CN108695074A - A kind of graphene ultracapacitor and preparation method thereof - Google Patents
A kind of graphene ultracapacitor and preparation method thereof Download PDFInfo
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- CN108695074A CN108695074A CN201810029819.9A CN201810029819A CN108695074A CN 108695074 A CN108695074 A CN 108695074A CN 201810029819 A CN201810029819 A CN 201810029819A CN 108695074 A CN108695074 A CN 108695074A
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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
-
- 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
- H01G11/22—Electrodes
- H01G11/26—Electrodes characterised by their structure, e.g. multi-layered, porosity or surface features
- H01G11/28—Electrodes characterised by their structure, e.g. multi-layered, porosity or surface features arranged or disposed on a current collector; Layers or phases between electrodes and current collectors, e.g. adhesives
-
- 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
- H01G11/22—Electrodes
- H01G11/30—Electrodes characterised by their material
- H01G11/32—Carbon-based
- H01G11/36—Nanostructures, e.g. nanofibres, nanotubes or fullerenes
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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
- H01G11/66—Current collectors
- H01G11/72—Current collectors specially adapted for integration in multiple or 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
-
- 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
- H01G11/86—Processes for the manufacture of hybrid or EDL capacitors, or components thereof specially adapted for electrodes
-
- 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 present invention relates to the preparation field of electronic component, more particularly to a kind of graphene ultracapacitor and preparation method thereof.The graphene ultracapacitor includes capacitor body, and the capacitor body includes multiple monomer capacitances and interior lug, wherein is connected in series or in parallel by interior lug between adjacent monomer capacitance in the multiple monomer capacitance;Two outer lugs;And outer packing.The preparation method of the graphene ultracapacitor includes:(1) thin polymer film substrate is fixed on base material;(2) CO is used2Infrared laser irradiates thin polymer film substrate, obtains patterned graphene anode, graphene cathode and interior lug;(3) graphene anode, graphene cathode and interior lug are cut out;(4) coating electrolyte forms multiple monomer capacitances, wherein being connected by interior lug between adjacent monomer capacitance in the multiple monomer capacitance;(5) it is disposably encapsulated after outer lug being installed, obtains graphene ultracapacitor.
Description
Technical field
The present invention relates to the preparation field of electronic component, more particularly to a kind of graphene ultracapacitor and its preparation side
Method.
Background technology
Ultracapacitor is a kind of a kind of novel energy storage apparatus between physical capacitor and secondary cell.This dress
Set its energy savings and release during it is unique, be not only presented as burst rate charge and discharge process, while also having
There are the advantages of high-energy and high-specific-power, i.e. charge and discharge time only tens of seconds, power density to be higher by 10- compared with accumulator
100 times;Energy density is then as many as 100 times of physical capacitor.
The active material of capacitor is generally powder body material, and electrode is by matching powder body material, conductive agent and binder etc.
At after slurry coated in preparing in conductive substrates.Also there is the specific shape that preparation is combined using mask and spraying technology
Electrode method, but the technique for substantially still falling within slurry.
Occur preparing the new method of Graphene electrodes using laser irradiation in the recent period.Since graphene is a kind of former by carbon
Son is arranged according to hexagon and carbon molecules made of being connected with each other, and structure is highly stable, and with high conductivity, high-ductility
The features such as degree, high intensity, extra specific surface area so that the ultracapacitor using graphene as electrode material shows excellent
Performance is more suitable for the storage of energy.
In order to adjust capacity and the pressure resistance of capacitor module, generally realized by the series/parallel of capacitor.And it goes here and there
Connection/parallel way can substantially be divided into external monomer series-connected/in parallel and internal monomer series-connected/two kinds in parallel again.External series
It operates fairly simple, it is only necessary to the positive and negative anodes of addition monomers are subjected to corresponding serial/parallel connection, and internal series-connection is then
It is directly to form serial/parallel connection in internal structure before packaging during capacitor fabrication, disposable progress is outer later
Encapsulation.In contrast, internal series/parallel only need to be encapsulated once, save partial encapsulation material and lug.
However, the graphene ultracapacitor for being prepared internal series/parallel using laser irradiation at present is but rarely reported.
Invention content
In order to solve the above technical problem, the present invention provides a kind of graphene ultracapacitors and preparation method thereof.
According to an aspect of the invention, there is provided a kind of graphene ultracapacitor, including:
Capacitor body, the capacitor body include multiple monomer capacitances and interior lug;
Wherein, it is connected in series with by interior lug between adjacent monomer capacitance in the multiple monomer capacitance, the monomer electricity
Appearance includes graphene anode, graphene cathode and electrolyte, and the graphene anode of the monomer capacitance and the first adjacent monomer are electric
The graphene cathode of appearance by interior lug integrally connected, the graphene cathode of the monomer capacitance and the second adjacent monomer capacitance
Graphene anode passes through interior lug integrally connected;
Two outer lugs, described two outer lugs are connected with head end monomer capacitance and tail end monomer capacitance respectively;And
Outer packing, the outer packing is for being packaged the capacitor body.
Optionally, the electrolyte is colloidal electrolyte.
Optionally, the electrolyte includes PVA/ sulfuric acid, PVA/ hydrochloric acid or PVA/ phosphoric acid.
Optionally, the graphene anode, graphene cathode and interior lug are by the same thin polymer film of laser irradiation
What the surface of substrate was formed.
Optionally, the thin polymer film substrate is Kapton or polyetherimide film.
Optionally, interdigitated, parallel strip, helical form or combinations thereof shape is presented in the graphene anode and graphene cathode
Any one of shape.
Optionally, the distance between the graphene anode and graphene cathode are 0.1-0.5mm.
Optionally, the distance between the graphene anode and graphene cathode are 0.2mm.
