CN111864082A - Positive structure perovskite solar cell adopting doped nickel oxide as hole transport layer and preparation method thereof - Google Patents
Positive structure perovskite solar cell adopting doped nickel oxide as hole transport layer and preparation method thereof Download PDFInfo
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- CN111864082A CN111864082A CN202010527776.4A CN202010527776A CN111864082A CN 111864082 A CN111864082 A CN 111864082A CN 202010527776 A CN202010527776 A CN 202010527776A CN 111864082 A CN111864082 A CN 111864082A
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Abstract
The invention discloses an upright perovskite solar cell with a doped nickel oxide as a hole transport layer and a preparation method thereof. The solar cell is structurally characterized in that: on the FTO, the area of part is completely blank, and the rest part is coated with an electron transport layer, a perovskite layer, a hole transport layer and a carbon layer in sequence; the hole transport layer is doped nickel oxide. The invention takes nickel-aluminum hydrotalcite with a nano structure as a precursor, obtains aluminum-doped nickel oxide through annealing pyrolysis, and can absorb water and CO in the air due to the structural memory effect of the hydrotalcite2The hole transport layer can improve the photoelectric conversion efficiency and stability of the cellAnd (5) performing qualitative determination. The perovskite solar cell with the positive structure and the doped nickel oxide as the hole transport layer is simple to prepare, convenient and fast to operate, capable of simplifying the requirements on device packaging, capable of reducing the manufacturing cost and good in commercial application prospect.
Description
Technical Field
The invention belongs to the technical field of new energy photoelectric materials, and particularly relates to an upright perovskite solar cell with a doped nickel oxide as a hole transport layer and a preparation method thereof.
Background
Developments in the field of solar cells are divided into conventional cells and new concept solar cells. The conventional solar cell is mainly a silicon solar cell, because silicon is a semiconductor material, and can generate a certain photovoltaic effect after absorbing sunlight. Conventional solar cells are cells based on silicon wafers, monocrystalline and polycrystalline silicon, and GaAs as the main materials. However, such a battery is still expensive, and therefore, development of a solar battery using a new material is becoming a trend. The solar cell of the new concept is mainly based on a thin film, such as a dye-sensitized cell and a perovskite solar cell. Dye-sensitized cells dye-sensitized solar cells (DSSCs) are mainly composed of a working electrode, a redox electrolyte and a counter electrode. The photo-anode is a working electrode and is nc-TiO sensitized by dye2A porous membrane; the titanium dioxide photo-anode is the core part of the whole DSSCs, and plays a role in not only loading dye, but also receiving electrons and transmitting electrons in the battery. However, the energy conversion efficiency of the dye-sensitized cell is not very high. From a 9.7% efficiency battery reported in 2012, perovskite batteries (PSCs) have made dramatic progress over several years of research, with excellent reproducibility, with Power Conversion Efficiencies (PCEs) as high as 21.6%, and PCEs of 21.02% certified under the conditions of standard AM 1.5G. PSC has good development prospect and is expected to be put into human life in the future.
In the research of perovskite solar cells, nickel oxide can be applied to a hole transport layer, but the nickel oxide is used as the hole transport layer and is the perovskite solar cell adopting an inverted structure, because the sintering temperature of the nickel oxide is far higher than the bearing temperature of a perovskite layer, the nickel oxide cannot be fully diffused into an organic solvent without a nano structure in the traditional nickel oxide and is prepared by spin coating, so that the nickel oxide needs to be generated in situ and then is made into the inverted structure, namely, the nickel oxide film is firstly generated in situ by high-temperature sintering and then is prepared into the perovskite film. The invention adopts Layered Double Hydroxides (LDHs), also called hydrotalcite, which is a novel inorganic functional nano material with a layered structure and is composed of a positively charged layerPlate metal cations and interlayer anions. The general chemical formula can be used as [ M ]II 1-xMIII x(OH)2]z+(An-)z/n·yH2O, wherein MIIAnd MIIIDivalent and trivalent metals, respectively; a. then-It is an interlayer anion. The material has the characteristics of simple and convenient synthesis, relatively large specific surface volume and high anion exchange capacity, and the doped ions of the doped oxide prepared by taking LDHs as precursors are highly uniformly distributed.
