CN100505407C - Lithium ion battery and its preparing method - Google Patents
Lithium ion battery and its preparing method Download PDFInfo
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- CN100505407C CN100505407C CNB2005101323839A CN200510132383A CN100505407C CN 100505407 C CN100505407 C CN 100505407C CN B2005101323839 A CNB2005101323839 A CN B2005101323839A CN 200510132383 A CN200510132383 A CN 200510132383A CN 100505407 C CN100505407 C CN 100505407C
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- 229910001416 lithium ion Inorganic materials 0.000 title claims description 39
- HBBGRARXTFLTSG-UHFFFAOYSA-N Lithium ion Chemical compound [Li+] HBBGRARXTFLTSG-UHFFFAOYSA-N 0.000 title claims description 38
- 238000000034 method Methods 0.000 title claims description 17
- 239000000919 ceramic Substances 0.000 claims abstract description 66
- 239000003792 electrolyte Substances 0.000 claims abstract description 15
- 230000004888 barrier function Effects 0.000 claims description 47
- 238000002360 preparation method Methods 0.000 claims description 28
- 102000002151 Microfilament Proteins Human genes 0.000 claims description 25
- 108010040897 Microfilament Proteins Proteins 0.000 claims description 25
- 210000003632 microfilament Anatomy 0.000 claims description 25
- MCMNRKCIXSYSNV-UHFFFAOYSA-N Zirconium dioxide Chemical compound O=[Zr]=O MCMNRKCIXSYSNV-UHFFFAOYSA-N 0.000 claims description 22
- 239000008151 electrolyte solution Substances 0.000 claims description 12
- 238000009954 braiding Methods 0.000 claims description 7
- 239000012528 membrane Substances 0.000 abstract description 6
- 239000000463 material Substances 0.000 description 20
- -1 polyethylene Polymers 0.000 description 16
- 239000000853 adhesive Substances 0.000 description 15
- 230000001070 adhesive effect Effects 0.000 description 15
- 239000007773 negative electrode material Substances 0.000 description 15
- 229910052744 lithium Inorganic materials 0.000 description 13
- IAZDPXIOMUYVGZ-UHFFFAOYSA-N Dimethylsulphoxide Chemical compound CS(C)=O IAZDPXIOMUYVGZ-UHFFFAOYSA-N 0.000 description 12
- WHXSMMKQMYFTQS-UHFFFAOYSA-N Lithium Chemical compound [Li] WHXSMMKQMYFTQS-UHFFFAOYSA-N 0.000 description 12
- ZMXDDKWLCZADIW-UHFFFAOYSA-N N,N-Dimethylformamide Chemical compound CN(C)C=O ZMXDDKWLCZADIW-UHFFFAOYSA-N 0.000 description 12
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- 229920002981 polyvinylidene fluoride Polymers 0.000 description 11
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- 238000012360 testing method Methods 0.000 description 8
- ZPOLNCDBPYJDSE-UHFFFAOYSA-N 3-[4-[bis(2-chloroethyl)amino]phenyl]-2-formamidopropanoic acid Chemical compound O=CNC(C(=O)O)CC1=CC=C(N(CCCl)CCCl)C=C1 ZPOLNCDBPYJDSE-UHFFFAOYSA-N 0.000 description 6
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- 239000011737 fluorine Substances 0.000 description 5
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- 150000001298 alcohols Chemical class 0.000 description 2
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- MTAZNLWOLGHBHU-UHFFFAOYSA-N butadiene-styrene rubber Chemical compound C=CC=C.C=CC1=CC=CC=C1 MTAZNLWOLGHBHU-UHFFFAOYSA-N 0.000 description 2
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- 229920003088 hydroxypropyl methyl cellulose Polymers 0.000 description 2
- UFVKGYZPFZQRLF-UHFFFAOYSA-N hydroxypropyl methyl cellulose Chemical compound OC1C(O)C(OC)OC(CO)C1OC1C(O)C(O)C(OC2C(C(O)C(OC3C(C(O)C(O)C(CO)O3)O)C(CO)O2)O)C(CO)O1 UFVKGYZPFZQRLF-UHFFFAOYSA-N 0.000 description 2
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- 229910003002 lithium salt Inorganic materials 0.000 description 2
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- 229910018871 CoO 2 Inorganic materials 0.000 description 1
- GYHNNYVSQQEPJS-UHFFFAOYSA-N Gallium Chemical compound [Ga] GYHNNYVSQQEPJS-UHFFFAOYSA-N 0.000 description 1
- 229910013872 LiPF Inorganic materials 0.000 description 1
- 101150058243 Lipf gene Proteins 0.000 description 1
- FYYHWMGAXLPEAU-UHFFFAOYSA-N Magnesium Chemical compound [Mg] FYYHWMGAXLPEAU-UHFFFAOYSA-N 0.000 description 1
- 229910019142 PO4 Inorganic materials 0.000 description 1
- QOSMNYMQXIVWKY-UHFFFAOYSA-N Propyl levulinate Chemical compound CCCOC(=O)CCC(C)=O QOSMNYMQXIVWKY-UHFFFAOYSA-N 0.000 description 1
- 239000005864 Sulphur Substances 0.000 description 1
- RTAQQCXQSZGOHL-UHFFFAOYSA-N Titanium Chemical compound [Ti] RTAQQCXQSZGOHL-UHFFFAOYSA-N 0.000 description 1
