CN114242824A - All-inorganic perovskite solar cell and preparation method thereof - Google Patents
All-inorganic perovskite solar cell and preparation method thereof Download PDFInfo
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Abstract
The application belongs to the technical field of perovskite solar cells. The application provides an all-inorganic perovskite solar cell, from sensitive surface one side, include transparent conductive substrate, electron transport layer, the passive all-inorganic perovskite light absorption layer and the electrode layer of rare earth ion in proper order. The all-inorganic perovskite solar cell improves the growth mode of all-inorganic perovskite crystals, increases the grain size, reduces gaps among grain boundaries, forms a compact perovskite film, effectively improves the transmission efficiency of current carriers, prolongs the service life of the current carriers and reduces the charge recombination rate in the all-inorganic perovskite film by introducing rare earth ions; the formed perovskite thin film has excellent hydrophobicity and is not easy to generate phase change, so that the photoelectric conversion efficiency and stability of the all-inorganic perovskite solar cell are improved. The all-inorganic perovskite solar cell prepared by the preparation method is more compact in structure layer, and the photoelectric conversion efficiency and stability of the all-inorganic perovskite solar cell are improved.
Description
Technical Field
The application belongs to the technical field of perovskite solar cells, and particularly relates to an all-inorganic perovskite solar cell and a preparation method thereof.
Background
The scale of solar energy development and utilization is rapidly enlarged, the technical progress and the industrial upgrading are accelerated, the cost is obviously reduced, and the solar energy conversion system becomes an important field of global energy conversion. The solar photovoltaic technology is an important guarantee for sustainable development and development of low-carbon circular economy in China. The perovskite solar cell is regarded as a ten-step scientific breakthrough in the world due to low cost, and is thought to promote the photovoltaic energy industry to revolutionarily change, so that the solar power generation is expected to really move to the civilization era. The development to the present day, the all-inorganic perovskite solar cell breaks through the biggest bottleneck of poor stability of the traditional organic-inorganic perovskite solar cell device. All-inorganic perovskite material CsPbIBr2Due to the characteristics of excellent stability of illumination, temperature and humidity and high temperature resistance of more than 300 ℃, the material becomes a new generation of research hotspot of scientific researchers.
Among them, the perovskite light absorption layer plays an important role in the photoelectric conversion efficiency of the solar cell. However, since the inorganic perovskite has small crystal grains and many grain boundaries, and is influenced by external environments such as temperature and humidity, a large number of defect states are generated at the grain boundaries on the surface of the polycrystalline perovskite thin film. When photons penetrate through the glass substrate to excite the perovskite light absorption layer to generate photo-generated electron-hole pairs, the electrons and the holes are compounded at the interface due to the existence of defect states, and the transmission of photocurrent to an external circuit is blocked. The defect state may also induce a shallow state near the edge of the perovskite light absorption layer, hindering hole diffusion, resulting in a reduction in photoelectric conversion capability. Therefore, the perovskite light absorption layer is always an obstacle to the optimization of the performance of the perovskite solar cell due to the defects of photoelectric conversion efficiency and stability.
Disclosure of Invention
In view of this, the present application provides an all-inorganic perovskite solar cell and a preparation method thereof, which improve photoelectric conversion efficiency and stability of the all-inorganic perovskite solar cell.
The specific technical scheme of the application is as follows:
the application provides an all-inorganic perovskite solar cell, from sensitive surface one side, include transparent conductive substrate, electron transport layer, the passive all-inorganic perovskite light absorption layer and the electrode layer of rare earth ion in proper order.
Preferably, the rare earth ion is Yb3+、Er3+、Tm3+、Ho3+、Eu3+Or Dy3+；
The raw material of the all-inorganic perovskite is CsPbIBr2；
The concentration of the rare earth ions in the all-inorganic perovskite is 0-10 mol%.
