CN101202361A - Lithium ion battery - Google Patents

Lithium ion battery Download PDF

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Publication number
CN101202361A
CN101202361A CNA2007100681934A CN200710068193A CN101202361A CN 101202361 A CN101202361 A CN 101202361A CN A2007100681934 A CNA2007100681934 A CN A2007100681934A CN 200710068193 A CN200710068193 A CN 200710068193A CN 101202361 A CN101202361 A CN 101202361A
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ion battery
carbonate
lithium ion
electrolyte
battery according
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王清泉
刘昊
邓龙征
郑利锋
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Wanxiang Group Corp
Wanxiang Electric Vehicle Co Ltd
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Wanxiang Group Corp
Wanxiang Electric Vehicle Co Ltd
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Priority to CNA2007100681934A priority Critical patent/CN101202361A/en
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    • Y—GENERAL TAGGING OF NEW TECHNOLOGICAL DEVELOPMENTS; GENERAL TAGGING OF CROSS-SECTIONAL TECHNOLOGIES SPANNING OVER SEVERAL SECTIONS OF THE IPC; TECHNICAL SUBJECTS COVERED BY FORMER USPC CROSS-REFERENCE ART COLLECTIONS [XRACs] AND DIGESTS
    • Y02—TECHNOLOGIES OR APPLICATIONS FOR MITIGATION OR ADAPTATION AGAINST CLIMATE CHANGE
    • Y02E—REDUCTION OF GREENHOUSE GAS [GHG] EMISSIONS, RELATED TO ENERGY GENERATION, TRANSMISSION OR DISTRIBUTION
    • Y02E60/00—Enabling technologies; Technologies with a potential or indirect contribution to GHG emissions mitigation
    • Y02E60/10—Energy storage using batteries

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Abstract

The invention relates to a li-ion battery, in particular to a power li-ion battery anode material. The invention improves the compaction density and processing performance of the anode material by mixing LiFePO4 and other lithium-contained anode materials such as LimAnOx. Compared with lithium manganate batteries and lithium cobalt oxide batteries which have been poured for industrialization, the battery prepared by the method has close ratio performance, more excellent circulation performance, safety performance and high-temperature performance, and completely meets the performance requirement of power supplies; meanwhile, the batteries which are prepared by the method have low cost, simple technique and realize industrialized application of lithium iron phosphate material.

Description

A kind of lithium ion battery
Technical field
The present invention relates to a kind of lithium ion battery, particularly relate to a kind of power lithium-ion battery positive electrode.
Background technology
Ferrousphosphate lithium material is reliable with its fail safe, have extended cycle life, advantages such as charge and discharge platform is stable, high-temperature behavior, become one of power lithium-ion battery positive electrode that has application prospect, but following shortcoming has hindered its practical application: (1) lithium ion spreads difficulty in LiFePO4, cause the utilance of active material low; (2) electronic conductivity of LiFPO4 is low, causes its heavy-current discharge performance poor.Existing research improves the performance of LiFePO4 by following several respects: the LiFePO4 of synthetic small particle diameter; Doping or coating improve the diffusivity of lithium ion; Add conductive agent and improve electronic conductivity; The LiFePO4 of solid phase synthesis cation defect etc.; But it is limited that high rate performance improves.(3) owing to LiFePO4 particle diameter little (1～5 μ m), the low (1～1.5g/cm of tap density 3), the big (10～30m of specific area 2/ g), the cathode slurry viscosity of using ferrousphosphate lithium material to make separately is rarer, is difficult for film forming and the heavy instability of film when the system film, causes battery consistency to be guaranteed.Therefore the ferrousphosphate lithium material commercial application that still is unrealized at present.