According to another aspect of the present invention, a kind of graphene ultracapacitor is provided, including:
Capacitor body, the capacitor body include multiple monomer capacitances and interior lug, wherein the multiple monomer electricity
It is connected in parallel by interior lug between adjacent monomer capacitance in appearance, the monomer capacitance includes graphene anode, graphene cathode
And electrolyte, the graphene anode of the monomer capacitance and the graphene anode of adjacent monomer capacitance are integrally connected by interior lug
It connects, the graphene cathode of the monomer capacitance and the graphene cathode of adjacent monomer capacitance pass through interior lug integrally connected;
Two outer lugs, described two outer lugs are connected with head end monomer capacitance and tail end monomer capacitance respectively;And
Outer packing, the outer packing is for being packaged the capacitor body.
Optionally, the graphene anode, graphene cathode and interior lug are by the same thin polymer film of laser irradiation
What the surface of substrate was formed.
Optionally, the thin polymer film substrate is Kapton or polyetherimide film.
Optionally, interdigitated, parallel strip, helical form or combinations thereof shape is presented in the graphene anode and graphene cathode
Any one of shape.
According to another aspect of the present invention, a kind of graphene ultracapacitor, including capacitor body, the electricity are provided
Vessel is the combination of the first capacitor body and the second capacitor body;
Wherein, the first capacitor body includes multiple monomer capacitances and interior lug;Adjacent list in the multiple monomer capacitance
It is connected in series with by interior lug between body capacitance, the monomer capacitance includes graphene anode, graphene cathode and electrolyte, institute
The graphene cathode of the graphene anode and the first adjacent monomer capacitance of stating monomer capacitance passes through interior lug integrally connected, the list
The graphene anode of the graphene cathode of body capacitance and the second adjacent monomer capacitance passes through interior lug integrally connected;
Wherein, the second capacitor body includes multiple monomer capacitances and interior lug;Wherein, phase in the multiple monomer capacitance
It is connected in parallel by interior lug between adjacent monomer capacitance, the monomer capacitance includes graphene anode, graphene cathode and electrolysis
Liquid, the graphene anode of the monomer capacitance and the graphene anode of adjacent monomer capacitance are described by interior lug integrally connected
The graphene cathode of monomer capacitance and the graphene cathode of adjacent monomer capacitance pass through interior lug integrally connected.
According to another aspect of the present invention, a kind of preparation method of graphene ultracapacitor is provided, including:
(1) thin polymer film substrate is fixed on base material;
(2) CO is used2Infrared laser irradiates thin polymer film substrate, obtains patterned graphene anode, graphene
Cathode and interior lug;
(3) graphene anode, graphene cathode and interior lug are cut out;
(4) coating electrolyte forms multiple monomer capacitances, wherein in the multiple monomer capacitance between adjacent monomer capacitance
It is connected by interior lug;
(5) it is disposably encapsulated after outer lug being installed, obtains graphene ultracapacitor.
Optionally, wherein patterned graphene anode, graphene cathode and interior lug include single described in step (2)
The graphene cathode of the graphene anode of body capacitance and the first adjacent monomer capacitance by interior lug integrally connected, monomer capacitance
The graphene anode of graphene cathode and the second adjacent monomer capacitance passes through interior lug integrally connected.
Optionally, wherein patterned graphene anode, graphene cathode and interior lug include single described in step (2)
The graphene anode of body capacitance and the graphene anode of adjacent monomer capacitance pass through interior lug integrally connected, the graphite of monomer capacitance
The graphene cathode of alkene cathode and adjacent monomer capacitance passes through interior lug integrally connected.
Optionally, the thin polymer film substrate is Kapton or polyetherimide film.
Optionally, the CO2The power of infrared laser is 2-10mW, and it is 1-5mm/s that laser, which sweeps speed,.
Optionally, the CO2The power of infrared laser is 3mW, and it is 2mm/s that laser, which sweeps speed,.
The present invention prepares graphene using laser irradiation, introduces the structure of internal series/parallel to realize capacitor module
Capacity regulating.Compared with prior art, the present invention has the advantages that:
1. preparing Graphene electrodes without slurry feedstocks such as additional conductive agent, adhesives;
2. being not necessarily to additional diaphragm and interior lug, Graphene electrodes are integrally formed simultaneously with interior lug;
3. prepared by electrode and capacitor package technique relatively coating and mask plate technique significantly simplify, it is readily produced.
Description of the drawings
Fig. 1 shows the structural schematic diagram of graphene ultracapacitor;
Fig. 2 shows the graphene ultracapacitors of internal series-connection provided in an embodiment of the present invention to remove the knot after outer packing
Structure schematic diagram;
Wherein, 11 be outer lug, and 12 be electrolyte, and 13 be Graphene electrodes, and 14 be interior lug;
Fig. 3 shows the knot after the graphene ultracapacitor removal outer packing of internal series-connection provided in an embodiment of the present invention
Structure material object photo;
Fig. 4 shows the structural schematic diagram of the graphene ultracapacitor of internal parallel provided in an embodiment of the present invention;
Fig. 5 shows the knot after the graphene ultracapacitor removal outer packing of internal parallel provided in an embodiment of the present invention
Structure schematic diagram;
Wherein, 21 be outer lug, and 22 be electrolyte, and 23 be Graphene electrodes, and 24 be interior lug;
Fig. 6 shows the structural representation of the graphene ultracapacitor of internal series-connection-parallel connection provided in an embodiment of the present invention
Figure;
Fig. 7 shows the preparation method flow chart of graphene ultracapacitor provided in an embodiment of the present invention;
Fig. 8 shows the preparation method flow of the graphene ultracapacitor of internal series-connection provided in an embodiment of the present invention
Figure;
Fig. 9 shows the preparation method flow of the graphene ultracapacitor of internal parallel provided in an embodiment of the present invention
Figure;
Figure 10 shows the preparation of the graphene ultracapacitor of internal series-connection-parallel combination provided in an embodiment of the present invention
Method flow diagram;
Figure 11 shows the charge and discharge data of the graphene ultracapacitor of internal series-connection provided in an embodiment of the present invention;With
And
Figure 12 shows the charge and discharge data of the graphene ultracapacitor of non-internal series-connection.