In the application, the rare earth ions are uniformly distributed on the surface of the all-inorganic perovskite light absorption layer, and are partially embedded into the adjacent oxide skeleton with the mesoporous structure and are in close contact with the oxide skeleton, so that a lattice with a stable structure can be formed. The introduction of rare earth ions can passivate defect states occurring in the perovskite light-absorbing layer, due to RE3+With Br-Strong interaction between them, RE3+The surface of the colloidal particles in the precursor solution is collected. Spin coating the precursor solution on m-TiO2After the growth, the crystal grows gradually, and the RE is highly ionized3+Mainly present at the surface and grain boundaries, while the radius (e.g., Tm) of the rare earth ions3+ 
Ho3+ 
Er3+ 
Or Yb3+ 
) With Pb2+Radius of (2)
The difference value is large, when rare earth ions are introduced into a stable perovskite structure, the expansion and contraction of crystal lattices can be realized, further, the gap between the boundaries of the all-inorganic perovskite light absorption layer can be effectively reduced, the formed compact structure layer can effectively improve the transmission efficiency of carriers, the charge recombination rate is reduced, and the photoelectric conversion efficiency of the all-inorganic perovskite solar cell is improved. Meanwhile, the perovskite thin film with large grain size can be obtained by introducing rare earth ions, the surface of the perovskite thin film is uniform and compact, so that the perovskite thin film has more excellent hydrophobicity and is not easy to generate phase change, and the perovskite thin film has higher stability when being applied to a device.
Preferably, the transparent conductive substrate is FTO conductive glass, and the electron transport layer is C-TiO2Film and m-TiO2And the electrode layer is a carbon electrode.
In the application, the all-inorganic perovskite solar cell belongs to a mesoporous structure solar cell. Spin coating a dense layer (C-TiO) on a conductive oxide of transparent conductive glass (FTO)2) Then spin-coating the oxide (m-TiO) with mesoporous structure attached with the all-inorganic perovskite film2) A framework material, and finally depositing a hole transport layer on the surface of the framework material. In the structure of the n-i-p type mesoporous PSCs, the oxide of the mesoporous structure can play a role in transmitting electrons and is also a framework material, so that the electron extraction and transmission efficiency is improved.
The application also provides a preparation method of the all-inorganic perovskite solar cell, which comprises the steps of spin-coating a lead precursor solution containing rare earth ions on a transparent conductive substrate-electron transport layer substrate, soaking the substrate in a cesium precursor solution, annealing, coating an electrode layer, and drying to obtain the all-inorganic perovskite solar cell.
In the application, the spin coating-soaking method is simple to operate, the prepared all-inorganic perovskite solar cell is high in film coverage rate, the number of holes in the surface of the film is small, the roughness is small, and the film coverage rate can reach nearly 100%. In addition, the growth speed of the crystal can be effectively controlled by adopting a spin coating-soaking method, so that large-size crystal grains and a high-quality perovskite light absorption layer are obtained, and the prepared all-inorganic perovskite structure layer is more compact, so that the photoelectric conversion efficiency and the stability of the all-inorganic perovskite solar cell are improved.
Preferably, the electrode layer is a carbon electrode.
Preferably, the lead precursor solution containing rare earth ions is prepared by heating and dissolving a lead precursor material and a nitrate solution containing rare earth ions in an organic solvent;
the rare earth ion is Yb3+、Er3+、Tm3+、Ho3+、Eu3+Or Dy3+；
The lead precursor material is PbBr2；
The concentration of the rare earth ions in the lead precursor solution is 0-10 mol%.
Preferably, the organic solvent is DMF, and the heating and dissolving temperature is 80-100 ℃.
Preferably, after the lead precursor solution containing rare earth ions is spin-coated on the transparent conductive substrate-electron transport layer substrate, before the lead precursor solution is soaked in the cesium precursor solution, a drying step is further performed to remove the organic solvent. The drying temperature is 80-100 ℃, and the drying time is 1-2 h.
Preferably, the solute of the cesium precursor solution is CsI, the solvent is methanol, and the content of the solute is 10-15 mg/mL.
Preferably, the soaking time is 10-20 min;
the annealing temperature is 300-350 ℃, and the annealing time is 10-20 min;
the drying temperature is 110-130 ℃, and the drying time is 10-20 min.
Preferably, the transparent conductive substrate-electron transport layer substrate is made of C-TiO2Coating the film on FTO conductive glass by spin coating, sintering, and spin coating m-TiO2And (3) preparing the film after sintering.