Summary of the invention:
The objective of the invention is to overcome the above-mentioned defective of prior art, provide a kind of under the condition that does not change the existing production technology of LiFePO 4, LiFePO 4Contain lithium anode material Li with other mA nO xThe method of mixing use improves the tap density and the processing characteristics of positive electrode.Adopt the battery of the method preparation to compare the lithium manganate battery and the cobalt acid lithium battery of invested in plantization, high rate performance is close, cyclicity, fail safe and high-temperature behavior are more excellent, the performance requirement that very meets electrical source of power, the battery of the method preparation simultaneously, cost is low, and technology is simple, has realized the commercial application of ferrousphosphate lithium material.
Above-mentioned purpose of the present invention is achieved in that a kind of lithium ion battery, comprise positive plate, negative plate, barrier film, electrolyte, positive plate and negative plate are made up of positive and negative collector and positive and negative active material layer bonded thereto respectively, electrolyte is by electrolytic salt and solvent composition, and described positive electrode active materials is LiFePO 4And Li mA nO xMixture, wherein A is one or more of Co, Ni, Mn, Li, B, Mg, Al, Ti, Cr, Fe, Co, Ni, Cu, Zn, Ga, Y, La, F, O, I, S, Se, m=1～4, n=1～5, x=2～12, LiFePO 4Account for 20～80% of positive electrode active materials weight.Battery of the present invention comprises positive plate respectively, and negative plate, barrier film, electrolyte, positive plate and negative plate are made up of positive and negative collector and bonding positive and negative active material layer thereon respectively.Described collector adopts paper tinsel shape collector usually, and positive electrode active materials is by LiFePO 4And Li mA nO xMix described Li in proportion according to particle size distribution mA nO xIn fact can be formed by the different kinds of ions compound, that its is represented is LiMn 2O 4, LiCoO 2, LiNiO 2In any one or multiple mixture.LiFePO 4And Li mA nO xSimple mixing can reach purpose of the present invention.
Matrix oxide involved in the present invention can be used Li mA nO xExpression, wherein A represents the non-lithium metallic element of electrode material, as Co, Mn, Ni etc. or their mixed system and doping vario-property system but preferred Co, Mn, Ni, m, n, x represent the ratio of various elements, their scope is m=1～4, n=1～5, x=2～12 it should be noted that m, n, x are not must be integer.Li mA nO xPrimary structure comprises LiCoO 2, LiNiO 2, LiMn 2O 4And on their bases, replace LiCoO by one or more elements among Li, B, Mg, Al, Ti, Cr, Fe, Co, Ni, Cu, Zn, Ga, Y, La, F, O, I, S, the Se 2, LiNiO 2, LiMn 2O 4In the compound that obtained of non-lithium metallic element or with LiBO2, Li2CO3, LiCoO2, LiNi 0.2Co 0.8O 2, surface such as ZnO coats LiCoO 2, LiNiO 2, LiMn 2O 4The various materials that obtained.Related positive electrode can be used (100-y) LiFePO4/yLi mA nO xExpression, y represents Li mA nO xPercetage by weight in positive electrode, scope are 20%～80%, and optimum range is 30%～60%, works as Li mA nO xContent is lower than at 20% o'clock, and positive electrode high-rate discharge ability and tap density are improved limited, work as Li mA nO xSurpass at 80% o'clock,, can obviously reduce battery security and high-temperature behavior simultaneously the not significant effect of the raising of performance.Preparing the employed raw material of these materials can be chemical pure or analytical reagent, also can be the various compounds that satisfy the actual instructions for use of battery.
Compare with existing the whole bag of tricks, characteristics of the present invention are:
(1) Li mA nO xDo not enter the lattice of basis material, thereby do not influence LiFePO 4The stability of material itself and key property can be brought into play LiFePO simultaneously 4The cyclical stability of battery and resistance to elevated temperatures.
(2) compare LiFePO 4, Li mA nO xHave higher conductivity, also have lithium simultaneously and can embed-Tuo embedding performance, can improve the battery high rate performance simultaneously.
(3) do not changing existing LiFePO 4Under the condition of production technology, by mixing Li mA nO xMaterial, the tap density of positive electrode is from 1.3g/cm 3Rise to 2.0g/cm 3More than, improved the viscosity of cathode slurry, be easy to film forming, film is heavily stable, has improved the consistency of battery greatly, has realized the commercial application of ferrousphosphate lithium material.
