CN104425846B - The lithium secondary battery for preparing the method for lithium secondary battery and being prepared using this method - Google Patents
The lithium secondary battery for preparing the method for lithium secondary battery and being prepared using this method Download PDFInfo
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- CN104425846B CN104425846B CN201410167785.1A CN201410167785A CN104425846B CN 104425846 B CN104425846 B CN 104425846B CN 201410167785 A CN201410167785 A CN 201410167785A CN 104425846 B CN104425846 B CN 104425846B
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- H—ELECTRICITY
- H01—ELECTRIC ELEMENTS
- H01M—PROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
- H01M10/00—Secondary cells; Manufacture thereof
- H01M10/05—Accumulators with non-aqueous electrolyte
- H01M10/058—Construction or manufacture
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- H—ELECTRICITY
- H01—ELECTRIC ELEMENTS
- H01M—PROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
- H01M10/00—Secondary cells; Manufacture thereof
- H01M10/05—Accumulators with non-aqueous electrolyte
- H01M10/058—Construction or manufacture
- H01M10/0585—Construction or manufacture of accumulators having only flat construction elements, i.e. flat positive electrodes, flat negative electrodes and flat separators
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- H—ELECTRICITY
- H01—ELECTRIC ELEMENTS
- H01M—PROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
- H01M10/00—Secondary cells; Manufacture thereof
- H01M10/05—Accumulators with non-aqueous electrolyte
- H01M10/052—Li-accumulators
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- H—ELECTRICITY
- H01—ELECTRIC ELEMENTS
- H01M—PROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
- H01M10/00—Secondary cells; Manufacture thereof
- H01M10/05—Accumulators with non-aqueous electrolyte
- H01M10/052—Li-accumulators
- H01M10/0525—Rocking-chair batteries, i.e. batteries with lithium insertion or intercalation in both electrodes; Lithium-ion batteries
-
- H—ELECTRICITY
- H01—ELECTRIC ELEMENTS
- H01M—PROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
- H01M50/00—Constructional details or processes of manufacture of the non-active parts of electrochemical cells other than fuel cells, e.g. hybrid cells
- H01M50/10—Primary casings, jackets or wrappings of a single cell or a single battery
- H01M50/116—Primary casings, jackets or wrappings of a single cell or a single battery characterised by the material
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- H—ELECTRICITY
- H01—ELECTRIC ELEMENTS
- H01M—PROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
- H01M50/00—Constructional details or processes of manufacture of the non-active parts of electrochemical cells other than fuel cells, e.g. hybrid cells
- H01M50/10—Primary casings, jackets or wrappings of a single cell or a single battery
- H01M50/116—Primary casings, jackets or wrappings of a single cell or a single battery characterised by the material
- H01M50/124—Primary casings, jackets or wrappings of a single cell or a single battery characterised by the material having a layered structure
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- H—ELECTRICITY
- H01—ELECTRIC ELEMENTS
- H01M—PROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
- H01M50/00—Constructional details or processes of manufacture of the non-active parts of electrochemical cells other than fuel cells, e.g. hybrid cells
- H01M50/40—Separators; Membranes; Diaphragms; Spacing elements inside cells
- H01M50/46—Separators, membranes or diaphragms characterised by their combination with electrodes
- H01M50/461—Separators, membranes or diaphragms characterised by their combination with electrodes with adhesive layers between electrodes and separators
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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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- 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
- Y02P—CLIMATE CHANGE MITIGATION TECHNOLOGIES IN THE PRODUCTION OR PROCESSING OF GOODS
- Y02P70/00—Climate change mitigation technologies in the production process for final industrial or consumer products
- Y02P70/50—Manufacturing or production processes characterised by the final manufactured product
Abstract
The present invention provides the methods for preparing lithium secondary battery and the lithium secondary battery prepared using the method, the method includes preparing lithium secondary battery and carrying out ageing process circulation at least twice on the electrode assembly in the stacking for being injected with electrolyte, wherein, the lithium secondary battery for preparing includes carrying out hot pressing circulation at least once under 95 DEG C or higher temperature on the electrode assembly between ageing process circulation.
Description
Cross reference to related applications
This application claims in the South Korea patent application 10-2013- submitted to Korean Intellectual Property Office on the 22nd of August in 2013
No. 0099878 equity, entire contents are incorporated herein by reference.
Technical field
One or more embodiments of the invention are related to preparing the method for lithium secondary battery and be prepared using the method
Lithium secondary battery.
Background technique
For being used in filling for information and the mobile electron of communication including personal digital assistant, mobile phone and laptop
Set and the demand of the secondary cell in electric bicycle or electric car rapidly increase, and according to manufacture compact size and
The trend of light-weight electronic device, can for it is compact, light-weight and can the lithium secondary battery that recharges of high capacity just in quotient
Industry.
Lithium secondary battery it is all types of in, lithium ion polymer battery is significantly paid close attention to.Lithium ion polymer electricity
The size and shape in pond can be controlled freely, and the energy density of the Unit Weight of lithium ion polymer battery is high.In order to make
These features of lithium ion polymer battery maximize, usually using pouch-type lithium ion polymer battery.
However, as safety detection, in 130 DEG C or heated higher temperature detection, since pouch-type lithium ion is poly-
Close the generation of object electricity pool gas, it may occur that short so as to cause with the deformation for the electrode assembly that the shape of film is wound
Road.It equally, include that partition in electrode assembly can be shunk on the direction MD or the direction TD, thus may occur in which hard short circuit or micro- short
Road (fine short).