Preferably, the rotation speed of the spin coating is 3000-5000 rpm/min, and the time is 10-30 s;
the sintering temperature is 450-500 ℃, and the sintering time is 30-60 min.
Preferably, the preparation method of the FTO conductive glass comprises the following steps:
and etching the FTO glass by using Zn powder and HCl (2.0mol/L), and sequentially carrying out ultrasonic cleaning for multiple times by using deionized water, acetone and ethanol to obtain the FTO conductive glass.
Preferably, the C-TiO2The film is obtained by spin coating a mixed solution of hydrochloric acid, isopropyl titanate and ethanol;
the m-TiO2The film is prepared by dissolving 18NR-T in m-TiO2Spin coating in ethanol solution.
To sum up, the application provides an all inorganic perovskite solar cell, from sensitive surface one side, includes transparent conductive substrate, electron transport layer, the passive all inorganic perovskite light absorption layer and the electrode layer of rare earth ion in proper order. According to the all-inorganic perovskite solar cell, the size of crystal grains is increased by introducing rare earth ions, gaps among crystal boundaries are reduced, a compact perovskite thin film is formed, the transmission efficiency of current carriers is effectively improved, the service life of the current carriers is prolonged, the charge recombination rate in the all-inorganic perovskite thin film is reduced, the energy loss in charge carrier transfer is minimized, and therefore the photoelectric conversion efficiency of the all-inorganic perovskite solar cell is improved; meanwhile, the formed perovskite thin film has excellent hydrophobicity, is not easy to generate phase change, and has higher stability when being applied to a device. The all-inorganic perovskite solar cell prepared by the preparation method has high film coverage rate, the all-inorganic perovskite structure layer is tighter, and the photoelectric conversion efficiency and stability of the all-inorganic perovskite solar cell are improved.
Drawings
In order to more clearly illustrate the embodiments of the present application or the technical solutions in the prior art, the drawings needed to be used in the description of the embodiments or the prior art will be briefly introduced below, and it is obvious that the drawings in the following description are only some embodiments of the present application, and it is obvious for those skilled in the art that other drawings can be obtained according to the drawings without inventive exercise.
Fig. 1 is a schematic structural view of an all-inorganic perovskite solar cell of example 1 of the present application;
FIG. 2 is a J-V plot of an all inorganic perovskite solar cell of example 1 of the present application;
FIG. 3 is a J-V plot of an all inorganic perovskite solar cell of example 2 of the present application;
FIG. 4 is a J-V plot of an all inorganic perovskite solar cell of comparative example 1 of the present application;
illustration of the drawings: 1. FTO conductive glass; 2. C-TiO2A film; 3. m-TiO2 film; 4. an all-inorganic perovskite light-absorbing layer; 5. a carbon electrode; 6. RE3+。
Detailed Description
In order to make the objects, features and advantages of the present application more obvious and understandable, the technical solutions in the embodiments of the present application will be clearly and completely described below with reference to the drawings in the embodiments of the present application, and it is apparent that the embodiments described below are only a part of the embodiments of the present application, and not all of the embodiments. All other embodiments, which can be derived by a person skilled in the art from the embodiments given herein without making any creative effort, shall fall within the protection scope of the present application.
