CN113646172A - 层叠体 - Google Patents
层叠体 Download PDFInfo
- Publication number
- CN113646172A CN113646172A CN202080025790.2A CN202080025790A CN113646172A CN 113646172 A CN113646172 A CN 113646172A CN 202080025790 A CN202080025790 A CN 202080025790A CN 113646172 A CN113646172 A CN 113646172A
- Authority
- CN
- China
- Prior art keywords
- group
- polyamide
- hfc
- laminate
- layer
- 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.)
- Pending
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- 229920000098 polyolefin Polymers 0.000 claims abstract description 109
- 150000001875 compounds Chemical class 0.000 claims abstract description 62
- 239000004953 Aliphatic polyamide Substances 0.000 claims abstract description 52
- 229920003231 aliphatic polyamide Polymers 0.000 claims abstract description 52
- 239000000203 mixture Substances 0.000 claims abstract description 52
- 125000000524 functional group Chemical group 0.000 claims abstract description 31
- 125000003178 carboxy group Chemical group [H]OC(*)=O 0.000 claims abstract description 30
- 239000000178 monomer Substances 0.000 claims abstract description 29
- 125000003277 amino group Chemical group 0.000 claims abstract description 18
- 239000004711 α-olefin Substances 0.000 claims abstract description 17
- 125000004432 carbon atom Chemical group C* 0.000 claims abstract description 15
- 125000003368 amide group Chemical group 0.000 claims abstract description 12
- 125000002887 hydroxy group Chemical group [H]O* 0.000 claims abstract description 8
- 125000003396 thiol group Chemical group [H]S* 0.000 claims abstract description 8
- 125000003700 epoxy group Chemical group 0.000 claims abstract description 7
- 125000005462 imide group Chemical group 0.000 claims abstract description 7
- IQPQWNKOIGAROB-UHFFFAOYSA-N isocyanate group Chemical group [N-]=C=O IQPQWNKOIGAROB-UHFFFAOYSA-N 0.000 claims abstract description 7
- 125000002560 nitrile group Chemical group 0.000 claims abstract description 7
- 229920002647 polyamide Polymers 0.000 claims description 102
- 239000004952 Polyamide Substances 0.000 claims description 101
- -1 polypropylene Polymers 0.000 claims description 80
- 239000003795 chemical substances by application Substances 0.000 claims description 34
- 238000000034 method Methods 0.000 claims description 34
- 239000004014 plasticizer Substances 0.000 claims description 19
- 239000004743 Polypropylene Substances 0.000 claims description 18
- 229920001155 polypropylene Polymers 0.000 claims description 18
- 239000002994 raw material Substances 0.000 claims description 15
- 229920000299 Nylon 12 Polymers 0.000 claims description 13
- 229920001577 copolymer Polymers 0.000 claims description 13
- 230000009102 absorption Effects 0.000 claims description 10
- 238000010521 absorption reaction Methods 0.000 claims description 10
- 238000000465 moulding Methods 0.000 claims description 10
- 238000005033 Fourier transform infrared spectroscopy Methods 0.000 claims description 8
- 229920000571 Nylon 11 Polymers 0.000 claims description 6
- 229920000305 Nylon 6,10 Polymers 0.000 claims description 6
- 229920001519 homopolymer Polymers 0.000 claims description 6
- 229920000572 Nylon 6/12 Polymers 0.000 claims description 5
- 229920006152 PA1010 Polymers 0.000 claims description 5
- 125000001570 methylene group Chemical group [H]C([H])([*:1])[*:2] 0.000 claims description 5
- 229920006396 polyamide 1012 Polymers 0.000 claims description 5
- 230000004048 modification Effects 0.000 claims description 4
- 238000012986 modification Methods 0.000 claims description 4
- 239000010410 layer Substances 0.000 description 133
- 239000000243 solution Substances 0.000 description 37
- 239000000126 substance Substances 0.000 description 32
- 125000006367 bivalent amino carbonyl group Chemical group [H]N([*:1])C([*:2])=O 0.000 description 28
- 230000000704 physical effect Effects 0.000 description 19
- 229920005989 resin Polymers 0.000 description 19
- 239000011347 resin Substances 0.000 description 19
- 230000000052 comparative effect Effects 0.000 description 16
- 239000000463 material Substances 0.000 description 16
- VZSRBBMJRBPUNF-UHFFFAOYSA-N 2-(2,3-dihydro-1H-inden-2-ylamino)-N-[3-oxo-3-(2,4,6,7-tetrahydrotriazolo[4,5-c]pyridin-5-yl)propyl]pyrimidine-5-carboxamide Chemical compound C1C(CC2=CC=CC=C12)NC1=NC=C(C=N1)C(=O)NCCC(N1CC2=C(CC1)NN=N2)=O VZSRBBMJRBPUNF-UHFFFAOYSA-N 0.000 description 14
- 238000006116 polymerization reaction Methods 0.000 description 14
- XSQUKJJJFZCRTK-UHFFFAOYSA-N Urea Chemical compound NC(N)=O XSQUKJJJFZCRTK-UHFFFAOYSA-N 0.000 description 12
- 229920000642 polymer Polymers 0.000 description 12
- 230000004888 barrier function Effects 0.000 description 11
- 239000012530 fluid Substances 0.000 description 11
- 239000003507 refrigerant Substances 0.000 description 11
- 150000001412 amines Chemical class 0.000 description 10
- 238000004519 manufacturing process Methods 0.000 description 10
- OFOBLEOULBTSOW-UHFFFAOYSA-N Malonic acid Chemical compound OC(=O)CC(O)=O OFOBLEOULBTSOW-UHFFFAOYSA-N 0.000 description 9
- FPYJFEHAWHCUMM-UHFFFAOYSA-N maleic anhydride Chemical compound O=C1OC(=O)C=C1 FPYJFEHAWHCUMM-UHFFFAOYSA-N 0.000 description 9
- QQONPFPTGQHPMA-UHFFFAOYSA-N propylene Natural products CC=C QQONPFPTGQHPMA-UHFFFAOYSA-N 0.000 description 9
- 125000004805 propylene group Chemical group [H]C([H])([H])C([H])([*:1])C([H])([H])[*:2] 0.000 description 9
- XLYOFNOQVPJJNP-UHFFFAOYSA-N water Substances O XLYOFNOQVPJJNP-UHFFFAOYSA-N 0.000 description 9
- AFFLGGQVNFXPEV-UHFFFAOYSA-N 1-decene Chemical compound CCCCCCCCC=C AFFLGGQVNFXPEV-UHFFFAOYSA-N 0.000 description 8
- LFQSCWFLJHTTHZ-UHFFFAOYSA-N Ethanol Chemical compound CCO LFQSCWFLJHTTHZ-UHFFFAOYSA-N 0.000 description 8
- VGGSQFUCUMXWEO-UHFFFAOYSA-N Ethene Chemical compound C=C VGGSQFUCUMXWEO-UHFFFAOYSA-N 0.000 description 8
- 239000005977 Ethylene Substances 0.000 description 8
- AFCARXCZXQIEQB-UHFFFAOYSA-N N-[3-oxo-3-(2,4,6,7-tetrahydrotriazolo[4,5-c]pyridin-5-yl)propyl]-2-[[3-(trifluoromethoxy)phenyl]methylamino]pyrimidine-5-carboxamide Chemical compound O=C(CCNC(=O)C=1C=NC(=NC=1)NCC1=CC(=CC=C1)OC(F)(F)F)N1CC2=C(CC1)NN=N2 AFCARXCZXQIEQB-UHFFFAOYSA-N 0.000 description 8
- IPRJXAGUEGOFGG-UHFFFAOYSA-N N-butylbenzenesulfonamide Chemical compound CCCCNS(=O)(=O)C1=CC=CC=C1 IPRJXAGUEGOFGG-UHFFFAOYSA-N 0.000 description 8
- 238000006243 chemical reaction Methods 0.000 description 8
- 238000001816 cooling Methods 0.000 description 8