Therefore, there is still a need for being manufactured and preventing the contraction for the partition for including in electrode assembly has improved safety
Lithium secondary battery method and using the method manufacture lithium secondary battery.
Summary of the invention
One or more embodiments of the invention include the method that preparation has the lithium secondary battery of improved safety.
One or more embodiments of the invention include the lithium secondary battery prepared using the method.
Other aspects will be partially illustrated in the following description, and to a certain extent, pass through these aspects of specification
It will be apparent or these aspects can be understood by implementing embodiment presented herein.
One or more embodiment according to the present invention, the method for preparing lithium secondary battery include by the first electricity of arrangement
Pole, second electrode and partition between the first electrode and the second electrode and prepare electrode assembly；Described in stacking
Electrode assembly simultaneously injects in electrolyte to the electrode assembly of the stacking；With by the stacking for being injected with the electrolyte
Electrode assembly on carry out at least twice ageing process (aging process, ageing process) recycle and prepare lithium secondary battery,
Wherein, it is described prepare lithium secondary battery include the ageing process circulation between on the electrode assembly in 95 DEG C or higher
At a temperature of carry out at least once hot pressing circulation.
In one embodiment, in about 200kgf/cm2To about 500kgf/cm2The heat is carried out under pressure in range
Press through journey.
In one embodiment, at a temperature in the range of about 95 DEG C to about 120 DEG C and about 250kgf/cm2To about
450kgf/cm2The hot pressing is carried out under pressure in range.
In one embodiment, the hot pressing carries out about 100 seconds to about 180 seconds.
In one embodiment, the ageing process is carried out at room temperature.
In one embodiment, in the preparation of the electrode assembly, the partition include substrate at least one
Polymer coating on surface.
In one embodiment, in the preparation of the electrode assembly, the polymer coating includes poly- based on fluorine
Close object or the copolymer based on fluorine.
In one embodiment, the polymer based on fluorine includes Kynoar.
In one embodiment, the copolymer based on fluorine is selected from by Kynoar-hexafluoropropene (PVdF-
HFP) copolymer, Kynoar-polytetrafluoroethylene (PTFE) (PVdF-PTFE) copolymer and Kynoar-polytetrafluoroethylene (PTFE)-hexafluoro
At least one of the group of propylene (PVdF-PTFE-HFP) copolymer composition
In one embodiment, the electrolyte is organic electrolyte.
One or more embodiment according to the present invention, provides the lithium secondary battery prepared using the method.
In one embodiment, the lithium secondary battery can be pouch-type battery.
Detailed description of the invention
By in the following explanation of the embodiment in conjunction with attached drawing, these and/or other aspects will be apparent and be easier
Understand, in which:
Fig. 1 is to illustrate that embodiment according to the present invention prepares the flow chart of the method for lithium secondary battery；
Fig. 2 is the diagrammatic cross-sectional view of the electrode assembly prepared according to embodiments of the present invention；
Fig. 3 be the lithium secondary battery that illustrates to prepare in embodiment 1 after the charge/discharge of standard 130 DEG C at a temperature of
The figure of the result of heated detection；
Fig. 4 be the lithium secondary battery that illustrates to prepare in comparative example 1 after the charge/discharge of standard 130 DEG C at a temperature of
The figure of the result of heated detection；
Fig. 5 be the lithium secondary battery that illustrates to prepare in comparative example 2 after the charge/discharge of standard 130 DEG C at a temperature of
The figure of the result of heated detection；
After Fig. 6 is standard charging/electric discharge, 130 DEG C at a temperature of kept for about 1 hour and prepared in the embodiment 1 decomposed
Lithium secondary battery optical microscope image.
Specific embodiment
It hereafter will be described in detail preparing described in the method and use of lithium secondary battery for embodiment according to the present invention
The lithium secondary battery of method preparation.Reference will now be made in detail to each embodiment, embodiment is shown in the drawings, wherein in the whole text
In identical appended drawing reference refer to identical element.In this respect, present embodiment can have different forms, should not explain
To be limited to the explanation proposed here.Therefore, these embodiments are described to explain this explanation only by reference to attached drawing below
The various aspects of book.As used herein, term "and/or" includes any and all group of one or more relevant listed items
It closes.It is modification permutation element, rather than modifying should when the expression of such as " at least one (one kind) " is when after a series of elements
Single element in column.
Embodiment according to the present invention provides the method for preparing lithium secondary battery, wherein the method includes passing through
Arrangement first electrode, second electrode and partition between the first electrode and second electrode and prepare electrode assembly；Heap
It folds the electrode assembly and injects in electrolyte to the electrode assembly of the stacking；With by the institute for being injected with the electrolyte
It states and carries out ageing process circulation at least twice on the electrode assembly of stacking and prepare lithium secondary battery, wherein is described to prepare lithium two
Primary cell includes carrying out at least under 95 DEG C or higher temperature on the electrode assembly between ageing process circulation
Hot pressing circulation.
Partition such as polyolefin in electrode assembly can be shunk under specific higher temperature, thus first electrode and
Adhesive strength between second electrode can weaken.Equally, it may appear that the short circuit in safety issue, such as lithium secondary battery.
As shown in Figure 1, the method for preparing lithium secondary battery is enterprising by the electrode assembly in the stacking for being injected with electrolyte
Ageing process recycles and prepares lithium secondary battery row at least twice, wherein can be between ageing process circulation in the heap
Hot pressing of at least one circulation, therefore first electrode and the are carried out on folded electrode assembly under 95 DEG C or higher temperature
Adhesive strength between two electrodes can enhance, to improve the intensity and safety of lithium secondary battery.
