CN102938325A - Hybrid capacitor and preparation method thereof - Google Patents
Hybrid capacitor and preparation method thereof Download PDFInfo
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- CN102938325A CN102938325A CN2011102333161A CN201110233316A CN102938325A CN 102938325 A CN102938325 A CN 102938325A CN 2011102333161 A CN2011102333161 A CN 2011102333161A CN 201110233316 A CN201110233316 A CN 201110233316A CN 102938325 A CN102938325 A CN 102938325A
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Abstract
The invention belongs to the capacitor field, and discloses a hybrid capacitor and electrodes of the hybrid capacitor. The electrodes of the hybrid capacitor comprise a positive electrode and a negative electrode. Materials of the positive electrode comprise aluminum foil and positive electrode active materials composed of a graphene mixture, a first conductive agent and a first binder which are coated on the aluminum foil, and the graphene mixture comprises graphene and nickel cobalt manganese ternary materials in a mass ratio of 1: (0.1-1). Materials of the negative electrode comprise aluminum foil and negative electrode active materials composed of graphite, a second conductive agent and a second binder which are coated on the aluminum foil. According to the hybrid capacitor and a preparation method thereof, the negative electrode materials are provided with a low potential platform, so that the average working voltage of the hybrid capacitor is higher than that of a traditional double electric layer capacitor, and the system energy density is raised; and the positive electrode uses graphene with a high specific area and an outstanding conductivity, so that the internal resistance of the whole capacitor can be reduced effectively, and the hybrid capacitor can form a high specific capacitance.
Description
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, to the exploitation of electric automobile and to the demand of pulse power supply, more stimulated the research of people to electrochemical capacitor.The specific energy of electrochemical capacitor is still lower at present, and the specific power of battery is lower, and people are just attempting to address this problem from two aspects: (1) unites use with battery and ultracapacitor, during normal operation, provides required power by battery; Start or when needing heavy-current discharge, then provided by capacitor, can improve on the one hand the bad shortcoming of cryogenic property of battery; Can solve the application scenario for the higher pulse current of power requirement, such as GSM, GPRS etc.Capacitor and battery are united use and can be extended 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 present energy device.(2) utilize the principle of electrochemical capacitor and battery, the exploitation capacitor is as new energy storage unit.
It is so-called fake capacitance device or the title pseudo-capacitance device (Pseudo-capacitor) of electrode material that nineteen ninety Giner company has released metal oxide containing precious metals.For further improving the specific energy of electrochemical capacitor, nineteen ninety-five, D.A.Evans etc. have proposed ideal polarized electrode and faraday's reaction electrode are combined the concept that consists of capacitor (Electrochemical Hybrid Capacitor, EHC or be called Hybrid capacitor).1997, ESMA company disclosed the concept of NiOOH/AC mixed capacitor, had disclosed the new technology of accumulator material and electrochemical mixed capacitor combination of materials.Calendar year 2001, G.G.Amatucci has reported 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.
Do the mixed capacitor of negative pole for graphite, the capacity of positive electrode has determined the capacity of whole system.But the most micropore specific area of active carbon with high specific surface area that adopts at present can't form effective capacitance, and the conductivity of absorbent charcoal material itself is not high simultaneously, has affected the capacitor internal resistance, so that capacitor energy density is low, causes the ratio electric capacity of capacitor low.
Summary of the invention
The object of the present invention is to provide a kind of energy density and than electric capacity higher mixed capacitor all.
A kind of mixed capacitor comprises positive pole, negative pole, the barrier film between described positive pole and negative pole and electrolyte; Described positive pole, negative pole and barrier film are immersed in the described electrolyte; Wherein, the material of described positive pole comprises aluminium foil and the mass ratio that is coated on the described aluminium foil is respectively 80～93: the positive electrode active materials that 2～10: 5～10 Graphene mixture, the first conductive agent and the first binding agent form, and described Graphene mixture comprises that mass ratio is 1: 0.1～1 Graphene and nickel-cobalt-manganese ternary material; The material of described negative pole comprises Copper Foil and the mass ratio that is coated on the described Copper Foil is respectively 80～93: the negative active core-shell material that 2～10: 5～10 graphite, the second conductive agent and the second binding agent form.
