CN112382511B - Self-charging micro optical capacitor device and preparation method thereof - Google Patents
Self-charging micro optical capacitor device and preparation method thereof Download PDFInfo
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Abstract
The invention relates to a self-charging micro optical capacitor device and a preparation method thereof, belonging to the technical field of energy storage devices. The photoelectric capacitor device comprises a micro super capacitor, a perovskite solar cell, a shared cathode lead, a shared anode lead, a series lead, a packaging material and electrolyte, wherein the perovskite solar cell and the micro super capacitor are seamlessly connected on the same conductive glass through smart graphic design, so that the internal resistance is reduced; through the adaptability among the activated carbon, the RGO, the PEDOT and the electrolyte, the structural parameters of the perovskite solar cell and the micro super capacitor can be optimized, and the series integration of a plurality of perovskite solar cells can be realized, so that the large capacitance, the high energy density and the excellent large-current charging and discharging performance of the photoelectric capacitor device can be realized; in addition, the preparation process of the photoelectric capacitor device is simple, large-scale preparation can be realized, the size is small, the photoelectric capacitor device is green and environment-friendly, and the photoelectric capacitor device has a good application prospect.
Description
Technical Field
The invention relates to a self-charging micro optical capacitor device and a preparation method thereof, belonging to the technical field of energy storage devices.
Background
Portable integrated microelectronic devices have become a mainstream in the current electronic industry development. As one of the most important components of microelectronic devices, high-performance micro power systems have been the subject of research to meet energy and integration requirements. Energy supply systems including micro batteries, micro supercapacitors and photovoltaic cells have been developed and studied to date. In the above energy supply system, the photovoltaic cell can directly generate electricity using clean and renewable solar energy, but its output is strongly influenced by the diurnal cycle and light fluctuations. On the other hand, although supercapacitors can provide uninterrupted power supply and have the advantages of high power density, long cycle life and fast charge and discharge rates, they must be externally charged due to the lack of continuous self-generating power.
In this case, the use of photovoltaic cells to collect solar energy and charge the supercapacitors is a good choice. At present, a super capacitor device with light charging capacity mostly adopts a splicing mode, namely, a photovoltaic cell and a super capacitor are connected through conducting materials such as extra wires, but the system connected through the outside has the following problems: firstly, in the method, the conducting wire is very easy to tangle, and the whole system has a large volume, so that the requirements of wearable electronic equipment cannot be met; secondly, due to the difference of materials among the photovoltaic cell, the capacitor and the lead, a large resistance is generated in the connection process, and the overall photoelectric conversion efficiency of the device is affected. Therefore, the advent of a highly integrated photoelectric conversion-energy storage device, i.e., a photo capacitor, has effectively solved the above-mentioned problems. The optical capacitor is an in-situ energy storage device, wherein the solar cell and the super capacitor share electrodes to simultaneously realize energy conversion and storage.
However, most of the existing optical capacitors are based on macroscopic super capacitor preparation, so that the integration can only be carried out through external wires, which results in poor uniformity and low integration, and is not favorable for carrying and supplying power according to requirements. In addition, since the open circuit voltage of most photovoltaic cells is low, the working voltage and energy density of the photo-capacitor are generally low, most of the photo-capacitors are limited to lighting a small LED lamp and cannot drive other electric devices, and therefore, a micro photo-capacitor with high energy density, high integration and high working voltage is urgently needed to solve the problems.
Disclosure of Invention
Aiming at the defects of the existing photoelectric capacitor, the invention provides a self-charging micro photoelectric capacitor device and a preparation method thereof, wherein the seamless connection between a perovskite solar cell and a micro super capacitor is realized on the same conductive glass through a smart graphic design, so that the internal resistance of the micro photoelectric capacitor is reduced; through the adaptability among the activated carbon, the reduced-Redox Graphene Oxide (RGO), the poly 3, 4-ethylenedioxythiophene (PEDOT) and the electrolyte, a plurality of perovskite solar cells can be integrated in series, and the large capacitance, the high energy density and the excellent large-current charging and discharging performance of the device are realized; in addition, the device has simple preparation process and strong operability, and can be used for large-scale preparation.
The purpose of the invention is realized by the following technical scheme.