It can be in about 200kgf/cm2To about 500kgf/cm2The hot pressing is carried out under pressure in range.For example, can be
At a temperature in the range of about 95 DEG C to about 120 DEG C and about 250kgf/cm2To about 450kgf/cm2Institute is carried out under pressure in range
State hot pressing.The hot pressing can carry out about 100 seconds to about 180 seconds, preferably carry out about 100 seconds to about 150 seconds.
Hereinafter, it will illustrate the method for preparing lithium secondary battery of embodiment according to the present invention.
Firstly, preparing electrode assembly 10.Fig. 2 is the schematic of the electrode assembly 10 prepared according to embodiments of the present invention
Section view.
It can arrange by arrangement first electrode 11, second electrode 15 and between first electrode 11 and second electrode 15
Partition 16 and prepare electrode assembly 10.Partition 16 may include that substrate 13 and the polymer being formed on two surfaces of substrate 13 apply
Layer 12 and 14.
First electrode 11 is positive electrode, which can be prepared as the first electrode plate as positive electrode plate.
Preparation first electrode as described below: pass through mixed cathode active material, conductive material, jointing material and solvent system
Standby positive electrode active compound composition.It can be by being directly coated with and drying positive electrode active compound composition and system on aluminium electrode substrate
The standby first electrode plate for being formed with positive electrode active material layer thereon.Alternatively, positive electrode active compound composition may be cast in individually
On supporter, and the positive electrode active material films removed from above support can be laminated on aluminium electrode substrate, to prepare it
On be formed with the first electrode plate of the positive electrode active material layer.First electrode plate can be cut into suitably sized with the first electricity of preparation
Pole 11.
Any material usually used in this field can be used for positive active material, but particularly, and can be used can
It is embedded in the compound with deintercalate lithium ions inversely.In particular selected from cobalt, manganese, nickel and their combination metal, or selected from containing
At least one of compound of lithium.The example of the compound containing lithium includes by selected from LiaA1-bB1bD2(0.90≤a≤
1.8,0≤b≤0.5)；LiaE1-bB1bO2-cDc(0.90≤a≤1.8,0≤b≤0.5,0≤c≤0.05)；LiE2-bB1bO4-cDc
(0≤b≤0.5,0≤c≤0.05)；LiaNi1-b-cCobB1cDα(0.90≤a≤1.8,0≤b≤0.5,0≤c≤0.05,0 < α
≤2)；LiaNi1-b-cCobB1cO2-αF1α(0.90≤a≤1.8,0≤b≤0.5,0≤c≤0.05,0 < α < 2)；LiaNi1-b- cCobB1cO2-αF12(0.90≤a≤1.8,0≤b≤0.5,0≤c≤0.05,0 < α < 2)；LiaNi1-b-cMnbB1cDα(0.90≤a
≤ 1.8,0≤b≤0.5,0≤c≤0.05,0 < α≤2)；LiaNi1-b-cMnbB1cO2-αF1α(0.90≤a≤1.8,0≤b≤
0.5,0≤c≤0.05,0 < α < 2)；LiaNi1-b-cMnbB1cO2-αF12(0.90≤a≤1.8,0≤b≤0.5,0≤c≤0.05,0
<α<2)；LiaNibEcGdO2(0.90≤a≤1.8,0≤b≤0.9,0≤c≤0.5,0.001≤d≤0.1)；
LiaNibCocMndGeO2(0.90≤a≤1.8,0≤b≤0.9,0≤c≤0.5,0≤d≤0.5,0.001≤e≤0.1)；
LiaNiGbO2(0.90≤a≤1.8,0.001≤b≤0.1)；LiaCoGbO2(0.90≤a≤1.8,0.001≤b≤0.1)；
LiaMnGbO2(0.90≤a≤1.8,0.001≤b≤0.1)；LiaMn2GbO4(0.90≤a≤1.8,0.001≤b≤0.1)；
LiQO2；LiQS2；LiV2O5；LiZO2；LiNiVO4；Li(3-f)J2(PO4)3(0≤f≤2)；Li(3-f)Fe2(PO4)3(0≤f≤2)；
And LiFePO4Chemical formula indicate compound.Moreover, the example of the positive active material includes LiMn2O4、LiNi2O4、
LiCoO2、LiNiO2、LiMnO2、Li2MnO3、LiFePO4And LiNixCoyO2(0 < x≤0.15,0 < y≤0.85).
In the above formula, A Ni, Co, Mn or their combination；B1 be Al, Ni, Co, Mn, Cr, Fe, Mg, Sr,
V, rare earth element or their combination；D is O, F, S, P or their combination；E is Co, Mn or their combination；F1 be F, S,
P or their combination；G is Al, Cr, Mn, Fe, Mg, La, Ce, Sr, V or their combination；Q is Ti, Mo, Mn or their group
It closes；Z is Cr, V, Fe, Sc, Y or their combination；And J is V, Cr, Mn, Co, Ni, Cu or their combination.
The compound can have coating or the compound and the cated compound of tool combinable.It is described
Coating may include coating element compound, such as coating element oxide, hydroxide, be coated with element oxyhydroxide,
It is coated with the carbonic acid oxonium salt of element or is coated with the hydroxyl carbonate of element.It can be amorphous or crystallization for forming the compound of coating.
Example including coating element in the coating includes Mg, Al, Co, K, Na, Ca, Si, Ti, V, Sn, Ge, Ga, B, As, Zr and it
Mixture.Coating forming procedure can be in a manner of not adversely affecting to the performance of positive active material in describedization
Any coating method (such as spraying, impregnating) that the element is coated on object is closed, because well known within the skill of those ordinarily skilled
This process, so omitting the detailed description of the process.
