WO2019078155A1 - タブリード用フィルム、及びこれを用いたタブリード - Google Patents
タブリード用フィルム、及びこれを用いたタブリード Download PDFInfo
- Publication number
- WO2019078155A1 WO2019078155A1 PCT/JP2018/038311 JP2018038311W WO2019078155A1 WO 2019078155 A1 WO2019078155 A1 WO 2019078155A1 JP 2018038311 W JP2018038311 W JP 2018038311W WO 2019078155 A1 WO2019078155 A1 WO 2019078155A1
- Authority
- WO
- WIPO (PCT)
- Prior art keywords
- film
- tab lead
- surface layer
- inorganic filler
- thickness
- Prior art date
Links
- 239000002344 surface layer Substances 0.000 claims abstract description 90
- 229910052751 metal Inorganic materials 0.000 claims abstract description 80
- 239000002184 metal Substances 0.000 claims abstract description 80
- 239000011256 inorganic filler Substances 0.000 claims abstract description 69
- 229910003475 inorganic filler Inorganic materials 0.000 claims abstract description 69
- KRHYYFGTRYWZRS-UHFFFAOYSA-N Fluorane Chemical compound F KRHYYFGTRYWZRS-UHFFFAOYSA-N 0.000 claims abstract description 56
- 229910000040 hydrogen fluoride Inorganic materials 0.000 claims abstract description 55
- 239000012792 core layer Substances 0.000 claims abstract description 46
- 229920005672 polyolefin resin Polymers 0.000 claims abstract description 30
- VTYYLEPIZMXCLO-UHFFFAOYSA-L Calcium carbonate Chemical group [Ca+2].[O-]C([O-])=O VTYYLEPIZMXCLO-UHFFFAOYSA-L 0.000 claims description 60
- 229910000019 calcium carbonate Inorganic materials 0.000 claims description 30
- BVKZGUZCCUSVTD-UHFFFAOYSA-L Carbonate Chemical compound [O-]C([O-])=O BVKZGUZCCUSVTD-UHFFFAOYSA-L 0.000 claims description 5
- 210000005239 tubule Anatomy 0.000 claims 1
- WHXSMMKQMYFTQS-UHFFFAOYSA-N Lithium Chemical compound [Li] WHXSMMKQMYFTQS-UHFFFAOYSA-N 0.000 abstract description 15
- 229910052744 lithium Inorganic materials 0.000 abstract description 15
- 238000004519 manufacturing process Methods 0.000 abstract description 15
- 230000007423 decrease Effects 0.000 abstract description 13
- 230000000694 effects Effects 0.000 abstract description 3
- 239000003795 chemical substances by application Substances 0.000 abstract 5
- 238000011109 contamination Methods 0.000 abstract 1
- 239000010410 layer Substances 0.000 description 29
- 238000012360 testing method Methods 0.000 description 25
- 229920005989 resin Polymers 0.000 description 15
- 239000011347 resin Substances 0.000 description 15
- 239000000853 adhesive Substances 0.000 description 14
- 230000001070 adhesive effect Effects 0.000 description 14
- -1 polyethylene Polymers 0.000 description 14
- 229920000098 polyolefin Polymers 0.000 description 14
- 230000014759 maintenance of location Effects 0.000 description 12
- PXHVJJICTQNCMI-UHFFFAOYSA-N Nickel Chemical compound [Ni] PXHVJJICTQNCMI-UHFFFAOYSA-N 0.000 description 11
- 239000004743 Polypropylene Substances 0.000 description 9
- 239000005001 laminate film Substances 0.000 description 9
- 229920001155 polypropylene Polymers 0.000 description 9
- 239000002245 particle Substances 0.000 description 7
- 239000005022 packaging material Substances 0.000 description 6
- 239000000565 sealant Substances 0.000 description 6
- 238000007789 sealing Methods 0.000 description 6
- 239000008151 electrolyte solution Substances 0.000 description 5
- 238000011156 evaluation Methods 0.000 description 5
- 239000000945 filler Substances 0.000 description 5
- 238000007654 immersion Methods 0.000 description 5
- 238000000034 method Methods 0.000 description 5
- VGGSQFUCUMXWEO-UHFFFAOYSA-N Ethene Chemical compound C=C VGGSQFUCUMXWEO-UHFFFAOYSA-N 0.000 description 4
- 239000005977 Ethylene Substances 0.000 description 4
- HBBGRARXTFLTSG-UHFFFAOYSA-N Lithium ion Chemical compound [Li+] HBBGRARXTFLTSG-UHFFFAOYSA-N 0.000 description 4
- 239000004698 Polyethylene Substances 0.000 description 4
- 229910052782 aluminium Inorganic materials 0.000 description 4
- XAGFODPZIPBFFR-UHFFFAOYSA-N aluminium Chemical compound [Al] XAGFODPZIPBFFR-UHFFFAOYSA-N 0.000 description 4
- 230000000052 comparative effect Effects 0.000 description 4
- 229910001416 lithium ion Inorganic materials 0.000 description 4
- 229910052759 nickel Inorganic materials 0.000 description 4
- 229920000573 polyethylene Polymers 0.000 description 4
- QQONPFPTGQHPMA-UHFFFAOYSA-N propylene Natural products CC=C QQONPFPTGQHPMA-UHFFFAOYSA-N 0.000 description 4
- 125000004805 propylene group Chemical group [H]C([H])([H])C([H])([*:1])C([H])([H])[*:2] 0.000 description 4
- 239000002253 acid Substances 0.000 description 3
- 150000001732 carboxylic acid derivatives Chemical class 0.000 description 3
- 230000007797 corrosion Effects 0.000 description 3
- 238000005260 corrosion Methods 0.000 description 3
- 239000011342 resin composition Substances 0.000 description 3
- CURLTUGMZLYLDI-UHFFFAOYSA-N Carbon dioxide Chemical compound O=C=O CURLTUGMZLYLDI-UHFFFAOYSA-N 0.000 description 2
- RYGMFSIKBFXOCR-UHFFFAOYSA-N Copper Chemical compound [Cu] RYGMFSIKBFXOCR-UHFFFAOYSA-N 0.000 description 2
- 150000008064 anhydrides Chemical class 0.000 description 2
- 229920001400 block copolymer Polymers 0.000 description 2
- 239000003990 capacitor Substances 0.000 description 2
- 150000004649 carbonic acid derivatives Chemical class 0.000 description 2
- 238000006243 chemical reaction Methods 0.000 description 2
- 239000003086 colorant Substances 0.000 description 2
- 229910052802 copper Inorganic materials 0.000 description 2
- 239000010949 copper Substances 0.000 description 2
- 239000011888 foil Substances 0.000 description 2
- 230000004927 fusion Effects 0.000 description 2
- 229920001903 high density polyethylene Polymers 0.000 description 2
- 239000004700 high-density polyethylene Substances 0.000 description 2
- WABPQHHGFIMREM-UHFFFAOYSA-N lead(0) Chemical compound [Pb] WABPQHHGFIMREM-UHFFFAOYSA-N 0.000 description 2
- 229920000092 linear low density polyethylene Polymers 0.000 description 2
- 239000004707 linear low-density polyethylene Substances 0.000 description 2
- 229920001684 low density polyethylene Polymers 0.000 description 2
- 239000004702 low-density polyethylene Substances 0.000 description 2
- 239000000463 material Substances 0.000 description 2
- 238000005259 measurement Methods 0.000 description 2
- 229920001179 medium density polyethylene Polymers 0.000 description 2
- 239000004701 medium-density polyethylene Substances 0.000 description 2
- 239000007769 metal material Substances 0.000 description 2
- 229910044991 metal oxide Inorganic materials 0.000 description 2
- 150000004706 metal oxides Chemical class 0.000 description 2
- 229920005629 polypropylene homopolymer Polymers 0.000 description 2
- 229920005604 random copolymer Polymers 0.000 description 2
- 239000000126 substance Substances 0.000 description 2
- 229920001897 terpolymer Polymers 0.000 description 2
- 229920002725 thermoplastic elastomer Polymers 0.000 description 2
- XLYOFNOQVPJJNP-UHFFFAOYSA-N water Substances O XLYOFNOQVPJJNP-UHFFFAOYSA-N 0.000 description 2
- SMZOUWXMTYCWNB-UHFFFAOYSA-N 2-(2-methoxy-5-methylphenyl)ethanamine Chemical compound COC1=CC=C(C)C=C1CCN SMZOUWXMTYCWNB-UHFFFAOYSA-N 0.000 description 1
