JP5139140B2 - Polyolefin resin sheet - Google Patents
Polyolefin resin sheet Download PDFInfo
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- JP5139140B2 JP5139140B2 JP2008103657A JP2008103657A JP5139140B2 JP 5139140 B2 JP5139140 B2 JP 5139140B2 JP 2008103657 A JP2008103657 A JP 2008103657A JP 2008103657 A JP2008103657 A JP 2008103657A JP 5139140 B2 JP5139140 B2 JP 5139140B2
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- 229920005672 polyolefin resin Polymers 0.000 title claims description 50
- 229920005989 resin Polymers 0.000 claims description 45
- 239000011347 resin Substances 0.000 claims description 45
- -1 polypropylene Polymers 0.000 claims description 44
- 239000002216 antistatic agent Substances 0.000 claims description 41
- 125000004122 cyclic group Chemical group 0.000 claims description 33
- 239000004743 Polypropylene Substances 0.000 claims description 25
- 229920001155 polypropylene Polymers 0.000 claims description 25
- 239000004711 α-olefin Substances 0.000 claims description 19
- 229920000089 Cyclic olefin copolymer Polymers 0.000 claims description 15
- 239000002736 nonionic surfactant Substances 0.000 claims description 8
- 239000011342 resin composition Substances 0.000 claims description 8
- 238000003856 thermoforming Methods 0.000 claims description 5
- 125000004432 carbon atom Chemical group C* 0.000 claims description 2
- 229920000098 polyolefin Polymers 0.000 description 21
- XAGFODPZIPBFFR-UHFFFAOYSA-N aluminium Chemical compound [Al] XAGFODPZIPBFFR-UHFFFAOYSA-N 0.000 description 12
- 229910052782 aluminium Inorganic materials 0.000 description 12
- 229920000642 polymer Polymers 0.000 description 9
- LIKMAJRDDDTEIG-UHFFFAOYSA-N 1-hexene Chemical compound CCCCC=C LIKMAJRDDDTEIG-UHFFFAOYSA-N 0.000 description 8
- 229920003171 Poly (ethylene oxide) Polymers 0.000 description 8
- 230000000052 comparative effect Effects 0.000 description 8
- 229920001577 copolymer Polymers 0.000 description 7
- 230000003287 optical effect Effects 0.000 description 7
- VXNZUUAINFGPBY-UHFFFAOYSA-N 1-Butene Chemical compound CCC=C VXNZUUAINFGPBY-UHFFFAOYSA-N 0.000 description 6
- 235000014113 dietary fatty acids Nutrition 0.000 description 6
- 229930195729 fatty acid Natural products 0.000 description 6
- 239000000194 fatty acid Substances 0.000 description 6
- KWKAKUADMBZCLK-UHFFFAOYSA-N 1-octene Chemical compound CCCCCCC=C KWKAKUADMBZCLK-UHFFFAOYSA-N 0.000 description 5
- VGGSQFUCUMXWEO-UHFFFAOYSA-N Ethene Chemical compound C=C VGGSQFUCUMXWEO-UHFFFAOYSA-N 0.000 description 5
- IAYPIBMASNFSPL-UHFFFAOYSA-N Ethylene oxide Chemical compound C1CO1 IAYPIBMASNFSPL-UHFFFAOYSA-N 0.000 description 5
- 230000009477 glass transition Effects 0.000 description 5
- 239000005022 packaging material Substances 0.000 description 5
- QQONPFPTGQHPMA-UHFFFAOYSA-N propylene Natural products CC=C QQONPFPTGQHPMA-UHFFFAOYSA-N 0.000 description 5
- 125000004805 propylene group Chemical group [H]C([H])([H])C([H])([*:1])C([H])([H])[*:2] 0.000 description 5
- ZGEGCLOFRBLKSE-UHFFFAOYSA-N 1-Heptene Chemical compound CCCCCC=C ZGEGCLOFRBLKSE-UHFFFAOYSA-N 0.000 description 4
- AFFLGGQVNFXPEV-UHFFFAOYSA-N 1-decene Chemical compound CCCCCCCCC=C AFFLGGQVNFXPEV-UHFFFAOYSA-N 0.000 description 4
- WSSSPWUEQFSQQG-UHFFFAOYSA-N 4-methyl-1-pentene Chemical compound CC(C)CC=C WSSSPWUEQFSQQG-UHFFFAOYSA-N 0.000 description 4
- 239000005977 Ethylene Substances 0.000 description 4
- VQTUBCCKSQIDNK-UHFFFAOYSA-N Isobutene Chemical compound CC(C)=C VQTUBCCKSQIDNK-UHFFFAOYSA-N 0.000 description 4
- 239000004721 Polyphenylene oxide Substances 0.000 description 4
- 150000003973 alkyl amines Chemical class 0.000 description 4
- 238000001816 cooling Methods 0.000 description 4
- 238000004519 manufacturing process Methods 0.000 description 4
- 239000000463 material Substances 0.000 description 4
- 239000000155 melt Substances 0.000 description 4
- YWAKXRMUMFPDSH-UHFFFAOYSA-N pentene Chemical compound CCCC=C YWAKXRMUMFPDSH-UHFFFAOYSA-N 0.000 description 4
- 229920000570 polyether Polymers 0.000 description 4
- 239000002699 waste material Substances 0.000 description 4
- PEDCQBHIVMGVHV-UHFFFAOYSA-N Glycerol Natural products OCC(O)CO PEDCQBHIVMGVHV-UHFFFAOYSA-N 0.000 description 3
- 239000002202 Polyethylene glycol Substances 0.000 description 3
- 150000001993 dienes Chemical class 0.000 description 3
- 238000001125 extrusion Methods 0.000 description 3
- 239000000178 monomer Substances 0.000 description 3
- 229920001223 polyethylene glycol Polymers 0.000 description 3
- 150000003839 salts Chemical class 0.000 description 3
- 239000000126 substance Substances 0.000 description 3
- 239000004094 surface-active agent Substances 0.000 description 3
- QGKMIGUHVLGJBR-UHFFFAOYSA-M (4z)-1-(3-methylbutyl)-4-[[1-(3-methylbutyl)quinolin-1-ium-4-yl]methylidene]quinoline;iodide Chemical compound [I-].C12=CC=CC=C2N(CCC(C)C)C=CC1=CC1=CC=[N+](CCC(C)C)C2=CC=CC=C12 QGKMIGUHVLGJBR-UHFFFAOYSA-M 0.000 description 2
- MYRTYDVEIRVNKP-UHFFFAOYSA-N 1,2-Divinylbenzene Chemical compound C=CC1=CC=CC=C1C=C MYRTYDVEIRVNKP-UHFFFAOYSA-N 0.000 description 2
- YHQXBTXEYZIYOV-UHFFFAOYSA-N 3-methylbut-1-ene Chemical compound CC(C)C=C YHQXBTXEYZIYOV-UHFFFAOYSA-N 0.000 description 2
- QTBSBXVTEAMEQO-UHFFFAOYSA-N Acetic acid Natural products CC(O)=O QTBSBXVTEAMEQO-UHFFFAOYSA-N 0.000 description 2
- SOGAXMICEFXMKE-UHFFFAOYSA-N Butylmethacrylate Chemical compound CCCCOC(=O)C(C)=C SOGAXMICEFXMKE-UHFFFAOYSA-N 0.000 description 2
- OKTJSMMVPCPJKN-UHFFFAOYSA-N Carbon Chemical compound [C] OKTJSMMVPCPJKN-UHFFFAOYSA-N 0.000 description 2
- RTZKZFJDLAIYFH-UHFFFAOYSA-N Diethyl ether Chemical compound CCOCC RTZKZFJDLAIYFH-UHFFFAOYSA-N 0.000 description 2
- LYCAIKOWRPUZTN-UHFFFAOYSA-N Ethylene glycol Chemical compound OCCO LYCAIKOWRPUZTN-UHFFFAOYSA-N 0.000 description 2
- UQSXHKLRYXJYBZ-UHFFFAOYSA-N Iron oxide Chemical compound [Fe]=O UQSXHKLRYXJYBZ-UHFFFAOYSA-N 0.000 description 2
- 239000004594 Masterbatch (MB) Substances 0.000 description 2
- BAPJBEWLBFYGME-UHFFFAOYSA-N Methyl acrylate Chemical compound COC(=O)C=C BAPJBEWLBFYGME-UHFFFAOYSA-N 0.000 description 2
- PPBRXRYQALVLMV-UHFFFAOYSA-N Styrene Chemical compound C=CC1=CC=CC=C1 PPBRXRYQALVLMV-UHFFFAOYSA-N 0.000 description 2
- XLOMVQKBTHCTTD-UHFFFAOYSA-N Zinc monoxide Chemical compound [Zn]=O XLOMVQKBTHCTTD-UHFFFAOYSA-N 0.000 description 2
- 239000002253 acid Substances 0.000 description 2
- 150000005215 alkyl ethers Chemical class 0.000 description 2
- 150000001412 amines Chemical class 0.000 description 2
- 229920001400 block copolymer Polymers 0.000 description 2
- 239000002981 blocking agent Substances 0.000 description 2
- CJOBVZJTOIVNNF-UHFFFAOYSA-N cadmium sulfide Chemical compound [Cd]=S CJOBVZJTOIVNNF-UHFFFAOYSA-N 0.000 description 2
- 229910052799 carbon Inorganic materials 0.000 description 2
