CN108122682B - Random-shape stacked super capacitor on same substrate and preparation method thereof - Google Patents
Random-shape stacked super capacitor on same substrate and preparation method thereof Download PDFInfo
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- CN108122682B CN108122682B CN201611057486.8A CN201611057486A CN108122682B CN 108122682 B CN108122682 B CN 108122682B CN 201611057486 A CN201611057486 A CN 201611057486A CN 108122682 B CN108122682 B CN 108122682B
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- H—ELECTRICITY
- H01—ELECTRIC ELEMENTS
- H01G—CAPACITORS; CAPACITORS, RECTIFIERS, DETECTORS, SWITCHING DEVICES OR LIGHT-SENSITIVE DEVICES, OF THE ELECTROLYTIC TYPE
- H01G11/00—Hybrid capacitors, i.e. capacitors having different positive and negative electrodes; Electric double-layer [EDL] capacitors; Processes for the manufacture thereof or of parts thereof
- H01G11/10—Multiple hybrid or EDL capacitors, e.g. arrays or modules
- H01G11/12—Stacked hybrid or EDL capacitors
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- H—ELECTRICITY
- H01—ELECTRIC ELEMENTS
- H01G—CAPACITORS; CAPACITORS, RECTIFIERS, DETECTORS, SWITCHING DEVICES OR LIGHT-SENSITIVE DEVICES, OF THE ELECTROLYTIC TYPE
- H01G11/00—Hybrid capacitors, i.e. capacitors having different positive and negative electrodes; Electric double-layer [EDL] capacitors; Processes for the manufacture thereof or of parts thereof
- H01G11/84—Processes for the manufacture of hybrid or EDL capacitors, or components thereof
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- Y—GENERAL TAGGING OF NEW TECHNOLOGICAL DEVELOPMENTS; GENERAL TAGGING OF CROSS-SECTIONAL TECHNOLOGIES SPANNING OVER SEVERAL SECTIONS OF THE IPC; TECHNICAL SUBJECTS COVERED BY FORMER USPC CROSS-REFERENCE ART COLLECTIONS [XRACs] AND DIGESTS
- Y02—TECHNOLOGIES OR APPLICATIONS FOR MITIGATION OR ADAPTATION AGAINST CLIMATE CHANGE
- Y02E—REDUCTION OF GREENHOUSE GAS [GHG] EMISSIONS, RELATED TO ENERGY GENERATION, TRANSMISSION OR DISTRIBUTION
- Y02E60/00—Enabling technologies; Technologies with a potential or indirect contribution to GHG emissions mitigation
- Y02E60/13—Energy storage using capacitors
Abstract
The invention discloses an arbitrarily-shaped stacked super capacitor on the same substrate and a preparation method thereof. The preparation method comprises the steps of spraying and manufacturing a lower electrode thin film layer with any shape on the same substrate, then spraying and manufacturing a graphene oxide diaphragm layer on the lower electrode thin film, and then manufacturing an upper electrode thin film layer on the diaphragm layer to obtain the super capacitor with a stacked structure. The stacked super capacitor with any shape manufactured by the invention can realize shape control and large-scale production, can be effectively compatible and integrated with different flexible, portable and wearable electronic devices, and has wide market application prospect.
Description
Technical Field
The invention belongs to the field of manufacturing of super capacitors, and particularly relates to a stacked super capacitor with any shape on the same substrate and a preparation method thereof.
Background
The conventional stacked supercapacitor is constructed by stacking in the form of current collector (substrate)/positive electrode/separator/negative electrode/current collector (substrate). The stack-type super capacitor with the structural form takes long time to manufacture, the process is complex, and the structural form involves two substrates; the current collector and the electrode material are not integrated, so that the volume of the traditional stacked super capacitor is large, and the application of the traditional stacked super capacitor in a miniaturized integrated circuit is not facilitated.
With the rapid development of light, thin and bendable electronic equipment with various shapes, the demand of people on novel energy storage devices is greatly stimulated. Current energy storage devices, such as lithium batteries and supercapacitors, are fixed in shape, large in size and heavy in weight, and are difficult to meet the requirements of flexible electronic equipment. Furthermore, conventional power supplies do not allow for shape-controlled flexible energy storage devices due to structural design and performance limitations, such as the need for polymer binders and additional conductive agents, as well as thick membranes.