The example of conductive material includes carbon black, graphite particle, natural graphite, artificial graphite, acetylene black, Ketjen black, carbon fiber
Dimension, carbon nanotube；Copper, nickel, aluminium or silver metal powder, metallic fiber or metal tube；And conducting polymer, such as polyphenylene
Derivative, but not limited to this, and any conductive material as known in the art can be used.
The example of jointing material includes vinylidene fluoride/hexafluoropropylene copolymer, Kynoar, polyacrylonitrile, poly- first
Base methyl acrylate, polytetrafluoroethylene (PTFE) (PTFE), their mixture and butadiene-styrene rubber quasi polymer.The example of solvent includes N-
Methyl pyrrolidone (NMP), acetone and water, but not limited to this, and any solvent as known in the art can be used.
In some embodiments, plasticizer can be further added in positive electrode active compound composition, in electrode plate
Interior formation stomata.Positive active material, conductive material, jointing material and solvent amount can be usually to make in lithium secondary battery field
Amount.
Second electrode 15 is negative electrode, and is formed as second electrode 15 for the second electrode plate of negative electrode plate.
It, can side identical with preparation first electrode 11 other than using negative electrode active material to replace positive active material
Formula prepares second electrode 15.
That is, passing through mixing negative electrode active material, conductive material, jointing material and molten as when preparation first electrode 11
Agent and prepare composition of cathode active materials.It then, can be by being directly coated with negative electrode active material combination on copper electrode substrate
Object and prepare second electrode plate.Alternatively, composition of cathode active materials may be cast on individual supporter, and from the branch
The negative electrode active material plasma membrane removed on support object can be laminated on copper electrode substrate, to prepare second electrode plate.Second electrode plate can
It is cut into suitably sized to prepare second electrode 15.
The example of negative electrode active material include lithium salts, can be formed with lithium the metal material of alloy, transition metal oxide, can
The material of elements doped lithium adulterate/can be removed, and can reversibly be embedded in the material with deintercalate lithium ions.
Can with lithium formed alloy metal material example include Si, Sn, Al, Ge, Pb, Bi, Sb, Si-Y alloy (here,
Y is alkali metal, alkaline-earth metal, the 13rd to 16 race's element, transition metal, rare earth element or their combination, and is not Si),
With Sn-Y alloy (Y be alkali metal, alkaline-earth metal, the 13rd to 16 race's element, transition metal, rare earth element or their combination, and
And be not Sn).The example of Y can for Mg, Ca, Sr, Ba, Ra, Sc, Y, Ti, Zr, Hf, Rf, V, Nb, Ta, Db, Cr, Mo, W, Sg,
Tc、Re、Bh、Fe、Pb、Ru、Os、Hs、Rh、Ir、Pd、Pt、Cu、Ag、Au、Zn、Cd、B、Al、Ga、Sn、In、Tl、Ge、P、As、
Sb, Bi, S, Se, Te, Po or their combination.
The example of transition metal oxide include barium oxide and lithium-barium oxide, and can doping and dedoping lithium material
The example of material includes Si, SiOx(Y is alkali metal, alkaline-earth metal, the 13rd to 16 race's element, transition gold for (0 < x < 2), Si-Y alloy
Category, rare earth element or their combination, and be not Si), Sn, SnO2(Y is alkali metal, alkaline-earth metal, the 13rd with Sn-Y alloy
To 16 race's elements, transition metal, rare earth element or their combination, and it is not Sn), or by least the one of above-mentioned substance selection
Kind and SiO2Mixture.The example of Y include Mg, Ca, Sr, Ba, Ra, Sc, Y, Ti, Zr, Hf, Rf, V, Nb, Ta, Db, Cr, Mo,
W、Sg、Tc、Re、Bh、Fe、Pb、Ru、Os、Hs、Rh、Ir、Pd、Pt、Cu、Ag、Au、Zn、Cd、B、Al、Ga、Sn、In、Tl、Ge、
P, As, Sb, Bi, S, Se, Te, Po and their combination.
Can reversibly be embedded in the material of deintercalate lithium ions is carbon material, and can be used and be generally used for lithium secondary battery
In any negative electrode active material based on carbon.The example of negative electrode active material based on carbon include crystalline carbon, amorphous carbon or
Their mixture.The example of crystalline carbon includes graphite, such as unbodied, plate, sheet, spherical or fibrous
Natural or artificial graphite.The example of amorphous carbon includes soft carbon (in the carbon that relatively low temperature is heat-treated) or hard carbon, interphase
The coke of bitumencarb compound and heat treatment.
However, negative electrode active material is without being limited thereto, and can be used as reversibly being embedded in and deintercalate lithium ions
Negative electrode active material any material.
In composition of cathode active materials, conductive material, jointing material and solvent can in preparation first electrode 11
It is identical used in situation.In some embodiments, plasticizer can further be added into composition of cathode active materials, with
Stomata is formed in second electrode plate.
Negative electrode active material, conductive material, jointing material and solvent amount can be usually used in lithium secondary battery field
Amount.According to the purposes and structure of lithium secondary battery, at least one of conductive material, jointing material and solvent can be omitted.
Then, preparation is arranged in the partition 16 between first electrode 11 and second electrode 15.Partition 16 can have relative to
The lower resistance of the Ion transfer of electrolyte and excellent electrolyte absorbability.