Table 1 is LiFePO 4+ LiMn 2O 4Each proportioning material tap density;
Figure A20071006819300061
Table 2 is LiMn 2O 4, C-LiFePO 4(carbon coating) and 60%LiFePO 4+ 40%LiMn 2O 4The contrast of battery high rate performance;
LiMn 2O 4 C-LiFePO 4 60％LiFePO 4+40％LiMn 2O 4
2C/1C 97％ 94％ 95％
5C/1C 83％ 29％ 83％
The data of last table are respectively with LiMn 2O 4, C-LiFePO 4(carbon coating) and 60%LiFePO 4+ 40%LiMn 2O 4For positive electrode is made battery, other condition is identical resulting, and these three kinds of battery 2C discharge capacity/0.3C discharge capacities are respectively 97%, 94%, 95%; 5C discharge capacity/0.3C discharge capacity is respectively 83%, 29%, 83%.
Positive electrode is preferably a kind of mixture that mixes in the following manner among the present invention: with Li mA nO xAnd LiFePO 4Prepare burden in proportion according to particle size distribution separately, fully mix in batch mixer, the present invention uses above two kinds of materials with, can overcome deficiency, mutual supplement with each other's advantages.Accompanying drawing 1,2,3 has shown the obvious contrast of this change.
Lithium ion battery of the present invention can adopt liquid system or polymeric system.
Description of drawings
Fig. 1 is the multiplying power discharging curve of LiMn2O4;
Fig. 2 is LiFePO 4The multiplying power discharging curve;
Fig. 3 is 60%LiFePO 4/ 40%LiMn 2O 4The multiplying power discharging curve.
Embodiment
Embodiment 1:
Its concrete manufacture method of a kind of making of lithium ion battery is as follows:
1.1 anodal preparation
1.1.1 the preparation of cathode film
LiFePO 4 (LiFePO 4): 420g
LiMn2O4 (LiMn 2O 4) 280g
Polyvinylidene fluoride (PVDF): 110g
Acetylene black: 60g
Dibutyl phthalate: 80g
Acetone: 2000g
Above-mentioned material mixed stir into slurry, mixing speed is 2800r/min, and stirring the duration is 3 hours.Make film with film-making machine and heavily be 250g/m 2Cathode film, film-making machine walking speed 10cm/s, bake out temperature are 90 ℃.
1.1.2 collector preliminary treatment
Acetylene black 100g
Ethylene acrylic acid co polymer (EAA) 30g
Acetone 1200g
Above material even stirring in mixer made slurry, mixing speed 3000r/min, mixing time 3 hours is sprayed on slurry on the aluminium collector with spray net machine then, and spray pressure is 3 atmospheric pressure, and distance is 0.5m, again with 120 ℃ of oven dry.
1.1.3 anodal last preparation
Cathode film is cut into the size of 200*130mm, carry out hot pressing after cathode film that a slice cuts and the stack of a slice aluminium collector, hot pressing temperature is 110 ℃, pressure gap 50 μ m.
1.2 negative pole preparation
1.2.1 the preparation of negative electrode film
Carbonaceous mesophase spherules 300g
Polyvinylidene fluoride (PVDF): 60g
Acetylene black: 30g
Dibutyl phthalate: 40g
Acetone: 2500g
Above-mentioned material even stirring in mixer made slurry, mixing speed 3000r/min, mixing time two hours.Make film with film-making machine and heavily be 210g/m 2Cathode film, film-making machine walking speed 10cm/s, bake out temperature are 80 ℃.
1.2.2 the two sides preliminary treatment of copper collector is identical with above-mentioned aluminium collector processing mode.
1.2.3 the last preparation of negative pole
Negative electrode film is cut into the size of 200*130mm, a slice copper collector two sides two negative electrode film of stack are carried out hot pressing, hot pressing temperature is 130 ℃, pressure gap 45 μ m.
