CN103249554B - 层叠体 - Google Patents
层叠体 Download PDFInfo
- Publication number
- CN103249554B CN103249554B CN201180054477.2A CN201180054477A CN103249554B CN 103249554 B CN103249554 B CN 103249554B CN 201180054477 A CN201180054477 A CN 201180054477A CN 103249554 B CN103249554 B CN 103249554B
- Authority
- CN
- China
- Prior art keywords
- layer
- diazabicylo
- sulphur
- duplexer
- rubber
- Prior art date
- Legal status (The legal status is an assumption and is not a legal conclusion. Google has not performed a legal analysis and makes no representation as to the accuracy of the status listed.)
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- 229920001971 elastomer Polymers 0.000 claims abstract description 129
- 239000005060 rubber Substances 0.000 claims abstract description 128
- 239000000203 mixture Substances 0.000 claims abstract description 56
- 239000004811 fluoropolymer Substances 0.000 claims abstract description 39
- 229920002313 fluoropolymer Polymers 0.000 claims abstract description 39
- UUAGAQFQZIEFAH-UHFFFAOYSA-N chlorotrifluoroethylene Chemical group FC(F)=C(F)Cl UUAGAQFQZIEFAH-UHFFFAOYSA-N 0.000 claims abstract description 31
- 150000001875 compounds Chemical class 0.000 claims abstract description 30
- 239000003822 epoxy resin Substances 0.000 claims abstract description 22
- 229920000647 polyepoxide Polymers 0.000 claims abstract description 22
- 150000003839 salts Chemical class 0.000 claims abstract description 10
- NINIDFKCEFEMDL-UHFFFAOYSA-N Sulfur Chemical compound [S] NINIDFKCEFEMDL-UHFFFAOYSA-N 0.000 claims description 159
- 239000005864 Sulphur Substances 0.000 claims description 159
- 239000010410 layer Substances 0.000 claims description 153
- 239000003795 chemical substances by application Substances 0.000 claims description 73
- 239000000446 fuel Substances 0.000 claims description 49
- RZQNBTMGBODDSK-UWVGGRQHSA-N ethyl (2r)-2-[2-[[(2r)-1-ethoxy-1-oxo-3-sulfanylpropan-2-yl]amino]ethylamino]-3-sulfanylpropanoate Chemical compound CCOC(=O)[C@H](CS)NCCN[C@@H](CS)C(=O)OCC RZQNBTMGBODDSK-UWVGGRQHSA-N 0.000 claims description 39
- -1 alkyl vinyl ether Chemical compound 0.000 claims description 34
- 229910052751 metal Inorganic materials 0.000 claims description 16
- 239000002184 metal Substances 0.000 claims description 16
- IISBACLAFKSPIT-UHFFFAOYSA-N bisphenol A Chemical compound C=1C=C(O)C=CC=1C(C)(C)C1=CC=C(O)C=C1 IISBACLAFKSPIT-UHFFFAOYSA-N 0.000 claims description 14
- XSCHRSMBECNVNS-UHFFFAOYSA-N quinoxaline Chemical compound N1=CC=NC2=CC=CC=C21 XSCHRSMBECNVNS-UHFFFAOYSA-N 0.000 claims description 14
- UMGDCJDMYOKAJW-UHFFFAOYSA-N thiourea Chemical compound NC(N)=S UMGDCJDMYOKAJW-UHFFFAOYSA-N 0.000 claims description 14
- 238000007334 copolymerization reaction Methods 0.000 claims description 12
- LRWZZZWJMFNZIK-UHFFFAOYSA-N 2-chloro-3-methyloxirane Chemical compound CC1OC1Cl LRWZZZWJMFNZIK-UHFFFAOYSA-N 0.000 claims description 10
- 239000013047 polymeric layer Substances 0.000 claims description 9
- 229930185605 Bisphenol Natural products 0.000 claims description 7
- 229920000459 Nitrile rubber Polymers 0.000 claims description 7
- WPYMKLBDIGXBTP-UHFFFAOYSA-N benzoic acid Chemical compound OC(=O)C1=CC=CC=C1 WPYMKLBDIGXBTP-UHFFFAOYSA-N 0.000 claims description 6
- KXGFMDJXCMQABM-UHFFFAOYSA-N 2-methoxy-6-methylphenol Chemical class [CH]OC1=CC=CC([CH])=C1O KXGFMDJXCMQABM-UHFFFAOYSA-N 0.000 claims description 5
- 150000001732 carboxylic acid derivatives Chemical class 0.000 claims description 5
- ISWSIDIOOBJBQZ-UHFFFAOYSA-M phenolate Chemical compound [O-]C1=CC=CC=C1 ISWSIDIOOBJBQZ-UHFFFAOYSA-M 0.000 claims description 5
- 229940031826 phenolate Drugs 0.000 claims description 5
- XNGIFLGASWRNHJ-UHFFFAOYSA-L phthalate(2-) Chemical compound [O-]C(=O)C1=CC=CC=C1C([O-])=O XNGIFLGASWRNHJ-UHFFFAOYSA-L 0.000 claims description 5
- STMDPCBYJCIZOD-UHFFFAOYSA-N 2-(2,4-dinitroanilino)-4-methylpentanoic acid Chemical compound CC(C)CC(C(O)=O)NC1=CC=C([N+]([O-])=O)C=C1[N+]([O-])=O STMDPCBYJCIZOD-UHFFFAOYSA-N 0.000 claims description 4
- RYGMFSIKBFXOCR-UHFFFAOYSA-N Copper Chemical compound [Cu] RYGMFSIKBFXOCR-UHFFFAOYSA-N 0.000 claims description 4
- BDAGIHXWWSANSR-UHFFFAOYSA-M Formate Chemical compound [O-]C=O BDAGIHXWWSANSR-UHFFFAOYSA-M 0.000 claims description 4
- QAOWNCQODCNURD-UHFFFAOYSA-L Sulfate Chemical compound [O-]S([O-])(=O)=O QAOWNCQODCNURD-UHFFFAOYSA-L 0.000 claims description 4
- 229910052802 copper Inorganic materials 0.000 claims description 4
- 239000010949 copper Substances 0.000 claims description 4
- 150000001879 copper Chemical class 0.000 claims description 4
- WWZKQHOCKIZLMA-UHFFFAOYSA-M octanoate Chemical compound CCCCCCCC([O-])=O WWZKQHOCKIZLMA-UHFFFAOYSA-M 0.000 claims description 4
- 229910052717 sulfur Inorganic materials 0.000 claims description 4
- 239000011593 sulfur Substances 0.000 claims description 4
- 229950004288 tosilate Drugs 0.000 claims description 4
- OYPRJOBELJOOCE-UHFFFAOYSA-N Calcium Chemical compound [Ca] OYPRJOBELJOOCE-UHFFFAOYSA-N 0.000 claims description 3
- IAYPIBMASNFSPL-UHFFFAOYSA-N Ethylene oxide Chemical compound C1CO1 IAYPIBMASNFSPL-UHFFFAOYSA-N 0.000 claims description 3
- FYYHWMGAXLPEAU-UHFFFAOYSA-N Magnesium Chemical compound [Mg] FYYHWMGAXLPEAU-UHFFFAOYSA-N 0.000 claims description 3
- 239000011575 calcium Substances 0.000 claims description 3
- 229910052791 calcium Inorganic materials 0.000 claims description 3
- IXPUJMULXNNEHS-UHFFFAOYSA-L copper;n,n-dibutylcarbamodithioate Chemical compound [Cu+2].CCCCN(C([S-])=S)CCCC.CCCCN(C([S-])=S)CCCC IXPUJMULXNNEHS-UHFFFAOYSA-L 0.000 claims description 3
