CN105448534A - Combined electrode, preparation method thereof and application in super capacitor - Google Patents
Combined electrode, preparation method thereof and application in super capacitor Download PDFInfo
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Abstract
The invention discloses a combined electrode, a preparation method thereof and an application in a super capacitor. A combined electrode active material is arranged on the surface of a current collector. The combined electrode active material simultaneously includes a fake capacitor electrode active material and a double electric layer capacitor electrode active material. The fake capacitor electrode active material is at least one of conductive polymers or metal oxides. The double electric layer capacitor electrode active material is a carbon active material. The combined electrode including the fake capacitor electrode active material and the double electric layer capacitor electrode active material is used as the electrode of the super capacitor, so that the energy density and the power density are high, the technology is simple, the performance is controllable, and the application field of the super capacitor is expanded.
Description
Technical field
The invention belongs to the preparation field of ultracapacitor, be specifically related to a kind of combination electrode and preparation method thereof and the application in ultracapacitor.
Background technology
Along with the aggravation of global resource shortage and craving for green technology and high performance-price ratio alternative energy source, countries in the world are all at the environmental type energy that research and development are new.Ultracapacitor, as the novel energy-storing product given priority to this century, is one of core product of low-carbon economy, just by countries in the world institute extensive concern, also for increasing country and enterprise fall over each other research and production.
Ultracapacitor is the green energy storage device between battery and traditional capacitor, has the energy density higher than traditional capacitor, the power density higher than battery; Both there is the energy storage characteristic of battery, there is again the characteristic of traditional capacitor fast charging and discharging, and its material used is commonly environmental protection.Ultracapacitor has huge using value and market potential in various fields such as new-energy automobile, the renewable energy resources, aviation military affairs, communication, industry, consumer electronics.The electrode active material of ultracapacitor is divided into electrical double layer capacitor electrodes active material and pseudocapacitors electrode active material, wherein electrical double layer capacitor electrodes active material is that carbon active material is as business-like active carbon, its Large ratio surface sum fast charging and discharging characteristic, therefore the ultracapacitor being electrode active material with it has high power density, but the specific capacitance of active carbon is lower, therefore the energy density of ultracapacitor is far below lithium ion battery.Pseudocapacitors electrode active material is metal oxide or conducting polymer, and they have the higher specific capacitance of specific activity charcoal and voltage window, according to E=1/2CV
2known, the energy density of ultracapacitor can be improved.
Summary of the invention
The present invention is directed to above-mentioned prior art Problems existing and make improvement, the object of this invention is to provide a kind of combination electrode and preparation method thereof and the application in ultracapacitor, the electrode of combination electrode as ultracapacitor of pseudocapacitors electrode active material and electrical double layer capacitor electrodes active material will be comprised, not only there is high-energy-density and power density, and technique is simple, performance is controlled, can widen the application of ultracapacitor.
For achieving the above object, the present invention adopts following technical scheme:
A kind of combination electrode, arrange composite electrode active material at collection liquid surface, described composite electrode active material comprises pseudocapacitors electrode active material and electrical double layer capacitor electrodes active material simultaneously; Described pseudocapacitors electrode active material is at least one in conducting polymer or metal oxide, and described electrical double layer capacitor electrodes active material is carbon active material.
Electrical double layer capacitor electrodes active material is first set at collection liquid surface, then pseudocapacitors electrode active material is set; Or pseudocapacitors electrode active material is first set at collection liquid surface, then electrical double layer capacitor electrodes active material is set; Wherein 20 ~ 100% of collection liquid surface electrical double layer capacitor electrodes active material is set.
The Thickness Ratio of electrical double layer capacitor electrodes active material and pseudocapacitors electrode active material is 80:1 ~ 1:80, and more preferably Thickness Ratio is 40:1 ~ 1:40.
Conducting polymer is polypyrrole and derivative, polythiophene and derivative thereof, Polyaniline and its derivative, polystyrene and derivative, polypyridine and derivative thereof, gathers at least one in benzene and its derivative, poly quinoline and derivative thereof.