1.3 barrier film preparation
Polyvinylidene fluoride (PVDF): 350g
Dibutyl phthalate: 175g
Silicon dioxide: 120g
Acetone: 5000g
Above-mentioned material is mixed in mixer, mixing speed 6000r/min, mixing time is four hours, uses film-making machine to make the barrier film that thickness is 40 μ m, and walking speed is 100mm/s, and bake out temperature is 90 ℃.
1.4 the preparation of monolithic electricity core
Mode with positive pole/barrier film/negative pole/barrier film/positive pole stacks gradually, and carries out hot pressing on hot press, 130 ℃ of hot pressing temperatures, and the thickness after the hot pressing is 0.7mm.
1.5 extraction
Battery after synthetic is put in the absolute methanol extracts, in order to remove the plasticizer in the battery, 60 ℃ of dryings 15 hours in baking oven then.
1.6 the welding of lug
The positive and negative electrode collector of per 10 monolithics welds together with the nickel lug respectively, forms the exit of positive and negative electrode.
1.7 annotate electrolyte and battery pack
Use the aluminum-plastic composite membrane battery pack; the inlet that keeps electrolyte; in the glove box of argon shield, be that the mixture of 1: 1 ethylene carbonate and diethyl carbonate, the electrolyte of hexafluoro phosphorus lithium that solute is 1mol/L inject the aluminum-plastic composite membrane bag with organic solvent, seal liquid injection port.
1.8 changing into of battery
Battery was placed 6 hours, changed into the 0.3C system of changing into again.Test result is as follows:
Discharge capacity is 9.2Ah first.
1.9 the ageing of battery
With one week of battery ageing after changing into.
Above-mentioned battery parallel connection and series connection are assembled into battery pack, with practical requirement.
Embodiment 2:
2.1 positive plate preparation
LiFePO 4 (LiFePO 4): 420g
LiMn2O4 (LiMn2O 4) 280g
Polyvinylidene fluoride (PVDF): 110g
Conductive agent (KS): 70g
NMP (N-methyl arsenic is pressed against alkane ketone): 2000g
Above-mentioned material mixed stir into slurry, mixing speed is 2800r/min, and stirring the duration is 3 hours.Slurry is evenly coated on the aluminium foil of 22 μ m, and dry, compressing tablet, cut in flakes by 200 * 130mm size, and dry again.
2.2 negative plate preparation
Carbonaceous mesophase spherules 300g
Polyvinylidene fluoride (PVDF): 60g
Conductive agent (KS): 30g
NMP (N-methyl arsenic is pressed against alkane ketone) 2500g
Above-mentioned material mixed stir into slurry, mixing speed is 3000r/min, and stirring the duration is 2 hours.Slurry is evenly coated on the Copper Foil of 18 μ m, and dry, compressing tablet, cut in flakes by 200 * 130mm size, and dry again.
2.3 the preparation of electric core
Select Celgard2340 type porous polypropylene film for use, thickness is 40 μ m, cuts and is of a size of 210 * 140mm, stacks gradually in the mode of positive pole/barrier film/negative pole, and thickness is 7.6mm.
2.4 the welding of lug
The positive and negative electrode collector of per 10 monolithics welds together with the nickel lug respectively, forms the exit of positive and negative electrode.
2.5 annotate electrolyte and battery pack
Use the aluminum-plastic composite membrane battery pack; the inlet that keeps electrolyte; in the glove box of argon shield, be that the mixture of 1: 1 ethylene carbonate and diethyl carbonate, the electrolyte of hexafluoro phosphorus lithium that solute is 1mol/L inject the aluminum-plastic composite membrane bag with organic solvent, vacuum is sealed liquid injection port.
2.6 changing into of battery
Battery was placed 6 hours, changed into 0.3C again.
Test result is as follows: discharge capacity is 9.2Ah first.
2.7 the ageing of battery
With one week of battery ageing after changing into.
