Roll-to-roll-based square meter level flexible photoelectric storage integrated device and preparation method and application thereof

Abstract

The invention discloses a roll-to-roll-based square meter flexible photoelectric storage integrated device and a preparation method and application thereof, and the method comprises the steps: preparing a thin film current collector at one side of a square meter flexible substrate through a roll-to-roll magnetron sputtering technology, and preparing an interdigital structure thin film current collector through a laser etching technology; coating a photoresist functional layer by using a roll-to-roll slit coating technology; the photoresist functional layer on the negative electrode side is etched through laser, the negative electrode side current collector is exposed, and the zinc negative electrode is prepared through the roll-to-roll magnetron sputtering technology; coating a photoresist functional layer by using a roll-to-roll slit coating technology; etching the photoresist functional layer on the positive electrode side by using laser, exposing the current collector on the positive electrode side, and preparing a thin film positive electrode by using a roll-to-roll slit coating technology; removing the photoresist functional layer in the residual area by laser irradiation; preparing a quasi-solid electrolyte; and preparing the flexible solar cell on one side of the square-meter-level flexible substrate away from the thin film current collector, and integrating and packaging to obtain the flexible solar cell.

Description

Technical Field

[0001] The present invention relates to the field of self-powered technology, and more specifically, to a roll-to-roll square-meter flexible photovoltaic storage and integrated device, as well as a preparation method and application thereof. Background Art

[0002] With the continuous development of science and technology, flexible electronic devices have shown great potential in fields such as energy, the Internet of Things, and smart buildings. However, existing technologies mostly focus on miniaturization and lightweight design to meet the needs of portable devices (such as wearable electronics and mobile power supplies), ignoring the urgent need for large-area, high-stability devices in fixed or semi-fixed scenarios, such as building integrated photovoltaics (BIPV), industrial-grade energy storage curtain walls, and power supply for large-scale sensor networks. The core requirements of such application scenarios for devices are not portability, but large-area uniformity, long-term environmental tolerance, and the economic feasibility of large-scale manufacturing. Thin-film zinc-based energy storage batteries have potential application value in many fields due to their many advantages such as high energy density, good safety, flexibility, environmental friendliness, and low cost. In addition, flexible solar cells have many advantages such as flexibility, lightweight, impact resistance, and material diversity, and have great development potential in the field of solar energy conversion. Integrating thin-film zinc-based energy storage batteries with flexible solar cells to prepare square-meter-scale integrated photovoltaic storage and application devices for integrated applications can give full play to the advantages of both.

[0003] However, the current preparation process of square-level thin-film zinc-based energy storage batteries and square-level flexible solar cells still faces great challenges, including complex processes, high costs, and poor stability, which seriously restrict their large-scale development. Summary of the Invention

[0004] The purpose of the present invention is to overcome the above-mentioned defects of the prior art and provide a roll-to-roll square-meter flexible photovoltaic storage and integrated integrated device and its preparation method and application, which has the advantages of simple process, low cost and good stability.

[0005] To achieve the above object, the technical solution of the present invention is as follows:

[0006] A roll-to-roll method for preparing a square-meter-scale flexible photovoltaic integrated device comprises the following steps:

[0007] S1. Provide square meter flexible substrate;

[0008] S2. preparing a thin film current collector on one side of the square meter flexible substrate using a roll-to-roll magnetron sputtering technique, and preparing an interdigitated structure thin film current collector using a laser etching technique;

[0009] S3, coating a photoresist functional layer on the interdigitated structure thin film current collector using a roll-to-roll slit coating technique;

[0010] S4, using a laser to etch the photoresist functional layer on the negative electrode side to expose the negative electrode side current collector, and then using a roll-to-roll magnetron sputtering technology to prepare a zinc negative electrode on the negative electrode side current collector;

[0011] S5, coating a photoresist functional layer on the zinc negative electrode using a roll-to-roll slit coating technique;

[0012] S6. Etching the photoresist functional layer on the positive electrode side by laser to expose the positive electrode side current collector, and then preparing a thin film positive electrode on the positive electrode side current collector by roll-to-roll slit coating technology;

