CN102938325B - Mixed capacitor and preparation method thereof - Google Patents

Mixed capacitor and preparation method thereof Download PDF

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Publication number
CN102938325B
CN102938325B CN201110233316.1A CN201110233316A CN102938325B CN 102938325 B CN102938325 B CN 102938325B CN 201110233316 A CN201110233316 A CN 201110233316A CN 102938325 B CN102938325 B CN 102938325B
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graphene
mixed capacitor
capacitor
positive pole
mass ratio
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CN102938325A (en
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周明杰
钟玲珑
王要兵
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Oceans King Lighting Science and Technology Co Ltd
Shenzhen Oceans King Lighting Engineering Co Ltd
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Oceans King Lighting Science and Technology Co Ltd
Shenzhen Oceans King Lighting Engineering Co Ltd
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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

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  • Electric Double-Layer Capacitors Or The Like (AREA)
  • Battery Electrode And Active Subsutance (AREA)

Abstract

The invention belongs to capacitor area, it discloses a kind of mixed capacitor electrode and capacitor; This mixed capacitor electrode comprises positive pole and negative pole; The material of positive pole comprises aluminium foil and is coated in the positive electrode active materials be made up of Graphene mixture, the first conductive agent and the first binding agent on aluminium foil, and Graphene mixture comprises Graphene and nickel-cobalt-manganese ternary material that mass ratio is 1: 0.1 ~ 1; The material of negative pole comprises aluminium foil and is coated in the negative active core-shell material be made up of graphite, the second conductive agent and the second binding agent on aluminium foil.The invention provides mixed capacitor, its negative material has low potential plateau, makes the average working voltage of mixed capacitor higher than traditional double electric layer capacitor, thus makes the energy density of system increase; And positive pole have employed specific area is higher, conductivity is excellent Graphene, it can effectively reduce the internal resistance of integral capacitor device, can make again the ratio capacitance that the formation of mixed capacitor is higher.

