CN103178226A - Membrane and preparation method and application thereof - Google Patents
Membrane and preparation method and application thereof Download PDFInfo
- Publication number
- CN103178226A CN103178226A CN2011104351499A CN201110435149A CN103178226A CN 103178226 A CN103178226 A CN 103178226A CN 2011104351499 A CN2011104351499 A CN 2011104351499A CN 201110435149 A CN201110435149 A CN 201110435149A CN 103178226 A CN103178226 A CN 103178226A
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- China
- Prior art keywords
- barrier film
- lithium
- particle
- adhesive
- membrane
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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 discloses a membrane and a preparation method thereof as well as a combined electrode couple and a high voltage battery prepared by the membrane, belonging to the technical field of lithium ion batteries. The membrane provided by the invention does not have holes or is provided with few holes, and is formed by soluble salt particles, electronic nonconducting inorganic material particles and a polymer adhesive, wherein the volume ratio of the soluble salt particle is 20-90%, the percentage by volume of the polymer adhesive in the membrane is 5-70%, and the percent by volume of the electronic nonconducting inorganic material particle in the membrane is 5-10%. An anode mixture comprising an anode active material, a conductive agent and an adhesive is coated on one surface of the membrane, and a cathode mixture comprising a cathode active material, the conductive agent and the adhesive is coated on the other surface of the membrane, so that a combined electrode couple is formed, and a high voltage battery is manufactured by the combined electrode couple. The dynamic consistency and the safety of the high voltage battery can be improved in use process.
Description
Technical field
The invention belongs to technical field of lithium ion, the combination electrode that relates in particular to a kind of barrier film and utilize the preparation of this barrier film to and high-voltage battery.
Background technology
Now, for protection of the environment, the urgent discharge capacity that makes to reduce carbon dioxide of wishing by new forms of energy, with regard to automobile industry, expectation is by the discharging that makes to reduce carbon dioxide of hybrid vehicle, electric automobile etc.Therefore, furtherd investigate the exploitation that is used for electric motor driven secondary cell.Due to lithium ion battery have high-energy-density, operating voltage high, have extended cycle life, the advantages such as self discharge is low, memory-less effect are used as Prospect of EVS Powered with Batteries and receive much concern.It is the better method that solves Prospect of EVS Powered with Batteries fail safe and consistency problem that inner stack series connection electrode prepares high-voltage lithium ion batteries.
The right proposition of combination electrode is to solve the composite current collector that exists in inner stack series connection high-voltage battery compressing tablet process in case crushed and crackle occurs, the ideal scheme that will be short-circuited between the adjacent cell of high-voltage lithium ion batteries inside.But, usually combination electrode centering, electrode active material directly being coated on porous septum, electrode active material is easy to enter porous septum and stops up the duct, reduces the porosity of barrier film, increases the internal resistance of cell; Simultaneously, more seriously might cause positive active material directly to contact with negative electrode active material, make battery generation internal short-circuit.
Summary of the invention
The possibility that occurs for reducing the problems referred to above the invention provides a kind of barrier film that contains solubility lithium salts particle, this diaphragm application in combination electrode to the making of high-voltage battery.
The present invention is by the following technical solutions:
A kind of barrier film provided by the invention, this barrier film are atresia or the few hole barrier films that is made of solubility lithium salts particle, the nonconducting inorganic material particle of electronics and polymer adhesive.Wherein, the percent by volume of solubility lithium salts particle in barrier film is 20～90%; The percent by volume of polymer adhesive in barrier film is 5～70%; The nonconducting inorganic material particle of electronics shared percent by volume in barrier film is 5～10%.The thickness of described barrier film greater than 5 microns less than 200 microns.
Combination electrode need to be 60～100 ℃ of dryings to electrode active material in preparation process, therefore require the solubility lithium salts particle breakdown temperature that contains in barrier film 〉=60 ℃, due to LiPF
6Just begin to decompose at 30 ℃ of temperature, therefore be not suitable for this barrier film.The solubility lithium salts of described decomposition temperature 〉=60 ℃ comprises LiB (C
2O
4)
2(302 ℃ of decomposition temperatures), LiBF
2(C
2O
4) (240 ℃ of decomposition temperatures), LiB (OCOCF
3)
4(decomposition temperature＞100 ℃), LiC (CF
3SO
2)
3(340 ℃ of decomposition temperatures), LiN (CF
3SO
2)
2(decomposition temperature＞360 ℃), LiClO
4One or more mixtures in (decomposition temperature＞100 ℃).