- JAHNSTQSQJOJLO-UHFFFAOYSA-N 2-(3-fluorophenyl)-1h-imidazole Chemical compound FC1=CC=CC(C=2NC=CN=2)=C1 JAHNSTQSQJOJLO-UHFFFAOYSA-N 0.000 description 1
- NIXOWILDQLNWCW-UHFFFAOYSA-N 2-Propenoic acid Natural products OC(=O)C=C NIXOWILDQLNWCW-UHFFFAOYSA-N 0.000 description 1
- OFNISBHGPNMTMS-UHFFFAOYSA-N 3-methylideneoxolane-2,5-dione Chemical compound C=C1CC(=O)OC1=O OFNISBHGPNMTMS-UHFFFAOYSA-N 0.000 description 1
- OIFBSDVPJOWBCH-UHFFFAOYSA-N Diethyl carbonate Chemical compound CCOC(=O)OCC OIFBSDVPJOWBCH-UHFFFAOYSA-N 0.000 description 1
- KMTRUDSVKNLOMY-UHFFFAOYSA-N Ethylene carbonate Chemical compound O=C1OCCO1 KMTRUDSVKNLOMY-UHFFFAOYSA-N 0.000 description 1
- KRHYYFGTRYWZRS-UHFFFAOYSA-M Fluoride anion Chemical compound [F-] KRHYYFGTRYWZRS-UHFFFAOYSA-M 0.000 description 1
- UFHFLCQGNIYNRP-UHFFFAOYSA-N Hydrogen Chemical compound [H][H] UFHFLCQGNIYNRP-UHFFFAOYSA-N 0.000 description 1
- 229910013870 LiPF 6 Inorganic materials 0.000 description 1
- 229910019142 PO4 Inorganic materials 0.000 description 1
- OFOBLEOULBTSOW-UHFFFAOYSA-N Propanedioic acid Natural products OC(=O)CC(O)=O OFOBLEOULBTSOW-UHFFFAOYSA-N 0.000 description 1
- 239000012298 atmosphere Substances 0.000 description 1
- 230000015572 biosynthetic process Effects 0.000 description 1
- 239000002981 blocking agent Substances 0.000 description 1
- WUKWITHWXAAZEY-UHFFFAOYSA-L calcium difluoride Chemical compound [F-].[F-].[Ca+2] WUKWITHWXAAZEY-UHFFFAOYSA-L 0.000 description 1
- AXCZMVOFGPJBDE-UHFFFAOYSA-L calcium dihydroxide Chemical compound [OH-].[OH-].[Ca+2] AXCZMVOFGPJBDE-UHFFFAOYSA-L 0.000 description 1
- 239000000920 calcium hydroxide Substances 0.000 description 1
- 229910001861 calcium hydroxide Inorganic materials 0.000 description 1
- 239000001569 carbon dioxide Substances 0.000 description 1
- 229910002092 carbon dioxide Inorganic materials 0.000 description 1
- 150000007942 carboxylates Chemical class 0.000 description 1
- ZCDOYSPFYFSLEW-UHFFFAOYSA-N chromate(2-) Chemical compound [O-][Cr]([O-])(=O)=O ZCDOYSPFYFSLEW-UHFFFAOYSA-N 0.000 description 1
- 239000000470 constituent Substances 0.000 description 1
- LDHQCZJRKDOVOX-NSCUHMNNSA-N crotonic acid Chemical compound C\C=C\C(O)=O LDHQCZJRKDOVOX-NSCUHMNNSA-N 0.000 description 1
- 230000001186 cumulative effect Effects 0.000 description 1
- 230000003247 decreasing effect Effects 0.000 description 1
- IEJIGPNLZYLLBP-UHFFFAOYSA-N dimethyl carbonate Chemical compound COC(=O)OC IEJIGPNLZYLLBP-UHFFFAOYSA-N 0.000 description 1
- 230000005611 electricity Effects 0.000 description 1
- 239000003792 electrolyte Substances 0.000 description 1
- 230000002708 enhancing effect Effects 0.000 description 1
- 238000001125 extrusion Methods 0.000 description 1
- 239000007789 gas Substances 0.000 description 1
- 229910052739 hydrogen Inorganic materials 0.000 description 1
- 239000001257 hydrogen Substances 0.000 description 1
- CUPFNGOKRMWUOO-UHFFFAOYSA-N hydron;difluoride Chemical compound F.F CUPFNGOKRMWUOO-UHFFFAOYSA-N 0.000 description 1
- 239000012774 insulation material Substances 0.000 description 1
- ZLNQQNXFFQJAID-UHFFFAOYSA-L magnesium carbonate Chemical compound [Mg+2].[O-]C([O-])=O ZLNQQNXFFQJAID-UHFFFAOYSA-L 0.000 description 1
- 239000001095 magnesium carbonate Substances 0.000 description 1
- 229910000021 magnesium carbonate Inorganic materials 0.000 description 1
- VZCYOOQTPOCHFL-UPHRSURJSA-N maleic acid Chemical compound OC(=O)\C=C/C(O)=O VZCYOOQTPOCHFL-UPHRSURJSA-N 0.000 description 1
- 239000011976 maleic acid Substances 0.000 description 1
- FPYJFEHAWHCUMM-UHFFFAOYSA-N maleic anhydride Chemical compound O=C1OC(=O)C=C1 FPYJFEHAWHCUMM-UHFFFAOYSA-N 0.000 description 1
- LVHBHZANLOWSRM-UHFFFAOYSA-N methylenebutanedioic acid Natural products OC(=O)CC(=C)C(O)=O LVHBHZANLOWSRM-UHFFFAOYSA-N 0.000 description 1
- 239000000203 mixture Substances 0.000 description 1
- 238000012986 modification Methods 0.000 description 1
- 230000004048 modification Effects 0.000 description 1
- 238000000465 moulding Methods 0.000 description 1
- 239000011255 nonaqueous electrolyte Substances 0.000 description 1
- NBIIXXVUZAFLBC-UHFFFAOYSA-K phosphate Chemical compound [O-]P([O-])([O-])=O NBIIXXVUZAFLBC-UHFFFAOYSA-K 0.000 description 1
- 239000010452 phosphate Substances 0.000 description 1
- 239000000049 pigment Substances 0.000 description 1
- 239000000843 powder Substances 0.000 description 1
- 230000000630 rising effect Effects 0.000 description 1
- 150000003839 salts Chemical class 0.000 description 1
- 239000002356 single layer Substances 0.000 description 1
- 239000002904 solvent Substances 0.000 description 1
- 229920005992 thermoplastic resin Polymers 0.000 description 1
- VZCYOOQTPOCHFL-UHFFFAOYSA-N trans-butenedioic acid Natural products OC(=O)C=CC(O)=O VZCYOOQTPOCHFL-UHFFFAOYSA-N 0.000 description 1
- LDHQCZJRKDOVOX-UHFFFAOYSA-N trans-crotonic acid Natural products CC=CC(O)=O LDHQCZJRKDOVOX-UHFFFAOYSA-N 0.000 description 1
Images
Classifications
-
- 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
- H01M50/10—Primary casings; Jackets or wrappings
- H01M50/172—Arrangements of electric connectors penetrating the casing
- H01M50/174—Arrangements of electric connectors penetrating the casing adapted for the shape of the cells
- H01M50/178—Arrangements of electric connectors penetrating the casing adapted for the shape of the cells for pouch or flexible bag cells
-
- 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
- H01M50/10—Primary casings; Jackets or wrappings
- H01M50/172—Arrangements of electric connectors penetrating the casing
-
- B—PERFORMING OPERATIONS; TRANSPORTING
- B32—LAYERED PRODUCTS
- B32B—LAYERED PRODUCTS, i.e. PRODUCTS BUILT-UP OF STRATA OF FLAT OR NON-FLAT, e.g. CELLULAR OR HONEYCOMB, FORM
- B32B27/00—Layered products comprising a layer of synthetic resin
- B32B27/18—Layered products comprising a layer of synthetic resin characterised by the use of special additives
- B32B27/20—Layered products comprising a layer of synthetic resin characterised by the use of special additives using fillers, pigments, thixotroping agents
-
- B—PERFORMING OPERATIONS; TRANSPORTING
- B32—LAYERED PRODUCTS
- B32B—LAYERED PRODUCTS, i.e. PRODUCTS BUILT-UP OF STRATA OF FLAT OR NON-FLAT, e.g. CELLULAR OR HONEYCOMB, FORM
- B32B27/00—Layered products comprising a layer of synthetic resin
- B32B27/32—Layered products comprising a layer of synthetic resin comprising polyolefins
-
- H—ELECTRICITY
- H01—ELECTRIC ELEMENTS
- H01G—CAPACITORS; CAPACITORS, RECTIFIERS, DETECTORS, SWITCHING DEVICES, LIGHT-SENSITIVE OR TEMPERATURE-SENSITIVE DEVICES OF THE ELECTROLYTIC TYPE
- H01G11/00—Hybrid capacitors, i.e. capacitors having different positive and negative electrodes; Electric double-layer [EDL] capacitors; Processes for the manufacture thereof or of parts thereof
- H01G11/04—Hybrid capacitors
- H01G11/06—Hybrid capacitors with one of the electrodes allowing ions to be reversibly doped thereinto, e.g. lithium ion capacitors [LIC]
-
- H—ELECTRICITY
- H01—ELECTRIC ELEMENTS
- H01G—CAPACITORS; CAPACITORS, RECTIFIERS, DETECTORS, SWITCHING DEVICES, LIGHT-SENSITIVE OR TEMPERATURE-SENSITIVE DEVICES OF THE ELECTROLYTIC TYPE