Description

Mixed capacitor and preparation method thereof
Technical field
The invention belongs to capacitor area, it relates to a kind of mixed capacitor.The invention still further relates to a kind of preparation method of this mixed capacitor.
Background technology
The nineties in 20th century, the exploitation to electric automobile and the demand to pulse power supply, more have stimulated the research of people to electrochemical capacitor.The specific energy of current electrochemical capacitor is still lower, and the specific power of battery is lower, people are just attempting to address this problem from two aspects: (1), by battery and ultracapacitor conbined usage, when normally working, provides required power by battery; When starting or need heavy-current discharge, then provided by capacitor, the shortcoming that the cryogenic property of battery is bad can be improved on the one hand; The application scenario for the higher pulse current of power requirement can be solved, as GSM, GPRS etc.Capacitor and battery conbined usage can extend the life of a cell, but this will increase the annex of battery, disagree with the developing direction such as short and small frivolous of current energy device.(2) utilize the principle of electrochemical capacitor and battery, exploitation capacitor is as new energy storage unit.
Nineteen ninety Giner company is proposed the so-called pseudocapacitors or title pseudocapacitor (Pseudo-capacitor) that metal oxide containing precious metals is electrode material.For improving the specific energy of electrochemical capacitor further, nineteen ninety-five, D.A.Evans etc. propose and ideal polarized electrode and faraday's reaction electrode are combined the concept (ElectrochemicalHybridCapacitor, EHC or be called Hybridcapacitor) forming capacitor.1997, ESMA company disclosed the concept of NiOOH/AC mixed capacitor, disclosed the new technology of accumulator material and electrochemical mixed capacitor combination of materials.Calendar year 2001, G.G.Amatucci reports the Li of organic system lithium ion battery material and active carbon combination 4ti 5o 12/ AC electrochemical capacitor is another milestone of electrochemical capacitor development.
Graphite is done to the mixed capacitor of negative pole, the capacity of positive electrode determines the capacity of overall system.But the most micropore specific area of active carbon with high specific surface area adopted at present cannot form effective capacitance, the conductivity of absorbent charcoal material itself is not high simultaneously, have impact on capacitor internal resistance, makes capacitor energy density low, cause the ratio capacitance of capacitor low.
Summary of the invention
The object of the present invention is to provide the mixed capacitor that a kind of energy density and ratio capacitance are all higher.
A kind of mixed capacitor, comprises positive pole, negative pole, barrier film between described positive pole and negative pole and electrolyte; Described positive pole, negative pole and barrier film are immersed in described electrolyte; Wherein, the material of described positive pole comprises aluminium foil and the mass ratio be coated on described aluminium foil is respectively the Graphene mixture of 80 ~ 93: 2 ~ 10: 5 ~ 10, the positive electrode active materials of the first conductive agent and the first binding agent composition, and described Graphene mixture comprises Graphene and nickel-cobalt-manganese ternary material that mass ratio is 1: 0.1 ~ 1; The material of described negative pole comprises Copper Foil and the mass ratio be coated on described Copper Foil be respectively 80 ~ 93: 2 ~ 10: 5 ~ 10 graphite, the second conductive agent and the second binding agent composition negative active core-shell material.
In above-mentioned mixed capacitor, the mass ratio of described positive electrode active materials and described negative active core-shell material is 1: 1 ~ 1: 5.
In above-mentioned mixed capacitor, electrode material or electrolyte material as follows:
Described Graphene is specific area is 400 ~ 1000m 2the Graphene of/g;
Described first conductive agent and the second conductive agent are acetylene black, conductive black or carbon nano-tube, and these conductive agents all can be bought by market and obtain;
Described first binding agent and the second binding agent are Kynoar (PVDF) or polytetrafluoroethylene (PTFE);
Described electrolyte is the formulated electrolyte of lithium-ion electrolyte salt and Non-aqueous Organic Solvents;
The chemical formula of described nickel-cobalt-manganese ternary material is LiNi xco ymn zo 2; Wherein 0 < x < 1,0 < y < 1,0 < z < 1, x+y+z=1;
Described barrier film adopts the pp barrier film that capacitor is conventional.
Another object of the present invention is to the preparation method providing above-mentioned mixed capacitor, its step is as follows:
S1, by mass ratio be 1: 0.1 ~ 1 Graphene and nickel-cobalt-manganese ternary material mixing composition Graphene mixture;
S2, the described Graphene mixture, the first conductive agent and the first binding agent that mass ratio are respectively 80 ~ 93: 2 ~ 10: 5 ~ 10 are configured to positive electrode active materials, and the graphite, the second conductive agent and the second binding agent that mass ratio are respectively 80 ~ 93: 2 ~ 10: 5 ~ 10 are configured to negative active core-shell material;
S3, described positive electrode active materials is coated on aluminium foil, after drying process, obtained positive pole; Described negative active core-shell material is coated on Copper Foil, after drying process, obtained negative pole;
S4, the order assembling according to positive pole/barrier film/negative pole of described positive pole, negative pole and barrier film is rearmountedly entered to be equipped with in the container of electrolyte, obtain described mixed capacitor.
In above-mentioned preparation method, in step S3, the mass ratio of described positive electrode active materials and described negative active core-shell material is 1: 1 ~ 1: 5.