In order to overcome the above difficulties, in recent years, planar interdigital graphene-based energy storage devices have attracted extensive attention and are considered to be promising for application on miniature electronic chips. The planar structure enables the electrode, the diaphragm, the electrolyte and the current collector to be integrated on the same substrate, and is beneficial to combination of all components and shape design of the energy storage device. Although planar supercapacitors of various shapes can be manufactured using a variety of techniques, such as printing, photolithographic development, laser etching, the manufacture of supercapacitors of arbitrary shapes cannot be achieved.
Disclosure of Invention
Aiming at the problems, the invention aims to manufacture the super capacitor with the stacking structure in any shape on the same substrate by adopting a spraying method, and has the advantages of simple manufacturing process, low cost and wide market application prospect.
In order to achieve the purpose, the invention adopts the technical scheme that:
a stacking type super capacitor with any shape on the same substrate is a stacking type super capacitor with any shape, wherein a first layer of electrode film/a second layer of diaphragm/a third layer of electrode film/solid electrolyte are sequentially stacked on a substrate;
the first layer of electrode film and the third layer of electrode film are made of the following materials: graphene or a graphene composite;
the diaphragm is graphene oxide;
the solid electrolyte is polyvinyl alcohol/sulfuric acid (PVA/H)2SO4) Polyvinyl alcohol/sodium sulfate (PVA/Na)2SO4) And 1-butyl-3-methylimidazolium tetrafluoroborate/silicon dioxide solid electrolyte.
The substrate comprises any insulating plane substrate such as a polyethylene terephthalate substrate (PET), Polyetherimide (PEI), a silicon wafer, glass, paper or wood board and the like.
The thickness of the electrode film is 0.1-5 μm, and the thickness of the diaphragm is 1-3 μm.
The first layer electrode material and the third layer electrode material film electrode can be the same electrode material or different electrode materials.
The first layer of electrode material and the third layer of electrode material are the same electrode material, and the supercapacitor is a symmetrical supercapacitor; the first layer of electrode material and the third layer of electrode material are different electrode materials, and the super capacitor is an asymmetric super capacitor.
The certain shape described in the present invention may be any shape, which is not limited by the size, configuration, and dimension of the device;
the two electrode materials, the diaphragm, the electrolyte and the current collector are integrated on the same substrate.
A preparation method of a stacked supercapacitor in any shape on the same substrate specifically comprises the following steps:
(1) spraying graphene ink on a substrate through a template 1 with a certain shape to manufacture a first layer of film electrode with a certain shape, wherein the electrode layer serves as a current collector and also serves as an active substance;
(2) spraying graphene oxide ink on the first layer of thin film electrode through the template 2 with the same shape to prepare a second layer of diaphragm with the same shape, ion conduction and electronic insulation;
(3) spraying graphene ink on the second diaphragm layer through the template 1 with the same shape to prepare a third film electrode with the same shape, and forming a counter electrode with the first film electrode;
(4) and finally, adding the solid electrolyte with the same shape on the surface of the electrode material/diaphragm/electrode material structure with a certain shape to prepare the stacked supercapacitor with any shape.
The graphene ink in the step (1) is graphene dispersed in dispersion liquid, and the concentration of the graphene ink is 0.05-10mg mL-1；
The graphene in the graphene ink is one or more of electrochemical stripping graphene, reduced graphene oxide, liquid-phase stripping graphene, chemical vapor deposition graphene and graphene composite materials;
the dispersion is one of isopropanol, N-Dimethylformamide (DMF), and N-methylpyrrolidone (NMP).
The width of the template 2 described in the present invention is larger than the template 1 to 10 μm to 1000 μm.
The size of the graphene oxide is 0.1-100 mu m, and the thickness of the graphene oxide is 0.7-2.0 nm; the concentration is 0.5-8mg mL-1。
The spraying manufacturing method comprises mechanical spraying and electrostatic spraying.
The diameter of the spraying nozzle of the spraying device is 0.2-1.0mm, the gas used for spraying is one of nitrogen, argon or air, and the pressure of the spraying gas is 0.01-0.3M Pa.
