CN100466364C - Safety lithium-ion battery - Google Patents
Safety lithium-ion battery Download PDFInfo
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- CN100466364C CN100466364C CNB2005101223633A CN200510122363A CN100466364C CN 100466364 C CN100466364 C CN 100466364C CN B2005101223633 A CNB2005101223633 A CN B2005101223633A CN 200510122363 A CN200510122363 A CN 200510122363A CN 100466364 C CN100466364 C CN 100466364C
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- lithium ion
- safety
- ion cell
- negative
- battery
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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
Abstract
The invention is concerned with the safety lithium ion battery, including: the anode, the cathode, the septum and the non-water electrolyte, the anode and the cathode consists of the metal foil afflux and the active material coat, the characteristic is: the anode coat includes nickel cobaltous manganese lithium oxide active material with layer-shape structure; the cathode includes one or two kinds of active material, such as carbon fiber, sphere graphite and scaled graphite, the weight contain of the carbon fiber is 1%-5%. The invention can reduce the risk of heat un-control, improve the safety of the lithium ion battery.
Description
Technical field
The invention belongs to technical field of lithium ion, particularly relate to a kind of safety lithium ion cell.
Background technology
Lithium ion battery is by negative plate, positive plate, electrolyte and prevent that between between positive/negative plate the barrier film of its short circuit from forming.For example, its negative plate is to be fixed on absorption on the collector/the emit carbonaceous material of lithium ion; Positive plate is to be fixed on absorption on the collector/the emit composite oxides such as manganese oxide lithium that resembling of lithium ion has cobalt-lithium oxide, the nickel-based oxide of layer structure and have spinel structure; Electrolyte is to be dissolved with LiPF
6Deng the solution of aprotic organic solvent.
Positive plate and negative plate be made into thin plate or paper tinsel shape, then battery lead plate and intervenient barrier film is stacked in order or helical form spooling and form electric core.Again this electric core pack in the iron or lighter aluminum metal case or lamination A1 flexible packaging film battery case of stainless steel, nickel plating, the electrolyte that reinjects, sealing and make battery.
Because the capacity of cobalt-lithium oxide and nickel oxide lithium material is big, real density is also bigger, therefore adopts the lithium ion battery of above-mentioned two kinds of materials to have higher specific energy usually.But, use the security performance of overcharging resisting etc. of lithium ion battery of above-mentioned two kinds of materials relatively poor.And the discharge capacity of spinelle manganese oxide lithium is lower, but adopts the security performance of lithium ion battery of this kind material better.
At present, there is several different methods can improve the security performance of lithium ion battery, for example, use the barrier film of PP/PE/PP three-decker, methods such as additives such as adding fire retardant, the coating of employing ceramic material with hot blocking function.But when big multiplying power was overcharged, the reliability of these means and exploitativeness still can not be protected.
Summary of the invention
The present invention has the technical problem that lithium ion battery exists now for solving, and a kind of safety lithium ion cell is provided.
The purpose of this invention is to provide a kind of positive and negative electrode material and proportioning of safe lithium ion battery, the fail safe of lithium ion battery, particularly overcharge resistance performance can be improved.
Characteristics of the present invention are to select the active material of composite material as positive pole for use, and the ratio by preferred positive pole/negative active core-shell material, improve the large current charge bearing performance of electrode, to improve the security performance that comprises overcharging resisting of lithium ion battery.
The present invention adopts following technical scheme:
Safety lithium ion cell comprises positive pole, negative pole, barrier film and nonaqueous electrolytic solution, and anodal and negative pole constitutes by metal forming collector and the active material coating that contains that is coated in its surface, and be characterized in: anodal coating comprises the nickel cobaltous manganese lithium oxide active material of layer structure; The negative pole coating comprises one or both active materials of carbon fiber and spherical graphite, flaky graphite, and wherein the weight content of carbon fiber is 1-5%.
The overcharging resisting ability of positive pole and even battery is improved, and simultaneously negative pole adopts the carbon fiber that conducts electricity very well, thereby has reduced the internal resistance of cell, when having avoided high magnification to overcharge in the lithium electrolysis of negative terminal surface, thereby the thermal response that lowers negative pole is out of control.