A self-charging miniature photo-capacitor device comprising a miniature supercapacitor, a perovskite solar cell, a shared negative lead, a shared positive lead, a series lead, an encapsulant, and an electrolyte;
the micro super capacitor is formed by the interdigital cross arrangement of two interdigital electrodes, and the material composition of the interdigital electrodes is a gold current collector and a carbon-activated carbon layer and an RGO-PEDOT (reduced redox graphene oxide-poly 3,4 ethylene dioxythiophene) layer which are sequentially coated on the surface of the gold current collector;
the perovskite solar cell sequentially comprises conductive glass (such as FTO conductive glass or ITO conductive glass) and SnO2Barrier layer, MAPbI3A photosensitive layer and a composite electrode layer, the conductive glass comprises a non-conductive region after etching treatment andn (n is an integer more than or equal to 1) conductive areas, each conductive area is divided into an electrode area and a battery area, each conductive area comprises a perovskite solar cell, the perovskite solar cell is positioned in the battery area, a composite coating of a carbon-activated carbon layer and an RGO-PEDOT layer is coated on the electrode area, and the composite electrode layer is a composite electrode layer consisting of the carbon-activated carbon layer and the RGO-PEDOT layer;
the shared negative electrode lead, the shared positive electrode lead and the series lead are all made of carbon-activated carbon layers and RGO-PEDOT layers, namely the components of the shared negative electrode lead, the components of the coating on the gold current collector and the components of the coating on the electrode area are the same; wherein the thickness of the carbon-activated carbon layer is 60-100 mu m, the mass ratio of carbon to activated carbon is 3: 1-5: 1, the thickness of the RGO-PEDOT layer is 50-80 mu m, and the mass ratio of RGO to PEDOT is 1: 1-1: 1.5;
the solar cell comprises a micro super capacitor, perovskite solar cells, a shared cathode lead, a shared anode lead and a series lead, wherein one interdigital electrode of the micro super capacitor is connected with a composite coating of an electrode region in one conductive region on conductive glass through the shared cathode lead, the other interdigital electrode of the micro super capacitor is connected with a composite electrode of the perovskite solar cells in the other conductive region on the conductive glass through the shared anode lead, the series lead is used for realizing the series connection of two adjacent perovskite solar cells, and the composite electrode of one perovskite solar cell is connected with the composite coating of the electrode region in the conductive region where the other perovskite solar cell is located; the electrolyte is dripped on the surface of an interdigital electrode of the micro super capacitor, and the packaging material is used for packaging the micro super capacitor, the perovskite solar cell, the shared positive electrode lead, the shared negative electrode lead and the series lead;
when n is 1, the optical capacitor device does not comprise a series lead, one interdigital electrode of the miniature super capacitor is connected with the composite coating of the electrode area in one conductive area on the conductive glass through a shared negative lead, and the other interdigital electrode of the miniature super capacitor is connected with the composite electrode of the perovskite solar cell in the conductive area on the conductive glass through a shared positive lead.
When the device is charged, the n perovskite solar cells connected in series charge the micro super capacitor through the shared positive electrode lead and the shared negative electrode lead; when the device discharges, any point on the shared negative electrode lead is connected with the negative electrode of an external electrical appliance, and any point on the shared positive electrode lead is connected with the positive electrode of the external electrical appliance.
In addition, the number of the perovskite solar cells is determined by the output voltage of the micro super capacitor in the device, and the number of the perovskite solar cells connected in series is large when the output voltage value is large; the electrolyte is selected from electrolyte which can work under the output voltage of the device.
Furthermore, the number of the interdigital electrodes of each interdigital electrode in the micro super capacitor is 10-14, the width of each interdigital electrode is 0.45-0.6 mm, the length of each interdigital electrode is 4.8-5.0 mm, and the interval width between every two adjacent interdigital electrodes in crossed arrangement is 0.45-0.5 mm.
Further, the thickness of the gold current collector in the micro supercapacitor is preferably 150nm to 200 nm.
Further, the effective area of each perovskite solar cell is preferably 27mm2～48mm2The spacing between two adjacent perovskite solar cells is preferably no greater than 1.2 mm.
Further, the line width of the shared positive electrode lead and the shared negative electrode lead is preferably 1 mm-1.5 mm, the line width of the series lead is preferably equal to the width of the composite electrode on the perovskite solar cell, and the size of the electrode area (i.e. the size of the composite coating in the electrode area) is preferably equal to the size of the composite electrode on the perovskite solar cell.
Furthermore, the device comprises three perovskite solar cells connected in series, and the three perovskite solar cells are arranged in an inverted 'pin' shape; accordingly, the electrolyte is preferably formulated from 1-ethyl-3-methylimidazolium tetrafluoroborate, poly (vinylidene fluoride-co-hexafluoropropylene) (PVDF-HFP), and acetone; wherein the concentration of PVDF-HFP is 110 mg/mL-130 mg/mL, and the concentration of 1-ethyl-3-methylimidazolium tetrafluoroborate is 510 mg/mL-540 mg/mL.
Further, the encapsulating material is preferably polyethylene terephthalate (PET) or polyimide.