The nonconducting inorganic material particle of described electronics comprises MgO, SiO
2, Al
2O
3And TiO
2One or more in material, the average grain diameter of described inorganic material particle are 30～3000 nanometers.
Described polymer adhesive can be the lithium ion conducting material, also can be the lithium ion electrically non-conductive material, comprise one or more mixtures of Kynoar, Kynoar hexafluoropropylene, polymethyl methacrylate, polyacrylonitrile, sodium carboxymethylcellulose, butadiene-styrene rubber and all kinds of synthesizing polymeric materials.
The preparation method that described combination electrode is right:
The preparation of a, barrier film: polymer adhesive is dissolved in forms solution in solvent, again solubility lithium salts particle and the nonconducting inorganic material particle of electronics are dispersed in solution, then coat mixture on glass substrate or water and cast from the polytetrafluoroethylene mould, oven dry makes barrier film.
B, the right preparation of combination electrode: positive electrode active materials, conductive agent, adhesive (are consisted of positive electrode active materials: conductive agent: adhesive=85～98%: 1～8%: 1～7%) be mixed in and obtain anode sizing agent in solvent by mass percentage, coat the one side of described barrier film, oven dry; Then, negative active core-shell material, conductive agent, adhesive (are consisted of negative active core-shell material: conductive agent: adhesive=90～98%: 1～3%: 1～7%) be mixed in and obtain cathode size in solvent by mass percentage, coat the another side of described barrier film, oven dry; Then in pressure is 6～20MPa scope after compressing tablet cutting make combination electrode pair, can be used for the making of high-voltage battery.Width is left greater than the uncoated white space of 2mm in the edge of described barrier film.Described solvent is selected one or more mixtures in 1-METHYLPYRROLIDONE, N,N-DMAA, oxolane, DMF or dimethyl sulfoxide (DMSO), deionized water, ethanol.
The high-voltage battery of the combination electrode that the present invention makes to making:
The preparation of a, electron conduction adhesive layer: adopt existing technique that conductive agent and adhesive are mixed in solvent, make slurry, the combination electrode right two sides that is coated in above-mentioned preparation forms thickness less than the electron conduction adhesive layer of 10 microns;
B, a plurality of two sided coatings are had an electron conduction adhesive layer combination electrode to alternately stack of composite current collector, make a block;
After c, above-mentioned block vacuumize drying, inject electrolyte, after encapsulation, the parcel shell forms high-voltage battery.
Electrolyte described in high-voltage battery contains organic aprotic solvent of solubility lithium salts particle in the described barrier film of solubilized, comprises one or more of propene carbonate (PC), ethylene carbonate (EC), methyl ethyl carbonate (EMC), glycol dimethyl ether (DME) and dimethyl carbonate (DMC).
Technical advantage of the present invention is embodied in:
Atresia or the few hole barrier film that contains solubility lithium salts particle provided by the invention can be avoided or reduce combination electrode and positive electrode active materials in preparation process and negative active core-shell material directly be contacted the possibility that forms internal short-circuit; Simultaneously, can avoid or reduce combination electrode to the blocked possibility in preparation process septation duct.Can realize the pore-creating of barrier film and can not introduce the impurity that affects battery performance in electrolyte by solubility lithium salts grain dissolution.
Utilization directly applies cathode mix and negative pole mixture and prepares the right method of combination electrode on barrier film, after can avoiding electrode active material is coated on composite current collector, compressing tablet causes the local damage of collector and the problem of asymmetric bending, thereby has avoided causing because of the collector breakage potential safety hazard of high-voltage battery internal short-circuit.
By the electron conduction adhesive layer, combination electrode pair and composite current collector are bonded as one, and adopt above-mentioned combination electrode to the preparation high-voltage battery, improved dynamic conformance and the fail safe of high-voltage battery use procedure.
Embodiment
Embodiment 1:
The preparation of barrier film: PVDF (Kynoar)/polymethyl methacrylate is dissolved in forms solution in NMP (1-METHYLPYRROLIDONE), then with LiB (C
2O
4)
2And SiO
2Uniform particles is scattered in and forms slurry in solution (by volume percentage consists of Kynoar and polymethyl methacrylate: LiB (C
2O
4)
2: SiO
2=35: 60: 5), this slurry is evenly coated the surface of glass substrate, coating thickness is controlled at 25～40um, 60～100 ℃ of oven dry, makes barrier film.