- H01G11/00—Hybrid capacitors, i.e. capacitors having different positive and negative electrodes; Electric double-layer [EDL] capacitors; Processes for the manufacture thereof or of parts thereof
- H01G11/74—Terminals, e.g. extensions of current collectors
-
- H—ELECTRICITY
- H01—ELECTRIC ELEMENTS
- H01G—CAPACITORS; CAPACITORS, RECTIFIERS, DETECTORS, SWITCHING DEVICES, LIGHT-SENSITIVE OR TEMPERATURE-SENSITIVE DEVICES OF THE ELECTROLYTIC TYPE
- H01G11/00—Hybrid capacitors, i.e. capacitors having different positive and negative electrodes; Electric double-layer [EDL] capacitors; Processes for the manufacture thereof or of parts thereof
- H01G11/78—Cases; Housings; Encapsulations; Mountings
-
- H—ELECTRICITY
- H01—ELECTRIC ELEMENTS
- H01G—CAPACITORS; CAPACITORS, RECTIFIERS, DETECTORS, SWITCHING DEVICES, LIGHT-SENSITIVE OR TEMPERATURE-SENSITIVE DEVICES OF THE ELECTROLYTIC TYPE
- H01G11/00—Hybrid capacitors, i.e. capacitors having different positive and negative electrodes; Electric double-layer [EDL] capacitors; Processes for the manufacture thereof or of parts thereof
- H01G11/78—Cases; Housings; Encapsulations; Mountings
- H01G11/80—Gaskets; Sealings
-
- H—ELECTRICITY
- H01—ELECTRIC ELEMENTS
- H01M—PROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
- 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
-
- 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
- H01M50/10—Primary casings; Jackets or wrappings
- H01M50/183—Sealing members
-
- 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
- H01M50/50—Current conducting connections for cells or batteries
- H01M50/543—Terminals
-
- 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
- H01M50/50—Current conducting connections for cells or batteries
- H01M50/543—Terminals
- H01M50/552—Terminals characterised by their shape
- H01M50/553—Terminals adapted for prismatic, pouch or rectangular cells
- H01M50/557—Plate-shaped terminals
-
- 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
Definitions
- the present invention relates to a film for tab lead thermally fused to a tab lead for extracting electricity from the inside in a lithium ion battery, a lithium ion capacitor or the like using a laminate film as an outer packaging material.
- the present invention also relates to a tab lead using the tab lead film.
- lithium batteries etc. lithium ion batteries and lithium ion capacitors
- a laminate film in which a sealant layer made of polyolefin or the like is laminated on metal foil such as aluminum foil as an outer wrapping material, and inside the outer wrapping material, a positive electrode, a negative electrode, a separator, a non-aqueous electrolyte, etc.
- a tab lead for electrically connecting the inside and the outside of the lithium battery etc. is attached.
- Patent Document 1 discloses that the metal terminal (lead wire) is corroded by hydrogen fluoride (hydrofluoric acid) generated by the entry of water, and the film for tab lead (insulation material for lead wire) is prevented from peeling off. It is proposed to add an acid trapping function to a tab lead film.
- the main components are 100 parts by weight of a thermoplastic resin and one or more selected from carboxylic acid metal salts, metal oxides, and hydrotalcites in a total of 20 parts by weight or more and 100 parts by weight or less. It is proposed to use the resin composition to be used as a film for tab lead.
- the film for tab lead disclosed herein is a single layer film, and a large amount of filler (metal carboxylate, metal oxide, hydrotalcites, etc.) is present on the film surface. Therefore, the filler may fall off from the film surface, which may contaminate the production line of the tab lead and the production line such as a lithium battery.
- the filler may fall off from the film surface, which may contaminate the production line of the tab lead and the production line such as a lithium battery.
- the adhesion between the metal terminal and the film for tab lead is lowered.
- the tab lead film is heat-sealed to the metal terminal by heat sealing, but the filler does not melt even at the heat seal temperature (usually 150 to 250 ° C.) and does not heat-seal to the metal terminal.
- Patent document 2 is also invention which solves the problem that the metal terminal (lead terminal) is corroded by hydrogen fluoride, and the adhesive force between a metal terminal and the film for tab leads (tape for terminal adhesion) falls.
- a film for tab lead is made to have a three-layer structure, a layer containing an inorganic filler is used as an intermediate layer, one of the intermediate layers is a resin layer having good adhesion to metal terminals, and the other is an outer packaging material.
- Patent Document 2 It is disclosed to provide a resin layer with good adhesion to The three-layered tab lead film disclosed in Patent Document 2 does not contaminate a production line for a tab lead or a production line for a lithium battery or the like because there is no inorganic filler on the film surface. However, even in the case of the three-layered tab lead film, depending on the type of the metal terminal, the adhesive strength to the terminal is low.
- FIG. 9 is a schematic plan view (A) of a tab lead TL adopting a relatively thick metal terminal 2, its ⁇ - ⁇ sectional view (B), and its ⁇ - ⁇ sectional view (C).
- the present inventors often heat-seal the tab lead film 1 having a general three-layer structure to the relatively thick metal terminal 2, often breaking the surface layer 11 of the tab lead film 1 at the corner 2a of the metal terminal 2. It was discovered that the metal terminal 2 was in contact with the core layer 12.
- the core layer 12 Since the surface layer 11 of the general film 1 for tab lead is made of acid-modified polyolefin and the core layer 12 is made of a polyolefin resin, the core layer 12 usually has heat fusion with the metal terminal 2 more than the surface layer 11 It is inferior.
- a film containing an inorganic filler in the core layer such as a film for tab lead disclosed in Patent Document 2 has very poor heat fusion between the core layer and the metal terminal due to the influence of the inorganic filler. Therefore, the three-layered tab lead film disclosed in Patent Document 2 is not heat-sealed to the terminal at the corner of the metal terminal, and as a result, the adhesion between the metal terminal and the tab lead film is considered to be reduced.
- the present inventors made the thickness or thickness ratio of one surface layer (A) of the film for tab lead sufficiently large, and that the surface layer (A) of the film for tab lead is broken at the corner of the metal terminal. I decided to prevent it.
- the thickness or thickness ratio of the surface layer (A) increases, the thickness of the core layer (B) or the other surface layer (C) decreases, but the core layer (B) As the thickness of the layer decreases, the amount of inorganic filler contained in the layer also decreases. Therefore, the present inventors have further studied the addition amount of the inorganic filler and the influence on the hydrogen fluoride, and reached the present invention.