- 239000002253 acid Substances 0.000 description 7
- 125000001931 aliphatic group Chemical group 0.000 description 7
- 239000003963 antioxidant agent Substances 0.000 description 7
- 239000002826 coolant Substances 0.000 description 7
- 229920001971 elastomer Polymers 0.000 description 7
- 239000000446 fuel Substances 0.000 description 7
- 230000001681 protective effect Effects 0.000 description 7
- ZGEGCLOFRBLKSE-UHFFFAOYSA-N 1-Heptene Chemical compound CCCCCC=C ZGEGCLOFRBLKSE-UHFFFAOYSA-N 0.000 description 6
- CRSBERNSMYQZNG-UHFFFAOYSA-N 1-dodecene Chemical compound CCCCCCCCCCC=C CRSBERNSMYQZNG-UHFFFAOYSA-N 0.000 description 6
- JRZJOMJEPLMPRA-UHFFFAOYSA-N 1-nonene Chemical compound CCCCCCCC=C JRZJOMJEPLMPRA-UHFFFAOYSA-N 0.000 description 6
- LYCAIKOWRPUZTN-UHFFFAOYSA-N Ethylene glycol Chemical compound OCCO LYCAIKOWRPUZTN-UHFFFAOYSA-N 0.000 description 6
- VZCYOOQTPOCHFL-OWOJBTEDSA-N Fumaric acid Chemical compound OC(=O)\C=C\C(O)=O VZCYOOQTPOCHFL-OWOJBTEDSA-N 0.000 description 6
- OKKJLVBELUTLKV-UHFFFAOYSA-N Methanol Chemical compound OC OKKJLVBELUTLKV-UHFFFAOYSA-N 0.000 description 6
- ISWSIDIOOBJBQZ-UHFFFAOYSA-N Phenol Chemical compound OC1=CC=CC=C1 ISWSIDIOOBJBQZ-UHFFFAOYSA-N 0.000 description 6
- PPBRXRYQALVLMV-UHFFFAOYSA-N Styrene Chemical compound C=CC1=CC=CC=C1 PPBRXRYQALVLMV-UHFFFAOYSA-N 0.000 description 6
- YXFVVABEGXRONW-UHFFFAOYSA-N Toluene Chemical compound CC1=CC=CC=C1 YXFVVABEGXRONW-UHFFFAOYSA-N 0.000 description 6
- 239000004202 carbamide Substances 0.000 description 6
- 239000007789 gas Substances 0.000 description 6
- 239000003502 gasoline Substances 0.000 description 6
- 238000004898 kneading Methods 0.000 description 6
- 239000003921 oil Substances 0.000 description 6
- 235000019198 oils Nutrition 0.000 description 6
- 229920005992 thermoplastic resin Polymers 0.000 description 6
- VZCYOOQTPOCHFL-UHFFFAOYSA-N trans-butenedioic acid Natural products OC(=O)C=CC(O)=O VZCYOOQTPOCHFL-UHFFFAOYSA-N 0.000 description 6
- OFNISBHGPNMTMS-UHFFFAOYSA-N 3-methylideneoxolane-2,5-dione Chemical compound C=C1CC(=O)OC1=O OFNISBHGPNMTMS-UHFFFAOYSA-N 0.000 description 5
- LCGLNKUTAGEVQW-UHFFFAOYSA-N Dimethyl ether Chemical compound COC LCGLNKUTAGEVQW-UHFFFAOYSA-N 0.000 description 5
- CERQOIWHTDAKMF-UHFFFAOYSA-N Methacrylic acid Chemical compound CC(=C)C(O)=O CERQOIWHTDAKMF-UHFFFAOYSA-N 0.000 description 5
- 229920000459 Nitrile rubber Polymers 0.000 description 5
- 150000001336 alkenes Chemical class 0.000 description 5
- 230000003078 antioxidant effect Effects 0.000 description 5
- 150000001735 carboxylic acids Chemical class 0.000 description 5
- 150000001993 dienes Chemical class 0.000 description 5
- 150000002148 esters Chemical class 0.000 description 5
- 239000012760 heat stabilizer Substances 0.000 description 5
- 238000010438 heat treatment Methods 0.000 description 5
- 239000011229 interlayer Substances 0.000 description 5
- 230000007774 longterm Effects 0.000 description 5
- 229910052751 metal Inorganic materials 0.000 description 5
- 239000002184 metal Substances 0.000 description 5
- 150000004702 methyl esters Chemical class 0.000 description 5
- FJXWKBZRTWEWBJ-UHFFFAOYSA-N nonanediamide Chemical compound NC(=O)CCCCCCCC(N)=O FJXWKBZRTWEWBJ-UHFFFAOYSA-N 0.000 description 5
- 229920001748 polybutylene Polymers 0.000 description 5
- 230000008569 process Effects 0.000 description 5
- 239000000047 product Substances 0.000 description 5
- 150000007934 α,β-unsaturated carboxylic acids Chemical class 0.000 description 5
- XWJBRBSPAODJER-UHFFFAOYSA-N 1,7-octadiene Chemical compound C=CCCCCC=C XWJBRBSPAODJER-UHFFFAOYSA-N 0.000 description 4
- VXNZUUAINFGPBY-UHFFFAOYSA-N 1-Butene Chemical compound CCC=C VXNZUUAINFGPBY-UHFFFAOYSA-N 0.000 description 4
- VQOXUMQBYILCKR-UHFFFAOYSA-N 1-Tridecene Chemical compound CCCCCCCCCCCC=C VQOXUMQBYILCKR-UHFFFAOYSA-N 0.000 description 4
- ADOBXTDBFNCOBN-UHFFFAOYSA-N 1-heptadecene Chemical compound CCCCCCCCCCCCCCCC=C ADOBXTDBFNCOBN-UHFFFAOYSA-N 0.000 description 4
- GQEZCXVZFLOKMC-UHFFFAOYSA-N 1-hexadecene Chemical compound CCCCCCCCCCCCCCC=C GQEZCXVZFLOKMC-UHFFFAOYSA-N 0.000 description 4
- LIKMAJRDDDTEIG-UHFFFAOYSA-N 1-hexene Chemical compound CCCCC=C LIKMAJRDDDTEIG-UHFFFAOYSA-N 0.000 description 4
- KWKAKUADMBZCLK-UHFFFAOYSA-N 1-octene Chemical compound CCCCCCC=C KWKAKUADMBZCLK-UHFFFAOYSA-N 0.000 description 4
- PJLHTVIBELQURV-UHFFFAOYSA-N 1-pentadecene Chemical compound CCCCCCCCCCCCCC=C PJLHTVIBELQURV-UHFFFAOYSA-N 0.000 description 4
- HFDVRLIODXPAHB-UHFFFAOYSA-N 1-tetradecene Chemical compound CCCCCCCCCCCCC=C HFDVRLIODXPAHB-UHFFFAOYSA-N 0.000 description 4
- DCTOHCCUXLBQMS-UHFFFAOYSA-N 1-undecene Chemical compound CCCCCCCCCC=C DCTOHCCUXLBQMS-UHFFFAOYSA-N 0.000 description 4
- SMZOUWXMTYCWNB-UHFFFAOYSA-N 2-(2-methoxy-5-methylphenyl)ethanamine Chemical compound COC1=CC=C(C)C=C1CCN SMZOUWXMTYCWNB-UHFFFAOYSA-N 0.000 description 4
- NIXOWILDQLNWCW-UHFFFAOYSA-N 2-Propenoic acid Natural products OC(=O)C=C NIXOWILDQLNWCW-UHFFFAOYSA-N 0.000 description 4
- AYKYXWQEBUNJCN-UHFFFAOYSA-N 3-methylfuran-2,5-dione Chemical compound CC1=CC(=O)OC1=O AYKYXWQEBUNJCN-UHFFFAOYSA-N 0.000 description 4
- KAKZBPTYRLMSJV-UHFFFAOYSA-N Butadiene Chemical compound C=CC=C KAKZBPTYRLMSJV-UHFFFAOYSA-N 0.000 description 4
- 229920002302 Nylon 6,6 Polymers 0.000 description 4
- OAICVXFJPJFONN-UHFFFAOYSA-N Phosphorus Chemical compound [P] OAICVXFJPJFONN-UHFFFAOYSA-N 0.000 description 4
- 239000005062 Polybutadiene Substances 0.000 description 4
- 125000004018 acid anhydride group Chemical group 0.000 description 4
- 239000000654 additive Substances 0.000 description 4
- WNLRTRBMVRJNCN-UHFFFAOYSA-N adipic acid Chemical compound OC(=O)CCCCC(O)=O WNLRTRBMVRJNCN-UHFFFAOYSA-N 0.000 description 4
- 150000008064 anhydrides Chemical group 0.000 description 4
- MGNZXYYWBUKAII-UHFFFAOYSA-N cyclohexa-1,3-diene Chemical compound C1CC=CC=C1 MGNZXYYWBUKAII-UHFFFAOYSA-N 0.000 description 4
- MTHSVFCYNBDYFN-UHFFFAOYSA-N diethylene glycol Chemical compound OCCOCCO MTHSVFCYNBDYFN-UHFFFAOYSA-N 0.000 description 4
- 239000000806 elastomer Substances 0.000 description 4
- QQHJDPROMQRDLA-UHFFFAOYSA-N hexadecanedioic acid Chemical compound OC(=O)CCCCCCCCCCCCCCC(O)=O QQHJDPROMQRDLA-UHFFFAOYSA-N 0.000 description 4
- JJOJFIHJIRWASH-UHFFFAOYSA-N icosanedioic acid Chemical compound OC(=O)CCCCCCCCCCCCCCCCCCC(O)=O JJOJFIHJIRWASH-UHFFFAOYSA-N 0.000 description 4
- QQVIHTHCMHWDBS-UHFFFAOYSA-N isophthalic acid Chemical compound OC(=O)C1=CC=CC(C(O)=O)=C1 QQVIHTHCMHWDBS-UHFFFAOYSA-N 0.000 description 4