The invention relates to a preparation method of a self-charging micro-optical capacitor device, which comprises the following steps:
(1) carrying out laser etching treatment on the conductive glass to form a non-conductive area (an area after laser etching) and n conductive areas (an area which is not etched by laser); preparing SnO in each conductive region in turn2Barrier layer, MAPbI3A photosensitive layer, followed by laser etching to remove a portion of SnO2Barrier layers and MAPbI3A photosensitive layer, exposed partial conductive region is an electrode region, SnO2Barrier layers and MAPbI3The conductive area covered by the photosensitive layer is a battery area;
(2) preparing a mask plate based on the patterns of the miniature super capacitor, the shared cathode lead, the shared anode lead, the series lead and the electrode area by utilizing laser etching; preparing a gold current collector of the micro supercapacitor in a non-conductive area of conductive glass by adopting a gold spraying technology with the aid of a micro supercapacitor pattern in a mask plate, then coating carbon-activated carbon slurry on the gold current collector, and simultaneously under the aid of a shared negative electrode wire, a shared positive electrode wire, a series wire and an electrode area pattern in the mask plate, forming the non-conductive area, the electrode area and the MAPbI of the conductive glass in the non-conductive area, the electrode area and the MAPbI3Coating carbon-activated carbon slurry on the photosensitive layer, realizing the integrated connection between the miniature super capacitor and the n perovskite solar cells by coating the carbon-activated carbon slurry, coating RGO-PEDOT powder on all the carbon-activated carbon slurry coating layers, removing a mask plate, annealing at 100-120 ℃ for 40-60 min, and obtaining an integrated structure of the miniature super capacitor, the perovskite solar cells, the shared cathode lead, the shared anode lead and the series lead on conductive glass;
(3) and (3) dropwise coating electrolyte on the surface of the interdigital electrode of the micro super capacitor, respectively leading out an external lead from the shared cathode lead and the shared anode lead for connecting with an external electric appliance, and finally packaging by adopting a packaging material to obtain the photoelectric capacitor device.
Wherein, the RGO-PEDOT powder is a composite powder formed by depositing PEDOT on RGO foam, and the RGO-PEDOT powder can be prepared by the following method: RGO foam is used as a working electrode, a silver/silver chloride electrode is used as a reference electrode, a platinum electrode is used as a counter electrode, emulsion of 3,4 Ethylene Dioxythiophene (EDOT) and lithium perchlorate is used as electrolyte, PEDOT is deposited on the RGO foam, and the RGO-PEDOT foam obtained after deposition is ground and sieved after being dried to obtain RGO-PEDOT powder; the concentration of EDOT in the electrolyte is 14.0 mg/mL-14.5 mg/mL, the concentration of lithium perchlorate is 10.5 mg/mL-11.0 mg/mL, the voltage of electrodeposition is 0.8V-0.9V, and the time of electrodeposition is 150 min-170 min;
the carbon-activated carbon slurry is prepared from activated carbon and conductive carbon slurry.
Further, the particle size of the RGO-PEDOT powder is preferably not larger than 200 mesh.
Furthermore, the mask plate can be made of stainless steel, aluminum foil, polyimide and the like, and polyimide with the thickness of 0.10 mm-0.12 mm is preferred.
Has the advantages that:
(1) according to the invention, the carbon-activated carbon/RGO-PEDOT composite material is used as the materials of the perovskite solar cell composite electrode, the micro super capacitor interdigital electrode, the shared anode and cathode lead and the series lead, and the perovskite solar cell and the micro super capacitor are prepared on the same conductive glass through ingenious graphic design, so that the integrated design of the perovskite solar cell and the micro super capacitor is realized, the integrity and the connectivity of the photoelectric capacitor device are ensured, and the internal resistance of the photoelectric capacitor device is reduced;
(2) according to the invention, a plurality of perovskite solar cells can be integrated in series mainly through the adaptability among the activated carbon, the RGO, the PEDOT and the electrolyte, so that the large capacitance, the high energy density and the excellent large-current charging and discharging performance of the photoelectric capacitor device are realized, the LED lamp array can be lightened, and the operation of electrical appliances with larger power, such as a fan and the like, can be driven; in addition, structural parameters of the perovskite solar cell and the micro super capacitor can be optimized, and the electrochemical performance of the optical capacitor is further improved;
(3) the optical capacitor device has the optical charging function, can convert solar energy into optical energy to charge the micro super capacitor, and is green and environment-friendly; the preparation method of the photoelectric capacitor device is simple to operate, the open circuit condition is not easy to occur in the preparation process, the photoelectric capacitor device can be prepared in a large scale, and the photoelectric capacitor device is small in size, easy to carry and good in application prospect.
Drawings
Fig. 1 is a schematic structural view of a mask plate prepared in example 1.