The invention provides mixed capacitor, the material of its negative pole has low potential plateau, makes the average working voltage of mixed capacitor higher than traditional electric double layer mixed capacitor, thus makes the energy density of system increase; And positive pole have employed specific area is higher, conductivity is excellent Graphene, it can effectively reduce the internal resistance of overall mixed capacitor, can make again the ratio capacitance that the formation of mixed capacitor is higher; Ion can be added after positive pole mixed Ni cobalt-manganese ternary material and embed a deintercalation mechanism, improve capacity, and the low price of ternary material, and stable cycle performance.
Accompanying drawing explanation
Fig. 1 is mixed capacitor structural representation of the present invention;
Fig. 2 is preparation technology's flow chart of mixed capacitor of the present invention.
Embodiment
A kind of mixed capacitor, as shown in Figure 1, comprise positive pole 6, negative pole 7, barrier film 3 between described positive pole 6 and negative pole 7 and electrolyte 8, described positive pole 6, negative pole 7, barrier film 3 are assembled according to positive pole 6/ barrier film 3/ negative pole 7 order and are rearmountedly entered to fill in the container 9 of electrolyte 8; The material of positive pole 6 comprises aluminium foil 1 and the mass ratio be coated on described aluminium foil 1 is respectively the Graphene mixture of 80 ~ 93: 2 ~ 10: 5 ~ 10, the positive electrode active materials 2 of the first conductive agent and the first binding agent composition, and described Graphene mixture comprises Graphene and nickel-cobalt-manganese ternary material that mass ratio is 1: 0.1 ~ 1; The material of negative pole 7 comprises Copper Foil 5 and the mass ratio be coated on described Copper Foil 5 be respectively 80 ~ 93: 2 ~ 10: 5 ~ 10 graphite, the second conductive agent and the second binding agent composition negative active core-shell material 4; Wherein, in the material of positive pole 6, Graphene is used for surface and forms electric double layer, and nickel-cobalt-manganese ternary material is used for ion embedding-deintercalation memory capacity.
In above-mentioned mixed capacitor, the mass ratio of described positive electrode active materials and described negative active core-shell material is 1: 1 ~ 1: 5.
In above-mentioned mixed capacitor, electrode material or electrolyte material as follows:
Graphene is specific area is 400 ~ 1000m 2the Graphene of/g, also can select the Graphene carrying out surface modification, e.g., carries out the surface modified graphite alkene of the elements such as doping B, N, O, F;
The chemical formula of nickel-cobalt-manganese ternary material is LiNi xco ymn zo 2, wherein 0 < x < 1,0 < y < 1,0 < z < 1, x+y+z=1;
First conductive agent and the second conductive agent are acetylene black, conductive black or carbon nano-tube, and these conductive agents all can be bought by market and obtain;
First binding agent and the second binding agent are Kynoar (PVDF) or polytetrafluoroethylene (PTFE);
Described electrolyte is the formulated electrolyte of lithium-ion electrolyte salt and Non-aqueous Organic Solvents; Lithium-ion electrolyte salt in electrolyte is LiPF 6, LiBF 4, LiBOB, LiCF 3sO 3, LiN (SO 2cF 3) or LiAsF 6in one or more; Non-aqueous Organic Solvents in electrolyte is one or more in dimethyl carbonate, diethyl carbonate, propene carbonate, ethylene carbonate, ethylene sulfite, propylene sulfite, butylene, r-butyrolactone, methyl ethyl carbonate alkene ester, methyl propyl carbonate, ethyl acetate or acetonitrile;
Described barrier film can adopt pp barrier film.
Another object of the present invention is to the preparation method that above-mentioned mixed capacitor is provided, as shown in Figure 2, comprise step as follows:
S1, by mass ratio be 1: 0.1 ~ 1 Graphene and nickel-cobalt-manganese ternary material mixing composition Graphene mixture; Wherein, the chemical formula of nickel-cobalt-manganese ternary material is LiNi xco ymn zo 2, in formula, 0 < x < 1,0 < y < 1,0 < z < 1, x+y+z=1;
S2, the described Graphene mixture, the first conductive agent and the first binding agent that mass ratio are respectively 80 ~ 93: 2 ~ 10: 5 ~ 10 are configured to positive electrode active materials, and the graphite, the second conductive agent and the second binding agent that mass ratio are respectively 80 ~ 93: 2 ~ 10: 5 ~ 10 are configured to negative active core-shell material;
S3, described positive electrode active materials is coated on aluminium foil, after drying process, obtained positive pole; Described negative active core-shell material is coated on Copper Foil, after drying process, obtained negative pole;
S4, described positive pole, negative pole and barrier film are rearmountedly entered to be equipped with in the container of electrolyte according to required specification requirement and according to the order assembling of positive pole/barrier film/negative pole, obtain described mixed capacitor.
In above-mentioned preparation method, in step S3, the mass ratio of described positive electrode active materials and described negative active core-shell material is 1: 1 ~ 1: 5.
In the preparation method of above-mentioned mixed capacitor, electrode material, electrolyte material are as follows:
Graphene is specific area is 400 ~ 1000m 2the Graphene of/g, also can select the Graphene carrying out surface modification, e.g., carries out the surface modified graphite alkene of the elements such as doping B, N, O, F;
First conductive agent and the second conductive agent are acetylene black, conductive black (e.g., conductive black superP) or carbon nano-tube, and these conductive agents all can be bought by market and obtain;
First binding agent and the second binding agent are Kynoar (PVDF) or polytetrafluoroethylene (PTFE);
