WO2013091817A1 - Hochporöse separator-folie mit beschichtung und abschaltfunktion - Google Patents
Hochporöse separator-folie mit beschichtung und abschaltfunktion Download PDFInfo
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- WO2013091817A1 WO2013091817A1 PCT/EP2012/005204 EP2012005204W WO2013091817A1 WO 2013091817 A1 WO2013091817 A1 WO 2013091817A1 EP 2012005204 W EP2012005204 W EP 2012005204W WO 2013091817 A1 WO2013091817 A1 WO 2013091817A1
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- Prior art keywords
- film
- inorganic
- coating
- porous
- film according
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- H—ELECTRICITY
- H01—ELECTRIC ELEMENTS
- H01M—PROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
- 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
- H01M50/403—Manufacturing processes of separators, membranes or diaphragms
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- H—ELECTRICITY
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- H01M—PROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
- 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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- B—PERFORMING OPERATIONS; TRANSPORTING
- B29—WORKING OF PLASTICS; WORKING OF SUBSTANCES IN A PLASTIC STATE IN GENERAL
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- B29C48/00—Extrusion moulding, i.e. expressing the moulding material through a die or nozzle which imparts the desired form; Apparatus therefor
- B29C48/001—Combinations of extrusion moulding with other shaping operations
- B29C48/0018—Combinations of extrusion moulding with other shaping operations combined with shaping by orienting, stretching or shrinking, e.g. film blowing
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- B—PERFORMING OPERATIONS; TRANSPORTING
- B29—WORKING OF PLASTICS; WORKING OF SUBSTANCES IN A PLASTIC STATE IN GENERAL
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- B29C48/00—Extrusion moulding, i.e. expressing the moulding material through a die or nozzle which imparts the desired form; Apparatus therefor
- B29C48/03—Extrusion moulding, i.e. expressing the moulding material through a die or nozzle which imparts the desired form; Apparatus therefor characterised by the shape of the extruded material at extrusion
- B29C48/07—Flat, e.g. panels
- B29C48/08—Flat, e.g. panels flexible, e.g. films
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- B—PERFORMING OPERATIONS; TRANSPORTING
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- B29C55/00—Shaping by stretching, e.g. drawing through a die; Apparatus therefor
- B29C55/005—Shaping by stretching, e.g. drawing through a die; Apparatus therefor characterised by the choice of materials
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- B—PERFORMING OPERATIONS; TRANSPORTING
- B29—WORKING OF PLASTICS; WORKING OF SUBSTANCES IN A PLASTIC STATE IN GENERAL
- B29C—SHAPING OR JOINING OF PLASTICS; SHAPING OF MATERIAL IN A PLASTIC STATE, NOT OTHERWISE PROVIDED FOR; AFTER-TREATMENT OF THE SHAPED PRODUCTS, e.g. REPAIRING
- B29C55/00—Shaping by stretching, e.g. drawing through a die; Apparatus therefor
- B29C55/02—Shaping by stretching, e.g. drawing through a die; Apparatus therefor of plates or sheets
- B29C55/10—Shaping by stretching, e.g. drawing through a die; Apparatus therefor of plates or sheets multiaxial
- B29C55/12—Shaping by stretching, e.g. drawing through a die; Apparatus therefor of plates or sheets multiaxial biaxial
- B29C55/14—Shaping by stretching, e.g. drawing through a die; Apparatus therefor of plates or sheets multiaxial biaxial successively
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- B—PERFORMING OPERATIONS; TRANSPORTING
- B29—WORKING OF PLASTICS; WORKING OF SUBSTANCES IN A PLASTIC STATE IN GENERAL
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- B29C55/02—Shaping by stretching, e.g. drawing through a die; Apparatus therefor of plates or sheets
- B29C55/10—Shaping by stretching, e.g. drawing through a die; Apparatus therefor of plates or sheets multiaxial
- B29C55/12—Shaping by stretching, e.g. drawing through a die; Apparatus therefor of plates or sheets multiaxial biaxial
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- B29C55/143—Shaping by stretching, e.g. drawing through a die; Apparatus therefor of plates or sheets multiaxial biaxial successively firstly parallel to the direction of feed and then transversely thereto
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- B—PERFORMING OPERATIONS; TRANSPORTING
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- B32B27/00—Layered products comprising a layer of synthetic resin
- B32B27/32—Layered products comprising a layer of synthetic resin comprising polyolefins
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- C—CHEMISTRY; METALLURGY
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- C—CHEMISTRY; METALLURGY
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- C—CHEMISTRY; METALLURGY
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- C08K5/09—Carboxylic acids; Metal salts thereof; Anhydrides thereof
- C08K5/098—Metal salts of carboxylic acids
