WO2013070031A1 - 세퍼레이터 및 이를 구비한 전기화학소자 - Google Patents
세퍼레이터 및 이를 구비한 전기화학소자 Download PDFInfo
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- WO2013070031A1 WO2013070031A1 PCT/KR2012/009484 KR2012009484W WO2013070031A1 WO 2013070031 A1 WO2013070031 A1 WO 2013070031A1 KR 2012009484 W KR2012009484 W KR 2012009484W WO 2013070031 A1 WO2013070031 A1 WO 2013070031A1
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- H01M50/40—Separators; Membranes; Diaphragms; Spacing elements inside cells
- H01M50/46—Separators, membranes or diaphragms characterised by their combination with electrodes
- H01M50/461—Separators, membranes or diaphragms characterised by their combination with electrodes with adhesive layers between electrodes and separators
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- H01M50/40—Separators; Membranes; Diaphragms; Spacing elements inside cells
- H01M50/409—Separators, membranes or diaphragms characterised by the material
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- H01M10/058—Construction or manufacture
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- H01M10/00—Secondary cells; Manufacture thereof
- H01M10/42—Methods or arrangements for servicing or maintenance of secondary cells or secondary half-cells
- H01M10/4235—Safety or regulating additives or arrangements in electrodes, separators or electrolyte
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- H01M50/40—Separators; Membranes; Diaphragms; Spacing elements inside cells
- H01M50/409—Separators, membranes or diaphragms characterised by the material
- H01M50/411—Organic material
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- H01M50/40—Separators; Membranes; Diaphragms; Spacing elements inside cells
- H01M50/409—Separators, membranes or diaphragms characterised by the material
- H01M50/411—Organic material
- H01M50/414—Synthetic resins, e.g. thermoplastics or thermosetting resins
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- H01M50/40—Separators; Membranes; Diaphragms; Spacing elements inside cells
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- H01M50/431—Inorganic material
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- H01M50/443—Particulate material
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- H01M50/40—Separators; Membranes; Diaphragms; Spacing elements inside cells
- H01M50/409—Separators, membranes or diaphragms characterised by the material
- H01M50/449—Separators, membranes or diaphragms characterised by the material having a layered structure
- H01M50/451—Separators, membranes or diaphragms characterised by the material having a layered structure comprising layers of only organic material and layers containing inorganic material
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- H01M50/40—Separators; Membranes; Diaphragms; Spacing elements inside cells
- H01M50/409—Separators, membranes or diaphragms characterised by the material
- H01M50/449—Separators, membranes or diaphragms characterised by the material having a layered structure
- H01M50/457—Separators, membranes or diaphragms characterised by the material having a layered structure comprising three or more layers
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- H01M50/40—Separators; Membranes; Diaphragms; Spacing elements inside cells
- H01M50/489—Separators, membranes, diaphragms or spacing elements inside the cells, characterised by their physical properties, e.g. swelling degree, hydrophilicity or shut down properties
- H01M50/491—Porosity
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- H01M10/00—Secondary cells; Manufacture thereof
- H01M10/05—Accumulators with non-aqueous electrolyte
- H01M10/052—Li-accumulators
- H01M10/0525—Rocking-chair batteries, i.e. batteries with lithium insertion or intercalation in both electrodes; Lithium-ion batteries
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- H—ELECTRICITY
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- H01M50/40—Separators; Membranes; Diaphragms; Spacing elements inside cells
- H01M50/403—Manufacturing processes of separators, membranes or diaphragms
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- H—ELECTRICITY
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- H01M50/00—Constructional details or processes of manufacture of the non-active parts of electrochemical cells other than fuel cells, e.g. hybrid cells
- H01M50/40—Separators; Membranes; Diaphragms; Spacing elements inside cells
- H01M50/409—Separators, membranes or diaphragms characterised by the material
- H01M50/411—Organic material
- H01M50/414—Synthetic resins, e.g. thermoplastics or thermosetting resins
- H01M50/417—Polyolefins
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- H01M50/40—Separators; Membranes; Diaphragms; Spacing elements inside cells
- H01M50/409—Separators, membranes or diaphragms characterised by the material
- H01M50/44—Fibrous material
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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
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- Y02E—REDUCTION OF GREENHOUSE GAS [GHG] EMISSIONS, RELATED TO ENERGY GENERATION, TRANSMISSION OR DISTRIBUTION
- Y02E60/00—Enabling technologies; Technologies with a potential or indirect contribution to GHG emissions mitigation
- Y02E60/10—Energy storage using batteries
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- Y—GENERAL TAGGING OF NEW TECHNOLOGICAL DEVELOPMENTS; GENERAL TAGGING OF CROSS-SECTIONAL TECHNOLOGIES SPANNING OVER SEVERAL SECTIONS OF THE IPC; TECHNICAL SUBJECTS COVERED BY FORMER USPC CROSS-REFERENCE ART COLLECTIONS [XRACs] AND DIGESTS
- Y02—TECHNOLOGIES OR APPLICATIONS FOR MITIGATION OR ADAPTATION AGAINST CLIMATE CHANGE
- Y02P—CLIMATE CHANGE MITIGATION TECHNOLOGIES IN THE PRODUCTION OR PROCESSING OF GOODS
- Y02P70/00—Climate change mitigation technologies in the production process for final industrial or consumer products
- Y02P70/50—Manufacturing or production processes characterised by the final manufactured product
Definitions
- the present invention relates to a separator of an electrochemical device such as a lithium secondary battery and an electrochemical device having the same, and more particularly, a separator having a second porous coating layer, which is a binder layer using a first porous coating layer and a non-solvent, including an organic-inorganic mixture. And it relates to an electrochemical device having the same.