Described electrolyte is the formulated electrolyte of lithium-ion electrolyte salt and Non-aqueous Organic Solvents; Lithium-ion electrolyte salt in electrolyte is LiPF 6, LiBF 4, LiBOB, LiCF 3sO 3, LiN (SO 2cF 3) or LiAsF 6in one or more; Non-aqueous Organic Solvents in electrolyte is one or more in dimethyl carbonate, diethyl carbonate, propylene carbonate vinegar, ethylene carbonate, ethylene sulfite, propylene sulfite, butylene, r-butyrolactone, methyl ethyl carbonate alkene ester, methyl propyl carbonate, ethyl acetate or acetonitrile;
Barrier film can adopt pp barrier film.
The invention provides mixed capacitor, the material of its negative pole has low potential plateau, makes the average working voltage of mixed capacitor higher than traditional electric double layer mixed capacitor, thus makes the energy density of system increase; And positive pole have employed specific area is higher, conductivity is excellent Graphene, it can effectively reduce the internal resistance of overall mixed capacitor, can make again the ratio capacitance that the formation of mixed capacitor is higher; Ion embedding-deintercalation mechanism can be added after positive pole mixed Ni cobalt-manganese ternary material, improve capacity, and the low price of ternary material, and stable cycle performance.
Below in conjunction with accompanying drawing, preferred embodiment of the present invention is described in further detail.
Embodiment 1
1, mixed capacitor electrode preparation:
Positive pole.By Graphene, (specific area is 400m 2/ g) and nickel-cobalt-manganese ternary material (e.g., LiNi 0.15co 0.45mn 0.4o 2) stir 30 minutes according to after the ratio mixing of mass ratio 1: 1, obtain Graphene mixture; Then be the Graphene mixture of 85: 10: 5 by mass ratio, acetylene black conductor, PVDF binding agent mixing after make positive electrode active materials, positive electrode active materials is coated on aluminium foil, in vacuum 80 DEG C baking 12h, obtain positive pole;
Negative pole.Be the graphite of 85: 10: 5 by mass ratio, acetylene black conductor, PVDF binding agent mixing after make negative active core-shell material, negative active core-shell material is coated on Copper Foil, in vacuum 80 DEG C baking 12h, obtain negative pole.
Wherein, the mass ratio of the positive electrode active materials on positive pole and the negative active core-shell material on negative pole is 1: 1.
2, mixed capacitor is assembled:
Above-mentioned obtained positive pole and annex are cut into required specification, and in glove box, assemble according to the order of positive pole/pp barrier film/negative pole, inject LiBF 4, propene carbonate and diethyl carbonate mixed electrolytic solution, obtain mixed capacitor.
Embodiment 2
1, mixed capacitor electrode preparation:
Positive pole.By Graphene, (specific area is 700m 2/ g) and nickel-cobalt-manganese ternary material (e.g., LiNi 0.65co 0.15mn 0.2o 2) stir 30 minutes according to after the ratio mixing of mass ratio 1: 0.2, obtain Graphene mixture; Then be the Graphene mixture of 93: 2: 5 by mass ratio, carbon nanotube conducting agent, PVDF binding agent mixing after make positive electrode active materials, positive electrode active materials is coated on aluminium foil, in vacuum 80 DEG C baking 12h, obtain positive pole;
Negative pole.Be the graphite of 93: 2: 5 by mass ratio, carbon nanotube conducting agent, PVDF binding agent mixing after make negative active core-shell material, negative active core-shell material is coated on Copper Foil, in vacuum 80 DEG C baking 12h, obtain negative pole.
Wherein, the mass ratio of the positive electrode active materials on positive pole and the negative active core-shell material on negative pole is 1: 2.
2, mixed capacitor is assembled:
Above-mentioned obtained positive pole and annex are cut into required specification, and in glove box, assemble according to the order of positive pole/pp barrier film/negative pole, inject LiCF 3sO 3and the mixed electrolytic solution of acetonitrile, obtain mixed capacitor.
Embodiment 3
1, mixed capacitor electrode preparation:
Positive pole.By Graphene, (specific area is 1000m 2/ g) and nickel-cobalt-manganese ternary material (e.g., LiNi 0.25co 0.1mn 0.65o 2) stir 30 minutes according to after the ratio mixing of mass ratio 1: 0.5, obtain Graphene mixture; Then be the Graphene mixture of 80: 10: 10 by mass ratio, conductive black conductive agent, PTFE binding agent mixing after make positive electrode active materials, positive electrode active materials is coated on aluminium foil, in vacuum 80 DEG C baking 12h, obtain positive pole;
Negative pole.Be the graphite of 80: 10: 10 by mass ratio, conductive black superP conductive agent, PTFE binding agent mixing after make negative active core-shell material, negative active core-shell material is coated on Copper Foil, in vacuum 80 DEG C baking 12h, obtain negative pole.
Wherein, the mass ratio of the positive electrode active materials on positive pole and the negative active core-shell material on negative pole is 1: 5.
2, mixed capacitor is assembled:
Positive pole and annex are cut into required specification, and in glove box, dress up according to the der group of positive pole/pp barrier film/negative pole, inject LiBF 4, dimethyl carbonate and ethylene carbonate mixed electrolytic solution, obtain mixed capacitor.
The mixed capacitor above embodiment be assembled into carries out constant current charge-discharge test, and the different energy density obtained and cycle life, as table 1.The energy density of current commercial maxwell ultracapacitor BCAP0350E270T09 is 5.62Wh/kg, and the energy density of other model is 1.38 ~ 5.62Wh/kg; Therefore, the more existing commercial mixed capacitor of mixed capacitor energy density of the present invention improves a lot.
Table 1
Should be understood that, the above-mentioned statement for present pre-ferred embodiments is comparatively detailed, and therefore can not think the restriction to scope of patent protection of the present invention, scope of patent protection of the present invention should be as the criterion with claims.

