CN103117374B - Anode pole piece of lithium rechargeable battery and preparation method thereof - Google Patents
Anode pole piece of lithium rechargeable battery and preparation method thereof Download PDFInfo
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- CN103117374B CN103117374B CN201310053579.3A CN201310053579A CN103117374B CN 103117374 B CN103117374 B CN 103117374B CN 201310053579 A CN201310053579 A CN 201310053579A CN 103117374 B CN103117374 B CN 103117374B
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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
- Y02E60/10—Energy storage using batteries
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Abstract
The invention provides anode pole piece of a kind of lithium rechargeable battery and preparation method thereof.The anode pole piece of described lithium rechargeable battery comprises: plus plate current-collecting body; Primer coating, covers plus plate current-collecting body upper surface, comprises lithium complex metal oxide active material, conductive agent, bonding agent; And top coat, cover and together with primer coating compacting at plus plate current-collecting body and embed primer coating, comprise super capacitor Carbon Materials, conductive agent, bonding agent.Anode pole piece of lithium rechargeable battery provided by the invention and preparation method thereof, it can under the prerequisite not reducing volume energy density, obviously can improve the wettability of anode pole piece and electrolyte, therefore improve the utilance of positive electrode active materials, make efficiency first improve and can cycle performance be significantly improved.
Description
Technical field
The present invention relates to a kind of lithium rechargeable battery, particularly relate to anode pole piece of a kind of lithium rechargeable battery and preparation method thereof.
Background technology
Due to lithium rechargeable battery, there is volume energy density and mass energy density is high, the life-span is long, self discharge is low and the advantage such as environmental protection, be therefore widely used in the fields such as the portable electric appts such as mobile communication equipment, notebook computer and electric automobile.
Along with the fast development in the field such as consumer electronics product and electric automobile, more and more higher to the requirement of performance of lithium-ion secondary battery, especially also need to keep certain low temperature performance and cycle performance while volume energy density significantly improves.Volume energy density is got over high request and play more energy in limited space, on the basis of existing active material, therefore usually adopt higher compacted density to realize in limited space, storing more active materials to improve volume energy density.But when the compacted density of positive electrode active materials is too high, cause electrolyte to absorb difficulty, cycle performance is poor; Active material cannot make full use of, and it is low that gram volume plays efficiency, decrease in efficiency first; Electrolyte becomes difficulty by liquid phase to pole piece diffusion inside, and especially when low temperature, electrolyte becomes more difficult through the solid liquid interface of anode pole piece and electrolyte to the diffusion of anode pole piece internal particle by liquid phase, and therefore low temperature discharge polarization greatly, poor performance.Prior art causes the problem such as low temperature performance and cycle performance difference in order to improve because electrolyte infiltrates absorption, realize, but the increase of porosity can cause the reduction of volume energy density by controlling porosity.
Summary of the invention
In view of background technology Problems existing, the object of the present invention is to provide anode pole piece of a kind of lithium rechargeable battery and preparation method thereof, it can under the prerequisite not reducing volume energy density, obviously can improve the wettability of anode pole piece and electrolyte, thus improve positive electrode active materials utilance, make first efficiency improve and can cycle performance be significantly improved.
Another object of the present invention is to anode pole piece providing a kind of lithium rechargeable battery and preparation method thereof, when it can solve low temperature, electrolyte spreads slow problem by the solid liquid interface of anode pole piece and electrolyte to anode pole piece internal particle by liquid phase and can reduce the polarization resistance that lithium rechargeable battery discharges at low temperatures.
To achieve these goals, in a first aspect of the present invention, the invention provides a kind of anode pole piece of lithium rechargeable battery, it comprises: plus plate current-collecting body; Primer coating, covers plus plate current-collecting body upper surface, comprises lithium complex metal oxide active material, conductive agent, bonding agent; And top coat, cover and together with primer coating compacting at plus plate current-collecting body and embed primer coating, comprise super capacitor Carbon Materials, conductive agent, bonding agent.