- HCHKCACWOHOZIP-UHFFFAOYSA-N Zinc Chemical compound [Zn] HCHKCACWOHOZIP-UHFFFAOYSA-N 0.000 description 1
- NOJZFGZMTUAHLD-UHFFFAOYSA-N [Li].[Cl] Chemical compound [Li].[Cl] NOJZFGZMTUAHLD-UHFFFAOYSA-N 0.000 description 1
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- 229910052796 boron Inorganic materials 0.000 description 1
- 239000006229 carbon black Substances 0.000 description 1
- BVKZGUZCCUSVTD-UHFFFAOYSA-N carbonic acid Chemical compound OC(O)=O BVKZGUZCCUSVTD-UHFFFAOYSA-N 0.000 description 1
- SIXOAUAWLZKQKX-UHFFFAOYSA-N carbonic acid;prop-1-ene Chemical compound CC=C.OC(O)=O SIXOAUAWLZKQKX-UHFFFAOYSA-N 0.000 description 1
- 239000011651 chromium Substances 0.000 description 1
- 229910052804 chromium Inorganic materials 0.000 description 1
- 229910017052 cobalt Inorganic materials 0.000 description 1
- 239000010941 cobalt Substances 0.000 description 1
- GUTLYIVDDKVIGB-UHFFFAOYSA-N cobalt atom Chemical compound [Co] GUTLYIVDDKVIGB-UHFFFAOYSA-N 0.000 description 1
- 230000019771 cognition Effects 0.000 description 1
- 239000000571 coke Substances 0.000 description 1
- 238000010281 constant-current constant-voltage charging Methods 0.000 description 1
- 229910052802 copper Inorganic materials 0.000 description 1
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- JBTWLSYIZRCDFO-UHFFFAOYSA-N ethyl methyl carbonate Chemical compound CCOC(=O)OC JBTWLSYIZRCDFO-UHFFFAOYSA-N 0.000 description 1
- NBVXSUQYWXRMNV-UHFFFAOYSA-N fluoromethane Chemical compound FC NBVXSUQYWXRMNV-UHFFFAOYSA-N 0.000 description 1
- 229910052733 gallium Inorganic materials 0.000 description 1
- 238000002347 injection Methods 0.000 description 1
- 239000007924 injection Substances 0.000 description 1
- PNDPGZBMCMUPRI-UHFFFAOYSA-N iodine Chemical compound II PNDPGZBMCMUPRI-UHFFFAOYSA-N 0.000 description 1
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- 239000007788 liquid Substances 0.000 description 1
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- MHCFAGZWMAWTNR-UHFFFAOYSA-M lithium perchlorate Chemical compound [Li+].[O-]Cl(=O)(=O)=O MHCFAGZWMAWTNR-UHFFFAOYSA-M 0.000 description 1
- 229910001486 lithium perchlorate Inorganic materials 0.000 description 1
- 229910001496 lithium tetrafluoroborate Inorganic materials 0.000 description 1
- 229910052749 magnesium Inorganic materials 0.000 description 1
- 239000011777 magnesium Substances 0.000 description 1
- 239000000155 melt Substances 0.000 description 1
- VNWKTOKETHGBQD-UHFFFAOYSA-N methane Chemical compound C VNWKTOKETHGBQD-UHFFFAOYSA-N 0.000 description 1
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- 239000010452 phosphate Substances 0.000 description 1
- 229920000647 polyepoxide Polymers 0.000 description 1
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- 239000002296 pyrolytic carbon Substances 0.000 description 1
- 238000005245 sintering Methods 0.000 description 1
- 150000008053 sultones Chemical class 0.000 description 1
- 229910052719 titanium Inorganic materials 0.000 description 1
- 239000010936 titanium Substances 0.000 description 1
- 229910052723 transition metal Inorganic materials 0.000 description 1
- 150000003624 transition metals Chemical group 0.000 description 1
- 238000009736 wetting Methods 0.000 description 1
- 229910052727 yttrium Inorganic materials 0.000 description 1
- VWQVUPCCIRVNHF-UHFFFAOYSA-N yttrium atom Chemical compound [Y] VWQVUPCCIRVNHF-UHFFFAOYSA-N 0.000 description 1
- 229910052725 zinc Inorganic materials 0.000 description 1
- 239000011701 zinc Substances 0.000 description 1
Classifications
-
- 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
-
- 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
This invention relates to Li ioninc cells including a pole set and non-solution electrolyte sealed in a shell, and the pole includes a positive, a negative pole and ceramic membranes, which is stable under high temperature and safe.
Description
Technical field
The invention relates to a kind of battery and preparation method thereof, specifically, the invention relates to a kind of lithium ion battery and its preparation method.
Background technology
Lithium ion battery is as a kind of chemical power source, refers to respectively the secondary cell that constitutes as both positive and negative polarity with two compounds that can reversibly embed with the removal lithium embedded ion.When battery charge, lithium ion takes off embedding from positive pole, in negative pole, embed, otherwise during discharge.