- 239000003795 chemical substances by application Substances 0.000 description 2
- 239000003086 colorant Substances 0.000 description 2
- 230000000694 effects Effects 0.000 description 2
- 230000005611 electricity Effects 0.000 description 2
- 235000011187 glycerol Nutrition 0.000 description 2
- 238000004898 kneading Methods 0.000 description 2
- 238000000465 moulding Methods 0.000 description 2
- TVMXDCGIABBOFY-UHFFFAOYSA-N n-Octanol Natural products CCCCCCCC TVMXDCGIABBOFY-UHFFFAOYSA-N 0.000 description 2
- 229920006146 polyetheresteramide block copolymer Polymers 0.000 description 2
- 229920000573 polyethylene Polymers 0.000 description 2
- 150000003242 quaternary ammonium salts Chemical class 0.000 description 2
- 229920005604 random copolymer Polymers 0.000 description 2
- 239000002994 raw material Substances 0.000 description 2
- 230000003068 static effect Effects 0.000 description 2
- 230000037303 wrinkles Effects 0.000 description 2
- PRBHEGAFLDMLAL-GQCTYLIASA-N (4e)-hexa-1,4-diene Chemical compound C\C=C\CC=C PRBHEGAFLDMLAL-GQCTYLIASA-N 0.000 description 1
- DNIAPMSPPWPWGF-GSVOUGTGSA-N (R)-(-)-Propylene glycol Chemical compound C[C@@H](O)CO DNIAPMSPPWPWGF-GSVOUGTGSA-N 0.000 description 1
- WKBPZYKAUNRMKP-UHFFFAOYSA-N 1-[2-(2,4-dichlorophenyl)pentyl]1,2,4-triazole Chemical compound C=1C=C(Cl)C=C(Cl)C=1C(CCC)CN1C=NC=N1 WKBPZYKAUNRMKP-UHFFFAOYSA-N 0.000 description 1
- SMZOUWXMTYCWNB-UHFFFAOYSA-N 2-(2-methoxy-5-methylphenyl)ethanamine Chemical compound COC1=CC=C(C)C=C1CCN SMZOUWXMTYCWNB-UHFFFAOYSA-N 0.000 description 1
- OEPOKWHJYJXUGD-UHFFFAOYSA-N 2-(3-phenylmethoxyphenyl)-1,3-thiazole-4-carbaldehyde Chemical compound O=CC1=CSC(C=2C=C(OCC=3C=CC=CC=3)C=CC=2)=N1 OEPOKWHJYJXUGD-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
- JLBJTVDPSNHSKJ-UHFFFAOYSA-N 4-Methylstyrene Chemical compound CC1=CC=C(C=C)C=C1 JLBJTVDPSNHSKJ-UHFFFAOYSA-N 0.000 description 1
- VSQLAQKFRFTMNS-UHFFFAOYSA-N 5-methylhexa-1,4-diene Chemical compound CC(C)=CCC=C VSQLAQKFRFTMNS-UHFFFAOYSA-N 0.000 description 1
- UCKITPBQPGXDHV-UHFFFAOYSA-N 7-methylocta-1,6-diene Chemical compound CC(C)=CCCCC=C UCKITPBQPGXDHV-UHFFFAOYSA-N 0.000 description 1
- NLHHRLWOUZZQLW-UHFFFAOYSA-N Acrylonitrile Chemical compound C=CC#N NLHHRLWOUZZQLW-UHFFFAOYSA-N 0.000 description 1
- 238000006677 Appel reaction Methods 0.000 description 1
- FBPFZTCFMRRESA-FSIIMWSLSA-N D-Glucitol Natural products OC[C@H](O)[C@H](O)[C@@H](O)[C@H](O)CO FBPFZTCFMRRESA-FSIIMWSLSA-N 0.000 description 1
- LFQSCWFLJHTTHZ-UHFFFAOYSA-N Ethanol Chemical compound CCO LFQSCWFLJHTTHZ-UHFFFAOYSA-N 0.000 description 1
- JIGUQPWFLRLWPJ-UHFFFAOYSA-N Ethyl acrylate Chemical compound CCOC(=O)C=C JIGUQPWFLRLWPJ-UHFFFAOYSA-N 0.000 description 1
- WOBHKFSMXKNTIM-UHFFFAOYSA-N Hydroxyethyl methacrylate Chemical compound CC(=C)C(=O)OCCO WOBHKFSMXKNTIM-UHFFFAOYSA-N 0.000 description 1
- CERQOIWHTDAKMF-UHFFFAOYSA-N Methacrylic acid Chemical compound CC(=C)C(O)=O CERQOIWHTDAKMF-UHFFFAOYSA-N 0.000 description 1
- VVQNEPGJFQJSBK-UHFFFAOYSA-N Methyl methacrylate Chemical compound COC(=O)C(C)=C VVQNEPGJFQJSBK-UHFFFAOYSA-N 0.000 description 1
- 239000004698 Polyethylene Substances 0.000 description 1
- 229920001214 Polysorbate 60 Polymers 0.000 description 1
- OFOBLEOULBTSOW-UHFFFAOYSA-N Propanedioic acid Natural products OC(=O)CC(O)=O OFOBLEOULBTSOW-UHFFFAOYSA-N 0.000 description 1
- BUGBHKTXTAQXES-UHFFFAOYSA-N Selenium Chemical compound [Se] BUGBHKTXTAQXES-UHFFFAOYSA-N 0.000 description 1
- GWEVSGVZZGPLCZ-UHFFFAOYSA-N Titan oxide Chemical compound O=[Ti]=O GWEVSGVZZGPLCZ-UHFFFAOYSA-N 0.000 description 1
- BZHJMEDXRYGGRV-UHFFFAOYSA-N Vinyl chloride Chemical compound ClC=C BZHJMEDXRYGGRV-UHFFFAOYSA-N 0.000 description 1
- 230000001476 alcoholic effect Effects 0.000 description 1
- 150000001336 alkenes Chemical class 0.000 description 1
- 125000000217 alkyl group Chemical group 0.000 description 1
- 150000001408 amides Chemical class 0.000 description 1
- 239000002280 amphoteric surfactant Substances 0.000 description 1
- 239000003945 anionic surfactant Substances 0.000 description 1
- 239000003963 antioxidant agent Substances 0.000 description 1
- 230000003078 antioxidant effect Effects 0.000 description 1
- IRERQBUNZFJFGC-UHFFFAOYSA-L azure blue Chemical compound [Na+].[Na+].[Na+].[Na+].[Na+].[Na+].[Na+].[Na+].[Al+3].[Al+3].[Al+3].[Al+3].[Al+3].[Al+3].[S-]S[S-].[O-][Si]([O-])([O-])[O-].[O-][Si]([O-])([O-])[O-].[O-][Si]([O-])([O-])[O-].[O-][Si]([O-])([O-])[O-].[O-][Si]([O-])([O-])[O-].[O-][Si]([O-])([O-])[O-] IRERQBUNZFJFGC-UHFFFAOYSA-L 0.000 description 1
- CQEYYJKEWSMYFG-UHFFFAOYSA-N butyl acrylate Chemical compound CCCCOC(=O)C=C CQEYYJKEWSMYFG-UHFFFAOYSA-N 0.000 description 1
- 229910052793 cadmium Inorganic materials 0.000 description 1
- BDOSMKKIYDKNTQ-UHFFFAOYSA-N cadmium atom Chemical compound [Cd] BDOSMKKIYDKNTQ-UHFFFAOYSA-N 0.000 description 1
- 239000006229 carbon black Substances 0.000 description 1
- 150000001732 carboxylic acid derivatives Chemical class 0.000 description 1
- 239000003093 cationic surfactant Substances 0.000 description 1
- 229920006026 co-polymeric resin Polymers 0.000 description 1
- 230000000536 complexating effect Effects 0.000 description 1
- 150000001875 compounds Chemical class 0.000 description 1
- 235000019628 coolness Nutrition 0.000 description 1
- XCJYREBRNVKWGJ-UHFFFAOYSA-N copper(II) phthalocyanine Chemical compound [Cu+2].C12=CC=CC=C2C(N=C2[N-]C(C3=CC=CC=C32)=N2)=NC1=NC([C]1C=CC=CC1=1)=NC=1N=C1[C]3C=CC=CC3=C2[N-]1 XCJYREBRNVKWGJ-UHFFFAOYSA-N 0.000 description 1
- 230000007423 decrease Effects 0.000 description 1
- 230000006866 deterioration Effects 0.000 description 1
- ZBCBWPMODOFKDW-UHFFFAOYSA-N diethanolamine Chemical compound OCCNCCO ZBCBWPMODOFKDW-UHFFFAOYSA-N 0.000 description 1
- 238000005553 drilling Methods 0.000 description 1
- 150000002148 esters Chemical class 0.000 description 1
- SUPCQIBBMFXVTL-UHFFFAOYSA-N ethyl 2-methylprop-2-enoate Chemical compound CCOC(=O)C(C)=C SUPCQIBBMFXVTL-UHFFFAOYSA-N 0.000 description 1
- 229920005648 ethylene methacrylic acid copolymer Polymers 0.000 description 1
- 150000004665 fatty acids Chemical class 0.000 description 1
- 239000006260 foam Substances 0.000 description 1
- 125000005456 glyceride group Chemical group 0.000 description 1
- WGCNASOHLSPBMP-UHFFFAOYSA-N hydroxyacetaldehyde Natural products OCC=O WGCNASOHLSPBMP-UHFFFAOYSA-N 0.000 description 1
- 150000002462 imidazolines Chemical class 0.000 description 1
- 238000009863 impact test Methods 0.000 description 1
- 239000003112 inhibitor Substances 0.000 description 1
- 238000001746 injection moulding Methods 0.000 description 1
- 229910010272 inorganic material Inorganic materials 0.000 description 1
- 239000011147 inorganic material Substances 0.000 description 1
- 229910017053 inorganic salt Inorganic materials 0.000 description 1