In a second aspect of the present invention, present invention also offers a kind of preparation method of anode pole piece of lithium rechargeable battery, it comprises the following steps: lithium-contained composite metal oxide active material, conductive agent, bonding agent and solvent are obtained base pastes; By barrier coating slurry at plus plate current-collecting body on the surface, the solvent of evaporation barrier coating slurry, forms the bottom pole piece being coated with primer coating; Super capacitor Carbon Materials, conductive agent, bonding agent and solvent are obtained top level slurry; Top level slurry be coated in bottom pole piece, the solvent of evaporation top level slurry, forms the top layer pole piece being coated with top coat; By the roll-in of described top layer pole piece, obtain the anode pole piece of lithium rechargeable battery.
Beneficial effect of the present invention is as follows:
By lithium rechargeable battery prepared by anode pole piece of the present invention, under the prerequisite not reducing volume energy density, obviously can improve the wettability of anode pole piece and electrolyte, therefore improve the utilance of positive electrode active materials, make efficiency first improve and can cycle performance be significantly improved; Solve the electrolyte when low temperature simultaneously and spread slow problem by the solid liquid interface of anode pole piece and electrolyte to anode pole piece internal particle by liquid phase, reduce the polarization resistance that lithium rechargeable battery discharges at low temperatures.
Accompanying drawing explanation
Fig. 1 be according to anode pole piece roll-in of the present invention before and after cutaway view, wherein (a) is the cutaway view before roll-in, and (b) is the cutaway view after roll-in.
Wherein, description of reference numerals is as follows:
1 plus plate current-collecting body 2 primer coating 3 top coat
Embodiment
The following detailed description of anode pole piece and preparation method thereof and the embodiment of lithium rechargeable battery according to the present invention.
First the anode pole piece of lithium rechargeable battery is according to a first aspect of the present invention described.
As shown in Figure 1, wherein, the anode pole piece of lithium rechargeable battery according to a first aspect of the present invention comprises: plus plate current-collecting body 1; Primer coating 2, covers plus plate current-collecting body 1 upper surface, comprises lithium complex metal oxide active material, conductive agent, bonding agent; And top coat 3, to cover and compacting embeds primer coating 2 at plus plate current-collecting body 1 and comprises super capacitor Carbon Materials, conductive agent, bonding agent together with primer coating 2.Because Supercapacitor carbon material internal has flourishing crossover network passage for lithium ion fast transferring, the complicated pore structure in surface makes super capacitor Carbon Materials have higher specific surface, can the organic solvent of adsorption desorption electrolyte and lithium ion fast.
As shown in Figure 1, plus plate current-collecting body 1 is formed the liquid-adsorption layer (with dashed rectangle sign and hereinafter referred to as sponge liquid-adsorption layer) of similar " sponge ", thus the anode pole piece surface imbibition difficulty improved because high compacted density brings, under shortening low temperature, electrolyte is by the path of liquid phase to electrode interior particles diffusion.In actual production, primer coating 2 and top coat 3 are set plus plate current-collecting body 1 positive and negative two surfaces (as shown in Figure 1), can certainly only arrange at a face (front or reverse side).
In the anode pole piece of lithium rechargeable battery according to a first aspect of the present invention, preferably, the lithium-contained composite metal oxide active material in primer coating 2 is selected from one in lithium and cobalt oxides, lithium nickel oxide, lithium manganese oxide, manganese nickel cobalt composite oxides, lithium-barium oxide, oxide/lithium ferrite or two or more.
In the anode pole piece of lithium rechargeable battery according to a first aspect of the present invention, preferably, the thickness of top coat 3 is 1.0 ~ 12 μm, is more preferably 3.0 ~ 9.0 μm.It should be noted, thickness here refers to top coat 3 and to cover after primer coating 2 and at the thickness of compacting before plus plate current-collecting body 1 together with primer coating 2.The described thickness benefits of top coat 3 is in the sponge liquid-adsorption layer forming suitable thickness in primer coating 2, the compacted density of lithium complex metal oxide active material in such increase primer coating 2 within reason, and increase adsorbance, minimizing lithium ion the evolving path, increasing lithium ion diffusion rate.
