CN102651484A - Energy storage device combining with characteristics of lithium ion battery and super-capacitor - Google Patents
Energy storage device combining with characteristics of lithium ion battery and super-capacitor Download PDFInfo
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Abstract
The invention relates to an energy storage device combining with characteristics of a lithium ion battery and a super-capacitor, which comprises a positive pole, a negative electrode, a diaphragm, electrolyte and a shell, wherein the positive pole and the negative electrode are respectively formed in a way that an active substance, a conductive additive and a binder are respectively coated on a current collector, wherein the positive pole active substance is a biomass activated carbon material which can perform ion reversible adsorption, and the negative electrode active substance is a lithium-titanium-oxygen compound which can perform lithium-ion reversible de-intercalation. The energy storage device combining with the characteristics of the lithium ion battery and the super-capacitor is formed as follows: the activated carbon material with the double-electrode-layer energy storage characteristic of the super-capacitor is combined with the lithium-titanium-oxygen compound with a de-intercalation lithium energy storage characteristic of the lithium ion battery, wherein the materials used in the forming process of the energy storage device are mature materials which are widely applied to energy storage devices, and the materials are environment-friendly, rich in resource, and relatively low in cost.
Description
Technical field
The present invention relates to a kind of energy storage device that has lithium ion battery and super capacitor characteristic concurrently, belong to battery and super capacitor technical field.
Background technology
The continuous development of new-energy automobile has promoted the continuous lifting of chemical power sources such as lead-acid battery, Ni-MH battery, lithium ion battery, fuel cell, super capacitor, metal-air cell, Zinc ion battery technology.Single dynamical system is difficult to satisfy instructions for use.The energy storage device that will have different-energy and the power characteristic use that combines when satisfying instructions for use, can improve the efficient of device greatly, increases the service life.For example; Lithium ion battery and super capacitor are formed composite power source, and as the power source of automobile, super capacitor can be in high-power output operating mode work such as startup, acceleration, climbing; Lithium ion battery provides the continual mileage required drive of automobile; The combination of the two has improved the power performance of automobile, has prolonged the useful life of battery.Lot of domestic and foreign car enterprise forms composite power source with itself and battery, is used for the operating mode of the high-power outputs such as startup, climbing, acceleration of car, raising battery utilization ratio, extending battery life; On the other hand, be applied to the city electric bus, utilize website to get on or off the bus the time, accomplish charging as main power source; Recently, have car enterprise that super capacitor is used for extended-range electric vehicle again, effect is obvious.But the energy density of super capacitor is lower, has limited its scale onboard and has used.
In order to improve the energy density of super capacitor, people carry out developing material from improving than two angles of electric capacity and raising voltage.Metal oxide can produce fake capacitance as electrode active material in the charge and discharge process of electric capacity, increase substantially the specific capacity of monomer.Application number 200910043613.2 has been reported a kind of ultracapacitor RuO that is used to prepare
2The coating and thermal decomposition process of electrode material.With RuCl
3And SnCl
2Be mixed with thick shape solution, evenly be coated on the substrate,, obtain RuO through 200～500 ℃ of heat treatments
2Thin-film material carries out electrochemical property test, reaches 612～634F/g than electric capacity.Application number 200910133119.5 has been introduced a kind of preparation method that is used for the expanded graphite/metal oxide composite of electrode of super capacitor.Transition metal oxide nano-particles is evenly disperseed to form stable dispersions through surfactant, expanded graphite is added in the dispersion liquid, placed 10～24 hours, the dry expanded graphite/metal oxide composite that gets.It is simple that this method prepares super capacitor active material technology, and cost is low, have very strong industrial application value.Application number 00819536.6 has been reported a kind of through gas phase process or liquid phase process preparation 2～20nm mesoporous carbon/metal oxide precursor; Change it into mesoporous carbon/metal oxide through heat treatment; The super capacitor of assembling significantly improves than electric capacity, reaches 254F/g.Application number 200910012011.0 newspapers
The road a kind of aqueous super electric capacity; 1.2～1.6V operating voltage by routine is brought up to 2.4～3.0V; This capacitor by manganese oxide/absorbent charcoal composite material as positive active material; Active carbon has electrochemical behavior and comparatively ideal power density and energy density preferably as negative electrode active material.