- 229920003049 isoprene rubber Polymers 0.000 description 4
- 239000007788 liquid Substances 0.000 description 4
- 238000005259 measurement Methods 0.000 description 4
- 238000002844 melting Methods 0.000 description 4
- 230000008018 melting Effects 0.000 description 4
- VNWKTOKETHGBQD-UHFFFAOYSA-N methane Chemical compound C VNWKTOKETHGBQD-UHFFFAOYSA-N 0.000 description 4
- VAMFXQBUQXONLZ-UHFFFAOYSA-N n-alpha-eicosene Natural products CCCCCCCCCCCCCCCCCCC=C VAMFXQBUQXONLZ-UHFFFAOYSA-N 0.000 description 4
- BDJRBEYXGGNYIS-UHFFFAOYSA-N nonanedioic acid Chemical compound OC(=O)CCCCCCCC(O)=O BDJRBEYXGGNYIS-UHFFFAOYSA-N 0.000 description 4
- CCCMONHAUSKTEQ-UHFFFAOYSA-N octadec-1-ene Chemical compound CCCCCCCCCCCCCCCCC=C CCCMONHAUSKTEQ-UHFFFAOYSA-N 0.000 description 4
- BNJOQKFENDDGSC-UHFFFAOYSA-N octadecanedioic acid Chemical compound OC(=O)CCCCCCCCCCCCCCCCC(O)=O BNJOQKFENDDGSC-UHFFFAOYSA-N 0.000 description 4
- YWAKXRMUMFPDSH-UHFFFAOYSA-N pentene Chemical compound CCCC=C YWAKXRMUMFPDSH-UHFFFAOYSA-N 0.000 description 4
- 229910052698 phosphorus Inorganic materials 0.000 description 4
- 239000011574 phosphorus Substances 0.000 description 4
- WLJVNTCWHIRURA-UHFFFAOYSA-N pimelic acid Chemical compound OC(=O)CCCCCC(O)=O WLJVNTCWHIRURA-UHFFFAOYSA-N 0.000 description 4
- 229920002857 polybutadiene Polymers 0.000 description 4
- CXMXRPHRNRROMY-UHFFFAOYSA-N sebacic acid Chemical compound OC(=O)CCCCCCCCC(O)=O CXMXRPHRNRROMY-UHFFFAOYSA-N 0.000 description 4
- TYFQFVWCELRYAO-UHFFFAOYSA-N suberic acid Chemical compound OC(=O)CCCCCCC(O)=O TYFQFVWCELRYAO-UHFFFAOYSA-N 0.000 description 4
- LWBHHRRTOZQPDM-UHFFFAOYSA-N undecanedioic acid Chemical compound OC(=O)CCCCCCCCCC(O)=O LWBHHRRTOZQPDM-UHFFFAOYSA-N 0.000 description 4
- KMOUUZVZFBCRAM-OLQVQODUSA-N (3as,7ar)-3a,4,7,7a-tetrahydro-2-benzofuran-1,3-dione Chemical compound C1C=CC[C@@H]2C(=O)OC(=O)[C@@H]21 KMOUUZVZFBCRAM-OLQVQODUSA-N 0.000 description 3
- HITROERJXNWVOI-SOFGYWHQSA-N (5e)-octa-1,5-diene Chemical compound CC\C=C\CCC=C HITROERJXNWVOI-SOFGYWHQSA-N 0.000 description 3
- 229920002818 (Hydroxyethyl)methacrylate Polymers 0.000 description 3
- LVGUZGTVOIAKKC-UHFFFAOYSA-N 1,1,1,2-tetrafluoroethane Chemical compound FCC(F)(F)F LVGUZGTVOIAKKC-UHFFFAOYSA-N 0.000 description 3
- BOUGCJDAQLKBQH-UHFFFAOYSA-N 1-chloro-1,2,2,2-tetrafluoroethane Chemical compound FC(Cl)C(F)(F)F BOUGCJDAQLKBQH-UHFFFAOYSA-N 0.000 description 3
- FXRLMCRCYDHQFW-UHFFFAOYSA-N 2,3,3,3-tetrafluoropropene Chemical compound FC(=C)C(F)(F)F FXRLMCRCYDHQFW-UHFFFAOYSA-N 0.000 description 3
- 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 3
- ZWEHNKRNPOVVGH-UHFFFAOYSA-N 2-Butanone Chemical compound CCC(C)=O ZWEHNKRNPOVVGH-UHFFFAOYSA-N 0.000 description 3
- OMIGHNLMNHATMP-UHFFFAOYSA-N 2-hydroxyethyl prop-2-enoate Chemical compound OCCOC(=O)C=C OMIGHNLMNHATMP-UHFFFAOYSA-N 0.000 description 3
- LDTAOIUHUHHCMU-UHFFFAOYSA-N 3-methylpent-1-ene Chemical compound CCC(C)C=C LDTAOIUHUHHCMU-UHFFFAOYSA-N 0.000 description 3
- HBPSHRBTXIZBDI-UHFFFAOYSA-N 4-ethylidene-8-methylnona-1,7-diene Chemical compound C=CCC(=CC)CCC=C(C)C HBPSHRBTXIZBDI-UHFFFAOYSA-N 0.000 description 3
- WSSSPWUEQFSQQG-UHFFFAOYSA-N 4-methyl-1-pentene Chemical compound CC(C)CC=C WSSSPWUEQFSQQG-UHFFFAOYSA-N 0.000 description 3
- QTBSBXVTEAMEQO-UHFFFAOYSA-N Acetic acid Chemical compound CC(O)=O QTBSBXVTEAMEQO-UHFFFAOYSA-N 0.000 description 3
- CSCPPACGZOOCGX-UHFFFAOYSA-N Acetone Chemical compound CC(C)=O CSCPPACGZOOCGX-UHFFFAOYSA-N 0.000 description 3
- GVNWZKBFMFUVNX-UHFFFAOYSA-N Adipamide Chemical compound NC(=O)CCCCC(N)=O GVNWZKBFMFUVNX-UHFFFAOYSA-N 0.000 description 3
- IJGRMHOSHXDMSA-UHFFFAOYSA-N Atomic nitrogen Chemical compound N#N IJGRMHOSHXDMSA-UHFFFAOYSA-N 0.000 description 3
- UHOVQNZJYSORNB-UHFFFAOYSA-N Benzene Chemical compound C1=CC=CC=C1 UHOVQNZJYSORNB-UHFFFAOYSA-N 0.000 description 3
- WVDDGKGOMKODPV-UHFFFAOYSA-N Benzyl alcohol Chemical compound OCC1=CC=CC=C1 WVDDGKGOMKODPV-UHFFFAOYSA-N 0.000 description 3
- 229920000089 Cyclic olefin copolymer Polymers 0.000 description 3
- 229920002943 EPDM rubber Polymers 0.000 description 3
- YCKRFDGAMUMZLT-UHFFFAOYSA-N Fluorine atom Chemical compound [F] YCKRFDGAMUMZLT-UHFFFAOYSA-N 0.000 description 3
- WOBHKFSMXKNTIM-UHFFFAOYSA-N Hydroxyethyl methacrylate Chemical compound CC(=C)C(=O)OCCO WOBHKFSMXKNTIM-UHFFFAOYSA-N 0.000 description 3
- 239000004698 Polyethylene Substances 0.000 description 3
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- HEMHJVSKTPXQMS-UHFFFAOYSA-M Sodium hydroxide Chemical compound [OH-].[Na+] HEMHJVSKTPXQMS-UHFFFAOYSA-M 0.000 description 3
- 239000000853 adhesive Substances 0.000 description 3
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- 230000000694 effects Effects 0.000 description 3
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- VZCYOOQTPOCHFL-UPHRSURJSA-N maleic acid Chemical compound OC(=O)\C=C/C(O)=O VZCYOOQTPOCHFL-UPHRSURJSA-N 0.000 description 3
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- 238000012545 processing Methods 0.000 description 3
- KIDHWZJUCRJVML-UHFFFAOYSA-N putrescine Chemical compound NCCCCN KIDHWZJUCRJVML-UHFFFAOYSA-N 0.000 description 3
- 239000007870 radical polymerization initiator Substances 0.000 description 3
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- 239000005060 rubber Substances 0.000 description 3
- 239000002904 solvent Substances 0.000 description 3
- 239000003381 stabilizer Substances 0.000 description 3
- NUMQCACRALPSHD-UHFFFAOYSA-N tert-butyl ethyl ether Chemical compound CCOC(C)(C)C NUMQCACRALPSHD-UHFFFAOYSA-N 0.000 description 3
- 125000000999 tert-butyl group Chemical group [H]C([H])([H])C(*)(C([H])([H])[H])C([H])([H])[H] 0.000 description 3
- 238000012360 testing method Methods 0.000 description 3
- LDHQCZJRKDOVOX-UHFFFAOYSA-N trans-crotonic acid Natural products CC=CC(O)=O LDHQCZJRKDOVOX-UHFFFAOYSA-N 0.000 description 3
- OJOWICOBYCXEKR-APPZFPTMSA-N (1S,4R)-5-ethylidenebicyclo[2.2.1]hept-2-ene Chemical compound CC=C1C[C@@H]2C[C@@H]1C=C2 OJOWICOBYCXEKR-APPZFPTMSA-N 0.000 description 2
- RRKODOZNUZCUBN-CCAGOZQPSA-N (1z,3z)-cycloocta-1,3-diene Chemical compound C1CC\C=C/C=C\C1 RRKODOZNUZCUBN-CCAGOZQPSA-N 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 2
- HYBLFDUGSBOMPI-BQYQJAHWSA-N (4e)-octa-1,4-diene Chemical compound CCC\C=C\CC=C HYBLFDUGSBOMPI-BQYQJAHWSA-N 0.000 description 2
- RJUCIROUEDJQIB-GQCTYLIASA-N (6e)-octa-1,6-diene Chemical compound C\C=C\CCCC=C RJUCIROUEDJQIB-GQCTYLIASA-N 0.000 description 2