Lithium rechargeable battery because have specific energy height, operating voltage height, self-discharge rate low, have extended cycle life, advantage such as pollution-free and in modern mobile electronic device and communication apparatus, being used widely, as mobile phone, notebook computer, Hand Personal Computer, PDA(Personal Digital Assistant), small-sized camera, digital camera, portable DVD player/VCD and MP3 player.In recent years, lithium rechargeable battery also obtains application progressively in electric tool and electronic toy field.
But lithium rechargeable battery exists safety problem.Such as, there is a lot of several microns high salient points in surface at battery positive and negative electrode pole piece, and the barrier film that lithium rechargeable battery is commonly used at present is the porousness polyolefine material, as PE (polyethylene), PP (polypropylene) individual layer microporous barrier or three layers of microporous barrier of PP/PE/PP, in battery making, transhipment, use can since extruding, vibrations, collision the barrier film that is placed between the positive/negative plate is produced scratches or puncture, cause positive and negative electrode pole piece contact short circuit, produce heat internal temperature of battery is risen.And for example in the use of electronic equipment and communication apparatus, can cause that over-charging of battery produces heat owing to the inefficacy of protection circuit plate, the savings of heat rises internal temperature of battery.When temperature surpasses 170 ℃, violent chemical reaction can take place in the positive and negative electrode active material and the organic electrolyte of inside battery, and temperature is elevated to rapidly more than 200 ℃, even can reach more than 500 ℃, causes battery burning or blast.
Summary of the invention
Goal of the invention of the present invention is to overcome the shortcoming that existing lithium rechargeable battery poor high temperature stability causes the battery security difference, and lithium ion battery that a kind of high-temperature stability is good, battery security is good and preparation method thereof is provided.
The present inventor finds, when internal temperature of battery reaches 120-140 ℃, the micropore fusion on traditional battery diaphragm layers of polyethylene layer, closes, and blocked the passage that lithium ion passes through, thus cut-off current and suppress the further rising of internal temperature of battery.But, if internal temperature of battery has risen to above 160 ℃, so, fusion and decomposition takes place in membrane layer polyethylene and/or this cognition of polypropylene diaphragm, can't recur to and isolate the effect of positive and negative electrode, cause battery short circuit, the temperature of inside battery is raise rapidly and positive active material is contacted with the negative electrode active material large tracts of land, can take place violent the decomposition and reaction in positive and negative electrode active material and organic electrolyte, causes battery burning or blast.If the present inventor finds to adopt a kind of new barrier film, can address the above problem.
The invention provides a kind of lithium ion battery, this battery comprises electrode group and nonaqueous electrolytic solution, and described electrode group and nonaqueous electrolytic solution are sealed in the battery container, and described electrode group comprises positive pole, negative pole and barrier film, and wherein, described barrier film is a ceramic diaphragm.
The invention provides a kind of preparation method of lithium ion battery, this method comprises positive pole and the negative pole for preparing battery, and positive pole, negative pole and barrier film are prepared into an electrode group, and electrode group and the electrolyte that obtains is sealed in the battery case, wherein, described barrier film is a ceramic diaphragm.
The barrier film of lithium ion battery provided by the invention is a ceramic diaphragm, the melt temperature of described ceramic diaphragm is between 600-800 ℃, when abnormal conditions take place, particularly when internal temperature of battery rises to above 160 ℃, fusion and decomposition can not take place in ceramic diaphragm, still can play the effect of isolating anodal and negative pole well, positive active material and negative electrode active material are come in contact, therefore can not cause the short circuit of battery, thereby further suppressed the rising of temperature, just avoided, violent decomposition reaction takes place in negative electrode active material and organic electrolyte, thereby has avoided battery that violent burning or blast take place.Therefore, lithium ion battery provided by the invention has good high-temperature stability and security performance.
Embodiment
According to lithium ion battery provided by the invention, the thickness of described ceramic diaphragm is the 5-60 micron, is preferably the 15-40 micron.
The porosity of described ceramic diaphragm refers to the area that the lip-deep hole of ceramic diaphragm is shared and the ratio of film total surface area, for gas permeability and the assurance electrolyte that guarantees described ceramic diaphragm can fully permeate the electrode material that is coated on the positive and negative electrode pole piece of barrier film both sides with wetting, the porosity of described ceramic diaphragm is 20-90%, is preferably 40-80%; The aperture of described ceramic diaphragm is meant the diameter of circular hole or class circular hole, and under the preferable case, the aperture of described ceramic diaphragm is the 20-200 micron, more preferably the 50-150 micron.
Described ceramic diaphragm can be the ceramic diaphragm that has above-mentioned thickness, porosity and aperture arbitrarily.Under the preferable case, described ceramic diaphragm is to be the 20-200 micron by diameter, and the tow braiding that is preferably the 50-120 micron forms, and described tow comprises the 5-50 root, and being preferably 10-30 root diameter is the 1-15 micron, is preferably the microfilament bar of 5-10 micron; Described microfilament bar comprises the 100-500 root, and being preferably 200-300 root diameter is the 0.01-0.10 micron, is preferably the ceramic hollow microfilament of 0.02-0.04 micron.Such ceramic diaphragm has better pliability, is beneficial to coiling.Described ceramic diaphragm can be commercially available, and also can make the microfilament bar with ceramic hollow microfilament, forms tow by the microfilament bar again, obtains described barrier film by the tow braiding at last.