The preparation that combination electrode is right: PVDF adhesive, carbon black and modified lithium manganate (are consisted of adhesive: carbon black: LiMn2O4=8: 7: 85) be mixed in NMP (1-METHYLPYRROLIDONE), fully be mixed and made into anode sizing agent by mass percentage.This slurry is coated the one side of above-mentioned barrier film, 60～100 ℃ of oven dry; PVDF, lithium titanate and carbon black (are consisted of lithium titanate: carbon black: adhesive=90: 3: 7) be mixed in NMP by mass percentage, fully be mixed and made into cathode size, again this slurry is uniformly coated on the another side of above-mentioned barrier film, 60～100 ℃ of oven dry, compressing tablet in pressure is 6～20MPa scope, make combination electrode pair after cutting, be used for the making of high-voltage battery.
The preparation of electron conduction adhesive layer: carbon black and Kynoar are carbon black by weight percentage: Kynoar=be mixed in NMP at 7: 3, make slurry, be coated in the right two sides formation thickness of combination electrode less than the electron conduction adhesive layer of 10um.
The combination electrode that 10 two sided coatings is had an electron conduction adhesive layer to the alternately stack of 11 composite current collectors, make a block, after vacuumizing drying, exert pressure less than the pressure of 6MPa and inject 1mol/LLiPF in the upper and lower surface of block
6/ PC+EC+DMC electrolyte, then adopt dielectric adhesive with the bonding sealing in the edge of composite current collector and mutually insulated, and the surface of block anodal (the aluminium foil one side of composite current collector) is connected with positive pole ear, the surperficial negative pole of block (the Copper Foil one side of composite current collector) is connected with negative lug, wrap up shell after cleaning encapsulation, obtain the high-voltage battery that operating voltage is about 20V.
Embodiment 2:
Prepare high-voltage battery in the mode identical with embodiment 1, the polymer adhesive that just uses in the preparation process of barrier film is Kynoar-hexafluoropropylene and polymethyl methacrylate; Lithium salts is LiBF
2(C
2O
4).Electrolyte is 1mol/LLiPF in the high-voltage battery preparation process
6/ PC+EC+EMC.
Embodiment 3:
Prepare high-voltage battery in the mode identical with embodiment 1, the polymer adhesive that just uses in the preparation process of barrier film is polyacrylonitrile and polymethyl methacrylate; Lithium salts is LiC (CF
3SO
2)
3Inorganic material particle is Al
2O
3Electrolyte is 1mol/LLiPF in the high-voltage battery preparation process
6/ EC+DMC.
Embodiment 4:
Prepare high-voltage battery in the mode identical with embodiment 1, the polymer adhesive that just uses in the preparation process of barrier film is sodium carboxymethylcellulose and butadiene-styrene rubber, and solvent is deionized water; Lithium salts is LiB (OCOCF
3)
4
Embodiment 5:
Prepare high-voltage battery in the mode identical with embodiment 1, the lithium salts that just uses in the preparation process of barrier film is LiClO
4(anion has certain oxidizability, but the consumption in the present invention seldom, does not affect battery performance); Inorganic material particle is TiO
2
Embodiment 6:
Prepare high-voltage battery in the mode identical with embodiment 1, the lithium salts that just uses in the preparation of barrier film is LiN (CF
3SO
2)
2(collector is had certain corrosivity, but the consumption in the present invention seldom, do not affect battery performance); Inorganic material particle is MgO.Electrolyte is 1mol/LLiPF in the high-voltage battery preparation process
6/ EC+DMC.
The specific embodiment of the invention is not to limit the present invention.Any those of ordinary skill in the art, do not breaking away from technical solution of the present invention scope situation, all can utilize method and the technology contents of above-mentioned announcement to make many possible changes and modification to technical solution of the present invention, or be revised as the equivalent embodiment of equivalent variations.Therefore, every content that does not break away from technical solution of the present invention, all still belongs in the scope of technical solution of the present invention protection any simple modification made for any of the above embodiments, equivalent variations and modification according to technical spirit of the present invention.
Claims (10)
1. barrier film is characterized in that: this barrier film is atresia or the few hole barrier film that is made of solubility lithium salts particle, the nonconducting inorganic material particle of electronics and polymer adhesive, and wherein, the percent by volume of solubility lithium salts particle in barrier film is 20～90%; The percent by volume of polymer adhesive in barrier film is 5～70%; The nonconducting inorganic material particle of electronics shared percent by volume in barrier film is 5～10%.