[0013] S7, removing the photoresist functional layer in the remaining area by laser irradiation;

[0014] S8, preparing a quasi-solid electrolyte, injecting the quasi-solid electrolyte and encapsulating it to obtain a thin-film zinc-based energy storage battery;

[0015] S9, preparing a flexible solar cell on a side of the square meter flexible substrate facing away from the thin film current collector;

[0016] S10. Connect the negative electrode and the positive electrode of the thin-film zinc-based energy storage battery to the anode and cathode of the flexible perovskite solar cell respectively, and encapsulate them to obtain the square-meter-level flexible photovoltaic storage integrated device.

[0017] Optionally, the thin film zinc-based energy storage battery includes any one of a zinc ion battery, a Zn-I2 battery, a Zn-S battery and a Zn-Air battery.

[0018] Optionally, the flexible solar cell includes any one of a crystalline silicon cell, a cadmium telluride cell, a copper indium gallium selenide cell, a perovskite cell and a stacked solar cell.

[0019] Optionally, the tandem solar cell includes any one of a III-V group tandem solar cell, a silicon-based tandem solar cell, a perovskite / silicon tandem solar cell, an organic solar cell and a perovskite tandem solar cell, an all-organic tandem solar cell, a quantum dot and perovskite tandem solar cell, and a CIGS tandem solar cell.

[0020] Optionally, in step S1, the material of the square meter flexible substrate includes polyimide (PI), polyethylene terephthalate (PET), polyethylene naphthalate (PVN), polycarbonate (PC), polypropylene (PP), polybutylene terephthalate (PBT), polyethylene naphthalate (PEN), polytrimethylene terephthalate (PTT), polyester elastomer (COPE), polyethylene terephthalate (PCT), polyethylene terephthalate-co-dimethyl terephthalate (PETG), polyethylene ...PTT), polyethylene terephthalate (COPE), polyethylene terephthalate (PCT), polyethylene terephthalate-co-dimethyl terephthalate (PETG), polyethylene terephthalate (PET), polyethylene terephthalate (PET), polyethylene terephthalate (PTT), polyethylene terephthalate (PE), polyethylene terephthalate (PCT), polyethylene terephthalate (PET), polyethylene terephthalate (PET), polyethylene terephthalate (PET), polyethylene terephthalate (PET), polyethylene terephthalate (PET), polyethylene terephthalate (PE), polyethylene terephthalate (PE Any one of glycol ester-co-butylene terephthalate (PBTG), polydimethylsiloxane (PDMS), polyethylene (PE), polyvinylidene fluoride (PVDF), polyvinyl alcohol (PVA), polyurethane (PU), polystyrene (PS), polyvinylidene chloride (PVDC), polymethyl methacrylate (PMMA), polyphenylene sulfide (PPS), polyvinyl chloride (PVC), nylon, cellulose nanofiber (CNF), cellulose acetate (CA), cellulose acetate butyrate (CAB), paper and textile.

[0021] Optionally, in step S2, the material of the thin film current collector includes any one of copper, nickel, aluminum, titanium, gold, silver, platinum, iron, tungsten, molybdenum, tin, chromium, tantalum, indium tin oxide (ITO), fluorine-containing tin oxide (FTO), zinc aluminum oxide, conductive metal oxide particles, titanium carbide, tungsten carbide, silicide, indium tin, molybdenum disulfide, cuprous sulfide, and silicon nitride.

[0022] Optionally, in step S2, the thickness of the thin film current collector is 500 nm to 10 μm, and the width of the interdigital electrode is 1 μm to 1000 mm.

[0023] Optionally, in step S2, the width of the roll-to-roll magnetron sputtering technology is 10 mm to 1000 mm, the rotation speed is 0.01 m / s to 0.1 m / s, and the power is 400 W to 2000 W; the power of the laser etching technology is 0.1 W to 20 W.

[0024] Optionally, in step S3, the material of the photoresist functional layer includes any one of Norland Optical Adhesive 81, acrylate, KrF photoresist, ArF photoresist, EUV photoresist, g / i line photoresist, and ultraviolet broadband photoresist.