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- C08—ORGANIC MACROMOLECULAR COMPOUNDS; THEIR PREPARATION OR CHEMICAL WORKING-UP; COMPOSITIONS BASED THEREON
- C08L—COMPOSITIONS OF MACROMOLECULAR COMPOUNDS
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- C08L23/02—Compositions of homopolymers or copolymers of unsaturated aliphatic hydrocarbons having only one carbon-to-carbon double bond; Compositions of derivatives of such polymers not modified by chemical after-treatment
- C08L23/04—Homopolymers or copolymers of ethene
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- C08—ORGANIC MACROMOLECULAR COMPOUNDS; THEIR PREPARATION OR CHEMICAL WORKING-UP; COMPOSITIONS BASED THEREON
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- C08L23/02—Compositions of homopolymers or copolymers of unsaturated aliphatic hydrocarbons having only one carbon-to-carbon double bond; Compositions of derivatives of such polymers not modified by chemical after-treatment
- C08L23/10—Homopolymers or copolymers of propene
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- H01M50/406—Moulding; Embossing; Cutting
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- Y02E60/00—Enabling technologies; Technologies with a potential or indirect contribution to GHG emissions mitigation
- Y02E60/10—Energy storage using batteries
Definitions
- the present invention relates to a coated, double-backed porous film and its use as a separator, and to a process for producing the film.
- NiCd nickel-cadmium
- lithium, lithium-ion, lithium-polymer, and alkaline-earth batteries are increasingly being used as accumulators.
- the separator must be a barrier which electrically insulates the two electrodes from each other to avoid internal short circuits. At the same time, however, the separator must be permeable to ions so that the electrochemical reactions in the cell can proceed.
- a battery separator must be thin, so that the internal resistance is as low as possible and a high packing density can be achieved. That's the only way to be good
- Separator also has a large porosity. Furthermore, they must be lightweight so that a low specific gravity is achieved and they must be absolutely safe. This means that in the event of overheating or mechanical damage, the positive and negative electrodes must be kept separate in order to prevent further chemical reactions that lead to the fire or explosion of the batteries.
- US2007020525 describes a ceramic separator obtained by processing inorganic particles with a polymer-based binder. This separator also ensures that the anode and cathode in the battery remain disconnected in the event of severe overheating. But the manufacturing process is complicated and the mechanical properties of the separator are insufficient.
- the coating is a continuous, porous, electrically non-conductive ceramic
- the pores are in principle produced by dissolving out a component from the polymer matrix by means of suitable solvents.
- suitable solvents a variety of variants have developed, which differ in the nature of the additives and the appropriate solvents.
- Both organic and inorganic additives can be extracted. This extraction can be done as the last step in the production of the film or combined with a subsequent drawing.
- the disadvantage in this case is the ecologically and economically questionable extraction step. An older but successful procedure is based on a stretching of the
- ceramic, coated Separatorfolien based on porous polyolefin films are produced when the inorganic, preferably ceramic, coating on a biaxially oriented, single or multilayer porous film whose porosity is produced by conversion of ß-crystalline polypropylene during stretching of the film, which at least comprises a porous layer and this layer contains at least one propylene and polyethylene polymer and ⁇ -nucleating agent, wherein the film before the coating has a Gurley value of ⁇ 1000s, is applied.
- the subject of the present invention is thus a
- the films used according to the invention for the coating can be constructed in one or more layers.
- the production of such single-layered or multi-layered porous polypropylene film in which propylene polymer and ⁇ -nucleating agent is melted in an extruder and extruded through a flat die onto a take-off roll has already been described in detail in DE-A-102010018374.
- the melt film cools on the take-off roll to form ⁇ -crystallites and solidifies. Subsequently, this film is stretched in the longitudinal direction and then directly in the transverse direction.
- the films used according to the invention for coating can also be wound in the longitudinal direction after drawing and at a later time in a second Unwrapped transverse stretching process, heated to transverse stretching temperature and in
- Neutralizing agent constructed. Again, preferably at least 5% by weight, more preferably at least 10% by weight, of polyethylenes are present.
- Propylene block copolymers have a melting point of about 140 to 170 ° C, preferably from 145 to 165 ° C, especially 150 to 160 ° C and a
- ⁇ -nucleating agents are basically all known for the porous layer Suitable additives which promote the formation of ß-crystals of the polypropylene during cooling of a polypropylene melt.
