Perovskite solar cell-supercapacitor integrated device and preparation method thereof

Abstract

The invention relates to the technical field of photoelectric energy conversion and electric energy storage, in particular to a perovskite solar cell-supercapacitor integrated device and a preparation method thereof. And preparing the perovskite solar cell-supercapacitor integrated device by adopting a roll-to-roll process. According to the invention, the reel-to-reel process is selected as a process technical route, and the preparation of the perovskite solar cell and the supercapacitor can be completed only through the reel-to-reel process. The method has the advantages of low cost, simple process, high flexibility and the like.

Description

Technical Field

[0001] The present invention relates to the technical field of photoelectric energy conversion and electric energy storage, and in particular to a perovskite solar cell-supercapacitor integrated device and a preparation method thereof. Background Art

[0002] Light energy is an inexpensive, readily available, and environmentally friendly energy resource. Based on the photoelectric conversion effect, people have developed photovoltaic technology - a technical means to directly and efficiently convert light energy into electrical energy. In addition to being a component of the grid power supply, miniaturized photovoltaic cells can also be used as a power source for low-power electronic devices. For low-power electronic device applications, batteries usually need to be replaced frequently during their use cycle, which brings many inconveniences. If only solar cells are used, the volatility of photovoltaic power generation makes it impossible to use the equipment continuously and stably. If a combination of solar cells and lithium batteries is used, due to the short life of lithium batteries, stable self-power supply throughout the week cannot be achieved. Therefore, it is necessary to design a photovoltaic-energy storage integrated power supply with a long life.

[0003] Among photovoltaic devices, perovskite solar cells have become a popular technology due to their flexible manufacturing process and low cost. In the solar power generation sector, the efficiency of perovskite cell modules has exceeded 25%, and in indoor photovoltaic power generation, the efficiency has surpassed 35%. While photovoltaic cells can directly and simply convert light energy into electricity, they currently cannot address the fluctuations in power generation caused by light source fluctuations, which is unacceptable for electricity demand. Among energy storage devices, lithium-ion batteries and supercapacitors have been widely researched and applied as DC power storage methods. Supercapacitors, with their advantages of long charge and discharge life and fast charge and discharge rates, play a vital role in many practical applications. Notably, planar doped graphene supercapacitors using a gel solid electrolyte have demonstrated a charge and discharge life of over 100,000 cycles.

[0004] At present, when producing integrated devices of perovskite solar cells and supercapacitors, the process compatibility between battery manufacturing and capacitor manufacturing is poor, and there is a lack of simple and universal process preparation methods.

[0005] Therefore, the existing technology still needs to be improved and developed. Summary of the Invention

[0006] In view of the above-mentioned deficiencies in the prior art, the present invention provides a perovskite solar cell-supercapacitor integrated device and a preparation method thereof, so as to solve the problem of poor process compatibility between the battery manufacturing and capacitor manufacturing links in the existing production and preparation of perovskite solar cell and supercapacitor integrated devices.

[0007] The technical solutions adopted by the present invention to solve the above technical problems are as follows:

[0008] A first aspect of the present invention provides a method for preparing a perovskite solar cell-supercapacitor integrated device, wherein the perovskite solar cell-supercapacitor integrated device is prepared by a roll-to-roll process.

[0009] Preferably, the steps of preparing the perovskite solar cell-supercapacitor integrated device by a roll-to-roll process are specifically as follows:

[0010] providing a first substrate;

[0011] coating a hole transport solution on the surface of the first substrate using a roll-to-roll process, followed by drying and annealing to obtain a hole transport layer;

[0012] The perovskite solution is coated on the surface of the hole transport layer by a roll-to-roll process, followed by drying and annealing to obtain a perovskite light absorption layer;

[0013] The electron transport solution is coated on the surface of the perovskite light absorption layer by a roll-to-roll process, followed by drying and annealing to obtain an electron transport layer;

[0014] preparing a first metal electrode layer on the electron transport layer to obtain a perovskite solar cell;

[0015] coating a graphene slurry on the surface of the first metal electrode layer using a roll-to-roll process to obtain a first graphene functional layer;