[0025] Optionally, in step S3, the thickness of the photoresist functional layer is 1 um to 100 um.

[0026] Optionally, in step S3, the slit spacing of the roll-to-roll slit coating technology is 10um to 1000um, and the rotation speed is 0.001m / s to 0.5m / s.

[0027] Optionally, in step S4, the power of the laser etching is 0.4W to 10W.

[0028] Optionally, in step S4, the rotation speed of the roll-to-roll magnetron sputtering technology is 0.001 m / s to 0.5 m / s, and the power is 100 W to 3000 W; the thickness of the zinc negative electrode is 1 um to 1000 um.

[0029] Optionally, in step S5, the slit spacing of the roll-to-roll slit coating technology is 50um to 500um, the rotation speed is 0.01m / s to 0.1m / s; and the thickness of the photoresist functional layer is 1um to 100um.

[0030] Optionally, in step S6, the power of the laser etching is 0.4W to 100W.

[0031] Optionally, in step S6, the slit spacing of the roll-to-roll slit coating technology is 10um to 5000um, and the rotation speed is 0.001m / s to 0.5m / s.

[0032] Optionally, in step S6, in the roll-to-roll slit coating technology, a planetary vacuum centrifugal mixer is used for mixing before coating, with a rotation speed of 600 rpm to 2000 rpm and a mixing time of 0.5 h to 5 h.

[0033] Optionally, in step S6, the thickness of the thin film positive electrode is 100 nm to 5 mm.

[0034] Optionally, the material of the thin film positive electrode includes any one of iodine, sulfur, iodine-containing inorganic conductive materials, iodine-containing organic molecules, sulfur-containing inorganic conductive materials, sulfur-containing organic molecules, C=O type organic molecules, C=S type organic molecules, C=N type organic molecules, N=N type organic molecules, -NO2 type organic molecules, conductive polymers, covalent organic frameworks (COFs), metal organic frameworks (MOFs), vanadium oxide, vanadium sulfide, manganese oxide, molybdenum sulfide, titanium sulfide, MXene, and manganese oxide.

[0035] Optionally, in step S7, the power of the laser etching is 0.1W to 200W.

[0036] Optionally, in step S8, the quasi-solid electrolyte includes a polymer or macromolecular organic matter, a zinc salt and a solvent; the concentration of the zinc salt in the quasi-solid electrolyte is 0.5 mol / L to 50 mol / L; the solvent includes an organic solvent and water, and the organic solvent is 1 wt.% to 100 wt.% relative to the mass of water.

[0037] Optionally, the polymer or macromolecular organic matter includes one or more of carboxymethyl cellulose, hydroxypropyl cellulose, chitosan, alginate, gelatin, starch and its derivatives, guar gum, pectin, protein, polyvinylidene fluoride, polyethylene glycol, polyacrylonitrile, polymethyl methacrylate, polymethyl methacrylate, polyurethane, polyvinyl methacrylate, polyacrylic acid, polyacrylamide, polyhydroxyethyl acrylate, polyvinyl alcohol, polyvinyl pyrrolidone, poly[3-(methacrylamido)propyl]dimethyl(3-thiopropyl)ammonium, poly 3-[[2-(methacryloyloxy)ethyl]dimethylammonium]propionate, polydopamine, polyvinylphosphonic acid, and poly(2-methacryloyloxyethylphosphorylcholine).

[0038] Optionally, the zinc salt includes any one of zinc trifluoromethanesulfonate (Zn(OTF)2), zinc sulfate (ZnSO4), zinc chloride (ZnCl2), zinc perchlorate (Zn(ClO4)2), bis(trifluoromethanesulfonyl)imide zinc (Zn(TFSI)2) and zinc tetrafluoroborate (Zn(BF4)2).

[0039] Optionally, the organic solvent includes any one of ethylene glycol (EG), acetonitrile (ACN), dimethyl sulfoxide (DMSO), N,N-dimethylformamide (DMF), N-methylpyrrolidone (NMP), polyethylene glycol (PEG), glycerol, liquid surfactant, diethylene glycol dimethyl ether, carbonate, diethylene glycol, butyrolactam, cyclopentane, ethylene glycol monomethyl ether, dimethyl methylphosphonate, polyethylene glycol diacid, diethylene glycol monoethyl ether, N,N-dimethyltrifluoroacetamide and tributyl phosphate.

