar cell.
In the perovskite solar cell prepared in the embodiment 1 of the invention, the thickness of the electron transport layer (titanium dioxide layer) is 20nm, the thickness of the reduced graphene oxide layer is 2nm, the thickness of the perovskite layer is 400nm, the thickness of the hole transport layer is 200nm, and the thickness of the silver electrode is 70nm.
Example 2
A perovskite solar cell was prepared according to the method of example 1, differing from example 1 in that the reduced graphene oxide layer had a thickness of 5nm.
Comparative example 1
A perovskite solar cell was produced according to the method of example 1, which differs from example 1 in that a reduced graphene oxide layer was not produced, and the perovskite solar cell obtained did not contain a reduced graphene oxide layer.
Performance detection
At room temperature, using a 3A solar simulator at 100mW/cm 2 The perovskite solar cells prepared in examples and comparative examples were tested for photoelectric conversion efficiency under light intensity, and the effective area of the cells was 0.09cm 2 The method comprises the steps of carrying out a first treatment on the surface of the As shown in FIGS. 1 to 3, it is understood that the battery prepared in example 1 has a short-circuit current density of 25.60mA/cm 2 Open circuit voltage 1.115V, fill factor 81.03%, photoelectric conversion efficiency 23.14%; the battery prepared in example 2 had a short-circuit current density of 25.76mA/cm 2 Open circuit voltage 1.101V, fill factor 81.80%, photoelectric conversion efficiency 23.23%; short-circuit current Density 25.60mA/cm of the cell prepared in comparative example 1 2 Open circuit voltage 1.083V, fill factor 79.59%, photoelectric conversion efficiency 22.07%.
According to the invention, the graphene modified inorganic oxide electron transport layer with high carrier mobility is adopted, so that the interface carrier transport efficiency can be effectively improved, and the device performance can be improved. In addition, by adopting an electrochemical modification method, the rapid and efficient deposition can be realized, the thickness is controllable, and the electron transport layer is not damaged.
While the invention has been described and illustrated with reference to specific embodiments thereof, the description and illustration is not intended to limit the invention. It will be apparent to those skilled in the art that various changes may be made in this particular situation, material, composition of matter, substance, method or process without departing from the true spirit and scope of the invention as defined by the following claims, so as to adapt the objective, spirit and scope of the present application. All such modifications are intended to be within the scope of this appended claims. Although the methods disclosed herein have been described with reference to particular operations being performed in a particular order, it should be understood that these operations may be combined, sub-divided, or reordered to form an equivalent method without departing from the teachings of the present disclosure. Thus, unless specifically indicated herein, the order and grouping of operations is not a limitation of the present application.
Claims (10)
1. A perovskite solar cell having a reduced graphene oxide modified electron transport layer, comprising:
a substrate;
an electron transport layer disposed on the surface of the substrate;
the reduced graphene oxide layer is arranged on the surface of the electron transport layer;
the perovskite absorption layer is arranged on the surface of the reduced graphene oxide modification layer;
a hole transport layer disposed on the surface of the perovskite absorption layer;
and an electrode arranged on the surface of the hole transport layer.
2. The perovskite solar cell of the reduced graphene oxide modified electron transport layer according to claim 1, wherein the electron transport layer is made of one or more materials selected from titanium dioxide, tin dioxide and zinc oxide.
3. The reduced graphene oxide modified electron transport layer perovskite solar cell of claim 1, wherein the reduced graphene oxide layer has a thickness of 1-10 nm.
4. The reduced graphene oxide modified electron transport layer perovskite solar cell of claim 1, wherein the perovskite absorber layer is selected from the group consisting of halide perovskites.
5. The perovskite solar cell of the reduced graphene oxide modified electron transport layer according to claim 1, wherein the hole transport layer is made of one or more materials selected from Spiro-ome tad and PTAA.
6. The reduced graphene oxide modified electron transport layer perovskite solar cell of claim 1, wherein the electrode is selected from at least one of a metal electrode, a conductive oxide electrode, a carbon electrode.
7. The reduced graphene oxide modified electron transport layer perovskite solar cell of claim 1, wherein the electron transport layer has a thickness of 10-40 nm;
the thickness of the perovskite absorption layer is 300-800 nm;
the thickness of the hole transport layer is 100-300 nm;
the thickness of the electrode is 50-150 nm.
8. A method of preparing a perovskite solar cell having a reduced graphene oxide modified electron transport layer according to claim 1, comprising:
preparing an electron transport layer on the surface of a substrate;
preparing a reduced graphene oxide layer on the surface of the electron transport layer;
preparing a perovskite absorption layer on the surface of the reduced graphene oxide layer;
preparing a hole transport layer on the surface of the perovskite absorption layer;
and preparing an electrode on the surface of the hole transport layer.
9. The method of preparation according to claim 8, wherein the method of preparation of the reduced graphene oxide layer is preferably selected from electrochemical deposition methods; the electrochemical deposition method adopts a three-electrode system;
the electrolyte solution in the electrochemical deposition process is graphene oxide dispersion liquid;
the counter electrode in the electrochemical deposition process is a metal platinum electrode;
the reference electrode in the electrochemical deposition process is an Ag/AgCl electrode;
the working electrode in the electrochemical deposition process is a substrate with an electron transport layer.
10. The method according to claim 9, wherein the deposition voltage during the electrochemical deposition method is-0.8 to-1.2V;
the deposition time in the electrochemical deposition process is 0.5-5 minutes.
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