[0016] Providing a second substrate, and preparing a second metal electrode layer on a surface of the second substrate;

[0017] coating the graphene slurry on the surface of the second metal electrode layer using a roll-to-roll process, followed by drying and annealing to obtain a second graphene functional layer;

[0018] coating a gel electrolyte on the surface of the second graphene functional layer using a roll-to-roll process, followed by drying and annealing to obtain a gel electrolyte layer;

[0019] The first graphene functional layer is electrically connected to the gel electrolyte layer, and then the first graphene functional layer and the gel electrolyte layer are pressed together to obtain the perovskite solar cell-supercapacitor integrated device.

[0020] Preferably, in the step of coating the hole transport solution on the surface of the first substrate using a roll-to-roll process, the hole transport solution is one of 2PACz, PTAA, and NiOx, and the parameters of the roll-to-roll process are: the roll-to-roll coating speed is 1-100 mm / s, and the slit width is set to 50-200 μm.

[0021] Preferably, in the step of coating the perovskite solution on the surface of the hole transport layer using a roll-to-roll process, the perovskite solution is FA 1-x Cs x Pb(Br 1-y I y )3 solution, wherein 0≤x≤1, 0≤y≤1, and the parameters of the roll-to-roll process are: the roll-to-roll coating speed is 1-100 mm / s, and the slit width is set to 50-200 μm.

[0022] Preferably, in the step of coating the electron transport solution on the surface of the perovskite light absorption layer using a roll-to-roll process, the electron transport solution is one of PFBO-C12, PCBM, and SnO2 solutions, and the parameters of the roll-to-roll process are: the roll-to-roll coating speed is 1-100 mm / s, and the slit width is set to 50-300 μm.

[0023] Preferably, in the step of coating the graphene slurry on the surface of the first metal electrode layer using a roll-to-roll process, the parameters of the roll-to-roll process are: a roll-to-roll coating speed of 1-100 mm / s, and a slit width of 100 μm-2 mm.

[0024] Preferably, in the step of coating the graphene slurry on the surface of the second metal electrode layer using a roll-to-roll process, the parameters of the roll-to-roll process are: a roll-to-roll coating speed of 1-100 mm / s, and a slit width of 100 μm-2 mm.

[0025] Preferably, in the step of coating the gel electrolyte on the surface of the second graphene functional layer using a roll-to-roll process, the gel electrolyte is one of polyvinyl alcohol-sulfuric acid gel, polyethylene oxide-lithium bistrifluoromethanesulfonimide, and polyacrylonitrile-propylene carbonate-ionic liquid, and the parameters of the roll-to-roll process are: the roll-to-roll coating speed is 1-50 mm / s, and the slit width is set to 100 μm-2 mm.

[0026] Preferably, before the step of preparing the first metal electrode layer on the electron transport layer, the method further comprises the step of preparing a barrier layer on the surface of the electron transport layer, wherein the barrier layer material is SnO2.

[0027] In a second aspect of the present invention, a perovskite solar cell-supercapacitor integrated device is provided, wherein the perovskite solar cell-supercapacitor integrated device is prepared by the above-mentioned preparation method.

[0028] Beneficial effects:

[0029] The present invention discloses a perovskite solar cell-supercapacitor integrated device and its preparation method. The present invention uses a roll-to-roll process as a technological route, and can complete the preparation of both the perovskite solar cell and the supercapacitor using only one roll-to-roll process.

[0030] Specifically, the roll-to-roll (R2R) process for preparing perovskite solar cell-supercapacitor integrated devices has the following significant advantages and principles: Material and process compatibility: The R2R process uses low-temperature deposition (such as sputtering and coating) to prepare the light-absorbing layer of the perovskite solar cell (such as the perovskite light-absorbing layer) and the electrode of the supercapacitor (such as carbon material or conductive polymer), avoiding damage to the flexible substrate caused by high temperature. High efficiency and low cost: The R2R process achieves large-area, high-speed production by continuously winding the substrate, significantly reducing the manufacturing cost per unit area. It is suitable for flexible substrates (such as polymers and metal foils) and suitable for large-scale mass production. The coating, drying, and packaging steps of R2R are completed in an integrated manner to ensure device consistency and avoid the misalignment problem of traditional step-by-step assembly. Advantages of flexible integration: Thin-film solar cells (such as perovskite or CIGS) and supercapacitors can be prepared on flexible substrates. The R2R process ensures that the device is light, thin, and flexible, suitable for wearable devices or curved application scenarios. Energy collaborative management: The integrated design converts light energy into electrical energy in real time through solar cells, and quickly stores / releases it through supercapacitors, solving the problem of intermittent lighting and improving the system's energy utilization efficiency.