- lithium secondary batteries developed in the early 1990s have a higher operating voltage and greater energy density than conventional batteries such as Ni-MH, Ni-Cd, and sulfuric acid-lead batteries that use an aqueous electrolyte solution. I am in the spotlight.
- lithium ion batteries have safety problems such as ignition and explosion due to the use of the organic electrolyte, and are difficult to manufacture.
- the lithium ion polymer battery has been considered as one of the next generation batteries by improving the weakness of the lithium ion battery, but the capacity of the battery is still relatively low compared to the lithium ion battery, and the discharge capacity is improved due to insufficient discharge capacity at low temperatures. This is urgently needed.
- electrochemical devices are produced by many companies, but their safety characteristics show different aspects. It is very important to evaluate the safety and secure the safety of these electrochemical devices. The most important consideration is that the electrochemical device should not cause injury to the user in the event of a malfunction. For this purpose, safety standards strictly regulate the ignition and smoke in the electrochemical device. In the safety characteristics of the electrochemical device, there is a high possibility that an explosion occurs when the electrochemical device is overheated to cause thermal runaway or the separator penetrates. In particular, polyolefin-based porous substrates commonly used as separators of electrochemical devices exhibit extreme heat shrinkage behavior at temperatures of 100 degrees or more due to material characteristics and manufacturing process characteristics including stretching, and thus, a short circuit between the anode and the cathode. There is a problem that causes.
- a separator having an organic-inorganic porous coating layer formed by coating a mixture of excess inorganic particles and a binder polymer on at least one surface of a porous substrate having a plurality of pores In order to solve such a safety problem of the electrochemical device, a separator having an organic-inorganic porous coating layer formed by coating a mixture of excess inorganic particles and a binder polymer on at least one surface of a porous substrate having a plurality of pores.
- the thickness of the separator becomes too thick, so that the capacity of the electrochemical device is reduced and the resistance is increased, and only one surface of the porous substrate is organic-.
- the adhesive strength of the other surface is lowered.
- the problem to be solved by the present invention is to provide a separator having an excellent thermal stability while having an excellent organic-inorganic porous coating layer and excellent adhesion.
- a porous substrate In order to solve the above problems, a porous substrate; A first porous coating layer formed on one surface of the porous substrate and made of a mixture of inorganic particles and a first binder polymer; And a second porous coating layer formed on the other surface of the porous substrate and including a drying result of a mixture of a solvent, a non-solvent, and a second binder polymer.
- the second porous coating layer may be formed only on a portion of the other surface of the porous substrate.
- the separator of the present invention is formed on the surface of the first porous coating layer, it may further include an electrode adhesive layer containing a third binder polymer.
- the kind of the porous substrate is not particularly limited, but a polyolefin-based porous substrate may be used, and such polyolefin-based porous substrate is preferably polyethylene, polypropylene, polybutylene, polypentene, or the like.
- the solvent is not particularly limited in kind, but acetone, tetrahydrofuran, methylene chloride, chloroform, dimethylformamide, N-methyl-2-pyrrolidone, cyclohexane and the like can be used.
- the non-solvent is not particularly limited in kind, but methanol, ethanol, isopropyl alcohol, water and the like can be used.
- the weight ratio of the solvent and the non-solvent is preferably 50:50 ⁇ 99: 1.
- inorganic particles of the present invention inorganic particles having a dielectric constant of 5 or more, inorganic particles having lithium ion transfer ability, mixtures thereof, and the like can be used.
- the inorganic particles having a dielectric constant of 5 or more are not particularly limited in kind, but BaTiO 3 , Pb (Zr x , Ti 1-x ) O 3 (PZT, 0 ⁇ x ⁇ 1), Pb 1-x La x Zr 1-y Ti y O 3 (PLZT, 0 ⁇ x ⁇ 1, 0 ⁇ y ⁇ 1), (1-x) Pb (Mg 1/3 Nb 2/3 ) O 3 -xPbTiO 3 (PMN-PT, 0 ⁇ x ⁇ 1), hafnia (HfO 2 ), SrTiO 3 , SnO 2 , CeO 2 , MgO, NiO, CaO, ZnO, ZrO 2 , SiO 2 , Y 2 O 3 , Al 2 O 3 , SiC and TiO 2 to use any of the inorganic particles or a mixture of two or more of them are preferred, such as selected from the group consisting of.
- the inorganic particles having the lithium ion transport ability include lithium phosphate (Li 3 PO 4 ), lithium titanium phosphate (Li x Ti y (PO 4 ) 3 , 0 ⁇ x ⁇ 2, 0 ⁇ y ⁇ 3), lithium Aluminum titanium phosphate (Li x Al y Ti z (PO 4 ) 3 , 0 ⁇ x ⁇ 2, 0 ⁇ y ⁇ 1, 0 ⁇ z ⁇ 3), (LiAlTiP) x O y series glass (0 ⁇ x ⁇ 4, 0 ⁇ y ⁇ 13), lithium lanthanum titanate (Li x La y TiO 3 , 0 ⁇ x ⁇ 2, 0 ⁇ y ⁇ 3), lithium germanium thiophosphate (Li x Ge y P z S w , 0 ⁇ x ⁇ 4, 0 ⁇ y ⁇ 1, 0 ⁇ z ⁇ 1, 0 ⁇ w ⁇ 5), Lithium Nitride (Li x x
- the separator of the present invention can be applied to both separators of electrochemical devices such as lithium secondary electrons and supercapacitor devices.