- Suitable additives which promote the formation of ß-crystals of the polypropylene during cooling of a polypropylene melt.
- Such ⁇ -nucleating agents, as well as their mode of action in a polypropylene matrix, are per se known in the art and will be described in detail below.
- highly active ⁇ -nucleating agents are preferably used which, on cooling a propylene homopolymer melt, produce a ⁇ content of 40-95%, preferably of 50-85% (DSC).
- the ß-portion is cooled from the DSC
- both the shutdown layer I and the porous layer II may contain other polyolefins in addition to the propylene homopolymer and propylene block copolymers as long as they do not adversely affect the properties, particularly porosity and mechanical strengths and shutdown function
- polystyrene resins include, for example, random copolymers of ethylene and propylene having an ethylene content of 20% by weight or less, random copolymers of propylene with C 4 -C 8 olefins having an olefin content of 20% by weight or less, terpolymers of propylene, Ethylene and butylene having an ethylene content of 10% by weight or less and having a butylene content of 15% by weight or less, or other polyethylenes such as LDPE, VLDPE, and LLDPE.
- the porous film may be one or more layers.
- the thickness of the film is generally in a range of 10 to 100 ⁇ , preferably 15 to 60 ⁇ , for example 15 to 40pm.
- the porous film may be provided on its surface with a corona, flame or plasma treatment to improve the filling with electrolytes.
- the film comprises further porous ones
- the density of the porous film to be coated is generally in a range of 0.1 to 0.6 g / cm 3 , preferably 0.2 to 0.5 g / cm 3 .
- the mean pore diameter should be in the range 50 to 100 nm, preferably in the range 60-80 nm.
- the coating is electrically insulating.
- the particles used according to the invention consist of electrically insulating materials, preferably a non-electrically conductive oxide of the metals Al, Zr, Si, Sn, Ti and / or Y.
- electrically insulating materials preferably a non-electrically conductive oxide of the metals Al, Zr, Si, Sn, Ti and / or Y.
- the production of such particles is described in detail, for example, in DE-A-10208277.
- the inventive inorganic, preferably ceramic, coating comprises inorganic, preferably ceramic, particles which preferably have a compressive strength of min. 100 kPa, more preferably from min. 150kPa,
- the inorganic, preferably ceramic, coating preferably not greater than 33% of the thickness of the inorganic, preferably ceramic, coating, in particular not greater than 25% of the thickness of the inorganic, preferably ceramic, coating.
- binders used according to the invention should be electrically insulating, ie have no electrical conductivity. Electrically insulating or no electrical conductivity means that these properties are minor but can not increase the values for the uncoated film.
- Machine direction is stretched.
- the cooled prefilm is first passed over one or more heating rollers, which heat the film to the appropriate temperature. In general, this temperature is less than 140 ° C, preferably 70 to 120 ° C.
- the longitudinal stretching is then generally carried out with the help of two according to the desired stretch ratio different schnei securedder rollers.
- the longitudinal stretch ratio lies within a range from 2: 1 to 6: 1, preferably 3: 1 to 5: 1. To avoid too high orientation in the longitudinal direction of the latitudinal recess is kept low in the longitudinal paths, for example, by setting a comparatively narrow
- the film is wound in the usual way with a take-up device.
- Separator films based on porous polyolefin films comprises a porous, biaxially oriented film of polypropylene with a porosity of 30 to 80% and a Permeability of ⁇ 1000s (Gurley value) and the permeability of the inventive separator films with ceramic coating is ⁇ 1500s (Gurley value).
- the inorganic, preferably ceramic, coating present on the separator film according to the invention exhibits a good adhesion behavior, this being achieved without the use of adhesion promoters. The detention behavior is assessed as follows:
- a suitable particle size analyzer is
- Microtrac S 3500 for example, a Microtrac S 3500.
- the melt flow index of the propylene polymers was measured according to DIN 53 735 at 2, 16 kg load and 230 ° C.
- the determination of the ⁇ -content of the precursor film is likewise carried out by means of a DSC measurement which is carried out on the prefilmate film as follows: The precursor film is first heated to 220 ° C. in the DSC at a heating rate of 10 K / min and melted and cooled again 1 .