[0031] In summary, the R2R process achieves performance optimization and large-scale application of flexible integrated devices through efficient and low-cost continuous production, providing innovative solutions for renewable energy storage. BRIEF DESCRIPTION OF THE DRAWINGS

[0032] Figure 1 Schematic diagram of the structure of the perovskite solar cell-supercapacitor integrated device in a preferred embodiment of the present invention.

[0033] Figure 2 The perovskite solar cell-supercapacitor integrated device prepared in Example 2 of the present invention was subjected to AM1.5G simulated sunlight, and the current-voltage curve of the perovskite solar cell portion was measured.

[0034] Figure 3 The charge-discharge curve of the supercapacitor portion of the perovskite solar cell-supercapacitor integrated device prepared in Example 2 of the present invention was measured under AM1.5G simulated sunlight. Under the test conditions, the charge cut-off voltage was 4V and the discharge current was 40.0mA.

[0035] Figure 4The current-voltage curve of the perovskite solar cell part of the perovskite solar cell-supercapacitor integrated device prepared in Example 2 of the present invention was measured under indoor white LED light. The light source used for the test was a 4000K white light LED lamp with an illumination of 1000 lux and 200 lux.

[0036] Figure 5 The charge-discharge curve of the supercapacitor portion of the perovskite solar cell-supercapacitor integrated device prepared in Example 2 of the present invention was measured under indoor white LED light. The light source used for the test was a 4000K white LED lamp with an illumination of 1000 lux. The test conditions were a charge cutoff voltage of 3 V and a discharge current of 60 μA. DETAILED DESCRIPTION

[0037] The present invention provides a perovskite solar cell-supercapacitor integrated device and a method for preparing the same. To clarify the objectives, technical solutions, and effects of the present invention, the present invention is described in further detail below. It should be understood that the specific embodiments described herein are intended only to illustrate the present invention and are not intended to limit the present invention.

[0038] An embodiment of the present invention provides a method for preparing a perovskite solar cell-supercapacitor integrated device, wherein the perovskite solar cell-supercapacitor integrated device is prepared by a roll-to-roll process.

[0039] This embodiment effectively reduces the manufacturing difficulty and process cost of the integrated perovskite solar cell-supercapacitor device, enabling the fabrication of the primary structures of the perovskite solar cell and supercapacitor using only a roll-to-roll process. The process is simple and highly flexible, adapting to the fabrication of devices of varying sizes and shapes.

[0040] Specifically, the roll-to-roll process uses a combination of roller and slot coating to evenly coat a solution onto a flexible substrate. This method offers a wide range of parameter adjustments and high flexibility. By adjusting process parameters, both perovskite solar cells and supercapacitors can be fabricated using the same method and equipment.

[0041] In some embodiments, the steps of preparing the perovskite solar cell-supercapacitor integrated device using a roll-to-roll process are specifically as follows:

[0042] providing a first substrate;

[0043] coating a hole transport solution on the surface of the first substrate using a roll-to-roll process, followed by drying and annealing to obtain a hole transport layer;

[0044] The perovskite solution is coated on the surface of the hole transport layer by a roll-to-roll process, followed by drying and annealing to obtain a perovskite light absorption layer;

[0045] The electron transport solution is coated on the surface of the perovskite light absorption layer by a roll-to-roll process, followed by drying and annealing to obtain an electron transport layer;

[0046] preparing a first metal electrode layer on the electron transport layer to obtain a perovskite solar cell;