- the separator of the present invention has an organic-inorganic porous coating layer formed on one surface, and thus has excellent thermal safety.
- a porous coating layer made of a dry binder thin film is formed by mixing a binder polymer with a non-solvent and having excellent adhesion. Reducing the thickness of the separator can reduce the resistance and improve the capacity of the electrochemical device.
- FIG. 1 is a cross-sectional view of a separator according to a preferred embodiment of the present invention.
- Figure 2 is a SEM photograph of the surface of the porous coating layer of the binder polymer thin film according to an embodiment of the present invention.
- FIG. 3 is a SEM photograph of a cross section of a separator according to a preferred embodiment of the present invention.
- FIG. 1 schematically shows an embodiment of a separator according to the present invention.
- the configuration described in the embodiments and drawings described below are only the most preferred embodiment of the present invention and do not represent all of the technical idea of the present invention, which can be replaced at the time of the present application It should be understood that there may be various equivalents and variations.
- the separator 100 of the present invention is a porous substrate 10; A first porous coating layer 20 formed on one surface of the porous substrate and made of a mixture of inorganic particles and a first binder polymer; And a second porous coating layer 30 formed on the other surface of the porous substrate and dried after applying the mixture of the non-solvent and the second binder polymer.
- the porous substrate 10 may be used as long as it is a planar porous substrate commonly used in electrochemical devices such as porous membranes or nonwoven fabrics formed of various polymers.
- a polyolefin-based porous membrane or a nonwoven fabric made of polyethylene terephthalate fiber which is used as an electrochemical device, in particular, a separator of a lithium secondary battery, may be used.
- the polyolefin-based porous membrane is a polyolefin-based polymer such as polyethylene, polypropylene, polybutylene, polypentene, such as high density polyethylene, linear low density polyethylene, low density polyethylene, ultra high molecular weight polyethylene, or a mixture thereof.
- the polymer may be formed, and the nonwoven fabric may also be made of a polyolefin-based polymer or a fiber using a polymer having higher heat resistance.
- the thickness of the porous substrate is not particularly limited, but is preferably 1 to 100 ⁇ m, more preferably 5 to 50 ⁇ m, and the pore size and pore present in the porous substrate are also not particularly limited, but 0.01 to 50 ⁇ m and 10, respectively. It is preferably from 95%.
- One surface of the porous substrate 10 of the present invention is formed with a first porous coating layer 20 made of a mixture of inorganic particles and a first binder polymer.
- the first porous coating layer 20 is formed by applying a slurry containing a mixture of inorganic particles and the first binder polymer to one surface of the porous substrate 10 and then drying.
- the first porous coating layer 20 is attached to each other (that is, the binder polymer is connected and fixed between the inorganic particles) so that the first binder polymer can maintain the state in which the inorganic particles are bound to each other, and the first porous coating layer ( 20) maintains the binding state with the porous substrate 10 by the binder polymer, and has an adhesive force with the electrode active material of the electrode.
- the inorganic particles of the first porous coating layer 20 are present in the closest packed structure in a substantially contact state with each other, and the interstitial volume generated when the inorganic particles are in contact with each other is formed in the first porous coating layer 20. It becomes a pore.
- the separator 100 on which the first porous coating layer 20 is formed has excellent heat resistance and thus stability is increased, but electrical resistance may increase due to the binder polymer.
- the separator 100 of the present invention minimizes the electrical resistance due to the binder polymer by having the first porous coating layer 20 on only one surface of the porous substrate.
- the thickness of the separator is thick, which hinders the capacity improvement of the electrochemical device.
- the first porous coating layer 20 may be formed only on one surface of 10 to contribute to the capacity improvement of the electrochemical device.
- the other surface of the porous substrate on which the first porous coating layer 20 is not formed may decrease adhesiveness with the electrode, and the separator 100 of the present invention may have a second porous surface made of a binder polymer on the other surface of the porous substrate.
- the coating layer 30 may be provided to provide excellent adhesion with the electrode.
- the binder polymer when the binder polymer is coated and coated on the porous substrate by a general method, the binder polymer may penetrate into the pores of the porous substrate to decrease the porosity of the porous substrate, thereby increasing resistance. Therefore, the separator 100 of the present invention minimizes the penetration of the second binder polymer into the pores of the porous substrate by accelerating the phase separation rate between the second binder polymer and the non-solvent by using a non-solvent.
- the second porous coating layer 30 may be formed only on a portion of the surface of the porous substrate to minimize the decrease in porosity and increase in resistance of the porous substrate.
- the separator of the present invention is formed on the surface of the first porous coating layer, it may further include an electrode adhesive layer containing a third binder polymer.
- the inorganic particles are not particularly limited as long as they are electrochemically stable. That is, the inorganic particles that can be used in the present invention are not particularly limited as long as the oxidation and / or reduction reactions do not occur in the operating voltage range (for example, 0 to 5 V on the basis of Li / Li + ) of the applied electrochemical device.