In recent years; When the outside of carrying out battery and super capacitor composite power power supply is optimized; The inside that has begun energy storage device combines, and mainly is with the characteristic element of a certain energy storage device and the characteristic element of other energy storage devices, through the optimal design of system; In same monomer, realize merging the power density of raising energy storage device, energy density etc.For example, the ultra battery of plumbous charcoal that lead-acid battery and super capacitor combine, the nickel charcoal super capacitor that Ni-MH battery combines with super capacitor, the lithium ion super battery capacitor that lithium ion battery combines with super capacitor (lithium ion super capacitor batteries, lithium-ion capacitor).
Application number 200910212790. 9 has been reported a kind of leaching colloidal charcoal super capacitor, and negative pole adopts activated carbon negative electrode, and the anodal lead that adopts is anodal, and electrolyte adopts colloidal electrolyte, and discharge capacity and high temperature performance significantly improve.It is anodal that application number 200810111891.2 has been introduced a kind of hickelous nydroxide that mixes CNT and carbonyl nickel, the ultracapacitor of the carbon fiber composition of handling with electronickelling, and maximum energy storage density reaches 20Wh/kg.Application number 201010265362. 5 has been introduced a kind of nano-nickel oxide combination electrode that is used for ultracapacitor and preparation method thereof, in Powdered nano oxidized nickel material, mixes a certain amount of metallic element and processes composite material, and the electrode specific capacity is high, and cost is low.Application number is 200410093962. 2 to have reported a kind of high voltage ultracapacitor; The negative material of the oxide of argentiferous is processed pastel to be coated on the metal forming; After negative plate is processed in dry, roll-in; Embedding lithium part again takes off lithiumation, with the anodal ultracapacitor of forming of active carbon, has the maximum operating voltage of about 4V.Application number 200710035205.3 has been reported a kind of superbattery electric capacity; Anodal active electrode material adopts lithium ion to embed the mixture of compound and porous carbon material; The negative electrode active electrode material adopts the mixture of porous carbon material and graphite type material; Have the characteristics of electric capacity and the difunctional energy storage of battery concurrently, when keeping lithium ion battery high voltage, high-energy-density, also have the high power density, heavy-current discharge of ultracapacitor, good characteristics such as cycle life.Application number 200810046091.7 has been reported a kind of C of containing, the high potential super capacitor electrode material of Fe and P element, and wherein the mass content of C is not less than 10%, and operating potential is with respect to Li
Ten/ Li can reach 4.3V, and good cyclical stability is arranged.Application number 201010280801.X has reported that a kind of LiFePO4 loads on active carbon as positive active material, and preparation method's cost is low, and the charge-discharge performance of superbattery electric capacity monomer is good, and specific capacity is greater than 60mAh/g under the 20C multiplying power.
Super capacitor has limited its scale and has used because it relies on the adsorpting aggregation ion energy storage of porous material, and energy density is lower.For battery, because electrode material generation chemical reaction, the power density of battery can't reach the level of super capacitor; The composite power source that forms is mated in battery and super capacitor outside, has increased the complexity of system, and the advantage of the two can not be given full play to.
Summary of the invention
The object of the present invention is to provide a kind of energy storage device that has lithium ion battery and super capacitor characteristic concurrently; The biomass-based active carbon of the electric double layer energy storage characteristic through having super capacitor; Be combined in the same monomer with the lithium titanyl material of doff lithium energy storage characteristic with lithium ion battery; Realized coupling, to the fusion of the energy storage device that has lithium ion battery and super capacitor characteristic concurrently of inside by the lithium ion battery and the super capacitor of outside.