- Tab lead having a core layer (B) mainly composed of an inorganic filler reacting with hydrogen and / or the polyolefin resin, and a surface layer (C) mainly composed of an acid-modified polyolefin resin and / or a polyolefin resin
- the content of the inorganic filler in the surface layer (A) and the content of the inorganic filler in the surface layer (C) are each 0 to 10% by weight
- the film for tab lead is hydrogen fluoride.
- a film for tab lead characterized by containing 9.0% by weight or more of an inorganic filler which reacts with.
- the film for a tab lead contains 9.6% by weight or more of an inorganic filler which reacts with hydrogen fluoride.
- the median diameter of the inorganic filler which reacts with the hydrogen fluoride in the said film for tab leads is 1.0 micrometer or less.
- a film for tab lead wherein the content of the inorganic filler that reacts with the hydrogen fluoride in the core layer is 13 to 60% by weight. Furthermore, when the thickness of the surface layer (A) is t1, the thickness of the core layer (B) is t2, and the thickness of the surface layer (C) is t3, the following equation (1) and equation (1) A film for tab lead characterized by satisfying 2) is provided.
- the inorganic filler which reacts with the hydrogen fluoride is a metal carbonate.
- the metal carbonate is calcium carbonate.
- the calcium carbonate is a synthetic calcium carbonate.
- the tab lead film is heat-sealed on at least one surface of the metal terminal, and the surface of the metal terminal and the surface layer (A) of the tab lead film are heat-sealed.
- a featured tab lead is provided. Furthermore, when the thickness of the metal terminal is T (mt) and the thickness of the tab lead film is T (tf), the tab lead is characterized by 0.5 T (mt) ⁇ T (tf). Provided.
- the film for tab lead according to the present invention comprises a surface layer (A) containing an acid-modified polyolefin resin as a main component, an inorganic filler that reacts with hydrogen fluoride, and / or a core layer (B) containing a polyolefin resin as a main component
- Content of the inorganic filler in the surface layer (A) and the content of the inorganic filler in the surface layer (C) are sequentially provided with the surface layer (C) mainly composed of the acid-modified polyolefin resin and / or the polyolefin resin Since each of the amounts is 0 to 10% by weight, it does not contaminate the production line for tab leads and production lines for lithium batteries and the like.
- the film contains at least 9.0% by weight of an inorganic filler that reacts with hydrogen fluoride, even if hydrogen fluoride is generated from the inside of the battery, it is caused by the corrosion or corrosion of the metal terminal by the hydrogen fluoride. Can be efficiently suppressed.
- the film contains 9.6% by weight or more of an inorganic filler that reacts with hydrogen fluoride, it is possible to further suppress the decrease in the adhesion between the tab lead film and the metal terminal due to the hydrogen fluoride.
- the median diameter of the inorganic filler that reacts with hydrogen fluoride is 1.0 ⁇ m or less, it is suitable for suppressing the decrease in adhesion due to the hydrogen fluoride.
- the resin layer breaks off at the corner of the terminal when heat-sealed with the metal terminal. Is suppressed.
- the content of the inorganic filler that reacts with hydrogen fluoride in the core layer is 13 to 60% by weight, the corrosion of the metal terminal due to the hydrogen fluoride can be effectively suppressed, and the film forming property of the film for tab lead Also stable.
- the inorganic filler that reacts with hydrogen fluoride is a metal carbonate, the decrease in adhesion due to hydrogen fluoride can be particularly suppressed without using an expensive filler.
- FIG. 1 is a schematic plan view (A) of a tab lead according to the present invention, an ⁇ - ⁇ sectional view (B) thereof, and a ⁇ - ⁇ sectional view (C) thereof.
- 7 is a photograph of a digital microscope of the tab lead cross section of Test Example 1; 7 is a photograph of a digital microscope of the tab lead cross section of Test Example 2.
- FIG. 7 is a photograph of a digital microscope of the tab lead cross section of Test Example 3.
- FIG. 21 is a photograph of a digital microscope of the tab lead cross section of Test Example 4.
- FIG. 21 is a photograph of a digital microscope of the tab lead cross section of Test Example 5.
- FIG. 1 is a schematic plan view (A) of a tab lead according to the present invention, an ⁇ - ⁇ sectional view (B) thereof, and a ⁇ - ⁇ sectional view (C) thereof.
- FIG. 1 is a schematic cross-sectional view of a tablead film 1 of the present invention.
- the tab lead film 1 of the present invention comprises a surface layer (A) 11, a core layer (B) 12 and a surface layer (C) 13 in this order.
- the surface layer (A) 11 is a layer in contact with a metal terminal in a tab lead described later, and is mainly composed of an acid-modified polyolefin excellent in metal adhesiveness.
- the acid-modified polyolefin is not particularly limited as long as it is an acid-modified polyolefin, but a polyolefin grafted and modified with an unsaturated carboxylic acid or an anhydride thereof is preferably used.
- polyethylene such as low density polyethylene, medium density polyethylene, high density polyethylene, linear low density polyethylene, homopolypropylene, block copolymer of propylene and ethylene, polypropylene such as random copolymer of propylene and ethylene
- polyethylene and polypropylene are preferably used.
- unsaturated carboxylic acid or its anhydride used for the acid modification of polyolefin maleic acid, acrylic acid, itaconic acid, crotonic acid, maleic anhydride, itaconic anhydride etc. are mentioned, for example.
- the surface layer (A) 11 may contain one or more of acid-modified polyolefins as appropriate, and may contain other resins such as non-modified polyolefins and thermoplastic elastomers as long as it is a main component.
- the "main component” means the component having the largest weight ratio among the components constituting the layer.
- the surface layer (A) 11 has an inorganic filler content of 10% by weight or less. If the content of the inorganic filler exceeds 10% by weight, the adhesion between the tab lead film and the metal terminal may be reduced. In addition, there is a risk that the inorganic filler may fall off in the step of producing the tab lead, and contaminate the production line.
- the amount of the inorganic filler in the surface layer (A) 11 is preferably 5% by weight or less, preferably 3% by weight or less, and particularly preferably 1% by weight or less. In addition, as an inorganic filler, it does not restrict to the inorganic filler which reacts with the hydrogen fluoride mentioned later, An anti blocking agent etc. are also contained in an inorganic filler.
- the thickness t1 of the surface layer (A) 11 is preferably 23 ⁇ m or more, particularly 27 ⁇ m or more, and further preferably 30 ⁇ m or more. If the thickness t1 of the surface layer (A) 11 is less than 23 ⁇ m, the surface layer (A) 11 may be broken at the corners of the metal terminal, and the metal terminal may be in contact with the core layer of the tab lead film.
- the ratio of the thickness t1 of the surface layer (A) 11 in the entire tab lead film is 23% or more of the thickness T (tf) of the entire tab lead film 1 (t1 T 0.23 T (tf)), 80%
- the following (t1 ⁇ 0.8 T (tf)) is preferable.
- the upper limit value of 75%, 70%, 65%, 60%, 55% or 50% is preferred.
- the thickness T (tf) of the tab lead film 1 and the thickness T (mt) of the metal terminal are almost equal.
- the thickness t1 of the surface layer (A) 11 is If it is less than 23% of the thickness T (tf) of the film 1, as described above, the surface layer (A) 11 is broken at the corners of the metal terminal, and the metal terminal is the core layer (B) of the tab lead film 1 There is a risk of contact with 12.
- the thickness t1 of the surface layer (A) 11 exceeds 80% of the film 1, the core layer (B) 12 becomes too thin and can not contain sufficient inorganic filler, or the other surface layer ( C) 13 may be too thin, and the adhesion to the outer packaging material such as a lithium battery may be reduced.
- the core layer (B) 12 in the tab lead film 1 of the present invention is composed of an inorganic filler that reacts with hydrogen fluoride and a polyolefin resin, and one or both of them are main components.
- the inorganic filler that reacts with hydrogen fluoride is not particularly limited, but it is particularly preferable to be an inorganic filler that reacts with hydrogen fluoride having a median diameter of 1.0 ⁇ m or less.