- the ionic conductivity of the electrolyte may be improved by contributing to an increase in the dissociation degree of the electrolyte salt, such as lithium salt, in the liquid electrolyte.
- the inorganic particles preferably include high dielectric constant inorganic particles having a dielectric constant of 5 or more, preferably 10 or more.
- Non-limiting examples of inorganic particles having a dielectric constant greater than 5 include BaTiO 3 , Pb (Zr x , Ti 1-x ) O 3 (PZT, 0 ⁇ x ⁇ 1), Pb 1-x La x Zr 1-y Ti y O 3 (PLZT, 0 ⁇ x ⁇ 1, 0 ⁇ y ⁇ 1), (1-x) Pb (Mg 1/3 Nb 2/3 ) O 3 -xPbTiO 3 (PMN-PT, 0 ⁇ x ⁇ 1), Hafnia (HfO 2 ), SrTiO 3 , SnO 2 , CeO 2 , MgO, NiO, CaO, ZnO, ZrO 2 , Y 2 O 3 , Al 2 O 3 , TiO 2, SiC Or mixtures thereof.
- the inorganic particles may be inorganic particles having lithium ion transfer capability, that is, inorganic particles containing lithium elements but having a function of transferring lithium ions without storing lithium.
- inorganic particles having a lithium ion transfer capacity include lithium phosphate (Li 3 PO 4 ), lithium titanium phosphate (Li x Ti y (PO 4 ) 3 , 0 ⁇ x ⁇ 2, 0 ⁇ y ⁇ 3), Lithium aluminum titanium phosphate (Li x Al y Ti z (PO 4 ) 3 , 0 ⁇ x ⁇ 2, 0 ⁇ y ⁇ 1, 0 ⁇ z ⁇ 3), 14Li 2 O-9Al 2 O 3 -38TiO 2 -39P 2 (LiAlTiP) x O y series glass such as O 5 (0 ⁇ x ⁇ 4, 0 ⁇ y ⁇ 13), lithium lanthanum titanate (Li x La y TiO 3 , 0 ⁇ x ), lithium lanthan
- the average particle diameter of the inorganic particles is not particularly limited, but for forming a coating layer of uniform thickness and proper porosity, it is preferably in the range of 0.001 to 10 ⁇ m. When the thickness is less than 0.001 ⁇ m, the dispersibility may be decreased, and when the thickness is more than 10 ⁇ m, the thickness of the coating layer formed may be increased.
- the binder polymer it is preferable to use a polymer having a glass transition temperature (T g ) of -200 to 200 ° C, because it can improve mechanical properties such as flexibility and elasticity of the finally formed coating layer. .
- T g glass transition temperature
- the binder polymer does not necessarily have an ion conducting ability, but when a polymer having an ion conducting ability is used, the performance of the electrochemical device may be further improved. Therefore, the binder polymer is preferably as high as possible dielectric constant. In fact, since the dissociation degree of the salt in the electrolyte depends on the dielectric constant of the solvent of the electrolyte, the higher the dielectric constant of the binder polymer, the higher the dissociation of the salt in the electrolyte.
- the binder polymer may have a feature that can exhibit a high degree of swelling of the electrolyte by gelling upon impregnation of the liquid electrolyte. Accordingly, it is preferred to use polymers having a solubility index of 15 to 45 MPa 1/2 , more preferred solubility indices in the range of 15 to 25 MPa 1/2 and 30 to 45 MPa 1/2 . Therefore, it is preferable to use hydrophilic polymers having more polar groups than hydrophobic polymers such as polyolefins. This is because when the solubility index is less than 15 MPa 1/2 and more than 45 MPa 1/2 , it is difficult to be swelled by a conventional battery liquid electrolyte.
- binder polymers include polyvinylidene fluoride-co-hexafluoropropylene, polyvinylidene fluoride-co-trichloroethylene, polymethylmethacryl Polymethylmethacrylate, polybutylacrylate, polyacrylonitrile, polyvinylpyrrolidone, polyvinylacetate, polyvinyl alcohol, ethylene vinyl acetate copolymer (polyethylene-co-vinyl acetate), polyethylene oxide, polyarylate, cellulose acetate, cellulose acetate butyrate, cellulose acetate propionate , Cyanoethylfuran (cyanoeth ylpullulan, cyanoethylpolyvinylalcohol, cyanoethylcellulose, cyanoethylsucrose, pullulan, carboxyl methyl cellulose and molecular weight 10,000 g / mol The following low molecular weight compounds etc. are mentioned.
- the weight ratio of the inorganic particles and the binder polymer is preferably in the range of 50:50 to 99: 1, more preferably 70:30 to 95: 5.
- the content ratio of the inorganic particles to the binder polymer is less than 50:50, the pore size and porosity of the coating layer formed by increasing the content of the polymer may be reduced.
- the content of the inorganic particles exceeds 99 parts by weight, since the binder polymer content is small, the peeling resistance of the coating layer formed may be weakened.
- the first porous coating layer 20 is a slurry of a mixture of inorganic particles and the first binder polymer is prepared by using a solvent to be applied to one surface of the porous substrate and dried, wherein the solvent is to be used as a binder It is preferable that the polymer and the solubility index are similar, and the boiling point is low. This is to facilitate uniform mixing and subsequent solvent removal.