[0047] coating a graphene slurry on the surface of the first metal electrode layer using a roll-to-roll process to obtain a first graphene functional layer;

[0048] Providing a second substrate, and preparing a second metal electrode layer on a surface of the second substrate;

[0049] coating the graphene slurry on the surface of the second metal electrode layer using a roll-to-roll process, followed by drying and annealing to obtain a second graphene functional layer;

[0050] coating a gel electrolyte on the surface of the second graphene functional layer using a roll-to-roll process, followed by drying and annealing to obtain a gel electrolyte layer;

[0051] The first graphene functional layer is electrically connected to the gel electrolyte layer, and then the first graphene functional layer and the gel electrolyte layer are pressed together to obtain the perovskite solar cell-supercapacitor integrated device.

[0052] In some embodiments, before the step of preparing the first metal electrode layer on the electron transport layer, the method further includes the step of preparing a barrier layer on the surface of the electron transport layer, wherein the barrier layer material is SnO2.

[0053] The preparation of the barrier layer includes the following steps: using tetrakis(dimethylamino)tin(IV) as a tin source and deionized water as an oxygen source, using an ALD atomic layer deposition device, and preparing a dense SnO2 layer with a thickness of 7.5 nm on the surface of the electron transport layer at a substrate temperature of 90°C.

[0054] In some embodiments, the graphene in the graphene slurry is modified graphene, which is prepared as follows: iron, cobalt, and nickel nano-oxides are prepared by a hydrothermal method, and loaded between graphene nanosheets to form modified graphene with a double-layer hydrotalcite structure.

[0055] Layered graphene structures have good conductivity but low capacity. The presence of numerous hydroxyl groups on the graphene surface allows for the loading of nanomaterials through hydrogen bonding. This example selects iron-cobalt-nickel oxide nanosheets with high specific capacity as a modifying material and loads them onto the graphene surface, resulting in a modified graphene material with both good conductivity and high specific capacity. The capacitance of supercapacitors using modified graphene materials is significantly improved. Compared to the control group graphene supercapacitor, the specific capacity of the modified graphene capacitor is more than doubled.

[0056] In a second aspect of the present invention, a perovskite solar cell-supercapacitor integrated device is provided, wherein the perovskite solar cell-supercapacitor integrated device is prepared by the above-mentioned preparation method.

[0057] The perovskite solar cell-supercapacitor integrated device provided in this embodiment has a structure as follows Figure 1 As shown, the device structure includes, from bottom to top: a conductive glass layer (first substrate), a hole transport layer, a perovskite light absorption layer, an electron transport layer, a copper metal electrode layer (first metal electrode layer), a first graphene functional layer, a gel electrolyte layer, a second graphene functional layer, and a copper metal electrode layer (second metal electrode layer).

[0058] The role of each layer in the perovskite solar cell-supercapacitor integrated device: transparent conductive glass substrate, hole transport layer, perovskite light absorption layer, electron transport layer, and copper metal electrode layer belong to perovskite solar cells. The copper metal electrode is shared with the supercapacitor. The copper metal electrode layer, graphene functional layer, gel electrolyte layer, graphene functional layer and copper metal electrode layer constitute a supercapacitor. The supercapacitor developed in this embodiment is a double-layer capacitor, so the electrodes at both ends of the capacitor are symmetrical structures. Among them, the copper metal electrode is mainly the substrate layer, which plays the role of connecting the external circuit and supporting the graphene functional layer. The graphene functional layer is mainly a high specific capacity modified graphene material, which plays the role of adsorbing and storing charged ions in the electrolyte. The gel electrolyte plays the role of transporting ions and separating the two electrode layers of the capacitor.

[0059] The operating principle of the perovskite solar cell-supercapacitor integrated device of this embodiment is as follows: in the light state, control switch 1 is closed, and the perovskite solar cell charges the supercapacitor. After the supercapacitor is charged, control switch 1 is opened. In the dark state, control switch 1 is opened to prevent the electrical energy stored in the supercapacitor from flowing back into the perovskite solar cell and discharging. When control switch 2 is closed, the perovskite solar cell-supercapacitor integrated device supplies power to the load electrical appliance; when control switch 2 is opened, the perovskite solar cell-supercapacitor integrated device stops outputting electrical energy.