- the inorganic filler that reacts with hydrogen fluoride having a median diameter of 1.0 ⁇ m or less has the same amount of inorganic filler for tabled as compared to the inorganic filler that reacts with hydrogen fluoride having a median diameter of more than 1.0 ⁇ m.
- the adhesive fall by hydrogen fluoride can be controlled more.
- the inorganic filler that reacts with hydrogen fluoride having a median diameter of 1.0 ⁇ m or less has a median diameter of greater than 1.0 ⁇ m when the decrease in adhesion (adhesion retention) due to hydrogen fluoride is made to the same extent.
- the amount to be contained in the tab lead film can be smaller than that of the inorganic filler that reacts with hydrogen fluoride.
- the lower limit value of the median diameter is preferably 0.05 ⁇ m, 0.1 ⁇ m or 0.2 ⁇ m, because it is difficult to produce an inorganic filler that reacts with hydrogen fluoride to a very small diameter.
- the upper limit value of the median diameter is particularly preferably 0.8 ⁇ m, 0.6 ⁇ m or 0.5 ⁇ m from the viewpoint of being able to further suppress the decrease in adhesiveness due to hydrogen fluoride.
- metal carbonates such as calcium carbonate and magnesium carbonate
- calcium carbonate is preferably used because it is inexpensive and easy to obtain.
- synthetic calcium carbonate is excellent in the function of catching hydrogen fluoride and can be suitably used.
- the synthetic calcium carbonate can be produced, for example, by reacting calcium hydroxide with carbon dioxide gas, and it is possible to produce particles having a particle size (median diameter) smaller than that of ground calcium carbonate.
- the polyolefin-based resin used for the core layer (B) 12 is not particularly limited, but, for example, polyethylene such as low density polyethylene, medium density polyethylene, high density polyethylene, linear low density polyethylene, homopolypropylene, propylene and the like
- polyethylene such as low density polyethylene, medium density polyethylene, high density polyethylene, linear low density polyethylene, homopolypropylene, propylene and the like
- a block copolymer of ethylene, a polypropylene such as a random copolymer of propylene and ethylene, a terpolymer of ethylene-butene-propylene, and the like can be used.
- polyethylene and polypropylene are preferably used. One or more of these may be selected to form a polyolefin resin that forms the core layer (B) 12.
- the core layer (B) 12 may contain, in addition to the above-mentioned polyolefin resin, another resin such as a thermoplastic elastomer, a colorant and the like.
- another resin such as a thermoplastic elastomer, a colorant and the like.
- an acid-modified resin such as an acid-modified polyolefin is contained, the hydrophilicity is increased, the water resistance is decreased, and the generation of hydrogen fluoride may be promoted.
- the content of the inorganic filler that reacts with the hydrogen fluoride blended in the core layer (B) 12 is preferably 13 to 60% by weight.
- the content of the inorganic filler in the core layer (B) 12 is less than 13% by weight, the content of the inorganic filler in the film for tab lead 1 is 9 while the film thickness of the surface layer (A) is 23% or more.
- the thickness t2 of the core layer (B) 12 is preferably 15 to 72%, more preferably 20 to 60%, and further preferably 25 to 50% of the thickness T (tf) of the entire film.
- the tablead film 1 is blended with an inorganic filler that reacts with hydrogen fluoride of 9.0 wt% or more It becomes difficult.
- the thickness t2 of the core layer (B) 12 exceeds 72% of the total film thickness T (tf), the thicknesses of the surface layer (A) 11 and the surface layer (C) 13 become too thin, and There is a fear that the function can not be exhibited.
- the surface layer (C) 13 is a layer to be the outermost layer (surface layer not in contact with metal terminals) in a tab lead described later, and is a layer thermally fused with a laminate film which is an outer packaging material in a lithium battery or the like.
- the surface layer (C) 13 contains an acid-modified polyolefin resin and / or a polyolefin resin as a main component.
- the sealant layer of the laminate film is made of a resin having poor adhesion to the film for tab lead, it is recommended to select an acid-modified polyolefin resin as the main component of the surface layer (C) 13, and the sealant layer of the laminate film is adhesive When rich, it is good to select polyolefin resin as a main component of surface layer (C) 13.
- the acid-modified polyolefin resin a resin similar to the resin exemplified as the main component of the surface layer (A) 11 can be appropriately adopted, and the polyolefin resin is the resin exemplified in the core layer (B) 12 Similar resins can be employed.
- the thickness t3 of the surface layer (C) 13 is preferably 5 ⁇ m or more. If the thickness is less than 5 ⁇ m, thickness control in film formation is difficult, and adhesion to the sealant layer of the laminate film may be insufficient. Further, the ratio of the thickness t3 of the surface layer (C) 13 in the entire tab lead film 1 is preferably 5 to 62% of the thickness T (tf) of the entire film, in particular 10 to 50%, more preferably It is preferably 15 to 30%. If the thickness t3 of the surface layer (C) 13 is less than 5% of the thickness T (tf) of the entire film, the adhesion of the laminate film to the sealant layer may be insufficient.
- the surface layer (C) 13 has an inorganic filler content of 10% by weight or less. If the content of the inorganic filler exceeds 10% by weight, the adhesion between the tab lead film 1 and the laminate film may be reduced. In addition, there is a risk that the inorganic filler may fall off in the step of manufacturing a tab lead or the step of manufacturing a lithium battery or the like to contaminate the manufacturing line.
- the amount of the inorganic filler in the surface layer (C) 13 is preferably 5% by weight or less, preferably 3% by weight or less, and particularly preferably 1% by weight or less.
- the tab lead film 1 is a three-layer film of surface layer (A) 11 / core layer 12 (B) / surface layer (C) 13 has been described, but the film 1 has the effect of the present invention. May contain other resin layers.
- FIG. 2 is a plan view (A) of the tab lead TL of the present invention and its ⁇ - ⁇ sectional view (B).
- the tab lead TL of the present invention comprises the tab lead film 1 and the metal terminal 2 of the present invention.
- the metal terminal 2 is a member electrically connected to an electrode (positive electrode or negative electrode) of a lithium battery or the like, and is made of a metal material. It does not restrict
- the metal terminal connected to the positive electrode of a lithium battery or the like is usually made of aluminum or the like.
- the metal terminal connected to the negative electrode of a lithium battery or the like is usually made of copper, nickel or the like.
- the surface of the metal terminal 2 is preferably subjected to a chemical conversion treatment from the viewpoint of enhancing the electrolytic solution resistance. For example, when the metal terminal is formed of aluminum, specific examples of the chemical conversion treatment include known methods for forming an acid-resistant film such as phosphate, chromate, fluoride, triazine thiol compound and the like.
- the size of the metal terminal 2 may be appropriately set according to the size of the battery to be used.
- the thickness T (mt) of the metal terminal 2 is preferably 50 ⁇ m to 400 ⁇ m, more preferably 100 ⁇ m to 300 ⁇ m.
- the length of the metal terminal 2 is preferably 1 mm or more and 200 mm or less, more preferably 3 mm or more and 150 mm or less.
- variety of the metal terminal 2 Preferably 1 mm or more and 200 mm or less, More preferably, 3 mm or more and 150 mm or less are mentioned.
- the present invention exhibits its effect particularly when using the metal terminal 2 which is not chamfered.
- the resin composition, thickness, and thickness ratio of each layer constituting the tab lead film 1 are as described above.
- the total thickness T (tf) of the tab lead film 1 is not particularly limited, but it is desirable to determine the thickness of the metal terminal 2 determined by the size of the battery or the like based on T (mt). Specifically, it is preferable that 0.5T (mt) ⁇ T (tf), and particularly preferably 0.7T (mt) ⁇ T (tf), and further, 0.8T (mt) ⁇ T (tf). Is desirable.
- the film 1 for tab lead 1 When the thickness T (tf) of the film for tab lead 1 is less than 0.5 times the thickness T (mt) of the metal terminal 2, the film 1 for tab lead is attached to the side portion 2b of the metal terminal 2 There is a possibility that the tab lead film 1 may be lifted from the terminal 2 at the side portion 2 b without turning around. If the thickness T (tf) of the tab lead film 1 is sufficiently thicker than the thickness T (mt) of the metal terminal 2, the problem of the tab lead film 1 rising from the metal terminal 2 is eliminated, but lithium When heat-sealed to an outer packaging material such as a battery, the outer packaging material may be lifted from the tab lead film 1 on the side portion 1 a of the tab lead film 1.