Fig. 2 is a schematic structural diagram of three conductive regions in the FTO glass after laser etching in example 1.
Fig. 3 is a schematic structural view of an integrated structure of the micro supercapacitor, the perovskite solar cell, the shared negative electrode lead, the shared positive electrode lead, and the series lead prepared in example 1.
Fig. 4 is a cross-sectional Scanning Electron Microscope (SEM) image of the perovskite solar cell prepared in example 1.
Fig. 5 is a current-voltage graph of the perovskite solar cell prepared in example 1.
Fig. 6 is a surface Scanning Electron Microscope (SEM) image of the interdigitated electrodes in the micro supercapacitor fabricated in example 1.
FIG. 7 is a comparison of cyclic voltammograms of the micro-supercapacitors prepared in example 1 at different scan rates.
FIG. 8 is a comparative plot of constant current charge and discharge curves at different current densities for the micro-supercapacitors prepared in example 1.
FIG. 9 is a graph of power density, energy density, and area specific capacitance for the micro-supercapacitors prepared in example 1 at different current densities.
Fig. 10 is a graph comparing the photo-charge-constant current discharge curves at different discharge current densities for the self-charged micro-supercapacitor devices prepared in example 1.
Fig. 11 is a graph of energy density, power density, and area specific capacitance for different discharge current densities for the self-charging micro-supercapacitor devices prepared in example 1.
Detailed Description
The present invention is further illustrated by the following figures and detailed description, wherein the processes are conventional unless otherwise specified, and the starting materials are commercially available from a public source without further specification.
In the following examples:
scanning Electron Microscope (SEM): SUPRA 55, Call. Chuiss GmbH;
laser instrument: LAJAMIN LASER (LM-YLP-20F-III), Beijing radium Jigming LASER technology development Limited;
solar simulator: XP150, Beijing Sanyou Dingsheng science and technology Limited;
digital source table: 2400, Tektronix corporation;
an electrochemical workstation: CHI 760E, shanghai chenhua instruments ltd;
conductive carbon paste: DD-10, carbon content 40 wt% to 50 wt%, Guangzhou Seddy technologies, Inc.;
the charge-discharge curve of the micro super capacitor part in the photo-capacitor device prepared in the example is tested by adopting a chronopotentiometry and a cyclic voltammetry, and the used instrument is a CHI 760E electrochemical workstation in Shanghai Chen Hua, China; during testing, a working electrode of the electrochemical workstation is connected with any point in a shared cathode lead (or a shared anode lead) in the photoelectric capacitor device, and a counter electrode and a reference electrode of the electrochemical workstation are both connected with any point in a shared anode lead (or a shared anode lead);
the perovskite solar cell portion in the photo-capacitor device prepared in the examples was subjected to a test of a current-voltage curve using the solar simulator XP150 and the digital source meter 2400; during testing, the positive electrode of the digital source meter is connected with any point (marked as point b) in a shared positive electrode lead in the photoelectric capacitor device, and the negative electrode of the digital source meter is connected with any point (marked as point a) in a shared negative electrode lead;
the photoelectric capacitor device prepared in the embodiment is subjected to a photo-charging-constant current discharging curve test by adopting a time potential method, and the used instruments are a CHI 760E electrochemical workstation and an XP150 sunlight simulator in Shanghai China; during testing, the working electrode of the electrochemical workstation is connected with any point in a shared cathode lead (or a shared anode lead) in the photoelectric capacitor device, and the counter electrode and the reference electrode of the electrochemical workstation are both connected with any point in a shared anode lead (or a shared anode lead).
Example 1
Preparation of RGO-PEDOT powder
(A1) Preparing a Graphene Oxide (GO) solution by using a conventional oxidation-reduction method: mixing 9g of graphite powder, 9g of sodium nitrate and 240mL of concentrated sulfuric acid (mass fraction is 98%), placing the mixture in an ice-water bath, stirring for 2 hours, slowly adding 27g of potassium permanganate, controlling the temperature of the system to be always lower than 10 ℃, continuously stirring at low temperature for 1 hour, heating the mixture in the water bath to 36 ℃, and stirring at the temperature for 2 hours; then adding 600mL of ice water, continuously heating to 85 ℃, stirring for 40min at the temperature, then adding 1000mL of ice water and 60mL of hydrogen peroxide solution, then adding 400mL of hydrochloric acid with the volume fraction of 10% into the liquid in batches, carrying out suction filtration, transferring the GO obtained by suction filtration into a beaker, adding 650mL of distilled water, carrying out ultrasonic treatment for 6h after stirring, and finally adding the liquid after ultrasonic treatment into a dialysis bag for dialysis for 1 week to obtain a GO solution with the concentration of 5 mg/mL;
(A2) adding 80mL of GO solution into a 100mL hydrothermal kettle, and performing hydrothermal treatment at 150 ℃ for 12h to obtain RGO foam;
(A3) adding 0.432g of lithium perchlorate and 424 muL of EDOT (0.568g) into 40mL of water, then carrying out ultrasonic treatment for 10min to form a uniform emulsion serving as an electrolyte, taking RGO foam as a working electrode, a silver/silver chloride electrode as a reference electrode and a platinum electrode as a counter electrode, and depositing at 0.8V for 160min to form RGO-PEDOT foam on the working electrode; the RGO-PEDOT foam was freeze dried for 48h, ground and sieved using a 200 mesh screen to obtain RGO-PEDOT powder.