- OBBCYCYCTJQCCK-UHFFFAOYSA-L copper;n,n-diethylcarbamodithioate Chemical compound [Cu+2].CCN(CC)C([S-])=S.CCN(CC)C([S-])=S OBBCYCYCTJQCCK-UHFFFAOYSA-L 0.000 claims description 3
- MZGNSEAPZQGJRB-UHFFFAOYSA-N dimethyldithiocarbamic acid Chemical compound CN(C)C(S)=S MZGNSEAPZQGJRB-UHFFFAOYSA-N 0.000 claims description 3
- 150000004678 hydrides Chemical class 0.000 claims description 3
- 239000011777 magnesium Substances 0.000 claims description 3
- 229910052749 magnesium Inorganic materials 0.000 claims description 3
- 229920006395 saturated elastomer Polymers 0.000 claims description 3
- JXSRRBVHLUJJFC-UHFFFAOYSA-N 7-amino-2-methylsulfanyl-[1,2,4]triazolo[1,5-a]pyrimidine-6-carbonitrile Chemical compound N1=CC(C#N)=C(N)N2N=C(SC)N=C21 JXSRRBVHLUJJFC-UHFFFAOYSA-N 0.000 claims description 2
- QTBSBXVTEAMEQO-UHFFFAOYSA-M Acetate Chemical compound CC([O-])=O QTBSBXVTEAMEQO-UHFFFAOYSA-M 0.000 claims description 2
- DGAQECJNVWCQMB-PUAWFVPOSA-M Ilexoside XXIX Chemical compound C[C@@H]1CC[C@@]2(CC[C@@]3(C(=CC[C@H]4[C@]3(CC[C@@H]5[C@@]4(CC[C@@H](C5(C)C)OS(=O)(=O)[O-])C)C)[C@@H]2[C@]1(C)O)C)C(=O)O[C@H]6[C@@H]([C@H]([C@@H]([C@H](O6)CO)O)O)O.[Na+] DGAQECJNVWCQMB-PUAWFVPOSA-M 0.000 claims description 2
- 229910052708 sodium Inorganic materials 0.000 claims description 2
- 239000011734 sodium Substances 0.000 claims description 2
- GNVMUORYQLCPJZ-UHFFFAOYSA-N carbamothioic s-acid Chemical compound NC(S)=O GNVMUORYQLCPJZ-UHFFFAOYSA-N 0.000 claims 1
- 239000000126 substance Substances 0.000 abstract description 24
- XLYOFNOQVPJJNP-UHFFFAOYSA-N water Substances O XLYOFNOQVPJJNP-UHFFFAOYSA-N 0.000 abstract description 22
- 229920001577 copolymer Polymers 0.000 abstract description 4
- 238000004073 vulcanization Methods 0.000 abstract description 3
- GQHTUMJGOHRCHB-UHFFFAOYSA-N 2,3,4,6,7,8,9,10-octahydropyrimido[1,2-a]azepine Chemical compound C1CCCCN2CCCN=C21 GQHTUMJGOHRCHB-UHFFFAOYSA-N 0.000 abstract 1
- 229920005558 epichlorohydrin rubber Polymers 0.000 abstract 1
- 238000000034 method Methods 0.000 description 31
- 230000004888 barrier function Effects 0.000 description 23
- 239000000178 monomer Substances 0.000 description 23
- 229920005989 resin Polymers 0.000 description 23
- 239000011347 resin Substances 0.000 description 23
- 239000003921 oil Substances 0.000 description 21
- MTHSVFCYNBDYFN-UHFFFAOYSA-N diethylene glycol Chemical compound OCCOCCO MTHSVFCYNBDYFN-UHFFFAOYSA-N 0.000 description 16
- 230000035699 permeability Effects 0.000 description 16
- BFKJFAAPBSQJPD-UHFFFAOYSA-N tetrafluoroethene Chemical compound FC(F)=C(F)F BFKJFAAPBSQJPD-UHFFFAOYSA-N 0.000 description 13
- 239000000463 material Substances 0.000 description 12
- 238000007789 sealing Methods 0.000 description 12
- 229910052799 carbon Inorganic materials 0.000 description 10
- 239000000843 powder Substances 0.000 description 10
- OKTJSMMVPCPJKN-UHFFFAOYSA-N Carbon Chemical compound [C] OKTJSMMVPCPJKN-UHFFFAOYSA-N 0.000 description 9
- LFQSCWFLJHTTHZ-UHFFFAOYSA-N Ethanol Chemical compound CCO LFQSCWFLJHTTHZ-UHFFFAOYSA-N 0.000 description 9
- YXFVVABEGXRONW-UHFFFAOYSA-N Toluene Chemical compound CC1=CC=CC=C1 YXFVVABEGXRONW-UHFFFAOYSA-N 0.000 description 9
- 229960002447 thiram Drugs 0.000 description 9
- 150000001412 amines Chemical class 0.000 description 8
- OSGAYBCDTDRGGQ-UHFFFAOYSA-L calcium sulfate Chemical compound [Ca+2].[O-]S([O-])(=O)=O OSGAYBCDTDRGGQ-UHFFFAOYSA-L 0.000 description 8
- 238000004132 cross linking Methods 0.000 description 8
- 229920000642 polymer Polymers 0.000 description 8
- 230000008569 process Effects 0.000 description 8
- 239000003566 sealing material Substances 0.000 description 8
- BQCIDUSAKPWEOX-UHFFFAOYSA-N 1,1-Difluoroethene Chemical compound FC(F)=C BQCIDUSAKPWEOX-UHFFFAOYSA-N 0.000 description 7
- ZRALSGWEFCBTJO-UHFFFAOYSA-N Guanidine Chemical compound NC(N)=N ZRALSGWEFCBTJO-UHFFFAOYSA-N 0.000 description 7
- 239000000654 additive Substances 0.000 description 7
- 238000010438 heat treatment Methods 0.000 description 7
- KUAZQDVKQLNFPE-UHFFFAOYSA-N thiram Chemical compound CN(C)C(=S)SSC(=S)N(C)C KUAZQDVKQLNFPE-UHFFFAOYSA-N 0.000 description 7
- 239000012190 activator Substances 0.000 description 6
- 230000005540 biological transmission Effects 0.000 description 6
- DKVNPHBNOWQYFE-UHFFFAOYSA-N carbamodithioic acid Chemical compound NC(S)=S DKVNPHBNOWQYFE-UHFFFAOYSA-N 0.000 description 6
- 150000001735 carboxylic acids Chemical class 0.000 description 6
- 229910052801 chlorine Inorganic materials 0.000 description 6
- KRKNYBCHXYNGOX-UHFFFAOYSA-N citric acid Chemical compound OC(=O)CC(O)(C(O)=O)CC(O)=O KRKNYBCHXYNGOX-UHFFFAOYSA-N 0.000 description 6
- 238000001125 extrusion Methods 0.000 description 6
- 239000011229 interlayer Substances 0.000 description 6
- 229910052757 nitrogen Inorganic materials 0.000 description 6
- PNEYBMLMFCGWSK-UHFFFAOYSA-N Alumina Chemical compound [O-2].[O-2].[O-2].[Al+3].[Al+3] PNEYBMLMFCGWSK-UHFFFAOYSA-N 0.000 description 5
- 241001597008 Nomeidae Species 0.000 description 5
- 239000003153 chemical reaction reagent Substances 0.000 description 5
- 125000001309 chloro group Chemical group Cl* 0.000 description 5
- 230000006378 damage Effects 0.000 description 5
- 238000009826 distribution Methods 0.000 description 5
- 230000000694 effects Effects 0.000 description 5
- 229910052731 fluorine Inorganic materials 0.000 description 5
- 125000004435 hydrogen atom Chemical group [H]* 0.000 description 5