[0040] The present invention also discloses a square-level flexible photovoltaic storage integrated device prepared by the above-mentioned preparation method, comprising a square-level flexible substrate, a thin-film zinc-based energy storage battery and a flexible solar cell; wherein the thin-film zinc-based energy storage battery and the flexible solar cell are respectively located on both sides of the square-level flexible substrate; the area of ​​the square-level flexible photovoltaic storage integrated device is greater than 0.5m 2 , mass / area ratio <1kg / m 2 .

[0041] The present invention also discloses an application of a square-meter-level flexible photovoltaic storage integrated device prepared by the above-mentioned preparation method in power generation devices, storage devices and power consumption systems.

[0042] Optionally, the power consumption system includes any one of building photovoltaic integration, urban public facilities (smart bus stops, self-powered road signs), distributed microgrids, cars, ships, large drones and other mobile platforms, smart homes, smart agriculture, intelligent transportation systems, environmental monitoring and military equipment.

[0043] The implementation of the present invention will have the following beneficial effects:

[0044] The present invention is based on a roll-to-roll preparation process and integrates square-meter-scale thin-film zinc-based energy storage batteries with flexible solar cells for the first time. The thin-film zinc-based energy storage battery is prepared on one side of the square-meter-scale flexible substrate, and the flexible solar cell is prepared on the other side. This breaks through the bottleneck of process compatibility between the power generation part and the energy storage part of the integrated photovoltaic storage device, effectively improves the integration level and reduces the energy loss of the overall system. It has broad application potential in many fields such as renewable energy, large mobile electronic devices, and industrial energy storage curtain walls. In the process of preparing square-meter-scale thin-film zinc-based energy storage batteries, the roll-to-roll process can achieve continuous coil processing, replacing traditional single-piece production and significantly improving production efficiency. In addition, the zinc-philic current collector can effectively improve the adhesion between the zinc negative electrode and the current collector, which is conducive to the preparation of a very high proportion of zinc (002) crystal planes, thereby improving the overall cycle stability of the battery. The positive electrode adopts a roll-to-roll slit coating process, which enriches the flexibility of the positive electrode material selection. The use of quasi-solid-state electrolytes can improve the safety, mechanical stability and service life of thin-film zinc-based energy storage batteries; the square-meter-level flexible integrated photovoltaic storage device prepared can face sunlight, weak light (cloudy days, indoors) and other conditions, and the obtained electricity can be used for the power system. BRIEF DESCRIPTION OF THE DRAWINGS

[0045] Figure 1 This is the light charge and discharge curve of the square meter-level flexible photovoltaic integrated device in Example 1 of the present invention.

[0046] Figure 2 This is a schematic structural diagram of the square meter-level flexible photovoltaic storage and integrated device in Example 1 of the present invention. DETAILED DESCRIPTION

[0047] The present invention will be further described below with reference to specific examples, but the present invention is not limited thereto in any way.

[0048] Example 1

[0049] The method for preparing a square-meter-level flexible photovoltaic storage and use integrated device based on roll-to-roll in this embodiment includes the following steps:

[0050] S1. Provide square-level flexible polyimide (PI) substrate.

[0051] S2. A Cu current collector with a thickness of approximately 1 μm was prepared on one side of the PI substrate using roll-to-roll magnetron sputtering technology with a width of 350 mm, a rotation speed of 0.05 m / s, and a power of 1000 W. A cross-finger structure thin film current collector was prepared using laser etching technology with a power of 0.5 W and a cross-finger electrode width of 1 mm.

[0052] S3. Coat a 50 μm thick acrylic photoresist functional layer on the interdigitated structure thin film current collector using a roll-to-roll slit coating technique with a width of 350 mm and a rotation speed of 0.05 m / s.