[0060] The following is a clear and complete description of the technical solutions in the embodiments of the present invention. Obviously, the embodiments described are only some of the embodiments of the present invention, not all of them, and are intended only to illustrate the present invention and in no way limit the present invention. All other embodiments derived by persons of ordinary skill in the art based on the embodiments of the present invention without inventive effort are also within the scope of protection of the present invention.

[0061] Example 1

[0062] A preparation method of a perovskite solar cell-supercapacitor integrated device comprises the following steps:

[0063] Clean the ITO transparent conductive glass substrate (first substrate): soak the ITO in deionized water, acetone, and sewage ethanol and perform ultrasonic cleaning for 15 minutes each. Then, use a nitrogen air gun to blow dry and treat it with ultraviolet ozone for 20 minutes to clean the residual organic matter on the surface and improve the wettability of the substrate.

[0064] Preparation of the hole transport layer: Use deionized water to prepare an aqueous dispersion of nickel oxide nanoparticles (concentration of 7 mg / mL); use isopropyl alcohol to prepare a 2PACz solution (concentration of 0.4 mg / mL), and use a roll-to-roll coating method to sequentially coat the aqueous dispersion of nickel oxide nanoparticles and the 2PACz solution on the surface of the first substrate. The roll-to-roll coating speed is 3 mm / s, and the slit width is set to 100 μm. After roll-to-roll film formation, bake on a hot plate at 100°C for 10 minutes.

[0065] Preparation of perovskite light absorption layer: 1.8 mol / L FA 0.83 Cs 0.17 Pb(Br 0.4 I 0.6 )3's perovskite solution, the solvent is a mixed solvent of DMF and DMSO in a volume ratio of 65:35, the slit width is set to 50μm, the roll-to-roll coating speed is 2mm / s, and the nitrogen air knife pressure is 55psi, and the perovskite solution is coated on the surface of the hole transport layer to form a wet film, which is placed on a 100℃ hot plate and baked for 10 minutes.

[0066] Preparation of the electron transport layer: A 4 mg / mL polymer electron transport layer (PFBO-C12) solution was prepared in chlorobenzene. The slit width was set to 130 μm, the roll-to-roll coating speed was 4.5 mm / s, and the nitrogen air knife pressure was set to 15 psi. The polymer electron transport layer (PFBO-C12) solution was then coated on the surface of the perovskite light absorption layer to form a wet film. The wet film was then placed on a hot plate at 100°C for 10 minutes. The barrier layer was then prepared: a dense SnO2 layer with a thickness of 7.5 nm was deposited using an atomic layer deposition (ALD) system using tetrakis(dimethylamino)tin(IV) as the tin source and deionized water as the oxygen source at a substrate temperature of 90°C.

[0067] Evaporation of copper metal electrode layer (first metal electrode layer): using vacuum thermal evaporation equipment, the pressure in the evaporation chamber is less than 1×10 -4 After Pa hours, 150nm Cu was evaporated, thus completing the preparation process of the perovskite solar cell part.

[0068] Printing the first graphene functional layer: Use a roll-to-roll coating process with a slit width of 100 μm and a roll-to-roll coating speed of 3 mm / s to roll-coat the graphene slurry on the surface of the first metal electrode layer, and then place it in a vacuum oven at 40°C to dry for 1 hour.

[0069] Preparation of the copper metal electrode layer (second metal electrode layer) and the second graphene functional layer on the top of the device: Use a vacuum thermal evaporator to evaporate a metal copper electrode layer with a thickness of 200 nm and a specific shape on the glass surface according to the shape of the mask. Then use a roll-to-roll coating process with a slit width of 100 μm and a roll-to-roll coating speed of 3 mm / s to roll-coat the graphene slurry on the surface of the second metal electrode layer, and then place it in a vacuum oven at 40°C to dry for 1 hour.