- YXIWHUQXZSMYRE-UHFFFAOYSA-N 1,3-benzothiazole-2-thiol Chemical compound C1=CC=C2SC(S)=NC2=C1 YXIWHUQXZSMYRE-UHFFFAOYSA-N 0.000 description 4
- VGGSQFUCUMXWEO-UHFFFAOYSA-N Ethene Chemical compound C=C VGGSQFUCUMXWEO-UHFFFAOYSA-N 0.000 description 4
- XEEYBQQBJWHFJM-UHFFFAOYSA-N Iron Chemical compound [Fe] XEEYBQQBJWHFJM-UHFFFAOYSA-N 0.000 description 4
- CPLXHLVBOLITMK-UHFFFAOYSA-N Magnesium oxide Chemical compound [Mg]=O CPLXHLVBOLITMK-UHFFFAOYSA-N 0.000 description 4
- CHJJGSNFBQVOTG-UHFFFAOYSA-N N-methyl-guanidine Natural products CNC(N)=N CHJJGSNFBQVOTG-UHFFFAOYSA-N 0.000 description 4
- PXHVJJICTQNCMI-UHFFFAOYSA-N Nickel Chemical compound [Ni] PXHVJJICTQNCMI-UHFFFAOYSA-N 0.000 description 4
- KYQCOXFCLRTKLS-UHFFFAOYSA-N Pyrazine Chemical compound C1=CN=CC=N1 KYQCOXFCLRTKLS-UHFFFAOYSA-N 0.000 description 4
- PMZURENOXWZQFD-UHFFFAOYSA-L Sodium Sulfate Chemical compound [Na+].[Na+].[O-]S([O-])(=O)=O PMZURENOXWZQFD-UHFFFAOYSA-L 0.000 description 4
- 125000003368 amide group Chemical group 0.000 description 4
- 125000003917 carbamoyl group Chemical group [H]N([H])C(*)=O 0.000 description 4
- 125000002915 carbonyl group Chemical group [*:2]C([*:1])=O 0.000 description 4
- 230000000052 comparative effect Effects 0.000 description 4
- 238000001816 cooling Methods 0.000 description 4
- ARUVKPQLZAKDPS-UHFFFAOYSA-L copper(II) sulfate Chemical compound [Cu+2].[O-][S+2]([O-])([O-])[O-] ARUVKPQLZAKDPS-UHFFFAOYSA-L 0.000 description 4
- 150000001993 dienes Chemical class 0.000 description 4
- SWSQBOPZIKWTGO-UHFFFAOYSA-N dimethylaminoamidine Natural products CN(C)C(N)=N SWSQBOPZIKWTGO-UHFFFAOYSA-N 0.000 description 4
- 239000000945 filler Substances 0.000 description 4
- 125000000524 functional group Chemical group 0.000 description 4
- HCDGVLDPFQMKDK-UHFFFAOYSA-N hexafluoropropylene Chemical compound FC(F)=C(F)C(F)(F)F HCDGVLDPFQMKDK-UHFFFAOYSA-N 0.000 description 4
- NAQMVNRVTILPCV-UHFFFAOYSA-N hexane-1,6-diamine Chemical compound NCCCCCCN NAQMVNRVTILPCV-UHFFFAOYSA-N 0.000 description 4
- 239000004816 latex Substances 0.000 description 4
- 229920000126 latex Polymers 0.000 description 4
- 238000004519 manufacturing process Methods 0.000 description 4
- QIQXTHQIDYTFRH-UHFFFAOYSA-N octadecanoic acid Chemical compound CCCCCCCCCCCCCCCCCC(O)=O QIQXTHQIDYTFRH-UHFFFAOYSA-N 0.000 description 4
- XNGIFLGASWRNHJ-UHFFFAOYSA-N phthalic acid Chemical compound OC(=O)C1=CC=CC=C1C(O)=O XNGIFLGASWRNHJ-UHFFFAOYSA-N 0.000 description 4
- 229920002493 poly(chlorotrifluoroethylene) Polymers 0.000 description 4
- 239000005023 polychlorotrifluoroethylene (PCTFE) polymer Substances 0.000 description 4
- YGSDEFSMJLZEOE-UHFFFAOYSA-N salicylic acid Chemical compound OC(=O)C1=CC=CC=C1O YGSDEFSMJLZEOE-UHFFFAOYSA-N 0.000 description 4
- KDYFGRWQOYBRFD-UHFFFAOYSA-N succinic acid Chemical compound OC(=O)CCC(O)=O KDYFGRWQOYBRFD-UHFFFAOYSA-N 0.000 description 4
- 239000004636 vulcanized rubber Substances 0.000 description 4
- KMYAABORDFJSLR-UHFFFAOYSA-N (carbamothioyltrisulfanyl) carbamodithioate Chemical compound NC(=S)SSSSC(N)=S KMYAABORDFJSLR-UHFFFAOYSA-N 0.000 description 3
- ODIGIKRIUKFKHP-UHFFFAOYSA-N (n-propan-2-yloxycarbonylanilino) acetate Chemical compound CC(C)OC(=O)N(OC(C)=O)C1=CC=CC=C1 ODIGIKRIUKFKHP-UHFFFAOYSA-N 0.000 description 3
- QTBSBXVTEAMEQO-UHFFFAOYSA-N Acetic acid Chemical compound CC(O)=O QTBSBXVTEAMEQO-UHFFFAOYSA-N 0.000 description 3
- UHOVQNZJYSORNB-UHFFFAOYSA-N Benzene Chemical compound C1=CC=CC=C1 UHOVQNZJYSORNB-UHFFFAOYSA-N 0.000 description 3
- 229920000049 Carbon (fiber) Polymers 0.000 description 3
- BVKZGUZCCUSVTD-UHFFFAOYSA-L Carbonate Chemical compound [O-]C([O-])=O BVKZGUZCCUSVTD-UHFFFAOYSA-L 0.000 description 3
- LYCAIKOWRPUZTN-UHFFFAOYSA-N Ethylene glycol Chemical compound OCCO LYCAIKOWRPUZTN-UHFFFAOYSA-N 0.000 description 3
- MHAJPDPJQMAIIY-UHFFFAOYSA-N Hydrogen peroxide Chemical compound OO MHAJPDPJQMAIIY-UHFFFAOYSA-N 0.000 description 3
- NHTMVDHEPJAVLT-UHFFFAOYSA-N Isooctane Chemical compound CC(C)CC(C)(C)C NHTMVDHEPJAVLT-UHFFFAOYSA-N 0.000 description 3
- BPQQTUXANYXVAA-UHFFFAOYSA-N Orthosilicate Chemical compound [O-][Si]([O-])([O-])[O-] BPQQTUXANYXVAA-UHFFFAOYSA-N 0.000 description 3
- MUBZPKHOEPUJKR-UHFFFAOYSA-N Oxalic acid Chemical compound OC(=O)C(O)=O MUBZPKHOEPUJKR-UHFFFAOYSA-N 0.000 description 3
- 239000004721 Polyphenylene oxide Substances 0.000 description 3
- 235000021355 Stearic acid Nutrition 0.000 description 3
- XLOMVQKBTHCTTD-UHFFFAOYSA-N Zinc monoxide Chemical compound [Zn]=O XLOMVQKBTHCTTD-UHFFFAOYSA-N 0.000 description 3
- 239000005083 Zinc sulfide Substances 0.000 description 3
- 230000000996 additive effect Effects 0.000 description 3
- 239000000853 adhesive Substances 0.000 description 3
- 125000001931 aliphatic group Chemical group 0.000 description 3
- 229940106691 bisphenol a Drugs 0.000 description 3
- 239000006229 carbon black Substances 0.000 description 3
- 239000004917 carbon fiber Substances 0.000 description 3
- 125000005587 carbonate group Chemical group 0.000 description 3
- 230000008859 change Effects 0.000 description 3
- 230000006835 compression Effects 0.000 description 3
- 238000007906 compression Methods 0.000 description 3
- MAWOHFOSAIXURX-UHFFFAOYSA-N cyclopentylcyclopentane Chemical compound C1CCCC1C1CCCC1 MAWOHFOSAIXURX-UHFFFAOYSA-N 0.000 description 3
- 235000014113 dietary fatty acids Nutrition 0.000 description 3
- JVSWJIKNEAIKJW-UHFFFAOYSA-N dimethyl-hexane Natural products CCCCCC(C)C JVSWJIKNEAIKJW-UHFFFAOYSA-N 0.000 description 3
- 238000000605 extraction Methods 0.000 description 3
- 239000000194 fatty acid Substances 0.000 description 3