In the anode pole piece of lithium rechargeable battery according to a first aspect of the present invention, preferably, the super capacitor Carbon Materials in top coat 3 is the amorphous activated carbon granule of porous of high-ratio surface, activated carbon fiber or their combination.
In the anode pole piece of lithium rechargeable battery according to a first aspect of the present invention, preferably, the super capacitor Carbon Materials in top coat 3 accounts for the mass percent 37 ~ 62% of top coat 3, is more preferably 45 ~ 55%.Super capacitor Carbon Materials appropriate in top coat 3 is conducive to forming processing characteristics when preparing anode pole piece better for the nonactive slurry of top coat 3.
In the anode pole piece of lithium rechargeable battery according to a first aspect of the present invention, preferably, the conductive agent of top coat 3 is selected from least one in acetylene black, carbon black, carbon nano-tube, Delanium, native graphite.The electronics that conductive agent increases after making pole piece roll-in between lithium complex metal oxide active material in primer coating 2 and the super capacitor Carbon Materials in top coat 3 contacts.
In the anode pole piece of lithium rechargeable battery according to a first aspect of the present invention, preferably, the solvent in the bonding agent of top coat 3 is oleaginous system or water-based system.When the top level slurry of the base pastes and preparation top coat 3 of preparing primer coating 2 is oleaginous system, its bonding agent can select poly-inclined fluorine divinyl or derivatives thereof, and corresponding solvent can select 1-METHYLPYRROLIDONE or corresponding derivative; When base pastes and top level slurry are water-based systems, its binding agent can select butadiene-styrene rubber class or derivatives thereof, and thickener can select sodium carboxymethylcellulose, and solvent can select pure water.
In the anode pole piece of lithium rechargeable battery according to a first aspect of the present invention, in order to make to have higher adsorption capacity to the organic solvent in electrolyte and the short diffusion rate of lithium ion the evolving path is fast, preferably, the specific surface of the super capacitor Carbon Materials in top coat 3 is 800 ~ 2000m
2/ g; Be more preferably 1000 ~ 1600m
2/ g.
Secondly the preparation method of anode piece of lithium ion secondary battery is according to a second aspect of the present invention described.
The preparation method of the anode pole piece of lithium rechargeable battery according to a second aspect of the present invention, it, for the preparation of the anode pole piece of lithium rechargeable battery described according to a first aspect of the present invention, comprises the following steps: lithium-contained composite metal oxide active material, conductive agent, bonding agent and solvent are obtained base pastes; By barrier coating slurry at plus plate current-collecting body 1 on the surface, the solvent of evaporation barrier coating slurry, forms the bottom pole piece being coated with primer coating 2; Super capacitor Carbon Materials, conductive agent, bonding agent and solvent are obtained top level slurry; Top level slurry be coated in bottom pole piece, the solvent of evaporation top level slurry, forms the top layer pole piece being coated with top coat 3; By the roll-in of described top layer pole piece, obtain the anode pole piece of lithium rechargeable battery.
Embodiment, comparative example and test result according to the anode pole piece of lithium rechargeable battery of the present invention and preparation method thereof is finally described.