Metal oxide is at least one in the oxide of manganese, ruthenium, cobalt, nickel, vanadium.
Carbon active material is at least one in active carbon, Graphene, CNT (carbon nano-tube), carbon gel, carbon fiber, soft carbon, hard carbon, graphite.
Described current collector material is at least one in aluminium, copper, nickel, tantalum, titanium, lead, stainless steel, carbon, graphite, conducting polymer or Graphene.
Electrical double layer capacitor electrodes active material comprises coating, spraying, dipping, printing, printing, electro-deposition in the method to set up of collection liquid surface; Pseudocapacitors electrode active material comprises coating, spraying, dipping, printing, printing, chemical deposition, electrochemical deposition in the method to set up of collection liquid surface.
Described combination electrode is as the electrode of ultracapacitor.At least one electrode in ultracapacitor in negative or positive electrode is described combination electrode; The assembling of ultracapacitor: arrange barrier film between positive pole and negative pole, add electrolyte, lamination or winding are assembled into ultracapacitor.
Remarkable advantage of the present invention is: will comprise the electrode of combination electrode as ultracapacitor of pseudocapacitors electrode active material and electrical double layer capacitor electrodes active material, not only there is high-energy-density and power density, and technique is simple, performance is controlled, can widen the application of ultracapacitor.
Embodiment
A kind of combination electrode, arranges composite electrode active material at collection liquid surface, as the electrode of ultracapacitor.This combination electrode comprises pseudocapacitors electrode active material and electrical double layer capacitor electrodes active material simultaneously, pseudocapacitors electrode active material is at least one in conducting polymer or metal oxide, and electrical double layer capacitor electrodes active material is carbon active material.
In the present invention, electrical double layer capacitor electrodes active material is first set at the collection liquid surface of combination electrode, then pseudocapacitors electrode active material is set; Or pseudocapacitors electrode active material is first set at collection liquid surface, then electrical double layer capacitor electrodes active material is set.Combination electrode 20 ~ 100% more preferably 80 ~ 100% collection liquid surfaces electrical double layer capacitor electrodes active material is set, residual set flow surface arranges pseudocapacitors electrode active material.
In the present invention, the Thickness Ratio of electrical double layer capacitor electrodes active material and pseudocapacitors electrode active material is 80:1 ~ 1:80, and more preferably Thickness Ratio is 40:1 ~ 1:40, and more preferably thickness is 10:1 ~ 1:10.
In the present invention, conducting polymer is polypyrrole and derivative, polythiophene and derivative thereof, Polyaniline and its derivative, polystyrene and derivative, polypyridine and derivative thereof, gathers at least one in benzene and its derivative, poly quinoline and derivative thereof; Metal oxide is at least one in the oxide of manganese, ruthenium, cobalt, nickel, vanadium; Carbon active material is at least one in active carbon, Graphene, CNT (carbon nano-tube), carbon gel, carbon fiber, soft carbon, hard carbon, graphite.
Technical scheme two in the present invention is: a kind of ultracapacitor is by positive pole, negative pole, and the barrier film between positive pole and negative pole and electrolyte composition, at least one electrode wherein in negative or positive electrode is described combination electrode.The making step of ultracapacitor:
(1) preparation of combination electrode: to be coated with, to spray, to flood, to print, to print, the carbon active materials such as active carbon, Graphene, carbon nano-tube are arranged at collection liquid surface by the method such as electro-deposition; With methods such as coating, spraying, dipping, printing, printing, chemical deposition or electrochemical depositions, the fake capacitance such as conducting polymer, metal oxide active material is arranged at collector and carbon surface of active material, makes combination electrode.Or with methods such as coating, spraying, dipping, printing, printing, chemical deposition or electrochemical depositions, the fake capacitance such as conducting polymer, metal oxide active material is arranged at collection liquid surface, with methods such as coating, spraying, dipping, printing, printing, electro-deposition, the carbon active materials such as active carbon, Graphene, carbon nano-tube are arranged at the surface of collector and fake capacitance active material, make combination electrode.