Technical scheme of the present invention is achieved in that a kind of energy storage device that has lithium ion battery and super capacitor characteristic concurrently, it is characterized in that its preparation method is following: positive active material, conductive agent and binding agent are coated on the aluminium foil by mass ratio 80:15:5, cut; Dry; Apply another side and process positive plate, negative electrode active material, conductive agent and binding agent are coated on the aluminium foil by mass ratio 80～85:10～15:5, cut; Drying applies another side and processes negative plate; Separate with barrier film in the middle of the positive/negative plate, inject electrolyte, encapsulating housing obtains the energy storage device monomer; Wherein positive active material is to be processed by the biomass active charcoal, and its raw material adopts a kind of in rice husk, apricot shell, the stalk, specific area>=1200m
2/ g, (1) rice husk matrix activated carbon: will clean, the rice husk after the removal of impurities, and, be immersed in the potassium hydroxide solution of 2M and stirred 6 hours, and use deionized water wash, drying 380 ℃ of nitrogen atmosphere charings 2 hours; Then according to the rice husk of alkali carbon ratio 3:1 mixing potassium hydroxide and charing, leave standstill 12 hours after, 700 ℃ of activation 2 hours, deionized water wash, drying obtains the rice husk matrix activated carbon; (2) apricot based active carbon: the apricot shell after will cleaning, pulverizing, 400 ℃ of nitrogen atmosphere charings 2 hours, then according to the rice husk of alkali carbon ratio 3:1 mixing potassium hydroxide and charing; After leaving standstill 12 hours, at 750 ℃ of activation 1 hour, deionized water wash; Drying obtains the apricot based active carbon; (3) stalk matrix activated carbon: the stalk after will cleaning, pulverizing, 300 ℃ of nitrogen atmosphere charings 1 hour, then according to the stalk of alkali carbon ratio 3:1 mixing potassium hydroxide and charing; After leaving standstill 12 hours, at 700 ℃ of activation 1 hour, deionized water wash; Drying obtains the stalk matrix activated carbon; Negative electrode active material is the compound that lithium titanyl, Graphene and expanded graphite constitute, and deviates from energy storage through the embedding of lithium ion, and its quality ratio of components is 90～99:0.5～5:0.5～9.5; Barrier film is a kind of in polypropylene diaphragm, polyethylene barrier film, polypropylene and polyethylene composite film, the cellulose barrier film.
The expansion multiplying power of described expanded graphite is 250～380ml/g, particle diameter≤15um; Graphene is a sandwich construction, and thickness is 5～20nm, purity>=99.5%;
Described negative electrode active material is composited through mechanical means, comprises ball mill mixing, mechanical agitation, ultrasonic dispersion; Also can adopt the synthetic method of original position to obtain, in-situ synthesis is that lithium titanyl, Graphene, the expanded graphite that titanium dioxide and lithium salts generate mixes according to product metering proportion 90～99:0.5～5:0.5～9.5, fires for 600～800 ℃ to form;
Described electrolyte is by lithium salts and solvent composition, and lithium salts comprises that a kind of in hexafluoro phosphorus lithium, trifluoromethyl sulfonic acid lithium, lithium perchlorate, the LiBF4, solvent comprise a kind of in dimethyl carbonate, diethyl carbonate, propene carbonate, the acetonitrile solution.
Described conductive agent is a kind of in acetylene black, CNT, Graphene, the carbon nano-fiber.
Described binding agent is a Kynoar.
Good effect of the present invention is the material of the doff lithium energy storage characteristic of its electric double layer that will have super capacitor, lithium ion battery, merges in same monomer, has realized the coupling by the battery and the super capacitor of outside; To the combination of the battery and the super capacitor of inside, used material is the maturing material of energy storage device extensive use; Environmental friendliness, raw material sources are extensive, help reducing cost; It is high to have the ratio super capacitance energy density, bigger than power of battery density, the characteristics that have extended cycle life.
Description of drawings
Fig. 1 is a negative pole lithium titanyl compound XRD curve of the present invention.