The present invention can also adopt following technical measures:
Described a kind of safety lithium ion cell is characterized in: anodal coating comprises the cobalt-lithium oxide of layer structure and the nickel cobaltous manganese lithium oxide active material of layer structure.
Described a kind of safety lithium ion cell is characterized in: the weight content of active material cobalt nickel oxide manganses lithium is not less than 20% in the anodal coating.
Adopt the positive pole of the blended anode active material of the above cobalt nickel oxide manganses lithium of 20wt%, under the prerequisite of the chemical property that does not change lithium ion battery substantially, can guarantee fully that lithium ion battery is overcharging etc. under the abuse conditions, battery is not on fire not to explode.
Described a kind of safety lithium ion cell is characterized in: positive electrode active materials weight is 1.5-2.2 times of negative active core-shell material coating weight.
Described a kind of safety lithium ion cell is characterized in: positive electrode active materials weight is 1.75-2 times of negative active core-shell material coating weight.
Described a kind of safety lithium ion cell is characterized in: the negative active core-shell material carbon fiber is a carbon nano-fiber.
Described a kind of safety lithium ion cell is characterized in: being shaped as of battery is cylindrical, oval, square or button shaped.
Though the present invention has adopted the mixture of cobalt-lithium oxide and cobalt nickel oxide manganses lithium as positive electrode active materials, the present invention is not limited in cobalt-lithium oxide, can be used for positive electrode active materials LiNiO of the present invention
2, LiCo
xNi
1-xO
2Deng, another kind of positive electrode active materials can be LiNi
xCo
yMn
1-x-yO
2, LiMn
2O
4, Li
2Mn
2O
4, LiFePO
4Deng.Certainly the derivative that also comprises the above-claimed cpd that elements such as Al, Mg mix.
As lithium ion battery of the present invention, it is characterized in that being that negative pole comprises the carbon nano-fiber of 1-5wt%.This is because a certain amount of by adding, the carbon nano-fiber of certain-length, can fully guarantee in the electrode between active material and and collector between conductivity.Simultaneously, can make that again the combination property of electrode is guaranteed.The length of fiber surpasses 20 microns, then might make the part fiber pass barrier film and arrive electrode, causes the micro-short circuit between positive/negative plate.In addition, if addition surpasses 5wt%, then must add the adhesive force that a large amount of binding agents could keep electrode material layer simultaneously.Excessive binding agent then is the reason that causes the electrode internal resistance to raise.Therefore, the addition of carbon nano-fiber is to be no more than 5wt% for well; If addition very little＜1wt%, then do not reach and improve negative maximum current charges performance.
The present invention exemplifies is gas-phase grown nanometer carbon fibre (VGCF), also carbon black, acetylene black (AB) and stable metal nano fiber such as Ni etc. in addition.Optimum fiber shape electric conducting material.Because fibrous electric conducting material is suitable for the conduction approach of keeping.
Stratiform nickel-based oxide of the present invention is LiNi
1/3Co
1/3Mn
1/3O
2, form but be not limited only to this, also can be that Mn content is no more than the ternary layered compound that the transition metal molar content gets other components of 1/2, but with the component of high manganese low Ni, Co for well.But the also compound of the molar content of doped with Al, Mg or Li between 1-1.1.
Though lifted spherical graphite and scale shape graphite, can be used for negative active core-shell material of the present invention and be not limited only to this, also can be the carbonaceous material of easy graphitized carbon material and hard carbon etc. and the mixture of above-mentioned material as can be used for negative material class of the present invention.
As electrolyte of the present invention, can comprise one or more mixture of following organic solvent.Ethyl carbonate (EC), propene carbonate (PC), dimethyl carbonate (DMC), ethyl-methyl carbonic ester (EMC), diethyl carbonate (DEC), gamma-butyrolacton (GBL), sulfolane, methyl-sulfoxide, acetonitrile (AN), dimethyl formamide, diethylformamide, 1,2-dimethoxy-ethane, 1,2-diethoxyethane, oxolane (THF), 2-methyltetrahydrofuran, dioxolanes, methyl acetic acid ester isopolarity solvent.For obtaining good cell discharge performance and life-span, preferably make and in above-mentioned solvent, contain ethylene carbonate (EC).