- 229920000554 ionomer Polymers 0.000 description 1
- 230000005923 long-lasting effect Effects 0.000 description 1
- 229920001684 low density polyethylene Polymers 0.000 description 1
- 239000004702 low-density polyethylene Substances 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
- 238000005259 measurement Methods 0.000 description 1
- 238000000691 measurement method Methods 0.000 description 1
- 239000012968 metallocene catalyst Substances 0.000 description 1
- 238000005649 metathesis reaction Methods 0.000 description 1
- 238000000034 method Methods 0.000 description 1
- 238000002156 mixing Methods 0.000 description 1
- 239000000203 mixture Substances 0.000 description 1
- 239000000615 nonconductor Substances 0.000 description 1
- JFNLZVQOOSMTJK-KNVOCYPGSA-N norbornene Chemical compound C1[C@@H]2CC[C@H]1C=C2 JFNLZVQOOSMTJK-KNVOCYPGSA-N 0.000 description 1
- JRZJOMJEPLMPRA-UHFFFAOYSA-N olefin Natural products CCCCCCCC=C JRZJOMJEPLMPRA-UHFFFAOYSA-N 0.000 description 1
- TWNQGVIAIRXVLR-UHFFFAOYSA-N oxo(oxoalumanyloxy)alumane Chemical compound O=[Al]O[Al]=O TWNQGVIAIRXVLR-UHFFFAOYSA-N 0.000 description 1
- 239000011087 paperboard Substances 0.000 description 1
- 239000008188 pellet Substances 0.000 description 1
- PNJWIWWMYCMZRO-UHFFFAOYSA-N pent‐4‐en‐2‐one Natural products CC(=O)CC=C PNJWIWWMYCMZRO-UHFFFAOYSA-N 0.000 description 1
- 229940083254 peripheral vasodilators imidazoline derivative Drugs 0.000 description 1
- 150000003014 phosphoric acid esters Chemical class 0.000 description 1
- 239000000049 pigment Substances 0.000 description 1
- 229920006149 polyester-amide block copolymer Polymers 0.000 description 1
- 229920001451 polypropylene glycol Polymers 0.000 description 1
- 229920005629 polypropylene homopolymer Polymers 0.000 description 1
- 238000003825 pressing Methods 0.000 description 1
- HJWLCRVIBGQPNF-UHFFFAOYSA-N prop-2-enylbenzene Chemical compound C=CCC1=CC=CC=C1 HJWLCRVIBGQPNF-UHFFFAOYSA-N 0.000 description 1
- 238000004080 punching Methods 0.000 description 1
- 150000003222 pyridines Chemical class 0.000 description 1
- 238000004064 recycling Methods 0.000 description 1
- 230000001105 regulatory effect Effects 0.000 description 1
- 238000007151 ring opening polymerisation reaction Methods 0.000 description 1
- 229910052711 selenium Inorganic materials 0.000 description 1
- 239000011669 selenium Substances 0.000 description 1
- 229910052708 sodium Inorganic materials 0.000 description 1
- 239000011734 sodium Substances 0.000 description 1
- 239000000600 sorbitol Substances 0.000 description 1
- 239000003381 stabilizer Substances 0.000 description 1
- 150000005846 sugar alcohols Polymers 0.000 description 1
- OGIDPMRJRNCKJF-UHFFFAOYSA-N titanium oxide Inorganic materials [Ti]=O OGIDPMRJRNCKJF-UHFFFAOYSA-N 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
- 235000013799 ultramarine blue Nutrition 0.000 description 1
- 239000006097 ultraviolet radiation absorber Substances 0.000 description 1
- 229920002554 vinyl polymer Polymers 0.000 description 1
- XLYOFNOQVPJJNP-UHFFFAOYSA-N water Substances O XLYOFNOQVPJJNP-UHFFFAOYSA-N 0.000 description 1
- 239000011787 zinc oxide Substances 0.000 description 1
Description
本発明は、優れた耐衝撃性を有し、かつ成形加工性に優れたポリオレフィン系樹脂シ−ト及びその成形品に関するものである。 The present invention relates to a polyolefin resin sheet having excellent impact resistance and excellent moldability, and a molded product thereof.
環状ポリオレフィン系樹脂は、透明性、耐熱性、機械的強度、寸法安定性に優れており、レンズ、光ディスク、プリズム、シートなどの光学部品の材料として用いられている。このような光学部品の成形体を得る際に、スプール部やランナー部内に残る製品外の樹脂材料、フィルムまたはシート両端に発生する耳と呼ばれる余剰部分、あるいは規格外品などの廃材が発生する。これらの廃材は溶融してペレット化して再利用することも検討されているが、透明性が低下することから光学部品への再利用は困難である。従って、一般的には焼却処理や埋め立て処理が行なわれており、環状ポリオレフィン系樹脂の廃材を有効に処理するための他の方策が模索されている。 Cyclic polyolefin resins are excellent in transparency, heat resistance, mechanical strength, and dimensional stability, and are used as materials for optical components such as lenses, optical disks, prisms, and sheets. When obtaining such a molded article of an optical component, a resin material outside the product remaining in the spool portion or the runner portion, an excess portion called an ear generated at both ends of the film or the sheet, or a waste material such as a nonstandard product is generated. Although these waste materials are also considered to be melted, pelletized, and reused, their transparency is lowered, so that it is difficult to reuse them for optical parts. Accordingly, incineration treatment and landfill treatment are generally performed, and other measures for effectively treating the waste material of the cyclic polyolefin resin are being sought.
環状ポリオレフィン系樹脂を添加した熱成形用シートも提案されているが、ポリプロピレン系樹脂シートの熱成形時のたるみを改善させるためのものであり、得られたシート及び成形品は耐衝撃性に劣り、包装材や緩衝材用のシートとしては不適であった(特許文献1を参照)。 A sheet for thermoforming to which a cyclic polyolefin resin is added has also been proposed, but it is for improving the sag of a polypropylene resin sheet during thermoforming, and the resulting sheet and molded product have poor impact resistance. It was unsuitable as a sheet for packaging material or cushioning material (see Patent Document 1).
また、環状ポリオレフィン系樹脂とポリオレフィン樹脂と水添されたジエン系重合体の樹脂組成物が提案されているが、水添されたジエン系重合体のコストが高いことに加え、耐衝撃性が不十分であることから、得られたトレー状の成形品では耐衝撃性が不十分であった(特許文献2を参照)。 Further, a resin composition of a diene polymer hydrogenated with a cyclic polyolefin resin and a polyolefin resin has been proposed, but in addition to the high cost of the hydrogenated diene polymer, the impact resistance is poor. Since it was sufficient, the obtained tray-shaped molded article was insufficient in impact resistance (see Patent Document 2).
一方、一般的に環状ポリオレフィン系樹脂は単体で良好な電気絶縁体であるため、静電気を帯電しやすい。従って、環状ポリオレフィン系樹脂を用いたシ−トを電子部品包装材に使用する場合、帯電防止性能を付与する必要があるが、非晶性でかつガラス転移温度の高い特性を有する環状ポリオレフィン系樹脂は帯電防止性能が発現し難いという問題があった。 On the other hand, since cyclic polyolefin resin is generally a good electrical insulator, it is easy to be charged with static electricity. Therefore, when a sheet using a cyclic polyolefin resin is used for an electronic component packaging material, it is necessary to provide antistatic performance, but the cyclic polyolefin resin has a non-crystalline property and a high glass transition temperature. Has a problem that it is difficult to exhibit antistatic performance.
さらには、環状ポリオレフィンは比較的脆く、かつポリプロピレン系樹脂と混ざり難いことから、単純にポリプロピレン系樹脂と混合して溶融混練しただけでは耐衝撃性及び成形性に優れたシートを得ることは困難であった。 Furthermore, since cyclic polyolefin is relatively brittle and difficult to mix with polypropylene resin, it is difficult to obtain a sheet having excellent impact resistance and moldability simply by mixing with polypropylene resin and melt-kneading. there were.
本発明は、優れた耐衝撃性を有し、かつ、成形加工性に優れたポリオレフィン系樹脂シ−ト及びその成形品に関するものである。 The present invention relates to a polyolefin resin sheet having excellent impact resistance and excellent molding processability, and a molded product thereof.