Specific implementation mode
To fully understand the purpose, feature and effect of the present invention, by following specific implementation modes, the present invention is done in detail
Illustrate, but the present invention is not restricted to this.
According to an aspect of the present invention, a kind of graphene ultracapacitor is provided, as shown in Figure 1, including:
Capacitor body 101, the capacitor body include multiple monomer capacitances 102 and interior lug 103;
Wherein, it is connected in series with by interior lug 103 between adjacent monomer capacitance 102 in the multiple monomer capacitance, it is described
Monomer capacitance 102 includes graphene anode, graphene cathode and electrolyte, the graphene anode of the monomer capacitance 102 and the
For the graphene cathode of one adjacent monomer capacitance 102 by 103 integrally connected of interior lug, the graphene of the monomer capacitance 102 is negative
The graphene anode of pole and the second adjacent monomer capacitance 102 is connected by interior lug one 103;
Two outer lugs 104, described two outer lugs 104 respectively with head end monomer capacitance 102 and tail end monomer capacitance 102
It is connected;And
Outer packing 105, the outer packing is for being packaged the capacitor body.
Further, the electrolyte is colloidal electrolyte.The electrolyte be preferably PVA/ sulfuric acid, PVA/ hydrochloric acid or
It is one or more in PVA/ phosphoric acid.It on the one hand can ensure that electrolyte is adhesively fixed in graphene electricity using the colloidal electrolyte
Polar region domain prevents electrolyte flow to interior lug position, on the other hand eliminates additional diaphragm, simplifies preparation process.This field
Technical staff can also be by reasonably attempting that other kinds of electrolyte, the present invention is used to be not especially limited this.
Wherein, graphene anode, graphene cathode and the interior lug 103 of the monomer capacitance 102 are to pass through laser irradiation
What the surface of same thin polymer film substrate was formed.The graphene ultracapacitor of the present invention, without additional interior lug connection
Technique.
More preferred, the thin polymer film substrate is Kapton or polyetherimide film.Through CO2It is infrared
The irradiation of laser, the thin polymer film substrate surface form porous graphene.Wherein, the carbon atom structure of porous graphene
At micron order or nano level pentagon-heptagon polycrystalline lattice, be connected with each other between lattice, have extra specific surface area, compared with
The features such as good electric conductivity and electrochemical stability, therefore the porous graphene that the thin polymer film substrate surface is formed was both
It can be used as capacitor electrode material, interior lug is can also be used as and use, greatly improve the chemical property of capacitor.
Further, interdigitated, parallel strip, helical form or combinations thereof is presented in the graphene anode and graphene cathode
Any one of shape.
More preferred, the shape of the graphene anode and graphene cathode is interdigitated.Using the graphite of interdigitated
Alkene electrode can increase the unilateral effective area of electrode, to increase the capacitance of graphene ultracapacitor.
Further, the distance between graphene anode and graphene cathode are 0.1-0.5mm in the monomer capacitance, excellent
Choosing, the distance between the graphene anode and graphene cathode are 0.2mm.If spacing is too small, graphene electricity is easily caused
The short circuit of interpolar, spacing is excessive, then is unfavorable for the migration of ion between the electrodes, increases the charge and discharge of graphene ultracapacitor
Time.
Further, quantity >=2 of monomer capacitance 102 can be specifically adjusted according to actual needs, not done herein specific
It limits.
Fig. 2 shows the graphene ultracapacitors of the removal outer packing of an internal series-connection provided in an embodiment of the present invention
Structural schematic diagram, the electrode shape of graphene is interdigitated, it will be appreciated to those of skill in the art that the super electricity of graphene
The electrode of the graphene of container may be other shapes.Wherein, 11 be outer lug, and 12 be electrolyte, and 13 be graphene electricity
Pole, 14 be interior lug;Wherein, which includes 4 monomer capacitances and 3 interior lugs 14, wherein 4 monomer capacitances
It is connected in series with by interior lug 14 between middle adjacent monomer capacitance, wherein the monomer capacitance includes Graphene electrodes 13 and electricity
Solve liquid 12;Capacitor body head and the tail both ends are connect with an outer lug 11 respectively.
The graphene ultracapacitor of internal series-connection provided by the invention, Graphene electrodes are without additional conductive agent, bonding
The slurry feedstocks such as agent prepare, it is simple for process, and capacitor body be not necessarily to additional diaphragm and interior lug, Graphene electrodes material with
Interior lug integrally connected, is greatly saved material.The material object of the graphene ultracapacitor of the removing outer packing of internal series-connection
As shown in Figure 3.
According to another aspect of the present invention, a kind of graphene ultracapacitor is provided, as shown in figure 4, including:
Capacitor body 201, the capacitor body include multiple monomer capacitances 202 and interior lug 203;
Wherein, it is connected in parallel by interior lug 203 between adjacent monomer capacitance 202 in the multiple monomer capacitance 202, institute
It includes graphene anode, graphene cathode and electrolyte to state monomer capacitance 202, the graphene anode of the monomer capacitance 202 and
The graphene anode of adjacent monomer capacitance passes through 203 integrally connected of interior lug, the graphene cathode and phase of the monomer capacitance 202
The graphene cathode of adjacent monomer capacitance 202 passes through 203 integrally connected of interior lug;
Two outer lugs 204, described two outer lugs 204 respectively with head end monomer capacitance 202 and tail end monomer capacitance 202
It is connected;And
Outer packing 205, the outer packing 205 is for being packaged the capacitor body.