The electrolytic salt that is dissolved in the electrolyte solvent can comprise following single electrolytic salt and composition thereof.LiPF for example
6, LiClO
4, LiBF
4, LiAsF
6, LiCF
3CO
2, LiCF
3(CF)
3, LiCF
3(C
2F
5)
3, LiCF
3SO
3, LiN (SO
2CF
3)
2, LiN (SO
2CF
2CF
3)
2, LiN (COCF
3)
2, LiN (COCF
2CF
3)
2, LiBOB and LiPF
3(CF
2CF
3)
3Be preferably in and partly contain LiPF in the electrolytic salt
6Or LiBF
4, and can on negative pole, form good epithelium and obtain good flash-over characteristic and life-span.
Simultaneously for the transition that suppresses irreversible capacity and negative material surface SEI epithelium grow up, preferably add additive such as vinylene carbonate (VC) and derivative thereof, as 4,5-dimethyl vinylene carbonate, 4,5-diethyl vinylene carbonate, 4,5-dipropyl vinylene carbonate, 4-ethyl-5-methyl carbonic acid vinylene, 4-ethyl-5-propyl group vinylene carbonate.Annular in addition sulfuric ester also helps forming good SEI, as glycol sulfate, 1,2-propylene glycol sulfuric ester, 1,2-butanediol sulfuric ester, 1,3-butanediol sulfuric ester, 2,3-butanediol, benzoglycols sulfuric ester etc.
Slider of the present invention can adopt braid, non-woven fabric, micropore synthetic resin film etc.In the above-mentioned diaphragm material, the polyolefin micro-porous film of special preferred microporous synthetic resin film, especially preferably polyethylene and microporous polypropylene membrane or their composite micro porous film etc.The adopted reason of these TPO micro-porous films is that it is better than thickness preferably, film-strength, film resistance characteristic.
If the employing colloidal electrolyte, then it can doublely do separator again.In this case, can use porose copolymer solid electrolyte, make it contain electrolyte again.
Battery of the present invention can be made into column type, oval, square, button shaped and the folded film flexible package of A1 etc.Capacity can be tens of mAh to tens of Ah even more than the 100Ah.But when making high capacity lithium ion battery, with column type, oval, square for well.
Advantage that the present invention has and good effect:
By adopting positive pole of the present invention, when the caloric value of battery when overcharging is inhibited, reduce the danger of thermal runaway, adopt both positive and negative polarity proportioning of the present invention, and adopting the negative pole that adds the fiber conductive agent, the electron conduction of negative pole is improved, and has realized the large current charge performance of lithium ion battery negative, avoid the lithium electrolysis, improve the security performance of lithium ion battery.
Lithium ion battery of the present invention can be widely used in 3C electronic equipment, space power supply, electric motor car, hybrid vehicle, power supplys such as electric tool and various boost motors.
Description of drawings
Fig. 1. safety lithium ion cell structural representation of the present invention;
Wherein, 1-battery cover, 2-insulating washer, 3-anode ear, 4-positive pole, 5-barrier film, 6-battery case, 7-safety valve, 8-negative electrode lug, 9-negative pole.
Fig. 2. Fig. 1 safety lithium ion cell positive plate and negative plate sectional schematic diagram;
Wherein, 10,12 is positive electrode active materials coating (positive and negative), and 11 is plus plate current-collecting body; 13,15 is negative active core-shell material coating (positive and negative), and 14 is negative current collector.
Fig. 3. the present invention adopts the charging and discharging curve of the lithium ion battery of blended anode material and comparative example cobalt-lithium oxide material to compare schematic diagram; 16: adopt LiCoO
2The battery of positive electrode active materials; 17: adopt in the active material to contain 20%LiNi
1/3Co
1/3Mn
1/3O
2And 80%LiCoO
2The battery of positive pole.