Above-mentioned battery parallel connection and series connection are assembled into battery pack, with practical requirement.
Embodiment 3～8 is substantially the same manner as Example 1, and different is that its positive electrode that adopts sees Table 3
Figure A20071006819300111
。

Claims (10)

1. lithium ion battery, comprise positive plate, negative plate, barrier film, electrolyte, positive plate and negative plate are made up of positive and negative collector and positive and negative active material layer bonded thereto respectively, electrolyte is characterized in that by electrolytic salt and solvent composition described positive electrode active materials is LiFePO 4And Li mA nO xMixture, wherein A is one or more of Co, Ni, Mn, Li, B, Mg, Al, Ti, Cr, Fe, Cu, Zn, Ga, Y, La, F, O, I, S, Se, m=1～4, n=1～5, x=2～12, LiFePO 4Account for 20～80% of positive electrode active materials weight.
2. lithium ion battery according to claim 1 is characterized in that: Li mA nO xIn A be one or more of Co, Ni, Mn, the tap density of described positive electrode active materials is at 1.7～2.1g/m 3Between.
3. lithium ion battery according to claim 1 and 2 is characterized in that: barrier film is selected polypropylene microporous film or three layers of compound microporous membrane of polypropylene, polyethylene/polypropylene or above-mentioned two kinds of modified diaphragms that barrier film is a matrix for use.
4. lithium ion battery according to claim 1 and 2 is characterized in that: negative active core-shell material is one or more of carbon dust, carbonaceous mesophase spherules, native graphite or its modifier, oil coke or its modifier.
5. lithium ion battery according to claim 1 and 2 is characterized in that: lithium salts can be selected LiPF for use in the electrolyte 6, LiASF 6, LiClO 4, LiN (CF 3SO 2) 2, LiBF 4, LiSbF 6, LiCF 3SO 3In one or more, electrolyte solvent is one or more in propene carbonate, ethylene carbonate, diethyl carbonate, dimethyl carbonate, carbonic acid Methylethyl ester, diethyl carbonate, the dimethyl ethane, electrolytical concentration is 0.1～2mol/L.
6. lithium ion battery according to claim 3 is characterized in that: negative active core-shell material is a carbon dust, as one or more of carbonaceous mesophase spherules, native graphite or its modifier, oil coke or its modifier.
7. lithium ion battery according to claim 3 is characterized in that: lithium salts can be selected LiPF for use in the electrolyte 6, LiASF 6, LiClO 4, LiN (CF 3SO 2) 2, LiBF 4, LiSbF 6, LiCF 3SO 3In one or more, electrolyte solvent is one or more in propene carbonate, ethylene carbonate, diethyl carbonate, dimethyl carbonate, carbonic acid Methylethyl ester, diethyl carbonate, the dimethyl ethane, electrolytical concentration is 0.1～2mol/L.
8. lithium ion battery according to claim 4 is characterized in that: lithium salts can be selected LiPF for use in the electrolyte 6, LiASF 6, LiClO 4, LiN (CF 3SO 2) 2, LiBF 4, LiSbF 6, LiCF 3SO 3In one or more, electrolyte solvent is one or more in propene carbonate, ethylene carbonate, diethyl carbonate, dimethyl carbonate, carbonic acid Methylethyl ester, diethyl carbonate, the dimethyl ethane, electrolytical concentration is 0.1～2mol/L.
9. lithium ion battery according to claim 1 and 2 is characterized in that: Li mA nO xIon is by LiBO2, Li2CO3, LiCoO2, LiNi 0.2Co 0.8O 2, behind one or more parcels among the ZnO again and LiFePO 4Mix.