[0053] S4. Use laser etching on the photoresist functional layer on the negative electrode side with a power of 1 W to expose the negative electrode side current collector, and then use roll-to-roll magnetron sputtering technology to prepare a zinc negative electrode with a thickness of 50 μm on the negative electrode side current collector. The width of the roll-to-roll magnetron sputtering technology is 350 mm, the rotation speed is 0.05 m / s, and the power is 1000 W.

[0054] S5. Use roll-to-roll slit coating technology to coat a photoresist functional layer with a thickness of 50 μm on the zinc negative electrode; the width of the roll-to-roll magnetron sputtering technology is 350 mm and the rotation speed is 0.05 m / s.

[0055] S6. Use laser etching on the photoresist functional layer on the positive electrode side with a laser etching power of 5W to expose the positive electrode side current collector, and then use roll-to-roll slit coating technology to coat the iodine-loaded ink on the porous activated carbon host (AC@I2) on the positive electrode side current collector to prepare a positive electrode. The ink ratio is AC@I2: superconducting carbon black: PVDF = 0.07g: 0.02g: 0.01g dissolved in 10mL NMP.

[0056] S7. Remove the photoresist functional layer in the remaining area by laser irradiation, with the power of laser etching being 10W.

[0057] S8. Cover the interdigitated electrodes with a 1 mm thick gel electrolyte to assemble a square meter-scale flexible thin-film Zn-I2 battery. The gel electrolyte is composed of a hydrogel of polyacrylamide and zinc trifluoromethanesulfonate, with a zinc trifluoromethanesulfonate concentration of 3 mol / L.

[0058] S9, preparing a flexible solar cell on the side of the PI substrate away from the thin film current collector, specifically comprising: preparing NiO on the other side of the PI substrate X Hole transport layer, FA is prepared by blade coating on the hole transport layer x Cs 1-x PbI3 perovskite film, followed by preparation of PC 61 BM electron transport layer and BCP layer, and finally deposit metal Ag electrode, use conductive copper tape to connect the negative electrode and positive electrode of thin-film zinc-based energy storage battery and the anode and cathode of flexible perovskite solar cell respectively, and finally encapsulate the thin-film zinc-based energy storage battery and flexible perovskite solar cell respectively to prepare square-meter-level flexible photovoltaic storage and integrated integrated device.

[0059] S10. Under low-light conditions indoors, the square meter-level flexible photovoltaic storage and integrated integrated device is charged and powered for daily LED lights.

[0060] The square-meter-level flexible photovoltaic storage integrated device of this embodiment includes a square-meter-level flexible substrate, a thin-film zinc-based energy storage battery and a flexible solar cell; wherein the thin-film zinc-based energy storage battery and the flexible solar cell are respectively located on both sides of the square-meter-level flexible substrate; the area of ​​the square-meter-level flexible photovoltaic storage integrated device is greater than 0.5m 2 , mass / area ratio <1kg / m 2 . Figure 1 is the light charge and discharge curve of the integrated device for photoelectric storage and use in Example 1, Figure 2 Schematic diagram of the structure of the flexible photoelectric storage and integrated device in Example 1.

[0061] Example 2

[0062] Compared with Example 1, the only difference is that the PI substrate is replaced by a flexible polyethylene terephthalate (PET) substrate.

[0063] Example 3

[0064] Compared with Example 1, the only difference is that the Cu current collector is replaced by a Ti current collector.

[0065] Example 4

[0066] Compared with Example 1, the only difference is that the active material of the positive electrode material in the thin-film zinc-based energy storage battery is replaced by AC@S from AC@I2.

[0067] Example 5

[0068] Compared with Example 1, the only difference is that the active material of the positive electrode material in the thin-film zinc-based energy storage battery is replaced by NiFe LDH catalyst from AC@I2.

[0069] Example 6

[0070] Compared with Example 1, the only difference is that the PVDF in the positive electrode ink is replaced by sodium alginate.

[0071] Example 7

[0072] Compared with Example 1, the only difference is that the NMP in the positive electrode ink is replaced by a mixed solution containing water and glacial acetic acid.