In the 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 the above-mentioned mixed capacitor, electrode material or electrolyte material are as follows:
Described Graphene is that specific area is 400～1000m
2The Graphene of/g;
Described the 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 the market and obtain;
Described the 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 solvent;
The chemical formula of described nickel-cobalt-manganese ternary material is LiNi
xCo
yMn
zO
20＜x＜1,0＜y＜1,0＜z＜1 wherein, x+y+z=1;
Described barrier film adopts capacitor pp barrier film commonly used.
Another object of the present invention is to provide the preparation method of above-mentioned mixed capacitor, its step is as follows:
S1, be that 1: 0.1～1 Graphene and nickel-cobalt-manganese ternary material mix and form the Graphene mixture with mass ratio;
S2, mass ratio is respectively 80～93: 2～10: 5～10 described Graphene mixture, the first conductive agent and the first binding agent are configured to positive electrode active materials, and mass ratio is respectively 80～93: 2～10: 5～10 graphite, the second conductive agent and the second binding agent are configured to negative active core-shell material;
S3, described positive electrode active materials is coated on the aluminium foil, drying makes positive pole after processing; Described negative active core-shell material is coated on the Copper Foil, and drying makes negative pole after processing;
S4, described positive pole, negative pole and barrier film are entered to be equipped with in the container of electrolyte according to the assembling of the order of positive pole/barrier film/negative pole is rearmounted, obtain described mixed capacitor.
Among the above-mentioned preparation method, among the 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 current potential platform, so that the average working voltage of mixed capacitor is higher than traditional electric double layer mixed capacitor, thereby the energy density of system is risen; And positive pole has adopted the Graphene that specific area is higher, conductivity is good, and it can effectively reduce the internal resistance of whole mixed capacitor, can make again the higher ratio electric capacity of formation of mixed capacitor; Can add ion embedding one behind the anodal mixed Ni cobalt-manganese ternary material and take off embedding mechanism, improve capacity, and the low price of ternary material, and stable cycle performance.
Description of drawings
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 anodal 6, negative pole 7, between described anodal 6 and negative pole 7 between barrier film 3 and electrolyte 8, the order assembling is rearmounted enters to fill in the container 9 of electrolyte 8 according to anodal 6/ barrier film, 3/ negative pole 7 for described anodal 6, negative pole 7, barrier film 3; Anodal 6 material comprises aluminium foil 1 and the mass ratio that is coated on the described aluminium foil 1 is respectively 80～93: the positive electrode active materials 2 that 2～10: 5～10 Graphene mixture, the first conductive agent and the first binding agent form, and described Graphene mixture comprises that mass ratio is 1: 0.1～1 Graphene and nickel-cobalt-manganese ternary material; The material of negative pole 7 comprises Copper Foil 5 and the mass ratio that is coated on the described Copper Foil 5 is respectively 80～93: the negative active core-shell material 4 that 2～10: 5～10 graphite, the second conductive agent and the second binding agent form; Wherein, in anodal 6 the material, Graphene is used for the surface and forms electric double layer, and the nickel-cobalt-manganese ternary material is used for ion embedding-Tuo embedding memory capacity.
In the 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 the above-mentioned mixed capacitor, electrode material or electrolyte material are as follows:
Graphene is that specific area is 400～1000m
2The Graphene of/g also can be selected the Graphene that carries out surface modification, as, the surface modified graphite alkene of the elements such as the B that mixes, N, O, F;
The chemical formula of nickel-cobalt-manganese ternary material is LiNi
xCo
yMn
zO
2, 0＜x＜1,0＜y＜1,0＜z＜1 wherein, x+y+z=1;
The 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 the market and obtain;
The 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 solvent; Lithium-ion electrolyte salt in the electrolyte is LiPF
6, LiBF
4, LiBOB, LiCF
3SO
3, LiN (SO
2CF
3) or LiAsF
6In one or more; Non-aqueous organic solvent in the 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 the acetonitrile;
Described barrier film can adopt the pp barrier film.