Substrate 13 may include polyolefin.Polyolefin has excellent anti-short-circuit effect, and can improve electricity due to closing effect
The stability in pond.For example, substrate 13 can be for by the resin comprising polyolefin such as polyethylene, polypropylene, polybutene, polychlorostyrene second
The film that alkene or their mixture or copolymer are formed, but substrate 13 is without being limited thereto, but any polyolefins can be used
Film.For example, substrate 13 can for is formed by polyolefin resin film, by the film that is formed of manufacture polyolefin fibrids including
The non-woven fabrics of polyolefin or the aggregation of insulating material particle.For example, the substrate 13 comprising polyolefin can have excellent be used for
The coating performance of the polymer solution of polymer coating 12 and 14 is prepared, and since the film thickness by reducing partition 16 increases
The active substance part in battery is added, so the capacity of every volume can be improved.
For example, the polyolefin of the material as substrate 13 can be the homopolymer of polyethylene, polypropylene etc., copolymer or mixing
Object.Polyethylene can be low-density, intermediate density and highdensity polyethylene, and according to mechanical strength, can be used highdensity
Polyethylene.Also, in order to provide flexibility to substrate 13, the polyethylene selected from least two types above can be mixed.Used in poly-
Polymerization catalyst in the preparation of ethylene does not limit specifically, but Ziegler-Natta catalyst, Philips type can be used
Catalyst or metallocene type catalyst.According to keeping mechanical strength and high light transmittance, the weight of polyethylene simultaneously
Average molecular weight can be in the range of 100,000 to 12,000,000, such as 200,000 to 3,000,000.Polypropylene can be homopolymerization
Object, random copolymer or block copolymer or their mixture.Moreover, polymerization catalyst does not limit specifically, and can
Use Ziegler-Natta catalyst or the catalyst of metallocene type.In addition, polyacrylic tacticity is not specific
Limitation.Polypropylene can be isotactic, syndiotactic or atactic, but can be used it is opposite spend it is few complete same
The polypropylene of vertical structure.Moreover, in the range of not violating effect of the invention, other than polyethylene or polypropylene, polyolefin
Additive or antioxidant can be added to polyolefin.
The thickness of substrate 13 can be in the range of about 1 μm to about 100 μm.For example, the thickness of substrate 13 can be at about 1 μm to about
In the range of 30 μm.For example, the thickness of substrate 13 can be in the range of about 5 μm to about 30 μm.When the thickness of substrate 13 is less than 1 μm
When, it is not able to maintain the mechanical performance of substrate 13, and when the thickness of substrate 13 is greater than 100 μm, the resistance of battery be will increase.
Substrate 13 can be porous.Porous substrate 13 can have the porosity in about 5% to about 95% range.Work as base
When the porosity of plate 13 is less than 5%, the resistance of battery be will increase, and when the porosity of substrate 13 is greater than 95%, Bu Nengbao
Hold the mechanical performance of porous substrate 13.
Polymer coating 12 and 14 may include the polymer based on fluorine or the copolymer based on fluorine.The polymerization based on fluorine
Object may include Kynoar.The copolymer based on fluorine can be for selected from by Kynoar-hexafluoropropene (PVdF-HFP)
Copolymer, Kynoar-polytetrafluoroethylene (PTFE) (PVdF-PTFE) copolymer and Kynoar-polytetrafluoroethylene (PTFE)-hexafluoropropene
(PVdF-PTFE-HFP) at least one of the group of copolymer composition.The polymer based on fluorine and the copolymer based on fluorine
It is without being limited thereto, and available any polymer based on fluorine or the copolymer based on fluorine in this field can be used.
Then, then stacked electrodes component 10 injects the electrolyte into the electrode assembly 10 of stacking.
Electrolyte can be the organic electrolyte that wherein may include lithium salts.
Organic electrolyte may include high dielectric solvent and low boiling point solvent.High dielectric solvent can be for selected from by carbonic acid Asia
At least one of ethyl ester, propylene carbonate, butylene carbonate and group of gamma butyrolactone composition.Low boiling point solvent can for selected from by
Dimethyl carbonate, ethyl methyl carbonate, diethyl carbonate, dipropyl carbonate, dimethoxy-ethane, diethoxyethane and fatty acid
At least one of the group of the derivative composition of ester.
Lithium salts can be for selected from by LiPF6、LiBF4、LiClO4、Li(CF3SO2)2、LiCF3SO3、LiSbF6And LiAsF6Composition
At least one of group.The concentration of lithium salts can be in the range of about 0.1M to about 0.2M.When the concentration of lithium salts is in above range
When interior, the electrolyte has suitable conductivity and viscosity, thus battery can have an excellent electrolyte property, and lithium from
Son can be migrated effectively.
Then, twice-aged process circulation is carried out, on the electrode assembly for the stacking for being injected with electrolyte to prepare lithium two
Primary cell.
For example, the process of the lithium secondary battery can be carried out preparing in a manner of described below.
That is, the process may include the first ageing process, it is pre-charge process, the first degassing procedure, hot pressing, second old
Change process and the second degassing procedure.
First ageing process and the second ageing process are to store in the state of static for stability and be injected with electrolysis
The process of the electrode assembly of the stacking of liquid.For example, can to carry out about 22 at room temperature small for the first ageing process and the second ageing process
Up to about 26 hours.When the first ageing process and the second ageing process carry out being longer than 26 hours, preparation process can be extended, and
When the first ageing process and the second ageing process were carried out less than 22 hours, electrolyte cannot equably be inhaled in electrode assembly
It receives, thus the generation of uniform solid electrolyte interface (SEI) layer in pre-charge process hereafter can be interfered.