- YWWVWXASSLXJHU-AATRIKPKSA-N (9E)-tetradecenoic acid Chemical compound CCCC\C=C\CCCCCCCC(O)=O YWWVWXASSLXJHU-AATRIKPKSA-N 0.000 description 2
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Classifications
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- F—MECHANICAL ENGINEERING; LIGHTING; HEATING; WEAPONS; BLASTING
- F16—ENGINEERING ELEMENTS AND UNITS; GENERAL MEASURES FOR PRODUCING AND MAINTAINING EFFECTIVE FUNCTIONING OF MACHINES OR INSTALLATIONS; THERMAL INSULATION IN GENERAL
- F16L—PIPES; JOINTS OR FITTINGS FOR PIPES; SUPPORTS FOR PIPES, CABLES OR PROTECTIVE TUBING; MEANS FOR THERMAL INSULATION IN GENERAL
- F16L9/00—Rigid pipes
- F16L9/12—Rigid pipes of plastics with or without reinforcement
-
- B—PERFORMING OPERATIONS; TRANSPORTING
- B32—LAYERED PRODUCTS
- B32B—LAYERED PRODUCTS, i.e. PRODUCTS BUILT-UP OF STRATA OF FLAT OR NON-FLAT, e.g. CELLULAR OR HONEYCOMB, FORM
- B32B1/00—Layered products having a non-planar shape
- B32B1/08—Tubular products
-
- B—PERFORMING OPERATIONS; TRANSPORTING
- B32—LAYERED PRODUCTS
- B32B—LAYERED PRODUCTS, i.e. PRODUCTS BUILT-UP OF STRATA OF FLAT OR NON-FLAT, e.g. CELLULAR OR HONEYCOMB, FORM
- B32B27/00—Layered products comprising a layer of synthetic resin
- B32B27/06—Layered products comprising a layer of synthetic resin as the main or only constituent of a layer, which is next to another layer of the same or of a different material
- B32B27/08—Layered products comprising a layer of synthetic resin as the main or only constituent of a layer, which is next to another layer of the same or of a different material of synthetic resin
-
- B—PERFORMING OPERATIONS; TRANSPORTING
- B32—LAYERED PRODUCTS
- B32B—LAYERED PRODUCTS, i.e. PRODUCTS BUILT-UP OF STRATA OF FLAT OR NON-FLAT, e.g. CELLULAR OR HONEYCOMB, FORM
- B32B27/00—Layered products comprising a layer of synthetic resin
- B32B27/18—Layered products comprising a layer of synthetic resin characterised by the use of special additives
-
- B—PERFORMING OPERATIONS; TRANSPORTING
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Abstract
提供一种即便是改性聚烯烃的层厚的构成,其低温耐冲击性、高温时的破坏压强度也优异的层叠体。一种层叠体,其为包含(a)层和(b)层的两层以上的层叠体,前述(a)层包含脂肪族聚酰胺组合物(A),前述(b)层包含改性聚烯烃(B),前述改性聚烯烃(B)含有由基于碳原子数为2以上且10以下的α‑烯烃的单体衍生的单元、以及由具有官能团的不饱和化合物衍生的单元,所述具有官能团的不饱和化合物为选自由具有选自羧基、羟基、环氧基、氨基、酰胺基、酰亚胺基、腈基、硫醇基和异氰酸酯基中的至少1种基团的不饱和化合物、以及具有羧基的不饱和化合物的衍生物组成的组中的至少1种,前述改性聚烯烃(B)按照ASTM D2240而测得的邵氏硬度(D标尺)为30以上且61以下。
Description
技术领域
本发明涉及层叠体。
背景技术
在油压管、水压管等各种压力管、真空管和汽车所使用的燃料配管管路、制动器管、冷却液用软管、空调配管管路、SCR(柴油发动机尾气去除装置)管、控制电缆套筒等中使用大量的软管(hose)/管(tube)类。在这些软管/管中运输冷却液(醇和水)、制冷剂、油、尿素溶液等化学溶液。对于在汽车工业领域中使用的各种软管/管等而言,要求在高温下的高破坏压强度、长期维持的耐热性、耐化学药品性、水蒸气和/或化学溶液阻隔性、柔软性等极高的性能。
尤其,循环流体是用于防止冬季的冻结而以乙二醇作为主体的冷却液(LLC)、作为用于去除从柴油发动机释放的NOx的催化剂而封入的尿素溶液、空调/散热器等所使用的二氧化碳、氟利昂、氟利昂替代物、丙烷、水等制冷剂等时,若对这些化学溶液的阻隔性不充分,则在实际使用时无法充分地发挥冷却效果、催化作用效果。另外,随着臭氧层破坏气体的蒸散管控的加强,对于汽车等中使用的制冷剂运输用管的制冷剂阻隔性的要求变得严苛。
另一方面,随着臭氧层破坏气体的蒸散管控的加强,近年来汽车等中使用的制冷剂的品质也得以改良。例如,作为HFC-134a制冷剂的替代制冷剂而开发了R-1234yf制冷剂,其与HFC-134a制冷剂相比臭氧破坏系数和全球变暖潜能值低,是对于地球环境而言极其友善的制冷剂。然而,尤其是R-1234yf制冷剂在高温环境下因与水接触而容易发生水解并产生酸(甲酸等),主要由于该酸的因素,视与化学溶液接触的材料而异,容易发生水解、劣化,最差的情况下,存在产生裂纹、流体泄漏而无法实现流体运输目的这样的问题。或者,化学溶液、水有时也会透过管主体而对接触的部件造成不良影响。
以往使用的单独使用聚酰胺系树脂、尤其是强度、韧性、耐化学药品性、柔软性等优异的聚酰胺11或聚酰胺12得到的单层管对于前述化学溶液的长期耐久性和阻隔性不充分。
乙烯/四氟乙烯共聚物(ETFE)等氟系树脂可以认为是对各种化学溶液的耐性极其优异、且对水蒸气具有阻隔性能的材料部件之一。近年来,具有与聚酰胺的粘接性的氟系树脂的开发变得活跃(参照专利文献1~3)。然而,在环保方面避免使用含卤素材料的同时,存在比重高、成本高的问题,正在寻求开发出使用无卤素材料、对化学溶液的阻隔性优异且对各种化学溶液具有耐性的配管***。
另一方面,聚烯烃的价格低廉,抗化学溶液透过性、化学溶液长期耐性优异。例如,提出了一种由包含聚酰胺的外层、包含交联聚乙烯的内层构成的冷却用配管(参照专利文献4)。另外,提出了一种由包含聚酰胺的外层、具有一定以上的厚度且包含含有特定添加剂的聚丙烯的内层构成的冷却用配管(参照专利文献5)。同样地,提出了一种冷却用配管,其特征在于,其由对冷却剂为非活性且不能溶胀的内层、以及包含聚酰胺的外层形成,内层由卤代或非卤代的均聚聚烯烃或共聚烯烃构成,该冷却用配管通过挤出吹塑成形来制造,在导管的整个长度上,层的壁厚不同,且内层和外层的聚合物的挠性明显不同(参照专利文献6)。另外,提出了一种多层管,其从内侧朝向外侧包含聚烯烃的内层、以粘接剂为基础的第一中间层、乙烯/乙烯醇共聚物的第二中间层、聚酰胺的第三中间层和外侧的保护层(参照专利文献7)。进而,还提出了一种燃料电池用配管,其中,将以聚酰胺系树脂和苯乙烯-异丁烯嵌段共聚物为必需成分的外层用材料制成外层,并将以聚烯烃系树脂和苯乙烯-异丁烯嵌段共聚物为必需成分的内层用材料制成内层(参照专利文献8)。
现有技术文献
专利文献
专利文献1:国际公开第2001/058686号
专利文献2:国际公开第2001/060606号
专利文献3:日本特开2004-301247号公报
专利文献4:日本特开平9-29869号公报
专利文献5:日本特表2008-507436号公报
专利文献6:日本特开平7-214647号公报
专利文献7:日本特开2006-116966号公报
专利文献8:日本特开2005-216725号公报
发明内容
发明要解决的问题
寻求能够根据使用时的要求项目来变更聚酰胺层和聚烯烃层的厚度,且任意的层厚度均显示出高温和低温下的优异的机械特性。
然而,专利文献4所公开的配管在使用聚乙烯作为内层的情况下,高温下的长期耐性、管物性差。
另外,因聚烯烃层变厚而难以兼顾高温和低温下的机械强度,但专利文献5~8没有具体的技术数据、技术启示。
尤其,对于电动汽车等而言,寻求进一步提高对LLC的阻隔性、高温耐性,对于层叠体而言,寻求阻隔性、高温耐性优异,且增加廉价的聚烯烃的厚度,另一方面,要求兼顾能够耐受高温气氛下的LLC的内压的高耐压性和低温下的耐冲击性。
本发明的目的在于,解决前述问题点,提供即便是改性聚烯烃的层较厚的构成,其低温耐冲击性、高温时的破坏压强度也优异的层叠体。
用于解决问题的方案
本发明人等为了解决前述问题点而进行了深入研究,结果发现:具有包含脂肪族聚酰胺树脂组合物的层和包含具备特定机械物性、材料特性的改性聚烯烃的层的层叠体即便是前述改性聚烯烃变厚的构成,其低温耐冲击性、高温时的破坏压强度也优异。
即,本发明为一种层叠体,其为包含(a)层和(b)层的两层以上的层叠体,
前述(a)层包含脂肪族聚酰胺组合物(A),
前述(b)层包含改性聚烯烃(B),
前述改性聚烯烃(B)含有由基于碳原子数为2以上且10以下的α-烯烃的单体衍生的单元、以及由具有官能团的不饱和化合物衍生的单元,所述具有官能团的不饱和化合物为选自由具有选自羧基、羟基、环氧基、氨基、酰胺基、酰亚胺基、腈基、硫醇基和异氰酸酯基中的至少1种基团的不饱和化合物、以及具有羧基的不饱和化合物的衍生物组成的组中的至少1种,
前述改性聚烯烃(B)按照ASTM D2240而测得的邵氏硬度(D标尺)为30以上且61以下。
以下示出层叠体的优选方式。优选方式可以组合多种。
[1]一种层叠体,其中,前述脂肪族聚酰胺组合物(A)包含聚酰胺(A1),前述聚酰胺(A1)是亚甲基数量相对于酰胺基数量之比为7.0以上的脂肪族聚酰胺。
[2]一种层叠体,其中,前述聚酰胺(A1)为选自由聚酰胺11、聚酰胺12、聚酰胺610、聚酰胺612、聚酰胺1010、聚酰胺1012和聚酰胺1212组成的组中的至少1种的均聚物,和/或使用多种形成它们的原料单体而得的至少1种共聚物。
[3]一种层叠体,其中,前述脂肪族聚酰胺组合物(A)还包含选自由增塑剂、耐冲击剂和耐热剂组成的组中的1种以上的其它成分。
[4]一种层叠体,其中,前述(a)层与(b)层相互邻接。
[5]一种层叠体,其中,前述改性聚烯烃(B)按照ASTM D638而测得的拉伸屈服点应力为23MPa以下,按照ASTM D638而测得的拉伸断裂点应力为25MPa以上。
[6]一种层叠体,其中,前述改性聚烯烃(B)按照ASTM D1238而测得的MFR(230℃、2160g)为3.5g/10min以上。
[7]一种层叠体,其中,前述改性聚烯烃(B)在FT-IR测定中,波数处于710cm-1以上且740cm-1以下的吸收之中显示最大强度的波数为721cm-1cm以上。
[8]一种层叠体,其中,前述改性聚烯烃(B)通过下述方法来制造:使改性前的聚烯烃熔融,添加前述具有官能团的不饱和化合物而进行接枝共聚化。
[9]一种层叠体,其中,前述改性聚烯烃(B)为马来酸酐改性聚丙烯。
[10]一种层叠体,其仅由前述(a)层和(b)层组成。
[11]一种层叠体,其通过共挤出成形法来制造。
[12]一种层叠体,其为层叠中空成形体。
[13]一种层叠中空成形体,其从外侧起按照前述(a)层、(b)层的顺序配置。
[14]一种层叠中空成形体,其中,前述(b)层配置于最内层。
[15]一种层叠中空成形体,其在最内层还包含其它层。
[16]一种层叠中空成形体,其为管。
发明的效果
根据本发明,可提供即便是改性聚烯烃的层较厚的构成,其低温耐冲击性、高温时的破坏压强度也优异的层叠体。
具体实施方式
层叠体为包含(a)层和(b)层的两层以上,
前述(a)层包含脂肪族聚酰胺组合物(A),
前述(b)层包含改性聚烯烃(B),前述改性聚烯烃(B)含有由基于碳原子数为2以上且10以下的α-烯烃的单体衍生的单元、以及由不饱和化合物衍生的单元,所述不饱和化合物为选自由具有选自羧基、羟基、环氧基、氨基、酰胺基、酰亚胺基、腈基、硫醇基和异氰酸酯基中的至少1种基团的不饱和化合物、以及具有羧基的不饱和化合物的衍生物组成的组中的至少1种,
前述改性聚烯烃(B)按照ASTM D2240而测得的邵氏硬度(D标尺)が30以上且61以下。
层叠体即便为改性聚烯烃的层较薄的构成时,其低温耐冲击性和高温时的破坏压强度也优异。
1.(a)层
层叠体的(a)层包含脂肪族聚酰胺组合物(A)。
<脂肪族聚酰胺组合物(A)>
脂肪族聚酰胺组合物(A)只要是包含在主链中具有酰胺键(-CONH-)的脂肪族聚酰胺的组合物,就没有特别限定。作为脂肪族聚酰胺,可列举出聚酰胺6(聚己酰胺)、聚酰胺11(聚十一酰胺)、聚酰胺12(聚十二酰胺)、聚酰胺26(聚己二酰乙二胺)、聚酰胺44(聚丁二酰丁二胺)、聚酰胺45(聚戊二酰丁二胺)、聚酰胺46(聚己二酰丁二胺)、聚酰胺48(聚辛二酰丁二胺)、聚酰胺49(聚壬二酰丁二胺)、聚酰胺410(聚癸二酰丁二胺)、聚酰胺412(聚十二烷二酰丁二胺)、聚酰胺54(聚丁二酰戊二胺)、聚酰胺55(聚戊二酰戊二胺)、聚酰胺56(聚己二酰戊二胺)、聚酰胺58(聚己二酰戊二胺)、聚壬二酰戊二胺(聚酰胺59)、聚癸二酰戊二胺(聚酰胺510)、聚十二烷二酰戊二胺(聚酰胺512)、聚丁二酰己二胺(聚酰胺64)、聚戊二酰己二胺(聚酰胺65)、聚己二酰己二胺(聚酰胺66)、聚辛二酰己二胺(聚酰胺68)、聚壬二酰己二胺(聚酰胺69)、聚癸二酰己二胺(聚酰胺610)、聚十二烷二酰己二胺(聚酰胺612)、聚十四烷二酰己二胺(聚酰胺614)、聚十六烷二酰己二胺(聚酰胺616)、聚十八烷二酰己二胺(聚酰胺618)、聚己二酰壬二胺(聚酰胺96)、聚辛二酰壬二胺(聚酰胺98)、聚壬二酰壬二胺(聚酰胺99)、聚癸二酰壬二胺(聚酰胺910)、聚十二烷二酰壬二胺(聚酰胺912)、聚己二酰癸二胺(聚酰胺106)、聚辛二酰癸二胺(聚酰胺108)、聚壬二酰癸二胺(聚酰胺109)、聚癸二酰癸二胺(聚酰胺1010)、聚十二烷二酰癸二胺(聚酰胺1012)、聚己二酰十二烷二胺(聚酰胺126)、聚辛二酰十二烷二胺(聚酰胺128)、聚壬二酰十二烷二胺(聚酰胺129)、聚癸二酰十二烷二胺(聚酰胺1210)、聚十二烷二酰十二烷二胺(聚酰胺1212)等均聚物、使用多种形成它们的原料单体而得的共聚物等。