そこで、本発明者らは鋭意検討した結果、ポリプロピレン系樹脂60〜20重量%及び環状ポリオレフィン系樹脂40〜80重量%からなる樹脂組成物100重量部に対して、エチレン−α−オレフィン共重合体樹脂5〜30重量部を添加し、さらに帯電防止剤を含み、JIS K6911 5.13に準拠した温度22℃、湿度65%のときの表面固有抵抗率が1×1013(Ω)未満であるポリオレフィン系樹脂シ−ト及びその成形品であれば、上記の如き問題を解決できることを見出した。 Therefore, as a result of intensive studies, the present inventors have found that an ethylene-α-olefin copolymer is used with respect to 100 parts by weight of a resin composition comprising 60 to 20% by weight of a polypropylene resin and 40 to 80% by weight of a cyclic polyolefin resin. 5-30 parts by weight of a resin is added, and an antistatic agent is further included. The specific surface resistivity is less than 1 × 10 13 (Ω) when the temperature is 22 ° C. and the humidity is 65% in accordance with JIS K6911 5.13. It has been found that the above-mentioned problems can be solved by using a polyolefin resin sheet and a molded product thereof.
これにより、優れた耐衝撃性を有し、かつ、成形加工性に優れたポリオレフィン系樹脂シ−ト及びその成形品を提供できる。従って、たとえ環状ポリオレフィン系樹脂が含まれていても、廃材の有効利用は勿論、耐衝撃性に優れているため包装材や緩衝材用のシートのほか、トレー状の成形品として好適である。また環状ポリオレフィン系樹脂を用いたシ−トを電子部品包装材に使用する場合も、帯電防止剤を含み、JIS K6911 5.13に準拠した温度22℃、湿度65%のときの表面固有抵抗率が1×1013(Ω)未満であることによって、たとえ環状ポリオレフィン系樹脂を含むポリオレフィン系樹脂シートであっても帯電防止性能を付与することができる。 Thereby, it is possible to provide a polyolefin resin sheet having excellent impact resistance and excellent molding processability, and a molded product thereof. Therefore, even if a cyclic polyolefin-based resin is contained, it is suitable for use as a tray-shaped molded product in addition to a sheet for a packaging material or a cushioning material because of its excellent impact resistance as well as effective use of waste materials. In addition, when a sheet using a cyclic polyolefin resin is used as an electronic component packaging material, it contains an antistatic agent, and has a surface resistivity at a temperature of 22 ° C. and a humidity of 65% in accordance with JIS K6911 5.13. Is less than 1 × 10 13 (Ω), it is possible to impart antistatic performance even to a polyolefin resin sheet containing a cyclic polyolefin resin.
以下、本発明の実施の形態について説明する。
(ポリプロピレン系樹脂)
本発明のポリプロピレン系樹脂とは、従来から用いられているものであり、特に限定されず、例えばホモポリプロピレン、プロピレンとこれと共重合可能なモノマーとのブロック共重合体又はランダム共重合体等が挙げられる。
上記プロピレンと共重合可能なモノマーとしては、例えば、エチレン、1−ブテン、イソブテン、1−ペンテン、3−メチル−1−ブテン、1−ヘキセン、4−メチル−1−ペンテン、1−ヘプテン、1−オクテン、1−デセン等のα−オレフィン、1,4−ヘキサジエン、5−メチル−1,4−ヘキサジエン、7−メチル−1,6−オクタジエン等のジエン、塩化ビニル、塩化ビニリデン、アクリロニトリル、酢酸ビニル、アクリル酸、メタクリル酸、マレイン酸、アクリル酸メチル、アクリル酸エチル、アクリル酸ブチル、メタクリル酸メチル、メタクリル酸エチル、メタクリル酸ブチル、無水マレイン酸、スチレン、メチルスチレン、ビニルトルエン、ジビニルベンゼン等のビニル単量体が挙げられ、得られるポリオレフィン系シートの耐衝撃性が優れている点でエチレンが好ましい。
そして、上記プロピレンとこれと共重合可能なモノマーとのブロック共重合体又はランダム共重合体中におけるプロピレン成分は、少ないと、得られるポリオレフィン系樹脂シートの耐熱性、剛性、耐衝撃性が低下することがあるので、80重量%以上が好ましく、90重量%以上がより好ましい。
Embodiments of the present invention will be described below.
(Polypropylene resin)
The polypropylene resin of the present invention is conventionally used, and is not particularly limited. For example, homopolypropylene, a block copolymer of propylene and a monomer copolymerizable therewith or a random copolymer, and the like. Can be mentioned.
Examples of the monomer copolymerizable with propylene include ethylene, 1-butene, isobutene, 1-pentene, 3-methyl-1-butene, 1-hexene, 4-methyl-1-pentene, 1-heptene, 1 Α-olefins such as octene and 1-decene, dienes such as 1,4-hexadiene, 5-methyl-1,4-hexadiene and 7-methyl-1,6-octadiene, vinyl chloride, vinylidene chloride, acrylonitrile, acetic acid Vinyl, acrylic acid, methacrylic acid, maleic acid, methyl acrylate, ethyl acrylate, butyl acrylate, methyl methacrylate, ethyl methacrylate, butyl methacrylate, maleic anhydride, styrene, methyl styrene, vinyl toluene, divinyl benzene, etc. Polyolefin sheet obtained by using Ethylene is preferred in that impact resistance is excellent.
And if there are few propylene components in the block copolymer or random copolymer of the said propylene and a monomer copolymerizable with this, the heat resistance of the polyolefin resin sheet obtained, rigidity, and impact resistance will fall. Therefore, 80% by weight or more is preferable, and 90% by weight or more is more preferable.
上記ポリプロピレン系樹脂のメルトフローレートは、低いと、製造時の押出加工性が低下して生産性を低下することがあり、又、高いと環状ポリオレフィン系樹脂との混練性が低下するため、0.5〜20g/10分が好ましく、1〜10g/10分がより好ましい。
なお、上記ポリプロピレン系樹脂のメルトフローレートとは、樹脂の流れ特性を表わす指標であって、JIS K7210に準じて測定することにより得ることができる。本発明では、ポリプロピレン系樹脂を用いる点から、230℃、2.16kg荷重で測定を行なっている。
If the melt flow rate of the polypropylene resin is low, the extrusion processability during production may be reduced and productivity may be reduced. If the melt flow rate is high, the kneadability with the cyclic polyolefin resin may be reduced. 5 to 20 g / 10 min is preferable, and 1 to 10 g / 10 min is more preferable.
The melt flow rate of the polypropylene resin is an index representing the flow characteristics of the resin, and can be obtained by measuring according to JIS K7210. In the present invention, measurement is performed at 230 ° C. and a load of 2.16 kg from the point of using a polypropylene resin.
(環状ポリオレフィン系樹脂)
本発明の環状ポリオレフィン系樹脂とは、主鎖あるいは側鎖に環状脂肪族炭化水素を有するポリオレフィン系樹脂をいう。環状脂肪族炭化水素としては、例えば「化1」にあげる構造式で表されるものがある。
The cyclic polyolefin resin of the present invention refers to a polyolefin resin having a cyclic aliphatic hydrocarbon in the main chain or side chain. Examples of the cyclic aliphatic hydrocarbon include those represented by the structural formula shown in “Chemical Formula 1”.
環状ポリオレフィン系樹脂の市販品としては、例えば、日本ゼオン社製のゼオネックス(登録商標)およびゼオノア(登録商標)、JSR社製のアートン(登録商標)、三井化学社製のアペル(登録商標)、ポリプラスチックス社製のトパスなどをあげることができる。 Examples of commercially available cyclic polyolefin-based resins include ZEONEX (registered trademark) and ZEONOR (registered trademark) manufactured by ZEON Corporation, Arton (registered trademark) manufactured by JSR, APPEL (registered trademark) manufactured by Mitsui Chemicals, For example, Topas made by Polyplastics.
より好ましく用いられる環状ポリオレフィン系樹脂としては、ガラス転移温度100℃〜160℃のものである。この範囲であればポリプロピレンとエチレン−α−オレフィン共重合体とで溶融混合した場合に良好な混練性を示す。なお、上記環状ポリオレフィン系樹脂のガラス転移温度とは、示差走査熱量計(セイコー電子工業社製RDC220型)を用い、JIS K7121に規定されている測定方法で測定した中間点ガラス転移温度である。 More preferable cyclic polyolefin-based resins are those having a glass transition temperature of 100 ° C to 160 ° C. Within this range, good kneadability is exhibited when melt-mixed with polypropylene and an ethylene-α-olefin copolymer. In addition, the glass transition temperature of the said cyclic polyolefin-type resin is a midpoint glass transition temperature measured by the measuring method prescribed | regulated to JISK7121 using the differential scanning calorimeter (Seiko Denshi Kogyo RDC220 type | mold).
また、環状ポリオレフィン系樹脂には、ノルボルネンとエチレンをメタロセン触媒にて共重合したシクロオレフィンコポリマー(COC)タイプとメタセシス開環重合タイプのシクロオレフィンポリマー(COP)タイプがあるが、そのどちらを用いてもかまわない。 Cyclic polyolefin resins include cycloolefin copolymer (COC) type obtained by copolymerizing norbornene and ethylene with a metallocene catalyst, and cycloolefin polymer (COP) type of metathesis ring-opening polymerization type. It doesn't matter.
上記の環状オレフィン樹脂はバージン原料を用いてもかまわないが、例えば光学レンズ、プリズムなどの光学部品自身や、その光学部品を射出成形等で製造する際に発生するスプール部やランナー部の破砕品およびリペレット品を用いてもかまわない。
ポリプロピレン系樹脂と環状ポリオレフィン系樹脂の割合は、ポリプロピレン系樹脂60〜20重量%および環状ポリオレフィン系樹脂40〜80重量%である。ポリプロピレン系樹脂が60重量%より多いと環状ポリオレフィンの使用量が少なく、リサイクルの点から好ましくない。また、ポリプロピレン系樹脂が20重量%未満の場合は耐衝撃性と成形性が低下するので好ましくない。ポリプロピレン系樹脂の割合が60〜40重量%、環状ポリオレフィン系樹脂の割合が40〜60重量%であることがより好ましい。
Virgin raw materials may be used for the above cyclic olefin resin, but, for example, optical parts such as optical lenses and prisms, and crushed products of spool parts and runner parts that are generated when the optical parts are manufactured by injection molding or the like. Also, re-pellet products may be used.