(2) assembling of ultracapacitor: arrange barrier film between positive pole and negative pole, add electrolyte, lamination or winding are assembled into ultracapacitor.
Ultracapacitor preparation process (1) collector of the present invention is at least one in materials of aluminum, copper, nickel, tantalum, titanium, lead, stainless steel, carbon, graphite, conducting polymer or Graphene.
In step of the present invention (2), described barrier film can prevent positive plate from directly contacting and short circuit with negative plate, but allows the conduction of ion.Described barrier film is at least one in polyethene microporous membrane, microporous polypropylene membrane, polyvinylidene fluoride microporous film, polypropylene-polyethylene composite membrane, inorganic ceramic membrane, paper barrier film, nonwoven fabrics barrier film.
In the present invention, the electrode of described ultracapacitor is assembled into any one in sheet, square, button, cylindrical shell in the mode such as lamination, winding, also can be assembled into irregular external form.
embodiment 1: by active carbon, acetylene black, butadiene-styrene rubber (SBR), carboxymethyl cellulose (CMC) in mass ratio 80:10:7:3 be mixed into slurry, coat aluminium foil surface, and dry at 110 DEG C of temperature.By polyaniline, acetylene black, butadiene-styrene rubber (SBR), carboxymethyl cellulose (CMC) in mass ratio 80:10:7:3 be mixed into slurry, then coat aluminium foil and activated carbon surface, and dry at 110 DEG C of temperature, make combination electrode.Roll-in according to a conventional method again, cut into given size, vacuumize, between anode composite and composite negative pole, arrange barrier film, add electrolyte, winding is assembled into column ultracapacitor.100% collection liquid surface of combination electrode arranges active carbon, and activated carbon surface arranges polyaniline, and the Thickness Ratio of active carbon and polyaniline is 80:1.
embodiment 2: by Graphene, butadiene-styrene rubber (SBR), carboxymethyl cellulose (CMC) in mass ratio 40:7:3 be mixed into slurry, be sprayed at aluminium foil surface, and dry at 110 DEG C of temperature.By polypyrrole, acetylene black, butadiene-styrene rubber (SBR), carboxymethyl cellulose (CMC) in mass ratio 80:10:7:3 be mixed into slurry, then be sprayed at aluminium foil and graphenic surface, and dry at 110 DEG C of temperature, make combination electrode.By active carbon, acetylene black, butadiene-styrene rubber (SBR), carboxymethyl cellulose (CMC) in mass ratio 80:10:7:3 be mixed into slurry, coat aluminium foil surface, and dry at 110 DEG C of temperature, make activated carbon electrodes.Again according to a conventional method by electrode roll-in, cut into given size, vacuumize, between anode composite and activated carbon negative electrode, barrier film is set, add electrolyte, winding be assembled into column ultracapacitor.95% collection liquid surface of combination electrode arranges Graphene, remains 5% collection liquid surface and graphenic surface arranges polypyrrole, and the Thickness Ratio of Graphene and polypyrrole is 50:1.
embodiment 3: by CNT (carbon nano-tube), butadiene-styrene rubber (SBR), carboxymethyl cellulose (CMC) in mass ratio 40:7:3 be mixed into slurry, be sprayed at aluminum foil current collector surface, and dry at 110 DEG C of temperature.To 3 be gathered, 4 ethene dioxythiophenes, manganese dioxide, conductive black, butadiene-styrene rubber (SBR), carboxymethyl cellulose (CMC) in mass ratio 70:10:10:7:3 are mixed into slurry, be sprayed at CNT (carbon nano-tube) surface again, and dry at 110 DEG C of temperature, make combination electrode.Again according to a conventional method by electrode roll-in, cut into given size, vacuumize, between anode composite and composite negative pole, arrange barrier film, add electrolyte, winding is assembled into column ultracapacitor.90% collection liquid surface of combination electrode arranges CNT (carbon nano-tube), remains 10% collection liquid surface and CNT (carbon nano-tube) surface arranges poly-3,4 ethene dioxythiophenes, and CNT (carbon nano-tube) is 20:1 with the Thickness Ratio of poly-3,4 ethene dioxythiophenes.