Further, graphene anode, graphene cathode and interior lug 203 are to pass through laser in the monomer capacitance 202
Irradiate the surface formation of same thin polymer film substrate.The graphene ultracapacitor of the present invention, without additional interior lug
Joining Technology.
More preferred, the thin polymer film substrate is Kapton or polyetherimide film.Through CO2It is infrared
The irradiation of laser, the thin polymer film substrate surface form porous graphene.Wherein, the carbon atom structure of porous graphene
At micron order or nano level pentagon-heptagon polycrystalline lattice, be connected with each other between lattice, have extra specific surface area, compared with
The features such as good electric conductivity and electrochemical stability, therefore the porous graphene that the thin polymer film substrate surface is formed was both
It can be used as capacitor electrode material, interior lug is can also be used as and use, greatly improve the chemical property of capacitor.
Further, 202 graphene anodes of the monomer capacitance and graphene cathode present interdigitated, parallel strip,
Any one of helical form or combinations thereof shape.
More preferred, the shape of the graphene anode and graphene cathode is interdigitated.Using the graphite of interdigitated
Alkene electrode can increase the unilateral effective area of electrode, to increase the capacitance of graphene ultracapacitor.
Fig. 5 shows the knot of the graphene ultracapacitor of the removing outer packing of internal parallel provided in an embodiment of the present invention
Structure schematic diagram, Graphene electrodes shape are interdigitated, it will be appreciated to those of skill in the art that graphene ultracapacitor
Graphene electrodes may be other shapes.Wherein, 21 be outer lug, and 22 be electrolyte, and 23 be Graphene electrodes, and 24 be interior
Lug;Wherein, which includes 2 monomer capacitances and 2 interior lugs 24, wherein adjacent in 2 monomer capacitances
It is connected in parallel by interior lug 24 between monomer capacitance, wherein the monomer capacitance includes Graphene electrodes 23 and electrolyte 22;
Capacitor body head and the tail both ends are connect with an outer lug 21 respectively.
The graphene ultracapacitor of internal parallel provided by the invention, Graphene electrodes are without additional conductive agent, bonding
The slurry feedstocks such as agent prepare, it is simple for process, and capacitor body be not necessarily to additional diaphragm and interior lug, Graphene electrodes material with
Interior lug integrally connected, is greatly saved material.
According to another aspect of the present invention, a kind of graphene ultracapacitor is provided, as shown in fig. 6, including capacitor
Ontology, the capacitor body are the combination of the first capacitor body 301 and the second capacitor body 401.
Further, first capacitor body 301 includes multiple monomer capacitances 302 and interior lug 303, wherein institute
It states in multiple monomer capacitances and is connected in series with by interior lug 303 between adjacent monomer capacitance 302, the monomer capacitance 302 includes
Graphene anode, graphene cathode and electrolyte, the graphene anode of the monomer capacitance 302 and the first adjacent monomer capacitance
302 graphene cathode passes through 303 integrally connected of interior lug, the graphene cathode of the monomer capacitance 302 and the second adjacent list
The graphene anode of body capacitance 302 passes through 303 integrally connected of interior lug;Second capacitor body 401 includes multiple monomers
Capacitance 402 and interior lug 403, wherein in the multiple monomer capacitance between adjacent monomer capacitance 402 by interior lug 403 simultaneously
Connection connection, the monomer capacitance 402 include graphene anode, graphene cathode and electrolyte, the graphite of the monomer capacitance 402
The graphene anode of alkene anode and adjacent monomer capacitance 402 passes through 403 integrally connected of interior lug, the stone of the monomer capacitance 402
The graphene cathode of black alkene cathode and adjacent monomer capacitance 402 passes through 403 integrally connected of interior lug.
Wherein, the number of the first capacitor body of the present invention couple and the second capacitor body, the number and list of monomer capacitance
The connection relation of body capacitance is not particularly limited, and those skilled in the art can according to actual needs be adjusted it.
Further, the graphene anode, graphene cathode and interior lug are by the same polymer thin of laser irradiation
What the surface of film substrate was formed.
Further, interdigitated, parallel strip, helical form or combinations thereof is presented in the graphene anode and graphene cathode
Any one of shape.
According to another aspect of the invention, a kind of preparation method of graphene ultracapacitor is provided, as shown in fig. 7,
Including:
Step S110:Thin polymer film substrate is fixed on base material;
Step S120:Using CO2Infrared laser irradiates thin polymer film substrate, obtain patterned graphene anode,
Graphene cathode and interior lug;
Step S130:Cut out graphene anode, graphene cathode and interior lug;
Step S140:Coating electrolyte forms multiple monomer capacitances, wherein adjacent monomer electricity in the multiple monomer capacitance
It is connected by interior lug between appearance;
Step S150:It is disposably encapsulated after the outer lug of installation, obtains graphene ultracapacitor.
The preparation method of graphene ultracapacitor provided by the invention, using CO2Infrared laser irradiates polymer thin
The mode of film substrate prepares graphene anode, graphene cathode and interior lug.It can be by predefined parameter (such as before laser irradiation
Distance etc. between Graphene electrodes and interior lug integrally connected situation, graphene positive and negative anodes) design the stone with predetermined shape
Black alkene electrode and interior lug.Wherein, the shape of Graphene electrodes include but not limited to interdigitated, parallel strip, helical form and its
Any one of combined shaped.
A kind of preparation method of graphene ultracapacitor provided in an embodiment of the present invention, includes the following steps:
Step S210:Thin polymer film substrate is fixed on base material;
More preferred, thin polymer film substrate includes but not limited to Kapton and polyetherimide film.