- solvents that can be used include acetone, tetrahydrofuran, methylene chloride, chloroform, dimethylformamide, N-methyl-2-pyrrolidone ( N-methyl-2-pyrrolidone, NMP) and cyclohexane, or a mixture thereof.
- non-solvent methanol, ethanol, isopropyl alcohol, water and the like can be used, and a suitable non-solvent can be selected according to the type of the second binder used.
- the weight ratio of the solvent and the non-solvent is mixed and used in a range of 50:50 to 99: 1, and applied to the other surface of the porous substrate and dried to form a second porous coating layer 30. If the content of the non-solvent is less than 50% by weight, there is a problem in producing a binder solution due to gelation, and when the content of the non-solvent is less than 1% by weight, it is difficult to expect the effect of using the non-solvent.
- the thickness of the second porous coating layer is preferably 0.5 ⁇ 5 ⁇ m.
- Such a separator having a functional multilayer of the present invention can be interposed between the positive electrode and the negative electrode as in the conventional separator, in which case the first porous coating layer made of inorganic material prevents the short circuit of the positive electrode and the negative electrode even when overheated. .
- the electrochemical device of the present invention includes all devices that undergo an electrochemical reaction, and specific examples include capacitors such as all kinds of primary, secondary cells, fuel cells, solar cells, or supercapacitor elements.
- capacitors such as all kinds of primary, secondary cells, fuel cells, solar cells, or supercapacitor elements.
- a lithium secondary battery including a lithium metal secondary battery, a lithium ion secondary battery, a lithium polymer secondary battery or a lithium ion polymer secondary battery among the secondary batteries is preferable.
- an electrolyte in which a salt having a structure such as A + B ⁇ is dissolved in an organic solvent may be selectively used.
- a + is Li +, Na +, and contains an alkali metal cation or ion consisting of a combination thereof, such as K +
- B - is PF 6 -, BF 4 -, Cl -, Br -, I -, ClO 4 -, AsF 6 -, CH 3 CO 2 -, CF 3 SO 3 -, N (CF 3 SO 2) 2 -, C (CF 2 SO 2) 3 - and include such anions or an ion composed of a combination of do.
- Organic solvents include propylene carbonate (PC), ethylene carbonate (EC), diethyl carbonate (DEC), dimethyl carbonate (DMC), dipropyl carbonate (DPC), dimethyl sulfoxide, acetonitrile, dimethoxyethane, diethoxyethane , Tetrahydrofuran, N-methyl-2-pyrrolidone (NMP), ethylmethylcarbonate (EMC), gamma butyrolactone (g-butyrolactone) or mixtures thereof, but is not limited thereto. no.
- PC propylene carbonate
- EC ethylene carbonate
- DEC diethyl carbonate
- DMC dimethyl carbonate
- DPC dipropyl carbonate
- dimethyl sulfoxide acetonitrile, dimethoxyethane, diethoxyethane , Tetrahydrofuran, N-methyl-2-pyrrolidone (NMP), ethylmethylcarbonate (EMC), gam
- the injection of the electrolyte may be performed at an appropriate step in the battery manufacturing process, depending on the manufacturing process and the required physical properties of the final product. That is, it may be applied before the battery assembly or at the end of battery assembly.
- the separator of the present invention may be interposed between the positive electrode and the negative electrode of the secondary battery, and may be interposed between adjacent cells or electrodes when a plurality of cells or electrodes are assembled to form an electrode assembly.
- the electrode assembly may have various structures such as a simple stack type, a jelly roll, a stack type, and the like.
- the electrode assembly may be prepared by interposing the separator of the present invention between the positive electrode and the negative electrode to which the active material is applied, and winding the positive electrode / separation membrane / cathode continuously.
- the electrode assembly may be manufactured to have a zig-zag overlapping structure by bending the anode / separator / cathode at regular intervals.
- the electrode assembly to be wound or bent may include a plurality of electrodes and a separator that are alternately stacked to increase capacity.
- the electrode assembly may be prepared by stacking the anode / separator / cathode or the cathode / separator / anode in a repeating unit.
- the separator uses the separator of the present invention.
- a plurality of unit cells having a structure of a full cell or a bicell may be prepared by gathering a folding film.
- the folding film may use a general insulating film or the separator of the present invention.
- the full cell structure includes at least one cell structure having a separator interposed between electrodes having different polarities, but a cell structure having different polarities of electrodes located at the outermost sides. Examples of the full cell structure include an anode / separator / cathode or an anode / separator / cathode / separator / anode / separator / cathode.
- the bicell structure refers to a cell structure including at least one cell structure having a separator interposed between electrodes having different polarities, but having the same polarity as the electrode located at the outermost side.
- Examples of the bicell structure include an anode / separator / cathode / separator / anode or a cathode / separator / anode / separator / cathode.
- an electrode assembly may be manufactured by arranging a plurality of unit cells on one surface of the folding film extending in a longitudinal direction at predetermined intervals and winding the folding film in one direction together with the arranged unit cells.
- the electrode assembly thus manufactured has a structure in which unit cells are inserted between the wound folding films.
- an electrode assembly may be manufactured by arranging a plurality of unit cells on both sides of the folding film extending in a longitudinal direction at predetermined intervals and winding the folding film in one direction together with the arranged unit cells.
- the electrode assembly thus manufactured has a structure in which unit cells are inserted between the wound folding films.