Embodiment 1
Prepare anode pole piece
First bottom pole piece: get binding agent polyvinylidene fluoride (PVDF) and be dissolved in solvent N-methyl pyrilidone (NMP), fully dissolves until solution clarification; Conductive carbon (supper-P) and nickle cobalt lithium manganate (NCM) are added in above-mentioned solution, be mixed into slurry, wherein the ratio of the solid masses of NCM, supper-P and PVDF is 94:3:3, and the solid content of pulp solution is 70%; Be coated on by slurry in 16 μm of thick blank aluminum foil current collector (plus plate current-collecting body), volatilize completely through oven cooking cycle solvent, positive and negative coating layer thickness is respectively 70 μm, obtains the bottom pole piece being coated with primer coating;
Next prepares the top layer pole piece of anode pole piece: be 1300m by specific surface
2the activated carbon fiber of/g and conductive carbon (supper-P) mix and then add bonding agent butadiene-styrene rubber and fully mix and add thickener sodium carboxymethylcellulose CMC and pure water is modulated into the slurry that solid content is 9%, wherein by percentage to the quality, activated carbon fiber: conductive carbon: sodium carboxymethylcellulose: butadiene-styrene rubber=52:8:13:27, slurry is coated on the bottom pole piece of above-mentioned preparation, through oven cooking cycle until moisture volatilizees completely, the top coat of positive and negative is 5 μm, obtains the bottom pole piece being coated with top coat;
Final molding: finally by the roll-in of described top layer pole piece, obtained anode pole piece, compacted density is 3.4g/cm
3, the pole piece thickness after compacting is 113 μm.
Prepare cathode pole piece
By graphite, conductive agent supper-P, thickener carboxymethylcellulose sodium solution, bonding agent butadiene-styrene rubber and the even form slurry of pure water dispersed with stirring (wherein graphite: conductive agent: stabilizer: the mass ratio of bonding agent is 95.5:1.5:1.3:1.7), be coated on blank Copper Foil, obtain cathode pole piece through baking cold compaction;
Prepare lithium rechargeable battery
Both positive and negative polarity pole piece and barrier film (adopting PE single-layer septum) are made battery core by winding method; Then battery core is loaded battery case, through baking except desolventizing; Then electrolyte (1MLiPF is injected
6eC/EMC/DEC electrolyte, wherein the mass ratio of EC:EMC:DEC is 5:3:2); Welded seal, then through changing into, aging technique obtains lithium rechargeable battery.
Embodiment 2
Prepare anode pole piece: remainder is with to prepare anode pole piece step in embodiment 1 identical, and the specific surface of difference and top coat super capacitor Carbon Materials used is 2000m
2/ g; After compacting, pole piece thickness is 113 μm.
Prepare cathode pole piece, prepare lithium rechargeable battery all with embodiment 1.
Embodiment 3
Prepare anode pole piece: remainder is with to prepare anode pole piece step in embodiment 1 identical, and the specific surface of difference and top coat super capacitor Carbon Materials used is 800m
2/ g; After compacting, pole piece thickness is 113 μm.Prepare cathode pole piece, prepare lithium rechargeable battery all with embodiment 1.
Embodiment 4
Prepare anode pole piece: remainder is with to prepare anode pole piece step in embodiment 1 identical, and the specific surface of difference and top coat super capacitor Carbon Materials used is 2200m
2/ g; After compacting, pole piece thickness is 113 μm.Prepare cathode pole piece, prepare lithium rechargeable battery all with embodiment 1.
Embodiment 5
Prepare anode pole piece: remainder is with to prepare anode pole piece step in embodiment 1 identical, and the specific surface of difference and top coat super capacitor Carbon Materials used is 500m
2/ g; After compacting, pole piece thickness is 113 μm.
Prepare cathode pole piece, prepare lithium rechargeable battery all with embodiment 1.
Embodiment 6
Prepare anode pole piece: remainder is with to prepare anode pole piece step in embodiment 1 identical, and difference and top coat thickness are 12 μm; After compacting, pole piece thickness is 113 μm.
Prepare cathode pole piece, prepare lithium rechargeable battery all with embodiment 1.
Embodiment 7
Prepare anode pole piece: remainder is with to prepare anode pole piece step in embodiment 1 identical, and difference and top coat thickness are 1 μm; After compacting, pole piece thickness is 113 μm.
Prepare cathode pole piece, prepare lithium rechargeable battery all with embodiment 1.