The invention discloses a method for manufacturing a supercapacitor in any shape on the same substrate, which is used for manufacturing the supercapacitor in a stacking structure in any shape on the same substrate by adopting a spraying method. Specifically, a lower electrode thin film layer with any shape is manufactured on the same substrate in a spraying mode, then a graphene oxide diaphragm layer is manufactured on the lower electrode thin film in a spraying mode, then an upper electrode thin film layer is manufactured on the diaphragm layer, and the super capacitor with the stacked structure is obtained. The manufacturing process is simple, the cost is low, the shape can be controlled, the large-scale production can be realized, the device can be effectively compatible and integrated with different types of flexible, portable and wearable electronic devices, and the device has wide market application prospect.
Features and advantages of the invention
1. The invention discloses a stacked super capacitor with any shape manufactured on the same substrate, which is structurally composed of a substrate/an electrode/a diaphragm/an electrode; the electrodes and the diaphragm are integrated, and the manufacture of the supercapacitor in any shape can be realized.
2. The stacked super capacitor with any shape is manufactured on the same substrate, the shape, the size, the dimension and the thickness of a device can be easily controlled, the required equipment is simple, only one substrate is involved, and the stacked super capacitor with any shape has the characteristic of simple manufacturing process.
3. The stacked supercapacitor manufactured on the same substrate in any shape is manufactured on a flexible substrate, can be effectively compatible and integrated with different flexible, portable and wearable electronic devices, and has wide market application prospect.
Drawings
FIG. 1 is a schematic diagram of a stacked super capacitor having an arbitrary shape represented by a cross-point line type fabricated on the same substrate.
FIG. 2. example of manufacturing an arbitrary shaped supercapacitor by spray coating: cyclic voltammograms with cross-point linear supercapacitors and different scan rates.
FIG. 3. example of manufacturing an arbitrary shaped supercapacitor by spray coating: has a hollow square super capacitor.
Detailed Description
Example 1
Electrochemically exfoliated graphene (0.1mg mL) dispersed in isopropanol-1) And graphene oxide aqueous solution (1mg mL)-1) As a raw material, the average size of graphene oxide in this embodiment is 100nm, and the spray substrate is PET; spraying a graphene electrode layer with the thickness of 100nm through a cross-point linear template 1 (shown in figure 1), wherein the caliber diameter of a sprayed pen is 0.3mm, the pressure of sprayed nitrogen is 0.05MPa, and removing the template 1 to obtain one pole of the cross-point linear supercapacitor; then spraying a graphene oxide aqueous solution by using a 0.2mm spray pen through a cross-point linear template 2 (shown in figure 1), wherein the thickness of a graphene oxide diaphragm layer is 1.5 mu M, the pressure of spraying nitrogen is 0.1M Pa, and removing the template 2; spraying another electrode with the same thickness on the graphene oxide diaphragm layer through the cross-point linear template 1 by using a 0.3mm spray pen; then injecting PVA/H2SO4And then packaging; thus obtaining the cross-point linear symmetrical super capacitor (figure 2).
Electrochemical tests show that the voltage window of the obtained cross-point linear supercapacitor is 0.8V, and the sweep rate in cyclic voltammetry is 2mV s-1When the specific volume of the electrode surface is 0.88mF cm-2。
Example 2
Electrochemically exfoliated graphene (0.5mg mL) dispersed in isopropanol-1) And graphene oxide aqueous solution (1.5mg mL)-1) As a raw material, graphene oxide in the present example has an average size of 1 μm, and a substrate is sprayedIs PET; spraying a graphene electrode layer with the thickness of 170nm through a hollow square template 1, wherein the caliber diameter of a sprayed pen is 0.5mm, the pressure of spraying nitrogen is 0.2MPa, and removing the template 1 to obtain one electrode of the hollow square supercapacitor; then spraying a graphene oxide aqueous solution through a hollow square template 2 by using a 0.3mm spray pen, wherein the thickness of a graphene oxide diaphragm layer is 1 mu M, the pressure of spraying nitrogen is 0.1M Pa, and removing the template 2; spraying the other electrode with the same thickness on the graphene oxide diaphragm layer through a hollow square template 1 by using a 0.5mm spray pen; then injecting PVA/H2SO4And then packaging; thus obtaining the hollow square symmetrical super capacitor (figure 3).