embodiment 4: by active carbon, Ketjen black, butadiene-styrene rubber (SBR), carboxymethyl cellulose (CMC) in mass ratio 80:10:7:3 mix, and with water furnishing slurry, are printed in aluminum foil current collector surface, and dry at 110 DEG C of temperature.By polyaniline, acetylene black, butadiene-styrene rubber (SBR), carboxymethyl cellulose (CMC) in mass ratio 80:10:7:3 mix, with water furnishing slurry, republish in activated carbon surface, and dry at 110 DEG C of temperature, make combination electrode.Again according to a conventional method by electrode roll-in, cut into given size, vacuumize, between anode composite and composite negative pole, arrange barrier film, add electrolyte, winding is assembled into column ultracapacitor.85% collection liquid surface of combination electrode arranges active carbon, remains 15% collection liquid surface and activated carbon surface arranges polyaniline, and the Thickness Ratio of active carbon and polyaniline is 10:1.
embodiment 5: by polyaniline, acetylene black, butadiene-styrene rubber (SBR), carboxymethyl cellulose (CMC) in mass ratio 80:10:7:3 mix, with water furnishing slurry, then be sprayed at aluminium foil surface, and dry at 110 DEG C of temperature.By Graphene, acetylene black, butadiene-styrene rubber (SBR), carboxymethyl cellulose (CMC) in mass ratio 40:10:7:3 mix, with water furnishing slurry, be sprayed at polyaniline surface, and dry at 110 DEG C of temperature, make combination electrode.Again according to a conventional method by electrode roll-in, cut into given size, vacuumize, between anode composite and composite negative pole, arrange barrier film, add electrolyte, winding is assembled into column ultracapacitor.20% collection liquid surface of combination electrode arranges polyaniline, remains 80% collection liquid surface and polyaniline surface arranges Graphene, and the Thickness Ratio of Graphene and polyaniline is 5:1.
embodiment 6: by active carbon, acetylene black, butadiene-styrene rubber (SBR), carboxymethyl cellulose (CMC) in mass ratio 80:10:7:3 mix, with water furnishing slurry, coat aluminum foil current collector surface, and dry at 110 DEG C of temperature.Prepare polyaniline with chemical polymerization process in activated carbon surface, and dry at 80 DEG C of temperature, make combination electrode.Roll-in according to a conventional method, cuts into given size again, and vacuumize arranges barrier film between anode composite and composite negative pole, adds electrolyte, and winding is assembled into column ultracapacitor.70% collection liquid surface of combination electrode arranges active carbon, remains 30% collection liquid surface and activated carbon surface arranges polyaniline, and the Thickness Ratio of active carbon and polyaniline is 1:1.
embodiment 7: by active carbon, acetylene black, butadiene-styrene rubber (SBR), carboxymethyl cellulose (CMC) in mass ratio 80:10:7:3 mix, with water furnishing slurry, coat aluminum foil current collector surface, and dry at 110 DEG C of temperature.Prepare Polyglycolic acid fibre with chemical polymerization process in activated carbon surface, and dry at 80 DEG C of temperature, make combination electrode.By active carbon, acetylene black, butadiene-styrene rubber (SBR), carboxymethyl cellulose (CMC) in mass ratio 80:10:7:3 mix, with water furnishing slurry, be sprayed at aluminum foil current collector surface, and dry at 110 DEG C of temperature, preparation conventional electrodes.Again according to a conventional method by electrode roll-in, cut into given size, vacuumize, between anode composite and activated carbon negative electrode, arrange barrier film, add electrolyte, stack of laminations dresses up button ultracapacitor.60% collection liquid surface of combination electrode arranges active carbon, remains 40% collection liquid surface and activated carbon surface arranges Polyglycolic acid fibre, and the Thickness Ratio of active carbon and Polyglycolic acid fibre is 1:5.