Embodiment 8
Prepare anode pole piece: remainder is with to prepare anode pole piece step in embodiment 1 identical, and difference and top coat thickness are 15 μm; After compacting, pole piece thickness is 113 μm.
Prepare cathode pole piece, prepare lithium rechargeable battery all with embodiment 1.
Embodiment 9
Prepare anode pole piece: remainder is with to prepare anode pole piece step in embodiment 1 identical, and difference and top coat thickness are 0.5 μm; After compacting, pole piece thickness is 113 μm.
Prepare cathode pole piece, prepare lithium rechargeable battery all with embodiment 1.
Comparative example 1
Prepare anode pole piece: remainder is with to prepare anode pole piece step in embodiment 1 identical, and difference is namely without top coat, and the anode pole piece compacted density obtained is 3.4g/cm
3;
Prepare cathode pole piece, prepare lithium rechargeable battery all with embodiment 1.After compacting, pole piece thickness is 113 μm.
Finally provide the performance of lithium-ion secondary battery test result of embodiment 1-9 and comparative example 1.
(1) efficiency comparative first: when the potential range of 3.0-4.2V, the first ratio of discharge capacity value and initial charge capability value;
(2) cycle performance contrast: 1C/1C circulation at 45 DEG C, voltage range is 3.0-4.2V, with capability retention when getting the 600th week;
(3) low temperature direct internal resistance (DCR) contrasts: completely filled by battery under being then discharged to 90%SOC, cooling battery surface temperature, to-25 DEG C, continues constant temperature 2h, with 0.5C constant-current discharge 10s, calculate the DCR of its correspondence, namely with voltage V when discharging initial
0deduct terminal voltage V1 during electric discharge 10s, then divided by discharging current 0.5C, obtain-25 DEG C, the DCR value of pulsed discharge 10s under 90%SOC.
(4) volume energy density is measured: carry out discharge and recharge with 1C/1C electric current, first 1C is completely put into 2.8V, then 1C is completely charged to 4.1V, constant voltage is to 0.05C, 1C is completely put into 2.8V again, record the discharge energy of battery at 2.8-4.1V voltage range, then obtain battery actual volume energy density divided by battery case volume.
The performance of lithium-ion secondary battery test of table 1 embodiment 1-9 and comparative example 1
In sum, the present invention by adopting super capacitor Carbon Materials in top coat, by regulating top coat thickness, the solid content of super capacitor Carbon Materials in top coat, top coat is made to be embedded in primer coating through compacting, " spongy layer " is formed on pole piece top layer, the chemical property of lithium rechargeable battery is significantly improved like this under the prerequisite not reducing volume energy density, improve the utilance (namely first efficiency) of positive electrode active materials, extend the cycle life of battery, and reduce low temperature discharge internal resistance.
Claims (8)
1. an anode pole piece for lithium rechargeable battery, is characterized in that, comprising:
Plus plate current-collecting body (1);
Primer coating (2), covers plus plate current-collecting body (1) on the surface, comprises lithium-contained composite metal oxide active material, conductive agent, bonding agent; And
Top coat (3), cover primer coating (2), compacting is plus plate current-collecting body (1) is upper and top coat (3) embeds primer coating (2) together with primer coating (2) for top coat (3), and top coat (3) comprises super capacitor Carbon Materials, conductive agent, bonding agent;
Wherein,
The thickness of top coat (3) is 1.0 ~ 12 μm;
The anode pole piece of described lithium rechargeable battery is obtained by following steps:
Lithium-contained composite metal oxide active material, conductive agent, bonding agent and solvent are obtained base pastes;
Base pastes is coated on plus plate current-collecting body (1) on the surface, the solvent of evaporation barrier coating slurry, forms the bottom pole piece being coated with primer coating (2);
Super capacitor Carbon Materials, conductive agent, bonding agent and solvent are obtained top level slurry;
Top level slurry be coated in bottom pole piece, the solvent of evaporation top level slurry, forms the top layer pole piece being coated with top coat (3);
By the roll-in of described top layer pole piece, obtain the anode pole piece of lithium rechargeable battery.