The material of forming described ceramic diaphragm can be various existing materials, under the preferable case, described ceramic diaphragm contains zirconia and yittrium oxide, is benchmark with the total weight of this ceramic diaphragm, described zirconic content is 80-95 weight %, and the content of yittrium oxide is 5-20 weight %.
Because described ceramic diaphragm has higher melt temperature, especially with the zirconia ceramic diaphragm of main component, because zirconic fusing point is 2715 ℃, because its fusing point height, chemical property are stablized, fusion and decomposition can not take place in the ceramic diaphragm that therefore with the zirconia is main component under the high temperature of inside battery, and can well play the effect of isolating anodal and negative pole, positive active material and negative electrode active material are come in contact, thereby guaranteed the good high-temperature stability of lithium ion battery.
Described ceramic diaphragm is arranged between positive plate and the negative plate positive plate and negative plate is separated, and has electrical insulation capability and liquid retainability energy.
The preparation method of lithium ion battery provided by the invention comprises positive pole and the negative pole for preparing battery, and positive pole, negative pole and barrier film are prepared into an electrode group, the electrode group and the electrolyte that obtain are sealed in the battery case, and wherein, described barrier film is a ceramic diaphragm provided by the invention.
Described electrode group is by membrane layer the described positive pole for preparing and negative pole to be twined to separate to obtain, stacked, the method for winding of the membrane layer between positive pole and negative pole are conventionally known to one of skill in the art, for example, barrier film provided by the invention and electrode slice are formed takeup type electrode group through the back of reeling again according to the stacked electrode group of the stacked formation of the order of barrier film, negative plate or positive plate, barrier film, positive plate or negative plate or with aforementioned stacked electrode group, in electrolyte is sealed in battery container.
Described battery container can be the various housings that are applicable to various size battery, and as package compound film shell, metal square shell or round metal cylindricality shell, those skilled in the art can be easy to select as required suitable battery container.
The barrier film that the present invention only relates to battery improves, and the The Nomenclature Composition and Structure of Complexes of battery other parts is not particularly limited.
Consisting of of described positive pole is conventionally known to one of skill in the art.In general, positive pole comprises collector body and coating and/or is filled in positive electrode on the collector body that described positive electrode comprises positive active material, conductive agent and anodal adhesive.
Described positive active material is not particularly limited, and can be the positive active material of the embedded removal lithium embedded of this area routine, a kind of or its mixture: the Li in the preferred following material
xNi
1-yCoO
2(wherein, 0.9≤x≤1.1,0≤y≤1.0), Li
1+aM
bMn
2-bO
4(wherein ,-0.1≤a≤0.2,0≤b≤1.0, M is a kind of in lithium, boron, magnesium, aluminium, titanium, chromium, iron, cobalt, nickel, copper, zinc, gallium, yttrium, fluorine, iodine, the element sulphur), Li
mMn
2-nB
nO
2(wherein, B is a transition metal, 0.9≤m≤1.1,0≤n≤1.0).
Described anodal conductive agent is not particularly limited, and can be the anodal conductive agent of this area routine, at least a such as in acetylene black, conductive carbon black and the electrically conductive graphite.Weight with positive active material is benchmark, and the content of described conductive agent is 1-15 weight %, is preferably 2-10 weight %.
The kind of described anodal adhesive and content are conventionally known to one of skill in the art, for example one or more in fluorine resin and polyolefin compound such as polyvinylidene fluoride (PVDF), polytetrafluoroethylene (PTFE), butadiene-styrene rubber (SBR), polyvinyl alcohol, hydroxypropyl methylcellulose, sodium carboxymethylcellulose, the hydroxyethylcellulose.In general, according to the difference of used anodal adhesive kind, be benchmark with the weight of positive active material, the content of anodal adhesive is 0.5-8 weight %, is preferably 1-5 weight %.
Positive electrode collector can be positive electrode collector conventional in the lithium ion battery, uses aluminium foil as positive electrode collector in specific embodiments of the present invention.
The preparation method of described positive pole can adopt conventional preparation method.For example, with described positive active material, conductive agent and adhesive and solvent, apply and/or be filled on the described collector body, drying is rolled or is not rolled, and can obtain described positive pole.Wherein, described solvent can be selected from one or more in N-methyl pyrrolidone (NMP), dimethyl formamide (DMF), diethylformamide (DEF), dimethyl sulfoxide (DMSO) (DMSO), oxolane (THF) and water and the alcohols.The consumption of solvent can make described pastel have viscosity and flowability, can be coated on the described collector body to get final product.In general the weight with positive active material is benchmark, and the content 30-80 weight % of described solvent is preferably 35-60 weight %.Wherein, drying, the method for calendering and condition are conventionally known to one of skill in the art.
Consisting of of described negative pole is conventionally known to one of skill in the art.In general, negative pole comprises conducting base and coating and/or is filled in negative material on the conducting base that described negative material comprises negative electrode active material and negative pole adhesive.
