CN108400249B - Perovskite solar cell based on lanthanum nickelate hole transport layer and preparation method thereof - Google Patents

Perovskite solar cell based on lanthanum nickelate hole transport layer and preparation method thereof Download PDF

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CN108400249B
CN108400249B CN201810187406.3A CN201810187406A CN108400249B CN 108400249 B CN108400249 B CN 108400249B CN 201810187406 A CN201810187406 A CN 201810187406A CN 108400249 B CN108400249 B CN 108400249B
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transport layer
lanio
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陈炜
张艳君
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Huazhong University of Science and Technology
Ezhou Institute of Industrial Technology Huazhong University of Science and Technology
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    • H10K50/00—Organic light-emitting devices
    • H10K50/10—OLEDs or polymer light-emitting diodes [PLED]
    • H10K50/14—Carrier transporting layers
    • H10K50/15—Hole transporting layers
    • H—ELECTRICITY
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Abstract

The invention discloses a high-transparency conductive LaNiO-based material3A hole transport layer trans-planar perovskite solar cell and a preparation method thereof. The perovskite solar cell with the trans-form planar structure comprises a transparent conductive substrate, a hole transport layer, a perovskite light absorption layer, an electron transport layer, an interface modification layer and a metal electrode. The trans-planar perovskite solar cell has good electric conductivity, high optical transmittance and high work function, and LaNiO is prepared by reacting LaNiO with a metal oxide3The conductive film is used as a hole transport layer, so that the contact between the perovskite light absorption layer and the transparent electrode can be avoided, and the recombination of interface carriers is prevented.

Description

Perovskite solar cell based on lanthanum nickelate hole transport layer and preparation method thereof
Technical Field
The invention discloses a high-transparency conductive LaNiO-based material3A perovskite solar cell of a hole transport layer and a preparation method thereof belong to the field of solar cells made of new materials.
Background
With the development of social economy, the use demand of human beings on energy is increasing, but fossil energy such as petroleum and coal is limited due to excessive exploitation and energy pollution, and the development of new energy is urgent. Solar energy is an inexhaustible renewable clean energy, and a solar cell is a device for converting light energy into electric energy, so that the development of the solar cell is an important trend of new energy.
The perovskite material has the characteristics of narrow band gap, strong light absorption, high carrier mobility, small exciton confinement energy, simple preparation process, low cost and the like, thereby attracting great attention of researchers, rapidly developing perovskite solar cells in recent years, leading the photoelectric conversion efficiency to reach the authentication efficiency of 22.7 percent, and becoming a research hotspot of a new generation of solar cells.
Typical perovskite solar cells include mesoporous and planar structures, the perovskite layer is both a light absorption layer and an electron hole transport layer, and generated electron holes are respectively transported to a transparent conductive electrode and a metal electrode. In the trans-planar perovskite solar cell, when a hole transport layer is not added, the energy levels of the transparent conductive electrode and the perovskite light absorption layer are not matched, and the interface carrier recombination is serious. Currently, the commonly used hole transport layer materials can be classified into three categories: inorganic, polymeric, and small molecule. The polymer hole transport material has poor solubility and uncertain molecular weight, and the micromolecule hole transport material has long synthesis steps and instability to ultraviolet, so that the development of the micromolecule hole transport material is limited. The inorganic hole transport material has high hole mobility and good stability, and becomes a good hole transport material.
Disclosure of Invention
Under the strong support of national science foundation (51672094,51661135023), national focus research and development project (2016YFC0205002) and autonomous innovation research foundation (2016JCTD111) of Huazhong science and technology university, the invention provides a high-transparency conductive lanthanum nickelate (LaNiO) -based high-transparency conductive lanthanum nickelate (LaNiO)3) A perovskite solar cell with a hole transport layer and a preparation method thereof aim to solve the problems of mismatching of energy levels of a transparent conductive electrode of the perovskite solar cell with a trans-planar structure and a perovskite light absorption layer, serious interface carrier recombination and loss of internal resistance of a device.