- the arrangement interval of the unit cells and the polarity of the electrode positioned at the outermost portion of each unit cell are selected such that the polarities of the electrodes of the upper cell and the electrodes of the lower cell in contact with the folding film are reversed.
- an electrode disposed at an outermost interval of each unit cell and an arrangement interval of the unit cells so as to form an electrode assembly structure such as an anode / separator / cathode / folding film / anode / separator / cathode / folding film / anode.
- the polarity of can be selected.
- a plurality of unit cells are arranged on one surface of the folding film extending in a longitudinal direction at predetermined intervals, and the folding film is bent in a zigzag shape with the arranged unit cells, and the folded film is interposed therebetween.
- the electrode assembly may be manufactured in a structure in which the unit cells are arranged.
- the electrode assembly manufactured as described above has a structure in which unit cells are inserted between folded and stacked folding films.
- the folding film is bent in a zigzag shape with the arranged unit cells, and unit cells are formed between the folded folding films.
- the electrode assembly may be manufactured with the disposed structure.
- the electrode assembly manufactured as described above has a structure in which unit cells are inserted between folded and stacked folding films.
- the arrangement interval of the unit cells and the polarity of the electrode positioned at the outermost portion of each unit cell are selected such that the polarities of the electrodes of the upper cell and the electrodes of the lower cell in contact with the folding film are reversed.
- an electrode disposed at an outermost interval of each unit cell and an arrangement interval of the unit cells so as to form an electrode assembly structure such as an anode / separator / cathode / folding film / anode / separator / cathode / folding film / anode.
- the polarity of can be selected.
- a method of collecting electrodes using a folding film may be various.
- an electrode assembly may be manufactured by alternately arranging a cathode, an anode, a cathode, an anode, etc. on one surface of the folding film, and winding an electrode disposed together with the folding film in one direction.
- the electrode assembly thus manufactured has a structure in which electrodes are inserted between the wound folding films.
- the electrode assembly may be manufactured by arranging a plurality of electrodes on both sides of the folding film extending in the longitudinal direction at predetermined intervals and winding the folding film in one direction together with the arranged electrodes.
- the electrode assembly thus manufactured has a structure in which electrodes are inserted between the wound folding films.
- the spacing of the electrodes and the polarity of the electrodes are selected such that the polarities of the upper and lower electrodes in contact with the folding film are reversed.
- the arrangement interval of the electrodes and the polarity of each electrode may be selected to form the structure of the electrode assembly such as the anode / folding film / cathode / folding film / anode.
- an electrode, an anode, a cathode, an anode, etc. are alternately arranged on one side of the folding film, the electrodes arranged together with the folding film in one direction are bent, and the electrodes are disposed between the folded folding films.
- the electrode assembly can be manufactured with the structure.
- the electrode assembly thus manufactured has a structure in which the electrodes are inserted between the folded and stacked folding films.
- the folding film is bent together with the arranged electrodes, so that the unit cells are arranged between the bent folding films. The assembly can be manufactured.
- the electrode assembly thus manufactured has a structure in which the electrodes are inserted between the folded and stacked folding films.
- the spacing of the electrodes and the polarity of the electrodes are selected such that the polarities of the upper and lower electrodes in contact with the folding film are reversed.
- the arrangement interval of the electrodes and the polarity of each electrode may be selected to form the structure of the electrode assembly such as the anode / folding film / cathode / folding film / anode.
- the length of the folding film used to manufacture the electrode assembly may be selected to wrap the last unit cell or electrode in the manner described above, and then wrap the electrode assembly at least once.
- the electrode assemblies may be modified in various other forms, and the scope of the present invention is not limited thereto.
- PVdF-CTFE Polyvinylidene fluoride-chlorotrifluoroethylene copolymer
- cyanoethylpullulan cyanoethylpullulan
- PVdF-HFP polyvinylidene fluoride-hexafluoropropylene copolymer
- the slurry prepared above is coated on one side by a slot die coating method, and the polymer solution is coated on a reverse side by a roll coating method on a 70 ° C. oven. Dried at. At this time, it was confirmed that the thickness of the slurry-coated first porous coating layer was 6.9 ⁇ m, and the thickness of the second porous coating layer coated with the second polymer solution using non-solvent was 0.9 ⁇ m.
- the measured aeration time of the prepared separator was excellent as 772 sec / 100cc.
- a separator was manufactured in the same manner as in Example 1, except that the slurry was applied to the lower layer and the first polymer solution was applied to the upper layer in a slide-slot manner on one surface of the porous substrate.
- the thickness of the first porous coating layer in which the polymer thin film was further formed was found to be 7.5 ⁇ m, and the thickness of the second porous coating layer coated with the second polymer solution using the non-solvent was found to be 0.9 ⁇ m.
- the measured aeration time of the prepared separator was excellent as 780 sec / 100cc.
- a separator was prepared in the same manner as in Example 1, except that the second polymer solution was prepared by dissolving a polyvinylidene fluoride-hexafluoropropylene copolymer (PVdF-HFP) in acetone as a solvent. At this time, it was confirmed that the thickness of the slurry-coated first porous coating layer was 6.8 ⁇ m, and the thickness of the second porous coating layer coated with the second polymer solution was 0.9 ⁇ m. The measured aeration time of the prepared separator deteriorated to 1542 sec / 100 cc.