[0073] Example 8

[0074] Compared with Example 1, the only difference is that the polyacrylamide (PAM) gel electrolyte is replaced with polyacrylic acid (PAA).

[0075] Example 9

[0076] Compared with Example 1, the only difference is that the zinc salt used in the gel electrolyte is zinc sulfate (ZnSO4) with a concentration of 2 mol / L.

[0077] Example 10

[0078] Compared with Example 1, the only difference is that the zinc salt used in the gel electrolyte is zinc bis(trifluoromethanesulfonyl)imide (Zn(TFSI) 2 ) with a concentration of 2 mol / L.

[0079] Example 11

[0080] Compared with Example 1, the only difference is that the square meter-level flexible photovoltaic storage integrated device of this embodiment is integrated with a thin film zinc-based energy storage battery and a flexible perovskite / crystalline silicon stacked solar cell.

[0081] Example 12

[0082] Compared with Example 1, the only difference is that: under the condition of facing sunlight, the square meter-level flexible photovoltaic storage and use integrated device is charged and the daily LED lamp is powered.

[0083] The effects of Examples 2 to 12 are the same as those of Example 1.

[0084] The above-described embodiments merely represent several implementation methods of the present invention. While the descriptions are relatively specific and detailed, they should not be construed as limiting the scope of the patent application. It should be noted that a person skilled in the art would be able to make various modifications and improvements without departing from the spirit of the present invention, all of which fall within the scope of protection of the present invention. Therefore, the scope of protection of the patent for this invention shall be determined by the appended claims.

Claims

1. A method for preparing a square-meter flexible photovoltaic storage and integrated device based on roll-to-roll, characterized in that: The following steps are involved: S1. Provide square meter flexible substrate; S2. preparing a thin film current collector on one side of the square meter flexible substrate using a roll-to-roll magnetron sputtering technique, and preparing an interdigitated structure thin film current collector using a laser etching technique; S3, coating a photoresist functional layer on the interdigitated structure thin film current collector using a roll-to-roll slit coating technique; S4, using a laser to etch the photoresist functional layer on the negative electrode side to expose the negative electrode side current collector, and then using a roll-to-roll magnetron sputtering technology to prepare a zinc negative electrode on the negative electrode side current collector; S5, coating a photoresist functional layer on the zinc negative electrode using a roll-to-roll slit coating technique; S6. Etching the photoresist functional layer on the positive electrode side by laser to expose the positive electrode side current collector, and then preparing a thin film positive electrode on the positive electrode side current collector by roll-to-roll slit coating technology; S7, removing the photoresist functional layer in the remaining area by laser irradiation; S8, preparing a quasi-solid electrolyte, injecting the quasi-solid electrolyte and encapsulating it to obtain a thin-film zinc-based energy storage battery; S9, preparing a flexible solar cell on a side of the square meter flexible substrate facing away from the thin film current collector; S10. Connect the negative electrode and the positive electrode of the thin-film zinc-based energy storage battery to the anode and cathode of the flexible perovskite solar cell respectively, and encapsulate them to obtain the square-meter-level flexible photovoltaic storage integrated device.

2. The method for preparing a roll-to-roll square-meter flexible photovoltaic integrated device according to claim 1, characterized in that: The thin film zinc-based energy storage battery includes any one of a zinc ion battery, a Zn-I2 battery, a Zn-S battery and a Zn-Air battery; The flexible solar cell includes any one of a crystalline silicon cell, a cadmium telluride cell, a copper indium gallium selenide cell, a perovskite cell and a stacked solar cell.

3. The method for preparing a roll-to-roll square-meter flexible photovoltaic integrated device according to claim 1, characterized in that: In step S1, the material of the square meter flexible substrate includes any one of polyimide, polyethylene terephthalate, polyethylene naphthalate, polycarbonate, polypropylene, polybutylene terephthalate, polyethylene naphthalate, polypropylene terephthalate, polyester elastomer, polyethylene dimethyl terephthalate, polyethylene terephthalate-co-dimethyl terephthalate, polyethylene terephthalate-co-butylene terephthalate, polydimethylsiloxane, polyethylene, polyvinylidene fluoride, polyvinyl alcohol, polyurethane, polystyrene, polyvinylidene chloride, polymethyl methacrylate, polyphenylene sulfide, polyvinyl chloride, nylon, cellulose nanofiber, cellulose acetate, cellulose acetate butyrate, paper and textile.