Also, the first ageing process and the second ageing process in some embodiments, can be carried out at high temperature.When in height
When temperature the first ageing process of lower progress and the second ageing process, SEI layers can be stablized, and form SEI layers with uniform thickness.It can be
The first ageing process is carried out under high temperature and the second ageing process can be at a temperature in the range of for example at about 30 DEG C to about 45 DEG C about
12 hours to about 24 hours.It, can when carrying out the first ageing process and the second ageing process within the scope of the temperature and time
SEI layers of suitable thickness is kept, thus since the capacity in initial charge can be kept, it is assured that lithium secondary battery
Capacity.
Pre-charge process is the process that SEI layers are formed on the surface of negative electrode.Pre-charge process is by causing side reaction
Gas and reduce uncharged area, thus increase reversible capacity with can dramatically.It can be in for example, about 2.0V to about 2.4V range
Electric current within the scope of interior voltage and about 0.045C to about 0.055C carries out pre-charge process about 5 minutes to about 7 minutes.When upper
When carrying out pre-charge process under conditions of stating in range, can produce it is SEI layers uniform, and being capable of mass production lithium secondary battery.
First degassing procedure and the second degassing procedure remove the gas that the first ageing process and the second ageing process generate, because
This can prevent the swelling of electrode assembly.
As described above, the hot pressing of at least one circulation can be carried out under 95 DEG C or higher temperature.For example, can be about
200kgf/cm2To about 500kgf/cm2Hot pressing is carried out under pressure in range.For example, can be in about 95 DEG C to about 120 DEG C models
At a temperature of in enclosing and about 250kgf/cm2To about 450kgf/cm2Hot pressing about 100 seconds are carried out under pressure in range to about
150 seconds.
When carrying out hot pressing under conditions of within the above range, it can improve viscous between first electrode and second electrode
Intensity is closed, therefore the intensity and safety of lithium secondary battery can be improved.
According to another implementation of the invention, the lithium secondary battery prepared using the above method is provided.
The lithium secondary battery can have the structure of the substrate including melting on polymer coating as described above.Including
The partition of polymer coating can cover first electrode or second electrode, therefore heated even under 130 DEG C or higher temperature
The safety of lithium secondary battery can be improved down.
The lithium secondary battery may include pouch-type battery.
Equally, multiple pouch-type batteries can be stacked in the form of electrode assembly, thus form battery pack.The battery pack is available
In any device for needing high capacity and high output.For example, the battery pack can be used in laptop computer, smart phone or
In electric car.
The present invention will be described in more detail referring to the following examples.The purpose that these embodiments are merely to illustrate, without
It is intended to limit the scope of the invention.
[embodiment]
Preparation example 1: the preparation of lithium secondary battery
1.1: the preparation of first electrode
The LiCoO of 97.2 parts by weight is placed in solvent N-methyl pyrilidone2The polyvinylidene fluoride of powder, 1.5 parts by weight
The carbon black of alkene and 1.3 parts by weight, to prepare the first electrode slurry.It is coated on aluminium electrode substrate using scraper (gap: 170mm)
The thickness of the first electrode slurry to about 145 μm.Heat treatment is coated with the aluminium electricity of the first slurry in a vacuum at a temperature of 100 DEG C
It electrode substrate about 5.5 hours, dries later.Then, the aluminium electrode substrate of the drying is suppressed, using roll press to prepare it
On be formed with the first electrode plate of first electrode active material layer, and the first electrode plate is cut into the ruler of 457mm × 65.5mm
Very little and band shape, to prepare first electrode.
1.2: the preparation of second electrode
Disperse the graphite of 98 parts by weight, the butadiene-styrene rubber of 1 parts by weight and 1 parts by weight in solvent N-methyl pyrilidone
Carboxymethyl cellulose, to prepare the second electrode slurry.The second electricity is coated on copper electrode substrate using scraper (gap: 160mm)
The thickness of pole slurry to about 140 μm.It is heat-treated in a vacuum in 145 DEG C of temperature and is coated with the copper electrode substrate of the second slurry about
It 6.5 hours, dries later.Then, the copper electrode substrate of the drying is suppressed using roll press, is formed with thereon with preparation
The second electrode plate of second electrode active material layer, and the second electrode plate is cut into the size and band of 448mm × 66.5mm
Shape, to prepare second electrode.
1.3: the preparation of partition
The Kynoar (obtaining from Solvay) of 5 parts by weight is added to the solvent i.e. N- crassitude of 95 parts by weight
In ketone, to prepare slurry.Slurry is coated on two surfaces of polyethylene porous substrate (obtaining from Asahi) using rod coater
Expect to 9 μm of thickness, to prepare the partition of the polyvinylidene fluoride coating of the thickness with 3 μm.
1.4: embodiment 1: the preparation of lithium secondary battery
It will be made in first electrode and preparation example 1.2 that the baffle arrangement prepared in preparation example 1.3 is prepared in preparation example 1.1
Between standby second electrode, to prepare electrode assembly.It stacks the electrode assembly and is inserted into bag, then by the LiPF of 1.13M6
And the mixing of ethylene carbonate (EC), dimethyl carbonate (DMC) and diethyl carbonate (DEC) (with the volume ratio of 3:5:2)
Electrolyte injects in the electrode assembly of the stacking.At room temperature on the electrode assembly of the stacking for the electrolyte for being injected with mixing
Carry out the first ageing process about 24 hours.Next, at pre-charge electricity electrode assembly about 1 hour of 0.2C, then in vacuum
In the first degassing procedure is carried out on electrode assembly about 15 seconds.Then, the temperature and about 350kgf/cm at about 100 DEG C2Pressure
It is lower to be carried out on electrode assembly with heating plate hot pressing about 120 seconds, thus the electrode assembly that preparation completely stacks.Then,
It is carried out on the electrode assembly completely stacked at room temperature the second ageing process about 24 hours.Then, exist in a vacuum
The second degassing procedure is carried out on electrode assembly about 15 seconds and seal to prepare lithium secondary battery.