- PVdF-HFP polyvinylidene fluoride-hexafluoropropylene copolymer
- FIG. 1 A SEM photograph of the binder thin film of the separator prepared in Example 1 is shown in FIG.
- Example 1 The separator prepared in Example 1 and Comparative Example 1 was placed so that the first porous coating layer was in contact with the positive electrode surface and the second porous coating layer was in contact with the negative electrode, thereby preparing a stacked bicell, which was then again formed on the second porous coating layer.
- the electrode assembly was prepared by folding after bonding. The prepared electrode assembly is shown in Table 1 by measuring the discharge resistance at various states of charge (SOC).
- separator 10 porous substrate
- first porous coating layer 30 second porous coating layer
Abstract
Description
SOC | 실시예 1 | 비교예 1 |
95% | 57.1 mΩ | 59.5 mΩ |
50% | 58.7 mΩ | 60.0 mΩ |
30% | 63.9 mΩ | 65.5 mΩ |
Claims (15)
- 다공성 기재;상기 다공성 기재의 일면에 형성되어 있으며, 무기물 입자 및 제1 바인더 고분자의 혼합물을 포함하는 제1 다공성 코팅층; 및상기 다공성 기재의 타면에 형성되어 있으며, 용매, 비용매 및 제2 바인더 고분자의 혼합물의 건조 결과물을 포함하는 제2 다공성 코팅층을 구비하는 세퍼레이터.
- 제1항에 있어서,상기 제2 다공성 코팅층은 상기 다공성 기재의 타면의 일부분에만 형성되는 것을 특징으로 하는 세퍼레이터.
- 제1항에 있어서,상기 제1 다공성 코팅층의 표면에 형성되어 있으며, 제3 바인더 고분자를 포함하는 전극접착층을 더 구비하는 것을 특징으로 하는 세퍼레이터.
- 제1항에 있어서,상기 다공성 기재는 폴리올레핀계 다공성 기재인 것을 특징으로 하는 세퍼레이터.
- 제4항에 있어서,상기 폴리올레핀계 다공성 기재는 폴리에틸렌, 폴리프로필렌, 폴리부틸렌 및 폴리펜텐으로 이루어진 군으로부터 선택된 어느 하나의 고분자로 형성된 것을 특징으로 하는 세퍼레이터.
- 제1항에 있어서,상기 무기물 입자는 유전율 상수가 5 이상인 무기물 입자, 리튬 이온 전달 능력을 갖는 무기물 입자 및 이들의 혼합물로 이루어진 군으로부터 선택된 무기물 입자인 것을 특징으로 하는 세퍼레이터.
- 제6항에 있어서,상기 유전율 상수가 5 이상인 무기물 입자는 BaTiO3, Pb(Zrx,Ti1-x)O3 (PZT, 0<x<1), Pb1-xLaxZr1-yTiyO3(PLZT, 0<x<1, 0<y<1), (1-x)Pb(Mg1/3Nb2/3)O3-xPbTiO3(PMN-PT, 0<x<1), 하프니아(HfO2), SrTiO3, SnO2, CeO2, MgO, NiO, CaO, ZnO, ZrO2, SiO2, Y2O3, Al2O3, SiC 및 TiO2로 이루어진 군으로부터 선택된 어느 하나의 무기물 입자 또는 이들 중 2종 이상의 혼합물인 것을 특징으로 하는 세퍼레이터.
- 제6항에 있어서,상기 리튬 이온 전달 능력을 갖는 무기물 입자는 리튬포스페이트(Li3PO4), 리튬티타늄포스페이트(LixTiy(PO4)3, 0 < x < 2, 0 < y < 3), 리튬알루미늄티타늄포스페이트(LixAlyTiz(PO4)3, 0 < x < 2, 0 < y < 1, 0 < z < 3), (LiAlTiP)xOy 계열 glass(0 < x < 4, 0 < y < 13), 리튬란탄티타네이트(LixLayTiO3, 0 < x < 2, 0 < y < 3), 리튬게르마니움티오포스페이트(LixGeyPzSw, 0 < x < 4, 0 < y < 1, 0 < z < 1, 0 < w < 5), 리튬나이트라이드(LixNy, 0 < x < 4, 0 < y < 2), SiS2 (LixSiySz, 0 < x < 3, 0 < y < 2, 0 < z < 4) 계열 glass 및 P2S5 (LixPySz, 0 < x < 3, 0 < y < 3, 0 < z < 7) 계열 glass로 이루어진 군으로부터 선택된 어느 하나의 무기물 입자 또는 이들 중 2종 이상의 혼합물인 것을 특징으로 하는 세퍼레이터.