embodiment 8: by active carbon, Ketjen black, butadiene-styrene rubber (SBR), carboxymethyl cellulose (CMC) in mass ratio 80:10:7:3 mix, with water furnishing slurry, coat aluminum foil current collector surface, and dry at 110 DEG C of temperature.Prepare polypyrrole with electrochemical polymerization in activated carbon surface, and dry at 80 DEG C of temperature, make combination electrode.Again according to a conventional method by electrode roll-in, cut into given size, vacuumize, between anode composite and composite negative pole, arrange barrier film, add electrolyte, lamination or winding are assembled into Soft Roll ultracapacitor.50% collection liquid surface of combination electrode arranges active carbon, remains 50% collection liquid surface and activated carbon surface arranges polypyrrole, and the Thickness Ratio of active carbon and polypyrrole is 1:10.
embodiment 9: by Graphene, acetylene black, butadiene-styrene rubber (SBR), carboxymethyl cellulose (CMC) in mass ratio 40:10:7:3 mix, with water furnishing slurry, coat aluminum foil current collector surface, and dry at 110 DEG C of temperature.By polyaniline, acetylene black, butadiene-styrene rubber (SBR), carboxymethyl cellulose (CMC) in mass ratio 80:10:7:3 mix, with water furnishing slurry, then be sprayed at graphenic surface, and dry at 110 DEG C of temperature, make combination electrode.Again according to a conventional method by electrode roll-in, cut into given size, vacuumize, between anode composite and composite negative pole, arrange barrier film, add electrolyte, lamination or winding are assembled into ultracapacitor.40% collection liquid surface of combination electrode arranges Graphene, remains 60% collection liquid surface and graphenic surface arranges polyaniline, and the Thickness Ratio of Graphene and polyaniline is 1:20.
embodiment 10: by carbon nano-tube, acetylene black, butadiene-styrene rubber (SBR), carboxymethyl cellulose (CMC) in mass ratio 40:10:7:3 mix, with water furnishing slurry, coat aluminum foil current collector surface, and dry at 110 DEG C of temperature.By polyaniline, acetylene black, butadiene-styrene rubber (SBR), carboxymethyl cellulose (CMC) in mass ratio 80:10:7:3 mix, with water furnishing slurry, then be sprayed at carbon nano tube surface, and dry at 110 DEG C of temperature, make combination electrode.Roll-in according to a conventional method, cuts into given size again, and vacuumize arranges barrier film between anode composite and composite negative pole, and add electrolyte, lamination or winding are assembled into ultracapacitor.30% collection liquid surface of combination electrode arranges carbon nano-tube, remains 70% collection liquid surface and carbon nano tube surface arranges polyaniline, and the Thickness Ratio of carbon nano-tube and polyaniline is 1:50.
embodiment 11: by active carbon, Ketjen black, butadiene-styrene rubber (SBR), carboxymethyl cellulose (CMC) in mass ratio 80:10:7:3 mix, with water furnishing slurry, coat aluminum foil current collector surface, and dry at 110 DEG C of temperature.Prepare polypyrrole with electrochemical polymerization in activated carbon surface, and dry at 80 DEG C of temperature, make combination electrode.Again according to a conventional method by electrode roll-in, cut into given size, vacuumize, between anode composite and composite negative pole, arrange barrier film, add electrolyte, lamination or winding are assembled into Soft Roll ultracapacitor.20% collection liquid surface of combination electrode arranges active carbon, remains 80% collection liquid surface and activated carbon surface arranges polypyrrole, and the Thickness Ratio of active carbon and polypyrrole is 1:80.
comparative example 1:by active carbon, acetylene black, butadiene-styrene rubber (SBR), carboxymethyl cellulose (CMC) in mass ratio 80:10:7:3 mix, with water furnishing slurry, then coat aluminum foil current collector surface, and dry at 110 DEG C of temperature, preparation conventional electrodes.Again according to a conventional method by electrode roll-in, cut into given size, vacuumize, between active carbon positive pole and activated carbon negative electrode, arrange barrier film, add electrolyte, lamination or winding are assembled into ultracapacitor.