One aspect of the invention relates to a high-transparency conductive LaNiO-based material3A hole transport layer perovskite solar cell characterized by: the perovskite solar cell sequentially comprises: the light-absorbing material comprises a transparent conductive substrate, a hole transport layer, a perovskite light-absorbing layer, an electron transport layer, an interface modification layer and a metal electrode, wherein the hole transport layer is LaNiO3A conductive film.
The invention also relates to a high-transparency conductive LaNiO-based material3The preparation method of the perovskite solar cell of the hole transport layer is characterized by comprising the following steps: the method comprises the following steps:
(1) preparing a hole transport layer on a transparent conductive substrate;
(2) preparing a perovskite light absorption layer on the hole transport layer;
(3) preparing an electron transport layer on the perovskite light absorption layer;
(4) preparing an interface modification layer on the electron transport layer;
(5) preparing a metal electrode on the interface modification layer;
wherein the hole transport layer in the step (1) is LaNiO3A conductive film.
Description
The term "transparent conductive substrate" used in the present invention is a transparent electrode having a transparent material as a substrate. The substrate is made of transparent materials such as glass, flexible plastics and the like; the transparent electrode is located on the inner surface of the substrate, and the commonly used transparent electrode material can be Fluorine Tin Oxide (FTO), Indium Tin Oxide (ITO), aluminum neoxide (AZO), or the like.
The term "hole transport layer" as used herein collects and transports holes injected from the perovskite absorption layer and functions to block electrons.
The term "perovskite light absorption layer" used in the present invention can generate electron-hole pairs by absorbing energy of photons in sunlight and transport electrons and holes to the corresponding electron or hole transport layer, respectively.
The term "electron transport layer" as used herein is used to collect and transport electrons injected from the perovskite absorption layer and to act as a hole blocking layer.
The term "interface modification layer" used in the present invention can transmit electrons and block holes. Ohmic contact can be formed at the interface between the metal electrode and the electrode by adding the interface modification layer, so that the transmission of electrons and the efficiency of collecting the electrons by the metal electrode are improved.
In certain embodiments of the present invention, the transparent conductive substrate used in the present invention is selected from FTO conductive glass, ITO conductive glass, or AZO conductive glass.
In certain embodiments of the invention, the perovskite light absorbing layer used in the invention is ABX3，A＝CH3NH3 +、CH(NH2)2 +、Cs+Or mixtures thereof; b ═ Pb2+、Sn2+Or mixtures thereof; x ═ Cl-、Br-、I-Or mixtures thereof.
In certain embodiments of the present invention, the electron transport layer used in the present invention is C60、C70Or fullerene derivative PC61CM、PC71BM。
In some embodiments of the present invention, the interface modification layer used in the present invention is LiF, 2, 9-dimethyl-4, 7-diphenyl-1, 10-phenanthroline (hereinafter abbreviated as "BCP"), TiOx。
In certain embodiments of the present invention, the metal electrode used in the present invention is Ag, Al.
The invention relates to a high-transparency conductive LaNiO-based material3A method of making a hole transport layer perovskite solar cell, comprising:
(1) preparing a hole transport layer on a transparent conductive substrate;
(2) preparing a perovskite light absorption layer on the hole transport layer;
(3) preparing an electron transport layer on the perovskite light absorption layer;
(4) preparing an interface modification layer on the electron transport layer;
(5) and preparing a metal electrode on the interface modification layer.
Wherein the hole transport layer in the step (1) is LaNiO3A conductive film.
The high-transparency conductive LaNiO-based material prepared by the invention3In some specific embodiments of the perovskite solar cell of the hole transport layer, the transparent conductive substrate is sequentially cleaned by adopting a glass cleaning agent, deionized water, industrial alcohol, absolute ethyl alcohol and acetone in the step (1), ultrasonic treatment is carried out for 20min respectively, and nitrogen is blown dry for use; the La (NO)3)3·6H2O and NiN2O6·6H2The molar ratio of O is 1: 1; preparing LaNiO with the molar concentration of 0.01-0.1mol/L3A precursor solution which is spin-coated on the transparent conductive substrate at a rotation speed of 3000-(ii) a Annealing in a heating plate at the temperature of 400-900 ℃ for 0.5-6 hours, and cooling to room temperature.