Described negative electrode active material is not particularly limited, can use embedding of this area routine to disengage the negative electrode active material of lithium, material with carbon element for example, described material with carbon element be selected from non-graphitized charcoal, graphite or the charcoal that obtains by high-temperature oxydation by polyyne family macromolecule material or pyrolytic carbon, coke, organic polymer sinter, active carbon in one or more.Described organic polymer sinter can be by with products therefrom after sintering such as phenolic resins, epoxy resin and the charing.
The kind of described negative pole adhesive and content are conventionally known to one of skill in the art, for example one or more in fluorine resin and polyolefin compound such as polyvinylidene fluoride (PVDF), polytetrafluoroethylene (PTFE), butadiene-styrene rubber (SBR), hydroxypropyl methylcellulose, sodium carboxymethylcellulose, hydroxyethylcellulose, the polyvinyl alcohol; In general, according to the difference of adhesive therefor kind, be benchmark with the weight of negative electrode active material, the content of negative pole adhesive is 0.01-8 weight %, is preferably 0.02-5 weight %.
Described negative material can also comprise that conductive agent to increase the conductivity of electrode, reduces the internal resistance of cell.Described conductive agent is not particularly limited, and can be the cathode conductive agent of this area routine, such as in carbon black, nickel powder, the copper powder one or more.Weight with negative electrode active material is benchmark, and the content of described conductive agent is 0-12 weight %, is preferably 2-10 weight %.
The negative pole conducting base can be for negative pole conducting base conventional in the lithium ion battery, as stamped metal, and metal forming, net metal, foamed metal uses Copper Foil as the negative pole conducting base in specific embodiments of the present invention.
The preparation method of described negative pole can adopt conventional preparation method.For example, with negative material and solvent, apply and/or be filled on the described conducting base, drying is rolled or is not rolled, and can obtain described negative pole.Wherein, described solvent can be selected from one or more in N-methyl pyrrolidone (NMP), dimethyl formamide (DMF), diethylformamide (DEF), dimethyl sulfoxide (DMSO) (DMSO), oxolane (THF) and water and the alcohols.The consumption of solvent can make described pastel have viscosity and flowability, can be coated on the described conducting base to get final product.In general, be benchmark with the weight of negative electrode active material, the content of described solvent is 100-150 weight %.Wherein, drying, the method for calendering and condition are conventionally known to one of skill in the art.For example, the temperature of described drying is generally 100-150 ℃.
Described electrolyte can be non-water liquid electrolyte or gel state electrolyte.
Described gel state electrolyte is not particularly limited, and can use the gel state electrolyte of this area routine, such as the basic gel state electrolyte of PVdF (poly-difluoroethylene) etc.
Nonaqueous electrolytic solution is the mixed solution of electrolyte lithium salt and nonaqueous solvents, and it is not particularly limited, and can use the nonaqueous electrolytic solution of this area routine.Be selected from lithium hexafluoro phosphate (LiPF such as electrolyte lithium salt
6), in lithium perchlorate, LiBF4, hexafluoroarsenate lithium, lithium halide, chlorine lithium aluminate and the fluorocarbon based sulfonic acid lithium one or more.Organic solvent is selected chain acid esters and ring-type acid esters mixed solution for use, wherein the chain acid esters can be dimethyl carbonate (DMC), diethyl carbonate (DEC), methyl ethyl carbonate (EMC), carbonic acid first propyl ester (MPC), dipropyl carbonate (DPC) and other are fluorine-containing, sulfur-bearing or contain at least a in the chain organosilane ester of unsaturated bond, the ring-type acid esters can be ethylene carbonate (EC), propene carbonate (PC), vinylene carbonate (VC), gamma-butyrolacton (γ-BL), sultone and other are fluorine-containing, sulfur-bearing or contain at least a in the ring-type organosilane ester of unsaturated bond.The injection rate of electrolyte is generally 1.5-4.9 gram/ampere-hour, the concentration of electrolyte be generally 0.1-2.0 rub/liter.
According to the preparation method of lithium ion battery provided by the invention, except barrier film adopted ceramic diaphragm provided by the invention, other step was conventionally known to one of skill in the art.
To the present invention be described in more detail by embodiment below.
Embodiment 1
This embodiment illustrates the preparation of lithium ion battery provided by the invention.
(1) Zheng Ji preparation
With the anodal active component LiCoO of 100 weight portions
2, 5 weight portion adhesive polyvinylidene fluoride (PVDF), 4 weight portion conductive agent acetylene blacks join in the 60 weight portion n-formyl sarcolysine base pyrrolidones (NMP), in de-airing mixer, stir then and form uniform anode sizing agent.
This slurry is coated on the thick 20 microns aluminium foil equably, 120 ℃ of oven dry then, roll-in is cut on cutting machine and obtain being of a size of 52 millimeters * 32 millimeters * 130 microns positive pole afterwards, wherein contains the anodal material of 0.65 gram.
(2) preparation of negative pole
100 weight portion negative electrode active material native graphites, 5 weight portion adhesive polytetrafluoroethylene (PTFE)s are joined in the 100 weight portion n-formyl sarcolysine base pyrrolidones (NMP), in de-airing mixer, stir then and form cathode size stable, homogeneous.
This slurry is coated on the thick 12 microns Copper Foil equably, after 120 ℃ of oven dry, rolling, on cutting machine, cuts and obtain being of a size of 53 millimeters * 32 millimeters * 140 microns negative pole, wherein contain 0.3 gram negative pole material.