The selection of base material is not particularly limited, those skilled in the art can according to actual needs be adjusted it.
More preferred, the base material is glass or acrylic board.
Further, further include cleaning base material step, i.e.,:Base material is put into and is contained in spirituous container, then container is put
Enter supersonic wave cleaning machine and carry out ultrasonic cleaning, then replaces alcohol to repeat the above steps with water, to remove substrate surface
Dust.
Thin polymer film substrate is fixed on using well known method on base material, further limit is not done to fixing means herein
It is fixed.
Step S220:Using CO2Infrared laser irradiates thin polymer film substrate, obtain patterned graphene anode,
Graphene cathode and interior lug;
The effect of this step is:On the one hand, by thin polymer film substrate surface laser irradiation at the graphite of pre-set dimension
Alkene electrode and interior lug;On the other hand, the thin polymer film substrate surface of insulation is made to form conductive porous stone through laser irradiation
Black alkene electrode and interior lug.
Further, the CO2The power of infrared laser is 2-10mW, and it is 1-5mm/s that laser, which sweeps speed, if laser
Power and sweep speed are less than this range, then can not form grapheme material, if laser power and sweep speed exceed this model
It encloses, then graphene can be peeled off from thin polymer film substrate surface, and Structural Faults can not be used as electrode.
In addition, CO2The power control of infrared laser is swashed in which can ensure thin polymer film substrate portions in 2-10mW
At graphene, i.e., light irradiates:Close to CO2The part of infrared laser is illuminated at graphene, and close to the polymer thin of base material
Film substrate is not illuminated at graphene, and ingredient is still the polymer of insulation.
Preferably, the CO2The power of infrared laser is 3mW, and it is 2mm/s, the graphite obtained at this time that laser, which sweeps speed,
Alkene structure is most complete, and it is best to do the ultracapacitor electrical property that electrode is prepared using this graphene.
Further, the distance between the graphene anode in monomer capacitance and graphene cathode are 0.1-0.5mm, preferably
For 0.2mm.The size of spacing can be realized by being pre-adjusted the size of laser aperture.If spacing is too small, graphite is easily caused
The interelectrode short circuit of alkene, spacing is excessive, then is unfavorable for the migration of ion between the electrodes, increases filling for graphene ultracapacitor
Discharge time.
Step S230:Cut out graphene anode, graphene cathode and interior lug;
Specifically, by thin polymer film substrate along through CO2The patterned graphene that infrared laser irradiates is just
The outer profile of pole, graphene cathode and interior lug is integrally cut;
Step S240:Coating electrolyte forms multiple monomer capacitances, wherein adjacent monomer electricity in the multiple monomer capacitance
It is connected by interior lug between appearance;
Further, the electrolyte is colloidal electrolyte, preferably in PVA/ sulfuric acid, PVA/ hydrochloric acid or PVA/ phosphoric acid
It is one or more.It on the one hand can ensure that electrolyte is adhesively fixed in Graphene electrodes region using the colloidal electrolyte, prevent
On the other hand electrolyte flow eliminates additional diaphragm to interior lug position, simplify preparation process.
Step S250:It is disposably encapsulated after the outer lug of installation, obtains graphene ultracapacitor.
Fig. 8 shows a kind of preparation method of the graphene ultracapacitor of internal series-connection provided in an embodiment of the present invention,
It is illustrated by taking interdigitated Graphene electrodes as an example below, it should be understood by those skilled in the art that, Graphene electrodes may be used also
Think other shapes.Specifically comprise the following steps:
Step S310:Thin polymer film substrate is fixed on base material;
More preferred, thin polymer film substrate is Kapton or polyetherimide film.
The selection of base material is not particularly limited, those skilled in the art can according to actual needs be adjusted it.
More preferred, the base material is glass or acrylic board.
Further, further include cleaning base material step, i.e.,:Base material is put into and is contained in spirituous container, then container is put
Enter supersonic wave cleaning machine and carry out ultrasonic cleaning, then replaces alcohol to repeat the above steps with water, to remove substrate surface
Dust.
Thin polymer film substrate is fixed on using well known method on base material, further limit is not done to fixing means herein
It is fixed.
Step S320:Using CO2Infrared laser irradiates thin polymer film substrate, is obtaining concatenated interdigitated graphene just
Pole, graphene cathode and interior lug;
The surface shape that graphene anode, graphene cathode and interior lug pass through the same thin polymer film substrate of laser irradiation
At.The graphene anode of monomer capacitance and the graphene cathode of the first adjacent monomer capacitance and interior lug are integrally connecteds;It is single
The graphene of the graphene cathode of body capacitance and the second adjacent monomer capacitance anode and interior lug are integrally connecteds.
Further, the CO2The power of infrared laser is 3mW, and it is 2mm/s that laser, which sweeps speed,.
Further, the distance between graphene anode and graphene cathode are 0.2mm.
Step S330:Cut out graphene anode, graphene cathode and the interior lug of interdigitated;
Wherein, the unilateral effective area that electrode can be increased using the Graphene electrodes of interdigitated, to increase graphene
The capacitance of ultracapacitor.
Specifically, by thin polymer film substrate along through CO2The graphene for the interdigitated that infrared laser irradiates is just
The outer profile of pole, graphene cathode and interior lug is integrally cut;
Step S340:Coating electrolyte forms multiple monomer capacitances, wherein adjacent monomer electricity in the multiple monomer capacitance
It is connected in series with by interior lug between appearance;
Further, the electrolyte is colloidal electrolyte, preferably in PVA/ sulfuric acid, PVA/ hydrochloric acid or PVA/ phosphoric acid
It is one or more.It on the one hand can ensure that electrolyte is adhesively fixed in Graphene electrodes region using the colloidal electrolyte, prevent
On the other hand electrolyte flow eliminates additional diaphragm to interior lug position, simplify preparation process.