Electrochemical tests show that the voltage window of the obtained hollow square supercapacitor is 0.8V, and the scanning rate of the hollow square supercapacitor in cyclic voltammetry is 2mV s-1When the specific volume of the electrode surface is 1.2mF cm-2。
Example 3
To reduced graphene oxide dispersed in isopropanol (2mg mL)-1) And graphene oxide aqueous solution (4mg mL)-1) As a raw material, the average size of graphene oxide in this embodiment is 1 μm, and the spray substrate is PET; spraying a graphene electrode layer with the thickness of 1 mu m through an A-shaped template 1, wherein the diameter of the caliber of a sprayed pen is 0.3mm, the pressure of sprayed nitrogen is 0.1MPa, and removing the template 1 to obtain one pole of the A-shaped supercapacitor; then spraying a graphene oxide aqueous solution by using a 0.3mm spray pen through an A-shaped template 2, wherein the thickness of a graphene oxide diaphragm layer is 2 microns, the pressure of spraying nitrogen is 0.1M Pa, and removing the template 2; spraying another electrode with the same thickness on the graphene oxide diaphragm layer through the letter A-shaped template 1 by using a 0.3mm spray pen; then injecting PVA/H2SO4And then packaging; thus obtaining the letter 'A' -shaped symmetrical super capacitor.
Electrochemical tests show that the voltage window of the obtained super capacitor with the letter 'A' is 0.8V, and the scanning rate of the super capacitor in cyclic voltammetry is 2mV s-1When the specific volume of the electrode surface is 8.9mF cm-2。
Example 4
As a solution dispersed in DMFPhase-exfoliated graphene (1.5mg mL)-1) And graphene oxide aqueous solution (6mg mL)-1) As a raw material, the average size of graphene oxide in this embodiment is 100nm, and the spray substrate is PET; spraying a graphene electrode layer with the thickness of 5 microns through a digital 1-shaped template 1, wherein the diameter of the caliber of a sprayed pen is 0.3mm, the pressure of sprayed nitrogen is 0.2MPa, and removing the template 1 to obtain one pole of the digital 1-shaped supercapacitor; then spraying a graphene oxide aqueous solution by using a 0.3mm spray pen through a digital 1-shaped template 2, wherein the thickness of a graphene oxide diaphragm layer is 3 mu M, the pressure of spraying nitrogen is 0.1M Pa, and removing the template 2; spraying another electrode with the same thickness on the graphene oxide diaphragm layer through a digital 1-shaped template 1 by using a 0.3mm spray pen; then injecting PVA/H2SO4And then packaging; and obtaining the digital 1-shaped symmetrical super capacitor.
Electrochemical tests show that the voltage window of the obtained digital 1-shaped supercapacitor is 0.8V, and the sweep rate in cyclic voltammetry is 2mV s-1When the specific volume of the electrode surface is 7.1mF cm-2。
Example 5
Electrochemically exfoliated graphene (10mg mL) dispersed in NMP-1) And graphene oxide aqueous solution (3mg mL)-1) As a raw material, the average size of graphene oxide in this example is 1 μm, and the spray substrate is paper; spraying a graphene electrode layer with the thickness of 2 microns through a digital 1-shaped template 1, wherein the diameter of the caliber of a sprayed pen is 0.3mm, the pressure of sprayed nitrogen is 0.1MPa, and removing the template 1 to obtain one pole of the digital 1-shaped supercapacitor; then spraying a graphene oxide aqueous solution by using a 0.5mm spray pen through a digital 1-shaped template 2, wherein the thickness of a graphene oxide diaphragm layer is 3 mu M, the pressure of spraying nitrogen is 0.1M Pa, and removing the template 2; spraying another electrode with the same thickness on the graphene oxide diaphragm layer by using a 0.3mm spray pen through a digital 1-shaped template 3; then injecting PVA/H2SO4And then packaging; and obtaining the digital 1-shaped symmetrical super capacitor.