- the thickness T (tf) of the tab lead film 1 is preferably 400 ⁇ m or less, particularly 200 ⁇ m or less, and more preferably 150 ⁇ m or less.
- the thickness T (tf) of the film for tab lead 1 is 50 ⁇ m or more, in particular 70 ⁇ m or more, and further 75 ⁇ m or more preferable.
- a film for tab lead was prepared in which the core layer (B) was colored in gray.
- a film for tablead having a three-layer structure in which the surface layer (A) is made of acid-modified polypropylene, the core layer (B) is made of polypropylene and a colorant (gray pigment), and the surface layer (C) is made of polypropylene 100 ⁇ m thick).
- the film was produced by coextrusion molding. The thickness of each layer was 50 ⁇ m for the surface layer (A), 30 ⁇ m for the core layer (B), and 20 ⁇ m for the surface layer (C).
- the tab lead using the tab lead film of Test Examples 1, 2, 4, and 5 in which the thickness of the surface layer (A) is 23% or more of the thickness of the tab lead film is also acid-modified even at the corner of the metal terminal The surface layer (A) made of polypropylene was in contact with the metal terminal. Particularly in the tab lead of Test Example 1 in which the thickness of the surface layer (A) was 50%, the surface layer (A) was hardly thinned. On the other hand, in the tab lead of Test Example 3 in which the thickness of the surface layer (A) was 20% of the whole, the corner portions of the metal terminals were in contact with the core layer (B).
- the core layer (B) contains polypropylene as a main component and therefore has poor adhesion.
- a film for tab lead of 15 mm in width is heat sealed on both sides of a nickel foil of 100 ⁇ m in thickness and 20 mm in width to form a test piece.
- the tab lead film is disposed such that the surface layer (A) is in contact with the nickel foil.
- the heat sealing was performed under the conditions of seal bar temperature of 190 ° C. for upper bar, 220 ° C. for lower bar, seal surface pressure of 1.0 MPa, and seal time of 3 seconds.
- the test piece immediately after sealing and the test piece after immersion in the electrolyte for 2 hours were each peeled 180 °, and the adhesive strength (peel strength) was measured with a tensile tester (Autograph / Shimadzu Corporation). Do.
- the tensile rate of the tensile tester is 100 mm / min, the measuring atmosphere is 23 ° C., the humidity is 50% RH, and the tab lead film heat-sealed on the upper bar side is peeled off. From the data obtained by the measurement, the adhesive retention ((“adhesive strength after immersion in an electrolyte solution for 2 hours” / “adhesive strength immediately after sealing”) ⁇ 100) was calculated.
- the median diameter of calcium carbonate to be used is measured using a laser diffraction particle size distribution measuring device, and particle sizes corresponding to 10%, 50% and 90% in the cumulative distribution curve of particle size based on particle size are calculated, The particle diameter (median diameter (D50)) to be 50% was determined.
- the tab lead films of Examples 1 to 4 hold 50% or more of the adhesion retention rate. This seems to be because calcium carbonate (CaCO 3 ) contained in the film for tab lead reacts with hydrogen fluoride (HF) and the hydrogen fluoride is confined in the film for tab lead in the form of calcium fluoride (CaF 2 ) .
- CaCO 3 calcium carbonate contained in the film for tab lead reacts with hydrogen fluoride (HF) and the hydrogen fluoride is confined in the film for tab lead in the form of calcium fluoride (CaF 2 ) .
- the films for tab lead of Comparative Examples 1 to 3 had good initial adhesion, but the adhesion strength after immersion for 2 hours was extremely low. This is considered to be because the nickel foil surface was corroded by hydrogen fluoride contained in the electrolytic solution.
- the relationship between the amount of added calcium carbonate and the adhesion retention rate in the films for tab lead of Examples 1 to 4 and Comparative Examples 1 to 3 is shown in FIG.
- the adhesive strength is 0 even if the addition amount is increased, and the tab lead film peels off from the metal terminal.
- the adhesion retention rate increased as the addition amount increased, but the adhesion retention rate was less than 50%.
- the adhesion retention rate increased as the addition amount increased, and the adhesion retention rate also exceeded 50%.
- the addition amount exceeds 11.5% by weight the adhesion retention does not change so much in the state of 80%.