Preparing carbon-activated carbon slurry: adding 10g of activated carbon into 100g of conductive carbon slurry, and ball-milling for 12h to uniformly mix to obtain the carbon-activated carbon slurry.
Preparing electrolyte: firstly, 0.3g of PVDF-HFP is added into 2.5mL of acetone and stirred for 10-15 h, then 1.3g of 1-ethyl-3-methylimidazolium boron tetrafluoride is added and stirred until the solution is clear, and the ionic liquid gel electrolyte is obtained.
Preparing a mask plate: preparing a pattern with a micro super capacitor, a shared cathode lead, a shared anode lead, a series lead and an electrode area structure on a polyimide adhesive tape with the thickness of 0.12mm by utilizing laser etching to be used as a mask plate, as shown in figure 1;
preparation of self-charging micro-optical capacitor device
(B1) Performing partial laser etching on the FTO conductive glass to form a non-conductive area and 3 conductive areas with the same size, wherein three rectangular areas which are arranged in an inverted 'pin' shape and have the size of 4mm multiplied by 9mm in the figure 2 are conductive areas, the distance between every two adjacent conductive areas is 1mm, and the other areas are non-conductive areas; then, sequentially carrying out ultrasonic treatment in a liquid detergent (such as a Libai fresh lemon liquid detergent), deionized water and ethanol to clean the FTO glass after laser etching, drying the cleaned FTO glass by using argon, and treating the dried FTO glass for 3min by using air plasma to obtain pretreated FTO glass;
(B2) respectively spin-coating SnO with the mass fraction of 2.67% on 3 conductive regions of the pretreated FTO glass2The colloidal dispersion liquid is prepared at the rotating speed of 3000rpm for 30s by spin coating, and is annealed at 150 ℃ for 30min to form SnO in a conductive region2A barrier layer; treatment of SnO with air plasma2After blocking for 1min, SnO2Spin-coating on the barrier layer with PbI2Solutions of (lead iodide) and MAI (methyl ammonium iodide) in DMF (N, N-dimethylformamide), PbI2And MAI concentration of 0.1M, rotation speed of 3000rpm, spin coating time of 30s, annealing at 100 deg.C for 5min, and annealing in SnO2Formation of MAPbI on barrier layer3A photosensitive layer;
(B3) on the left side of each conductive region, a portion of SnO is removed by laser etching2Barrier layers and MAPbI3A photosensitive layer, wherein the exposed conductive region with the size of 4mm multiplied by 4mm is an electrode region, SnO2Barrier layer and MAPbI3The conductive area covered by the photosensitive layer is a battery area;
(B4) preparing a gold current collector of the micro supercapacitor in a non-conductive area of the FTO glass by adopting a gold spraying technology with the aid of a micro supercapacitor pattern in a mask plate to obtain the gold current collector with the thickness of 200 nm; then coating carbon-activated carbon slurry on a gold current collector, and simultaneously under the auxiliary action of a shared negative electrode lead, a shared positive electrode lead, a series connection lead and an electrode area pattern in a mask plate, forming a non-conductive area, an electrode area and MAPbI of the FTO glass3Coating carbon-activated carbon slurry on the photosensitive layer, realizing the integrated connection between the miniature super capacitor and 3 perovskite solar cells through the coated carbon-activated carbon slurry layer with the thickness of 70 mu m, coating an RGO-PEDOT powder layer with the thickness of 70 mu m on all the carbon-activated carbon slurry coatings, removing a mask plate, annealing for 1h at 100 ℃, and obtaining an integrated structure of the miniature super capacitor, the perovskite solar cells, the shared cathode lead, the shared anode lead and the series lead on FTO glass, namely: an interdigital electrode on the upper side in the micro super capacitor is connected with a composite coating of an electrode area in a conductive area on the left side of FTO glass through a shared negative electrode lead wire with the line width of 1mm, an interdigital electrode on the lower side in the micro super capacitor is connected with a composite electrode of a perovskite solar cell in a conductive area on the right side of FTO glass through a shared positive electrode lead wire with the line width of 1mm, a composite coating of an electrode area in a conductive area on the upper side and the lower side of FTO glass is connected with a composite electrode of a perovskite solar cell in a conductive area on the left side of FTO glass through a series lead wire with the line width of 4mm, and a composite coating of an electrode area in a conductive area on the right side of FTO glass is connected with a composite electrode of a perovskite solar cell in a conductive area on the upper side and the lower side of FTO glass through a series lead wire with the line width of 4mm, as shown in figure 3;