Electrochemical tests show that the voltage window of the obtained digital 1-shaped supercapacitor is 0.8V, and the scanning speed is tested in cyclic voltammetryThe ratio is 2mV s-1When the specific volume of the electrode surface is 13.6mF cm-2。
Example 6
Electrochemically exfoliated graphene (2mg mL) dispersed in isopropanol-1) And graphene oxide aqueous solution (3mg mL)-1) As a raw material, the average size of graphene oxide in this embodiment is 100nm, and the spray substrate is a silicon wafer; spraying a graphene electrode layer with the thickness of 700nm through an A-shaped template 1, wherein the diameter of the caliber of a sprayed pen is 0.3mm, the pressure of sprayed nitrogen is 0.1MPa, and removing the template 1 to obtain one pole of the A-shaped supercapacitor; then spraying a graphene oxide aqueous solution through an A-shaped template 2 by using a 0.2mm spray pen, wherein the thickness of a graphene oxide diaphragm layer is 1 mu M, the pressure of spraying nitrogen is 0.1M Pa, and removing the template 2; spraying another electrode with the same thickness on the graphene oxide diaphragm layer through the letter A-shaped template 1 by using a 0.3mm spray pen; then injecting PVA/Na2SO4And then packaging; thus obtaining the letter 'A' -shaped symmetrical super capacitor.
Electrochemical tests show that the voltage window of the obtained super capacitor with the letter 'A' is 0.8V, and the scanning rate of the super capacitor in cyclic voltammetry is 2mV s-1When the specific volume of the electrode surface is 6.4mF cm-2。
Example 7
With graphene/polyaniline composite dispersed in isopropanol (0.5mg mL)-1) Electrochemically exfoliated graphene dispersed in isopropanol (1mg mL)-1) And graphene oxide aqueous solution (3mg mL)-1) As a raw material, the average size of graphene oxide in this embodiment is 100nm, and the spray substrate is PET; spraying a graphene/polyaniline composite material electrode layer with the thickness of 1 mu m through a square template 1, wherein the diameter of the caliber of a sprayed pen is 0.5mm, the pressure of sprayed nitrogen is 0.15MPa, and removing the template 1 to obtain one pole of the square super capacitor; then spraying a graphene oxide aqueous solution through a square template 2 by using a 0.2mm spray pen, wherein the thickness of a graphene oxide diaphragm layer is 2 mu M, the pressure of spraying nitrogen is 0.1M Pa, and removing the template 2; then spraying the electrochemical film with the thickness of 2 microns on the graphene oxide diaphragm layer by using a 0.5mm spray pen through a square template 1Chemically stripping the graphene electrode to form an asymmetric supercapacitor, and then injecting PVA/H2SO4And then packaging; and obtaining the square asymmetric super capacitor.
Electrochemical tests show that the voltage window of the obtained square supercapacitor is 1.4V, and the sweep rate in cyclic voltammetry is 10mV s-1When the specific volume of the electrode surface is 15.8mF cm-2。
Example 8
Electrochemically exfoliated graphene (0.3mg mL) dispersed in isopropanol-1) And graphene oxide aqueous solution (1.5mg mL)-1) As a raw material, the average size of graphene oxide in this embodiment is 100nm, and the spray substrate is PET; spraying an electrochemical stripping graphene electrode layer with the thickness of 1 mu m through a square template 1, wherein the diameter of the caliber of a sprayed pen is 0.5mm, the pressure of sprayed nitrogen is 0.15MPa, and removing the template 1 to obtain one electrode of the square supercapacitor; then spraying a graphene oxide aqueous solution through a square template 2 by using a 0.2mm spray pen, wherein the thickness of a graphene oxide diaphragm layer is 2 mu M, the pressure of spraying nitrogen is 0.1M Pa, and removing the template 2; spraying an electrochemical stripping graphene electrode with the thickness of 1 mu m on the graphene oxide diaphragm layer through a square template 1 by using a 0.5mm spray pen, then injecting 1-butyl-3-methylimidazolium tetrafluoroborate/silicon dioxide electrolyte, and then packaging; and obtaining the square symmetrical super capacitor.