Fig. 4. temperature and change in voltage schematic diagram during the overcharging of lithium ion battery that the present invention adopts blended anode material and comparative example cobalt-lithium oxide material.18: adopt LiCoO
2The overcharged voltage change curve of the battery of positive electrode active materials; 19: adopt in the active material to contain 20%LiNi
1/3Co
1/3Mn
1/3O
2And 80%LiCoO
2The overcharged voltage change curve of battery of positive pole; 20: adopt LiCoO
2Variations in temperature during the over-charging of battery of positive electrode active materials; 21: adopt in the active material to contain 20%LiNi
1/3Co
1/3Mn
1/3O
2And 80%LiCoO
2The over-charging of battery of positive pole the time variations in temperature.
Embodiment
For further understanding summary of the invention of the present invention, characteristics and effect, illustrative example is elaborated as follows now:
With reference to accompanying drawing 1, Fig. 2, Fig. 3 and Fig. 4.
Safety lithium ion cell, comprise anodal 4, negative pole 9, barrier film 5 and nonaqueous electrolytic solution, there are battery case 6, battery cover 1, insulating washer 2, safety valve 7 in the outside, wherein, anodal 4 by aluminum foil current collector 11 be coated in the cobalt-lithium oxide that comprises layer structure on its surface and the nickel cobaltous manganese lithium oxide active material coating 10 and 12 of layer structure constitutes; Plus plate current-collecting body 11 is connected with anode ear 3.Negative pole 9 by Copper Foil collector 14 and be coated in its surface comprise Nano carbon fibers peacekeeping spherical graphite, flaky graphite active material 13 and 15 constitutes, negative current collector 14 is connected with negative electrode lug 8.
1. the making of positive plate:
Take by weighing LiCoO by weight 4:1
2And LiNi
1/3Co
1/3Mn
1/3O
2Positive electrode active materials, with mixed powder machine mechanical mixture 30 minutes, weigh mixture, adhesive and conductive agent then, by N-N-methyl-2-2-pyrrolidone N-(NMP) solution of the positive electrode active materials mixture of 93wt%, polyvinylidene fluoride (PVdF) bonding agent and to make the content of PVdF be 4.5wt%, 2.5wt%VGCF as electric conducting material, mix and form cathode mix, in mixture, add NMP and prepare pastel with mixer, then this pastel is coated onto equably the two sides that thickness is 20 μ m aluminium foils, again drying, roll-in and make positive plate.Coating weight is 22mg/cm
2
2. the preparation of negative plate:
Carbonaceous mesophase spherules MCMB in 20% (weight), 70% flaky graphite, the PVdF of the VGCF of 2% (weight) and 8% (weight) (the solution mode with NMP adds) makes pastel, then this pastel is coated onto equably the two sides that thickness is 10 μ m Copper Foils, drying again, roll-in and make negative plate.Coating weight is 11mg/cm
2
The microporous polyethylene film that is about 25 microns with thickness is made diaphragm body.
The nonaqueous electrolyte that uses is for being dissolved with 1mol/lLiPF
6The mixed solvent solution of EC+DEC+DMC (volume ratio 1:1:1), add vinylene carbonate 1.0wt% (electrolyte total amount relatively) on this basis.
3. the assembling of battery:
Stacked winding forms electric core, inserts cylinder, welds electrode in order, fluid injection is sealed again after 60 ℃ of vacuumize above-mentioned anodal 4, barrier film 5, negative pole 9.So be assembled into cylindrical battery as battery A1, and carry out electro-chemical test as follows.
4. charge-discharge test:
At first carried out volume test.Be charged as the CC-CV pattern; Discharge is the CC pattern.Promptly use 0.2C multiplying power constant current charge to 4.2V, the 4.2V constant voltage is 2 hours then; Discharge ends to 2.75V with 0.2C multiplying power constant current discharge equally.The discharge capacity that obtains in order to last method is as initial capacity, and discharge and likening to of charge capacity are efficiency for charge-discharge.