Step S350:It is disposably encapsulated after the outer lug of installation, obtains the graphene ultracapacitor of internal series-connection.
Wherein, the packaging method and encapsulating material that the present invention uses are it is known in the art that can be aluminum plastic film, PPE
The encapsulating materials such as plastic cement, here, the present invention does not do excessive restriction.
Fig. 9 shows a kind of preparation method of the graphene ultracapacitor of internal parallel provided in an embodiment of the present invention,
It is illustrated by taking interdigitated Graphene electrodes as an example below, it should be understood by those skilled in the art that, Graphene electrodes may be used also
Think other shapes.Specifically comprise the following steps:
Step S410:Thin polymer film substrate is fixed on base material;
More preferred, thin polymer film substrate is Kapton or polyetherimide film.
The selection of base material is not particularly limited, those skilled in the art can according to actual needs be adjusted it.
More preferred, the base material is glass or acrylic board.
Further, further include cleaning base material step, i.e.,:Base material is put into and is contained in spirituous container, then container is put
Enter supersonic wave cleaning machine and carry out ultrasonic cleaning, then replaces alcohol to repeat the above steps with water, to remove substrate surface
Dust.
Thin polymer film substrate is fixed on using well known method on base material, further limit is not done to fixing means herein
It is fixed.Step S420:Using CO2Infrared laser irradiates thin polymer film substrate, obtains interdigitated graphene anode in parallel, stone
Black alkene cathode and interior lug;
Graphene anode, graphene cathode and interior lug are the surface shapes by the same thin polymer film substrate of laser irradiation
At.The graphene anode and interior lug of graphene anode and adjacent monomer capacitance are integrally connecteds in monomer capacitance;Monomer
Graphene cathode and interior lug are integrally connecteds in the graphene cathode and adjacent monomer capacitance of capacitance.
Further, the CO2The power of infrared laser is 3mW, and it is 2mm/s that laser, which sweeps speed,.
Further, the distance between graphene anode and graphene cathode are 0.2mm.
Step S430:Cut out graphene anode, graphene cathode and the interior lug of interdigitated;
The unilateral effective area that electrode can be increased using the Graphene electrodes of interdigitated, to increase the super electricity of graphene
Capacity of condenser.
Specifically, by thin polymer film substrate along through CO2The graphene for the interdigitated that infrared laser irradiates is just
The outer profile of pole, graphene cathode and interior lug is integrally cut;
Step S440:Coating electrolyte forms multiple monomer capacitances, wherein adjacent monomer electricity in the multiple monomer capacitance
It is connected in parallel by interior lug between appearance;
Further, the electrolyte is colloidal electrolyte, preferably in PVA/ sulfuric acid, PVA/ hydrochloric acid or PVA/ phosphoric acid
It is one or more.It on the one hand can ensure that electrolyte is adhesively fixed in Graphene electrodes region using the colloidal electrolyte, prevent
On the other hand electrolyte flow eliminates additional diaphragm, simplifies preparation process to interior lug position.
Step S450:It is disposably encapsulated after the outer lug of installation, obtains the graphene ultracapacitor of internal parallel.
Wherein, the packaging method and encapsulating material that the present invention uses are it is known in the art that can be aluminum plastic film, PPE
The encapsulating materials such as plastic cement, here, the present invention does not do excessive restriction.
Figure 10 shows a kind of graphene ultracapacitor of internal series-connection-parallel combination provided in an embodiment of the present invention
Preparation method is illustrated by taking interdigitated Graphene electrodes as an example below, it should be understood by those skilled in the art that, graphene
Electrode can also be other shapes.Specifically comprise the following steps:
Step S510:Thin polymer film substrate is fixed on base material;
More preferred, thin polymer film substrate is Kapton or polyetherimide film.
The selection of base material is not particularly limited, those skilled in the art can according to actual needs be adjusted it.
More preferred, the base material is glass or acrylic board.
Further, further include cleaning base material step, i.e.,:Base material is put into and is contained in spirituous container, then container is put
Enter supersonic wave cleaning machine and carry out ultrasonic cleaning, then replaces alcohol to repeat the above steps with water, to remove substrate surface
Dust.
Thin polymer film substrate is fixed on using well known method on base material, further limit is not done to fixing means herein
It is fixed.
Step S520:Using CO2Infrared laser irradiates thin polymer film substrate, obtains the first capacitor body and second
Interdigitated graphene anode, graphene cathode and the interior lug of capacitor body;
Interdigitated graphene anode, graphene cathode and the interior pole of first capacitor body and the second capacitor body
Ear is formed by the surface of the same thin polymer film substrate of laser irradiation.In first capacitor body in monomer capacitance
The graphene cathode and interior lug of graphene anode and the first adjacent monomer capacitance are integrally connecteds;The graphene of monomer capacitance
The graphene of cathode and the second adjacent monomer capacitance anode and interior lug are integrally connecteds.It is single in second capacitor body
The graphene anode and interior lug of body capacitance graphene anode and adjacent monomer capacitance are integrally connecteds;The graphite of monomer capacitance
Graphene cathode and interior lug are integrally connecteds in alkene cathode and adjacent monomer capacitance.
Further, the CO2The power of infrared laser is 3mW, and it is 2mm/s that laser, which sweeps speed,.
Further, the distance between graphene anode and graphene cathode are 0.2mm.