- 제1항에 있어서,상기 제1 바인더 고분자 및 제2 바인더 고분자는 서로 독립적으로, 폴리비닐리덴 플루오라이드-헥사플루오로프로필렌 (polyvinylidene fluoride-co-hexafluoropropylene), 폴리비닐리덴 플루오라이드-트리클로로에틸렌 (polyvinylidene fluoride-co-trichloroethylene), 폴리메틸메타크릴레이트 (polymethylmethacrylate), 폴리부틸아크릴레이트(polybutylacrylate), 폴리아크릴로니트릴 (polyacrylonitrile), 폴리비닐피롤리돈 (polyvinylpyrrolidone), 폴리비닐아세테이트 (polyvinylacetate), 폴리비닐알콜(polyvinyl alchol), 에틸렌 비닐 아세테이트 공중합체 (polyethylene-co-vinyl acetate), 폴리에틸렌옥사이드 (polyethylene oxide), 폴리아릴레이트(polyarylate), 셀룰로오스 아세테이트 (cellulose acetate), 셀룰로오스 아세테이트 부틸레이트 (cellulose acetate butyrate), 셀룰로오스 아세테이트 프로피오네이트 (cellulose acetate propionate), 시아노에틸플루란 (cyanoethylpullulan), 시아노에틸폴리비닐알콜 (cyanoethylpolyvinylalcohol), 시아노에틸셀룰로오스 (cyanoethylcellulose), 시아노에틸수크로오스 (cyanoethylsucrose), 플루란 (pullulan), 카르복실 메틸 셀룰로오스 (carboxyl methyl cellulose) 및 분자량 10,000 g/mol 이하의 저분자 화합물로 이루어진 군으로부터 선택된 어느 하나의 바인더 고분자 또는 이들 중 2종 이상의 혼합물인 것을 특징으로 하는 세퍼레이터.
- 제1항에 있어서,상기 용매는 아세톤, 테트라하이드로퓨란, 메틸렌클로라이드, 클로로포름, 디메틸포름아미드, N-메틸-2-피롤리돈 및 시클로헥산 중에서 선택된 1종의 화합물 또는 2종 이상의 혼합물인 것을 특징으로 하는 세퍼레이터.
- 제1항에 있어서,상기 비용매는 메탄올, 에탄올, 이소프로필알코올 및 물 중에서 선택된 1종의 화합물 또는 2종 이상의 혼합물인 것을 특징으로 하는 세퍼레이터.
- 제1항에 있어서,상기 용매와 비용매의 중량비는 50:50 내지 99:1인 것을 특징으로 하는 세퍼레이터.
- 제3항에 있어서,상기 제3 바인더 고분자는 폴리비닐리덴 플루오라이드-헥사플루오로프로필렌 (polyvinylidene fluoride-co-hexafluoropropylene), 폴리비닐리덴 플루오라이드-트리클로로에틸렌 (polyvinylidene fluoride-co-trichloroethylene), 폴리메틸메타크릴레이트 (polymethylmethacrylate), 폴리부틸아크릴레이트(polybutylacrylate), 폴리아크릴로니트릴 (polyacrylonitrile), 폴리비닐피롤리돈 (polyvinylpyrrolidone), 폴리비닐아세테이트 (polyvinylacetate), 폴리비닐알콜(polyvinyl alchol), 에틸렌 비닐 아세테이트 공중합체 (polyethylene-co-vinyl acetate), 폴리에틸렌옥사이드 (polyethylene oxide), 폴리아릴레이트(polyarylate), 셀룰로오스 아세테이트 (cellulose acetate), 셀룰로오스 아세테이트 부틸레이트 (cellulose acetate butyrate), 셀룰로오스 아세테이트 프로피오네이트 (cellulose acetate propionate), 시아노에틸플루란 (cyanoethylpullulan), 시아노에틸폴리비닐알콜 (cyanoethylpolyvinylalcohol), 시아노에틸셀룰로오스 (cyanoethylcellulose), 시아노에틸수크로오스 (cyanoethylsucrose), 플루란 (pullulan), 카르복실 메틸 셀룰로오스 (carboxyl methyl cellulose) 및 분자량 10,000 g/mol 이하의 저분자 화합물로 이루어진 군으로부터 선택된 어느 하나의 바인더 고분자 또는 이들 중 2종 이상의 혼합물인 것을 특징으로 하는 세퍼레이터.
- 양극, 음극, 상기 양극과 음극 사이에 개재된 세퍼레이터를 포함하는 전기화학소자에 있어서,상기 세퍼레이터가 제1항 내지 제13항 중 어느 한 항의 세퍼레이터인 것을 특징으로 하는 전기화학소자.
- 제14항에 있어서,상기 전기화학소자는 리튬 이차전지인 것을 특징으로 하는 전기화학소자.
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JP2014535673A JP6251680B2 (ja) | 2011-11-11 | 2012-11-09 | セパレータ及びそれを備える電気化学素子 |
EP12847056.4A EP2779275B1 (en) | 2011-11-11 | 2012-11-09 | Separator, and electrochemical device comprising same |
CN201280045750.XA CN103814460B (zh) | 2011-11-11 | 2012-11-09 | 隔膜及具有该隔膜的电化学器件 |
US13/920,505 US10033024B2 (en) | 2011-11-11 | 2013-06-18 | Separator and electrochemical device having the same |
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KR101358764B1 (ko) | 2014-02-07 |
JP6251680B2 (ja) | 2017-12-20 |
CN103814460B (zh) | 2017-05-17 |
JP2014530472A (ja) | 2014-11-17 |
EP2779275A1 (en) | 2014-09-17 |
TWI620368B (zh) | 2018-04-01 |
US20130280583A1 (en) | 2013-10-24 |
CN103814460A (zh) | 2014-05-21 |
TW201528591A (zh) | 2015-07-16 |
EP2779275B1 (en) | 2017-02-15 |
KR20130052526A (ko) | 2013-05-22 |
TW201324923A (zh) | 2013-06-16 |
US10033024B2 (en) | 2018-07-24 |
TWI484685B (zh) | 2015-05-11 |
EP2779275A4 (en) | 2016-03-02 |
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