Another object of the present invention is to provide the preparation method of above-mentioned mixed capacitor, as shown in Figure 2, comprise that step is as follows:
S1, be that 1: 0.1～1 Graphene and nickel-cobalt-manganese ternary material mix and form the Graphene mixture with mass ratio; Wherein, the chemical formula of nickel-cobalt-manganese ternary material is LiNi
xCo
yMn
zO
2, in the formula, 0＜x＜1,0＜y＜1,0＜z＜1, x+y+z=1;
S2, mass ratio is respectively 80～93: 2～10: 5～10 described Graphene mixture, the first conductive agent and the first binding agent are configured to positive electrode active materials, and mass ratio is respectively 80～93: 2～10: 5～10 graphite, the second conductive agent and the second binding agent are configured to negative active core-shell material;
S3, described positive electrode active materials is coated on the aluminium foil, drying makes positive pole after processing; Described negative active core-shell material is coated on the Copper Foil, and drying makes negative pole after processing;
S4, described positive pole, negative pole and barrier film are entered to be equipped with in the container of electrolyte according to required specification requirement and according to the assembling of the order of positive pole/barrier film/negative pole is rearmounted, obtain described mixed capacitor.
Among the above-mentioned preparation method, among the step S3, the mass ratio of described positive electrode active materials and described negative active core-shell material is 1: 1～1: 5.
Among the preparation method of above-mentioned mixed capacitor, electrode material, electrolyte material are as follows:
Graphene is that specific area is 400～1000m
2The Graphene of/g also can be selected the Graphene that carries out surface modification, as, the surface modified graphite alkene of the elements such as the B that mixes, N, O, F;
The first conductive agent and the second conductive agent are acetylene black, conductive black (such as, conductive black super P) or carbon nano-tube, and these conductive agents all can be bought by the market and obtain;
The 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 solvent; Lithium-ion electrolyte salt in the electrolyte is LiPF
6, LiBF
4, LiBOB, LiCF
3SO
3, LiN (SO
2CF
3) or LiAsF
6In one or more; Non-aqueous organic solvent in the 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 the acetonitrile;
Barrier film can adopt the pp barrier film.
The invention provides mixed capacitor, the material of its negative pole has low current potential platform, so that the average working voltage of mixed capacitor is higher than traditional electric double layer mixed capacitor, thereby the energy density of system is risen; And positive pole has adopted the Graphene that specific area is higher, conductivity is good, and it can effectively reduce the internal resistance of whole mixed capacitor, can make again the higher ratio electric capacity of formation of mixed capacitor; Can add ion embedding-Tuo embedding mechanism behind the anodal 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:
Anodal.(specific area is 400m with Graphene
2/ g) with the nickel-cobalt-manganese ternary material (such as, LiNi
0.15Co
0.45Mn
0.4O
2) mix rear the stirring 30 minutes according to 1: 1 ratio of mass ratio, obtain the Graphene mixture; The Graphene mixture, acetylene black conductor, the PVDF binding agent that then with mass ratio are 85: 10: 5 are made positive electrode active materials after mixing, and positive electrode active materials is coated on the aluminium foil, and 80 ℃ of baking 12h obtain anodal in vacuum;
Negative pole.Be to make negative active core-shell material after 85: 10: 5 graphite, acetylene black conductor, PVDF binding agent mixes with mass ratio, negative active core-shell material is coated on the Copper Foil, 80 ℃ of baking 12h obtain negative pole in vacuum.
Wherein, the mass ratio of the positive electrode active materials on the positive pole and the negative active core-shell material on the negative pole is 1: 1.
2, assembling mixed capacitor:
The above-mentioned positive pole that makes and annex are cut into required specification, and in glove box, according to the order assembling 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:
Anodal.(specific area is 700m with Graphene
2/ g) with the nickel-cobalt-manganese ternary material (such as, LiNi
0.65Co
0.15Mn
0.2O
2) mix rear the stirring 30 minutes according to 1: 0.2 ratio of mass ratio, obtain the Graphene mixture; The Graphene mixture, carbon nanotube conducting agent, the PVDF binding agent that then with mass ratio are 93: 2: 5 are made positive electrode active materials after mixing, and positive electrode active materials is coated on the aluminium foil, and 80 ℃ of baking 12h obtain anodal in vacuum;
Negative pole.Be to make negative active core-shell material after 93: 2: 5 graphite, carbon nanotube conducting agent, PVDF binding agent mixes with mass ratio, negative active core-shell material is coated on the Copper Foil, 80 ℃ of baking 12h obtain negative pole in vacuum.