5. security test:
Overcharge respectively after above-mentioned Experimental cell is full of electricity, cross to put and test with external short circuit.Promptly same with volume test, all be charged to 4.2V with CC-CV, again the different experiments battery of same composition and capacity is overcharged till safety device work with the electric current of 1C respectively, recording voltage changes and the battery hull-skin temperature changes; Overdischarge is to 0V; Resistance wire with 5 milliohms carries out the external short circuit experiment.The result who carries out safety experiment by above method is organized in the table 1.The security performance of wherein overcharging is by 5V, measurement in 2 hours.
Except LiCoO
2And LiNi
1/3Co
1/3Mn
1/3O
2Weight ratio 2:1 beyond, other all identical and made battery A2 of the present invention with embodiment 1, its measurement result is recited in the table 1 equally.
Except LiCoO
2And LiNi
1/3Co
1/3Mn
1/3O
2Weight ratio 1:1 beyond, other all identical and made battery A3 of the present invention with embodiment 1, its measurement result is recited in the table 1 equally.
Positive electrode active materials LiCoO
2And LiNi
1/3Co
1/3Mn
1/3O
2Weight ratio 1:1, the coating weight of negative pole is 12.6mg/cm
2In addition, other all identical and made battery A4 of the present invention with embodiment 1, its measurement result is recited in the table 1 equally.
Comparative example 1
Except positive electrode active materials uses LiCoO separately
2In addition, other all identical and made relatively battery B1 with embodiment 1, its measurement result is recited in the table 1 equally.
Comparative example 2
Except positive electrode active materials uses LiCoO separately
2, negative pole does not add conductive agent VGCF and coating weight is 10mg/cm
2In addition, other all identical and made relatively battery B2 with embodiment 1, its measurement result is recited in the table 1 equally.
Table 1
| Battery | Capacity mAh | Overcharge | The maximum temperature of battery lateral wall when overcharging | Cross and put | External short |
| Embodiment A | |||||
| 1 | 725 | No change | 65 | Safety | |
| Embodiment A | |||||
| 2 | 731 | No change | 62 | Safety | |
| Embodiment A | |||||
| 3 | 735 | No |
60 | Safety | |
| Embodiment A | |||||
| 4 | 715 | No change | 67 | Safety | Safety |
| Comparative example B1 | 720 | Thermal runaway | 85 (because thermal runaway makes safety valve work) | Safety | Safety |
| Comparative example B2 | 722 | On fire | >120 | Safety | Safety |
As can be known from the results of Table 1: in positive pole, add LiNi
1/3Co
1/3Mn
1/3O
2Amount is when being not less than 20wt%, and the highest outside wall temperature surpasses 70 ℃ during the overcharging of the battery A1-A4 that the both positive and negative polarity weight ratio is fashionable, and security performance is guaranteed.And thermal runaway phenomenon (B1) even (B2) on fire appear during the over-charging of battery of comparative example, the overcharging resisting performance fails to meet the demands.
Claims (7)
1. safety lithium ion cell, comprise positive pole, negative pole, barrier film and nonaqueous electrolytic solution, anodal and negative pole constitutes by metal forming collector and the active material coating that contains that is coated in its surface, and it is characterized in that: anodal coating comprises the nickel cobaltous manganese lithium oxide active material of layer structure; The negative pole coating comprises one or both active materials of carbon fiber and spherical graphite, flaky graphite, and wherein the weight content of carbon fiber is 1-5%.
2. safety lithium ion cell according to claim 1 is characterized in that: anodal coating comprises the cobalt-lithium oxide of layer structure and the nickel cobaltous manganese lithium oxide active material of layer structure.
3. safety lithium ion cell according to claim 1 is characterized in that: the weight content of active material cobalt nickel oxide manganses lithium is not less than 20% in the anodal coating.
4. safety lithium ion cell according to claim 1 is characterized in that: positive electrode active materials weight is 1.5-2.2 times of negative active core-shell material coating weight.
5. safety lithium ion cell according to claim 4 is characterized in that: positive electrode active materials weight is 1.75-2 times of negative active core-shell material coating weight.
6. safety lithium ion cell according to claim 1 is characterized in that: the negative active core-shell material carbon fiber is a carbon nano-fiber.