Fig. 2 is the N of anodal rice husk matrix activated carbon of the present invention
2The adsorption-desorption thermoisopleth.
Fig. 3 is the charging and discharging curve of energy storage device of the present invention.
Embodiment
Below in conjunction with accompanying drawing and embodiment the present invention is described further: like Fig. 1,2, shown in 3; A kind of energy storage device that has lithium ion battery and super capacitor characteristic concurrently is characterized in that its preparation method is following: positive active material, conductive agent and binding agent are coated on the aluminium foil by mass ratio 80:15:5, cut; Dry; Apply another side and process positive plate, negative electrode active material, conductive agent and binding agent are coated on the aluminium foil by mass ratio 80～85:10～15:5, cut; Drying applies another side and processes negative plate; Separate with barrier film in the middle of the positive/negative plate, inject electrolyte, encapsulating housing obtains the energy storage device monomer; Positive active material is to be processed by the biomass active charcoal, and its raw material adopts a kind of in rice husk, apricot shell, the stalk, specific area>=1200m
2/ g, (1) rice husk matrix activated carbon: will clean, the rice husk after the removal of impurities, and, be immersed in the potassium hydroxide solution of 2M and stirred 6 hours, and use deionized water wash, drying 380 ℃ of nitrogen atmosphere charings 2 hours; Then according to the rice husk of alkali carbon ratio 3:1 mixing potassium hydroxide and charing, leave standstill 12 hours after, 700 ℃ of activation 2 hours, deionized water wash, drying obtains the rice husk matrix activated carbon; (2) apricot based active carbon: the apricot shell after will cleaning, pulverizing, 400 ℃ of nitrogen atmosphere charings 2 hours, then according to the rice husk of alkali carbon ratio 3:1 mixing potassium hydroxide and charing; After leaving standstill 12 hours, at 750 ℃ of activation 1 hour, deionized water wash; Drying obtains the apricot based active carbon; (3) stalk matrix activated carbon: the stalk after will cleaning, pulverizing, 300 ℃ of nitrogen atmosphere charings 1 hour, then according to the stalk of alkali carbon ratio 3:1 mixing potassium hydroxide and charing; After leaving standstill 12 hours, at 700 ℃ of activation 1 hour, deionized water wash; Drying obtains the stalk matrix activated carbon; Negative electrode active material is the compound that lithium titanyl, Graphene and expanded graphite constitute, and deviates from energy storage through the embedding of lithium ion, and its quality ratio of components is 90～99:0.5～5:0.5～9.5; Barrier film is a kind of in polypropylene diaphragm, polyethylene barrier film, polypropylene and polyethylene composite film, the cellulose barrier film.
The expansion multiplying power of described expanded graphite is 250～380ml/g, particle diameter≤15um; Graphene is a sandwich construction, and thickness is 5～20nm, purity>=99.5%.
Described negative electrode active material is composited through mechanical means, comprises ball mill mixing, mechanical agitation, ultrasonic dispersion; Also can adopt the synthetic method of original position to obtain, in-situ synthesis is that titanium dioxide, lithium salts, Graphene, expanded graphite mix according to product metering proportion (90～99:0.5～5:0.5～9.5), and 600～800 ℃ of sintering are processed.
Described electrolyte is by lithium salts and solvent composition, and lithium salts comprises that a kind of in hexafluoro phosphorus lithium, trifluoromethyl sulfonic acid lithium, lithium perchlorate, the LiBF4, solvent comprise a kind of in dimethyl carbonate, diethyl carbonate, propene carbonate, the acetonitrile solution.
Described conductive agent is a kind of in acetylene black, CNT, Graphene, the carbon nano-fiber.
Described binding agent is a Kynoar.
Embodiment 1:
99:0.5:0.5 takes by weighing lithium titanyl, Graphene and expanded graphite according to the quality ratio of components, and expanded graphite and lithium titanyl were mixed in NMP 2 hours, adds the nmp solution of Graphene; Mixed 4 hours; Remove and desolvate, process negative electrode active material, be coated on the aluminium foil according to negative electrode active material, acetylene black, Kynoar mass ratio 80:15:5; Cut, dry back is as cathode pole piece.