Comparative example 1: the preparation of lithium secondary battery
It will be made in first electrode and preparation example 1.2 that the baffle arrangement prepared in preparation example 1.3 is prepared in preparation example 1.1
Between standby second electrode, to prepare electrode assembly.It stacks the electrode assembly and is inserted into bag, then by the LiPF of 1.13M6
And the mixing of ethylene carbonate (EC), dimethyl carbonate (DMC) and diethyl carbonate (DEC) (with the volume ratio of 3:5:2)
Electrolyte injects in the electrode assembly of the stacking.At room temperature on the electrode assembly of the stacking for the electrolyte for being injected with mixing
Carry out the first ageing process about 24 hours.Next, at pre-charge electricity electrode assembly about 1 hour of 0.2C, then in electrode
The first degassing procedure is carried out on component about 15 seconds.Then, the temperature and about 350kgf/cm at about 93 DEG C2Pressure under with heating
Plate carries out hot pressing about 120 seconds on electrode assembly, thus the electrode assembly that preparation completely stacks.Then, at room temperature
The second ageing process is carried out on the electrode assembly completely stacked about 24 hours.Then, in a vacuum in electrode assembly
The second degassing procedure of upper progress about 15 seconds is simultaneously sealed to prepare lithium secondary battery.
Comparative example 2: the preparation of lithium secondary battery
It will be made in first electrode and preparation example 1.2 that the baffle arrangement prepared in preparation example 1.3 is prepared in preparation example 1.1
Between standby second electrode, to prepare electrode assembly.It stacks the electrode assembly and is inserted into bag, then by the LiPF of 1.13M6
And the mixing of ethylene carbonate (EC), dimethyl carbonate (DMC) and diethyl carbonate (DEC) (with the volume ratio of 3:5:2)
Electrolyte injects in the electrode assembly of the stacking.At room temperature on the electrode assembly of the stacking for the electrolyte for being injected with mixing
Carry out the first ageing process about 24 hours.Next, at pre-charge electricity electrode assembly about 1 hour of 0.2C, then in electrode
The first degassing procedure is carried out on component about 15 seconds.Then, the temperature and about 350kgf/cm at about 100 DEG C2Pressure under with heating
Plate carries out hot pressing about 190 seconds on electrode assembly, thus the electrode assembly that preparation completely stacks.Then, at room temperature
The second ageing process is carried out on the electrode assembly completely stacked about 24 hours.Then, in a vacuum in electrode assembly
The second degassing procedure of upper progress about 15 seconds is simultaneously sealed to prepare lithium secondary battery.
Experimental example 1: heated experiment and security verification experiment
The chemical conversion of 2 circulations is carried out on the lithium secondary battery prepared in embodiment 1 and comparative example 1 and 2 at room temperature
Charge/discharge.In formation process, lithium secondary battery 0.7C constant current charging, until the voltage of lithium secondary battery reaches
To 4.35V, then lithium secondary battery discharges in the constant voltage of 4.35V, until the electric current of lithium secondary battery reaches 0.05C.It connects
Get off, constant current of the lithium secondary battery in 1.0C discharges, until the voltage of lithium secondary battery reaches 2.75V.Then, enterprising
Row has constant current of formation charging/electric discharge lithium secondary battery in 0.5C to charge in the same manner as described above, and with 0.2C
Constant current electric discharge, until the voltage of lithium secondary battery reaches 3.0V.Here, charge/discharge condition be standard charging/put
Electric condition, and discharge capacity used herein is the capacity of standard.
By each lithium secondary battery prepared in embodiment 1 and comparative example 1 and 2 under the conditions of the charge/discharge of standard
It is added in room, and the temperature of the room is increased to 130 DEG C from room temperature with 5 DEG C of speed per minute, and observe the secondary electricity of lithium
Temperature 1 hour for changing while being kept for 130 DEG C in pond.Fig. 3 to 5 shows result.Here, dotted line indicates the change of voltage at any time
Change, and solid line indicates that temperature changes with time.
Referring to Fig. 3 to 5, when the temperature for being exposed to 130 DEG C heats, the lithium secondary battery display prepared in embodiment 1 is permanent
Fixed voltage reaches 90 minutes, while keeping 130 DEG C of temperature.But when the temperature for being exposed to 130 DEG C heats, comparative example 1
With 2 in the quick temperature change that shows from 130 DEG C to 300 DEG C of each lithium secondary battery for preparing, and respectively at about 45 seconds and
Voltage at 28 seconds quicklys increase and reduces.That is, the voltage of the lithium secondary battery prepared in comparative example 1 and 2 quickly increase and
Reduction shows generation short-circuit in battery.
Therefore, it can be verified that the safety of the lithium secondary battery prepared in embodiment 1 is better than in comparative example 1 and comparative example 2
The safety of the lithium secondary battery of preparation.
Equally, the lithium secondary battery prepared in embodiment 1 is exposed to 130 DEG C of temperature, to observe the variation in battery, so
After decompose battery, with use optical microscopy observation first electrode, second electrode and be arranged in first electrode, second electrode it
Between partition.Result is shown in Fig. 6.
Referring to Fig. 6, or even when the temperature for being exposed to 130 DEG C and then when decomposing, the secondary electricity of each lithium that is prepared in embodiment 1
There is the polyvinylidene fluoride layer (part indicated for example, with reference to " A ") as the polymer coating in partition to be still adhered in pond
In first electrode and second electrode, and the polyethylene porous substrate melted in polyvinylidene fluoride layer is (for example, with reference to " B " table
The part shown) partly adhere to.