10. lithium ion battery according to claim 2, it is characterized in that: barrier film is selected polypropylene microporous film or three layers of compound microporous membrane of polypropylene, polyethylene/polypropylene or above-mentioned two kinds of modified diaphragms that barrier film is a matrix for use, negative active core-shell material is one or more of carbon dust, carbonaceous mesophase spherules, native graphite or its modifier, oil coke or its modifier, and lithium salts is selected LiPF for use in the electrolyte 6, LiASF 6, LiClO 4, LiN (CF 3SO 2) 2, LiBF 4, LiSbF 6, LiCF 3SO 3In one or more, electrolyte solvent is one or more in propene carbonate, ethylene carbonate, diethyl carbonate, dimethyl carbonate, carbonic acid Methylethyl ester, diethyl carbonate, the dimethyl ethane, electrolytical concentration is 0.1～2mol/L, LiFePO 4Account for 20%～80% of positive electrode active materials weight.
CNA2007100681934A 2007-04-24 2007-04-24 Lithium ion battery Pending CN101202361A (en)

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CN101800333A (en) * 2010-05-05 2010-08-11 天津力神电池股份有限公司 Lithium ion battery capable of improving safety
CN102024947A (en) * 2010-11-09 2011-04-20 罗绍华 LiFePO4/Li-Al-O composite positive electrode material and preparation method thereof
CN102315434A (en) * 2010-06-30 2012-01-11 株式会社日立制作所 Lithium rechargeable battery
WO2012079389A1 (en) * 2010-12-16 2012-06-21 天津力神电池股份有限公司 Method for inhibiting expansion of lithium ion polymer battery
CN102544571A (en) * 2010-11-02 2012-07-04 韩国电子通信研究院 Lithium rechargeable battery
CN103022552A (en) * 2012-12-20 2013-04-03 中国东方电气集团有限公司 Long-life lithium ion battery used under shallow charging and discharging conditions and preparation method of same
CN103165897A (en) * 2011-12-14 2013-06-19 比亚迪股份有限公司 A cathode material for lithium-ion batteries, lithium-ion battery cathodes, and lithium-ion batteries
CN105355853A (en) * 2015-12-15 2016-02-24 重庆裕祥新能源电池有限公司 Preparing method of lithium battery anode material for motorcycle
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CN105702961A (en) * 2014-11-27 2016-06-22 比亚迪股份有限公司 Positive pole material and lithium ion battery
CN106410169A (en) * 2016-12-08 2017-02-15 深圳市鑫永丰科技有限公司 Compound anode material used for lithium ion battery, preparation method of compound anode material, and lithium ion battery
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CN108183210A (en) * 2017-12-26 2018-06-19 北京国能电池科技有限公司 Anode material for lithium-ion batteries, lithium ion battery and preparation method thereof
CN109126804A (en) * 2018-08-24 2019-01-04 广东工业大学 A kind of boron doping LaCoO3Bifunctional catalyst and its preparation method and application
CN110048160A (en) * 2019-05-22 2019-07-23 湖北诺邦科技股份有限公司 A kind of preparation method of ferrousphosphate lithium material and matching compatibility electrolyte and its battery
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CN101800333A (en) * 2010-05-05 2010-08-11 天津力神电池股份有限公司 Lithium ion battery capable of improving safety
CN102315434A (en) * 2010-06-30 2012-01-11 株式会社日立制作所 Lithium rechargeable battery
US9083032B2 (en) 2010-11-02 2015-07-14 Intellectual Discovery Co., Ltd. Lithium rechargeable battery having a mixed anode active material including nanotubes
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CN102024947A (en) * 2010-11-09 2011-04-20 罗绍华 LiFePO4/Li-Al-O composite positive electrode material and preparation method thereof
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CN103165897A (en) * 2011-12-14 2013-06-19 比亚迪股份有限公司 A cathode material for lithium-ion batteries, lithium-ion battery cathodes, and lithium-ion batteries
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CN109126804A (en) * 2018-08-24 2019-01-04 广东工业大学 A kind of boron doping LaCoO3Bifunctional catalyst and its preparation method and application
CN110048160A (en) * 2019-05-22 2019-07-23 湖北诺邦科技股份有限公司 A kind of preparation method of ferrousphosphate lithium material and matching compatibility electrolyte and its battery
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