The proportions of the polypropylene resin and the cyclic polyolefin resin are 60 to 20% by weight of the polypropylene resin and 40 to 80% by weight of the cyclic polyolefin resin. When the amount of polypropylene resin is more than 60% by weight, the amount of cyclic polyolefin used is small, which is not preferable from the viewpoint of recycling. Further, when the polypropylene resin is less than 20% by weight, the impact resistance and moldability are lowered, which is not preferable. More preferably, the proportion of the polypropylene resin is 60 to 40% by weight and the proportion of the cyclic polyolefin resin is 40 to 60% by weight.
(エチレン−α−オレフィン共重合体樹脂)
エチレン−α−オレフィン共重合体樹脂のα−オレフィンとしては、例えば、プロピレン、1−ブテン、イソブテン、1−ペンテン、3−メチル−1−ブテン、1−ヘキセン、4−メチル−1−ペンテン、1−ヘプテン、1−オクテン、1−デセン等が挙げられる。
上記α―オレフィンは、その炭素数が多いとコストが高くなり、又、炭素数が少ないと、得られるポリオレフィン系樹脂シートの耐衝撃性が低下することから、炭素数が4〜8のα―オレフィンが好ましく、1−ブテン、1−ヘキセン、1−オクテンがより好ましく、1−ヘキセンが特に好ましい。
(Ethylene-α-olefin copolymer resin)
Examples of the α-olefin of the ethylene-α-olefin copolymer resin include propylene, 1-butene, isobutene, 1-pentene, 3-methyl-1-butene, 1-hexene, 4-methyl-1-pentene, Examples include 1-heptene, 1-octene, 1-decene and the like.
The α-olefin has a high cost when its carbon number is large, and when the carbon number is small, the impact resistance of the resulting polyolefin resin sheet is lowered. Olefin is preferable, 1-butene, 1-hexene and 1-octene are more preferable, and 1-hexene is particularly preferable.
なお、エチレンと炭素数が4〜8のα―オレフィンとの共重合体樹脂としては、たとえば、住友化学社から商品名「エクセレンFX CX3502」(エチレン−1−ブテン共重合体)、日本ポリエチレン社から商品名「カーネル KS240T」(エチレン−1−ヘキセン共重合体)、ダウ・ケミカル社から商品名「エンゲージ EG8100」(エチレン−1−オクテン共重合体)で販売されている。 Examples of the copolymer resin of ethylene and α-olefin having 4 to 8 carbon atoms include, for example, trade name “Excellen FX CX3502” (ethylene-1-butene copolymer) manufactured by Sumitomo Chemical Co., Ltd., Nippon Polyethylene Co., Ltd. Under the trade name “Kernel KS240T” (ethylene-1-hexene copolymer) and Dow Chemical Company under the trade name “engage EG8100” (ethylene-1-octene copolymer).
更に、上記エチレン−α−オレフィン共重合体樹脂の密度は、大きいと、得られるポリオレフィン系樹脂シートの耐衝撃性が低下して好ましくない。また、小さいと、得られるポリオレフィン系樹脂シートの機械的強度や高温での剛性が低下することがあるので、0.85〜0.91g/cm3が好ましく、0.86〜0.88g/cm3がより好ましい。 Furthermore, if the density of the ethylene-α-olefin copolymer resin is large, the impact resistance of the resulting polyolefin resin sheet is lowered, which is not preferable. Moreover, since the mechanical strength of the polyolefin-type resin sheet and rigidity at high temperature may fall when it is small, 0.85-0.91 g / cm < 3 > is preferable, 0.86-0.88 g / cm 3 is more preferable.
そして、上記エチレン−α−オレフィン共重合体の含有量は、少ないと、得られるポリオレフィン系樹脂シートの耐衝撃性が低下し、多いと、得られるポリオレフィン系樹脂シートの機械的強度や、高温時の剛性が低下するので好ましくない。従って、ポリプロピレン系樹脂60〜20重量%及び環状ポリオレフィン系樹脂40〜80重量%からなる樹脂組成物100重量部に対して、エチレン−α−オレフィン共重合体樹脂は5〜30重量部に限定され、好ましくは10〜30重量部、より好ましくは10〜20重量部である。エチレン−α−オレフィン共重合体樹脂を含有させることで、帯電防止剤の効果が高められる。 And if there is little content of the said ethylene-alpha-olefin copolymer, the impact resistance of the polyolefin-type resin sheet obtained will fall, and when large, the mechanical strength of the polyolefin-type resin sheet obtained, and at the time of high temperature This is not preferable because the rigidity of the resin decreases. Accordingly, the ethylene-α-olefin copolymer resin is limited to 5 to 30 parts by weight with respect to 100 parts by weight of the resin composition comprising 60 to 20% by weight of the polypropylene resin and 40 to 80% by weight of the cyclic polyolefin resin. The amount is preferably 10 to 30 parts by weight, more preferably 10 to 20 parts by weight. By including the ethylene-α-olefin copolymer resin, the effect of the antistatic agent is enhanced.
(帯電防止剤)
本発明に用いられる帯電防止剤としては、高分子型帯電防止剤あるいは界面活性剤型帯電防止剤のいずれの帯電防止剤も用いることができる。
(Antistatic agent)
As the antistatic agent used in the present invention, any one of a polymer type antistatic agent and a surfactant type antistatic agent can be used.
本発明の高分子型帯電防止剤とは、例えば持続性帯電防止剤や永久帯電防止剤と呼ばれるポリマ−タイプの帯電防止剤であり、具体的には、ポリエチレンオキシド、ポリプロピレンオキシド、ポリエチレングリコ−ル、ポリエステルアミド、ポリエ−テルエステルアミド、ポリエーテルポリオレフィン、エチレン-メタクリル酸共重合体などのアイオノマ−、ポリエチレングリコ−ルメタクリレ−ト系共重合体等の第四級アンモニウム塩から選択される1種、または2種以上の混合物、または2種以上の共重合体、更にそれらとポリプロピレンなどの他の樹脂との共重合体等の中で、分子鎖中に極性基を有し無機塩または低分子量有機プロトン酸塩を錯体形成または溶媒和することが可能な樹脂が挙げられ、無機塩または有機プロトン酸塩等を錯体形成または溶媒和せしめてあってもよい。この中でポリプロピレン系樹脂および環状ポリオレフィン系樹脂との相溶性や帯電防止性能の点からポリエーテルポリオレフィン、ポリエ−テルエステルアミドが好ましく、ポリエーテルポリオレフィンが特に好ましい。 The polymer type antistatic agent of the present invention is a polymer type antistatic agent called, for example, a long-lasting antistatic agent or a permanent antistatic agent, and specifically includes polyethylene oxide, polypropylene oxide, polyethylene glycol. A polyester amide, a polyether ester amide, a polyether polyolefin, an ionomer such as an ethylene-methacrylic acid copolymer, a quaternary ammonium salt such as a polyethylene glycol methacrylate copolymer, Or a mixture of two or more kinds, or two or more kinds of copolymers, and copolymers thereof with other resins such as polypropylene, etc., having a polar group in the molecular chain, or an inorganic salt or low molecular weight organic Examples include resins capable of complexing or solvating protonic acid salts such as inorganic salts or organic protonic acid salts. It may be complexed or solvated. Of these, polyether polyolefin and polyether ester amide are preferred, and polyether polyolefin is particularly preferred from the viewpoint of compatibility with polypropylene resin and cyclic polyolefin resin and antistatic performance.
高分子型帯電防止剤はポリプロピレン系樹脂60〜20重量%および環状ポリオレフィン系樹脂40〜80重量%からなる樹脂組成物100重量部に対して10〜20重量部であることが好ましい。高分子型帯電防止剤が10重量部より少ないと安定した所定の帯電防止性能が得られず、20重量部より多いと押出加工性が低下する上、それほど帯電防止性能の向上が認められず、コストアップになるので好ましくない。 The polymer type antistatic agent is preferably 10 to 20 parts by weight with respect to 100 parts by weight of a resin composition comprising 60 to 20% by weight of a polypropylene resin and 40 to 80% by weight of a cyclic polyolefin resin. If the amount of the polymer type antistatic agent is less than 10 parts by weight, stable predetermined antistatic performance cannot be obtained, and if it is more than 20 parts by weight, the extrusion processability is lowered, and the improvement in antistatic performance is not recognized so much. This is not preferable because it increases costs.