- 229930195729 fatty acid Natural products 0.000 description 3
- 239000000835 fiber Substances 0.000 description 3
- 235000013305 food Nutrition 0.000 description 3
- 239000007789 gas Substances 0.000 description 3
- 230000026030 halogenation Effects 0.000 description 3
- 238000005658 halogenation reaction Methods 0.000 description 3
- 229920006168 hydrated nitrile rubber Polymers 0.000 description 3
- 229910052739 hydrogen Inorganic materials 0.000 description 3
- 125000002887 hydroxy group Chemical group [H]O* 0.000 description 3
- 238000001746 injection moulding Methods 0.000 description 3
- 229910000765 intermetallic Inorganic materials 0.000 description 3
- 230000001050 lubricating effect Effects 0.000 description 3
- 238000002844 melting Methods 0.000 description 3
- 230000008018 melting Effects 0.000 description 3
- VNWKTOKETHGBQD-UHFFFAOYSA-N methane Chemical compound C VNWKTOKETHGBQD-UHFFFAOYSA-N 0.000 description 3
- 238000002156 mixing Methods 0.000 description 3
- VLKZOEOYAKHREP-UHFFFAOYSA-N n-Hexane Chemical compound CCCCCC VLKZOEOYAKHREP-UHFFFAOYSA-N 0.000 description 3
- OQCDKBAXFALNLD-UHFFFAOYSA-N octadecanoic acid Natural products CCCCCCCC(C)CCCCCCCCC(O)=O OQCDKBAXFALNLD-UHFFFAOYSA-N 0.000 description 3
- 229920000570 polyether Polymers 0.000 description 3
- 238000006116 polymerization reaction Methods 0.000 description 3
- 150000003141 primary amines Chemical class 0.000 description 3
- 150000003335 secondary amines Chemical class 0.000 description 3
- 238000007493 shaping process Methods 0.000 description 3
- 239000008117 stearic acid Substances 0.000 description 3
- 229920003048 styrene butadiene rubber Polymers 0.000 description 3
- 150000003512 tertiary amines Chemical class 0.000 description 3
- VZCYOOQTPOCHFL-UHFFFAOYSA-N trans-butenedioic acid Natural products OC(=O)C=CC(O)=O VZCYOOQTPOCHFL-UHFFFAOYSA-N 0.000 description 3
- DRDVZXDWVBGGMH-UHFFFAOYSA-N zinc;sulfide Chemical compound [S-2].[Zn+2] DRDVZXDWVBGGMH-UHFFFAOYSA-N 0.000 description 3
- WRIDQFICGBMAFQ-UHFFFAOYSA-N (E)-8-Octadecenoic acid Natural products CCCCCCCCCC=CCCCCCCC(O)=O WRIDQFICGBMAFQ-UHFFFAOYSA-N 0.000 description 2
- XUNLTYLWCMUZFO-UHFFFAOYSA-N 1,4-dihydropyrazine-2,3-dithione Chemical class S=C1NC=CNC1=S XUNLTYLWCMUZFO-UHFFFAOYSA-N 0.000 description 2
- YFBUDXNMBTUSOC-UHFFFAOYSA-N 1,4-dihydroquinoxaline-2,3-dithione Chemical group C1=CC=C2NC(=S)C(=S)NC2=C1 YFBUDXNMBTUSOC-UHFFFAOYSA-N 0.000 description 2
- UZKWTJUDCOPSNM-UHFFFAOYSA-N 1-ethenoxybutane Chemical compound CCCCOC=C UZKWTJUDCOPSNM-UHFFFAOYSA-N 0.000 description 2
- HAZJTCQWIDBCCE-UHFFFAOYSA-N 1h-triazine-6-thione Chemical compound SC1=CC=NN=N1 HAZJTCQWIDBCCE-UHFFFAOYSA-N 0.000 description 2
- XSQHUYDRSDBCHN-UHFFFAOYSA-N 2,3-dimethyl-2-propan-2-ylbutanenitrile Chemical compound CC(C)C(C)(C#N)C(C)C XSQHUYDRSDBCHN-UHFFFAOYSA-N 0.000 description 2
- JECYNCQXXKQDJN-UHFFFAOYSA-N 2-(2-methylhexan-2-yloxymethyl)oxirane Chemical compound CCCCC(C)(C)OCC1CO1 JECYNCQXXKQDJN-UHFFFAOYSA-N 0.000 description 2
- XMNIXWIUMCBBBL-UHFFFAOYSA-N 2-(2-phenylpropan-2-ylperoxy)propan-2-ylbenzene Chemical compound C=1C=CC=CC=1C(C)(C)OOC(C)(C)C1=CC=CC=C1 XMNIXWIUMCBBBL-UHFFFAOYSA-N 0.000 description 2
- LQJBNNIYVWPHFW-UHFFFAOYSA-N 20:1omega9c fatty acid Natural products CCCCCCCCCCC=CCCCCCCCC(O)=O LQJBNNIYVWPHFW-UHFFFAOYSA-N 0.000 description 2
- QSBYPNXLFMSGKH-UHFFFAOYSA-N 9-Heptadecensaeure Natural products CCCCCCCC=CCCCCCCCC(O)=O QSBYPNXLFMSGKH-UHFFFAOYSA-N 0.000 description 2
- 239000005711 Benzoic acid Substances 0.000 description 2
- FERIUCNNQQJTOY-UHFFFAOYSA-N Butyric acid Chemical compound CCCC(O)=O FERIUCNNQQJTOY-UHFFFAOYSA-N 0.000 description 2
- VTYYLEPIZMXCLO-UHFFFAOYSA-L Calcium carbonate Chemical compound [Ca+2].[O-]C([O-])=O VTYYLEPIZMXCLO-UHFFFAOYSA-L 0.000 description 2
- QPLDLSVMHZLSFG-UHFFFAOYSA-N Copper oxide Chemical compound [Cu]=O QPLDLSVMHZLSFG-UHFFFAOYSA-N 0.000 description 2
- RTZKZFJDLAIYFH-UHFFFAOYSA-N Diethyl ether Chemical compound CCOCC RTZKZFJDLAIYFH-UHFFFAOYSA-N 0.000 description 2
- 239000004593 Epoxy Substances 0.000 description 2
- VZCYOOQTPOCHFL-OWOJBTEDSA-N Fumaric acid Chemical compound OC(=O)\C=C\C(O)=O VZCYOOQTPOCHFL-OWOJBTEDSA-N 0.000 description 2
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Abstract
本发明涉及一种层叠体,是具有橡胶层(A)和层叠在橡胶层(A)上的氟树脂层(B)的层叠体,特征在于,橡胶层(A)是由加硫用橡胶组合物形成的层,加硫用橡胶组合物含有环氧氯丙烷橡胶(a1),从由1,8-二氮杂二环(5.4.0)十一烯-7及其盐、1,5-二氮杂二环(4.3.0)-壬烯-5及其盐组成的群中选择的至少1种化合物(a2),环氧树脂(a3),载水物质(a4);氟树脂层(B)是由氟聚合物组合物形成的层,氟聚合物组合物含有具有来自氯三氟乙烯的共聚单元的氟聚合物(b1)。
Description
技术领域
本发明涉及层叠体。
背景技术
以往,随着环境意识的提高,用于防止燃料挥发的法规得到了推进,特别在汽车业界,以美国为中心抑制燃料挥发的倾向非常明显,对于燃料阻挡性优秀的材料的需求正在增加。
特别是在燃料输送橡胶软管中,由于耐燃料透过性良好而使用以氟树脂作为阻挡层的层叠软管(阻挡层以外是橡胶),由于现今的降低环境负荷的强烈要求,需要使得阻挡层进一步降低燃料透过性。作为其手段,尝试着通过增加阻挡层的厚度或使用低透过性最优秀的全卤系(パ一ハロゲン系)的氟树脂的方法来确保低透过性。但是,增加阻挡层(氟树脂)的厚度,会增加软管重量,从节能的角度考虑也不利,而且,会不利于软管自身的弯曲性(柔软性),使用性(组装性)的方面也不利。
此外,在使用全卤系的氟树脂作为阻挡层时,与作为配套材料(相手材)的外内层橡胶的粘结有困难,为了改善粘结性,需要树脂的表面处理、施加薄膜、胶带的作法等的工序,产生作业工序的复杂化,生产性显著降低,且具有大幅提高了成本等的实用上的不良效果。
为了提高氟树脂层与橡胶层的粘结,已知有例如专利文献1所述的燃料软管,其具有二烯系橡胶层与偏二氟乙烯系共聚体(THV)层相邻接的层结构,其中的二烯系橡胶是在NBR等二烯系橡胶中在添加DBU盐等的同时,添加从硫系加硫剂、氨基甲酸金属盐以及噻唑系金属盐的至少一种以及氧化镁而形成的。
已知如专利文献2及3所示,使用至少具有1种含多个氢原子的单体的含氟聚合物或偏二氟乙烯作为必须的含氟聚合物,通过与脱氟化氢组合物混合,改良硬化性弹性体化合物对于含氟聚合物层的粘结性。
现有技术文献
专利文献
专利文献1:日本特开2007-261079号公报
专利文献2:日本特表2001-527104号公报
专利文献3:日本特表2001-526972号公报
发明内容
发明所要解决的问题
作为低透过性的氟树脂,已知有具有来自氯三氟乙烯的共聚单元的氟聚合物,但是,即使使用该氟聚合物作为氟树脂,也不能与环氧氯丙烷橡胶粘结。
本发明提供将具有来自氯三氟乙烯的共聚单元的氟聚合物与环氧氯丙烷橡胶牢固粘结的层叠体。
解决问题的手段