in fig. 3, the micro supercapacitor is formed by interdigitation arrangement of two interdigital electrodes, the number of the interdigital electrodes of each interdigital electrode is 12, the width of each interdigital electrode is 0.5mm, the length of each interdigital electrode is 4.9mm, and the interval width between two adjacent interdigital electrodes in the interdigitation arrangement is 0.46 mm;
of 3 perovskite solar cells in FIG. 3The composite electrodes are arranged in an inverted Chinese character 'pin'; each perovskite solar cell is in a strip shape, and the effective area is 4 multiplied by 4mm2(i.e., the area covered by the composite electrode); the interval between two adjacent perovskite solar cells is 1 mm;
(B5) electrolyte is dripped on the surface of an interdigital electrode of the micro super capacitor, an external lead (a strip copper foil, a strip aluminum foil, a gold wire or a silver wire can be selected for use) is respectively led out from a shared negative electrode lead and a shared positive electrode lead by utilizing conductive silver adhesive and is used for being connected with an external electrical appliance, and finally, a packaging material (PET or polyimide can be selected for use) is adopted for packaging to obtain the self-charging micro photoelectric capacitor device.
As can be seen from FIG. 4, SnO in the prepared perovskite solar cell2Barrier layer, MAPbI3The photosensitive layer, the carbon-activated carbon layer, and the RGO-PEDOT powder layer were about 0.6 μm, 1.6 μm, 70 μm, and 70 μm, respectively.
As can be seen from fig. 6, in the prepared micro supercapacitor, the width of each finger is 0.5mm, the spacing width between two adjacent fingers arranged in a crossing manner is 0.46mm, and the RGO-PEDOT having the multilayer pleat structure is uniformly adhered to the surface of the carbon-activated carbon layer to form a carbon-activated carbon @ RGO-PEDOT electrode.
The perovskite solar cell portion in the prepared photo-capacitor device was subjected to a test of a current-voltage curve, the test result being shown in fig. 5, and the open circuit voltage (V) of the prepared perovskite solar celloc) At 2.64V, short-circuit current density (J)sc) Is 5.4mA/cm2The Fill Factor (FF) was 0.44 and the Photoelectric Conversion Efficiency (PCE) was 6.31%.
Cyclic voltammetry measurements were performed on the micro supercapacitor part of the prepared photo-capacitor device, resulting in the curve in fig. 7. As can be seen from FIG. 7, the cyclic voltammetry curves of the prepared micro-supercapacitor are kept similar to rectangles at different sweep rates (0.02V/s-0.1V/s), which shows that the micro-supercapacitor has higher electrochemical stability and capacitance performance.
The constant current charge and discharge test was performed on the micro-supercapacitor part of the prepared photo-capacitor device, and from the test results of fig. 8It can be seen that the prepared micro-supercapacitors are operated at different current densities (0.4 mA/cm)2～1.2mA/cm2) The constant current charging and discharging curves of the capacitor are in a symmetrical triangular shape and almost have no voltage drop, and the good capacitance performance of the micro super capacitor is proved.
According to the curve of FIG. 8, the micro-supercapacitor can be calculated under different charging and discharging current densities (0.4 mA/cm)2～1.2mA/cm2) And plotting these data as the curves shown in fig. 9, shows that the prepared micro-supercapacitors are operated at different current densities (0.4 mA/cm)2～1.2mA/cm2) Has an energy density of 101. mu. Wh/cm2～55.2μWh/cm2The power density is 398 mu W/cm2～1200μW/cm2The area specific capacitance is 182.4mF/cm2～99.3mF/cm2。
The prepared photo-capacitor device was subjected to a photo-charge-constant current discharge test, and the test results are shown in FIG. 10, where the prepared micro-supercapacitor device was subjected to different discharge current densities (0.5 mA/cm)2～4.0mA/cm2) The photo-charging-constant current discharging curve of the micro-optical capacitor device has almost no voltage drop, and the good energy storage performance of the micro-optical capacitor device is proved.