In this respect, it can be verified that since the partition comprising the polymer coating surrounds the first electrode and described the
Two electrodes, so improving the safety of the lithium secondary battery prepared in embodiment 1.
As described above, one or more above embodiment according to the present invention, prepares the method packet of lithium secondary battery
It includes and prepares the secondary electricity of lithium and carrying out ageing process circulation at least twice on the electrode assembly in the stacking for being injected with electrolyte
Pond, therefore can have improved intensity and safety using lithium secondary battery prepared by the method.
It should be understood that illustrative embodiments described herein only consider in the sense that explanation, rather than the mesh limited
's.The explanation of features or aspect within each embodiment usually should be considered as to other similar in other embodiment
Features or aspect be effective.
Although with reference to the accompanying drawings of one or more embodiments of the invention, those skilled in the art will
Understand in the case where the spirit and scope of the present invention defined without departing substantially from the appended claims, it can be in form wherein and thin
Various changes can be made on section.
Claims (12)
1. a kind of method for preparing lithium secondary battery, which comprises
It is prepared by arrangement first electrode, second electrode and the partition between the first electrode and the second electrode
Electrode assembly；
It stacks the electrode assembly and injects in electrolyte to the electrode assembly of the stacking；With
And system is recycled by carrying out ageing process at least twice on the electrode assembly in the stacking for being injected with the electrolyte
Standby lithium secondary battery,
Wherein, it is described prepare lithium secondary battery include the ageing process circulation between on the electrode assembly in 95 DEG C or
Hot pressing circulation at least once is carried out at higher temperature, wherein the hot pressing carries out 100 seconds to 180 seconds.
2. according to the method described in claim 1, wherein, in 200kgf/cm2To 500kgf/cm2It is carried out under pressure in range
The hot pressing.
3. according to the method described in claim 1, wherein, at a temperature in the range of 95 DEG C to 120 DEG C and 250kgf/cm2Extremely
450kgf/cm2The hot pressing is carried out under pressure in range.
4. according to the method described in claim 1, wherein, carrying out the ageing process at room temperature.
5. according to the method described in claim 1, wherein, in the preparation of the electrode assembly, the partition include substrate and
Polymer coating at least one surface of the substrate.
6. according to the method described in claim 5, wherein, in the preparation of the electrode assembly, the polymer coating includes
Polymer based on fluorine.
7. according to the method described in claim 5, wherein, in the preparation of the electrode assembly, the polymer coating includes
Copolymer based on fluorine.
8. according to the method described in claim 6, wherein, the polymer based on fluorine includes Kynoar.
9. according to the method described in claim 7, wherein, the copolymer based on fluorine is selected from by Kynoar-hexafluoro
Propylene copolymer, Kynoar-teflon-copolymers and Kynoar-polytetrafluoroethylene (PTFE)-hexafluoropropylene copolymer
At least one of group of composition.
10. according to the method described in claim 1, wherein, the electrolyte is organic electrolyte.
11. a kind of lithium secondary battery, the lithium secondary battery is prepared using method described in any one of any one of claims 1 to 10 10.
12. lithium secondary battery according to claim 11, the lithium secondary battery is pouch-type battery.
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| US10840552B2 (en) | 2017-12-29 | 2020-11-17 | Uchicago Argonne, Llc | Additives for high voltage lithium ion batteries |
| KR102265741B1 (en) * | 2018-03-21 | 2021-06-16 | (주)엘지에너지솔루션 | Manufacturing method for secondary battery and secondary battery manufactured by the same |
| KR20210061111A (en) * | 2019-11-19 | 2021-05-27 | 주식회사 엘지화학 | Manufacturing method of secondary battery and device of manufacturing the same |
| US20220115738A1 (en) * | 2020-10-13 | 2022-04-14 | Electronics And Telecommunications Research Institute | Method of manufacturing secondary battery separator |
| EP4248514A1 (en) * | 2021-07-09 | 2023-09-27 | LG Energy Solution, Ltd. | Electrode assembly |
| CN115332637B (en) * | 2022-09-06 | 2024-03-26 | 香河昆仑新能源材料股份有限公司 | High-lithium-salt-concentration electrolyte and application method thereof in lithium ion battery |
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|---|---|---|---|---|
| JPH11288739A (en) * | 1998-03-31 | 1999-10-19 | Toyota Motor Corp | Manufacture for lithium ion secondary battery |
| CN102709603A (en) * | 2012-05-28 | 2012-10-03 | 上海电力学院 | Method for producing lithium ion battery directly taking FePO4 as positive electrode material |
| CN102738513A (en) * | 2012-01-12 | 2012-10-17 | 宁德新能源科技有限公司 | Preparation method of lithium ion secondary battery |
| CN103000956A (en) * | 2012-11-29 | 2013-03-27 | 东莞新能源科技有限公司 | Manufacturing method of lithium ion battery containing gel electrolyte |
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| JPH11288739A (en) * | 1998-03-31 | 1999-10-19 | Toyota Motor Corp | Manufacture for lithium ion secondary battery |
| CN102738513A (en) * | 2012-01-12 | 2012-10-17 | 宁德新能源科技有限公司 | Preparation method of lithium ion secondary battery |
| CN102709603A (en) * | 2012-05-28 | 2012-10-03 | 上海电力学院 | Method for producing lithium ion battery directly taking FePO4 as positive electrode material |
| CN103000956A (en) * | 2012-11-29 | 2013-03-27 | 东莞新能源科技有限公司 | Manufacturing method of lithium ion battery containing gel electrolyte |
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