Disclosure of Invention
The invention aims to provide an upright perovskite solar cell with a doped nickel oxide as a hole transport layer and a preparation method thereof. The invention takes nickel-aluminum hydrotalcite with a nano structure as a precursor, obtains aluminum-doped nickel oxide through annealing pyrolysis, and can absorb water and CO in the air due to the structural memory effect of the hydrotalcite 2The hole transport layer can be used as a hole transport layer, so that the photoelectric conversion efficiency and stability of the cell can be improved.
The structure of the perovskite solar cell with the positive structure and the doped nickel oxide as the hole transport layer is as follows: on the FTO, the area of part is completely blank, and the rest part is coated with an electron transport layer, a perovskite layer, a hole transport layer and a carbon layer in sequence; the hole transport layer is doped nickel oxide.
The electron transport layer is TiO2A layer or a ZnO layer.
The preparation method of the hole transport layer comprises the following steps: preparing nickel-aluminum hydrotalcite, then placing the nickel-aluminum hydrotalcite in a muffle furnace, calcining for 1-2h at the temperature of 300-400 ℃, ultrasonically dispersing the obtained doped nickel oxide by using an organic solvent, then coating the organic solvent on a perovskite layer, and heating to remove the organic solvent to obtain a hole transport layer.
The perovskite solar cell with the positive structure and the doped nickel oxide as the hole transport layer is simple to prepare, convenient and fast to operate, capable of simplifying the requirements on device packaging, capable of reducing the manufacturing cost and good in commercial application prospect.
Drawings
FIG. 1 is an XRD pattern of the nickel-aluminum hydrotalcites obtained in examples 1 to 4 of the present invention, wherein the nickel-aluminum ratios are 2:1, 3:1, 4:1, and 5:1, respectively.
FIG. 2 is an XRD pattern of Al-doped nickel oxide with Ni/Al ratios of 2:1, 3:1, 4:1, 5:1 obtained in examples 1-4 of the present invention.
FIG. 3 is an SEM image of nickel aluminum hydrotalcite obtained in example 4 with a nickel to aluminum ratio of 5: 1.
FIG. 4 is a schematic diagram of the perovskite solar cell structure of the present invention.
Fig. 5 is a graph of the photoelectric conversion efficiency of the solar cells obtained in examples 3 and 4.
Fig. 6 is a graph comparing the photoelectric conversion efficiency with time of the solar cells prepared in examples 3 and 4 and comparative example 1.
Detailed Description
The invention is further illustrated by the following specific examples.
Example 1
1. Compact TiO 22Layer preparation: ultrasonically cleaning an FTO (fluorine-doped tin oxide) with the length of 2cm and the width of 1.5cm in deionized water, acetone and absolute ethyl alcohol for 30 minutes respectively, cleaning the FTO by using a cotton swab, and pasting an adhesive tape on one side; preparing a mixed solution of 35 mu L of 2mol/L HCl and 2.53ml of EtOH, and then slowly dripping 369 mu L of titanic acid isopropanol to prevent the titanic acid isopropanol from hydrolyzing to obtain a transparent and clear solution; then 100 mul of the clear solution was spin coated on FTO for 30s, buffer for 3s, spin speed 2000 rpm; after the spin coating is finished, taking out the FTO, heating at 125 ℃ for 5min, and taking out to store in a culture dish;
2. Mesoporous TiO 22Layer preparation: TiO 22Mixing the mesoporous material and ethanol in a mass ratio of 1:3.5 to form slurry, performing ultrasonic treatment for 20min to disperse the slurry, stirring the slurry by using a magnetic stirrer, taking out 100 mu l of the slurry, and spin-coating the slurry on the FTO in the step 1 for 30s, the buffering time for 6s and the rotation speed for 5000 rpm; heating FTO to 100 deg.C, and maintaining for 5 min; then placing the FTO into a muffle furnace, programming to raise the temperature to 500 ℃, keeping the temperature at 500 ℃, heating for 30min, and cooling to room temperature;