(3) preparation of electrode group
With thickness is 20 microns, voidage is 40%, average pore size be 100 microns (pore diameter range is the 80-120 micron) ceramic diaphragm (the zirconia ceramics barrier film that Guangzhou Xinlaifu Magnetoelectric Co. Ltd. produces, the zirconia content of described ceramic diaphragm is 92 weight %, yittrium oxide content is 8 weight %.Described ceramic diaphragm is that diameter that 0.02 micron ceramic hollow microfilament is formed is 5 microns a microfilament bar by 250 diameters, and then to form diameter by 15 such microfilament bars be that 75 microns tow braiding obtains), cut into 55 * 33 millimeters diaphragm.The above-mentioned diaphragm that obtains, positive plate and negative plate is stacked successively according to the order of barrier film/positive plate/barrier film/negative plate, make the electrode group that is of a size of 3.2 * 33 * 55 millimeters.
(4) assembling of battery
LiPF6 and ethylene carbonate (EC), diethyl carbonate (DEC) and DMC (dimethyl carbonate) are configured to the solution that LiPF6 concentration is 1.0 mol (wherein, the volume ratio of EC, DEC and DMC is 1:1:1), obtain nonaqueous electrolytic solution.The package compound film with PET polyester/NY nylon/AL aluminium foil/CPP hydrostomia polypropylene multi-layer structure that is made of macromolecule membrane and metal forming that the electrode group that (3) are obtained is put into an end opening strikes out the battery case of the groove that has 3.5 * 33 * 55 millimeters, and inject above-mentioned nonaqueous electrolytic solution with the amount of 3.8g/Ah, the capacity of making after the sealing is 800mAh, and outside dimension is 3.8 * 35 * 62 millimeters laminated structure flexible packing lithium ion secondary battery A1.
Embodiment 2
This embodiment illustrates the preparation of lithium ion battery provided by the invention.
(1) Zheng Ji preparation
With the anodal active component LiCoO of 100 weight portions
2, 5 weight portion adhesive polyvinylidene fluoride (PVDF), 4 weight portion conductive agent acetylene blacks join in the 60 weight portion n-formyl sarcolysine base pyrrolidones (NMP), in de-airing mixer, stir then and form uniform anode sizing agent.
This slurry is coated on the thick 20 microns aluminium foil equably, 120 ℃ of oven dry then, roll-in is cut on cutting machine and obtain being of a size of 52 millimeters * 360 millimeters * 130 microns positive pole afterwards, wherein contains the anodal material of 6.5 grams.
(2) preparation of negative pole
100 weight portion negative electrode active material native graphites, 5 weight portion adhesive polytetrafluoroethylene (PTFE)s are joined in the 100 weight portion n-formyl sarcolysine base pyrrolidones (NMP), in de-airing mixer, stir then and form cathode size stable, homogeneous.
This slurry is coated on the thick 12 microns Copper Foil equably, after 120 ℃ of oven dry, rolling, on cutting machine, cuts and obtain being of a size of 53 millimeters * 325 millimeters * 140 microns negative pole, wherein contain 3.0 gram negative pole material.
(3) preparation of electrode group
With thickness is 20 microns, voidage is 60%, average pore size be 100 microns (pore diameter range is the 80-120 micron) ceramic diaphragm (the zirconia ceramics barrier film that Guangzhou Xinlaifu Magnetoelectric Co. Ltd. produces, the zirconia content of described ceramic diaphragm is 92 weight %, yittrium oxide content is 8 weight %.Described ceramic diaphragm is that diameter that 0.02 micron ceramic hollow microfilament is formed is 5 microns a microfilament bar by 250 diameters, and then to form diameter by 20 such microfilament bars be that 100 microns tow braiding obtains) cut into 55 * 740 millimeters diaphragm.The above-mentioned diaphragm that obtains, positive plate and negative plate are wound into the electrode group that is of a size of 3.2 * 33 * 55 millimeters according to the order of barrier film/negative plate/barrier film/positive plate after stacked successively.
(4) assembling of battery
LiPF6 and ethylene carbonate (EC), diethyl carbonate (DEC) and DMC (dimethyl carbonate) are configured to the solution that LiPF6 concentration is 1.0 mol (wherein, the volume ratio of EC, DEC and DMC is 1:1:1), obtain nonaqueous electrolytic solution.The electrode group that (3) are obtained is put into the aluminum metal battery case of an end opening, and injects above-mentioned nonaqueous electrolytic solution with the amount of 3.8g/Ah, and the capacity of making after the sealing is 800mAh, and outside dimension is 3.8 * 35 * 57 millimeters square lithium ion secondary battery A2.
Embodiment 3
This embodiment illustrates the preparation of lithium ion battery provided by the invention.
(1) Zheng Ji preparation
With the anodal active component LiCoO of 100 weight portions
2, 5 weight portion adhesive polyvinylidene fluoride (PVDF), 4 weight portion conductive agent acetylene blacks join in the 60 weight portion n-formyl sarcolysine base pyrrolidones (NMP), in de-airing mixer, stir then and form uniform anode sizing agent.