脂肪族聚酰胺组合物(A)优选包含聚酰胺(A1)。
[聚酰胺(A1)]
聚酰胺(A1)是亚甲基数量相对于酰胺基数量之比(以下有时称为[CH2]/[NHCO])为7.0以上的脂肪族聚酰胺(以下有时称为聚酰胺(A1))。通过使用[CH2]/[NHCO]为7.0以上的脂肪族聚酰胺,能够使层叠体的机械特性等各物性优异。[CH2]/[NHCO]的上限值没有特别限定,实用上为11.0以下。
作为聚酰胺(A1),例如可列举出聚酰胺11([CH2]/[NHCO]=10.0)、聚酰胺12([CH2]/[NHCO]=11.0)、聚酰胺412([CH2]/[NHCO]=7.0)、聚酰胺512([CH2]/[NHCO]=7.5)、聚酰胺610([CH2]/[NHCO]=7.0)、聚酰胺612([CH2]/[NHCO]=8.0)、聚酰胺614([CH2]/[NHCO]=9.0)、聚酰胺616([CH2]/[NHCO]=10.0)、聚酰胺618([CH2]/[NHCO]=11.0)、聚酰胺98([CH2]/[NHCO]=7.5)、聚酰胺99([CH2]/[NHCO]=8.0)、聚酰胺910([CH2]/[NHCO]=8.5)、聚酰胺912([CH2]/[NHCO]=9.5)、聚酰胺106([CH2]/[NHCO]=7.0)、聚酰胺108([CH2]/[NHCO]=8.0)、聚酰胺109([CH2]/[NHCO]=8.5)、聚酰胺1010([CH2]/[NHCO]=9.0)、聚酰胺1012([CH2]/[NHCO]=10.0)、聚酰胺126([CH2]/[NHCO]=8.0)、聚酰胺128([CH2]/[NHCO]=9.0)、聚酰胺129([CH2]/[NHCO]=9.5)、聚酰胺1210([CH2]/[NHCO]=10.0)、聚酰胺1212([CH2]/[NHCO]=11.0)等均聚物、和/或使用多种形成它们的原料单体而得的共聚物等。
作为聚酰胺(A1),从能够充分确保层叠体的机械特性、耐热性等各物性的观点、经济性、获取容易度的观点等出发,优选使用选自由聚酰胺11、聚酰胺12、聚酰胺610、聚酰胺612、聚酰胺1010、聚酰胺1012和聚酰胺1212组成的组中的至少1种均聚物、和/或使用多种形成它们的原料单体而得的至少1种共聚物。
[聚酰胺(A1)的特性]
从确保层叠体的机械性质、以及使熔融时的粘度为适当范围而确保层叠体的期望成形性的观点出发,按照JIS K-6920,在96%硫酸、聚合物浓度为1%、25℃的条件下测得的聚酰胺(A1)的相对粘度优选为1.5以上且5.0以下、更优选为2.0以上且4.5以下。
将每1g聚酰胺(A1)的末端氨基浓度记作[A](μeq/g),且将末端羧基浓度记作[B](μeq/g)时,从充分确保层叠体的层间粘接性的观点出发,优选为[A]>[B]+5、更优选为[A]>[B]+10、特别优选为[A]>[B]+15。进而,从聚酰胺的熔融稳定性、抑制凝胶状物产生的观点出发,优选为[A]>20、特别优选为30<[A]<120。
此处,末端氨基浓度[A](μeq/g)可通过将聚酰胺溶解于苯酚/甲醇混合溶液,并利用0.05N的盐酸进行滴定来测定。末端羧基浓度[B](μeq/g)可通过将该聚酰胺溶解于苄醇,并利用0.05N的氢氧化钠溶液进行滴定来测定。
聚酰胺(A1)只要满足上述末端基团浓度,则还优选为包含末端氨基浓度和/或末端羧基浓度不同的两种以上脂肪族聚酰胺的脂肪族聚酰胺混合物。此时,脂肪族聚酰胺混合物的末端氨基浓度和/或末端羧基浓度根据构成混合物的脂肪族聚酰胺的末端氨基浓度、末端羧基浓度及其配混比例来确定。
[聚酰胺(A1)的制造方法]
聚酰胺(A1)通过在胺类的存在下利用熔融聚合、溶液聚合、固相聚合或它们的组合等公知方法将聚酰胺原料进行聚合或共聚来制造。或者,聚酰胺(A1)通过将聚酰胺原料聚合后在胺类的存在下进行熔融混炼来制造。此处,聚酰胺原料的聚合可反复进行常压、减压、加压操作。
作为聚酰胺(A1)的原料,可列举出脂肪族内酰胺、脂肪族氨基羧酸、或者脂肪族二胺与脂肪族二羧酸的组合。
作为脂肪族内酰胺,可列举出己内酰胺、庚内酰胺、十一内酰胺、十二内酰胺、α-吡咯烷酮、α-哌啶酮等。它们可以使用1种或2种以上。
作为脂肪族氨基羧酸,可列举出6-氨基己酸、7-氨基庚酸、9-氨基壬酸、11-氨基十一烷酸、12-氨基十二烷酸等。它们可以使用1种或2种以上。
作为脂肪族二胺,可列举出1,4-丁二胺、1,5-戊二胺、1,6-己二胺、1,7-庚二胺、1,8-辛二胺、1,9-壬二胺、1,10-癸二胺、1,11-十一烷二胺、1,12-十二烷二胺、1,13-十三烷二胺、1,14-十四烷二胺、1,15-十五烷二胺、1,16-十六烷二胺、1,17-十七烷二胺、1,18-十八烷二胺、1,19-十九烷二胺、1,20-二十烷二胺、2-甲基-1,5-戊二胺、3-甲基-1,5-戊二胺、2-甲基-1,8-辛二胺、2,2,4-三甲基-1,6-己二胺、2,4,4-三甲基-1,6-己二胺、5-甲基-1,9-壬二胺等。它们可以使用1种或2种以上。
作为脂肪族二羧酸,可列举出戊二酸、己二酸、庚二酸、辛二酸、壬二酸、癸二酸、十一烷二酸、十二烷二酸、十三烷二酸、十四烷二酸、十五烷二酸、十六烷二酸、十八烷二酸、二十烷二酸等。它们可以使用1种或2种以上。
作为胺类,可列举出单胺、二胺、三胺和多胺。它们可以使用1种或2种以上。其中,聚酰胺(A1)的原料为脂肪族二胺与脂肪族二羧酸的组合时,胺类不包括脂肪族二胺。
作为单胺,可列举出甲胺、乙胺、丙胺、丁胺、戊胺、己胺、庚胺、辛胺、2-乙基己胺、壬胺、癸胺、十一烷基胺、十二烷基胺、十三烷基胺、十四烷基胺、十五烷基胺、十六烷基胺、十八烷基胺、十八烯基胺、二十烷基胺、二十二烷基胺等脂肪族单胺;环己胺、甲基环己胺等脂环式单胺;苄胺、β-苯基甲胺等芳香族单胺;N,N-二甲胺、N,N-二乙胺、N,N-二丙胺、N,N-二丁胺、N,N-二己胺、N,N-二辛胺等对称仲胺;N-甲基-N-乙胺、N-甲基-N-丁胺、N-甲基-N-十二烷基胺、N-甲基-N-十八烷基胺、N-乙基-N-十六烷基胺、N-乙基-N-十八烷基胺、N-丙基-N-十六烷基胺、N-丙基-N-苄胺等混合仲胺。它们可以使用1种或2种以上。
作为二胺,可列举出1,2-乙二胺、1,3-丙二胺、1,4-丁二胺、1,5-戊二胺、1,6-己二胺、1,7-庚二胺、1,8-辛二胺、1,9-壬二胺、1,10-癸二胺、1,11-十一烷二胺、1,12-十二烷二胺、1,13-十三烷二胺、1,14-十四烷二胺、1,15-十五烷二胺、1,16-十六烷二胺、1,17-十七烷二胺、1,18-十八烷二胺、2-甲基-1,5-戊二胺、3-甲基-1,5-戊二胺、2-甲基-1,8-辛二胺、2,2,4-三甲基-1,6-己二胺、2,4,4-三甲基-1,6-己二胺、5-甲基-1,9-壬二胺等脂肪族二胺;1,3-双(氨基甲基)环己烷、1,4-双(氨基甲基)环己烷、双(4-氨基环己基)甲烷、2,2-双(4-氨基环己基)丙烷、双(3-甲基-4-氨基环己基)甲烷、2,2-双(3-甲基-4-氨基环己基)丙烷、5-氨基-2,2,4-三甲基-1-环戊烷甲胺、5-氨基-1,3,3-三甲基环己烷甲胺、双(氨基丙基)哌嗪、双(氨基乙基)哌嗪、2,5-双(氨基甲基)降冰片烷、2,6-双(氨基甲基)降冰片烷、3,8-双(氨基甲基)三环癸烷、4,9-双(氨基甲基)三环癸烷等脂环式二胺;间苯二甲胺、对苯二甲胺等芳香族二胺。它们可以使用1种或2种以上。
胺类可以在聚酰胺原料的聚合时的任意阶段中添加,或者,在聚酰胺原料的聚合后在熔融混炼时的任意阶段中添加,考虑到层叠体的层间粘接性时,优选在聚合时的阶段进行添加。另外,关于胺类,为了满足上述末端氨基浓度的条件,优选在聚酰胺原料的聚合时添加二胺和/或多胺,从抑制凝胶产生的观点出发,特别优选在聚酰胺原料的聚合时添加选自由脂肪族二胺、脂环式二胺和聚亚烷基亚胺组成的组中的至少1种。
进而,在满足上述末端基团浓度的范围内,可根据需要而添加单羧酸、二羧酸、三羧酸等羧酸类。此时,胺类、羧酸类可以同时添加,也可以分别添加。
作为羧酸类,可列举出乙酸、丙酸、丁酸、戊酸、己酸、庚酸、辛酸、癸酸、壬酸、十一烷酸、月桂酸、十三烷酸、肉豆蔻酸、肉豆寇烯酸、棕榈酸、硬脂酸、油酸、亚油酸、花生酸、山嵛酸、芥酸等脂肪族单羧酸;环己烷羧酸、甲基环己烷羧酸等脂环式单羧酸;苯甲酸、甲苯甲酸、乙基苯甲酸、苯基乙酸等芳香族单羧酸;丙二酸、琥珀酸、戊二酸、己二酸、庚二酸、辛二酸、壬二酸、癸二酸、十一烷二酸、十二烷二酸、十六烷二酸、十六碳烯二酸、十八烷二酸、十八碳烯二酸、二十烷二酸、二十碳烯二酸、二十二烷二酸、二甘醇酸、2,2,4-三甲基己二酸、2,4,4-三甲基己二酸等脂肪族二羧酸;1,3-环己烷二羧酸、1,4-环己烷二羧酸、降冰片烷二羧酸等脂环式二羧酸;对苯二甲酸、间苯二甲酸、邻苯二甲酸、间苯二亚甲基二羧酸、对苯二亚甲基二羧酸、1,4-萘二甲酸、2,6-萘二甲酸、2,7-萘二甲酸等芳香族二羧酸;1,2,4-丁烷三羧酸、1,3,5-戊烷三羧酸、1,2,6-己烷三羧酸、1,3,6-己烷三羧酸、1,3,5-环己烷三羧酸、均苯三酸等三羧酸。它们可以使用1种或2种以上。
胺类的用量考虑聚酰胺(A1)的末端氨基浓度、末端羧基浓度和相对粘度,通过公知的方法来适当决定。通常,从获得充分的反应性、容易制造具有期望粘度的聚酰胺的观点出发,相对于聚酰胺原料1摩尔(构成重复单元的单体或单体单元1摩尔),胺类的添加量优选为0.5meq/摩尔以上且20meq/摩尔以下、更优选为1.0meq/摩尔以上且10meq/摩尔以下。此处,关于氨基的当量(eq),将与羧基以1:1发生反应而形成酰胺基的氨基量作为1当量。
作为聚酰胺(A1)的制造装置,可列举出间歇式反应釜、单槽式~多槽式的连续反应装置、管状连续反应装置、单螺杆型混炼挤出机、双螺杆型混炼挤出机等混炼反应挤出机等公知的聚酰胺制造装置。
[其它成分]
脂肪族聚酰胺组合物(A)可根据需要而包含其它成分。作为这种其它成分,可列举出除聚酰胺(A1)之外的聚酰胺、例如[CH2]/[NHCO]小于7.0的脂肪族聚酰胺、在主链或侧链具有脂环族或芳香族基团的聚酰胺树脂等;耐冲击剂、增塑剂、选自抗氧化剂和热稳定剂的耐热剂;紫外线吸收剂、光稳定剂、润滑剂、无机填充剂、抗静电剂、阻燃剂、结晶促进剂、着色剂等。作为其它成分,优选包含选自由增塑剂、耐冲击剂和耐热剂组成的组中的1种以上。它们可以使用1种或2种以上。
[耐冲击剂]
从对层叠体赋予耐冲击性的观点出发,脂肪族聚酰胺组合物(A)优选包含耐冲击剂。需要说明的是,耐冲击剂不是改性聚烯烃(B)。即,耐冲击剂按照ASTM D2240而测得的邵氏硬度(D标尺)小于30,优选小于20。耐冲击剂按照ASTM D2240而测得的邵氏硬度(D标尺)的下限没有特别限定,可以设为0.5以上。作为耐冲击剂,可列举出:包含由具有羧基和/或酸酐基的不饱和化合物衍生的结构单元,且按照ASTM D2240而测得的邵氏硬度(D标尺)小于30的弹性体聚合物。
作为弹性体聚合物,可列举出(乙烯和/或丙烯)/α-烯烃系共聚物、(乙烯和/或丙烯)/(α,β-不饱和羧酸酯)系共聚物等,它们可以使用1种或2种以上。
前述(乙烯和/或丙烯)/α-烯烃系共聚物是将乙烯和/或丙烯与碳原子数为3以上的α-烯烃共聚得到的聚合物,作为碳原子数为3以上的α-烯烃,可列举出丙烯、1-丁烯、1-戊烯、1-己烯、1-庚烯、1-辛烯、1-壬烯、1-癸烯、1-十一碳烯、1-十二碳烯、1-十三碳烯、1-十四碳烯、1-十五碳烯、1-十六碳烯、1-十七碳烯、1-十八碳烯、1-十九碳烯、1-二十碳烯、3-甲基-1-丁烯、3-甲基-1-戊烯、3-乙基-1-戊烯、4-甲基-1-戊烯、4-甲基-1-己烯、4,4-二甲基-1-己烯、4,4-二甲基-1-戊烯、4-乙基-1-己烯、3-乙基-1-己烯、9-甲基-1-癸烯、11-甲基-1-十二碳烯、12-乙基-1-十四碳烯等。它们可以使用1种或2种以上。另外,可以共聚有1,3-丁二烯等共轭二烯;1,4-戊二烯、1,4-己二烯、1,5-己二烯、1,4-辛二烯、1,5-辛二烯、1,6-辛二烯、1,7-辛二烯、2-甲基-1,5-己二烯、6-甲基-1,5-庚二烯、7-甲基-1,6-辛二烯、4-乙叉基-8-甲基-1,7-壬二烯、4,8-二甲基-1,4,8-癸三烯(DMDT)、二环戊二烯、环己二烯、环辛二烯、5-乙烯基降冰片烯、5-乙叉基-2-降冰片烯、5-亚甲基-2-降冰片烯、5-异丙叉基-2-降冰片烯、6-氯甲基-5-异丙烯基-2-降冰片烯、2,3-二异丙叉基-5-降冰片烯、2-乙叉基-3-异丙叉基-5-降冰片烯、2-丙烯基-2,5-降冰片二烯等非共轭二烯的多烯。它们可以使用1种或2种以上。
前述(乙烯和/或丙烯)/(α,β-不饱和羧酸酯)系共聚物是将乙烯和/或丙烯与α,β-不饱和羧酸酯单体进行共聚而得的聚合物,作为α,β-不饱和羧酸酯单体,可列举出丙烯酸甲酯、甲基丙烯酸甲酯、丙烯酸乙酯、甲基丙烯酸乙酯、丙烯酸丙酯、甲基丙烯酸丙酯、丙烯酸丁酯、甲基丙烯酸丁酯、丙烯酸戊酯、甲基丙烯酸戊酯、丙烯酸己酯、甲基丙烯酸己酯、丙烯酸庚酯、甲基丙烯酸庚酯、丙烯酸辛酯、甲基丙烯酸辛酯、丙烯酸壬酯、甲基丙烯酸壬酯、丙烯酸癸酯、甲基丙烯酸癸酯、丙烯酸2-乙基己酯、甲基丙烯酸2-乙基己酯、丙烯酸羟基乙酯、甲基丙烯酸羟基乙酯、马来酸单甲酯、衣康酸单甲酯、马来酸二甲酯、衣康酸二甲酯等。它们可以使用1种或2种以上。
作为弹性体聚合物中的具有羧基的不饱和化合物,可列举出丙烯酸、甲基丙烯酸、马来酸、富马酸、衣康酸、巴豆酸、中康酸、柠康酸、戊烯二酸、顺式-4-环己烯-1,2-二羧酸、内双环-[2.2.1]-5-庚烯-2,3-二羧酸、以及这些羧酸的金属盐等α,β-不饱和羧酸。作为具有酸酐基的不饱和化合物,可列举出马来酸酐、衣康酸酐、柠康酸酐、内双环-[2.2.1]-5-庚烯-2,3-二羧酸酐等具有α,β-不饱和键的二羧酸酐。它们可以使用1种或2种以上。这些之中,优选为具有α,β-不饱和键的二羧酸酐,更优选为马来酸酐、衣康酸酐。
从表现出与前述聚酰胺(A1)的良好相容性、以及脂肪族聚酰胺组合物(A)的流动性的观点出发,弹性体聚合物中的羧基和/或酸酐基浓度优选为25μeq/g以上且200μeq/g以下、更优选为50μeq/g以上且150μeq/g以下。
另外,弹性体聚合物中的羧基和/或酸酐基浓度可使用将该弹性体聚合物溶解于甲苯溶液,进而添加乙醇而制备的试样溶液,并以酚酞作为指示剂,利用0.1N的KOH乙醇溶液进行滴定来测定。
[增塑剂]