7. a kind of safety lithium ion cell according to claim 1 is characterized in that: being shaped as of battery is cylindrical, Long Circle, square or button shaped.
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| Application Number | Priority Date | Filing Date | Title |
|---|---|---|---|
| CNB2005101223633A CN100466364C (en) | 2005-12-15 | 2005-12-15 | Safety lithium-ion battery |
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| Application Number | Priority Date | Filing Date | Title |
|---|---|---|---|
| CNB2005101223633A CN100466364C (en) | 2005-12-15 | 2005-12-15 | Safety lithium-ion battery |
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| Publication Number | Publication Date |
|---|---|
| CN1983705A CN1983705A (en) | 2007-06-20 |
| CN100466364C true CN100466364C (en) | 2009-03-04 |
Family
ID=38166044
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| CNB2005101223633A Active CN100466364C (en) | 2005-12-15 | 2005-12-15 | Safety lithium-ion battery |
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Families Citing this family (5)
| Publication number | Priority date | Publication date | Assignee | Title |
|---|---|---|---|---|
| JP5934089B2 (en) * | 2010-03-04 | 2016-06-15 | Ｊｘ金属株式会社 | Positive electrode active material for lithium ion battery, positive electrode for lithium ion battery, and lithium ion battery |
| CN101841063A (en) * | 2010-05-25 | 2010-09-22 | 江苏天鹏电源有限公司 | Ultra-high multiplying power lithium ion battery |
| CN102508186B (en) * | 2011-11-01 | 2014-04-02 | 天津力神电池股份有限公司 | Storage device for cylindrical lithium ion cells |
| CN102751485B (en) * | 2012-07-17 | 2015-09-16 | 中国电子科技集团公司第十八研究所 | The preparation method of composite anode material for lithium ion battery |
| CN110350239A (en) * | 2019-07-08 | 2019-10-18 | 无锡市明杨新能源有限公司 | High magnification lithium ion battery with high energy density |
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|---|---|---|---|---|
| JPH11176442A (en) * | 1997-12-16 | 1999-07-02 | Matsushita Electric Ind Co Ltd | Nonaqueous electrolyte secondary battery |
| CN1418174A (en) * | 2000-11-16 | 2003-05-14 | 日立马库塞鲁株式会社 | Lithium containing composite oxide and monaqueous secondary ceil using the same and method for manufacturing the same |
| CN1472832A (en) * | 2002-07-08 | 2004-02-04 | 松下电器产业株式会社 | Cathode and lithium ion secondary battery therewith |
| CN1670991A (en) * | 2004-03-16 | 2005-09-21 | 中国科学院金属研究所 | A modified lithium-ion battery cathode material, cathode and battery |
| WO2005093891A1 (en) * | 2004-03-29 | 2005-10-06 | Sharp Kabushiki Kaisha | Lithium ion secondary cell |
-
2005
- 2005-12-15 CN CNB2005101223633A patent/CN100466364C/en active Active
Patent Citations (5)
| Publication number | Priority date | Publication date | Assignee | Title |
|---|---|---|---|---|
| JPH11176442A (en) * | 1997-12-16 | 1999-07-02 | Matsushita Electric Ind Co Ltd | Nonaqueous electrolyte secondary battery |
| CN1418174A (en) * | 2000-11-16 | 2003-05-14 | 日立马库塞鲁株式会社 | Lithium containing composite oxide and monaqueous secondary ceil using the same and method for manufacturing the same |
| CN1472832A (en) * | 2002-07-08 | 2004-02-04 | 松下电器产业株式会社 | Cathode and lithium ion secondary battery therewith |
| CN1670991A (en) * | 2004-03-16 | 2005-09-21 | 中国科学院金属研究所 | A modified lithium-ion battery cathode material, cathode and battery |
| WO2005093891A1 (en) * | 2004-03-29 | 2005-10-06 | Sharp Kabushiki Kaisha | Lithium ion secondary cell |
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| Publication number | Publication date |
|---|---|
| CN1983705A (en) | 2007-06-20 |
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