Wherein, the mass ratio of the positive electrode active materials on the positive pole and the negative active core-shell material on the negative pole is 1: 2.
2, assembling mixed capacitor:
The above-mentioned positive pole that makes and annex are cut into required specification, and in glove box, according to the order assembling of positive pole/pp barrier film/negative pole, inject LiCF
3SO
3And the mixed electrolytic solution of acetonitrile, obtain mixed capacitor.
1, mixed capacitor electrode preparation:
Anodal.(specific area is 1000m with Graphene
2/ g) with the nickel-cobalt-manganese ternary material (such as, LiNi
0.25Co
0.1Mn
0.65O
2) mix rear the stirring 30 minutes according to 1: 0.5 ratio of mass ratio, obtain the Graphene mixture; The Graphene mixture, conductive black conductive agent, the PTFE binding agent that then with mass ratio are 80: 10: 10 are made positive electrode active materials after mixing, and positive electrode active materials is coated on the aluminium foil, and 80 ℃ of baking 12h obtain anodal in vacuum;
Negative pole.Be to make negative active core-shell material after 80: 10: 10 graphite, conductive black super P conductive agent, PTFE binding agent mixes with mass ratio, negative active core-shell material is coated on the Copper Foil, 80 ℃ of baking 12h obtain negative pole in vacuum.
Wherein, the mass ratio of the positive electrode active materials on the positive pole and the negative active core-shell material on the negative pole is 1: 5.
2, assembling mixed capacitor:
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 that above embodiment is assembled into carries out the constant current charge-discharge test, and the different energy densities and the cycle life that obtain are such as table 1.The energy density of present 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, above-mentioned statement for preferred embodiment of the present invention is comparatively detailed, can not therefore think the restriction to scope of patent protection of the present invention, and 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, the barrier film between described positive pole and negative pole and electrolyte; Described positive pole, negative pole and barrier film are immersed in the described electrolyte; It is characterized in that, the material of described positive pole comprises aluminium foil and the mass ratio that is coated on the described aluminium foil is respectively 80～93: the positive electrode active materials that 2～10: 5～10 Graphene mixture, the first conductive agent and the first binding agent form, and described Graphene mixture comprises that mass ratio is 1: 0.1～1 Graphene and nickel-cobalt-manganese ternary material; The material of described negative pole comprises Copper Foil and the mass ratio that is coated on the described Copper Foil is respectively 80～93: the negative active core-shell material that 2～10: 5～10 graphite, the second conductive agent and the second binding agent form.
2. mixed capacitor according to claim 1 is characterized in that, described Graphene is that specific area is 400～1000m
2The Graphene of/g; Described the first conductive agent and the second conductive agent are acetylene black, conductive black or carbon nano-tube; Described the first binding agent and the second binding agent are Kynoar or polytetrafluoroethylene.
3. the mixed capacitor of stating according to claim 1 is characterized in that, the chemical formula of described nickel-cobalt-manganese ternary material is LiNi
xCo
yMn
zO
20＜x＜1,0＜y＜1,0＜z＜1 wherein, x+y+z=1.
4. according to claim 1 to 3 arbitrary described mixed capacitors, it is characterized in that, described electrolyte is the formulated electrolyte of lithium-ion electrolyte salt and non-aqueous organic solvent.
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. the preparation method of a mixed capacitor is characterized in that, comprises the steps:
S1, be that 1: 0.1～1 Graphene and nickel-cobalt-manganese ternary material mix and form the Graphene mixture with mass ratio;
S2, mass ratio is respectively 80～93: 2～10: 5～10 described Graphene mixture, the first conductive agent and the first binding agent are configured to positive electrode active materials, and mass ratio is respectively 80～93: 2～10: 5～10 graphite, the second conductive agent and the second binding agent are configured to negative active core-shell material;
S3, described positive electrode active materials is coated on the aluminium foil, drying makes positive pole after processing; Described negative active core-shell material is coated on the Copper Foil, and drying makes negative pole after processing;
S4, insert in the container that electrolyte is housed after described positive pole, negative pole and barrier film turned according to the der group of positive pole/barrier film/negative pole, obtain described mixed capacitor.