According to the curve of FIG. 10, the micro-optical capacitor device can be calculated under different charging and discharging current densities (0.5 mA/cm)2～4.0mA/cm2) And the data were plotted as curves, as shown in fig. 11, the prepared micro-sized photo-capacitor device was operated at different discharge current densities (0.5 mA/cm)2～4.0mA/cm2) Has an energy density of 58.6. mu. Wh/cm2～40.7μWh/cm2The power density was 500. mu.W/cm2～4000μW/cm2The area specific capacitance is 105.55mF/cm2～73.30mF/cm2。
The prepared micro-optical capacitor device is placed under a sunlight simulator (the light intensity of the simulated sunlight is 100 mW/cm)2) Charging, converting light energy into electric energy by the perovskite solar cell in the standing and placing process, and connecting the perovskite solar cell with the electric energyThe micro super capacitor is charged, after charging for 1min, the electric energy in the micro super capacitor is released, and 12 red LED lamps connected in series can be lightened; two micro-optical capacitor devices are connected in series, placed under simulated sunlight and charged for 1min, and 12 white LED lamps connected in series can be lightened by the series array; two micro-optical capacitor devices are connected in parallel, placed under simulated sunlight and charged for 1min, and the parallel array can drive a fan (product name: 716 electrode; size: 7mm × 16mm × 0.8 mm; product name: AB propeller; size: 46mm) to operate.
In summary, the above description is only a preferred embodiment of the present invention, and is not intended to limit the scope of the present invention. Any modification, equivalent replacement, or improvement made within the spirit and principle of the present invention should be included in the protection scope of the present invention.
Claims (10)
1. A self-charging miniature photo-capacitor device is characterized in that: the photoelectric capacitor device comprises a micro super capacitor, a perovskite solar cell, a shared cathode lead, a shared anode lead, a series lead, a packaging material and electrolyte;
the micro super capacitor is formed by interdigital cross arrangement of two interdigital electrodes, and the interdigital electrodes are made of a gold current collector and a carbon-activated carbon layer and an RGO-PEDOT layer which are sequentially coated on the surface of the gold current collector;
the perovskite solar cell sequentially consists of conductive glass and SnO2Barrier layer, MAPbI3A photosensitive layer and a composite electrode layer; the conductive glass is glass which is etched and contains a non-conductive area and n conductive areas, each conductive area is divided into an electrode area and a battery area, each conductive area contains a perovskite solar cell, the perovskite solar cells are located in the battery areas, a composite coating of a carbon-activated carbon layer and an RGO-PEDOT layer is coated on the electrode areas, and the composite electrode layer is a composite electrode layer consisting of the carbon-activated carbon layer and the RGO-PEDOT layer;
the shared cathode lead, the shared anode lead and the series lead are all made of carbon-activated carbon layers and RGO-PEDOT layers;
the solar cell comprises a micro super capacitor, perovskite solar cells, a shared cathode lead, a shared anode lead and a series lead, wherein one interdigital electrode of the micro super capacitor is connected with a composite coating of an electrode region in one conductive region on conductive glass through the shared cathode lead, the other interdigital electrode of the micro super capacitor is connected with a composite electrode of the perovskite solar cells in the other conductive region on the conductive glass through the shared anode lead, the series lead is used for realizing the series connection of two adjacent perovskite solar cells, and the composite electrode of one perovskite solar cell is connected with the composite coating of the electrode region in the conductive region where the other perovskite solar cell is located; the electrolyte is dripped on the surface of an interdigital electrode of the micro super capacitor, and the packaging material is used for packaging the micro super capacitor, the perovskite solar cell, the shared positive electrode lead, the shared negative electrode lead and the series lead;
the conductive glass is FTO conductive glass or ITO conductive glass;
n is an integer of 1 or more; when n is 1, the optical capacitor device does not comprise a series lead, one interdigital electrode of the miniature super capacitor is connected with the composite coating in the electrode area of one conductive area on the conductive glass through a shared negative lead, and the other interdigital electrode of the miniature super capacitor is connected with the composite electrode of the perovskite solar cell in the conductive area on the conductive glass through a shared positive lead;
the thickness of the carbon-activated carbon layer is 60-100 micrometers, and the mass ratio of carbon to activated carbon in the carbon-activated carbon layer is 3: 1-5: 1; the thickness of the RGO-PEDOT layer is 50-80 μm, and the mass ratio of RGO to PEDOT in the RGO-PEDOT layer is 1: 1-1: 1.5.
2. A self-charging miniature photo-capacitor device according to claim 1 wherein: the number of the interdigital electrodes of each interdigital electrode in the micro super capacitor is 10-14, the width of each interdigital electrode is 0.45-0.6 mm, the length of each interdigital electrode is 4.8-5.0 mm, and the interval width between every two adjacent interdigital electrodes in cross arrangement is 0.45-0.5 mm.