This slurry is coated on the thick 20 microns aluminium foil equably, 120 ℃ of oven dry then, roll-in is cut on cutting machine and obtain being of a size of 52 millimeters * 360 millimeters * 125 microns positive pole afterwards, wherein contains the anodal material of 6.1 grams.
(2) preparation of negative pole
100 weight portion negative electrode active material native graphites, 5 weight portion adhesive polytetrafluoroethylene (PTFE)s are joined in the 100 weight portion n-formyl sarcolysine base pyrrolidones (NMP), in de-airing mixer, stir then and form cathode size stable, homogeneous.
This slurry is coated on the thick 12 microns Copper Foil equably, after 120 ℃ of oven dry, rolling, on cutting machine, cuts and obtain being of a size of 53 millimeters * 325 millimeters * 135 microns negative pole, wherein contain 2.8 gram negative pole material.
(3) preparation of electrode group
With thickness is 30 microns, voidage is 80%, average pore size be 100 microns (pore diameter range is the 80-120 micron) ceramic diaphragm (the zirconia ceramics barrier film that Guangzhou Xinlaifu Magnetoelectric Co. Ltd. produces, the zirconia content of described ceramic diaphragm is 92 weight %, yittrium oxide content is 8 weight %.Described ceramic diaphragm is that diameter that 0.04 micron ceramic hollow microfilament is formed is 7 microns a microfilament bar by 200 diameters, and then to form diameter by 20 such microfilament bars be that 120 microns tow braiding obtains) cut into 55 * 740 millimeters diaphragm.The above-mentioned diaphragm that obtains, positive plate and negative plate is stacked successively according to the order of barrier film/negative plate/barrier film/positive plate, make the electrode group that is of a size of 3.2 * 33 * 55 millimeters.
(4) assembling of battery
LiPF6 and ethylene carbonate (EC), diethyl carbonate (DEC) and DMC (dimethyl carbonate) are configured to the solution that LiPF6 concentration is 1.0 mol (wherein, the volume ratio of EC, DEC and DMC is 1:1:1), obtain nonaqueous electrolytic solution.The package compound film with PET polyester/NY nylon/AL aluminium foil/CPP hydrostomia polypropylene multi-layer structure that is made of macromolecule membrane and metal forming that the electrode group that (3) are obtained is put into an end opening strikes out the battery case of the groove that has 3.5 * 33 * 55 millimeters, and inject above-mentioned nonaqueous electrolytic solution with the amount of 3.8g/Ah, the capacity of making after the sealing is 750mAh, and outside dimension is 3.8 * 35 * 62 millimeters laminated structure flexible packing lithium ion secondary battery A3.
Comparative Examples 1
The preparation of this Comparative Examples explanation reference lithium ion battery.
Prepare reference lithium ion battery AC1 according to the method for embodiment 1 and the content of each material, different is, is 20 microns with thickness, and voidage is that 40% PE individual layer microporous barrier replaces the ceramic diaphragm among the embodiment 1.
Comparative Examples 2
The preparation of this Comparative Examples explanation reference lithium ion battery.
Prepare reference lithium ion battery AC2 according to the method for embodiment 2 and the content of each material, different is, is 20 microns with thickness, and voidage is that three layers of microporous barrier of PP/PE/PP of 60% replace the ceramic diaphragm among the embodiment 2.
Comparative Examples 3
The preparation of this Comparative Examples explanation reference lithium ion battery.
Prepare reference lithium ion battery AC3 according to the method for embodiment 3 and the content of each material, different is, is 30 microns with thickness, and voidage is that three layers of microporous barrier of PP/PE/PP of 40% replace the ceramic diaphragm among the embodiment 3.
Performance test
The lithium ion battery AC1-AC3 that lithium ion battery A1-A3 that stove heat testing method below adopting obtains embodiment 1-3 respectively and Comparative Examples 1-3 obtain carries out the test of battery safety.
The test of stove heat:
Adopt lithium ion battery test cabinet with above-mentioned lithium ion cell charging (1C constant-current constant-voltage charging, charging upper limit 4.2V, cut-off current 20mA).Then battery is put in the high temperature furnace, the speed raising furnace temperature with 5 ℃ of per minute risings is elevated to 150 ℃, 160 ℃ and 170 ℃ up to temperature.Respectively battery was kept 60 minutes phenomenons such as whether the observation battery occurs smoldering, burning, blast down at 150 ℃, 160 ℃ and 170 ℃.The result is as shown in table 1.