- Example 5 A film for tab lead similar to that of Example 4 was produced except that another calcium carbonate (CaCO 3 -3) was used from calcium carbonate (CaCO 3 -2) used in Example 4, and the adhesive strength immediately after sealing and The adhesive strength after immersion in the electrolytic solution for 2 hours was measured to calculate the adhesive retention.
- Table 3 shows the comparison between calcium carbonate (CaCO 3 -2) used in Example 4 and calcium carbonate (CaCO 3 -3) obtained in Example 5. The measurement results of Example 5 are shown in Table 4.
- the relationship between the amount of added calcium carbonate and the adhesion retention rate in the film for tab lead of Example 5 is added to FIG.
- the film for tab lead according to Example 1 using calcium carbonate having a smaller median diameter than Example 5 using calcium carbonate having a large median diameter could be as small as two thirds.
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Abstract
Description
また該充填剤がフィルム表面に多く存在すると、金属端子とタブリード用フィルムの接着力が低下するという問題もあった。通常、タブリード用フィルムは金属端子にヒートシールにより熱融着するが、前記充填剤はヒートシール温度(通常、150~250℃)においても溶融せず、金属端子と熱融着しないのである。
特許文献2には、タブリード用フィルムを三層構成とし、無機充填剤を含有する層を中間層とし、該中間層の一方に金属端子との接着性が良好な樹脂層を、他方に外包材との接着性が良好な樹脂層を設けることが開示されている。
特許文献2に開示された三層構成のタブリード用フィルムは、フィルム表面に無機充填剤が存在しない為、タブリードの製造ラインやリチウム電池等の製造ラインを汚染することはない。しかしながら該三層構成のタブリード用フィルムであっても、金属端子の種類によっては、端子との接着力が低いものがあった。
一般的なタブリード用フィルム1の表面層11は酸変性ポリオレフィンから成り、コア層12はポリオレフィン系樹脂から成る為、通常、コア層12は表面層11よりも金属端子2との熱融着性に劣る。特に特許文献2に開示されたタブリード用フィルムのようにコア層に無機充填剤を含むものは、該無機充填剤の影響により、コア層と金属端子との熱融着性は非常に乏しい。そのため特許文献2に開示された三層のタブリード用フィルムは、金属端子の角部において端子に熱融着せず、その結果、金属端子とタブリード用フィルムとの接着力が低下したものと思われる。
また、前記タブリード用フィルムがフッ化水素と反応する無機充填剤を9.6重量%以上含有することを特徴とするタブリード用フィルムが提供される。
更に、前記タブリード用フィルム中のフッ化水素と反応する無機充填剤のメジアン径が1.0μm以下であることを特徴とするタブリード用フィルムが提供される。
また、前記表面層(A)の厚さが23μm以上であることを特徴とするタブリード用フィルムが提供される。
更に、前記表面層(A)の厚さがタブリードフィルム全体の厚さの23%以上であることを特徴とするタブリード用フィルムが提供される。
更に、前記表面層(A)の厚さをt1、前記コア層(B)の厚さをt2、前記表面層(C)の厚さをt3としたとき、下記の式(1)及び式(2)を満たすことを特徴とするタブリード用フィルムが提供される。
式(1) t1≧t3
式(2) t1:t2:t3=23~80:15~72:5~62
また、前記フッ化水素と反応する無機充填剤が金属炭酸塩であることを特徴とするタブリード用フィルムが提供される。
更に、前記金属炭酸塩が、炭酸カルシウムであることを特徴とするタブリード用フィルムが提供される。
また、前記炭酸カルシウムが、合成炭酸カルシウムであることを特徴とするタブリード用フィルムが提供される。
更に、前記金属端子の厚さをT(mt)、前記タブリード用フィルムの厚さをT(tf)としたとき、0.5T(mt)≦T(tf)であることを特徴とするタブリードが提供される。
また該フィルムがフッ化水素と反応する無機充填剤を9.0重量%以上含有する為、電池内部からフッ化水素が発生しても、該フッ化水素による金属端子の腐食や、腐食に起因する接着性の低下を効率よく抑制することができる。
加えて、該フィルムがフッ化水素と反応する無機充填剤を9.6重量%以上含有することで、フッ化水素によるタブリード用フィルムと金属端子の接着力低下をより抑制することができる。
特に、フッ化水素と反応する無機充填剤のメジアン径が1.0μm以下であることによりフッ化水素による接着性低下の抑制に適している。
またコア層におけるフッ化水素と反応する無機充填剤の含有量が13~60重量%であると、フッ化水素による金属端子の腐食を効果的に抑制でき、尚且つタブリード用フィルムの製膜性も安定する。
更にまたフッ化水素と反応する無機充填剤が金属炭酸塩であると、高価な充填剤を用いることなく、フッ化水素による接着性の低下を特に抑制することができる。
[表面層(A)]
表面層(A)11は、後述するタブリードにおいて金属端子と接する層で、金属接着性に優れる酸変性ポリオレフィンを主成分とする。該酸変性ポリオレフィンは、酸変性されたポリオレフィンであれば特に制限されないが、不飽和カルボン酸又はその無水物でグラフト変性されたポリオレフィンが好適に用いられる。
またポリオレフィンの酸変性に使用される不飽和カルボン酸又はその無水物としては、例えば、マレイン酸、アクリル酸、イタコン酸、クロトン酸、無水マレイン酸、無水イタコン酸等が挙げられる。
表面層(A)11は酸変性ポリオレフィンの一種或いはそれ以上を適宜選択し、これを主成分としていれば、変性されていないポリオレフィンや熱可塑性エラストマー等の他の樹脂を含んでいても良い。尚、本発明において「主成分」とは層を構成する成分のうち最も重量割合が大きい成分を意味する。
尚、無機充填剤としては、後述するフッ化水素と反応する無機充填剤に限るものではなく、アンチブロッキング剤なども無機充填剤に含まれる。
本発明のタブリード用フィルム1におけるコア層(B)12は、フッ化水素と反応する無機充填剤とポリオレフィン系樹脂からなり、これらのうちのいずれか一方、若しくは双方を主成分とする。
フッ化水素と反応する無機充填剤は特に限定されるものではないが、特に、メジアン径が1.0μm以下のフッ化水素と反応する無機充填剤であることが好ましい。メジアン径が1.0μm以下のフッ化水素と反応する無機充填剤は、メジアン径が1.0μmを超えるフッ化水素と反応する無機充填剤と比較して、同量の無機充填剤をタブリード用フィルムに含有させた場合に、フッ化水素による接着性低下をより抑制することができる。換言すれば、フッ化水素による接着性低下(接着性保持率)を同程度する際、メジアン径が1.0μm以下のフッ化水素と反応する無機充填剤は、メジアン径が1.0μmを超えるフッ化水素と反応する無機充填剤よりも、タブリード用フィルムに含有させる量を少量とすることができる。このように、タブリード用フィルム中の含有量を少量にすることができることで、無機充填剤による製造時の不具合(押出工程での樹脂圧変動やスクリュー摩耗など)をより抑制することができる。
尚、フッ化水素と反応する無機充填剤は、極めて小径に製造することが困難であることから、メジアン径の下限値は0.05μm、0.1μmまたは0.2μmであることが好ましい。また、メジアン径の上限値は、0.8μm、0.6μmまたは0.5μmであることがフッ化水素による接着性低下をより抑制することができる点から特に好ましい。
尚、該コア層(B)12は上述したポリオレフィン系樹脂の他に、熱可塑性エラストマー等の他の樹脂や着色剤等を含んでいても良い。しかしながら酸変性ポリオレフィンのような酸変性樹脂を含んでいると、親水性が高まり、耐水性が低下し、フッ化水素の発生を促進させる恐れがある。
コア層(B)12における該無機充填剤の含有量が13重量%未満では、表面層(A)の膜厚を23%以上としながら、タブリード用フィルム1における該無機充填剤の含有量を9.0重量%以上とすることが困難となり、表面層(C)13を薄くしたり、表面層(A)11や表面層(C)13に該無機充填剤を添加したりする必要が生じる。
またコア層(B)12における該無機充填剤の含有量が60重量%を超えると、コア層(B)12用の樹脂組成物を押出機から押出す際に樹脂圧が変動し易く、該層の厚さが安定し難い。また無機充填剤によって押出機のスクリューが摩耗し、タブリード用フィルムに金属粉が混入する恐れが生じる。
表面層(C)13は、後述するタブリードにおいて最表層(金属端子と接しない表面層)となる層であって、リチウム電池等において外包材であるラミネートフィルムと熱融着される層である。該表面層(C)13は酸変性ポリオレフィン系樹脂及び/又はポリオレフィン系樹脂を主成分とする。ラミネートフィルムのシーラント層が、タブリード用フィルムとの接着性に乏しい樹脂から成る場合、表面層(C)13の主成分として酸変性ポリオレフィン系樹脂を選択するとよく、ラミネートフィルムのシーラント層が接着性に富む場合は、表面層(C)13の主成分としてポリオレフィン系樹脂を選択するとよい。
尚、酸変性ポリオレフィン系樹脂は、表面層(A)11の主成分として例示した樹脂と同様の樹脂を適宜採用することができ、ポリオレフィン系樹脂は、コア層(B)12において例示した樹脂と同様の樹脂を採用することができる。