Step S530:Cut out graphene anode, graphene cathode and the interior lug of interdigitated;
Specifically, by thin polymer film substrate along through CO2The graphene for the interdigitated that infrared laser irradiates is just
The outer profile of pole, graphene cathode and interior lug is integrally cut;
Step S540:Coating electrolyte forms multiple monomer capacitances, wherein adjacent monomer electricity in the multiple monomer capacitance
It is connected in series or in parallel by interior lug between appearance;
Further, the electrolyte is colloidal electrolyte, preferably in PVA/ sulfuric acid, PVA/ hydrochloric acid or PVA/ phosphoric acid
It is one or more.It on the one hand can ensure that electrolyte is adhesively fixed in Graphene electrodes region using the colloidal electrolyte, prevent
On the other hand electrolyte flow eliminates additional diaphragm to interior lug position, simplify preparation process.
Step S550:It is disposably encapsulated after the outer lug of installation, obtains the graphene super capacitor of internal series-connection-parallel connection
Device.
Wherein, the packaging method and encapsulating material that the present invention uses are it is known in the art that can be aluminum plastic film, PPE
The encapsulating materials such as plastic cement, here, the present invention does not do excessive restriction.
The preparation method of graphene ultracapacitor provided in this embodiment, can effectively improve graphene ultracapacitor
Production efficiency, disposably can be completed required Graphene electrodes and interior lug, production technology relatively coating and mask plate work
Skill significantly simplifies, and is readily produced.
In addition, the graphene ultracapacitor in the present invention can be used as microelectronic device memory element, miniature electronic
Circuit voltage stabilizing element (such as logistics data tracks), is widely used in every field.
Performance test
Middle outside is gone here and there compared with the existing technology for the internal series-connection of the present invention and/or the graphene ultracapacitor of parallel-connection structure
The graphene ultracapacitor of connection/parallel-connection structure only need to be encapsulated once compared to preparation process is greatly simplified, save part
Encapsulating material and interior lug Joining Technology;And it is internal after the series connection of multiple monomer capacitances, capacitance is compared to side of the same race
The capacitance of the graphene ultracapacitor of the identical non-internal series-connection structure of unilateral effective area prepared by method improves 20~30
Times.
The performance for the graphene ultracapacitor of internal series-connection for confirming to provide through this embodiment below by experiment
Really it is better than the graphene ultracapacitor of non-internal series-connection:
Prepare the graphene ultracapacitor of a non-internal series-connection, material, preparation process and its parameter with this hair
The graphene ultracapacitor of the bright internal series-connection prepared using above-described embodiment method is identical, and uniquely different is exactly capacitance
Device ontology is a monomer capacitance, and capacitor body is the monomer capacitance of 4 internal series-connections in the embodiment of the present invention.
Wherein, the electrode unilateral side effective area of two kinds of ultracapacitors is 30mm2, between graphene positive and negative electrode between
Gap is 0.2mm, and the thin polymer film substrate used is Kapton, and the power of laser is 3mW, and laser sweeps speed and is
2mm/s.Then to the graphene ultracapacitor of the graphene ultracapacitor and non-internal series-connection of the internal series-connection assembled
Carry out charge-discharge test.
Figure 11 shows the charge and discharge data of the graphene ultracapacitor of internal series-connection provided in an embodiment of the present invention,
In, charging and discharging currents 1mA, charging-discharging cycle 262s, charging voltage 2.3V.
According to formula:Capacitance=charging and discharging currents × charging-discharging cycle/2 × charging voltage, can obtain internal series-connection stone
The capacitance of black alkene ultracapacitor is c=1 × 262/2 × 2.3=56.96mF.
Figure 12 shows the charge and discharge data of the graphene ultracapacitor of non-internal series-connection, wherein charging and discharging currents
0.2mA, charging-discharging cycle general 55s, charging voltage 2.3V.
According to formula:Capacitance=charging and discharging currents × charging-discharging cycle/2 × charging voltage, can obtain non-internal series-connection
The capacitance of graphene ultracapacitor is c=0.2 × 55/2 × 2.3=2.39mF.
By calculating it is found that the capacitance of the graphene ultracapacitor of internal series-connection is the graphene of non-internal series-connection
24 times of the capacitance of ultracapacitor.By using internal series-connection structure, graphene ultracapacitor is greatly improved
Capacitance, effect is very notable.
It will be appreciated by those skilled in the art that realizing that all or part of step in above-described embodiment method can pass through
Program instructs the related hardware to complete.
It will also be appreciated that apparatus structure shown in attached drawing or embodiment is only schematical, logic knot is indicated
Structure.Wherein, the module shown as separating component may be or may not be to be physically separated.
Obviously, various changes and modifications can be made to the invention without departing from essence of the invention by those skilled in the art
God and range.In this way, if these modifications and changes of the present invention belongs to the range of the claims in the present invention and its equivalent technologies
Within, then the present invention is also intended to include these modifications and variations.
Claims (19)
1. a kind of graphene ultracapacitor, which is characterized in that including:
Capacitor body, the capacitor body include multiple monomer capacitances and interior lug;
Wherein, it is connected in series with by interior lug between adjacent monomer capacitance in the multiple monomer capacitance, the monomer capacitance packet
Include graphene anode, graphene cathode and electrolyte, the graphene anode of the monomer capacitance and the first adjacent monomer capacitance
Graphene cathode passes through interior lug integrally connected, the graphite of the graphene cathode of the monomer capacitance and the second adjacent monomer capacitance
Alkene anode passes through interior lug integrally connected;
Two outer lugs, described two outer lugs are connected with head end monomer capacitance and tail end monomer capacitance respectively;And
Outer packing, the outer packing is for being packaged the capacitor body.
2. graphene ultracapacitor according to claim 1, which is characterized in that electrolyte is colloidal electrolyte.
3. graphene ultracapacitor according to claim 2, which is characterized in that the electrolyte include PVA/ sulfuric acid,
PVA/ hydrochloric acid or PVA/ phosphoric acid.