从对层叠体赋予柔软性的观点出发,脂肪族聚酰胺组合物(A)优选包含增塑剂。作为增塑剂,可列举出N-丁基苯磺酰胺、对羟基苯甲酸-2-己基癸酯等。它们可以使用1种或2种以上。
[耐热剂]
脂肪族聚酰胺组合物(A)优选包含选自抗氧化剂和热稳定剂中的耐热剂。作为抗氧化剂,可列举出酚系化合物等。热稳定剂也被称为加工稳定剂,例如可列举出硫醚系、磷系和卤化金属系的化合物,优选为磷系化合物。抗氧化剂和热稳定剂可以使用1种或2种以上。
[脂肪族聚酰胺组合物(A)的特性]
脂肪族聚酰胺组合物(A)按照ISO 178而测得的弯曲弹性模量优选为400MPa以上且1000MPa以下、更优选为450MPa以上且950MPa以下、特别优选为500MPa以上且900MPa以下。通过使脂肪族聚酰胺组合物(A)的弯曲弹性模量处于前述范围内,从而能够维持层叠体在高温时的破坏压强度,且使层叠体的柔软性优异。脂肪族聚酰胺组合物(A)的弯曲弹性模量可通过适当变更耐冲击剂、增塑剂的添加量来调整。
[脂肪族聚酰胺组合物(A)的组成]
脂肪族聚酰胺组合物(A)中的聚酰胺(A1)的含量相对于脂肪族聚酰胺组合物(A)100质量%优选为55质量%以上且95质量%以下、更优选为60质量%以上且95质量%以下、特别优选为70质量%以上且89质量%以下。通过使脂肪族聚酰胺组合物(A)中的聚酰胺(A1)的含量处于前述范围内,从而能够使层叠体在高温时的破坏压强度等特性充分优异。另外,若聚酰胺(A1)的含量为前述下限值以上,则能够充分获得层叠体在高温时的破坏压强度。若聚酰胺(A1)的含量为前述上限值以下,则能够充分获得层叠体的柔软性、低温冲击性。
脂肪族聚酰胺组合物(A)中的耐冲击剂的含量相对于脂肪族聚酰胺组合物(A)100质量%优选为5质量%以上且30质量%以下、更优选为7质量%以上且25质量%以下、特别优选为10质量%以上且20质量%以下。通过使脂肪族聚酰胺组合物(A)中的耐冲击剂的含量处于前述范围内,从而能够维持层叠体的机械特性,且使柔软性、低温耐冲击性更优异。另外,若耐冲击剂的含量为前述下限值以上,则能够充分获得层叠体的柔软性、低温耐冲击性。若耐冲击剂的含量为前述上限值以下,则能够充分获得层叠体在高温时的破坏压强度、其它机械特性。
脂肪族聚酰胺组合物(A)中的增塑剂的含量相对于脂肪族聚酰胺组合物(A)100质量%优选为0质量%以上且15质量%以下、特别优选为1质量%以上且10质量%以下。通过使增塑剂的含量处于前述范围内,从而能够维持层叠体在高温时的破坏压强度,且使层叠体的柔软性优异。另外,若增塑剂的含量为前述上限值以下,则能够充分获得层叠体在高温时的破坏压强度。
脂肪族聚酰胺组合物(A)中的耐热剂的含量相对于脂肪族聚酰胺组合物(A)100质量%优选为0质量%以上且5质量%以下、特别优选为0.5质量%以上且2质量%以下。若耐热剂的含量处于前述范围内,则能够取得层叠体的机械特性、耐热性等的平衡。
脂肪族聚酰胺组合物(A)中的除耐冲击剂、增塑剂和耐热剂之外的其它成分的含量可根据所要求的特性来适当设定。
[脂肪族聚酰胺组合物(A)的制造方法]
脂肪族聚酰胺组合物(A)的制造方法没有特别限定,可以采用以往公知的各种方法。例如,可以通过下述方法等来制造:使用转鼓、混合器,将聚酰胺(A1)、耐冲击剂、增塑剂和耐热剂与根据需要而添加的其它成分一同,以成为前述混合比例的方式将粒料彼此均匀地干混的方法;将聚酰胺(A1)、耐冲击剂、增塑剂和耐热剂与根据需要而添加的其它成分一同预先干混,并进行熔融混炼的方法;将聚酰胺(A1)、耐冲击剂、增塑剂和耐热剂与根据需要而添加的其它成分一同预先干混,分别将它们各自给料并进行熔融混炼的方法等。熔融混炼可使用单螺杆挤出机、双螺杆挤出机、捏合机、班伯里密炼机等混炼机来进行。
2.(b)层
层叠体的(b)层包含改性聚烯烃(B)。
<改性聚烯烃(B)>
改性聚烯烃(B)是下述聚合物(以下有时称为改性聚烯烃(B)),其含有由基于碳原子数为2以上且10以下的α-烯烃的单体衍生的单元、以及由具有官能团的不饱和化合物衍生的单元,所述具有官能团的不饱和化合物为选自由具有选自羧基、羟基、环氧基、氨基、酰胺基、酰亚胺基、腈基、硫醇基和异氰酸酯基组成的组中的至少1种基团的不饱和化合物、以及具有羧基的不饱和化合物的衍生物组成的组中的至少1种,且所述聚合物按照ASTMD2240而测得的邵氏硬度(D标尺)为30以上且61以下。
[基于碳原子数为2以上且10以下的α-烯烃的单体]
构成改性聚烯烃(B)的聚烯烃(B1)含有由基于碳原子数为2以上且10以下的α-烯烃的单体衍生的单元。
作为基于碳原子数为2以上且10以下的α-烯烃的单体,可列举出乙烯、丙烯、1-丁烯、1-戊烯、1-己烯、1-庚烯、1-辛烯、1-壬烯、1-癸烯、3-甲基-1-丁烯、3-甲基-1-戊烯、3-乙基-1-戊烯、4-甲基-1-戊烯、4,4-二甲基-1-戊烯、4-甲基-1-己烯、4,4-二甲基-1-己烯、4,4-二甲基-1-戊烯、4-乙基-1-己烯、3-乙基-1-己烯等。它们可以使用1种或2种以上。这些之中,从能够使层叠体的机械物性、柔软性特别优异的观点出发,优选基于碳原子数为2以上且8以下的α-烯烃的单体。
[其它单体]
只要在不损害层叠体的优异的各特性的范围内,聚烯烃(B1)就可以包含除基于碳原子数为2以上且10以下的α-烯烃的单体和具有官能团的不饱和化合物之外的、例如苯乙烯类、1,3-丁二烯等共轭二烯类、非共轭二烯类、环状烯烃类、含氧原子的烯烃类等其它单体。作为苯乙烯类,可列举出苯乙烯、邻甲基苯乙烯、间甲基苯乙烯、对甲基苯乙烯、1,5-二甲基苯乙烯、2,4-二甲基苯乙烯、乙烯基萘、乙烯基蒽、4-丙基苯乙烯、4-环己基苯乙烯、4-十二烷基苯乙烯、2-乙基-4-苄基苯乙烯、4-(苯基丁基)苯乙烯等。作为非共轭二烯类,可列举出1,4-戊二烯、1,4-己二烯、1,5-己二烯、1,4-辛二烯、1,5-辛二烯、1,6-辛二烯、1,7-辛二烯、2-甲基-1,5-己二烯、6-甲基-1,5-庚二烯、7-甲基-1,6-辛二烯、4-乙叉基-8-甲基-1,7-壬二烯、4,8-二甲基-1,4,8-癸三烯(DMDT)等。作为环状烯烃类,可列举出二环戊二烯、环己二烯、环辛二烯、5-乙烯基降冰片烯、5-乙叉基-2-降冰片烯、5-亚甲基-2-降冰片烯、5-异丙叉基-2-降冰片烯、6-氯甲基-5-异丙烯基-2-降冰片烯、2,3-二异丙叉基-5-降冰片烯、2-乙叉基-3-异丙叉基-5-降冰片烯、2-丙烯基-2,5-降冰片二烯等。作为含氧原子的烯烃类,可列举出己烯醇、己烯酸、辛烯酸甲酯等。
作为聚烯烃(B1),优选为聚乙烯、聚丙烯、聚丁烯-1、聚(4-甲基戊烯-1);乙烯、丙烯、1-丁烯、或者4-甲基戊烯-1与其它单体的α-烯烃共聚物等结晶性聚烯烃。它们可以使用1种或2种以上。
[聚烯烃(B1)的组成]
聚烯烃(B1)中,由基于碳原子数为2以上且10以下的α-聚烯烃的单体衍生的单元的含量相对于聚烯烃(B1)的全部聚合单元100摩尔%优选为60摩尔%以上、更优选为70摩尔%以上、特别优选为90摩尔%以上。通过使由基于碳原子数为2以上且10以下的α-聚烯烃的单体衍生的单元的含量为前述值以上,从而使层叠体的机械物性、柔软性更优异。另外,在聚烯烃(B1)中,由其它单体衍生的单元的含量相对于聚烯烃(B1)的全部聚合单元100摩尔%优选小于40摩尔%、更优选小于30摩尔%、特别优选小于10摩尔%。
因而,作为聚烯烃(B1),更优选为聚丙烯均聚物、丙烯与20摩尔%以下的其它α-烯烃的无规共聚物、丙烯与30摩尔%以下的其它α-烯烃的嵌段共聚物。
[聚烯烃(B1)的制造方法]
聚烯烃(B1)的制造也可通过以往公知的任意方法来进行,可以使用例如钛系催化剂、钒系催化剂、茂金属催化剂等来进行聚合。另外,聚烯烃(B1)可以是树脂和弹性体中的任意形态,全同立构结构、间同立构结构这两者均可使用,针对立构规整性没有特别限定。在聚烯烃(B1)为共聚物的情况下,可以为交替共聚、无规共聚、嵌段共聚中的任一者。
[具有官能团的不饱和化合物]
改性聚烯烃(B)含有由具有官能团的不饱和化合物衍生的单元,所述具有官能团的不饱和化合物为选自由具有选自羧基、羟基、环氧基、氨基、酰胺基、酰亚胺基、腈基、硫醇基和异氰酸酯基中的至少1种基团的不饱和化合物、以及具有羧基的不饱和化合物的衍生物组成的组中的至少1种。改性聚烯烃(B)通过包含由具有官能团的不饱和化合物(即,具有选自由特定基团组成的组中的至少1种基团的不饱和化合物和/或具有羧基的不饱和化合物的衍生物)衍生的单元,从而能够使(a)层与(b)层的层间粘接性高,能够使层叠体的耐久性高。
作为具有羧基的不饱和化合物,例如可列举出丙烯酸、甲基丙烯酸、马来酸、富马酸、四氢邻苯二甲酸、衣康酸、柠康酸、巴豆酸、异巴豆酸、降冰片烯二羧酸、双环[2,2,1]庚-2-烯-5,6-二羧酸、内双环-[2.2.1]-5-庚烯-2,3-二羧酸等不饱和羧酸。它们可以使用1种或2种以上。
具有羧基的不饱和化合物的衍生物例如可列举出前述具有羧基的不饱和化合物的酸酐、酰卤、酰胺、酰亚胺和/或酯。作为具有羧基的不饱和化合物的衍生物,例如可列举出马来酰氯、马来酰亚胺、马来酸酐、衣康酸酐、柠康酸酐、四氢邻苯二甲酸酐、双环[2,2,1]庚-2-烯-5,6-二羧酸酐、内双环-[2.2.1]-5-庚烯-2,3-二羧酸酐、马来酸二甲酯、马来酸单甲酯、马来酸二乙酯、富马酸二乙酯、衣康酸二甲酯、柠康酸二乙酯、四氢邻苯二甲酸二甲酯、双环[2,2,1]庚-2-烯-5,6-二羧酸二甲酯等。它们可以使用1种或2种以上。
作为具有羟基的不饱和化合物,例如可列举出丙烯酸羟基乙酯、甲基丙烯酸羟基乙酯、丙烯酸羟基丙酯、甲基丙烯酸羟基丙酯、甘油单(甲基)丙烯酸酯、季戊四醇单(甲基)丙烯酸酯等含有羟基的(甲基)丙烯酸酯;10-十一碳烯-1-醇、1-辛烯-3-醇、甘油单烯丙醚、烯丙醇、2-丁烯-1,4-二醇等。它们可以使用1种或2种以上。
作为具有环氧基的不饱和化合物,例如可列举出丙烯酸缩水甘油酯、甲基丙烯酸缩水甘油酯等不饱和羧酸的缩水甘油酯;或者马来酸、富马酸等不饱和二羧酸的单缩水甘油酯(单缩水甘油酯情况下的烷基的碳原子数为1以上且12以下)、对苯乙烯羧酸的烷基缩水甘油酯、2-甲基烯丙基缩水甘油醚、3,4-环氧-1-丁烯、3,4-环氧-3-甲基-1-丁烯、3,4-环氧-1-戊烯、3,4-环氧-3-甲基-1-戊烯、5,6-环氧-1-己烯、乙烯基环己烯单氧化物等。它们可以使用1种或2种以上。
作为具有氨基的不饱和化合物,例如可列举出丙烯酸氨基甲酯、甲基丙烯酸氨基甲酯、甲基丙烯酸二甲基氨基乙酯、丙烯酸氨基丙酯、甲基丙烯酸氨基丙酯、甲基丙烯酸环己基氨基乙酯等丙烯酸或甲基丙烯酸的氨基烷基酯系衍生物类;N-乙烯基二乙胺、N-乙酰基乙烯基胺等乙烯基胺系衍生物类。它们可以使用1种或2种以上。
作为具有酰胺基的不饱和化合物,例如可列举出丙烯酰胺、甲基丙烯酰胺、N-甲基丙烯酰胺、N,N-二甲基丙烯酰胺、N,N-二甲基氨基丙基丙烯酰胺等丙烯酰胺系衍生物。它们可以使用1种或2种以上。
作为具有酰亚胺基的不饱和化合物,例如可列举出N-丙烯酰氧基乙基-1,2,3,6-四氢邻苯二甲酰亚胺(东亚合成株式会社制,商品名:ARONIX TO-1428)、N-丙烯酰氧基乙基六氢邻苯二甲酰亚胺(东亚合成株式会社制、商品名:ARONIX TO-1429)、N-丙烯酰氧基乙基-3,4,5,6-四氢邻苯二甲酰亚胺(东亚合成株式会社制、商品名:ARONIX TO-1534)等。它们可以使用1种或2种以上。
作为具有腈基的不饱和化合物,例如可列举出丙烯腈、甲基丙烯腈、5-己烯腈、5-甲基-5-己烯腈、甲基-2-氰基丙烯酸酯、乙基-2-氰基丙烯酸酯、丁基-2-氰基丙烯酸酯、环己基-2-氰基丙烯酸酯、2-乙基己基-2-氰基丙烯酸酯、乙氧基乙基-2-氰基丙烯酸酯等。它们可以使用1种或2种以上。
作为具有硫醇基的不饱和化合物,例如可列举出2-巯基乙醇、乙二硫醇、1,2-丙二硫醇、1,3-丙二硫醇、对羟基苯硫酚、3-巯基-1,2-丙二硫醇、1,4-丁二硫醇、2-巯基***、2-巯基乙硫醚等脂肪族或芳香族的巯基醇或二硫醇等含硫醇基的化合物与丙烯酸或甲基丙烯酸形成的酯类等。它们可以使用1种或2种以上。
作为具有异氰酸酯基的不饱和化合物,例如可列举出2-甲基丙烯酰氧基乙基异氰酸酯(昭和电工株式会社制、商品名:Karenz MOI(注册商标))、2-丙烯酰氧基乙基异氰酸酯(昭和电工株式会社制、商品名:Karenz AOI(注册商标))等。它们可以使用1种或2种以上。
具有官能团的不饱和化合物优选为马来酸酐、衣康酸酐、柠康酸酐、四氢邻苯二甲酸酐、内双环-[2.2.1]-5-庚烯-2,3-二羧酸酐、丙烯酸、甲基丙烯酸、丙烯酸羟基乙酯、甲基丙烯酸羟基乙酯、甲基丙烯酸缩水甘油酯、甲基丙烯酸氨基丙酯,更优选为马来酸酐、衣康酸酐、柠康酸酐、四氢邻苯二甲酸酐、内双环-[2.2.1]-5-庚烯-2,3-二羧酸酐这些二羧酸酐,特别优选为马来酸酐。
从获得具有良好的机械特性、对化学溶液的长期耐性和良好的层间粘接性的层叠体的观点出发,改性聚烯烃(B)优选为马来酸酐改性聚丙烯。
[改性聚烯烃(B)的特性]
从获得具有低温下的机械物性和柔软性的层叠体的观点出发,改性聚烯烃(B)的按照ASTM D2240而测得的邵氏硬度(D标尺)的上限为61以下,优选为59以下。
另外,从层叠体的机械强度的观点出发,按照ASTM D2240而测得的邵氏硬度(D标尺)的下限为30以上,优选为45以上,特别优选为50以上。
从获得具有低温下的机械物性和柔软性的层叠体的观点出发,改性聚烯烃(B)的按照ASTM D638而测得的拉伸屈服点应力优选为23MPa以下,特别优选为21MPa以下。另外,从同样的观点出发,按照ASTM D638而测得的拉伸断裂点应力优选为25MPa以上,特别优选为27MPa以上。
改性聚烯烃(B)在230℃/2160g的条件下按照ASTM D1238而测得的MFR值优选为3.5g/10min以上且10.0g/10min以下、更优选为4.0g/10min以上且7.0g/10min以下。通过使改性聚烯烃(B)的MFR值在前述范围内,从而低温下的耐冲击性更优异,能够使层叠体的成形稳定性更高。
一般而言,在聚烯烃的FT-IR测定中,波数710cm-1~740cm-1的最大吸收因该聚烯烃是均聚物还是无规共聚物而发生变化,显示出越靠近710cm-1则越近似于均聚物、越靠近740cm-1则越近似于无规共聚物的结构。在改性聚烯烃(B)的FT-IR测定中,波数处于710cm-1以上且740cm-1以下的吸收之中显示最大强度的波数优选为721cm-1cm以上。如果为这种范围,则能够获得柔软性优异、在低温下的耐冲击性更优异的层叠管。
[改性聚烯烃(B)的组成]
改性聚烯烃(B)中,相对于改性聚烯烃(B)100质量%,前述具有官能团的不饱和化合物的含量优选为后述具有官能团的不饱和化合物的接枝量那样的量。另外,改性聚烯烃(B)为马来酸酐改性聚丙烯时,马来酸酐改性聚丙烯中的聚丙烯的含量相对于马来酸酐改性聚丙烯100质量%,优选为50质量%以上且99.5质量%以下、更优选为60质量%以上且97质量%以下、特别优选为70质量%以上且95质量%以下。通过使马来酸酐改性聚丙烯中的聚丙烯的含量为前述值以上,从而能够使层叠体的柔软性充分,且使低分子量物、离子的耐溶出性更优异。此处,马来酸酐改性聚丙烯中的聚丙烯的含量可以与后述具有官能团的不饱和化合物的接枝量同样地测定。