Table 1 performance parameter table
In embodiment of the present invention 1-11, in ultracapacitor, in negative or positive electrode, at least one electrode is combination electrode, the specific capacitance of combination electrode is all obviously high compared with the activated carbon electrodes of comparative example 1, particularly the thickness proportion of embodiment 4-8 double layer electrodes active material and pseudocapacitors electrode active material is 10:1 ~ 1:10, the ratio capacitance of combination electrode is the highest, visible, to the electrode of combination electrode as ultracapacitor of pseudocapacitors electrode active material and electrical double layer capacitor electrodes active material be comprised, the energy density of ultracapacitor can be significantly improved.
In the present invention, be not limited only to column ultracapacitor, electrode is assembled into any one in sheet, square, button, column external form in the mode such as lamination, winding, also can be assembled into irregular external form.The foregoing is only preferred embodiment of the present invention, all equalizations done according to the present patent application the scope of the claims change and modify, and all should belong to covering scope of the present invention.
Claims (10)
1. a combination electrode, arranges composite electrode active material at collection liquid surface, it is characterized in that: described composite electrode active material comprises pseudocapacitors electrode active material and electrical double layer capacitor electrodes active material simultaneously; Described pseudocapacitors electrode active material is at least one in conducting polymer or metal oxide, and described electrical double layer capacitor electrodes active material is carbon active material.
2. combination electrode according to claim 1, is characterized in that: first arrange electrical double layer capacitor electrodes active material at collection liquid surface, then arranges pseudocapacitors electrode active material; Or pseudocapacitors electrode active material is first set at collection liquid surface, then electrical double layer capacitor electrodes active material is set; Wherein 20 ~ 100% of collection liquid surface electrical double layer capacitor electrodes active material is set.
3. combination electrode according to claim 1, is characterized in that: the Thickness Ratio of electrical double layer capacitor electrodes active material and pseudocapacitors electrode active material is 80:1 ~ 1:80.
4. combination electrode according to claim 3, is characterized in that: the Thickness Ratio of electrical double layer capacitor electrodes active material and pseudocapacitors electrode active material is 40:1 ~ 1:40.
5. combination electrode according to claim 1, is characterized in that: conducting polymer is polypyrrole and derivative, polythiophene and derivative thereof, Polyaniline and its derivative, polystyrene and derivative, polypyridine and derivative thereof, gathers at least one in benzene and its derivative, poly quinoline and derivative thereof.
6. combination electrode according to claim 1, is characterized in that: metal oxide is at least one in the oxide of manganese, ruthenium, cobalt, nickel, vanadium.
7. combination electrode according to claim 1, is characterized in that: carbon active material is at least one in active carbon, Graphene, CNT (carbon nano-tube), carbon gel, carbon fiber, soft carbon, hard carbon, graphite.
8. prepare a method for combination electrode as claimed in claim 1, it is characterized in that: electrical double layer capacitor electrodes active material comprises coating, spraying, dipping, printing, printing, electro-deposition in the method to set up of collection liquid surface; Pseudocapacitors electrode active material comprises coating, spraying, dipping, printing, printing, chemical deposition, electrochemical deposition in the method to set up of collection liquid surface.
9. an application for combination electrode as claimed in claim 1, is characterized in that: described combination electrode is as the electrode of ultracapacitor.
10. application according to claim 9, is characterized in that: at least one electrode in ultracapacitor in negative or positive electrode is described combination electrode; The assembling of ultracapacitor: arrange barrier film between positive pole and negative pole, add electrolyte, lamination or winding are assembled into ultracapacitor.
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