4. according to claim 1-3 any one of them graphene ultracapacitors, which is characterized in that the graphene anode,
Graphene cathode and interior lug are formed by the surface of the same thin polymer film substrate of laser irradiation.
5. graphene ultracapacitor according to claim 4, which is characterized in that the thin polymer film substrate is polyamides
Imines film or polyetherimide film.
6. according to claim 1-5 any one of them graphene ultracapacitors, which is characterized in that the graphene anode and
Any one of interdigitated, parallel strip, helical form or combinations thereof shape is presented in graphene cathode.
7. according to claim 1-6 any one of them graphene ultracapacitors, which is characterized in that the graphene anode and
The distance between graphene cathode is 0.1-0.5mm.
8. graphene ultracapacitor according to claim 7, which is characterized in that the graphene anode and graphene are negative
The distance between pole is 0.2mm.
9. a kind of graphene ultracapacitor, which is characterized in that including:
Capacitor body, the capacitor body include multiple monomer capacitances and interior lug;
Wherein, it is connected in parallel by interior lug between adjacent monomer capacitance in the multiple monomer capacitance, the monomer capacitance packet
Include graphene anode, graphene cathode and electrolyte, the graphite of the graphene anode and adjacent monomer capacitance of the monomer capacitance
For alkene anode by interior lug integrally connected, the graphene cathode of the monomer capacitance and the graphene cathode of adjacent monomer capacitance are logical
Cross interior lug integrally connected;
Two outer lugs, described two outer lugs are connected with head end monomer capacitance and tail end monomer capacitance respectively;And
Outer packing, the outer packing is for being packaged the capacitor body.
10. graphene ultracapacitor according to claim 9, which is characterized in that the graphene anode, graphene are negative
Pole and interior lug are formed by the surface of the same thin polymer film substrate of laser irradiation.
11. graphene ultracapacitor according to claim 10, which is characterized in that the thin polymer film substrate is poly-
Imide membrane or polyetherimide film.
12. according to claim 9-11 any one of them graphene ultracapacitors, which is characterized in that the graphene anode
Any one of interdigitated, parallel strip, helical form or combinations thereof shape is presented with graphene cathode.
13. a kind of graphene ultracapacitor, including capacitor body, which is characterized in that the capacitor body is wanted for right
Ask any one of capacitor body and the claim 9-12 of any one of 1-8 graphene ultracapacitors graphenes super
The combination of the capacitor body of capacitor.
14. a kind of preparation method of such as claim 1-13 any one of them graphene ultracapacitors, which is characterized in that packet
It includes:
(1) thin polymer film substrate is fixed on base material;
(2) CO is used2Infrared laser irradiates thin polymer film substrate, obtain patterned graphene anode, graphene cathode and
Interior lug;
(3) graphene anode, graphene cathode and interior lug are cut out;
(4) coating electrolyte forms multiple monomer capacitances, wherein passing through between adjacent monomer capacitance in the multiple monomer capacitance
Interior lug connection;
(5) it is disposably encapsulated after outer lug being installed, obtains graphene ultracapacitor.
15. preparation method according to claim 14, which is characterized in that wherein, patterned graphite described in step (2)
Alkene anode, graphene cathode and interior lug include that the graphene anode of monomer capacitance and the graphene of the first adjacent monomer capacitance are born
By interior lug integrally connected, the graphene anode of the graphene cathode of monomer capacitance and the second adjacent monomer capacitance passes through interior for pole
Lug integrally connected.
16. preparation method according to claim 14, which is characterized in that wherein, patterned graphite described in step (2)
Alkene anode, graphene cathode and interior lug include that the graphene anode of monomer capacitance and the graphene anode of adjacent monomer capacitance lead to
It crosses interior lug integrally connected, the graphene cathode of monomer capacitance and the graphene cathode of adjacent monomer capacitance and passes through interior lug one
Connection.
17. according to the preparation method described in claim 13-16, which is characterized in that the thin polymer film substrate is that polyamides is sub-
Amine film or polyetherimide film.
18. according to claim 13-17 any one of them preparation methods, which is characterized in that the CO2The work(of infrared laser
Rate is 2-10mW, and it is 1-5mm/s that laser, which sweeps speed,.
19. preparation method according to claim 18, which is characterized in that the CO2The power of infrared laser is 3mW, is swashed
It is 2mm/s that light device, which sweeps speed,.
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| CN109440145A (en) * | 2018-12-30 | 2019-03-08 | 苏州碳素集电新材料有限公司 | A kind of graphene/copper composite conducting material and preparation method thereof |
| CN111211002A (en) * | 2019-09-16 | 2020-05-29 | 中国科学院大连化学物理研究所 | Method for preparing integrated planar super capacitor on polymer substrate |
| CN112097967A (en) * | 2020-09-15 | 2020-12-18 | 闽江学院 | Self-energy-supply-based flexible extensible mechanical sensing system and preparation method thereof |
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| CN114974936B (en) * | 2022-06-24 | 2023-09-08 | 安徽格兰科新材料技术有限公司 | Preparation method of graphene supercapacitor composite electrode with high pseudo-capacitance loading capacity |
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| WO2014190772A1 (en) * | 2013-05-30 | 2014-12-04 | 纳米新能源（唐山）有限责任公司 | Graphene, graphene electrode, graphene super capacitor and preparation method thereof |
| CN105914045A (en) * | 2016-04-08 | 2016-08-31 | 纳智源科技（唐山）有限责任公司 | Super capacitor |
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| CN107206741A (en) * | 2014-11-26 | 2017-09-26 | 威廉马歇莱思大学 | Graphene mixing material for the induced with laser of electronic installation |
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