[0070] Printing the gel electrolyte layer: A 10wt% polyvinyl alcohol / sulfuric acid electrolyte solution was prepared and deposited on the surface of the second graphene functional layer using a roll-to-roll process with a slit width of 150μm and a roll-to-roll coating speed of 2mm / s. The prepared gel electrolyte layer was then dried in a vacuum oven at 40°C for 24 hours.

[0071] After connecting the first graphene functional layer and the gel electrolyte layer with a wire, the two films with aligned patterns were pressed together using a pressure of 0.2 MPa, and the gap between the glass substrates was sealed with a two-component epoxy encapsulation glue. After standing for 24 hours for the glue to cure, the preparation of the perovskite solar cell-supercapacitor integrated device was completed.

[0072] Example 2

[0073] Preparation of a perovskite solar cell-supercapacitor integrated device. The method of this embodiment is basically the same as that of Example 1, with the only difference being:

[0074] The graphene in the graphene slurry is modified graphene, and the preparation of the modified graphene is as follows: iron, cobalt and nickel nano-oxides are prepared by a hydrothermal method, and loaded between graphene nanosheets to form modified graphene with a double-layer hydrotalcite structure.

[0075] The perovskite solar cell-supercapacitor integrated device prepared in Example 2 consists of four integrated devices connected in series, with an effective area of ​​10.4 square centimeters. The performance is as follows:

[0076] The open-circuit voltage of the perovskite solar cell under AM 1.5G simulated sunlight is 4.5V, the short-circuit current is 40.3mA, and the photoelectric conversion efficiency of the power supply system is 12.15%; the supercapacitor takes 16.5 minutes to charge to 4V and 15.2 minutes to discharge at a constant current.

[0077] Under an indoor white LED light source with an illumination of 1000 lux and a color temperature of 4000K, the perovskite solar cell has an open circuit voltage of 3.45V and a short circuit current of 68.1μA, and the system's photoelectric conversion efficiency is 14.5%; the time it takes for the supercapacitor to charge to 3V is 121.4 hours.

[0078] Under an indoor white LED light source with an illumination of 200 lux and a color temperature of 4000K, the perovskite solar cell has an open circuit voltage of 3.23V, a short circuit current of 14.1μA, and a photoelectric conversion efficiency of 13.8%.

[0079] in, Figure 2 The perovskite solar cell-supercapacitor integrated device prepared in Example 2 of the present invention was subjected to AM1.5G simulated sunlight, and the current-voltage curve of the perovskite solar cell portion was measured.

[0080] Figure 3 The charge-discharge curve of the supercapacitor portion of the perovskite solar cell-supercapacitor integrated device prepared in Example 2 of the present invention was measured under AM1.5G simulated sunlight. Under the test conditions, the charge cut-off voltage was 4V and the discharge current was 40.0mA.

[0081] Figure 4 The current-voltage curve of the perovskite solar cell part of the perovskite solar cell-supercapacitor integrated device prepared in Example 2 of the present invention was measured under indoor white LED light. The light source used for the test was a 4000K white light LED lamp with an illumination of 1000 lux and 200 lux.

[0082] Figure 5The charge-discharge curve of the supercapacitor portion of the perovskite solar cell-supercapacitor integrated device prepared in Example 2 of the present invention was measured under indoor white LED light. The light source used for the test was a 4000K white LED lamp with an illumination of 1000 lux. The test conditions were a charge cutoff voltage of 3 V and a discharge current of 60 μA.

[0083] It should be understood that the application of the present invention is not limited to the above examples. For those skilled in the art, improvements or changes can be made based on the above description. All these improvements and changes should fall within the scope of protection of the claims attached to the present invention.

Claims

1. A method for preparing a perovskite solar cell-supercapacitor integrated device, characterized in that: The perovskite solar cell-supercapacitor integrated device is prepared by a roll-to-roll process.