- Aufmorekurve is the
- the molten polymer mixture was withdrawn after extrusion via a first take-off roll and another rolling center and solidified, then longitudinally stretched, transversely stretched and fixed, the following in detail
- Composition Coating 1 (Table 1) applied by hand. The wetting of the film with the ceramic suspension is uniform. The thus coated film is then dried for one hour at 90 ° C in a drying oven. The coating shows good adhesion to the film after drying. Subsequently, coating weight, coat thickness of the coating and the air permeability determined by the Gurley value. Only a slight increase in the Gurley value from 360 s to 380 s is observed.
- Coating is the wetting of the film with the ceramic suspension evenly. After drying, the coating shows good adhesion to the film. An increase of the Gurley value from 360 s to 460 s is observed.
- the Polyolefin Separator Fa. ÜBE was as in Example 2 with a
- Example 4 PBS 30 Coat. 1 0.7 380 420> 5000s 52 63 yes yes
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- Chemical & Material Sciences (AREA)
- Chemical Kinetics & Catalysis (AREA)
- Engineering & Computer Science (AREA)
- Electrochemistry (AREA)
- General Chemical & Material Sciences (AREA)
- Manufacturing & Machinery (AREA)
- Mechanical Engineering (AREA)
- Health & Medical Sciences (AREA)
- Medicinal Chemistry (AREA)
- Polymers & Plastics (AREA)
- Organic Chemistry (AREA)
- Inorganic Chemistry (AREA)
- Materials Engineering (AREA)
- Ceramic Engineering (AREA)
- Crystallography & Structural Chemistry (AREA)
- Cell Separators (AREA)
- Laminated Bodies (AREA)
- Manufacture Of Porous Articles, And Recovery And Treatment Of Waste Products (AREA)
- Application Of Or Painting With Fluid Materials (AREA)
Abstract
Description
Claims
Priority Applications (11)
Application Number | Priority Date | Filing Date | Title |
---|---|---|---|
IN4445CHN2014 IN2014CN04445A (de) | 2011-12-20 | 2012-12-17 | |
EP12824794.7A EP2794271B1 (de) | 2011-12-20 | 2012-12-17 | Hochporöse separator-folie mit beschichtung und abschaltfunktion |
CN201280061535.9A CN103998240B (zh) | 2011-12-20 | 2012-12-17 | 具有涂层和切断功能的高孔隙度隔板膜 |
MX2014007475A MX2014007475A (es) | 2011-12-20 | 2012-12-17 | Pelicula separadora de alta porosidad con recubrimiento y funcion de desactivacion. |
CA2859851A CA2859851A1 (en) | 2011-12-20 | 2012-12-17 | High-porosity separator film with coating and shut down function |
JP2014547754A JP6118818B2 (ja) | 2011-12-20 | 2012-12-17 | コーティングおよびシャットダウン機能を備えた高多孔性セパレータフィルム |
PL12824794T PL2794271T3 (pl) | 2011-12-20 | 2012-12-17 | Silnie porowata folia separatorowa z powłoką i funkcją odcinającą |
KR1020147016921A KR20140116074A (ko) | 2011-12-20 | 2012-12-17 | 코팅 및 셧다운 기능을 갖는 고다공성 세퍼레이터 필름 |
ES12824794.7T ES2668819T3 (es) | 2011-12-20 | 2012-12-17 | Película separadora de alta porosidad con recubrimiento y función de desactivación |
US14/366,464 US20150017511A1 (en) | 2011-12-20 | 2012-12-17 | Highly porous separator film having a coating and a disconnecting function |
US16/664,063 US20200058915A1 (en) | 2011-12-20 | 2019-10-25 | High-porosity separator film with coating and shut down function |
Applications Claiming Priority (2)
Application Number | Priority Date | Filing Date | Title |
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DE102011121606.9 | 2011-12-20 | ||
DE102011121606A DE102011121606A1 (de) | 2011-12-20 | 2011-12-20 | Hochporöse Separator-Folie mit Beschichtung und Abschaltfunktion |
Related Child Applications (2)
Application Number | Title | Priority Date | Filing Date |
---|---|---|---|