[改性聚烯烃(B)的制造方法]
改性聚烯烃(B)的制造方法可以采用用于向聚烯烃(B1)中导入前述由具有官能团的不饱和化合物衍生的单元的公知方法。例如可列举出对聚烯烃(B1)接枝共聚前述具有官能团的不饱和化合物的方法;将烯烃单体与前述具有官能团的不饱和化合物进行自由基共聚的方法等,优选为对聚烯烃(B1)接枝共聚前述具有官能团的不饱和化合物的方法。
另外,作为对聚烯烃(B1)接枝共聚前述具有官能团的不饱和化合物的方法,可以采用公知的各种方法。例如可列举出:使改性前的聚烯烃熔融,添加前述具有官能团的不饱和化合物并使其接枝共聚的方法;或者使改性前的聚烯烃溶解于溶剂,添加接枝单体并使其接枝共聚的方法等。在任意情况下,为了使前述具有官能团的不饱和化合物高效地接枝聚合,优选在自由基聚合引发剂的存在下实施反应。
自由基聚合引发剂只要促进聚烯烃主链与具有前述官能团的不饱和化合物的反应,就没有特别限定,优选为有机过氧化物、有机过酸酯。具体而言,可列举出过氧化苯甲酰、过氧化二氯苯甲酰、过氧化二异丙苯、二叔丁基过氧化物、2,5-二甲基-2,5-二(过氧化苯甲酸酯)己炔-3、1,4-双(叔丁基过氧化异丙基)苯、过氧化月桂酰、过氧乙酸叔丁酯、2,5-二甲基-2,5-二(叔丁基过氧化)己炔-3、2,5-二甲基-2,5-二(叔丁基过氧化)己烷、苯甲酸叔丁酯、过氧苯基乙酸叔丁酯、过氧异丁酸叔丁酯、过氧仲辛酸叔丁酯、过氧特戊酸叔丁酯、过氧特戊酸枯基酯、过氧二乙基乙酸叔丁酯等,其它偶氮化合物例如可列举出偶氮双异丁腈、二甲基偶氮异丁腈等。它们可以使用1种或2种以上。这些之中,更优选为过氧化二异丙苯、二叔丁基过氧化物、2,5-二甲基-2,5-二(叔丁基过氧化)己炔-3、2,5-二甲基-2,5-二(叔丁基过氧化)己烷、1,4-双(叔丁基过氧化异丙基)苯等二烷基过氧化物。
自由基聚合引发剂优选以相对于聚烯烃(B1)100质量份为0.001~10质量份左右的量来使用。
前述具有官能团的不饱和化合物的接枝量相对于聚烯烃(B1)100质量%优选为0.05质量%以上且20质量%以下、更优选为0.05质量%以上且10质量%以下、进一步优选为0.05质量%以上且5质量%以下、特别优选为0.05质量%以上且3质量%以下。另外,聚烯烃(B1)的接枝量是从聚烯烃(B1)中去除具有前述官能团的不饱和化合物后测得的净重接枝量。另外,接枝量可通过13C-NMR、1H-NMR测定等公知手段来进行。另外,作为前述具有官能团的不饱和化合物,在使用不饱和羧酸及其酸酐等具有酸性官能团的单体的情况下,作为成为向聚烯烃(B1)导入的官能团量的基准的量,也可以使用例如酸值。另外,作为前述具有官能团的不饱和化合物而使用马来酸酐时,也可以使用红外分光光度计,基于通常在1780~1790cm-1附近检测到的马来酸酐的羰基的吸收光谱来求出接枝量。
改性聚烯烃(B)可根据需要与各种添加剂组合使用。此时,(b)层中,可以在包含改性聚烯烃的基础上包含各种添加剂。作为前述添加剂,可列举出导电性填料、抗氧化剂、热稳定剂、紫外线吸收剂、光稳定剂、润滑剂、无机质填充材料、抗静电剂、阻燃剂、结晶促进剂、增塑剂、着色剂、润滑剂和其它热塑性树脂等。它们可以使用1种或2种以上。
3.层结构
层叠体包含(a)层和(b)层的两层以上。
通过使层叠体包含(a)层,从而能够获得机械物性、耐化学药品性和柔软性优异的层叠体。另外,通过使层叠体包含(b)层,从而使层叠体的化学溶液阻隔性、尤其是对水蒸气、冷却液(LLC)和尿素溶液的阻隔性、长期化学溶液耐性良好。
层叠体优选从外侧朝向内侧按照(a)层、(b)层的顺序进行配置。由此,有效地赋予由(a)层实现的机械物性等特性和由(b)层实现的化学溶液阻隔性等特性这两者。此处,层叠体为片状时等,在层叠体的两个以上的面接触空气等但不接触化学溶液的情况下,将任意的接触空气等但不接触化学溶液的面设为外侧,并将相反侧的面设为内侧。另外,层叠体为中空层叠体时,层叠体的内侧是指与化学溶液接触的层叠体的一侧,外侧是指与空气等接触但不接触化学溶液的层叠体的一侧。
层叠体优选(a)层与(b)层相互邻接。由此,能够得到层间粘接性优异的层叠体。
层叠体优选仅由(a)层和(b)层组成。由此,能够有效地发挥由(a)层和(b)层起到的效果。此时,(a)层和(b)层可分别为1层,也可以为两层以上。
层叠体更优选(a)层配置于层叠体的最外层。通过使(a)层配置于最外层,从而能够得到高温时的破坏压强度更优异的层叠体。层叠体更优选(b)层配置于层叠体的最内层。通过使(b)层配置于最内层,从而能够进一步抑制由与化学溶液接触导致的机械物性降低。
层叠体中,除了(a)层和(b)层这两层之外,为了赋予更多的功能或获得经济上有利的层叠体,可以还具有1层或两层以上的其它层。作为这种其它层,可列举出包含其它热塑性树脂的层和/或除热塑性树脂之外的任意基材的层。层叠体还包含其它层时,优选在层叠体的最内层还包含其它层。通过使层叠体在最内层还包含其它层,从而能够有效地赋予由其它层实现的功能。
作为构成包含其它热塑性树脂的层的热塑性树脂,可列举出聚酰胺系树脂、含氟系聚合物、聚酯系树脂、聚醚系树脂、聚砜系树脂、聚硫醚系树脂、聚酮系树脂、聚腈系树脂、聚甲基丙烯酸酯系树脂、聚乙烯酯系树脂、聚氯乙烯系树脂、纤维素系树脂、聚碳酸酯系树脂、聚酰亚胺系树脂、热塑性聚氨酯系树脂等。
另外,也可以层叠除了热塑性树脂之外的任意基材,例如纸、金属系材料、未拉伸、单轴或双轴拉伸塑料薄膜或片、织布、无纺布、金属棉、木材等。作为金属系材料,可列举出铝、铁、铜、镍、金、银、钛、钼、镁、锰、铅、锡、铬、铍、钨、钴等金属和/或其金属化合物、以及由它们中的2种以上形成的不锈钢等合金钢、铝合金、黄铜、青铜等铜合金、镍合金等合金类等。
关于层叠体中的总层数,只要是具有至少1层(a)层和至少1层(b)层的至少两层,就没有特别限定。层叠体的总层数根据层叠体的制造装置的机构来判断,优选为8层以下、更优选为2层以上且7层以下。另外,出于材料管理、层叠体的成形制造装置的限制,层叠体的总层数特别优选为两层。
层叠体的形状是任意的,可以是片状,也可以是中空状(管状、瓶状等内部为空洞的形状)。作为中空状,优选为管状。层叠体可以具有波形区域。波形区域是指形成为波形形状、蛇腹形状、手风琴形状或波纹形状等的区域。不仅可以遍及层叠体全长地具有波形区域,也可以在中途的适当区域局部具有波形区域。
作为层叠体的具体方式,可列举出层叠中空成形体、层叠薄膜、层叠板,优选为层叠中空成形体。另外,作为层叠中空成形体的具体方式,可列举出层叠管。
层叠体中的(a)层的厚度优选为层叠体的总壁厚的30%以上且95%以下、更优选为40%以上且85%以下、特别优选为45%以上且80%以下。通过使(a)层的层厚度在前述范围内,从而能够有效地发挥前述的各特性。
层叠体中的(b)层的厚度优选大于层叠体的总壁厚的5%且小于70%、更优选大于15%且小于60%、特别优选大于20%且小于55%。通过使(b)层的层厚度在前述范围内,从而能够有效地发挥前述的各特性。
层叠体的总壁厚优选为0.5mm以上且25mm以下。
层叠体为层叠管时,关于层叠管的外径,考虑到循环化学溶液和/或气体(例如发动机冷却液)等的流量,壁厚被设计成化学溶液的透过性不会增大、且能够维持通常的管的破坏压力的厚度,并且,该厚度能够维持管的安装作业容易性和使用时的耐振动性良好这一程度的柔软性,但没有限定。优选的是:外径为4mm以上且300mm以下、内径为3mm以上且250mm以下、壁厚为0.5mm以上且25mm以下。
作为层叠体的制造方法,可列举出:使用与层数或材料数对应的挤出机进行熔融挤出,在模具内或模具外同时层叠的方法(共挤出成形法);或者,暂且预先制造单层管或者通过上述方法而制造的层叠体,根据需要使用粘接剂,在外侧依次使树脂一体化并层叠的方法(涂布法)。层叠体优选通过下述共挤出法来制造:将各种材料在熔融状态下共挤出,使两者热熔接(熔融粘接),从而通过一个阶段来制造层叠结构的管。即,层叠体的制造方法优选包括共挤出成形。
另外,层叠体为复杂形状的情况下、在成形后实施加热弯曲加工而制成成形品的情况下,为了去除成形品的残留应变,也可以在形成上述层叠体后,以低于构成前述层叠体的树脂的熔点之中最低的熔点的温度进行0.01小时以上且10小时以下的热处理,从而得到目标成形品。
具有波形区域的层叠体可通过首先成形为直管状的层叠体后,接着进行模具成形,制成特定的波形形状等来容易地形成。通过具有该波形区域,从而具有冲击吸收性,安装性变得容易。进而,例如通过附加连接器等必要的部件或者进行弯曲加工,能够制成L字、U字的形状等。
对于这样成形的层叠体的外周的全部或一部而言,考虑到飞石、与其他部件的磨耗、以及耐火性,可以配设由天然橡胶(NR)、丁二烯橡胶(BR)、异戊二烯橡胶(IR)、丁基橡胶(IIR)、氯丁橡胶(CR)、羧基化丁二烯橡胶(XBR)、羧基化氯丁橡胶(XCR)、环氧氯丙烷橡胶(ECO)、丙烯腈丁二烯橡胶(NBR)、氢化丙烯腈丁二烯橡胶(HNBR)、羧基化丙烯腈丁二烯橡胶(XNBR)、NBR与聚氯乙烯的混合物、丙烯腈异戊二烯橡胶(NIR)、氯化聚乙烯橡胶(CM)、氯砜化聚乙烯橡胶(CSM)、乙烯丙烯橡胶(EPR)、乙烯丙烯二烯橡胶(EPDM)、乙烯乙酸乙烯酯橡胶(EVM)、NBR与EPDM的混合物橡胶、丙烯酸类橡胶(ACM)、乙烯丙烯酸类橡胶(AEM)、丙烯酸酯丁二烯橡胶(ABR)、苯乙烯丁二烯橡胶(SBR)、羧基化苯乙烯丁二烯橡胶(XSBR)、苯乙烯异戊二烯橡胶(SIR)、苯乙烯异戊二烯丁二烯橡胶(SIBR)、氨基甲酸酯橡胶、硅橡胶(MQ,VMQ)、氟橡胶(FKM,FFKM)、氟硅橡胶(FVMQ)、氯化乙烯基系、烯烃系、酯系、氨基甲酸酯系、酰胺系等热塑性弹性体等构成的固体或海绵状的保护构件(保护件)。保护构件可以通过已知手法制成海绵状的多孔体。通过制成多孔体,能够形成轻量且绝热性优异的保护部。另外,也可以降低材料成本。或者,也可以添加玻璃纤维等来改善其强度。保护构件的形状没有特别限定,通常为筒状构件或具有用于容纳作为层叠体的一个方式的层叠管的凹部的块状构件。为筒状构件时,可以在预先制作的筒状构件中随后***层叠管,或者在层叠管上覆盖挤出筒状构件并使两者密合而制作。为了使两者粘接,根据需要在保护构件内面或前述凹面上涂布粘接剂,并将层叠管***或镶嵌于其中,使两者密合,由此形成层叠管与保护构件一体化而成的结构体。另外,也可以用金属等进行增强。
[层叠体的用途]
层叠体可以用于以汽车部件、内燃机用途、电动工具外壳类的机械部件为代表的工业材料、产业资材、电气/电子部件、医疗、食品、家庭/办公用品、建材相关部件、家具用部件等各种用途。
另外,层叠体因抗化学溶液透过性优异而适合用作化学溶液运输管。作为化学溶液,例如可列举出苯、甲苯、二甲苯、烷基苯类等芳香族烃溶剂;甲醇、乙醇、丙醇、丁醇、戊醇、乙二醇、丙二醇、二乙二醇、苯酚、甲酚、聚乙二醇、聚丙二醇、聚亚烷基二醇等醇;苯酚溶剂;二甲基醚、二丙基醚、甲基叔丁基醚、乙基叔丁基醚、二噁烷、四氢呋喃、多元醇酯类、聚乙烯醚类等醚溶剂;HFC-23、HFC-32、HFC-41、HFC-123、HFC-125、HFC-134、HFC-134a、HFC-143、HFC-143a、HFC-152、HFC-152a、HFC-161、HFC-227ea、HFC-227ca、HFC-236fa、HFC-236ea、HFC-236cb、HFC-236ca、HFC-245ca、HFC-245ea、HFC-245eb、HFC-245fa、HFC-245cb、HFC-254eb、HFC-254cb、HFC-254ca、HFC-263fb、HFC-263ca、HFC-272fb、HFC-272ea、HFC-272fa、HFC-272ca、HFC-281fa、HFC-281ea、HFC-329p、HFC-329mmz、HFC-338mf、HFC-338mcc、HFC-338pcc、HFC-347s、HFC-365mfc、HFC-4310mee、HFC-1123、HFC-1132a、FC-1216、HFC-1223、HFC-1225zc、HFC-1225ye、HFC-1225yc、HFC-1232xf、HFC-1234ye、HFC-1234ze、HFC-1234yf、HFC-1234yc、HFC-1234zc、HFC-1243yf、HFC-1243zc、HFC-1243ye、HFC-1243ze、HFC-1243zf、HFC-1243yc、HFC-1261yf、FC-1318my、FC-1318cy、HFC-1327my、HFC-1327ye、HFC-1327py、HFC-1327et、HFC-1327cz、HFC-1327cye、HFC-1327cyc、HFC-1336yf、HFC-1336ze、HFC-1336eye、HFC-1336eyc、HFC-1336pyy、HFC-1336pz、HFC-1336mzy、HFC-1336mzz、HFC-1336qc、HFC-1336pe、HFC-1336ft、HFC-1345qz、HFC-1345mzy、HFC-1345fz、HFC-1345mzz、HFC-1345sy、HFC-1345fyc、HFC-1345pyz、HFC-1345cyc、HFC-1345pyy、HFC-1345eyc、HFC-1345ctm、HFC-1345ftp、HFC1345fye、HFC-1345eyf、HFC-1345eze、HFC-1345ezc、HFC-1345eye、HFC-1354fzc、HFC-1354ctp、HFC-1354etm、HFC-1354tfp、HFC-1354my、HFC-1354mzy、FC-141-10myy、FC-141-10cy、HFC-1429mzt、HFC-1429myz、HFC-1429mzy、HFC-1429eyc、HFC-1429czc、HFC-1429cycc、HFC-1429pyy、HFC-1429myyc、HFC-1429myye、HFC-1429eyym、HFC-1429cyzm、HFC-1429mzt、HFC-1429czym、HFC-1438fy、HFC-1438eycc、HFC-1438ftmc(、HFC-1438czzm、HFC-1438ezym、HFC-1438ctmf、HFC-1447fzy、HFC-1447fz、HFC-1447fycc、HFC-1447cz、HFC-1447mytm、HFC-1447fyz、HFC-1447ezz、HFC-1447qzt、HFC-1447syt、HFC-1456szt、HFC-1456szy、HFC-1456mstz、HFC-1456fzce、HFC-1456ftmf、FC-151-12c、FC-151-12mcy、FC-151-12mmtt、FC-151-12mmzz、HFC-152-11mmtz、HFC-152-11mmyyz、HFC-152-11mmyyz、HFC-1549fz(PFBE)、HFC-1549fztmm、HFC-1549mmtts、HFC-1549fycz、HFC-1549myts、HFC-1549mzzz、HFC-1558szy、HFC-1558fzccc、HFC-1558mmtzc、HFC-1558ftmf、HFC-1567fts、HFC-1567szz、HFC-1567fzfc、HFC-1567sfyy、HFC-1567fzfy、HFC-1567myzzm(、HFC-1567mmtyf、FC-161-14myy、FC-161-14mcyy、HFC-162-13mzy、HFC162-13myz、HFC-162-13mczy、HFC-162-13mcyz、CFC-11(、CFC-114、CFC-114a、CFC-115、HCFC-21、HCFC-22、HCFC-122、HCFC-123、HCFC-124、HCFC-124a、HCFC-132、HCFC-133a、HCFC-141b、HCFC-142、HCFC-142b、HCFC-225ca、HCFC-225cb、HCFC-240db、HCFC-243db、HCFC-243ab、HCFC-244eb、HCFC-244bb、HCFC-244db、HCFC-1111、HCFC-1113、HCFC-1223xd、HCFC-1224xe、HCFC-1232xf、HCFC-1233xf、HCFC-1233zd、以及它们的混合物等卤代烯烃类;丙酮、甲乙酮、二乙酮、苯乙酮等酮溶剂;矿物油类、硅油类、天然石蜡类、环烷类、合成石蜡类、聚α-烯烃类等、汽油、煤油、柴油、菜籽油甲酯、大豆油甲酯、棕榈油甲酯、椰子油甲酯、天然气液化油(Gas To Liquid:GTL)、煤液化油(Coal To Liquid:CTL)、生物质液化油(Biomass ToLiquid:BTL)、含醇汽油、乙基叔丁醚共混含氧汽油、含胺汽油、酸性汽油、压缩天然气(CNG)、液化石油气(LPG)、液化烃气体(LHG)、液化天然气(LNG)、燃料用二甲醚(DME)、蓖麻油基制动液、二醇醚系制动液、硼酸酯系制动液、极地用制动液、硅油系制动液、矿物油系制动液、动力转向装置油、含硫化氢油、风窗洗涤液、发动机冷却液、尿素溶液、药剂、墨、涂料等。