3. preparation of perovskite layer: weighing 1.1g of PbI2Dissolved in 2mL of DMF, addStirring at 100 deg.C to form clear yellow liquid; weighing 400mg of iodomethylamine, and dissolving in 32mL of anhydrous isopropanol and 8mL of cyclohexane to form a clear colorless transparent solution; will PbI2Spin-coating the solution on the surface of the FTO containing the electron transport layer in the step 2 for 30s, buffering for 3s and rotating at 2000rpm, soaking in iodomethylamine solution for 15 min after the spin-coating is finished, and finally heating the FTO at 100 ℃ to volatilize the solvent;
4. preparing hydrotalcite by a urea method: weighing 5.82g Ni (NO)3)2·6H2O and 3.75g Al (NO)3)3·9H2Dissolving O in 40mL of deionized water to prepare a mixed salt solution, weighing 3.6g of urea, dissolving in 40mL of deionized water to prepare an alkali solution, adding the two solutions into a reaction kettle at the same time, reacting for 24 hours at 110 ℃, centrifuging for three times by using deoxygenated deionized water, dispersing and stirring for three times by using 200mL of acetone, and finally drying for 24 hours at 60 ℃ in a vacuum drying box to obtain nickel-aluminum hydrotalcite, wherein the label of the nickel-aluminum hydrotalcite is LDHs2: 1;
5. Putting the dried nickel-aluminum hydrotalcite into a mortar for full grinding, putting the obtained solid powder into a crucible, putting the crucible into a muffle furnace, and heating for 10 ℃ for min-1Heating to 300 ℃, keeping the temperature at 300 ℃, calcining for 2h, and naturally cooling to room temperature to obtain aluminum-doped nickel oxide, wherein the mark is MMO2: 1; weighing 0.01g of aluminum-doped nickel oxide, adding 10mL of chlorobenzene, and performing ultrasonic treatment for 24 hours to prepare a colloidal solution;
6. preparing a hole transport layer: sucking 100ul of the colloidal solution obtained in the step 4 by using a suction pipe, dripping the colloidal solution on the perovskite layer prepared in the step 5, spin-coating the colloidal solution for 30s at 3000r/min by using a spin coating instrument, placing the spin-coated FTO sheet in a muffle furnace, heating the FTO sheet for 10 minutes at 100 ℃, and then annealing the FTO sheet at high temperature to remove the organic solvent;
7. and (4) coating carbon slurry on the FTO in the step (6), after the carbon slurry is coated, putting the FTO into a drying oven at the temperature of 100 ℃ for drying for 15min, taking out the FTO to obtain the solar cell, and preparing for testing the performance.
In the preparation steps, the FTO is pasted by using an adhesive tape before coating, so that a part of area is blank, no substance is coated, the pasting position of the adhesive tape is the same or exceeds the original pasting area each time, but the pasting area cannot be smaller than the original pasting area. The tape can be removed each time it is heated or calcined.
The above products were characterized: for example, the XRD pattern of the nickel aluminum hydrotalcite obtained in step 4 is LDHs2:1 in figure 1, and the XRD pattern of the aluminum doped nickel oxide obtained in step 5 is MMO2:1 in figure 2.
Example 2
1. The same as example 1;
2. the same as example 1;
3. the same as example 1;
4. preparing hydrotalcite by a urea method: 8.73g of Ni (NO) are weighed out3)2·6H2O and 3.75g Al (NO)3)3·9H2Dissolving O in 40mL of deionized water to prepare a mixed salt solution, weighing 3.6g of urea, dissolving in 40mL of deionized water to prepare an alkali solution, adding the two solutions into a reaction kettle at the same time, reacting for 24 hours at 110 ℃, centrifuging for three times by using deoxygenated deionized water, dispersing and stirring for three times by using 200mL of acetone, and finally drying for 24 hours at 60 ℃ in a vacuum drying box to obtain nickel-aluminum hydrotalcite, wherein the label of the nickel-aluminum hydrotalcite is LDHs3: 1;
5. the same as example 1; preparing aluminum-doped nickel oxide, wherein the mark is MMO3: 1;
6. the same as example 1;
7. the same as in example 1.
The product was characterized: for example, the XRD pattern of the nickel aluminum hydrotalcite obtained in step 4 is LDHs3:1 in figure 1, and the XRD pattern of the aluminum doped nickel oxide obtained in step 5 is MMO3:1 in figure 2.