The high-transparency conductive LaNiO-based material prepared by the invention3In certain embodiments of the hole transport layer perovskite solar cell, the perovskite precursor APbX is prepared in step (2) at a molar concentration of 1-2mol/L3Solution spin-coating on LaNiO3The rotating speed is 4000-; annealing at 70-300 deg.C for 5-120min, and cooling to room temperature.
The high-transparency conductive LaNiO-based material prepared by the invention3In certain embodiments of the hole transport layer perovskite solar cell, 5-30mg/ml of PCBM solution is prepared in step (3) and spin-coated on the perovskite light absorption layer at a rotation speed of 1000-; annealing at 70 deg.C for 5-60min, and cooling to room temperature.
The high-transparency conductive LaNiO-based material prepared by the invention3In some embodiments of the perovskite solar cell of the hole transport layer, a BCP saturated solution is prepared in step (4), and is spin-coated on the electron transport layer at a rotation speed of 4000-; annealing at 70 deg.C for 5-60min, and cooling to room temperature.
The high-transparency conductive LaNiO-based material prepared by the invention3In certain embodiments of the hole transport layer perovskite solar cell, in step (5), Ag or Al is thermally vapor deposited onto the BCP interface modification layer at a deposition rate of 0.05-1A/s, at a deposition thickness of 60-300nm, and at an area of 0.09-10cm2。
Drawings
FIG. 1 is a schematic structural diagram of a trans-planar perovskite solar cell according to the present invention; wherein, 1 is a transparent conductive substrate, 2 is a hole transmission layer, 3 is a perovskite light absorption layer, 4 is an electron transmission layer, 5 is an interface modification layer, and 6 is a metal electrode.
FIG. 2 shows LaNiO according to an embodiment of the present invention3X-ray diffraction pattern of the film.
FIG. 3 shows an example of LaNiO3Ultraviolet electron energy spectrum of the film.
FIG. 4 is a scanning electron microscope image of the FTO conductive glass of the present invention.
FIG. 5 shows LaNiO on FTO conductive glass according to the present invention3Scanning electron micrographs of the films.
FIG. 6 shows the presence or absence of LaNiO on the FTO conductive glass according to the present invention3Ultraviolet-visible absorption curves of the films are compared.
FIG. 7 shows the presence or absence of LaNiO on the FTO conductive glass of the present invention3Photocurrent-voltage test curves of the films are compared.
Examples
In order to better understand the technical solution, the technical solution will be described in detail with reference to the drawings and the specific embodiments.
The reagents and raw materials used in the present invention are shown in table 1 below:
TABLE 1 reagents and starting materials for use in the invention
Figure GDA0002581668410000061
Instrument for measuring the position of a moving object：
Magnetic stirrer (MR Hei-standard, Heidolph, Germany)
Titanium substrate heating table (PZ28-3TD, Harry gestigkeit Germany)
Spin coating instrument (KW-4A, micro-electronic research institute of Chinese academy of sciences)
Vacuum thermal evaporation equipment (RV 10, IKA, Germany)
The preparation method of the perovskite solar cell comprises the following steps:
s1: the FTO conductive glass is sequentially cleaned by adopting a glass cleaning agent, deionized water, industrial alcohol, absolute ethyl alcohol and acetone, ultrasonic treatment is carried out for 20min, and nitrogen is blown dry for use.
S2 preparation of LaNiO on FTO conductive glass3Layer(s)
La(NO3)3·6H2O and NiN2O6·6H2O as solute in a molar ratio of 1:1 and a molar concentration of La of 0.05moL/L is dissolved in ethylene glycol monomethyl ether solution to be used as precursor solution. Mixing LaNiO3Spin-coating the precursor solution on the transparent conductive substrate at 2000 rpm for 30 s; annealing at 600 deg.C for 0.5 hr, and naturally cooling to room temperature.