本发明涉及一种层叠体,是具有橡胶层(A)与在橡胶层(A)上层叠的氟树脂层(B)的层叠体,特征在于,橡胶层(A)是由加硫用橡胶组合物形成的层,加硫用橡胶组合物含有环氧氯丙烷橡胶(a1)、从由1,8-二氮杂二环(5.4.0)十一烯-7盐、1,5-二氮杂二环(4.3.0)-壬烯-5盐、1,8-二氮杂二环(5.4.0)十一烯-7及1,5-二氮杂二环(4.3.0)-壬烯-5组成的群中选择的至少1种化合物(a2)、环氧树脂(a3)以及从吸水物和含水物中选择的至少1种载水物质(a4),氟树脂层(B)是由氟聚合物组合物形成的层,氟聚合物组合物含有具有来自氯三氟乙烯的共聚单元的氟聚合物(b1)。
本发明优选在加硫用橡胶组合物中进一步含有铜盐(a5)。
发明效果
本发明的层叠体是将氟树脂层与橡胶层进行层叠,不加入特别复杂的工序,由于在橡胶加硫时能得到化学性牢固的粘结,因此在粘结时不需要特别的工序,能够以低成本来成形,且成形容易。此外,由于能以挤出成形这样的普通方法来成形,能够薄膜化,在柔软性方面也得到改善。
具体实施方式
本发明的层叠体的特征在于,具有橡胶层(A)和层叠在橡胶层(A)上的氟树脂层(B)。
以下,对各层进行说明。
(A)橡胶层
橡胶层(A)是由加硫用橡胶组合物形成的层。
加硫用橡胶组合物作为必须成分含有环氧氯丙烷橡胶(a1)、化合物(a2)、环氧树脂(a3)以及载水物质(a4),优选进一步含有铜盐(a5)。此外,作为任意成分还可以含有加硫剂(a6)。特别地,加硫用橡胶组合物除了环氧氯丙烷橡胶(a1)及化合物(a2)之外,如果含有加硫剂(a6),则层(A)与层(B)能以更大的粘结强度来粘结。
环氧氯丙烷橡胶(a1)只要是具有基于环氧氯丙烷的聚合单元的未加硫橡胶就没有特别限定,可以是实质性地仅由基于环氧氯丙烷的聚合单元构成的1元聚合体,也可以是由基于环氧氯丙烷的聚合单元与基于环氧氯丙烷以外的其他单体的聚合单元构成的2元以上的聚合体。
环氧氯丙烷以外的其他单体,优选例如从由环氧乙烷、环氧丙烷及烯丙基缩水甘油醚组成的群中选择的至少1种单体。加硫粘结用组合物优选为具有基于环氧氯丙烷的聚合单元和基于环氧乙烷的聚合单元的聚合体,更优选为具有基于环氧氯丙烷的聚合单元与基于环氧乙烷的聚合单元与基于烯丙基缩水甘油醚的聚合单元的聚合体
作为环氧氯丙烷橡胶(a1),优选为例如从由环氧氯丙烷单独聚合体、环氧氯丙烷-环氧乙烷共聚体、环氧氯丙烷-烯丙基缩水甘油醚共聚体、环氧氯丙烷-环氧乙烷-烯丙基缩水甘油醚共聚体、环氧氯丙烷-环氧丙烷共聚体、环氧氯丙烷-环氧丙烷-烯丙基缩水甘油醚共聚体及环氧氯丙烷-环氧乙烷-环氧丙烷-烯丙基缩水甘油醚四元共聚体组成的群中选择的至少1种聚合体。更优选为从由环氧氯丙烷-环氧乙烷共聚体及环氧氯丙烷-环氧乙烷-烯丙基缩水甘油醚共聚体中选择的至少1种聚合体。这些可以单独使用,或2种以上混合使用。
化合物(a2)是从由1,8-二氮杂二环(5.4.0)十一烯-7盐、1,5-二氮杂二环(4.3.0)-壬烯-5盐、1,8-二氮杂二环(5.4.0)十一烯-7及1,5-二氮杂二环(4.3.0)-壬烯-5组成的群中选择的至少1种化合物。通过含有化合物(a2),可以改善加硫用橡胶组合物的加硫特性,能够提高粘结性。
化合物(a2)优选为从由1,8-二氮杂二环(5.4.0)十一烯-7的对甲苯磺酸盐、1,8-二氮杂二环(5.4.0)十一烯-7的苯酚盐、1,8-二氮杂二环(5.4.0)十一烯-7的苯酚树脂盐、1,8-二氮杂二环(5.4.0)十一烯-7的邻苯二甲酸盐、1,8-二氮杂二环(5.4.0)十一烯-7的蚁酸盐、1,8-二氮杂二环(5.4.0)十一烯-7的辛酸盐、1,5-二氮杂二环(4.3.0)-壬烯-5的对甲苯磺酸盐、1,5-二氮杂二环(4.3.0)-壬烯-5的苯酚盐、1,5-二氮杂二环(4.3.0)-壬烯-5的苯酚树脂盐、1,5-二氮杂二环(4.3.0)-壬烯-5的邻苯二甲酸盐、1,5-二氮杂二环(4.3.0)-壬烯-5的蚁酸盐、1,5-二氮杂二环(4.3.0)-壬烯-5的辛酸盐、1,8-二氮杂二环(5.4.0)十一烯-7及1,5-二氮杂二环(4.3.0)-壬烯-5组成的群中选择的至少1种化合物。
从提高粘结性的观点出发,化合物(a2)更优选为1,8-二氮杂二环(5.4.0)十一烯-7的苯酚盐。
化合物(a2),从粘结性良好的观点出发,相对于环氧氯丙烷橡胶(a1)100质量份优选为0.3质量份以上、3.0质量份以下。更优选为0.5质量份以上、2.0质量份以下。此外,从粘结性良好且同时加硫特性良好的角度出发,化合物(a2)相对于环氧氯丙烷橡胶(a1)100质量份优选为0.5质量份以上、1.5质量份以下。
加硫用橡胶组合物含有环氧树脂(a3)。作为环氧树脂(a3),优选为从例如双酚A型环氧树脂、双酚F型环氧树脂、酚醛清漆型环氧树脂、邻甲酚醛清漆型环氧树脂、胺型环氧树脂、加氢双酚A型环氧树脂及多官能环氧树脂组成的群中选择的至少1种树脂。其中,双酚A型环氧树脂从耐药品性、粘结性良好方面而优选,进而特别优选式(1)所表示的环氧树脂。
这里,式(1)中,n为平均值,优选为0.1~3,更优选为0.1~0.5,进而优选为0.1~0.3。如果n不足0.1,则有与氟聚合物(b1)的粘结下降的倾向。另一方面,如果n超过3,则有环氧树脂自身的粘度高,在加硫用橡胶组合物中难以均匀分散的倾向。
从与氟聚合物(b1)的粘结力进一步提高的观点出发,环氧树脂(a3)相对于环氧氯丙烷橡胶(a1)100质量份优选为0.1~5质量份,更优选为0.3~3质量份。
此外,加硫用橡胶组合物中,化合物(a2)与环氧树脂(a3)的合计,相对于环氧氯丙烷橡胶(a1)100质量份超过2.0质量份,是优选的实施方式之一。
加硫用橡胶组合物含有从吸水物和含水物中选择的至少1种载水物质(a4)。这里的吸水物是指将水吸收保持并通过加热而蒸发放出的化合物,含水物是指在结构内含有水且通过加热分解而生成水并放出的化合物。载水物质(a4)从操作方面来讲,优选为聚醚化合物、金属化合物等吸水而成的吸水物、金属盐水合物等含水物,特别优选金属盐水合物。通过含有载水物质(a4),能够提高粘结性。
作为载水物质(a4)的吸水物,例举聚醚化合物、金属化合物等吸水而成的吸水物。关于向化合物中吸水,是进行与水分的接触(例如,含浸等),没有特别限定。
作为聚醚化合物,例举聚环氧乙烷、聚乙二醇等。
金属化合物例举金属的氧化物、氢氧化物、碳酸盐、氯化物、硫酸盐、硅酸盐、合成水滑石等。
作为金属氢氧化物,例举氢氧化铝、氢氧化镁、氢氧化钙、氢氧化钡、氢氧化锌、氢氧化铁、氢氧化铜、氢氧化锰等。
作为金属氧化物,例举氧化铝、氧化钙、氧化镁、氧化钛、氧化铜等。
作为金属碳酸盐,例举碳酸铝、碳酸钙、碳酸镁、碳酸钡、碳酸铜等。
作为金属氯化物,例举氯化铝、氯化钙、氯化镁、氯化铜等。
作为金属硫化盐,例举硫化锌、硫化钙、硫化镁、硫化铜、硫化锌等。
作为金属硫酸盐,例举硫酸钙、硫酸钡、硫酸铝、硫酸钠、硫酸铜等。
作为金属硅酸盐,例举硅酸铝、硅酸钙、硅酸镁、硅酸铝、硅酸钠、硅酸铜等。
从改善粘结性的观点出发,载水物质(a4)的吸水物,优选为吸水保持率为5重量%以上的化合物。更优选吸水保持率为10重量%以上的化合物。吸水保持率是吸水物所保持的水分量的比例,由下式来算出。
吸水保持率(重量%)=(吸水物所保持的水分量(重量)/吸水物(重量))×100。
作为载水物质(a4)的含水物,例举金属盐水合物。
作为金属盐水合物,例举钙、铝、锌、锰、镧、钛、锆、铁、钴、镍、镁、铜这样的金属的硅酸、硼酸、磷酸、盐酸、硫化氢、硫酸、硝酸、碳酸等的无机酸盐水合物,安息香酸、邻苯二甲酸、马来酸、琥珀酸、水杨酸、柠檬酸等羧酸这样的有机酸盐水合物。优选为从醋酸钙、硫酸铝、硫酸钠、硫酸钙、硫酸镁、硫酸锌、硫酸锰、硫酸铜、硫酸镧、硫酸钛、硫酸锆、硫酸铁、硫酸钴及硫酸镍中选择的的金属盐的水合物,优选为从钙、镁、钠、铜中选择的金属的硫酸盐及/或醋酸盐的水合物,更优选为硫酸钙2水合物、硫酸钠10水合物、硫酸铜(II)5水合物,特别优选为硫酸钙2水合物、硫酸钠10水合物。
载水物质(a4)配合量,相对于环氧氯丙烷橡胶(a1)100质量份为0.1~80质量份,优选为0.5~70质量份,更优选为1~50质量份,特别优选为1~20质量份。在该范围内,得到充分的粘结效果,不损害加硫物的机械物性,因而优选。
加硫用橡胶组合物,从提高粘结性的观点出发,优选进一步含有铜盐(a5)。
作为铜盐(a5),优选为有机铜盐。作为有机铜盐,例举蚁酸、醋酸、丁酸、硬脂酸等饱和羧酸的铜盐,油酸、亚油酸等不饱和羧酸的铜盐,水杨酸、安息香酸、邻苯二甲酸等芳香族羧酸的铜盐,草酸、琥珀酸、己二酸、马来酸、富马酸等二羧酸的铜盐,乳酸、柠檬酸等羟基酸的铜盐,氨基甲酸的铜盐,二甲基二硫代氨基甲酸铜、二乙基二硫代氨基甲酸铜、二丁基二硫代氨基甲酸铜、N-乙基-N-苯基二硫代氨基甲酸铜、N-环戊烷二硫代氨基甲酸铜、二苄基二硫代氨基甲酸铜等硫代氨基甲酸、磺酸等的铜盐。作为有机铜盐,优选为饱和羧酸的铜盐、不饱和羧酸的铜盐、芳香族羧酸的铜盐、硫代氨基甲酸的铜盐,更优选硬脂酸铜、二甲基二硫代氨基甲酸铜、二乙基二硫代氨基甲酸铜、二丁基二硫代氨基甲酸铜。
从提高粘结性的观点出发,铜盐(a5)的配合量,相对于环氧氯丙烷橡胶(a1)100质量份为0.01~5质量份,优选为0.05~3质量份。更加优选为0.1~2质量份。在该范围内,得到充分的粘结效果,且不损害加硫物的机械物性,因而优选。
加硫用橡胶组合物优选含有加硫剂(a6)。可以对应于加硫用橡胶组合物的加硫系而使用以往公知的加硫剂。通过对环氧氯丙烷橡胶(a1)进行加硫,可以提高所得的加硫橡胶层的拉伸强度等机械强度,还可得到良好的弹性。
作为加硫剂(a6),可以使用利用氯原子的反应性的公知加硫剂,例举例如聚胺系加硫剂、硫脲系加硫剂、噻二唑系加硫剂、巯基三嗪系加硫剂、吡嗪系加硫剂、喹喔啉系加硫剂、双酚系加硫剂。
如果例举利用氯原子的反应性的公知加硫剂(e),作为聚胺系加硫剂有乙烯二胺、六亚甲基二胺、二乙烯三胺、三乙烯四胺、六亚甲基四胺、对亚苯基二胺、异丙苯二胺、N,N’-二亚肉桂基-1,6-己烷二胺、乙烯二胺氨基甲酸酯、六亚甲基二胺氨基甲酸酯等。
作为硫脲系加硫剂,例举乙烯硫脲、1,3-二乙基硫脲、1,3-二丁基硫脲、三甲基硫脲等。
作为噻二唑系加硫剂,有2,5-二巯基-1,3,4-噻二唑、2-巯基-1,3,4-噻二唑-5-硫代苯甲酸酯等。
作为巯基三嗪系加硫剂,有2,4,6-三巯基-1,3,5-三嗪、2-甲氧基-4,6-二巯基三嗪、2-己基氨基-4,6-二巯基三嗪、2-二乙基氨基-4,6-二巯基三嗪、2-环己烷氨基-4,6-二巯基三嗪、2-二丁基氨基-4,6-二巯基三嗪、2-苯胺-4,6-二巯基三嗪、2-苯基氨基-4,6-二巯基三嗪等。
作为吡嗪系加硫剂有2,3-二巯基吡嗪衍生物等,如果示例2,3-二巯基吡嗪衍生物,有吡嗪-2,3-二硫代碳酸酯、5-甲基-2,3-二巯基吡嗪、5-乙基吡嗪-2,3-二硫代碳酸酯、5,6-二甲基-2,3-二巯基吡嗪、5,6-二甲基吡嗪-2,3-二硫代碳酸酯等。
作为喹喔啉系加硫剂,有2,3-二巯基喹喔啉衍生物等,如果示例2,3-二巯基喹喔啉衍生物,有喹喔啉-2,3-二硫代碳酸酯、6-甲基喹喔啉-2,3-二硫代碳酸酯、6-乙基-2,3-二巯基喹喔啉、6-异丙基喹喔啉-2,3-二硫代碳酸酯、5,8-二甲基喹喔啉-2,3-二硫代碳酸酯等。
作为双酚系加硫剂,有4,4’-二羟基二苯基亚砜、4,4’-二羟基二苯基磺(双酚S)、1,1-环亚己基-双(4-羟基苯)、2-氯-1,4-环己烯-双(4-羟基苯)、2,2-异亚丙基-双(4-羟基苯)(双酚A)、六氟异亚丙基-双(4-羟基苯)(双酚AF)和2-氟-1,4-亚苯基-双(4-羟基苯)等。
在本发明中,加硫用橡胶组合物中可以与加硫剂一起直接使用公知的加硫促进剂、延迟剂。作为与利用氯原子的反应性的公知的加硫剂一起使用的加硫促进剂,可以例举伯胺、仲胺、叔胺、这些胺的有机酸盐或其加成物、胍系促进剂、秋兰姆系促进剂、二硫代氨基甲酸系促进剂等。此外,作为延迟剂,可以例举N-环己烷硫代邻苯二甲酰亚胺、二硫代氨基甲酸类的锌盐等。
如果示例加硫促进剂,作为伯胺、仲胺、叔胺特别优选碳原子数5~20的脂肪族或环式脂肪酸的伯胺、仲胺或叔胺,这样的胺的代表例有正己胺、辛胺、二丁基胺、三丁基胺、六亚甲基二胺等。
作为与胺形成盐的有机酸,示例羧酸、氨基甲酸、2-巯基苯并噻唑、二硫代磷酸等。此外,作为与上述胺形成加成物的物质,示例醇类、肟类等。作为胺的有机酸盐或加成物的具体例,例举正丁基胺·醋酸盐、六亚甲基二胺·氨基甲酸盐、2-巯基苯并噻唑的二环己胺盐等。
作为胍系促进剂的例子,例举二苯基胍,二甲苯基胍等。
作为秋兰姆系加硫促进剂的具体例,例举四甲基秋兰姆二硫化物、四甲基秋兰姆单硫化物、四乙基秋兰姆二硫化物、四丁基秋兰姆二硫化物、二环戊烷秋兰姆四硫化物等。
作为二硫代氨基甲酸系促进剂的例子,例举环戊烷二硫代氨基甲酸哌啶盐等。
与利用氯原子的反应性的公知加硫剂一起使用的加硫促进剂或延迟剂的配合量,相对于橡胶成分100重量份优选为0~10重量份,更优选为0.1~5重量份。