Example 3
1. The same as example 1;
2. the same as example 1;
3. the same as example 1;
4. preparing hydrotalcite by a urea method: 11.64g of Ni (NO) were weighed3)2·6H2O and 3.75g Al (NO)3)3·9H2Dissolving O in 40mL deionized water to obtain mixed salt solution, dissolving 3.6g urea in 40mL deionized water to obtain alkali solution, adding the two solutions into a reaction kettle at the same time, reacting at 110 deg.C for 24 hr, and removing Centrifuging deionized water containing oxygen for three times, dispersing and stirring with 200mL acetone for three times, and finally drying in a vacuum drying oven at 60 ℃ for 24 hours to obtain nickel-aluminum hydrotalcite, wherein the label of the nickel-aluminum hydrotalcite is LDHs4: 1;
5. the same as example 1; preparing aluminum-doped nickel oxide, wherein the mark is MMO4: 1;
6. the same as example 1;
7. the same as in example 1.
The product was characterized: for example, the XRD pattern of the nickel aluminum hydrotalcite obtained in step 4 is LDHs4:1 in figure 1, and the XRD pattern of the aluminum doped nickel oxide obtained in step 5 is MMO4:1 in figure 2.
Example 4
1. The same as example 1;
2. the same as example 1;
3. the same as example 1;
4. preparing hydrotalcite by a urea method: 14.55g of Ni (NO) are weighed3)2·6H2O and 3.75g Al (NO)3)3·9H2Dissolving O in 40mL of deionized water to prepare a mixed salt solution, weighing 3.6g of urea, dissolving in 40mL of deionized water to prepare an alkali solution, adding the two solutions into a reaction kettle at the same time, reacting for 24 hours at 110 ℃, centrifuging for three times by using deoxygenated deionized water, dispersing and stirring for three times by using 200mL of acetone, and finally drying for 24 hours at 60 ℃ in a vacuum drying box to obtain nickel-aluminum hydrotalcite, wherein the label of the nickel-aluminum hydrotalcite is LDHs5: 1;
5. the same as example 1; preparing aluminum-doped nickel oxide, wherein the mark is MMO5: 1;
6. The same as example 1;
7. the same as in example 1.
The product was characterized: for example, the XRD pattern of the nickel aluminum hydrotalcite obtained in step 4 is LDHs5:1 in figure 1, and the XRD pattern of the aluminum doped nickel oxide obtained in step 5 is MMO5:1 in figure 2.
Comparative example 1
1. The same as example 1;
2. the same as example 1;
3. the same as example 1;
4. and (4) coating carbon slurry on the FTO in the step (3), after the carbon slurry is coated, putting the FTO into a drying oven at the temperature of 100 ℃ for drying for 15min, taking out the FTO to obtain the solar cell without the hole transport layer doped with the nickel oxide, and preparing for testing the performance.
Claims (3)
1. The positive structure perovskite solar cell adopting the doped nickel oxide as the hole transport layer is characterized in that the structure of the solar cell is as follows: on the FTO, the area of part is completely blank, and the rest part is coated with an electron transport layer, a perovskite layer, a hole transport layer and a carbon layer in sequence; the hole transport layer is doped nickel oxide.
2. The perovskite solar cell with an orthosteric structure and a doped nickel oxide hole transport layer as claimed in claim 1, wherein the electron transport layer is TiO2A layer or a ZnO layer.
3. The perovskite solar cell with the positive structure and the doped nickel oxide as the hole transport layer according to claim 1, wherein the hole transport layer is prepared by the following steps: preparing nickel-aluminum hydrotalcite, then placing the nickel-aluminum hydrotalcite in a muffle furnace, calcining for 1-2h at the temperature of 300-400 ℃, ultrasonically dispersing the obtained doped nickel oxide by using an organic solvent, then coating the organic solvent on a perovskite layer, and heating to remove the organic solvent to obtain a hole transport layer.
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| Publication number | Priority date | Publication date | Assignee | Title |
|---|---|---|---|---|
| CN113206198A (en) * | 2021-04-19 | 2021-08-03 | 武汉大学 | Preparation method of lanthanum nickelate nanoparticle hole transport layer, trans-perovskite solar cell and preparation method of trans-perovskite solar cell |
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| CN104556728A (en) * | 2015-01-19 | 2015-04-29 | 北京化工大学 | Method for preparing aluminum-doped nickel oxide electrochromic film by virtue of hydrotalcite precursor pyrolysis |
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| CN113206198A (en) * | 2021-04-19 | 2021-08-03 | 武汉大学 | Preparation method of lanthanum nickelate nanoparticle hole transport layer, trans-perovskite solar cell and preparation method of trans-perovskite solar cell |
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