4. The method for preparing a roll-to-roll square-meter flexible photovoltaic integrated device according to claim 1, wherein: In step S2, the material of the thin film current collector includes any one of copper, nickel, aluminum, titanium, gold, silver, platinum, iron, tungsten, molybdenum, tin, chromium, tantalum, indium tin oxide, fluorine-containing tin oxide, zinc aluminum oxide, conductive metal oxide particles, titanium carbide, tungsten carbide, silicide, indium tin, molybdenum disulfide, cuprous sulfide, and silicon nitride; the thickness of the thin film current collector is 500 nm to 10 μm, and the width of the interdigital electrode is 1 μm to 1000 mm; The roll-to-roll magnetron sputtering technology has a width of 10 mm to 1000 mm, a rotation speed of 0.01 m / s to 0.1 m / s, and a power of 400 W to 2000 W; The power of the laser etching technology is 0.1W to 20W.

5. The method for preparing a roll-to-roll square-meter flexible photovoltaic integrated device according to claim 1, characterized in that: In step S3, the material of the photoresist functional layer includes any one of Norland Optical Adhesive 81, acrylate, KrF photoresist, ArF photoresist, EUV photoresist, g / i line photoresist, and ultraviolet broadband photoresist; the thickness of the photoresist functional layer is 1 μm to 100 μm; The slit spacing of the roll-to-roll slit coating technology is 10um to 1000um, and the rotation speed is 0.001m / s to 0.5m / s.

6. The method for preparing a roll-to-roll square-meter flexible photovoltaic integrated device according to claim 1, characterized in that: In step S4, the power of the laser etching is 0.4W to 10W; the rotation speed of the roll-to-roll magnetron sputtering technology is 0.001m / s to 0.5m / s, and the power is 100W to 3000W; the thickness of the zinc negative electrode is 1um to 1000um; In step S5 , the slit spacing of the roll-to-roll slit coating technology is 50 μm to 500 μm, the rotation speed is 0.01 m / s to 0.1 m / s; and the thickness of the photoresist functional layer is 1 μm to 100 μm.

7. The method for preparing a roll-to-roll square-meter flexible photovoltaic integrated device according to claim 1, characterized in that: In step S6, the power of the laser etching is 0.4W to 100W; the slit spacing of the roll-to-roll slit coating technology is 10um to 5000um, and the rotation speed is 0.001m / s to 0.5m / s; in the roll-to-roll slit coating technology, a planetary vacuum centrifugal mixer is used for mixing before coating, with a rotation speed of 600rpm to 2000rpm and a time of 0.5h to 5h; the thickness of the thin film positive electrode is 100nm to 5mm; In step S7, the power of the laser etching is 0.1W to 200W.

8. The method for preparing a roll-to-roll square-meter flexible photovoltaic integrated device according to claim 1, characterized in that: In step S8, the quasi-solid electrolyte includes a polymer or macromolecular organic matter, a zinc salt, and a solvent; the concentration of the zinc salt in the quasi-solid electrolyte is 0.5 mol / L to 50 mol / L; The solvent includes an organic solvent and water, and the organic solvent accounts for 1 wt.% to 100 wt.% relative to the mass of water.

9. A square-meter-scale flexible photovoltaic integrated device prepared by the preparation method according to any one of claims 1 to 8, characterized in that: It includes a square-level flexible substrate, a thin-film zinc-based energy storage battery and a flexible solar cell; wherein the thin-film zinc-based energy storage battery and the flexible solar cell are respectively located on both sides of the square-level flexible substrate; the area of ​​the square-level flexible photovoltaic storage integrated device is greater than 0.5m 2 , mass / area ratio <1kg / m 2 .

10. An application of a square-meter-scale flexible photovoltaic storage and use integrated device prepared by the preparation method according to any one of claims 1 to 8 in a power generation device, a storage device and a power consumption system.

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