また、タブリード用フィルム1全体における表面層(C)13の厚さt3の割合は、フィルム全体の厚さT(tf)の5~62%であることが好ましく、特に10~50%、更には15~30%であることが好ましい。表面層(C)13の厚さt3がフィルム全体の厚さT(tf)の5%未満では、ラミネートフィルムのシーラント層との接着が不十分となる恐れがある。また表面層(C)13の厚さt3がフィルム全体の厚さT(tf)の62%を超えると、表面層(A)11やコア層(B)12の厚さが薄くなり過ぎ、各層の機能を発揮できない恐れが生じる。
図2は本発明のタブリードTLの平面図(A)とそのα―α断面図(B)である。
本発明のタブリードTLは、本発明のタブリード用フィルム1と金属端子2とからなる。
金属端子2は、リチウム電池等の電極(正極又は負極)に電気的に接続される部材であり、金属材料により構成されている。金属端子2を構成する金属材料としては、特に制限されず、例えば、アルミニウム、ニッケル、銅等が挙げられる。尚、リチウム電池等の正極に接続される金属端子は、通常、アルミニウム等により構成されている。また、リチウム電池等の負極に接続される金属端子は、通常、銅、ニッケル等により構成されている。
金属端子2の表面は、耐電解液性を高める観点から、化成処理が施されていることが好ましい。例えば、金属端子がアルミニウムにより形成されている場合、化成処理の具体例としては、リン酸塩、クロム酸塩、フッ化物、トリアジンチオール化合物等の耐酸性被膜を形成する公知の方法が挙げられる。
尚、本発明のタブリード用フィルム1を用いれば、金属端子2が角部2aにおいて面取りされていないものであっても、該角部2aにおいて表面層(A)11が途切れにくい。よって本発明は面取りされていない金属端子2を用いる場合に、特にその効果を発揮する。
タブリード用フィルム1を構成する各層の樹脂組成や厚さ、厚さの比率は上述した通りである。
タブリード用フィルム1の全体の厚さT(tf)は特に限定されないが、電池の大きさ等により決定される金属端子2の厚さをT(mt)に基づき決定することが望ましい。詳しくは、0.5T(mt)≦T(tf)であることが望ましく、特に0.7T(mt)≦T(tf)であることが望ましく、更には0.8T(mt)≦T(tf)であることが望ましい。タブリード用フィルム1の厚さT(tf)が金属端子2の厚さT(mt)の0.5倍未満では、熱融着する際にタブリード用フィルム1が金属端子2の側辺部2bに回り込まず、該側辺部2bにおいてタブリード用フィルム1が端子2から浮き上がる恐れがある。
尚、タブリード用フィルム1の厚さT(tf)が、金属端子2の厚さT(mt)よりも十分に厚いと、金属端子2からタブリード用フィルム1が浮き上がる問題は解消されるが、リチウム電池等の外包材に熱融着される際に、タブリード用フィルム1の側辺部1aにおいて、外包材がタブリード用フィルム1から浮き上がる恐れがある。よってタブリード用フィルム1の厚さT(tf)は400μm以下、特に200μm以下、更には150μm以下であることが好ましい。
また、金属端子2及びラミネートフィルムのシーラント層との接着を十分保つためには、タブリード用フィルム1の厚さT(tf)は50μm以上、特に、70μm以上、更には、75μm以上であることが好ましい。
図9に示す酸変性ポリオレフィンを主成分とする表面層(A)の途切れの問題を確認する為に、コア層(B)をグレーに着色したタブリード用フィルムを製造した。
詳しくは、表面層(A)が酸変性ポリプロピレンからなり、コア層(B)がポリプロピレンと着色剤(グレー顔料)とからなり、表面層(C)がポリプロピレンからなる三層構成のタブリード用フィルム(厚さ100μm)を製造した。尚、フィルムの製造は共押出成形法により行った。各層の厚さは、表面層(A)が50μm、コア層(B)が30μm、表面層(C)が20μmであった。
表1に記すように、重質炭酸カルシウムのコア層(B)中への添加の有無、且つ各層の厚さを変更した以外は、試験例1と同様にしてタブリード用フィルムを製造した。該フィルムを用いて途切れ性の評価を行った。
厚さ100μmのニッケル製端子の両面にタブリード用フィルムをヒートシールし、タブリードを作成する。尚、タブリード用フィルムは表面層(A)がニッケル製端子と接するように配置する。またヒートシールは、シールバー温度は上下共に160℃、シール面圧1.0MPa、シール時間2秒の条件で行う。
得られたタブリードを切断し、切断面をデジタルマイクロスコープにて観察する。金属端子がグレーに着色されたコア層(B)と接していたものを×、金属端子の角部において表面層(A)が薄くなっていたものを△、金属端子の角部においても表面層(A)が十分に厚く残っていたものを○と評価する。
また、各層厚みが同じであり、コア層(B)中に炭酸カルシウムを含有する試験例4と、含有しない試験例5を比較すると、どちらも金属端子の角部において表面層(A)が同程度薄くなっており、炭酸カルシウムの有無による違いは見られなかった。
表2に記す樹脂を用いて、表2に記す厚さのタブリード用フィルム(膜厚100μm)を製造した。各フィルムのフッ化水素による接着性低下の評価は、以下の方法にて行った。
また、使用する炭酸カルシウム(CaCO3)のメジアン径の測定方法を以下に記す。
厚さ100μm、幅20mmのニッケル箔の両面に15mm幅のタブリード用フィルムをヒートシールして試験片とする。尚、タブリード用フィルムは表面層(A)がニッケル箔と接するように配置する。またヒートシールは、シールバー温度は上バー190℃、下バー220℃、シール面圧1.0MPa、シール時間3秒の条件で行った。
試験片は2組作成し、1組の試験片を電解液(エチレンカーボネート:ジメチルカーボネート:ジエチルカーボネート=1:1:1(v/v%)の溶媒にLiPF6を1mol/Lの割合で添加したもの)に浸漬し、85℃に加温して2時間保管する。
シール直後の試験片と、電解液に2時間浸漬後の試験片とを、それぞれ180°剥離し、引張試験機(オートグラフ/(株)島津製作所製)にて接着強度(剥離強度)を測定する。尚、引張試験機の引張速度は100mm/min、測定雰囲気は23℃、湿度50%RHとし、上バー側でヒートシールされたタブリード用フィルムを剥離して行う。
測定により得られたデータから、接着性保持率((「電解液に2時間浸漬後の接着強度」÷「シール直後の接着強度」)×100)を算出した。<炭酸カルシウムのメジアン径の測定方法>
使用する炭酸カルシウムのメジアン径は、レーザー回折式粒子径分布測定装置を用いて測定し、体積基準の粒子径の累積分布曲線において10%、50%および90%に相当する粒子径を算出し、50%となる粒子径(メジアン径(D50))を求めた。
実施例4で使用した炭酸カルシウム(CaCO3-2)から別の炭酸カルシウム(CaCO3-3)を用いた以外は、実施例4と同様のタブリード用フィルムを製造し、シール直後の接着強度と電解液に2時間浸漬後の接着強度を測定し接着性保持率を算出した。実施例4で使用した炭酸カルシウム(CaCO3-2)と実施例5した炭酸カルシウム(CaCO3-3)の比較を表3に、実施例5の測定結果を表4に示す。
約60%の接着保持率を有するタブリード用フィルムとする場合、メジアン径が大きい炭酸カルシウムを用いた実施例5よりも、メジアン径が小さい炭酸カルシウムを用いた実施例1の方が、タブリード用フィルムに添加する炭酸カルシウムの量が3分の2の少量とすることができた。
11 表面層(A)
12 コア層(B)
13 表面層(C)
1a 側辺部
2 金属端子
2a 角部
2b 側辺部
TL タブリード
Claims (12)
- 酸変性ポリオレフィン系樹脂を主成分とする表面層(A)、フッ化水素と反応する無機充填剤とポリオレフィン系樹脂を含み、前記フッ化水素と反応する無機充填剤及び/又は前記ポリオレフィン系樹脂が主成分であるコア層(B)、酸変性ポリオレフィン系樹脂及び/又はポリオレフィン系樹脂を主成分とする表面層(C)を順に備えるタブリード用フィルムにおいて、
前記表面層(A)における無機充填剤の含有量、及び前記表面層(C)における無機充填剤の含有量が、それぞれ0~10重量%で、
前記タブリード用フィルムがフッ化水素と反応する無機充填剤を9.0重量%以上含有することを特徴とするタブリード用フィルム。 - 前記タブリード用フィルムがフッ化水素と反応する無機充填剤を9.6重量%以上含有することを特徴とする請求項1記載のタブリード用フィルム。
- 前記タブリード用フィルム中のフッ化水素と反応する無機充填剤のメジアン径が1.0μm以下であることを特徴とする請求項1または2記載のタブリード用フィルム。
- 前記表面層(A)の厚さが23μm以上であることを特徴とする請求項1乃至3のいずれか1項に記載のタブリード用フィルム。
- 前記表面層(A)の厚さがタブリードフィルム全体の厚さの23%以上であることを特徴とする請求項1乃至4のいずれか1項に記載のタブリード用フィルム。
- 前記コア層(B)におけるフッ化水素と反応する無機充填剤の含有量が13~60重量%であることを特徴とする請求項1乃至5のいずれか1項に記載のタブリード用フィルム。
- 前記表面層(A)の厚さをt1、前記コア層(B)の厚さをt2、前記表面層(C)の厚さをt3としたとき、下記の式(1)及び式(2)を満たすことを特徴とする請求項1乃至6のいずれか1項に記載のタブリード用フィルム。
式(1) t1≧t3
式(2) t1:t2:t3=23~80:15~72:5~62 - 前記タブリード用フィルム中のフッ化水素と反応する無機充填剤が金属炭酸塩であることを特徴とする請求項1乃至7のいずれか1項に記載のタブリード用フィルム。
- 前記金属炭酸塩が、炭酸カルシウムであることを特徴とする請求項8記載のタブリード用フィルム。
- 前記炭酸カルシウムが、合成炭酸カルシウムであることを特徴とする請求項9記載のタブリード用フィルム。
- 金属端子の少なくとも一方の表面に、請求項1乃至10のいずれか1項に記載のタブリード用フィルムが熱融着されたタブリードであって、前記金属端子の表面と前記タブリード用フィルムの前記表面層(A)を熱融着したことを特徴とするタブリード。
- 前記金属端子の厚さをT(mt)、前記タブリード用フィルムの厚さをT(tf)としたとき、0.5T(mt)≦T(tf)であることを特徴とする請求項11記載のタブリード。
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