此外,环氧氯丙烷橡胶(a1)为环氧氯丙烷-烯丙基缩水甘油醚共聚物、环氧氯丙烷-环氧乙烷-烯丙基缩水甘油醚三元共聚物等具有双键的聚合体时,可以例举丁腈系橡胶的加硫中通常使用的公知加硫剂、加硫促进剂、加硫延迟剂、加硫促进助剂、交联助剂等。作为加硫剂,可以例举硫、吗啉二硫化物、四甲基秋兰姆二硫化物、四乙基秋兰姆二硫化物、四丁基秋兰姆二硫化物、N,N’-二甲基-N,N’-二苯基秋兰姆二硫化物、二戊烷亚甲基秋兰姆四硫化物、二环戊烷秋兰姆四硫化物、二环戊烷秋兰姆六硫化物等硫系加硫剂,叔-丁基过氧化氢、对薄荷烷过氧化氢、二异丙苯过氧化物、叔-丁基过氧化物、1,3-双(叔-丁基过氧异丙基)苯、2,5-二甲基-2,5-二(叔-丁基过氧)己烷、苯甲酰过氧化物、叔-丁基过氧苯甲酸酯等过氧化物系加硫剂系加硫剂,烷基酚甲醛树脂等树脂系加硫剂,对醌二肟、p-p’-二苯甲酰醌二肟等醌二肟系加硫剂等。这些加硫剂可以单独使用或2种以上混合使用。另外,作为加硫促进剂、加硫延迟剂、加硫促进助剂、交联助剂,能够例举例如醛铵系促进剂、醛胺系促进剂、硫脲系促进剂、胍系促进剂、噻唑系促进剂、亚磺酰胺系促进剂、秋兰姆系促进剂、二硫代氨基甲酸盐系促进剂、黄原酸盐系促进剂等各种加硫促进剂,N-亚硝基二苯基胺、邻苯二甲酸酐、N-环己基硫代邻苯二甲酰亚胺等加硫延迟剂,锌华、硬脂酸、硬脂酸锌等加硫促进助剂,醌二肟系交联助剂、甲基丙烯酸酯系交联助剂、烯丙基(allyl)系交联助剂、马来酰亚胺系交联助剂等各种交联助剂等。
从环氧氯丙烷橡胶(a1)的耐热性、橡胶层(A)与氟树脂层(B)的粘结性的观点出发,作为加硫剂,优选为从由硫脲系加硫剂、喹喔啉系加硫剂、硫系加硫剂、过氧化物系加硫剂及双酚系加硫剂组成的群中选择的至少1种加硫剂(a6),更优选从由硫脲系加硫剂、喹喔啉系加硫剂及双酚系加硫剂组成的群中选择的至少1种加硫剂,特别优选为喹喔啉系加硫剂。这些加硫剂可以单独使用或2种以上混合使用。
加硫用橡胶组合物,相对于环氧氯丙烷橡胶(a1)100重量份,优选含有0.1~10重量份的加硫剂(a6)。更优选为0.5~5重量份。加硫剂不足0.1重量份时,会有交联效果不充分的危险,如果超过10重量份,会有对本发明的层叠体进行成形而得到的成形体过于刚直,得不到实用性的橡胶物性的危险。
加硫用橡胶组合物中,除了硫脲系加硫剂、喹喔啉系加硫剂及双酚系加硫剂组成的群中选择的至少1种加硫剂之外,进一步含有过氧化物系加硫剂也是优选的实施方式之一。作为过氧化物系加硫剂,优选二异丙苯过氧化物。过氧化物系加硫剂相对于环氧氯丙烷橡胶(a1)100质量份优选为1.0质量份以上,更优选2.0质量份以上。此外,优选为5.0质量份以下。例如在加硫用橡胶组合物中,化合物(a2)、环氧树脂(a3)的含量少的情况下,会有得不到良好的粘结性的危险,通过含有过氧化物系加硫剂,即使在化合物(a2)、环氧树脂(a3)的含量少的情况下,也可得到与氟树脂层(B)的良好粘结性。
加硫用橡胶组合物,由于有阻碍加硫特性、损害橡胶的物性的危险,优选不含有胺化合物。
加硫用橡胶组合物中,为了赋予橡胶层(A)与环氧氯丙烷橡胶(a1)不同的特性,可以一进步含有环氧树脂以外的其他树脂。作为树脂,例举例如聚甲基丙烯酸甲酯(PMMA)树脂、聚苯乙烯(PS)树脂、聚氨酯(PUR)树脂、聚氯乙烯(PVC)树脂、乙烯-醋酸乙烯(EVA)树脂、苯乙烯-丙烯腈(AS)树脂、聚乙烯(PE)树脂、氯化聚苯乙烯、氯磺化聚乙烯等。这种情况下,树脂的配合量,相对于环氧氯丙烷橡胶(a1)100质量份优选为1~50质量份。
此外,本发明中,对应于目的或需要,可以配合一般的加硫用橡胶组合物所配合的通常的添加物,例如填充剂、酸接受体、加工助剂、塑化剂、软化剂、抗老化剂、着色剂、稳定剂、粘结助剂、离型剂、导电性赋予剂、热传导性赋予剂、表面非粘着剂、粘着赋予剂、柔软性赋予剂、耐热性改善剂、阻燃剂、紫外线吸收剂、耐油性改善剂、发泡剂、防焦剂、滑剂等各种添加剂。此外,也可以配合1种或2种以上与上述添加剂不同的常用的加硫剂、加硫促进剂。但是,这些添加剂,以不损害作为本发明目的的与氟树脂层(B)的粘结力的范围的量来配合。
作为填充剂,例举例如二硫化钼、硫化铁、硫化铜等金属硫化物,硅藻土、石棉、锌钡白(硫化锌/硫化钡)、石墨、碳黑、氟化碳、氟化钙、焦炭(コ一クス)、石英微粉末、滑石、粘土、云母粉末、钙硅石、碳素纤维、芳纶纤维、各种晶须、玻璃纤维、有机增强剂、有机填充剂等。
作为加工助剂,有硬脂酸、油酸、棕榈酸、月桂酸等高级脂肪酸,硬脂酸钠、硬脂酸锌等高级脂肪酸盐,硬脂酸酰胺、油酸酰胺等高级脂肪酸酰胺,油酸乙酯等高级脂肪酸酯,硬脂胺、油胺等高级脂肪族胺,巴西棕榈蜡、地蜡等石油系蜡,乙二醇、甘油、二乙二醇等多元醇,凡士林、石蜡等脂肪族烃,有机硅系油、有机硅系聚合物、低分子量聚乙烯、邻苯二甲酸酯类、磷酸酯类、松香、(卤化)二烷基胺、(卤化)二烷基砜、表面活性剂等。
作为塑化剂例举例如邻苯二甲酸衍生物、癸二酸衍生物,作为软化剂例举例如润滑油、加工油、焦油、蓖麻油、硬脂酸钙,作为抗老化剂例举例如亚苯基二胺类、磷酸盐类、喹啉类、甲酚类、苯酚类、二硫代氨基甲酸酯金属盐等。
加硫用橡胶组合物通过将环氧氯丙烷橡胶(a1)、化合物(a2)、环氧树脂(a3)以及载水物质(a4),进而优选的铜盐(a5),进一步如果需要的加硫剂(a6)以及其他添加剂进行混练来调制。
混练可以在例如100℃以下的温度通过使用开放辊、班伯里混炼机、加压捏合机等来进行。
接下来,对本发明的层叠体中的氟树脂层(B)进行说明。
(B)氟树脂层
氟树脂层(B)是由氟聚合物组合物形成的层。
氟聚合物组合物至少含有具有来自氯三氟乙烯的共聚单元的氟聚合物(b1)。
作为氟聚合物(b1),从燃料阻挡性的观点出发,优选为氟树脂,优选为从由聚氯三氟乙烯(PCTFE)及CTFE共聚体组成的群中选择的至少1种。
作为CTFE共聚体,优选含有来自CTFE的共聚单元(CTFE单元)与来自由四氟乙烯(TFE)、六氟丙烯(HFP)、全氟(烷基乙烯醚)(PAVE)、偏二氟乙烯(VdF)、氟乙烯、六氟异丁烯、式:CH2=CX1(CF2)nX2所示的单体、乙烯、丙烯、1-丁烯、2-丁烯、氯乙烯及偏二氯乙烯组成的群中选择的至少1种单体的共聚单元,式中,X1为H或F,X2为H、F或Cl,n为1~10的整数。此外,作为CTFE共聚体,优选为全卤聚合体。
作为CTFE共聚体,更优选含有CTFE单元与来自由TFE、HFP及PAVE组成的群中选择的至少1种单体的共聚单元,更优选实质的仅由这些的共聚单元构成的共聚体。此外,从燃料低透过的观点出发,优选不含有具有乙烯、偏二氟乙烯、氟乙烯等CH键的单体。虽然全卤聚合物与橡胶的粘结通常很困难,但是根据本发明的构成,即使氟树脂层是由全卤聚合物构成的层,氟树脂层与橡胶层的层间的粘结也牢固。
CTFE共聚体优选具有总单体单元的10~90mol%的CTFE单元。
作为CTFE共聚体,特别优选含有来自CTFE单元、TFE单元以及与这些能够共聚的单体(α)的单体(α)单元。
“CTFE单元”及“TFE单元”是指在CTFE共聚体的分子结构上分别具有来自CTFE的部分(-CFCl-CF2-)、来自TFE的部分(-CF2-CF2-),前述“单体(α)单元”,同样地,是指在CTFE系共聚体的分子结构上附加了单体(α)的部分。
作为单体(α),只要是能够与CTFE以及TFE共聚的单体就没有特别限定,有乙烯(Et)、偏二氟乙烯(VdF)、由CF2=CF-ORf1(式中,Rf1是碳原子数1~8的全氟烷基)所表示的全氟(烷基乙烯醚)(PAVE)、由CX3X4=CX5(CF2)nX6(式中,X3、X4以及X5相同或者不同,是氢原子或氟原子;X6是、氢原子、氟原子或氯原子;n为1~10整数)所表示的乙烯单体、由CF2=CF-OCH2-Rf2(式中,Rf2为碳原子数1~5的全氟烷基)所表示的烷基全氟乙烯醚衍生物等,其中,优选为从由PAVE、上述乙烯单体及烷基全氟乙烯醚衍生物组成的群中选择的至少1种,更优选为从由PAVE及HFP组成的群中选择的至少1种。
作为烷基全氟乙烯醚衍生物,优选Rf2为碳原子数1~3的全氟烷基,更优选为CF2=CF-OCH2-CF2CF3。
CTFE共聚体中,CTFE单元与TFE单元的比率,相对于CTFE单元为15~90mol%,TFE单元为85~10mol%;更优选CTFE单元为20~90mol%,TFE单元为80~10mol%。此外,更加优选CTFE单元为15~25mol%与TFE单元为85~75mol%所构成的共聚体。
CTFE共聚体优选CTFE单元与TFE单元的合计为90~99.9mol%,单体(α)单元为0.1~10mol%。如果单体(α)单元不足0.1mol%,在成形性、耐环境应力破裂性以及耐燃料开裂性方面易于变差,如果超过10mol%,燃料低透过性、耐热性、机械特性有变差的倾向。
氟聚合物(b1)最优选为PCTFE或CTFE-TFE-PAVE共聚体。上述CTFE-TFE-PAVE共聚体是实质性的仅有CTFE、TFE及PAVE构成的共聚体。PCTFE及CTFE-TFE-PAVE共聚体不存在直接结合在构成主链的碳原子上的氢原子,不进行脱氟化氢化反应。因此,不适合于利用通过脱氟化氢化反应在氟聚合物中形成的不饱和键的以往的粘结性改善方法。
作为PAVE,有全氟(甲基乙烯醚)(PMVE)、全氟(乙基乙烯醚)(PEVE)、全氟(丙基乙烯醚)(PPVE)、全氟(丁基乙烯醚)等,其中优选为从由PMVE、PEVE及PPVE组成的群中选择的至少1种。
PAVE单元优选为总单体单元0.5mol%以上,优选为5mol%以下。
CTFE单元等构成单元是通过进行19F-NMR分析所得到的值。
氟聚合物(b1)还可以在聚合物的主链末端以及/或侧链上导入从由羰基、羟基、杂环基以及氨基组成的群中选择的至少1种反应性官能基。
本说明书中,“羰基”是由碳-氧双键构成的碳2价的基团,由-C(=O)-所表示的基团来代表。作为具有前述羰基的反应性官能基没有特别限定,有例如碳酸酯基、羧酸酰卤基(卤化甲酰基)、甲酰基、羧基、酯键(-C(=O)O-)、酸酐键(-C(=O)O-C(=O)-)、异氰酸酯基、酰胺基、酰亚胺基(-C(=O)-NH-C(=O)-)、尿烷键(-NH-C(=O)O-)、氨基甲酰基(NH2-C(=O)-)、氨基甲酰氧基(NH2-C(=O)O-)、脲基(NH2-C(=O)-NH-)、草氨酰(oxamyl)基(NH2-C(=O)-C(=O)-)等在化学结构上作为一部分而含有羰基的物质。
在酰胺基、酰亚胺基、尿烷键、氨基甲酰基、氨基甲酰氧基、脲基、草氨酰基等中,与其氮原子结合的氢原子还可以被例如烷基等烃基来取代。
从易于导入方面、氟聚合物(b1)具有适度的耐热性和在较低温下的良好粘结性方面考虑,反应性官能基优选为酰胺基、氨基甲酰基、羟基、羧基、碳酸酯基、卤化羧酸基、酸酐结合,进一步优选为酰胺基、氨基甲酰基、羟基、碳酸酯基、卤化羧酸基、酸酐结合。
氟聚合物(b1)可以通过悬浊聚合、溶液聚合、乳化聚合、块状聚合等以往公知的聚合方法来获得。前述聚合中,温度、压力等各条件、聚合引发剂以及其他添加剂,可以对应于氟聚合物(b1)的组成、量来适宜设定。
对氟聚合物(b1)的熔点没有特别限定,但优选为160~270℃。
氟聚合物(b1)的熔点是通过使用DSC装置(セイコ一社制),以10℃/分钟的速度升温时作为熔化热曲线中对应于极大值的温度来求出。MFR是使用熔融指数仪(东洋精机制作所(株)制),在各温度、5kg荷重下测定从直径2mm、长度8mm的喷嘴在单元时间(10分钟)流出的聚合物的重量(g)。
此外,氟聚合物(b1)的分子量优选为在所得成形体发挥良好机械特性、燃料低透过性等的的范围内。例如,在将熔体流动速率(MFR)作为分子量的指标时,作为氟聚合物的一般成形温度范围的约230~350℃的范围内任意温度下的MFR优选为0.5~100g/10分钟。更优选为2~50g/10分钟,更加优选为5~35g/10分钟。
本发明中氟树脂层(B),可以含有这些氟聚合物(b1)中的1种,也可以含有2种以上。
本发明的层叠体中的氟树脂层(B),在将层叠体作为燃料周围的材料使用时,燃料透过系数优选为1.0g·mm/m2/天以下,更优选为0.6g·mm/m2/天以下,进一步优选为0.4g·mm/m2/天以下。
燃料透过系数是将由测定对象树脂所得的薄片放入装有异辛烷/甲苯/乙醇混合溶剂的燃料透过系数测定用杯中,由60℃测定的质量变化所算出的值,其中,异辛烷、甲苯以及乙醇以45∶45∶10的容积比进行混合。
本发明中,如果氟聚合物(b1)在末端具有特定的反应性官能基,则提高与橡胶层(A)的粘结性。因此,可以提供耐冲击性、强度优秀的成形品(例如燃料用箱等)。
此外,在氟聚合物(b1)为全卤聚合物时,耐药品性以及燃料低透过性变得更为优秀。全卤聚合物是指构成聚合体的主链的碳原子全部与卤原子结合的聚合体。
氟树脂层(B),进一步基于目的、用途,在无损于其性能的范围内,还可以配合无机质粉末、玻璃纤维、碳粉末、碳纤维、金属氧化物等各种填充剂。
例如,为了进一步降低燃料透过性,还可以添加蒙脱石、贝得石、皂石、绿脱石、水辉石、锌蒙脱石、硅镁石等蒙脱石系的层状粘度矿物、云母等具有高纵横比的微小层状矿物。