US14/366,464 A-371-Of-International US20150017511A1 (en) | 2011-12-20 | 2012-12-17 | Highly porous separator film having a coating and a disconnecting function |
US16/664,063 Continuation US20200058915A1 (en) | 2011-12-20 | 2019-10-25 | High-porosity separator film with coating and shut down function |
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WO2013091817A1 true WO2013091817A1 (de) | 2013-06-27 |
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ID=47722204
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PCT/EP2012/005204 WO2013091817A1 (de) | 2011-12-20 | 2012-12-17 | Hochporöse separator-folie mit beschichtung und abschaltfunktion |
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Country | Link |
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US (2) | US20150017511A1 (de) |
EP (1) | EP2794271B1 (de) |
JP (1) | JP6118818B2 (de) |
KR (1) | KR20140116074A (de) |
CN (1) | CN103998240B (de) |
CA (1) | CA2859851A1 (de) |
DE (1) | DE102011121606A1 (de) |
ES (1) | ES2668819T3 (de) |
HU (1) | HUE037658T2 (de) |
IN (1) | IN2014CN04445A (de) |
MX (1) | MX2014007475A (de) |
PL (1) | PL2794271T3 (de) |
WO (1) | WO2013091817A1 (de) |
Cited By (1)
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CN104112833A (zh) * | 2014-06-06 | 2014-10-22 | 珠海光宇电池有限公司 | 锂离子电池隔膜及其制备方法、应用 |
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DE102012004161A1 (de) * | 2012-03-05 | 2013-09-05 | Treofan Germany Gmbh & Co. Kg | Hochporöse Separator-Folie mit partieller Beschichtung |
DE102015013515A1 (de) * | 2015-10-20 | 2017-04-20 | Treofan Germany Gmbh & Co. Kg | Biaxial orientierte poröse Folie mit Partikel-haltiger poröser Schicht und anorganischer Beschichtung |
JP6567126B2 (ja) * | 2017-04-28 | 2019-08-28 | 住友化学株式会社 | 非水電解液二次電池用絶縁性多孔質層 |
JP6883263B2 (ja) * | 2017-09-11 | 2021-06-09 | トヨタ自動車株式会社 | 非水電解液二次電池 |
KR102316016B1 (ko) * | 2017-09-22 | 2021-10-22 | 주식회사 엘지화학 | 필름 및 히트 파이프의 제조 방법 |
CN110364661B (zh) * | 2018-04-11 | 2022-11-25 | 宁德新能源科技有限公司 | 隔离膜及储能装置 |
KR102613190B1 (ko) * | 2018-05-29 | 2023-12-14 | 현대자동차주식회사 | 리튬 이차전지용 전해액 및 이를 포함하는 리튬 이차전지 |
WO2020050924A1 (en) * | 2018-09-07 | 2020-03-12 | Applied Materials, Inc. | Ceramic coating on separator for batteries |
JP7298246B2 (ja) * | 2019-03-29 | 2023-06-27 | Ube株式会社 | ポリオレフィン多孔質フィルム、蓄電デバイス用セパレータ、および蓄電デバイス |
CN113527785B (zh) * | 2020-04-14 | 2022-12-09 | 中国石油化工股份有限公司 | 用于土工膜表面加糙的复合材料和糙面土工膜及各自的制备方法 |
US11976177B2 (en) | 2020-07-01 | 2024-05-07 | Celanese International Corporation | Polymer composition and membranes made therefrom with improved mechanical strength |
CN116207446B (zh) * | 2023-05-06 | 2023-08-01 | 深圳中兴新材技术股份有限公司 | 低短路率的锂电池隔膜及其制备方法 |
CN116387757B (zh) * | 2023-05-29 | 2023-08-08 | 合肥长阳新能源科技有限公司 | 一种高孔隙率钠离子电池拉伸隔膜及其制备方法 |
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- 2012-12-17 ES ES12824794.7T patent/ES2668819T3/es active Active
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- 2012-12-17 KR KR1020147016921A patent/KR20140116074A/ko active IP Right Grant
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Also Published As
Publication number | Publication date |
---|---|
ES2668819T3 (es) | 2018-05-22 |
KR20140116074A (ko) | 2014-10-01 |
JP6118818B2 (ja) | 2017-04-19 |
US20150017511A1 (en) | 2015-01-15 |
HUE037658T2 (hu) | 2018-09-28 |
CA2859851A1 (en) | 2013-06-27 |
EP2794271B1 (de) | 2018-02-21 |
PL2794271T3 (pl) | 2019-03-29 |
JP2015508553A (ja) | 2015-03-19 |
EP2794271A1 (de) | 2014-10-29 |
DE102011121606A1 (de) | 2013-06-20 |
IN2014CN04445A (de) | 2015-09-04 |
CN103998240A (zh) | 2014-08-20 |
MX2014007475A (es) | 2014-07-30 |
US20200058915A1 (en) | 2020-02-20 |
CN103998240B (zh) | 2017-05-24 |
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