With clean, rice husk after the removal of impurities, 380 ℃ of nitrogen atmosphere charings 2 hours, be immersed in the potassium hydroxide solution of 2M and stirred 6 hours, use deionized water wash, drying; Then according to the rice husk of alkali carbon ratio 3:1 mixing potassium hydroxide and charing, leave standstill 12 hours after, 700 ℃ of activation 2 hours, deionized water wash, drying obtains the rice husk matrix activated carbon; Be coated on the aluminium foil according to active carbon, acetylene black, Kynoar mass ratio 80:15:5, cut, dry back is as positive plate, and both positive and negative polarity pole piece carrying active substance mass ratio is 2:1.
Positive plate, polypropylene diaphragm, negative plate are superposeed successively, be put in the button shell, vacuum environment, the ethyl carbonate electrolyte of adding 1M hexafluoro phosphorus lithium, energy storage device is processed in sealing.
Embodiment 2:
With lithium titanyl, Graphene and expanded graphite according to quality ratio of components 98:1:1 ball mill mixing; Process negative electrode active material, be coated on the aluminium foil, cut according to negative electrode active material, Graphene, Kynoar mass ratio 85:10:5; Dry; Apply another side,, connect lug as cathode pole piece.
With the apricot shell after cleaning, pulverizing, 400 ℃ of nitrogen atmosphere charings 2 hours, then according to the rice husk of alkali carbon ratio 3:1 mixing potassium hydroxide and charing, leave standstill 12 hours after, 750 ℃ of activation 1 hour, deionized water wash, drying obtains the apricot based active carbon.
Be coated on the aluminium foil according to active carbon, conductive carbon black, Kynoar mass ratio 80:15:5, cut, drying applies another side, as anode pole piece, connects lug, and both positive and negative polarity pole piece carrying active substance mass ratio is 1.8:1.
Positive plate, polyethylene barrier film, negative plate are superposeed successively, be put into and dash in the good aluminum plastic film shell, vacuum environment, the ethyl carbonate electrolyte of adding 1M hexafluoro phosphorus lithium, energy storage device is processed in sealing.
Embodiment 3:
Take by weighing lithium carbonate, titanium dioxide, Graphene and expanded graphite (lithium carbonate and titanium dioxide product lithium titanyl in the product: Graphene: expanded graphite quality ratio of components 90:5:5); Ball mill mixing is even; 750 ℃ of calcinings of nitrogen atmosphere 4h processes negative electrode active material; Be coated on the aluminium foil according to negative electrode active material, carbon nano-fiber, Kynoar mass ratio 85:10:5, cut, dry back is as cathode pole piece.
With the stalk after cleaning, pulverizing, 300 ℃ of nitrogen atmosphere charings 1 hour, then according to the stalk of alkali carbon ratio 3:1 mixing potassium hydroxide and charing, leave standstill 12 hours after, 700 ℃ of activation 1 hour, deionized water wash, drying obtains the stalk matrix activated carbon.
Be coated on the aluminium foil according to active carbon, conductive carbon black, Kynoar mass ratio 80:15:5, cut, dry back is as anode pole piece, and both positive and negative polarity pole piece carrying active substance mass ratio is 1.5:1.
Positive plate, polyethylene polypropylene composite diaphragm, negative plate are superposeed successively, reel, be put in the box hat, vacuum environment, the propene carbonate electrolyte of adding 1M hexafluoro phosphorus lithium, energy storage device is processed in sealing.
The material that it is used is the maturing material of energy storage device extensive use, environmental friendliness, and raw material sources are extensive, help reducing cost, and it is high to have the ratio super capacitance energy density, bigger than power of battery density, the characteristics that have extended cycle life.