3. A self-charging miniature photo-capacitor device according to claim 1 wherein: the thickness of the gold current collector in the micro super capacitor is 150 nm-200 nm.
4. A self-charging miniature photo-capacitor device according to claim 1 wherein: the effective area of each perovskite solar cell in the photo-capacitor device is 27mm2～48mm2And the interval between two adjacent perovskite solar cells is not more than 1.2 mm.
5. A self-charging miniature photo-capacitor device according to claim 1 wherein: the line widths of the shared anode lead and the shared cathode lead are 1 mm-1.5 mm, the line width of the series lead is equal to the width of the composite electrode on the perovskite solar cell, and the size of the electrode area is equal to the size of the composite electrode on the perovskite solar cell.
6. A self-charging miniature photo-capacitor device according to claim 1 wherein: the device comprises three perovskite solar cells connected in series, and the three perovskite solar cells are arranged in an inverted 'article' shape; correspondingly, the electrolyte is prepared from 1-ethyl-3-methylimidazolium tetrafluoroborate, poly (vinylidene fluoride-co-hexafluoropropylene) and acetone, wherein the concentration of the poly (vinylidene fluoride-co-hexafluoropropylene) in the electrolyte is 110 mg/mL-130 mg/mL, and the concentration of the 1-ethyl-3-methylimidazolium tetrafluoroborate in the electrolyte is 510 mg/mL-540 mg/mL.
7. A self-charging miniature photo-capacitor device according to claim 1 wherein: the packaging material is polyethylene terephthalate or polyimide.
8. A method of making a self-charging micro-supercapacitor device according to any one of claims 1 to 7, comprising: the steps of the method are as follows,
(1) carrying out laser etching treatment on the conductive glass to form a non-conductive area and n conductive areas; preparing SnO in each conductive region in turn2Barrier layer, MAPbI3A photosensitive layer, followed by laser etching to remove a portion of SnO2Barrier layers and MAPbI3A photosensitive layer, exposed partial conductive region is an electrode region, SnO2Barrier layers and MAPbI3The conductive area covered by the photosensitive layer is a battery area;
(2) preparing a mask plate based on the patterns of the miniature super capacitor, the shared cathode lead, the shared anode lead, the series lead and the electrode area by utilizing laser etching; preparing a gold current collector of the micro supercapacitor in a non-conductive area of conductive glass by adopting a gold spraying technology with the aid of a micro supercapacitor pattern in a mask plate, then coating carbon-activated carbon slurry on the gold current collector, and simultaneously under the aid of a shared negative electrode wire, a shared positive electrode wire, a series wire and an electrode area pattern in the mask plate, forming the non-conductive area, the electrode area and the MAPbI of the conductive glass in the non-conductive area, the electrode area and the MAPbI3Coating carbon-activated carbon slurry on the photosensitive layer, realizing the integrated connection between the miniature super capacitor and the n perovskite solar cells by coating the carbon-activated carbon slurry, coating RGO-PEDOT powder on all the carbon-activated carbon slurry coating layers, removing a mask plate, annealing at 100-120 ℃ for 40-60 min, and obtaining an integrated structure of the miniature super capacitor, the perovskite solar cells, the shared cathode lead, the shared anode lead and the series lead on conductive glass;
(3) dropping electrolyte on the surface of an interdigital electrode of the micro super capacitor, respectively leading out an external lead from a shared cathode lead and a shared anode lead for connecting with an external electric appliance, and finally packaging by adopting a packaging material to obtain the photoelectric capacitor device;
the carbon-activated carbon slurry is prepared from activated carbon and conductive carbon slurry, and the RGO-PEDOT powder is composite powder formed by depositing PEDOT on RGO foam.
9. The method of claim 8, wherein the step of forming a self-charging micro-optical capacitor device comprises: RGO-PEDOT powder was prepared by the following method,
RGO foam is used as a working electrode, a silver/silver chloride electrode is used as a reference electrode, a platinum electrode is used as a counter electrode, emulsion of 3, 4-ethylenedioxythiophene and lithium perchlorate is used as electrolyte, PEDOT is deposited on the RGO foam, and the RGO-PEDOT foam obtained after deposition is ground and sieved after being dried to obtain RGO-PEDOT powder;
wherein, the concentration of the 3, 4-ethylenedioxythiophene in the electrolyte is 14.0 mg/mL-14.5 mg/mL, the concentration of the lithium perchlorate in the electrolyte is 10.5 mg/mL-11.0 mg/mL, the voltage of the electrodeposition is 0.8V-0.9V, and the time of the electrodeposition is 150 min-170 min.
10. The method of claim 8, wherein the step of forming a self-charging micro-optical capacitor device comprises: the mask plate is made of polyimide with the thickness of 0.10-0.12 mm.
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