Table 1
| 150 ℃ of stove heat test phenomenons | 160 ℃ of stove heat test phenomenons | 170 ℃ of stove heat test phenomenons | |
| Embodiment 1 | Do not have smolder, burning, explosion phenomenon | Do not have smolder, burning, explosion phenomenon | Do not have smolder, burning, explosion phenomenon |
| Embodiment 2 | Do not have smolder, burning, explosion phenomenon | Do not have smolder, burning, explosion phenomenon | Phenomenon appears smoldering |
| Embodiment 3 | Do not have smolder, burning, explosion phenomenon | Do not have smolder, burning, explosion phenomenon | Do not have smolder, burning, explosion phenomenon |
| Comparative Examples 1 | Phenomenon appears smoldering | Appearance is smoldered, combustion phenomena | Fried phenomenon occurs smoldering, burning |
| Comparative Examples 2 | Occur smoldering, burning, explosion phenomenon | Occur smoldering, burning, explosion phenomenon | Occur smoldering, burning, explosion phenomenon |
| Comparative Examples 3 | Do not have smolder, burning, explosion phenomenon | Appearance is smoldered, combustion phenomena | Appearance is smoldered, combustion phenomena |
From above-mentioned test result as can be seen, compare with the lithium ion battery of Comparative Examples 1-3 preparation, because what lithium ion battery of the present invention adopted is the excellent ceramic diaphragm of high-temperature stability, thereby the laminated structure flexible packing lithium ion secondary battery of wooden inventive embodiments 1, the square lithium ion secondary battery of embodiment 2, the winding flexible packing lithium ionic secondary cell of embodiment 3 at high temperature all has the excellent high-temperature security performance, and is better than the lithium ion battery that Comparative Examples 1-3 obtains greatly.
Claims (14)
1, a kind of lithium ion battery, this battery comprises electrode group and nonaqueous electrolytic solution, and described electrode group and nonaqueous electrolytic solution are sealed in the battery container, and described electrode group comprises positive pole, negative pole and barrier film, it is characterized in that, and described barrier film is a ceramic diaphragm; Described ceramic diaphragm is to be that the tow braiding of 20-200 micron forms by diameter, and every rhizoid bundle comprises that 5-50 root diameter is the microfilament bar of 1-15 micron, and every microfilament bar comprises that 100-500 root diameter is the ceramic hollow microfilament of 0.01-0.10 micron.
2, battery according to claim 1, wherein, the diameter of described tow is the 50-120 micron, and the radical of described microfilament bar is the 10-30 root, and diameter is the 5-10 micron, and the radical of described ceramic hollow microfilament is the 200-300 root, diameter is the 0.02-0.04 micron.
3, battery according to claim 1, wherein, the thickness of described ceramic diaphragm is the 5-60 micron.
4, battery according to claim 3, wherein, the thickness of described ceramic diaphragm is the 15-40 micron.
5, battery according to claim 1, wherein, the porosity of described ceramic diaphragm is 20-90%, the aperture is the 20-200 micron.
6, battery according to claim 5, wherein, the porosity of described ceramic diaphragm is 40-80%, the aperture is the 50-150 micron.
7, battery according to claim 1, wherein, described ceramic diaphragm contains zirconia and yittrium oxide, is benchmark with the total weight of described ceramic diaphragm, and described zirconic content is 80-95 weight %, and the content of yittrium oxide is 5-20 weight %.
8, the preparation method of the described battery of claim 1, this method comprises positive pole and the negative pole for preparing battery, and positive pole, negative pole and barrier film are prepared into an electrode group, and electrode group and the electrolyte that obtains is sealed in the battery case, it is characterized in that described barrier film is a ceramic diaphragm; Described ceramic diaphragm is to be that the tow braiding of 20-200 micron forms by diameter, and every rhizoid bundle comprises that 5-50 root diameter is the microfilament bar of 1-15 micron, and every microfilament bar comprises that 100-500 root diameter is the ceramic hollow microfilament of 0.01-0.10 micron.
9, method according to claim 8, wherein, the diameter of described tow is the 50-120 micron, and the radical of described microfilament bar is the 10-30 root, and diameter is the 5-10 micron, and the radical of described ceramic hollow microfilament is the 200-300 root, diameter is the 0.02-0.04 micron.
10, method according to claim 8, wherein, the thickness of described ceramic diaphragm is the 15-40 micron.
11, method according to claim 8, wherein, the porosity of described ceramic diaphragm is 40-80%, the aperture is the 50-150 micron.
12, method according to claim 8, wherein, described ceramic diaphragm contains zirconia and yittrium oxide, is benchmark with the total weight of described ceramic diaphragm, and described zirconic content is 80-95 weight %, and the content of yittrium oxide is 5-20 weight %.
13, method according to claim 8, wherein, the described method that anodal, negative pole and barrier film is prepared into an electrode group is for being stacked to stacked electrode group with positive plate, negative plate and barrier film according to the order of barrier film, positive plate, barrier film, negative plate or barrier film, negative plate, barrier film, positive plate.
14, method according to claim 8, wherein, the described method that anodal, negative pole and barrier film is prepared into an electrode group is for stacked and then be wound into the electrode group according to the order of barrier film, positive plate, barrier film, negative plate or barrier film, negative plate, barrier film, positive plate with positive plate, negative plate and barrier film earlier.
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| KR20140012109A (en) * | 2011-04-01 | 2014-01-29 | 스미토모덴키고교가부시키가이샤 | Molten salt battery |
| CN104485438B (en) * | 2014-12-25 | 2017-01-25 | 江苏清陶能源科技有限公司 | Ceramic diaphragm with high inorganic solid-phase content and application of ceramic diaphragm in lithium ion battery system |
| CN106711379A (en) * | 2016-12-06 | 2017-05-24 | 江苏楚汉新能源科技有限公司 | Ceramic diaphragm and preparation method and application thereof, and battery comprising ceramic diaphragm |
| CN108511785B (en) * | 2018-05-28 | 2020-12-01 | 名添科技（深圳）有限公司 | Anti-bulge power lithium battery |
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