S3: preparation of perovskite light absorption layer on LaNiO3 layer
Mixing PbI with a molar ratio of 1:12Powder and CH3NH3I, mixing and dissolving powder in a volume ratio of DMF: the mixed solution of DMSO ═ 4:1 was stirred at 30 ℃ until dissolved, to obtain CH having a Pb molar concentration of 1.5mol/L3NH3PbI3And (3) solution. The perovskite precursor solution is coated on LaNiO in a spin mode3The rotating speed is 6000 rpm/s and the time is 30 seconds on the hole transport layer; annealing at 100 deg.C for 10min, and naturally cooling to room temperature.
S4 preparation of an electron transport layer on the perovskite light absorption layer
Weighing a certain amount of PCBM, blending the PCBM into chlorobenzene to prepare a solution of 20mg/ml, stirring 45 liquid until the solution is dissolved, and spin-coating the prepared PCBM solution on a perovskite light absorption layer at the rotating speed of 1500 rpm for 30 seconds; annealing for 10min at 70 deg.C, and naturally cooling to room temperature.
S5 preparing an interface modification layer on the electron transport layer
BCP is blended into methanol to prepare saturated solution, and the prepared saturated solution of BCP is coated on the PCBM electronic transmission layer in a rotating speed of 6000 revolutions per second for 30 seconds; annealing for 10min at 70 deg.C, and naturally cooling to room temperature.
S6: preparing metal electrode on interface modifying layer
The pressure of the thermal evaporation equipment is pumped to 5 x 10-4After Pa, an evaporation power supply is started, Ag is thermally evaporated and deposited on the BCP interface modification layer, the deposition rate is 0.1 angstrom/second, the deposition thickness is 80nm, and the area is 0.09cm2。
3Characterization of LaNiO films
The invention adopts a PANalytical B.V.X-diffractometer to measure the LaNiO3The film was subjected to X-ray diffraction analysis to obtain XRD diffraction patterns of 32.1 deg., 47.1 deg. and 58.5 deg. as shown in FIG. 2Corresponding to respectively being LaNiO3Characteristic peak positions of crystal faces of the crystals (110), (200) and (211) indicate that the prepared film is LaNiO3And (4) crystals.
Ecopia HMS-3000 Hall effect tester is adopted to test the LaNiO3The film was tested and the results are shown in Table 2, which shows that LaNiO3The film had good conductivity, 3.827 × 102S/cm, the loss of the internal resistance of the battery can be effectively reduced.
3TABLE 2 Hall Effect test results for LaNiO films of the invention
Figure GDA0002581668410000081
The LaNiO is subjected to photoelectron spectroscopy on KratosAXIS-ULTRA DLD-600W3The film was subjected to UV-photoelectron spectroscopy and the measurements are shown in FIG. 3, with a lower cut-off of 0.41eV for the distance from the valence band top to the Fermi level, a higher cut-off of 16.48eV for the LaNiO, and a 21.21eV minus the higher cut-off for the LaNiO3Has a work function WF of 4.73 eV. To illustrate LaNiO3The hole transport layer has higher work function, and the work function of the electrode can be improved and the collection of holes can be promoted when the hole transport layer is prepared on the transparent conductive glass, so that the energy conversion efficiency of the device is improved; while LaNiO3The hole transport layer can avoid the contact between the perovskite light absorption layer and the transparent electrode and prevent the recombination of interface carriers.
Preparation of LaNiO on FTO conductive glass by adopting FEI silicon 200 scanning electron microscope for observation3A comparison between before and after the layers, as shown in FIGS. 4 and 5, illustrates LaNiO3The thin film is uniformly covered on the FTO conductive glass.
Method for detecting presence/absence of LaNiO on FTO conductive glass by adopting Perkin Elmer lambda 950UV/Vis/NIR3The films were subjected to UV-Vis absorption spectrum testing to obtain a UV-Vis absorption curve comparison chart, as shown in FIG. 6, which illustrates LaNiO3The film has high optical transmittance, and the light absorptivity of the film is only 2%, so that the light absorption loss is reduced.