Example 1
Example Yb of the present application3+The structure of the passivated all-inorganic perovskite solar cell is shown in fig. 1, and the specific preparation method is as follows:
(1) FTO conductive glass: etching the FTO glass by using Zn powder and HCl (2.0mol/L), then sequentially carrying out ultrasonic cleaning for multiple times by using deionized water, acetone and ethanol, wherein each ultrasonic cleaning is carried out for 15min, and finally, putting the FTO glass into an oven to be dried at 100 ℃ to eliminate stress, so that the FTO conductive glass with a clean surface can be obtained;
(2)FTO/C-TiO2substrate: preparation of C-TiO by mixing 70. mu.l of 2mol/L hydrochloric acid, 730ul of isopropyl titanate and 10ml of ethanol2The precursor solution is spin-coated on a transparent conductive substrate, and is placed on a spin-coating machine filled with nitrogen in a glove box, and a mechanical pump is used for pumping and sucking the sheet. The set rotation speed was 4000rpm for 20 s. Then standing on a hot bench at 150 ℃ for 10min, and then calcining in a muffle furnace at 500 ℃ for 60min to obtain FTO/C-TiO2A substrate;
(3)FTO/C-TiO2/m-TiO2substrate: dissolving 18NRT into m-TiO2In 10 wt% of an alcohol solution, spin-coated on FTO/C-TiO2The substrate was placed on a spin coater in a nitrogen-filled glove box and the wafer was sucked by a mechanical pump. The set rotation speed was 4000rpm for 20 s. Then standing on a hot bench at 120 ℃ for 10min, and then calcining in a muffle furnace at 450 ℃ for 30min to prepare FTO/C-TiO2/m-TiO2A substrate;
(4) precursor solution: 0.367g of PbBr was weighed2Adding into 1ml DMF solution, adding 5 mol% ytterbium nitrate, heating at 90 deg.C for 1 hr until completely dissolving to obtain PbBr of ytterbium nitrate2And (3) precursor solution. Preparing a methanol solution of 15mg/mL CsI, heating and stirring at 50 ℃, and dissolving to obtain a precursor solution of the CsI;
(5)FTO/C-TiO2/m-TiO2/RE:PbBr2layer (b): PbBr of ytterbium nitrate2The precursor solution is coated on FTO/C-TiO by spinning2/m-TiO2The substrate was placed on a spin coater in a nitrogen-filled glove box and the wafer was sucked by a mechanical pump. The set rotation speed was 2000rpm for 30 s. Then, the mixture was allowed to stand on a hot stage at 90 ℃ for 60 minutes and then immersed in a CsI methanol solution for 10 minutes. Thoroughly washing with isopropanol, annealing at 350 deg.C for 10min in muffle furnace to obtain FTO/C-TiO2/m-TiO2/RE:PbBr2A layer;
(6) all-inorganic perovskite solar cells: in FTO/C-TiO2/m-TiO2/RE:PbBr2And coating a layer of carbon slurry on the surface of the layer, and drying at 120 ℃ for 20min to obtain the all-inorganic perovskite solar cell.
And detecting the photovoltaic characteristics of the prepared all-inorganic perovskite solar cell by using a Keithley tester, and testing the I-V curve of the all-inorganic perovskite solar cell. Wherein Yb3+Doping ofThe performance of the all-inorganic perovskite solar cell is illustrated in fig. 2 at a concentration of 5 mol%: the open circuit voltage is: 1.18V; the short-circuit current of the battery is: 12.16mA/cm2The fill factor is: 43%, photoelectric conversion efficiency is: 6.31 percent.
Example 2
The preparation method of the all-inorganic perovskite solar cell in the embodiment of the application is the same as that in the embodiment 1, and the difference is only that in the step (4), 0.367g of PbBr is weighed2Adding into 1ml DMF solution, adding 10 mol% ytterbium nitrate, heating at 90 deg.C for 1 hr until completely dissolving to obtain PbBr of ytterbium nitrate2The precursor solution of (1).
And detecting the photovoltaic characteristics of the prepared all-inorganic perovskite solar cell by using a Keithley tester, and testing the I-V curve of the all-inorganic perovskite solar cell. Wherein Yb3+The doping concentration of (a) is 10 mol%, and the performance of the all-inorganic perovskite solar cell is illustrated in fig. 3: open circuit voltage: 1.21V; short-circuit current of battery: 11.25mA/cm2The fill factor: 44%, photoelectric conversion efficiency: 6.05 percent.
Comparative example 1
The preparation method of the all-inorganic perovskite solar cell in the embodiment of the application is the same as that in the embodiment 1, and the difference is only that in the step (4), 0.367g of PbBr is weighed2Adding into 1ml DMF solution, heating at 90 deg.C for 1h until completely dissolving to obtain PbBr2The precursor solution of (1). The PbBr obtained in step (5) is utilized2Preparing FTO/C-TiO by precursor solution2/m-TiO2/PbBr2And (4) preparing the layer in the step (6) to obtain the all-inorganic perovskite solar cell without the rare earth ions.