层叠体适宜作为运输前述化学溶液的管,具体而言,优选为进料管、回流管、蒸发器管、燃料供给管、ORVR管、贮存管、通风管等燃料管;油管、石油挖掘管、空压管、油压管、离合器管、制动器管、制动器负压管、悬架管、空气管、涡轮空气管、风管、漏气管、EGR阀控制管、风窗洗涤液用管、冷却液(LLC)冷却器管、储罐管、尿素溶液运输管、电池冷却加热用管、燃料电池用管、空调用管、加热器管、散热管、路面加热器管、地暖管、基础设施供给用管、灭火器和灭火设备用管、医疗用冷却机材料用管、油墨散布管、涂料散布管、其它化学溶液管,特别优选为冷却液(LLC)冷却器管、尿素溶液运输管、电池冷却加热用管和空调用管中的任一者。
实施例
以下示出实施例和比较例,具体地说明本发明,但本发明不限定于此。首先,示出实施例和比较例中的分析和物性的测定方法、以及实施例和比较例中使用的材料。
1.聚烯烃的特性利用下述方法进行测定。
[邵氏硬度(D标尺)]
按照ASTM D2240来测定邵氏硬度(D标尺)。
[拉伸试验]
按照ASTM D638来测定拉伸屈服点应力和拉伸断裂点应力。
[MFR(熔体流动速率)]
按照ASTM D1238,在230℃、2160g的条件下测定MFR。
[FT-IR]
使用JASCO公司制的FT/IR-4700,在4000cm-1~650cm-1的范围内进行测定。调查710cm-1~740cm-1的范围内的吸收之中的最大波数值。
2.层叠体的各物性利用下述方法进行测定。
[低温耐冲击性]
针对10根层叠管,利用SAE J 2260 7.5中记载的方法,在-40℃下实施冲击试验。其后,确认层叠管有无断裂。
[高温破坏压强度]
针对5根层叠管,利用SAE J 2260 7.2中记载的方法,将试验温度变更为125℃,实施破坏压强度试验。将所测得的破坏压强度的平均值示于表1。
3.实施例和比较例中使用的材料
(1)脂肪族聚酰胺(A1)
[聚酰胺12(A1-1)的制造]
向内容积为70升且附带搅拌机的耐压力反应容器中投入十二内酰胺19.73kg(100.0摩尔)、5-氨基-1,3,3-三甲基环己烷甲胺45.0g(0.264摩尔)和蒸馏水0.5L,将聚合槽内进行氮气置换后,加热至180℃,在该温度下搅拌以使得反应体系内成为均匀状态。接着,使聚合槽内温度升温至270℃,一边将槽内压力调整至3.5MPa,一边在搅拌下聚合2小时。其后,耗用约2小时释放压力至常压(0.1MPa),接着减压至53kPa,在减压下进行5小时的聚合。接着,将氮气导入至高压釜内,恢复压力至常压后,从反应容器的下部喷嘴以股线的形式排出,进行切割而得到粒料。将该粒料进行减压干燥,得到相对粘度为2.20、末端氨基浓度为48μeq/g、末端羧基浓度为24μeq/g的聚酰胺12(以下将该聚酰胺12称为(A1-1))。聚酰胺12(A1-1)的亚甲基数相对于酰胺基数的比值[CH2]/[NHCO]为11.0,满足7.0以上。另外,聚酰胺12(A1-1)的末端氨基浓度[A](μeq/g)、末端羧基浓度[B](μeq/g)满足[A]>[B]+5。
(2)耐冲击剂(A2)
马来酸酐改性乙烯/1-丁烯共聚物(A2-1)(三井化学公司制、Tafmer(注册商标)MH5020、酸酐基浓度:100μeq/g、邵氏硬度(D标尺):<20)
(3)增塑剂(A3)
N-丁基苯磺酰胺(A3-1)(Proviron公司制、Proviplast(注册商标)024)
(4)脂肪族聚酰胺组合物(A)
[脂肪族聚酰胺组合物(A-1)的制造]
向聚酰胺12(A1-1)中预先混合作为耐冲击剂的马来酸酐改性乙烯/1-丁烯共聚物(A2-1)、作为增塑剂的N-丁基苯磺酰胺(A3-1)、作为抗氧化剂的三乙二醇双[3-(3-叔丁基-5-甲基-4-羟基苯基)丙酸酯](BASF JAPAN公司制、IRGANOX(注册商标)245)和作为磷系加工稳定剂的三(2,4-二叔丁基苯基)亚磷酸酯(BASF JAPAN公司制、IRGAFOS168),供给至双螺杆熔融混炼机(株式会社日本制钢所制、型号:TEX(注册商标)44)中,以180℃~270℃的料筒温度进行熔融混炼,将熔融树脂挤出成股线状后,将其导入至水槽中,进行冷却、切割、真空干燥,得到相对于聚酰胺12(A1-1)/耐冲击剂(A2-1)/增塑剂(A3-1)=85.0/10.0/5.0(质量%)的合计100质量份包含抗氧化剂0.8质量份、磷系加工稳定剂0.2质量份的脂肪族聚酰胺组合物(A-1)的粒料。
(5)改性聚烯烃(B)
改性聚烯烃(B-1)马来酸酐改性聚丙烯(三井化学公司制、Admer(注册商标)QF551、邵氏硬度(D标尺):58、拉伸屈服点应力:19MPa、拉伸断裂点应力:31MPa、MFR:5.2g/10min、FT-IR测定中,波数处于710cm-1以上且740cm-1以下的吸收之中显示最大强度的波数:722.2cm-1)
改性聚烯烃(B-2)马来酸酐改性聚丙烯(三井化学公司制、Admer(注册商标)QB516、邵氏硬度(D标尺):62、拉伸屈服点应力:23MPa、拉伸断裂点应力:25MPa、MFR:2.8g/10min、FT-IR测定中,波数处于710cm-1以上且740cm-1以下的吸收之中显示最大强度的波数:720.3cm-1)
改性聚烯烃(B-3)马来酸酐改性聚丙烯(三井化学公司制、Admer(注册商标)QF500、邵氏硬度(D标尺):66、拉伸屈服点应力:24MPa、拉伸断裂点应力:38MPa、MFR:3.5g/10min、FT-IR测定中,波数处于710cm-1以上且740cm-1以下的吸收之中显示最大强度的波数:718.4cm-1)
改性聚烯烃(B-4)马来酸酐改性聚丙烯(三井化学公司制、Admer(注册商标)QB510、邵氏硬度(D标尺):65、拉伸屈服点应力:28MPa、拉伸断裂点应力:33MPa、MFR:2.7g/10min)
改性聚烯烃(B-5)马来酸酐改性聚丙烯(三井化学公司制、Admer(注册商标)QB520E、邵氏硬度(D标尺):64、拉伸屈服点应力:24MPa、拉伸断裂点应力:35MPa、MFR:1.8g/10min)
4.层叠体的制造
(实施例1-1)
使用前述示出的脂肪族聚酰胺组合物(A-1)、改性聚烯烃(B-1),利用PAL32(マイルファー公司制)双层管成形机,使(A-1)以270℃的挤出温度、使(B-1)以220℃的挤出温度分别进行熔融,利用合流器使排出的熔融树脂合流,并成形为层叠管状体。接着,通过用于尺寸控制的定型模进行冷却并脱除,制成由(A-1)形成的(a)层(最外层)、由(B-1)形成的(b)层(最内层)时,得到层构成为(a)/(b)=0.80/0.20mm且内径6.0mm、外径8.0mm的层叠管。将该层叠管的物性测定结果(即,针对5根层叠管的高温破坏压强度的结果和针对10根层叠管的低温耐冲击性的试验结果)示于表1。
(实施例1-2)
在实施例1-1中,变更层厚度,除此之外,利用与实施例1-1相同的方法,得到层构成为(a)/(b)=0.65mm/0.35mm且内径为6.0mm、外径为8.0mm的层叠管。将该层叠管的物性测定结果示于表1。
(实施例1-3)
在实施例1-1中,变更层厚度,除此之外,利用与实施例1-1相同的方法,得到层构成为(a)/(b)=0.50mm/0.50mm且内径为6.0mm、外径为8.0mm的层叠管。将该层叠管的物性测定结果示于表1。
(比较例1-1)
在实施例1-1中,将改性聚烯烃(B-1)变更为(B-2),除此之外,利用与实施例1-1相同的方法,得到表1所示的层构成的层叠管。将该层叠管的物性测定结果示于表1。
(比较例1-2)
在实施例1-2中,将改性聚烯烃(B-1)变更为(B-2),除此之外,利用与实施例1-2相同的方法,得到表1所示的层构成的层叠管。将该层叠管的物性测定结果示于表1。
(比较例1-3)
在实施例1-3中,将改性聚烯烃(B-1)变更为(B-2),除此之外,利用与实施例1-3相同的方法,得到表1所示的层构成的层叠管。将该层叠管的物性测定结果示于表1。
(比较例2-1)
在实施例1-1中,将改性聚烯烃(B-1)变更为(B-3),除此之外,利用与实施例1-1相同的方法,得到表1所示的层构成的层叠管。将该层叠管的物性测定结果示于表1。
(比较例2-2)
在实施例1-2中,将改性聚烯烃(B-1)变更为(B-3),除此之外,利用与实施例1-2相同的方法,得到表1所示的层构成的层叠管。将该层叠管的物性测定结果示于表1。
(比较例2-3)
在实施例1-3中,将改性聚烯烃(B-1)变更为(B-3),除此之外,利用与实施例1-3相同的方法,得到表1所示的层构成的层叠管。将该层叠管的物性测定结果示于表1。
(比较例3-1)
在实施例1-1中,将改性聚烯烃(B-1)变更为(B-4),除此之外,利用与实施例1-1相同的方法,得到表1所示的层构成的层叠管。将该层叠管的物性测定结果示于表1。
(比较例3-2)
在实施例1-2中,将改性聚烯烃(B-1)变更为(B-4),除此之外,利用与实施例1-2相同的方法,得到表1所示的层构成的层叠管。将该层叠管的物性测定结果示于表1。
(比较例3-3)
在实施例1-3中,将改性聚烯烃(B-1)变更为(B-4),除此之外,利用与实施例1-3相同的方法,得到表1所示的层构成的层叠管。将该层叠管的物性测定结果示于表1。
(比较例4-1)
在实施例1-1中,将改性聚烯烃(B-1)变更为(B-5),除此之外,利用与实施例1-1相同的方法,得到表1所示的层构成的层叠管。将该层叠管的物性测定结果示于表1。
(比较例4-2)
在实施例1-2中,将改性聚烯烃(B-1)变更为(B-5),除此之外,利用与实施例1-2相同的方法,得到表1所示的层构成的层叠管。将该层叠管的物性测定结果示于表1。
(比较例4-3)
在实施例1-3中,将改性聚烯烃(B-1)变更为(B-5),除此之外,利用与实施例1-3相同的方法,得到表1所示的层构成的层叠管。将该层叠管的物性测定结果示于表1。
[表1]
由表1可知:实施例的层叠管即便在改性聚烯烃的层变厚的情况下,低温耐冲击性、高温时的破坏压强度也优异。
Claims (17)
1.一种层叠体,其为包含(a)层和(b)层的两层以上的层叠体,
所述(a)层包含脂肪族聚酰胺组合物(A),
所述(b)层包含改性聚烯烃(B),
所述改性聚烯烃(B)含有由基于碳原子数为2以上且10以下的α-烯烃的单体衍生的单元、以及由具有官能团的不饱和化合物衍生的单元,所述具有官能团的不饱和化合物为选自由具有选自羧基、羟基、环氧基、氨基、酰胺基、酰亚胺基、腈基、硫醇基和异氰酸酯基中的至少1种基团的不饱和化合物、以及具有羧基的不饱和化合物的衍生物组成的组中的至少1种,
所述改性聚烯烃(B)按照ASTM D2240而测得的邵氏硬度(D标尺)为30以上且61以下。
2.根据权利要求1所述的层叠体,其中,所述脂肪族聚酰胺组合物(A)包含聚酰胺(A1),所述聚酰胺(A1)是亚甲基数量相对于酰胺基数量之比为7.0以上的脂肪族聚酰胺。
3.根据权利要求1或2所述的层叠体,其中,所述聚酰胺(A1)为选自由聚酰胺11、聚酰胺12、聚酰胺610、聚酰胺612、聚酰胺1010、聚酰胺1012和聚酰胺1212组成的组中的至少1种的均聚物,和/或使用多种形成它们的原料单体而得的至少1种共聚物。
4.根据权利要求1~3中任一项所述的层叠体,其中,所述脂肪族聚酰胺组合物(A)还包含选自由增塑剂、耐冲击剂和耐热剂组成的组中的1种以上的其它成分。
5.根据权利要求1~4中任一项所述的层叠体,其中,所述(a)层与(b)层相互邻接。
6.根据权利要求1~5中任一项所述的层叠体,其中,所述改性聚烯烃(B)按照ASTMD638而测得的拉伸屈服点应力为23MPa以下,按照ASTM D638而测得的拉伸断裂点应力为25MPa以上。
7.根据权利要求1~6中任一项所述的层叠体,其中,所述改性聚烯烃(B)按照ASTMD1238而测得的MFR(230℃、2160g)为3.5g/10min以上。
8.根据权利要求1~7中任一项所述的层叠体,其中,所述改性聚烯烃(B)在FT-IR测定中,波数处于710cm-1以上且740cm-1以下的吸收之中显示最大强度的波数为721cm-1cm以上。
9.根据权利要求1~8中任一项所述的层叠体,其中,所述改性聚烯烃(B)通过下述方法来制造:使改性前的聚烯烃熔融,添加所述具有官能团的不饱和化合物而进行接枝共聚化。
10.根据权利要求1~9中任一项所述的层叠体,其中,所述改性聚烯烃(B)为马来酸酐改性聚丙烯。
11.根据权利要求1~10中任一项所述的层叠体,其仅由所述(a)层和(b)层组成。
12.根据权利要求1~11中任一项所述的层叠体,其通过共挤出成形法来制造。
13.根据权利要求1~12中任一项所述的层叠体,其为层叠中空成形体。
14.根据权利要求13所述的层叠中空成形体,其从外侧起按照所述(a)层、(b)层的顺序配置。
15.根据权利要求14所述的层叠中空成形体,其中,所述(b)层配置于最内层。
16.根据权利要求15所述的层叠中空成形体,其在最内层还包含其它层。
17.根据权利要求13~16中任一项所述的层叠中空成形体,其为管。
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