Claims (10)

1. a mixed capacitor, comprises positive pole, negative pole, barrier film between described positive pole and negative pole and electrolyte; Described positive pole, negative pole and barrier film are immersed in described electrolyte; It is characterized in that, the material of described positive pole comprises aluminium foil and the mass ratio be coated on described aluminium foil is respectively the positive electrode active materials of the Graphene mixture of 80 ~ 93:2 ~ 10:5 ~ 10, the first conductive agent and the first binding agent composition, and described Graphene mixture comprises Graphene and nickel-cobalt-manganese ternary material that mass ratio is 1:0.1 ~ 1; The material of described negative pole comprises Copper Foil and the mass ratio be coated on described Copper Foil is respectively the negative active core-shell material of the graphite of 80 ~ 93:2 ~ 10:5 ~ 10, the second conductive agent and the second binding agent composition;
Wherein, in the material of positive pole, Graphene is used for surface and forms electric double layer, and nickel-cobalt-manganese ternary material is used for ion embedding-deintercalation memory capacity.
2. mixed capacitor according to claim 1, is characterized in that, described Graphene is specific area is 400 ~ 1000m 2the Graphene of/g; Described first conductive agent and the second conductive agent are acetylene black, conductive black or carbon nano-tube; Described first binding agent and the second binding agent are Kynoar or polytetrafluoroethylene.
3. according to the mixed capacitor that claim 1 is stated, it is characterized in that, the chemical formula of described nickel-cobalt-manganese ternary material is LiNi xco ymn zo 2; Wherein 0 < x < 1,0 < y < 1,0 < z < 1, x+y+z=1.
4. according to the arbitrary described mixed capacitor of claims 1 to 3, it is characterized in that, described electrolyte is the formulated electrolyte of lithium-ion electrolyte salt and Non-aqueous Organic Solvents.
5. mixed capacitor according to claim 1, is characterized in that, the mass ratio of described positive electrode active materials and described negative active core-shell material is 1:1 ~ 1:5.
6. a preparation method for mixed capacitor, is characterized in that, comprises the steps:
S1, be Graphene and the nickel-cobalt-manganese ternary material mixing composition Graphene mixture of 1:0.1 ~ 1 by mass ratio;
S2, described Graphene mixture mass ratio being respectively 80 ~ 93:2 ~ 10:5 ~ 10, the first conductive agent and the first binding agent are configured to positive electrode active materials, and mass ratio are respectively the graphite of 80 ~ 93:2 ~ 10:5 ~ 10, the second conductive agent and the second binding agent and are configured to negative active core-shell material;
S3, described positive electrode active materials is coated on aluminium foil, after drying process, obtained positive pole; Described negative active core-shell material is coated on Copper Foil, after drying process, obtained negative pole;
S4, described positive pole, negative pole and barrier film are turned according to the der group of positive pole/barrier film/negative pole after insert and be equipped with in the container of electrolyte, obtain described mixed capacitor;
Wherein, in the material of positive pole, Graphene is used for surface and forms electric double layer, and nickel-cobalt-manganese ternary material is used for ion embedding-deintercalation memory capacity.
7. the preparation method of mixed capacitor according to claim 6, is characterized in that, described Graphene is specific area is 400 ~ 1000m 2the Graphene of/g; Described first conductive agent and the second conductive agent are acetylene black, conductive black or carbon nano-tube; Described first binding agent and the second binding agent are Kynoar or polytetrafluoroethylene.
8. the preparation method of the mixed capacitor stated according to claim 6, it is characterized in that, the chemical formula of described nickel-cobalt-manganese ternary material is LiNi xco ymn zo 2; Wherein 0 < x < 1,0 < y < 1,0 < z < 1, x+y+z=1.
9., according to the preparation method of the arbitrary described mixed capacitor of claim 6 to 8, it is characterized in that, in step S3, the mass ratio of described positive electrode active materials and described negative active core-shell material is 1:1 ~ 1:5.
10. the preparation method of mixed capacitor according to claim 6, is characterized in that, in step S4, described electrolyte is the formulated electrolyte of lithium-ion electrolyte salt and Non-aqueous Organic Solvents.
CN201110233316.1A 2011-08-15 2011-08-15 Mixed capacitor and preparation method thereof Expired - Fee Related CN102938325B (en)

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