また、本発明の界面活性剤型帯電防止剤としては従来公知の化合物を用いることができる。例えば四級アンモニウム塩、ピリジン誘導体に代表される陽イオン界面活性剤、アルキル硫酸エステル塩、アルキル芳香属スルフォン酸塩、コハク酸スルフォン酸塩、リン酸エステル塩等に代表される陰イオン界面活性剤、多価アルコールの部分脂肪酸エステル及びそのエチレンオキサイド付加物、脂肪属アルコールのエチレンオキサイド付加物、脂肪属アミンのエチレンオキサイド付加物、脂肪酸アミドのエチレンオキサイド付加物、アルキルフェノールあるいはアルキルナフトールのエチレンオキサイド付加物に代表される非イオン界面活性剤、ベタイン形カルボン酸誘導体、イミダゾリン誘導体に代表される両性界面活性剤等が挙げられ、これらを単独で又は併用して用いる。なかでも本発明においては効果、取り扱いやすさ、人体への安全性から非イオン界面活性剤が好ましい。 Moreover, a conventionally well-known compound can be used as surfactant type antistatic agent of this invention. For example, cationic surfactants typified by quaternary ammonium salts, pyridine derivatives, alkyl sulfate esters, alkyl aromatic sulfonates, succinate sulfonates, phosphate esters, and the like , Partial fatty acid ester of polyhydric alcohol and its ethylene oxide adduct, ethylene oxide adduct of aliphatic alcohol, ethylene oxide adduct of aliphatic amine, ethylene oxide adduct of fatty acid amide, ethylene oxide adduct of alkylphenol or alkylnaphthol Nonionic surfactants typified by, amphoteric surfactants typified by betaine-type carboxylic acid derivatives, imidazoline derivatives, etc., are used alone or in combination. Of these, nonionic surfactants are preferred in the present invention from the viewpoints of effects, ease of handling, and safety to the human body.
非イオン性界面活性剤型帯電防止剤としては、特に限定されるものではないが、例えば、ポリエチレングリコール等のアルコール系帯電防止剤、ポリオキシエチレンアルキルエーテル、ポリオキシアルキレンアルキルエーテル等のエーテル系帯電防止剤、ソルビタン脂肪酸エステル、ポリオキシエチレンソルビタン脂肪酸エステル、ポリオキシエチレンソルビトール脂肪酸エステル、グリセリン脂肪酸エステル等のエステル系帯電防止剤、ポリオキシエチレンアルキルアミン等のアミン系帯電防止剤、ポリオキシエチレングリセリド等のグリセリン系帯電防止剤、アルキルアルカノールアミド等のアミド系帯電防止剤が挙げられ、ブリードアウト速度が速いという理由からアルコール系帯電防止剤やアミン系帯電防止剤が好ましく、ポリエチレングリコール、ポリオキシエチレンアルキルアミンがより好ましく、ポリオキシエチレンアルキルアミンが特に好ましい。なお、非イオン性界面活性剤型帯電防止剤は単独で用いられても併用されてもよい。 The nonionic surfactant type antistatic agent is not particularly limited. For example, an alcoholic antistatic agent such as polyethylene glycol, an ether-based charging agent such as polyoxyethylene alkyl ether or polyoxyalkylene alkyl ether, and the like. Antistatic agents, sorbitan fatty acid esters, polyoxyethylene sorbitan fatty acid esters, polyoxyethylene sorbitol fatty acid esters, ester antistatic agents such as glycerin fatty acid esters, amine-based antistatic agents such as polyoxyethylene alkylamine, polyoxyethylene glycerides, etc. Glycerin-based antistatic agents and amide-based antistatic agents such as alkyl alkanolamides. Alcohol-based antistatic agents and amine-based antistatic agents are preferred because of their high bleed-out speed. Glycol, polyoxyethylene alkylamines are more preferred, and polyoxyethylene alkyl amine is particularly preferred. The nonionic surfactant type antistatic agent may be used alone or in combination.
そして、上記界面活性剤型帯電防止剤の添加量は、多いと、得られるポリオレフィン系樹脂シートの表面がべたつき、又、少ないと、得られるポリオレフィン系樹脂シートの帯電防止性能が不足するので、ポリプロピレン系樹脂60〜20重量%および環状ポリオレフィン系樹脂40〜80重量%からなる樹脂組成物100重量部に対して0.2〜5重量部が好ましく、1〜4重量部がより好ましい。 If the amount of the surfactant type antistatic agent added is large, the surface of the resulting polyolefin resin sheet becomes sticky, and if it is small, the antistatic performance of the resulting polyolefin resin sheet is insufficient. The amount is preferably 0.2 to 5 parts by weight, more preferably 1 to 4 parts by weight with respect to 100 parts by weight of the resin composition comprising 60 to 20% by weight of the resin based on resin and 40 to 80% by weight of the cyclic polyolefin resin.
本発明において、必要であれば着色剤や光遮断剤を添加してもかまわない。このような着色剤や光遮断剤は例えば、カーボンブラック、酸化チタン、酸化亜鉛、酸化鉄、酸化アルミ等の無機物質、シアニンブルー、シアニングリーン、ミロリブルー、スレンブルー、カドミウムレッド、カドミウムイエロー、カドミウムオレンジ、弁柄、群青、フタロシアニンブルー等の顔料等があげられる。これらは直接添加してもかわまいないが、作業性の点からマスターバッチ化したものを用いることが好ましい。また、マスターバッチのベース樹脂はLDPEやPPなどが好ましい。 In the present invention, if necessary, a colorant or a light blocking agent may be added. Such colorants and light blocking agents include, for example, inorganic materials such as carbon black, titanium oxide, zinc oxide, iron oxide, aluminum oxide, cyanine blue, cyanine green, miloli blue, selenium blue, cadmium red, cadmium yellow, cadmium orange. And pigments such as petals, ultramarine blue, and phthalocyanine blue. These may be added directly, but it is preferable to use a master batch from the viewpoint of workability. The base resin of the master batch is preferably LDPE or PP.
また、必要に応じて酸化防止剤や劣化防止剤、紫外線吸収剤などの安定剤を添加してもかまわない。 Moreover, you may add stabilizers, such as antioxidant, a deterioration inhibitor, and an ultraviolet absorber, as needed.
(製造方法)
本発明のポリオレフィン系樹脂シートは、押出機内で上記樹脂組成物と帯電防止剤とを溶融混練し、押出機の先端に取付けた金型から大気中へ押出すことにより得ることができる。より具体的には、押出機先端にTダイを取り付け、そこから押出したシートを冷却ドラム(冷却ロール)で成形する製造方法、あるいは、押出機先端にサーキュラー金型を取り付け、そこから押出した円筒状シートをマンドレルで成形した後、切開してシート状とする製造方法のどちらも適用することができる。
(Production method)
The polyolefin-based resin sheet of the present invention can be obtained by melt-kneading the resin composition and the antistatic agent in an extruder and extruding it into the atmosphere from a mold attached to the tip of the extruder. More specifically, a manufacturing method in which a T-die is attached to the tip of the extruder and a sheet extruded therefrom is formed by a cooling drum (cooling roll), or a circular die is attached to the tip of the extruder and extruded from there. Either of the manufacturing methods in which a sheet-like sheet is formed with a mandrel and then cut into a sheet form can be applied.
本発明のポリオレフィン系樹脂シートは、JIS K6911 5.13に準拠して温度22℃、湿度65%のときの表面固有抵抗値が1×1013(Ω)未満である。表面固有抵抗値が1×1013(Ω)を超えると、電子部品の包装材として用いた時に静電気によって被包装物が破壊する恐れがある。 The polyolefin resin sheet of the present invention has a surface resistivity of less than 1 × 10 13 (Ω) when the temperature is 22 ° C. and the humidity is 65% in accordance with JIS K6911 5.13. If the surface specific resistance value exceeds 1 × 10 13 (Ω), the package may be destroyed by static electricity when used as a packaging material for electronic components.
本発明のポリオレフィン系樹脂シートの厚みは、0.3〜3mmの範囲が好ましく、0.5〜2mmの範囲がより好ましい。シートの厚みが0.3mm未満の場合は、成形性が悪く、成形品の強度が不足する恐れがある。3mmを超えるものは、成形性が悪く、成形品が重くなるので好ましくない。 The range of 0.3-3 mm is preferable and, as for the thickness of the polyolefin resin sheet of this invention, the range of 0.5-2 mm is more preferable. When the thickness of the sheet is less than 0.3 mm, the moldability is poor and the strength of the molded product may be insufficient. Those exceeding 3 mm are not preferable because the moldability is poor and the molded product becomes heavy.
以下、本発明を実施例及び比較例に基づいて詳細な説明する。
(実施例1)
メルトフローレートが2.5g/10分であるポリプロピレン系樹脂(日本ポリプロ社製 BC6C)60重量部と、ガラス転移温度が138℃である環状ポリオレフィン(日本ゼオン社製 ゼオネックス480R)40重量部に、密度が0.88g/cm3であるエチレン−α−オレフィン共重合体樹脂(日本ポリエチレン社製 カーネルKS240T)を20重量部、非イオン性界面活性剤(ポリオキシエチレンアルキルアミン型非イオン性界面活性剤)(花王社製 TS−2B)を2重量部添加してブレンダーで混合した。その後、シリンダ温度を220℃に維持した単軸押出機((口径65mmφ(L/D=37)の単軸押出機)に供給してシリンダ内で溶融、混練した。
次にこの押出機に接続したTダイ(幅300mm、スリット幅0.6mm)から下向きに押し出し、30℃の水で温度調整された、Tダイから100mmのところに敷設した2つの直径150mmφの冷却ドラム(ドラム間隔1.0mm、ドラム冷却温度40℃)で押出溶融物を冷却固化させてポリオレフィン系シ−トを得た。得られたシ−トの幅は270mmで厚みは1.0mmであった。
得られたシ−トの表面温度が170℃になるようにオ−ブンで加熱し、その後アルミで作られたカップ形状のマッチド型でプレスした後、10秒後にマッチド型を離型して離型性を確認した。成形品はマッチド型についたり、破れたりすることなく、離型性および成形性は良好であった。
Hereinafter, the present invention will be described in detail based on examples and comparative examples.