2. barrier film as claimed in claim 1 is characterized in that: described solubility lithium salts is decomposition temperature greater than the lithium salts of 60 ℃, comprises LiB (C
2O
4)
2, LiBF
2(C
2O
4), LiB (OCOCF
3)
4, LiN (CF
3SO
2)
2, LiC (CF
3SO
2)
3, LiClO
4In one or more mixtures.
3. barrier film as claimed in claim 1, it is characterized in that: the nonconducting inorganic material particle of described electronics comprises MgO, SiO
2, Al
2O
3And TiO
2One or more in material, the average grain diameter of described inorganic material particle are 30～3000 nanometers.
4. barrier film as claimed in claim 1, it is characterized in that: described polymer adhesive comprises one or more mixtures of Kynoar, Kynoar-hexafluoropropylene, polymethyl methacrylate, polyacrylonitrile, sodium carboxymethylcellulose, butadiene-styrene rubber and all kinds of synthesizing polymeric materials.
5. barrier film as claimed in claim 1 is characterized in that: the thickness of described barrier film greater than 5 microns less than 200 microns.
6. the preparation method of barrier film as claimed in claim 1, its step comprises:
1) polymer adhesive is dissolved in forms solution in solvent, described solvent is selected 1-METHYLPYRROLIDONE, N, N-DMAA, oxolane, N, one or more mixtures in dinethylformamide or dimethyl sulfoxide (DMSO), deionized water, ethanol are dispersed in solubility lithium salts particle and the nonconducting inorganic material particle of electronics in polymer binder solution;
2) coat above-mentioned mixed solution on glass substrate or water and cast from the polytetrafluoroethylene mould, oven dry makes barrier film.
7. a combination electrode pair, it is characterized in that: comprise barrier film as claimed in claim 1, the coated on one side of described barrier film has the cathode mix that comprises positive electrode active materials, conductive agent and adhesive, the another side of described barrier film is coated with the negative pole mixture that comprises negative active core-shell material, conductive agent and adhesive, leaves width in the edge of above-mentioned barrier film greater than the uncoated white space of 2mm.
8. combination electrode as claimed in claim 7 pair is characterized in that: described positive electrode active materials is that the LiFePO 4 that contains lithium, doped lithium manganese oxide, lithium and cobalt oxides, Li, Ni, Mn oxide, lithium nickel cobalt oxides, lithium-nickel-manganese-cobalt oxide and other contain one or more mixtures of lithium metal oxide; Described negative active core-shell material is acieral, silicon-base alloy, kamash alloy, Li-Ti oxide that can reversible embedding lithium, one or more mixtures of material with carbon element; Described conductive agent is one or more mixtures in carbon black, carbon fiber, metallic particles.
9. high-voltage battery is characterized in that: adopt combination electrode as claimed in claim 7 pair, the above-mentioned combination electrode that a plurality of two sided coatings is had an electron conduction adhesive layer to composite current collector alternately stack make a block; After above-mentioned block vacuumizes drying, inject the electrolyte encapsulation, and be enclosed with shell.
10. high-voltage battery as claimed in claim 9, it is characterized in that: described electrolyte contains organic aprotic solvent of solubility lithium salts particle in the right barrier film of solubilized combination electrode, and this organic aprotic solvent comprises one or more of propene carbonate, ethylene carbonate, methyl ethyl carbonate, glycol dimethyl ether and dimethyl carbonate.