此外,为了赋予导电性,还可以添加导电性填料。作为导电性填料没有特别限定,有例如金属、碳等导电性单体粉末或导电性单体纤维;氧化锌等导电性化合物的粉末;表面导电化处理粉末等。在配合导电性填料时,优选熔融混练制成预粒料。
作为前述导电性单体粉末或导电性单体纤维没有特别限定,有例如铜、镍等金属粉末,铁、不锈钢等金属纤维,碳黑、碳纤维、特开平3-174018号公报等中记载的碳纤维等。
前述表面导电化处理粉末是在玻璃微珠、氧化钛等非导电性粉末的表面实施导电化处理而得的粉末。
作为表面导电化处理的方法没有特别限定,有例如金属溅射、无电解电镀等。
导电性填料中的碳黑,由于经济性、防止静电蓄积的方面有利,适合使用。
配合了导电性填料而成的氟聚合物组合物的体积电阻率优选为1×100~1×109Ω·cm。更优选的下限为1×102Ω·cm,更优选的上限为1×108Ω·cm。
此外,除填充剂以外,还可以配合热稳定化剂、增强剂、紫外线吸收剂、颜料、其他任意添加剂。
本发明的层叠体可以通过将橡胶层(A)与氟树脂层(B)层叠来制造。本发明的层叠体可以在氟树脂层(B)的两侧层叠橡胶层(A),也可以在橡胶层(A)的两侧层叠氟树脂层(B)。此外,还可以在氟树脂层(B)的单侧层叠橡胶层(A)。
橡胶层(A)与氟树脂层(B)的层叠可以采用将橡胶层(A)与氟树脂层(B)各自成形后以压接等手段来层叠的方法、将橡胶层(A)与氟树脂层(B)同时成形来层叠的方法、在橡胶层(A)上涂布氟树脂层(B)的方法的任一种。
在将橡胶层(A)与氟树脂层(B)各自成形后以压接等手段来层叠的方法中,可以采用氟聚合物的成形方法与加硫用橡胶组合物各自单独的成形方法。
橡胶层(A)成形可以将加硫用橡胶组合物通过加热压缩成形法、传递成形法、挤出成形法、射出成形法、砑光成形法、涂装法等制成薄片状、管状等的各种形状的成形体。
氟树脂层(B)可以通过加热压缩成形、熔融挤出成形、射出成形、涂装(包括粉体涂装)等方法来成形。可以使用成形时通常使用的氟聚合物的成形机,例如射出成形机、吹塑成形机、挤出成形机、各种涂装装置等,制造成薄片状、管状等各种形状的层叠体。其中,从生产性优秀的角度,优选熔融挤出成形法。
作为将橡胶层(A)与氟树脂层(B)同时成形而层叠的方法,例举使用形成橡胶层(A)的加硫用橡胶组合物以及形成氟树脂层(B)的氟聚合物(b1),通过多层压缩成形法、多层传递成形法、多层挤出成形法、多层射出成形法、重叠(ダブリング)法等方法在成形的同时进行层叠的方法。这些方法中,由于可以将未加硫成形体的橡胶层(A)与氟树脂层(B)同时层叠,就不特别需要将橡胶层(A)与氟树脂层(B)接合的工序,此外,由于其后的加硫工序中能得到牢固的粘结,因而适合。
本发明的层叠体可以是未加硫的橡胶层(A)与氟树脂层(B)的层叠体,但进一步通过对该未加硫层叠体进行加硫,可以得到牢固的层间粘结力。
即,本发明涉及将本发明的未加硫层叠体进行加硫处理而得到的、将橡胶层(A)加硫而成的橡胶层(A1)与氟树脂层(B)进行加硫粘结而成的层叠体(以下也称为“加硫层叠体”)。
加硫处理可以采用以往公知的加硫用橡胶组合物的加硫方法及条件。例如有对未加硫层叠体长时间加硫的方法、对未加硫层叠体进行作为比较短时间的预处理的热处理(也发生加硫)、然后进行长时间的加硫的方法。其中,对未加硫层叠体进行作为比较短时间的预处理的热处理、然后进行长时间的加硫的方法,由于在预处理中易于得到橡胶层(A)与氟树脂层(B)的密着性,且预处理中即对橡胶层(A)进行加硫而形状稳定化,可以选择各种其后的加硫中层叠体的保持方法,因而优选。
对加硫处理的条件没有特别限定,可以在通常条件下进行,但优选在160~170℃、10分钟~80分钟通过使用蒸汽(スチ一ム)、压缩(プレス)、烤炉(オ一ブン)、空气浴(エア一バス)、红外线、微波、包铅加硫等来进行处理。更优选为在160℃进行20~45分。
所得的加硫层叠体中,加硫橡胶层(A1)与氟树脂层(B)加硫粘结,产生牢固的层间粘结力。
本发明层叠体(未加硫层叠体以及加硫层叠体)中,可以是橡胶层(A、A1,以下以橡胶层(A)来代表)与氟树脂层(B)的2层结构,也可以是(A)-(B)-(A)或(B)-(A)-(B)这样的3层结构。进而,也可以是粘结了橡胶层(A)以及氟树脂层(B)以外的聚合物层(C)的3层以上的多层结构,(A)-(B)-(C)的3层结构是优选的实施方式之一。本发明的层叠体可以是在氟树脂层(B)的单侧层叠橡胶层(A)且在另一侧层叠出了橡胶层(A)和氟树脂层(B)以外的聚合物层(C),也可以是在氟树脂层(B)的两侧层叠橡胶层(A),进一步在其两侧或单侧层叠氟树脂层(B)以外的聚合物层(C)。
作为聚合物层(C),可以是橡胶层(A)以外的橡胶层(C1)。此外,在(A)-(B)-(A)的(A)层的外侧的单侧或者两侧也可以具有(C)层。
作为橡胶层(C1)的材料,可以例举环氧氯丙烷橡胶以外的橡胶,可以是氟橡胶也可以是非氟橡胶。从耐燃料性、燃料阻挡性的观点出发,优选氟橡胶,从耐寒性良好的角度、成本方面优秀的角度出发,优选非氟橡胶。
作为非氟橡胶的具体例,例如有丙烯腈-丁二烯橡胶(NBR)或其氢化物(HNBR)、苯乙烯-丁二烯橡胶(SBR)、氯丁橡胶(CR)、丁二烯橡胶(BR)、天然橡胶(NR)、异戊橡胶(IR)等二烯系橡胶,乙烯-丙烯-三单体共聚体橡胶、有机硅橡胶、丁基橡胶、丙烯酸系橡胶等。
作为非氟橡胶,从耐热性、耐油性、耐候性、挤出成形性良好的角度出发,优选二烯系的橡胶。更优选NBR或HNBR。聚合物层(C)优选由丙烯腈-丁二烯橡胶或其氢化物构成。
此外,在形成橡胶层(C1)的未加硫橡胶组合物中,也可以配合加硫剂、其他配合剂。
接着,对本发明的层叠体层结构进行说明。
(1)橡胶层(A)-氟树脂层(B)的2层结构
是基本结构,如上所述,以往,由于氟树脂层(B)与橡胶层(A)层叠时,层间(氟树脂层-橡胶层)的粘结不充分,要实施树脂侧的表面处理、在层间涂布另外的粘结剂、缠绕胶带状的薄膜来固定等的工序,变得复杂,通过加硫而产生加硫粘结则不需要组合如此的复杂工序,得到化学性的牢固粘结。
(2)橡胶层-氟树脂层(B)-橡胶层的3层结构
是(A)-(B)-(A)以及(A)-(B)-(C1)。在要求密封性的场合,例如燃料配管等接合部,为了保持密封性,希望在两侧配置橡胶层。内外层的橡胶层可以是相同种类,也可以是不同种类。
作为(A)-(B)-(C1)的3层结构,作为橡胶层(C1)优选是由NBR或HNBR形成的层。
此外,将燃料配管设置成(A)-(B)-(C1)型结构,作为橡胶层(C1)而设置氟橡胶层,通过使配管的内层为橡胶层(C1),提高耐药品性、燃料低透过性。
(3)树脂层-橡胶层(A)-树脂层的3层结构
(B)-(A)-(B)的3层结构中,内外层的树脂层可以是相同种类,也可以是不同种类。
(4)氟树脂层(B)-橡胶层(A)-橡胶层(C1)的3层结构
(5)4层结构以上
除了(2)~(4)的3层结构以外,对应于目的可以进一步层叠任意的橡胶层(A)或(C1)、树脂层(B)。此外,也可以设置金属箔等的层,在橡胶层(C)与氟树脂层(B)的层间以外也可以介入粘结剂层。
此外,进而还可与聚合物层(C)层叠而构成衬里(ライニング)体。
此外,各层的厚度、形状等可以根据使用目的、使用实施方式等适宜选定。
此外,以提高耐压为目的,可以适当设置增强丝等增强层。
本发明的层叠体、特别是加硫层叠体,除了燃料低透过性优秀以外,耐热性、耐油性、耐燃料油性、耐LLC性、耐蒸汽性、耐侯性、耐臭氧性也优秀,此外,可以充分耐得住在苛酷条件下使用,可以用于各种用途。
例如,具有作为汽车用发动机的发动机本体、主运动系统、动阀系统、润滑冷却系统、燃料系统、吸气排气系统等、驱动系统的传输系统等、底盘转向系统、制动系统等、电装品的基本电装部品、控制系统电装部品、装备电装部品等的所要求的耐热性、耐油性、耐燃料油性、耐LLC性、耐蒸汽性的垫片、非接触型以及接触型的垫片类(自我密封垫片、活塞环、开口环形垫片、机械密封、油密封等)等的密封、波纹管、隔膜(ダイヤフラム)、软管、管、电线等的合适特性。
具体的,能用于下列用途。
发动机主体的缸盖垫片、缸盖罩垫片、油底壳垫片、一般垫片等垫片、O型环、垫片、正时皮带罩垫片等的密封、控制软管等的软管、发动机支架的防振橡胶、储氢系统内的高压阀用密封材等。
主运动系统的曲轴密封、凸轮轴密封等的轴密封等。
动阀系统的发动机气门的阀杆密封等。
润滑冷却系统的发动机油冷却器的发动机油冷却软管、回油软管、密封垫片等、散热器周边的水管、真空泵的真空泵油软管等。
燃料系统的燃料泵的油密封、隔膜、阀等、加油(颈部)软管、燃料供给软管、燃料回油软管、蒸气(蒸发)软管等燃料软管、燃料箱的箱内软管、加油密封、箱垫片、箱内燃料泵支架等、燃料配管的管主体、连接器O型环等、燃料喷射装置的喷油器垫环、喷油器密封环、喷油器O型环、压力调节器隔膜、止回阀类等、化油器的针型阀瓣、加速泵活塞、法兰垫片、控制软管等、复合空气控制装置(CAC)的阀薄片、隔膜等。其中,作为燃料软管及燃料箱的箱内软管而合适。
吸气排气系统的歧管的吸气歧管垫片、排气歧管垫片等、EGR(排气时循环)的隔膜、控制软管、排放控制软管等、BPT的隔膜等、AB阀的后燃防止阀薄片等、节流阀的节流阀体垫片、涡轮增压器的涡轮油管(供给)、涡轮油管(回流)、涡轮空气软管、中间冷却器软管、涡轮轴密封等。
传输系统的传输关联的轴承密封、油密封、O型环、垫片、变矩器软管等、AT的任务油(Mission oil)软管、ATF软管、O型环、垫片类等。
转向系统的转向助力油软管等。
制动系统的油密封、O型环、垫片、制动油软管等、主背板(マスタ一バツク)的大气阀、真空阀、隔膜等、主缸的活塞杯(橡胶杯)等、卡钳密封、护套(Boots)类等。
基本电装品的电线(线束)的绝缘体、鞘等、线束外装部品的管等。
控制系统电装品的各种传感器线的被覆材料等。
装备电装品的空调的O型环、垫片、冷却器软管、外装品的挡风玻璃雨刷等。
此外,除了汽车用以外,在例如船舶、航空器等的输送机器中的耐油、耐药品、耐热、耐蒸汽或耐候用的垫片、O型环、软管、其他密封材、隔膜、阀中,或者在化工厂中同样的垫片、O型环、密封材、隔膜、阀、软管、辊、管、耐药品用涂层、衬里中,在食品工厂机器以及食品机器(包括家庭用品)中同样的垫片、O型环、软管、密封材、带、隔膜、阀、辊、管中,在核电站机器中同样的垫片、O型环、软管、密封材、隔膜、阀、管中,在OA机器、一般工业部品中同样的垫片、O型环、软管、密封材、隔膜、阀、辊、管、衬里、芯棒(マンドレル)、电线、柔性连接、带、橡胶板、密封条、PPC复写机的辊片(Rollblade)等的用途中适用。例如,由于PTFE隔膜的支持(バツクアツプ)橡胶材防滑性差,在使用中有减薄、破裂的问题,但通过使用本发明的层叠体,能够改善该问题,适合于使用。
此外,在食品橡胶密封材用途中,以往会有橡胶密封材中的味道、橡胶的碎片等混入食品中的麻烦,通过使用本发明的层叠体,能够改善该问题,适合于使用。医药化学用途的橡胶密封材作为使用溶剂的配管的密封材,橡胶材料有被溶剂膨润的问题,通过使用本发明的层叠体,通过覆盖树脂而得到改善。在一般工业领域,为了改善橡胶材料的强度、防滑性、耐药品性、透过性,可以在例如橡胶辊、O型环、垫片、密封材等中适合于使用。特别地,在锂离子电池的垫片用途中,由于可以同时维持耐药品性和密封的两方面特性,而适合于好适。在其他的要求低摩擦的滑动性的用途中,适合于使用。
其中,上述层叠体特别适宜于用作管或软管。即,上述层叠体优选作为管或软管。在管中,基于耐热性、燃料低透过性的特点,可以适宜地用于汽车用的燃料配管或软管。
由本发明的前述层叠体构成的燃料配管可以由通常的方法来制造,没有特别限制。
【实施例】
接下来,通过实施例来说明本发明,但本发明不受这些实施例的限定。
以下,对实施例以及比较例中使用的氟树脂以及其测定方法进行说明。
(1)熔点
使用セイコ一型DSC装置,记录以10℃/min的速度升温时的熔化峰,以极大值所对应的温度为熔点。
(2)MFR(Melt Flo w Rate)
使用熔融指数仪(东洋精机制作所(株)制),在各种温度下,测定在5kg加重下在单位时间(10分钟)内由直径2mm、长度8mm的喷嘴流出的聚合物的重量(g)。
(3)单层的燃料透过系数的测定
将树脂粒料分别放入直径120mm的模具,放置到加热至300℃的加压机中,以约2.9MPa的压力熔融加压,得到厚度0.15mm的薄片。在投入有CE10(异辛烷与甲苯的的容量比50∶50的混合物中加入乙醇10容量%的混合燃料)18mL的内径高度20mm的SUS316制的透过系数测定用杯中,放入所得薄片,测定直至1000小时的60℃下的质量变化。由每小时的质量变化、接液部的薄片的表面积以及薄片的厚度算出燃料透过系数(g·mm/m2/day)。
以下,实施例以及比较例中的氟树脂如下记表1中所示。
【表1】
(加硫用橡胶组合物1~8及A~C)
将下记表2中所示的材料,由调温到40℃的8英寸开放辊来混练、得到约3mm厚度的薄片状的加硫用橡胶组合物1~8及A~C。其中,表2的各数值表示为质量份。