Example 1
To 60 parts by weight of a polypropylene resin (BC6C manufactured by Nippon Polypro Co., Ltd.) having a melt flow rate of 2.5 g / 10 min and 40 parts by weight of a cyclic polyolefin (ZEONEX 480R manufactured by Nippon Zeon Co., Ltd.) having a glass transition temperature of 138 ° C. 20 parts by weight of ethylene-α-olefin copolymer resin (Nippon Polyethylene Kernel KS240T) having a density of 0.88 g / cm 3 , nonionic surfactant (polyoxyethylene alkylamine type nonionic surfactant) 2 parts by weight of (agent) (TS-2B manufactured by Kao Corporation) was added and mixed with a blender. Thereafter, the cylinder was supplied to a single screw extruder (a single screw extruder having a diameter of 65 mmφ (L / D = 37)) maintained at 220 ° C. and melted and kneaded in the cylinder.
Next, it was extruded downward from a T-die (width 300 mm, slit width 0.6 mm) connected to this extruder, and the temperature was adjusted with water at 30 ° C. Two coolings with a diameter of 150 mmφ laid at 100 mm from the T-die The extruded melt was cooled and solidified with a drum (drum interval 1.0 mm, drum cooling temperature 40 ° C.) to obtain a polyolefin sheet. The obtained sheet had a width of 270 mm and a thickness of 1.0 mm.
The resulting sheet is heated in an oven so that the surface temperature becomes 170 ° C., and then pressed with a cup-shaped matched mold made of aluminum, and after 10 seconds, the matched mold is released and released. The type was confirmed. The molded product did not attach to the matched mold or was not torn, and the mold release and moldability were good.
(実施例2)
ポリプロピレン系樹脂の割合を20重量部、環状ポリオレフィン系樹脂の割合を80重量部としたこと以外は、実施例1と同様にしてポリオレフィン系シ−トを得た。得られたシ−トの幅は280mmで厚みは1.0mmであった。
得られたシ−トの表面温度が170℃になるようにオ−ブンで加熱し、その後アルミで作られたカップ形状のマッチド型でプレスした後、10秒後にマッチド型を離型して離型性を確認した。成形品はマッチド型についたり、破れたりすることなく、離型性および成形性は良好であった。
(Example 2)
A polyolefin sheet was obtained in the same manner as in Example 1 except that the proportion of the polypropylene resin was 20 parts by weight and the proportion of the cyclic polyolefin resin was 80 parts by weight. The obtained sheet had a width of 280 mm and a thickness of 1.0 mm.
The resulting sheet is heated in an oven so that the surface temperature becomes 170 ° C., and then pressed with a cup-shaped matched mold made of aluminum, and after 10 seconds, the matched mold is released and released. The type was confirmed. The molded product did not attach to the matched mold or was not torn, and the mold release and moldability were good.
(実施例3)
エチレン−α−オレフィン共重合体樹脂の添加量を10重量部としたこと以外は、実施例1と同様にしてポリオレフィン系シ−トを得た。得られたシ−トの幅は270mmで厚みは1.0mmであった。
得られたシ−トの表面温度が170℃になるようにオ−ブンで加熱し、その後アルミで作られたカップ形状のマッチド型でプレスした後、10秒後にマッチド型を離型して離型性を確認した。成形品はマッチド型についたり、破れたりすることなく、離型性および成形性は良好であった。
(Example 3)
A polyolefin sheet was obtained in the same manner as in Example 1 except that the addition amount of the ethylene-α-olefin copolymer resin was 10 parts by weight. The obtained sheet had a width of 270 mm and a thickness of 1.0 mm.
The resulting sheet is heated in an oven so that the surface temperature becomes 170 ° C., and then pressed with a cup-shaped matched mold made of aluminum, and after 10 seconds, the matched mold is released and released. The type was confirmed. The molded product did not attach to the matched mold or was not torn, and the mold release and moldability were good.
(実施例4)
帯電防止剤の添加量を0.3重量部としたこと以外は、実施例1と同様にしてポリオレフィン系シ−トを得た。得られたシ−トの幅は270mmで厚みは1.0mmであった。
得られたシ−トの表面温度が170℃になるようにオ−ブンで加熱し、その後アルミで作られたカップ形状のマッチド型でプレスした後、10秒後にマッチド型を離型して離型性を確認した。成形品はマッチド型についたり、破れたりすることなく、離型性および成形性は良好であった。
Example 4
A polyolefin sheet was obtained in the same manner as in Example 1 except that the addition amount of the antistatic agent was 0.3 parts by weight. The obtained sheet had a width of 270 mm and a thickness of 1.0 mm.
The resulting sheet is heated in an oven so that the surface temperature becomes 170 ° C., and then pressed with a cup-shaped matched mold made of aluminum, and after 10 seconds, the matched mold is released and released. The type was confirmed. The molded product did not attach to the matched mold or was not torn, and the mold release and moldability were good.
(実施例5)
帯電防止剤の添加量を4重量部としたこと以外は、実施例1と同様にしてポリオレフィン系シートを得た。得られたシートの幅は270mmで厚みは1.0mmであった。
得られたシートの表面温度が170℃になるようにオーブンで加熱し、その後アルミで作られたカップ形状のマッチド型でプレスした後、10秒後にマッチド型を離型して離型性を確認した。成形品はマッチド型についたり、破れたりすることなく、離型性および成形性は良好であった。
(Example 5)
A polyolefin-based sheet was obtained in the same manner as in Example 1 except that the addition amount of the antistatic agent was 4 parts by weight. The width of the obtained sheet was 270 mm and the thickness was 1.0 mm.
The obtained sheet is heated in an oven so that the surface temperature becomes 170 ° C., then pressed with a cup-shaped matched mold made of aluminum, and then the mold is released after 10 seconds to confirm the releasability. did. The molded product did not attach to the matched mold or was not torn, and the mold release and moldability were good.
(実施例6)
帯電防止剤を陰イオン性界面活性剤(アルキルスルホン酸ナトリウム)(大日精化社製 エレコンSS700)にしたこと以外は、実施例1と同様にしてポリオレフィン系シートを得た。得られたシートの幅は270mmで厚みは1.0mmであった。
得られたシートの表面温度が170℃になるようにオーブンで加熱し、その後アルミで作られたカップ形状のマッチド型でプレスした後、10秒後にマッチド型を離型して離型性を確認した。成形品はマッチド型についたり、破れたりすることなく、離型性および成形性は良好であった。
(Example 6)
A polyolefin-based sheet was obtained in the same manner as in Example 1 except that the antistatic agent was an anionic surfactant (sodium alkyl sulfonate) (ELECON SS700 manufactured by Dainichi Seika Co., Ltd.). The width of the obtained sheet was 270 mm and the thickness was 1.0 mm.
The obtained sheet is heated in an oven so that the surface temperature becomes 170 ° C., then pressed with a cup-shaped matched mold made of aluminum, and then the mold is released after 10 seconds to confirm the releasability. did. The molded product did not attach to the matched mold or was not torn, and the mold release and moldability were good.
(実施例7)
帯電防止剤として高分子型帯電防止剤(ポリエーテルポリオレフィン型高分子帯電防止剤)(三洋化成社製ペレスタット300)を12重量部添加したこと以外は、実施例1と同様にしてポリオレフィン系シートを得た。得られたシートの幅は280 mmで厚みは1.0mmであった。
得られたシートの表面温度が170℃になるようにオーブンで加熱し、その後アルミで作られたカップ形状のマッチド型でプレスした後、10秒後にマッチド型を離型して離型性を確認した。成形品はマッチド型についたり、破れたりすることなく、離型性および成形性は良好であった。
(Example 7)
A polyolefin sheet was prepared in the same manner as in Example 1 except that 12 parts by weight of a polymer type antistatic agent (polyether polyolefin type polymer antistatic agent) (Pelestat 300 manufactured by Sanyo Kasei Co., Ltd.) was added as an antistatic agent. Obtained. The obtained sheet had a width of 280 mm and a thickness of 1.0 mm.
The obtained sheet is heated in an oven so that the surface temperature becomes 170 ° C., then pressed with a cup-shaped matched mold made of aluminum, and then the mold is released after 10 seconds to confirm the releasability. did. The molded product did not attach to the matched mold or was not torn, and the mold release and moldability were good.
(実施例8)
帯電防止剤の添加量を20重量部添加したこと以外は、実施例7と同様にしてポリオレフィン系シートを得た。得られたシートの幅は280mmで厚みは1.0mmであった。
得られたシートの表面温度が170℃になるようにオーブンで加熱し、その後アルミで作られたカップ形状のマッチド型でプレスした後、10秒後にマッチド型を離型して離型性を確認した。成形品はマッチド型についたり、破れたりすることなく、離型性および成形性は良好であった。
(Example 8)
A polyolefin-based sheet was obtained in the same manner as in Example 7 except that 20 parts by weight of the antistatic agent was added. The width of the obtained sheet was 280 mm and the thickness was 1.0 mm.