2. the anode pole piece of lithium rechargeable battery according to claim 1, it is characterized in that, the lithium-contained composite metal oxide active material in primer coating (2) is selected from one in lithium and cobalt oxides, lithium nickel oxide, lithium manganese oxide, manganese nickel cobalt composite oxides, lithium-barium oxide, oxide/lithium ferrite or two or more.
3. the anode pole piece of lithium rechargeable battery according to claim 1, is characterized in that, the thickness of top coat (3) is 3.0 ~ 9.0 μm.
4. the anode pole piece of lithium rechargeable battery according to claim 1, is characterized in that, the super capacitor Carbon Materials in top coat (3) is the amorphous activated carbon granule of porous of high-ratio surface, activated carbon fiber or their combination.
5. the anode pole piece of lithium rechargeable battery according to claim 1, is characterized in that, the mass percent that the super capacitor Carbon Materials in top coat (3) accounts for top coat is 37 ~ 62%.
6. the anode pole piece of lithium rechargeable battery according to claim 5, is characterized in that, the mass percent that the super capacitor Carbon Materials in top coat (3) accounts for top coat is 45 ~ 55%.
7. the anode pole piece of lithium rechargeable battery according to claim 1, is characterized in that, the specific surface of the super capacitor Carbon Materials in top coat (3) is 800 ~ 2000m
2/ g.
8. the anode pole piece of lithium rechargeable battery according to claim 7, is characterized in that, the specific surface of the super capacitor Carbon Materials in top coat (3) is 1000 ~ 1600m
2/ g.
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| CN103117374B true CN103117374B (en) | 2016-02-10 |
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Cited By (1)
| Publication number | Priority date | Publication date | Assignee | Title |
|---|---|---|---|---|
| US11901561B2 (en) | 2021-12-01 | 2024-02-13 | Contemporary Amperex Technology Co., Limited | Positive electrode sheet and secondary battery including the same, battery module, battery pack, and electrical apparatus |
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| KR101734642B1 (en) * | 2015-04-17 | 2017-05-11 | 현대자동차주식회사 | Positiveelectrode for lithium secondary cell and lithium secondary cell using the same |
| CN105680046A (en) * | 2016-03-25 | 2016-06-15 | 江苏富朗特新能源有限公司 | Sizing agents for external coatings of positive and negative electrode coils of lithium ion batteries |
| CN105680089A (en) * | 2016-03-25 | 2016-06-15 | 江苏富朗特新能源有限公司 | Positive/negative pole roll with dual coating layers for lithium ion battery |
| CN106910870A (en) * | 2017-03-28 | 2017-06-30 | 华南师范大学 | A kind of preparation method of super lithium ion cell positive |
| EP3731310B1 (en) * | 2017-12-20 | 2023-01-11 | Vehicle Energy Japan Inc. | Positive electrode for lithium ion secondary cell, and lithium ion secondary cell using same |
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| CN114068868A (en) * | 2020-07-31 | 2022-02-18 | 北京小米移动软件有限公司 | Pole piece, battery pack and manufacturing method of pole piece |
| CN112467075B (en) * | 2020-11-05 | 2022-01-04 | 东莞塔菲尔新能源科技有限公司 | Pole piece, electric core and secondary battery |
| CN113036080A (en) * | 2021-02-26 | 2021-06-25 | 蜂巢能源科技有限公司 | Positive pole piece and preparation method and application thereof |
| CN113690435B (en) * | 2021-07-02 | 2022-11-29 | 青岛中科赛锂达新能源技术合伙企业(有限合伙) | Lithium ion secondary battery pole piece and preparation method and application thereof |
| CN116864609A (en) * | 2023-05-31 | 2023-10-10 | 深圳材启新材料有限公司 | Positive electrode or negative electrode plate, preparation method thereof and application thereof in preparation of battery |
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