2. The method for preparing a perovskite solar cell-supercapacitor integrated device according to claim 1, wherein: The steps of preparing the perovskite solar cell-supercapacitor integrated device by a roll-to-roll process are specifically as follows: providing a first substrate; coating a hole transport solution on the surface of the first substrate using a roll-to-roll process, followed by drying and annealing to obtain a hole transport layer; The perovskite solution is coated on the surface of the hole transport layer by a roll-to-roll process, followed by drying and annealing to obtain a perovskite light absorption layer; The electron transport solution is coated on the surface of the perovskite light absorption layer by a roll-to-roll process, followed by drying and annealing to obtain an electron transport layer; preparing a first metal electrode layer on the electron transport layer to obtain a perovskite solar cell; coating a graphene slurry on the surface of the first metal electrode layer using a roll-to-roll process to obtain a first graphene functional layer; Providing a second substrate, and preparing a second metal electrode layer on a surface of the second substrate; coating the graphene slurry on the surface of the second metal electrode layer using a roll-to-roll process, followed by drying and annealing to obtain a second graphene functional layer; coating a gel electrolyte on the surface of the second graphene functional layer using a roll-to-roll process, followed by drying and annealing to obtain a gel electrolyte layer; The first graphene functional layer is electrically connected to the gel electrolyte layer, and then the first graphene functional layer and the gel electrolyte layer are pressed together to obtain the perovskite solar cell-supercapacitor integrated device.

3. The method for preparing a perovskite solar cell-supercapacitor integrated device according to claim 2, wherein: In the step of coating the hole transport solution on the surface of the first substrate using a roll-to-roll process, the hole transport solution is one of 2PACz, PTAA, and NiOx. The parameters of the roll-to-roll process are: the roll-to-roll coating speed is 1-100 mm / s, and the slit width is set to 50-200 μm.

4. The method for preparing a perovskite solar cell-supercapacitor integrated device according to claim 2, wherein: In the step of coating the perovskite solution on the surface of the hole transport layer using a roll-to-roll process, the perovskite solution is FA 1-x Cs x Pb(Br 1-y I y )3 solution, wherein 0≤x≤1, 0≤y≤1, and the parameters of the roll-to-roll process are: the roll-to-roll coating speed is 1-100 mm / s, and the slit width is set to 50-200 μm.

5. The method for preparing a perovskite solar cell-supercapacitor integrated device according to claim 2, wherein: In the step of coating the electron transport solution on the surface of the perovskite light absorption layer using a roll-to-roll process, the electron transport solution is one of PFBO-C12, PCBM, and SnO2 solutions. The parameters of the roll-to-roll process are: the roll-to-roll coating speed is 1-100 mm / s, and the slit width is set to 50-300 μm.

6. The method for preparing a perovskite solar cell-supercapacitor integrated device according to claim 2, characterized in that: In the step of coating the graphene slurry on the surface of the first metal electrode layer using a roll-to-roll process, the parameters of the roll-to-roll process are: a roll-to-roll coating speed of 1-100 mm / s, and a slit width of 100 μm-2 mm.

7. The method for preparing a perovskite solar cell-supercapacitor integrated device according to claim 2, wherein: In the step of coating the graphene slurry on the surface of the second metal electrode layer using a roll-to-roll process, the parameters of the roll-to-roll process are: a roll-to-roll coating speed of 1-100 mm / s, and a slit width of 100 μm-2 mm.

8. The method for preparing a perovskite solar cell-supercapacitor integrated device according to claim 2, wherein: In the step of coating the gel electrolyte on the surface of the second graphene functional layer using a roll-to-roll process, the gel electrolyte is one of polyvinyl alcohol-sulfuric acid gel, polyethylene oxide-bistrifluoromethanesulfonyl imide lithium, and polyacrylonitrile-propylene carbonate-ionic liquid. The parameters of the roll-to-roll process are: the roll-to-roll coating speed is 1-50 mm / s, and the slit width is set to 100 μm-2 mm.

9. The method for preparing a perovskite solar cell-supercapacitor integrated device according to claim 2, wherein: Before the step of preparing the first metal electrode layer on the electron transport layer, the method further includes the step of preparing a barrier layer on the surface of the electron transport layer, wherein the barrier layer material is SnO2.

10. A perovskite solar cell-supercapacitor integrated device, characterized in that: The perovskite solar cell-supercapacitor integrated device is prepared by the preparation method according to any one of claims 1 to 9.

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