Electrochemical tests show that the voltage window of the obtained square supercapacitor is 3V, and the sweep rate in cyclic voltammetry is 50mV s-1When the specific volume of the electrode surface is 1.2mF cm-2。
Claims (7)
1. The stacked super capacitor is characterized in that the stacked super capacitor is formed by sequentially integrating a first layer of electrode film/a second layer of diaphragm/a third layer of electrode film/solid electrolyte on a substrate;
the first layer of electrode film and the third layer of electrode film are made of the following materials: graphene or a graphene composite;
the diaphragm is graphene oxide;
the solid electrolyte is one of polyvinyl alcohol/sulfuric acid, polyvinyl alcohol/sodium sulfate and 1-butyl-3-methylimidazole tetrafluoroborate/silicon dioxide solid electrolyte;
the thickness of the electrode film is 0.1-5 μm, and the thickness of the diaphragm is 1-3 μm;
the specific preparation method of the super capacitor comprises the following steps:
(1) spraying graphene ink on a substrate through a template 1 with a certain shape to manufacture a first layer of thin film electrode with the shape, wherein the electrode layer is used as a current collector and an active substance;
the graphene ink is graphene dispersed in dispersion liquid, and the concentration of the graphene ink is 0.05-10mg mL-1(ii) a The graphene is one or more of electrochemical stripping graphene, reduced graphene oxide, liquid phase stripping graphene, chemical vapor deposition graphene or graphene composite materials; the dispersion is one of isopropanol, N-Dimethylformamide (DMF) or N-methylpyrrolidone (NMP);
(2) spraying water-based graphene oxide ink on the first layer of the thin film electrode through the template 2 with the same shape to prepare a second layer of the diaphragm with the same shape, ion conduction and electronic insulation; the size of the graphene oxide is 0.1-100 mu m, and the thickness of the graphene oxide is 0.7-2.0 nm; the concentration is 0.5-8mg mL-1The solvent is water;
(3) spraying graphene ink on the second diaphragm layer through the template 1 with the same shape to prepare a third film electrode with the same shape, and forming a counter electrode with the first film electrode;
(4) finally, adding solid-state water-based electrolyte with the same shape to an electrode material/diaphragm/electrode material structure with a certain shape to prepare a stacked super capacitor with any shape;
the specific parameters of the spraying are as follows: the diameter of the nozzle is 0.2-1.0mm, the spraying gas is one of nitrogen, argon or air, and the pressure of the spraying gas is 0.01-0.3M Pa.
2. The stacked-type supercapacitor of arbitrary shape on the same substrate according to claim 1, wherein: the substrate comprises a polyethylene terephthalate substrate (PET), Polyetherimide (PEI), a silicon wafer, glass, paper or a wood board.
3. The method for preparing the random-shaped stacked supercapacitor as claimed in claim 1, which is characterized by comprising the following steps:
(1) spraying graphene ink on a substrate through a template 1 with a certain shape to manufacture a first layer of thin film electrode with the shape, wherein the electrode layer is used as a current collector and an active substance;
the graphene ink is graphene dispersed in dispersion liquid, and the concentration of the graphene ink is 0.05-10mg mL-1(ii) a The graphene is one or more of electrochemical stripping graphene, reduced graphene oxide, liquid phase stripping graphene, chemical vapor deposition graphene or graphene composite materials; the dispersion is one of isopropanol, N-Dimethylformamide (DMF) or N-methylpyrrolidone (NMP);
(2) spraying water-based graphene oxide ink on the first layer of the thin film electrode through the template 2 with the same shape to prepare a second layer of the diaphragm with the same shape, ion conduction and electronic insulation; the size of the graphene oxide is 0.1-100 mu m, and the thickness of the graphene oxide is 0.7-2.0 nm; the concentration is 0.5-8mg mL-1The solvent is water;
(3) spraying graphene ink on the second diaphragm layer through the template 1 with the same shape to prepare a third film electrode with the same shape, and forming a counter electrode with the first film electrode;
(4) finally, adding solid-state water-based electrolyte with the same shape to an electrode material/diaphragm/electrode material structure with a certain shape to prepare a stacked super capacitor with any shape;
the specific parameters of the spraying are as follows: the diameter of the nozzle is 0.2-1.0mm, the spraying gas is one of nitrogen, argon or air, and the pressure of the spraying gas is 0.01-0.3M Pa.
4. The stacked-type supercapacitor of arbitrary shape on the same substrate according to claim 1, wherein: the width of the template 2 is 10-1000 mu m larger than that of the template 1.
5. The method for preparing an arbitrarily shaped stacked supercapacitor according to claim 3, wherein: the width of the template 2 is 10-1000 mu m larger than that of the template 1.
6. The method for preparing an arbitrarily shaped stacked supercapacitor according to claim 3, wherein: the spraying method comprises mechanical spraying or electrostatic spraying.
7. The stacked-type supercapacitor of arbitrary shape on the same substrate according to claim 1, wherein: the spraying method comprises mechanical spraying or electrostatic spraying.
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| CN101162650A (en) * | 2007-05-29 | 2008-04-16 | 中南大学 | Flexible thin film type solid-state super capacitor and its manufacture process |
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