And detecting the photovoltaic characteristics of the prepared all-inorganic perovskite solar cell by using a Keithley tester, and testing the I-V curve of the all-inorganic perovskite solar cell. Wherein Yb3+The doping concentration of (a) is 10 mol%, and the performance of the all-inorganic perovskite solar cell is illustrated in fig. 4: open circuit voltage: 1.24V; short-circuit current of battery: 9.44mA/cm2And the fill factor: 44%, photoelectric conversion efficiency: 5.17 percent.
In summary, the introduction of a suitable amount of rare earth ions into the all-inorganic perovskite light-absorbing layer increases the cell efficiency of the solar cell. The rare earth ions increase the grain size of the all-inorganic perovskite crystal, prolong the service life of a current carrier, reduce charge recombination in the perovskite thin film and further improve the photoelectric conversion efficiency and stability of the all-inorganic perovskite solar cell. Therefore, the rare earth ions are reasonably utilized to prepare the all-inorganic perovskite light absorption layer, and the method has great significance for improving the photoelectric conversion efficiency of the perovskite solar cell.
The above embodiments are only used for illustrating the technical solutions of the present application, and not for limiting the same; although the present application has been described in detail with reference to the foregoing embodiments, it should be understood by those of ordinary skill in the art that: the technical solutions described in the foregoing embodiments may still be modified, or some technical features may be equivalently replaced; and such modifications or substitutions do not depart from the spirit and scope of the corresponding technical solutions in the embodiments of the present application.
Claims (10)
1. The all-inorganic perovskite solar cell is characterized by sequentially comprising a transparent conductive substrate, an electron transmission layer, an all-inorganic perovskite light absorption layer passivated by rare earth ions and an electrode layer from one side of a light receiving surface.
2. The all inorganic perovskite solar cell of claim 1, wherein the rare earth ion is Yb3+、Er3+、Tm3+、Ho3+、Eu3+Or Dy3+；
The raw material of the all-inorganic perovskite is CsPbIBr2；
The concentration of the rare earth ions in the all-inorganic perovskite is 0-10 mol%.
3. The all-inorganic perovskite solar cell according to claim 1, wherein the transparent conductive substrate is FTO conductive glass and the electron transport layer is C-TiO2Film and m-TiO2And the electrode layer is a carbon electrode.
4. The preparation method of the all-inorganic perovskite solar cell is characterized by comprising the steps of spin-coating a lead precursor solution containing rare earth ions on a transparent conductive substrate-electron transport layer substrate, soaking the substrate in a cesium precursor solution, annealing, coating an electrode layer and drying to obtain the all-inorganic perovskite solar cell.
5. The preparation method according to claim 4, wherein the lead precursor solution containing rare earth ions is prepared by heating and dissolving a lead precursor material and a nitrate solution containing rare earth ions in an organic solvent;
the rare earth ion is Yb3+、Er3+、Tm3+、Ho3+、Eu3+Or Dy3+；
The lead precursor material is PbBr2；
The concentration of the rare earth ions in the lead precursor solution is 0-10 mol%.
6. The preparation method according to claim 5, wherein the cesium precursor solution has a solute CsI, a solvent methanol, and a solute content of 10-15 mg/mL.
7. The preparation method according to claim 5, wherein the soaking time is 10-20 min;
the annealing temperature is 300-350 ℃, and the annealing time is 10-20 min;
the drying temperature is 110-130 ℃, and the drying time is 10-20 min.
8. The method according to claim 5, wherein the transparent conductive substrate-electron transport layer substrate is made of C-TiO2Coating the film on FTO conductive glass by spin coating, sintering, and spin coating m-TiO2And (3) preparing the film after sintering.
9. The preparation method according to claim 8, wherein the spin coating is performed at a rotation speed of 3000-5000 rpm/min for 10-30 s;
the sintering temperature is 450-500 ℃, and the sintering time is 30-60 min.
10. The method according to claim 8, wherein the C-TiO is2The film is obtained by spin coating a mixed solution of hydrochloric acid, isopropyl titanate and ethanol;
the m-TiO2The film is prepared by dissolving 18NR-T in m-TiO2Spin coating in ethanol solution.
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