An efficiency testing system consisting of a solar simulator and a Keithley 2400 digital source meter is adopted to test the existence/nonexistence of LaNiO on FTO conductive glass at room temperature3The film was measured. The measurement results are shown in FIG. 7, and LaNiO was obtained3The photovoltaic parameter of the perovskite solar cell as the hole transport layer is 20.7mA/cm of short-circuit current2The open circuit voltage is 1.06V, the filling factor is 79.3, the energy conversion efficiency is 17.4, and the performance is obviously higher than that of the non-LaNiO3Perovskite solar cell as hole transport layer.
While preferred embodiments of the present invention have been described, additional variations and modifications in those embodiments may occur to those skilled in the art once they learn of the basic inventive concepts. Therefore, it is intended that the appended claims be interpreted as including preferred embodiments and all such alterations and modifications as fall within the scope of the invention. It will be apparent to those skilled in the art that various changes and modifications may be made in the present invention without departing from the spirit and scope of the invention. Thus, if such modifications and variations of the present invention fall within the scope of the claims of the present invention and their equivalents, the present invention is also intended to include such modifications and variations.

Claims (10)

1. High-transparency-based conductive LaNiO3A hole transport layer perovskite solar cell characterized by: the perovskite solar cell sequentially comprises: the light-absorbing material comprises a transparent conductive substrate, a hole transport layer, a perovskite light-absorbing layer, an electron transport layer, an interface modification layer and a metal electrode, wherein the hole transport layer is LaNiO3A conductive film.
2. The method of claim 1 based on high transparent conductive LaNiO3A hole transport layer perovskite solar cell characterized by: the transparent conductive substrate is selected from FTO conductive glass, ITO conductive glass or AZO conductive glass.
3. The method of claim 1 based on high transparent conductive LaNiO3A hole transport layer perovskite solar cell characterized by: the perovskite absorbs lightThe layer is ABX3，A＝CH3NH3 +、CH(NH2)2 +、Cs+Or mixtures thereof; b ═ Pb2+、Sn2+Or mixtures thereof; x ═ Cl-、Br-、I-Or mixtures thereof.
4. The method of claim 1 based on high transparent conductive LaNiO3A hole transport layer perovskite solar cell characterized by: the electron transport layer is C60、C70Or fullerene derivative PC61CM、PC71BM。
5. The method of claim 1 based on high transparent conductive LaNiO3A hole transport layer perovskite solar cell characterized by: the interface modification layer is LiF, 2, 9-dimethyl-4, 7-diphenyl-1, 10-phenanthroline, TiOx。
6. The method of claim 1 based on high transparent conductive LaNiO3A hole transport layer perovskite solar cell characterized by: the metal electrode is Ag or Al.
7. The high transparent conductive LaNiO-based material of any one of claims 1-63The preparation method of the perovskite solar cell of the hole transport layer comprises the following steps:
(1) preparing a hole transport layer on a transparent conductive substrate;
(2) preparing a perovskite light absorption layer on the hole transport layer;
(3) preparing an electron transport layer on the perovskite light absorption layer;
(4) preparing an interface modification layer on the electron transport layer;
(5) preparing a metal electrode on the interface modification layer;
wherein the hole transport layer in the step (1) is LaNiO3A conductive film.
8. The method of claim 7The preparation method is characterized in that in the step (1), LaNiO with the molar concentration of 0.01-0.1mol/L is prepared3And spin-coating the precursor solution on the transparent conductive substrate at 3000-.
9. The production method according to claim 7, wherein the perovskite precursor APbX is produced in step (2) at a molar concentration of 1 to 2mol/L3Solution spin-coating on LaNiO3The rotating speed is 4000-; annealing at 70-300 deg.C for 5-120min, and cooling to room temperature.
10. The method as set forth in claim 7, wherein in step (3) a PCBM solution of 5-30mg/ml is prepared and spin-coated on the perovskite light-absorbing layer at a rotation speed of 1000 and 3000 rpm for 30 seconds; annealing at 70 deg.C for 5-60min, and cooling to room temperature.
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