The obtained sheet is heated in an oven so that the surface temperature becomes 170 ° C., then pressed with a cup-shaped matched mold made of aluminum, and then the mold is released after 10 seconds to confirm the releasability. did. The molded product did not attach to the matched mold or was not torn, and the mold release and moldability were good.
(比較例1)
エチレン−α−オレフィン共重合体樹脂を添加しなかったこと以外は、実施例1と同様にしてポリオレフィン系シ−トを得た。得られたシ−トの幅は270mmで厚みは1.0mmであった。
得られたシ−トの表面温度が170℃になるようにオ−ブンで加熱し、その後アルミで作られたカップ形状のマッチド型でプレスした後、10秒後にマッチド型を離型して離型性を確認した。成形品はマッチド型についたり、破れたりすることなく、離型性および成形性は良好であった。
(Comparative Example 1)
A polyolefin sheet was obtained in the same manner as in Example 1 except that the ethylene-α-olefin copolymer resin was not added. The obtained sheet had a width of 270 mm and a thickness of 1.0 mm.
The resulting sheet is heated in an oven so that the surface temperature becomes 170 ° C., and then pressed with a cup-shaped matched mold made of aluminum, and after 10 seconds, the matched mold is released and released. The type was confirmed. The molded product did not attach to the matched mold or was not torn, and the mold release and moldability were good.
(比較例2)
ポリプロピレン系樹脂の割合を10重量部、環状ポリオレフィン系樹脂の割合を90重量部としたこと以外は、実施例1と同様にしてポリオレフィン系シ−トを得た。得られたシ−トの幅は280mmで厚みは1.0mmであった。
得られたシ−トの表面温度が170℃になるようにオ−ブンで加熱し、その後アルミで作られたカップ形状のマッチド型でプレスした後、10秒後にマッチド型を離型して離型性を確認した。成形品はマッチド型に貼りつき、その後離型したために随所にシワが入っていた。また、マッチド型のプレス時のシート伸びが悪く、カップ側壁の部分にスジ状の破れが生じていた。
(Comparative Example 2)
A polyolefin sheet was obtained in the same manner as in Example 1 except that the proportion of the polypropylene resin was 10 parts by weight and the proportion of the cyclic polyolefin resin was 90 parts by weight. The obtained sheet had a width of 280 mm and a thickness of 1.0 mm.
The resulting sheet is heated in an oven so that the surface temperature becomes 170 ° C., and then pressed with a cup-shaped matched mold made of aluminum, and after 10 seconds, the matched mold is released and released. The type was confirmed. The molded product was stuck to the matched mold and then released, so wrinkles were found everywhere. Further, the sheet elongation at the time of the matched-type pressing was poor, and streaky tearing occurred at the cup side wall.
(比較例3)
帯電防止剤の添加量を0.1重量部としたこと以外は、実施例1と同様にしてポリオレフィン系シートを得た。得られたシートの幅は270mmで厚みは1.0mmであった。
得られたシートの表面温度が170℃になるようにオーブンで加熱し、その後アルミで作られたカップ形状のマッチド型でプレスした後、10秒後にマッチド型を離型して離型性を確認した。成形品はマッチド型についたり、破れたりすることなく、離型性および成形性は良好であった。
(Comparative Example 3)
A polyolefin-based sheet was obtained in the same manner as in Example 1 except that the addition amount of the antistatic agent was 0.1 parts by weight. The obtained sheet had a width of 270 mm and a thickness of 1.0 mm.
The obtained sheet is heated in an oven so that the surface temperature becomes 170 ° C., then pressed with a cup-shaped matched mold made of aluminum, and then the mold is released after 10 seconds to confirm the releasability. did. The molded product did not attach to the matched mold or was not torn, and the mold release and moldability were good.
(比較例4)
帯電防止剤の添加量を7重量部としたこと以外は、実施例1と同様にしてポリオレフィン系シートを押出した。しかし押出時に原料供給部で帯電防止剤がスリップしてしまい、安定してシートを得ることが困難であった。また、一時的に得られたシートの表面がべとついていた。
(Comparative Example 4)
A polyolefin-based sheet was extruded in the same manner as in Example 1 except that the addition amount of the antistatic agent was 7 parts by weight. However, the antistatic agent slips at the raw material supply part during extrusion, and it is difficult to obtain a sheet stably. Further, the surface of the temporarily obtained sheet was sticky.
(比較例5)
帯電防止剤の添加量を8重量部としたこと以外は、実施例7と同様にしてポリオレフィン系シートを押出した。得られたシートの幅は280mmで厚みは1.0mmであった。
得られたシートの表面温度が170℃になるようにオーブンで加熱し、その後アルミで作られたカップ形状のマッチド型でプレスした後、10秒後にマッチド型を離型して離型性を確認した。成形品はマッチド型についたり、破れたりすることなく、離型性および成形性は良好であった。
(Comparative Example 5)
A polyolefin-based sheet was extruded in the same manner as in Example 7 except that the addition amount of the antistatic agent was 8 parts by weight. The obtained sheet had a width of 280 mm and a thickness of 1.0 mm.
The obtained sheet is heated in an oven so that the surface temperature becomes 170 ° C., then pressed with a cup-shaped matched mold made of aluminum, and then the mold is released after 10 seconds to confirm the releasability. did. The molded product did not attach to the matched mold or was not torn, and the mold release and moldability were good.
以下の表1に実施例1〜8、比較例1〜2のシート幅、シート厚み、表面固有低効率、穿孔衝撃値、熱成形時の成形性をまとめて記載した。いずれも実施例が比較例と比較して良好であることが認められる。 Table 1 below summarizes the sheet width, sheet thickness, surface intrinsic low efficiency, perforation impact value, and moldability during thermoforming of Examples 1 to 8 and Comparative Examples 1 and 2. In any case, it is recognized that the examples are better than the comparative examples.
[各測定方法]
(表面固有抵抗率)
表面固有抵抗率測定装置(ADVANTEST社製 商品名「ULTRA HIGH RESISTANCE METER」を用いてJIS K6911 5.13に準拠して測定した。具体的には、一辺が10cmの平面正方形状の試験片を温度22℃、湿度65%の雰囲気下に24時間放置した後、この試験片を表面固有抵抗率測定装置にセットして500Vの電圧を試験片に印加して1分経過後の表面固有抵抗率を測定した。
[Each measurement method]
(Surface specific resistivity)
Surface specific resistivity measuring device (measured in accordance with JIS K6911 5.13 using a trade name “ULTRA HIGH RESISTANCE METER” manufactured by ADVANTEST Co. After being left for 24 hours in an atmosphere of 22 ° C. and 65% humidity, this test piece is set in a surface resistivity measuring apparatus, a voltage of 500 V is applied to the test piece, and the surface resistivity after one minute has elapsed. It was measured.
(穿孔衝撃値)
試験片を150mm角の発泡体とした以外は、板紙の衝突穴あけ強さ試験(穿孔衝撃試験)であるJIS P 8134に従って測定した。また、試験数は10個で、その平均値を採った。
(Drilling impact value)
The test piece was measured in accordance with JIS P 8134, which is a paperboard impact punching strength test (piercing impact test), except that a 150 mm square foam was used. The number of tests was 10, and the average value was taken.
(熱成形時の離型性)
φ100mmの開口部、φ80mmの底部を有し、深さ150mmのタテ型カップ形状のマッチド型にて、表面温度が170℃に加熱されたシートをプレス成形した後、10秒後にマッチド型を離型して目視にて離型性を確認した。離型時にマッチド型からの離型が良好である場合を離型性○とし、離型時にマッチド型からの離型が悪く、シワが入ったり、所定深さのカップが得られなかった場合を離型性×とした。また成形品が破れた場合を×、そうでない場合を○で示している。いずれも目視にて確認したものである。
(Releasability during thermoforming)
After press forming a sheet heated to a surface temperature of 170 ° C in a vertical cup-shaped matched mold having a φ100 mm opening and a φ80 mm bottom and a depth of 150 mm, the matched mold is released after 10 seconds. Then, the releasability was confirmed visually. When the mold release from the matched mold is good at the time of mold release, the mold release property ○, when the mold release from the matched mold is bad, wrinkles or a cup of the predetermined depth is not obtained Releasability x. In addition, the case where the molded product is torn is indicated by x, and the case where it is not is indicated by ◯. Both were confirmed visually.
Claims (4)
エチレン−α−オレフィン共重合体樹脂5〜30重量部とを含み、
帯電防止剤を含み、
JIS K6911 5.13に準拠した温度22℃、湿度65%のときの表面固有抵抗率が1×1013(Ω)未満であり、
前記エチレン−α−オレフィン共重合体樹脂のα−オレフィンは炭素数が4〜8のα―オレフィンである
ポリオレフィン系樹脂シート。 With respect to 100 parts by weight of a resin composition comprising 60 to 20% by weight of a polypropylene resin and 40 to 80% by weight of a cyclic polyolefin resin,
And 5 to 30 parts by weight of an ethylene-α-olefin copolymer resin,
Contains antistatic agents,
JIS K6911 5.13 Temperature 22 ° C. conforming to, Ri surface resistivity is 1 × 10 13 (Ω) under der when the 65% humidity,
The polyolefin resin sheet, wherein the α-olefin of the ethylene-α-olefin copolymer resin is an α-olefin having 4 to 8 carbon atoms .
A polyolefin resin sheet molded article obtained by thermoforming the polyolefin resin sheet according to any one of claims 1 to 3.
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