7. the preparation method of mixed capacitor according to claim 6 is characterized in that, described Graphene is that specific area is 400～1000m
2The Graphene of/g; Described the first conductive agent and the second conductive agent are acetylene black, conductive black or carbon nano-tube; Described the first binding agent and the second binding agent are Kynoar or polytetrafluoroethylene.
8. the preparation method of the mixed capacitor of stating according to claim 6 is characterized in that, the chemical formula of described nickel-cobalt-manganese ternary material is LiNi
xCo
yMn
zO
20＜x＜1,0＜y＜1,0＜z＜1 wherein, x+y+z=1.
9. according to claim 6 to the preparation method of 8 arbitrary described mixed capacitors, it is characterized in that, among the step S3, the mass ratio of described positive electrode active materials and described negative active core-shell material is 1: 1～1: 5.
10. mixed capacitor according to claim 6 is characterized in that, among the step S4, described electrolyte is the formulated electrolyte of lithium-ion electrolyte salt and non-aqueous organic solvent.
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Cited By (3)
| Publication number | Priority date | Publication date | Assignee | Title |
|---|---|---|---|---|
| CN106816316A (en) * | 2017-03-15 | 2017-06-09 | 苏州海凌达电子科技有限公司 | A kind of ultracapacitor preparation method of manganese cobalt nickel base electrode |
| CN107256947A (en) * | 2017-05-17 | 2017-10-17 | 中国东方电气集团有限公司 | A kind of preparation method of conducting polymer lithium-ion energy storage device |
| US10944100B2 (en) | 2016-06-01 | 2021-03-09 | GM Global Technology Operations LLC | Electrochemical cell including anode and cathode including battery and capacitor particles and having equal electrochemical capacities, and method for forming the same |
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| US20050002150A1 (en) * | 2003-04-09 | 2005-01-06 | Volfkovich Yuri Mironovich | Positive electrode of an Electric Double Layer capacitor |
| CN101572327A (en) * | 2009-06-11 | 2009-11-04 | 天津大学 | Lithium ion battery adopting graphene as cathode material |
| CN101710619A (en) * | 2009-12-14 | 2010-05-19 | 重庆大学 | Electrode plate for lithium ion battery and manufacturing method thereof |
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2011
- 2011-08-15 CN CN201110233316.1A patent/CN102938325B/en not_active Expired - Fee Related
Patent Citations (3)
| Publication number | Priority date | Publication date | Assignee | Title |
|---|---|---|---|---|
| US20050002150A1 (en) * | 2003-04-09 | 2005-01-06 | Volfkovich Yuri Mironovich | Positive electrode of an Electric Double Layer capacitor |
| CN101572327A (en) * | 2009-06-11 | 2009-11-04 | 天津大学 | Lithium ion battery adopting graphene as cathode material |
| CN101710619A (en) * | 2009-12-14 | 2010-05-19 | 重庆大学 | Electrode plate for lithium ion battery and manufacturing method thereof |
Cited By (4)
| Publication number | Priority date | Publication date | Assignee | Title |
|---|---|---|---|---|
| US10944100B2 (en) | 2016-06-01 | 2021-03-09 | GM Global Technology Operations LLC | Electrochemical cell including anode and cathode including battery and capacitor particles and having equal electrochemical capacities, and method for forming the same |
| CN106816316A (en) * | 2017-03-15 | 2017-06-09 | 苏州海凌达电子科技有限公司 | A kind of ultracapacitor preparation method of manganese cobalt nickel base electrode |
| CN106816316B (en) * | 2017-03-15 | 2019-01-18 | 苏州海凌达电子科技有限公司 | A kind of preparation method of supercapacitor manganese cobalt nickel base electrode |
| CN107256947A (en) * | 2017-05-17 | 2017-10-17 | 中国东方电气集团有限公司 | A kind of preparation method of conducting polymer lithium-ion energy storage device |
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