Priority Applications (1)
| Application Number | Priority Date | Filing Date | Title |
|---|---|---|---|
| CN2011104351499A CN103178226A (en) | 2011-12-22 | 2011-12-22 | Membrane and preparation method and application thereof |
Applications Claiming Priority (1)
| Application Number | Priority Date | Filing Date | Title |
|---|---|---|---|
| CN2011104351499A CN103178226A (en) | 2011-12-22 | 2011-12-22 | Membrane and preparation method and application thereof |
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|---|---|
| CN103178226A true CN103178226A (en) | 2013-06-26 |
Family
ID=48637950
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|---|---|---|---|
| CN2011104351499A Pending CN103178226A (en) | 2011-12-22 | 2011-12-22 | Membrane and preparation method and application thereof |
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Cited By (8)
| Publication number | Priority date | Publication date | Assignee | Title |
|---|---|---|---|---|
| CN105633326A (en) * | 2015-06-03 | 2016-06-01 | 北京星和众工设备技术股份有限公司 | Aromatic polyamide composite membrane |
| CN105679984A (en) * | 2016-03-29 | 2016-06-15 | 浙江地坤键新能源科技有限公司 | Non-porous separator and application thereof |
| CN105742560A (en) * | 2016-03-23 | 2016-07-06 | 合肥国轩高科动力能源有限公司 | Preparation method of lithium-ion battery membrane electrode |
| CN106544786A (en) * | 2016-11-08 | 2017-03-29 | 铜陵市启动电子制造有限责任公司 | A kind of titanium doped modified Static Spinning diaphragm of supercapacitor material of lanthanum lithium |
| JP2017073273A (en) * | 2015-10-07 | 2017-04-13 | トヨタ自動車株式会社 | Method for manufacturing nonaqueous electrolyte secondary battery |
| CN111987279A (en) * | 2020-08-28 | 2020-11-24 | 重庆金美新材料科技有限公司 | Lithium supplement diaphragm and preparation method thereof |
| CN117374515A (en) * | 2023-12-06 | 2024-01-09 | 天津力神电池股份有限公司 | Separator with lithium ion capacity compensation function, preparation method thereof and battery |
| CN117374515B (en) * | 2023-12-06 | 2024-04-19 | 天津力神电池股份有限公司 | Separator with lithium ion capacity compensation function, preparation method thereof and battery |
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| JP2010027553A (en) * | 2008-07-24 | 2010-02-04 | Hitachi Chem Co Ltd | Separator for electrochemical element and lithium-ion battery using the same |
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Cited By (16)
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|---|---|---|---|---|
| CN105633326B (en) * | 2015-06-03 | 2019-07-12 | 北京星和众工设备技术股份有限公司 | Aromatic polyamide composite diaphragm |
| CN105633326A (en) * | 2015-06-03 | 2016-06-01 | 北京星和众工设备技术股份有限公司 | Aromatic polyamide composite membrane |
| JP2017073273A (en) * | 2015-10-07 | 2017-04-13 | トヨタ自動車株式会社 | Method for manufacturing nonaqueous electrolyte secondary battery |
| CN105742560A (en) * | 2016-03-23 | 2016-07-06 | 合肥国轩高科动力能源有限公司 | Preparation method of lithium-ion battery membrane electrode |
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| CN105679984A (en) * | 2016-03-29 | 2016-06-15 | 浙江地坤键新能源科技有限公司 | Non-porous separator and application thereof |
| WO2017167195A1 (en) * | 2016-03-29 | 2017-10-05 | 浙江地坤键新能源科技有限公司 | Non-porous separator and use thereof |
| CN106544786A (en) * | 2016-11-08 | 2017-03-29 | 铜陵市启动电子制造有限责任公司 | A kind of titanium doped modified Static Spinning diaphragm of supercapacitor material of lanthanum lithium |
| CN111987279A (en) * | 2020-08-28 | 2020-11-24 | 重庆金美新材料科技有限公司 | Lithium supplement diaphragm and preparation method thereof |
| WO2022041929A1 (en) * | 2020-08-28 | 2022-03-03 | 重庆金美新材料科技有限公司 | Lithium replenishing diaphragm and preparation method for lithiumreplenishing diaphragm |
| JP2023505348A (en) * | 2020-08-28 | 2023-02-08 | 重慶金美新材料科技有限公司 | Lithium replenishment separator and method for manufacturing lithium replenishment separator |
| EP4089822A4 (en) * | 2020-08-28 | 2023-10-04 | Chongqing Jimat New Material Technology Co., Ltd. | Lithium replenishing diaphragm and preparation method for lithiumreplenishing diaphragm |
| JP7451706B2 (en) | 2020-08-28 | 2024-03-18 | 重慶金美新材料科技有限公司 | Lithium replenishment separator and method for manufacturing lithium replenishment separator |
| CN117374515A (en) * | 2023-12-06 | 2024-01-09 | 天津力神电池股份有限公司 | Separator with lithium ion capacity compensation function, preparation method thereof and battery |
| CN117374515B (en) * | 2023-12-06 | 2024-04-19 | 天津力神电池股份有限公司 | Separator with lithium ion capacity compensation function, preparation method thereof and battery |
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Application publication date: 20130626 |