(实施例1~8、比较例1~3)
将厚度约3mm的表2中所示的加硫用橡胶组合物的薄片与表1中所示厚度的氟树脂薄片重叠,在一个端部在两薄片之间夹入宽约10~15mm的树脂薄膜(厚度10μm的离形薄膜)后,插入到放有金属制隔离器的模具中,以使得所得薄片的厚度为2mm,通过在170℃加压15分钟加压,得到薄片状的层叠体。将所得层叠体裁切成宽10mm×长度40mm×3套的长条状,剥离离形薄膜,制成有抓握力的试验片。使用オ一トグラフ((株)岛津制作所制AGS-J 5kN),按照JIS-K-6256(交联橡胶的粘结试验方法)记载的方法,在25℃以50mm/min的拉伸速度,对该试验片进行剥离试验,观测剥离模式,以如下的基准来评价。所得结果如表2所示。
(粘结评价)
○…在层叠体的界面,加硫用橡胶组合物或氟树脂发生材料破坏,在界面不可能剥离。
×…在层叠体的界面比较容易剥离。
以下显示实施例以及比较例中使用的配合剂。
*1“エピクロマ一CG”ダイソ一株式会社制
*2“シ一ストSO”东海カ一ボン株式会社制
*3“アデカサイザ一RS107”株式会社ADEKA制
*4“スプレンダ一R300”花王株式会社制
*5“DHT-4A”协和化学工业株式会社制
*6“ダイソネツトXL-21S”ダイソ一株式会社制
*7“JER828”三菱化学株式会社制
*8“バ一ゲス#30”白石カルシウム社制
【产业上的利用可能性】
本发明的层叠体,特别是加硫层叠体,不仅燃料低透过性优秀,耐热性、耐油性、耐燃料油性、耐LLC性、耐蒸汽性也优秀,能够用于汽车用发动机的发动机本体、主运动系统、动阀系统、润滑冷却系统、燃料系统、吸气排气系统等、驱动系统的传输系统等、底盘转向系统、制动系统等、电装品的基本电装部品、控制系统电装部品、装备电装部品等的要求耐热性、耐油性、耐燃料油性、耐LLC性、耐蒸汽性的垫片、非接触型以及接触型的垫片类(自我密封垫片、活塞环、开口环形垫片、机械密封、油密封等)等的密封、波纹管、隔膜、软管、管、电线等。
Claims (20)
1.一种层叠体,是具有橡胶层(A)与层叠在橡胶层(A)上的氟树脂层(B)的层叠体,其特征在于,
橡胶层(A)是由加硫用橡胶组合物形成的层,加硫用橡胶组合物含有:
环氧氯丙烷橡胶(a1);
从由1,8-二氮杂二环(5.4.0)十一烯-7盐、1,5-二氮杂二环(4.3.0)-壬烯-5盐、1,8-二氮杂二环(5.4.0)十一烯-7及1,5-二氮杂二环(4.3.0)-壬烯-5组成的群中选择的至少1种化合物(a2);
环氧树脂(a3);以及
从钙、镁、钠、铜中选择的金属硫酸盐和/或醋酸盐的水合物,
氟树脂层(B)是由氟聚合物组合物形成的层,氟聚合物组合物含有具有来自氯三氟乙烯的共聚单元的氟聚合物(b1)。
2.如权利要求1所述的层叠体,其中,加硫用橡胶组合物进一步含有铜盐(a5)。
3.如权利要求2所述的层叠体,其中,铜盐(a5)是有机铜盐。
4.如权利要求2或3所述的层叠体,其中,铜盐(a5)是从饱和羧酸的铜盐、不饱和羧酸的铜盐、芳香族羧酸的铜盐及硫代氨基甲酸的铜盐中选择的至少1种。
5.如权利要求2所述的层叠体,其中,铜盐(a5)是从硬脂酸铜、二甲基二硫代氨基甲酸铜、二乙基二硫代氨基甲酸铜及二丁基二硫代氨基甲酸铜中选择的至少1种。
6.如权利要求2所述的层叠体,其中,相对于环氧氯丙烷橡胶(a1)100重量份,铜盐(a5)为0.01质量份以上、3质量份以下。
7.如权利要求1或2所述的层叠体,其中,化合物(a2)是从由1,8-二氮杂二环(5.4.0)十一烯-7的对甲苯磺酸盐、1,8-二氮杂二环(5.4.0)十一烯-7的苯酚盐、1,8-二氮杂二环(5.4.0)十一烯-7的苯酚树脂盐、1,8-二氮杂二环(5.4.0)十一烯-7的邻苯二甲酸盐、1,8-二氮杂二环(5.4.0)十一烯-7的蚁酸盐、1,8-二氮杂二环(5.4.0)十一烯-7的辛酸盐、1,5-二氮杂二环(4.3.0)-壬烯-5的对甲苯磺酸盐、1,5-二氮杂二环(4.3.0)-壬烯-5的苯酚盐、1,5-二氮杂二环(4.3.0)-壬烯-5的苯酚树脂盐、1,5-二氮杂二环(4.3.0)-壬烯-5的邻苯二甲酸盐、1,5-二氮杂二环(4.3.0)-壬烯-5的蚁酸盐、1,5-二氮杂二环(4.3.0)-壬烯-5的辛酸盐、1,8-二氮杂二环(5.4.0)十一烯-7及1,5-二氮杂二环(4.3.0)-壬烯-5组成的群中选择的至少1种化合物。
8.如权利要求1或2所述的层叠体,其中,相对于环氧氯丙烷橡胶(a1)100质量份,化合物(a2)为0.5质量份以上、3.0质量份以下。
9.如权利要求1或2所述的层叠体,其中,加硫用橡胶组合物进一步含有从由硫脲系加硫剂、喹喔啉系加硫剂、硫系加硫剂、过氧化物系加硫剂及双酚系加硫剂组成的群中选择的至少1种加硫剂(a6)。
10.如权利要求1或2所述的层叠体,其中,环氧氯丙烷橡胶(a1)是具有基于环氧氯丙烷的聚合单元和基于环氧乙烷的聚合单元的聚合体。
11.如权利要求1或2所述的层叠体,其中,环氧氯丙烷橡胶(a1)是具有基于环氧氯丙烷的聚合单元、基于环氧乙烷的聚合单元以及基于烯丙基缩水甘油醚的聚合单元的聚合体。
12.如权利要求1或2所述的层叠体,其中,氟聚合物(b1)是氯三氟乙烯-四氟乙烯-全氟(烷基乙烯醚)共聚体。
13.如权利要求1或2所述的层叠体,其中,在氟树脂层(B)的两侧层叠有橡胶层(A)。
14.如权利要求1或2所述的层叠体,其中,在氟树脂层(B)的单侧层叠有橡胶层(A),且在另一侧层叠有除了橡胶层(A)和氟树脂层(B)之外的聚合物层(C)。
15.如权利要求14所述的层叠体,其中,聚合物层(C)由丙烯腈-丁二烯橡胶或其氢化物构成。
16.如权利要求1或2所述的层叠体,其中,在氟树脂层(B)的两侧层叠有橡胶层(A),进而在其两侧或者单侧层叠有除氟树脂层(B)以外的聚合物层(C)。
17.如权利要求1或2所述的层叠体,其中,在橡胶层(A)的两侧层叠有氟树脂层(B)。
18.一种层叠体,特征在于,通过将权利要求1~17任一项所述的层叠体进行加硫处理而获得,
将对橡胶层(A)进行加硫而成的橡胶层(A1)与氟树脂层(B)进行加硫粘结。
19.一种管,特征在于,具有如权利要求1~18任一项所述的层叠体。
20.一种汽车用燃料配管,特征在于,具有如权利要求1~18任一项所述的层叠体。
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JP2010254309 | 2010-11-12 | ||
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JP2011-045942 | 2011-03-03 | ||
PCT/JP2011/075923 WO2012063893A1 (ja) | 2010-11-12 | 2011-11-10 | 積層体 |
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CN103249554B true CN103249554B (zh) | 2015-07-08 |
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US (1) | US20130230675A1 (zh) |
EP (1) | EP2639059B1 (zh) |
JP (1) | JP5955222B2 (zh) |
KR (1) | KR101509486B1 (zh) |
CN (1) | CN103249554B (zh) |
ES (1) | ES2768076T3 (zh) |
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US9404022B2 (en) | 2010-11-12 | 2016-08-02 | Osaka Soda Co., Ltd. | Composition for vulcanizing adhesion |
KR101840957B1 (ko) * | 2013-11-15 | 2018-03-21 | 다이킨 고교 가부시키가이샤 | 적층체, 적층체의 제조 방법 및 불소 고무 조성물 |
WO2015088940A1 (en) * | 2013-12-09 | 2015-06-18 | 3M Innovative Properties Company | A fluoroelastomer component for contacting ammonia and/or urea |
JP6357768B2 (ja) * | 2013-12-26 | 2018-07-18 | ダイキン工業株式会社 | 積層体 |
JP6954272B2 (ja) * | 2016-04-28 | 2021-10-27 | 株式会社大阪ソーダ | 積層体用組成物 |
US20190359801A1 (en) * | 2016-12-15 | 2019-11-28 | Unimatec Co., Ltd. | Carboxyl group-containing acrylic rubber composition and rubber laminate using the same |
KR101881819B1 (ko) * | 2018-01-25 | 2018-07-25 | 주식회사 엔시테크 | 고밀도 폴리에틸렌관 |
CN111867829A (zh) * | 2018-03-14 | 2020-10-30 | 三井化学株式会社 | 层叠体及其用途 |
JPWO2019220850A1 (ja) | 2018-05-14 | 2021-06-17 | ダイキン工業株式会社 | 積層体およびチューブ |
CN113056371B (zh) * | 2018-12-07 | 2023-05-05 | 日本瑞翁株式会社 | 表卤代醇系橡胶组合物、橡胶交联物、橡胶层叠体及软管 |
WO2023190177A1 (ja) * | 2022-03-31 | 2023-10-05 | 株式会社大阪ソーダ | 加硫接着用組成物、加硫接着積層体用組成物ならびにこれらを用いた積層体 |
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KR101487051B1 (ko) * | 2008-01-30 | 2015-01-28 | 다이소 가부시키가이샤 | 가황 고무 적층체 |
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- 2011-11-10 JP JP2012542970A patent/JP5955222B2/ja active Active
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- 2011-11-10 EP EP11840574.5A patent/EP2639059B1/en active Active
- 2011-11-10 ES ES11840574T patent/ES2768076T3/es active Active
- 2011-11-10 CN CN201180054477.2A patent/CN103249554B/zh active Active
- 2011-11-10 KR KR1020137014614A patent/KR101509486B1/ko active IP Right Grant
- 2011-11-10 WO PCT/JP2011/075923 patent/WO2012063893A1/ja active Application Filing
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KR101509486B1 (ko) | 2015-04-07 |
US20130230675A1 (en) | 2013-09-05 |
JPWO2012063893A1 (ja) | 2014-05-12 |
EP2639059A4 (en) | 2017-06-28 |
EP2639059B1 (en) | 2020-01-08 |
WO2012063893A1 (ja) | 2012-05-18 |
CN103249554A (zh) | 2013-08-14 |
JP5955222B2 (ja) | 2016-07-20 |
ES2768076T3 (es) | 2020-06-19 |
KR20130084319A (ko) | 2013-07-24 |
EP2639059A1 (en) | 2013-09-18 |
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