Claims (6)
1. an energy storage device that has lithium ion battery and super capacitor characteristic concurrently is characterized in that its preparation method is following: positive active material, conductive agent and binding agent are coated on the aluminium foil by mass ratio 80:15:5, cut; Dry; Apply another side and process positive plate, negative electrode active material, conductive agent and binding agent are coated on the aluminium foil by mass ratio 80～85:10～15:5, cut; Drying applies another side and processes negative plate; Separate with barrier film in the middle of the positive/negative plate, inject electrolyte, encapsulating housing obtains the energy storage device monomer; Positive active material is to be processed by the biomass active charcoal, and its raw material adopts a kind of in rice husk, apricot shell, the stalk, specific area>=1200m
2/ g, (1) rice husk matrix activated carbon: will clean, the rice husk after the removal of impurities, and, be immersed in the potassium hydroxide solution of 2M and stirred 6 hours, and use deionized water wash, drying 380 ℃ of nitrogen atmosphere charings 2 hours; Then according to the rice husk of alkali carbon ratio 3:1 mixing potassium hydroxide and charing, leave standstill 12 hours after, 700 ℃ of activation 2 hours, deionized water wash, drying obtains the rice husk matrix activated carbon; (2) apricot based active carbon: the apricot shell after will cleaning, pulverizing, 400 ℃ of nitrogen atmosphere charings 2 hours, then according to the rice husk of alkali carbon ratio 3:1 mixing potassium hydroxide and charing; After leaving standstill 12 hours, at 750 ℃ of activation 1 hour, deionized water wash; Drying obtains the apricot based active carbon; (3) stalk matrix activated carbon: the stalk after will cleaning, pulverizing, 300 ℃ of nitrogen atmosphere charings 1 hour, then according to the stalk of alkali carbon ratio 3:1 mixing potassium hydroxide and charing; After leaving standstill 12 hours, at 700 ℃ of activation 1 hour, deionized water wash; Drying obtains the stalk matrix activated carbon; Negative electrode active material is the compound that lithium titanyl, Graphene and expanded graphite constitute, and deviates from energy storage through the embedding of lithium ion, and its quality ratio of components is 90～99:0.5～5:0.5～9.5; Barrier film is a kind of in polypropylene diaphragm, polyethylene barrier film, polypropylene and polyethylene composite film, the cellulose barrier film.
2. according to a kind of energy storage device that has lithium ion battery and super capacitor characteristic concurrently described in the claim 1, the expansion multiplying power that it is characterized in that described expanded graphite is 250～380ml/g, particle diameter≤15um; Graphene is a sandwich construction, and thickness is 5～20nm, purity>=99.5%.
3. according to a kind of energy storage device that has lithium ion battery and super capacitor characteristic concurrently described in the claim 1, it is characterized in that described negative electrode active material is composited through mechanical means, comprise ball mill mixing, mechanical agitation, ultrasonic dispersion; Also can adopt the synthetic method of original position to obtain, in-situ synthesis is that titanium dioxide, lithium salts, Graphene, expanded graphite mix according to product metering proportion 90～99:0.5～5:0.5～9.5, and 600～800 ℃ of sintering are processed.
4. according to a kind of energy storage device that has lithium ion battery and super capacitor characteristic concurrently described in the claim 1; It is characterized in that described electrolyte is by lithium salts and solvent composition; Lithium salts comprises that a kind of in hexafluoro phosphorus lithium, trifluoromethyl sulfonic acid lithium, lithium perchlorate, the LiBF4, solvent comprise a kind of in dimethyl carbonate, diethyl carbonate, propene carbonate, the acetonitrile solution.
5. according to a kind of energy storage device that has lithium ion battery and super capacitor characteristic concurrently described in the claim 1, it is characterized in that described conductive agent is a kind of in acetylene black, CNT, Graphene, the carbon nano-fiber.
6. according to a kind of energy storage device that has lithium ion battery and super capacitor characteristic concurrently described in the claim 1, it is characterized in that described binding agent is a Kynoar.
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