CN1670066A - 改进耐候性的阻燃聚烯烃 - Google Patents
改进耐候性的阻燃聚烯烃 Download PDFInfo
- Publication number
- CN1670066A CN1670066A CNA2005100594388A CN200510059438A CN1670066A CN 1670066 A CN1670066 A CN 1670066A CN A2005100594388 A CNA2005100594388 A CN A2005100594388A CN 200510059438 A CN200510059438 A CN 200510059438A CN 1670066 A CN1670066 A CN 1670066A
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- CN
- China
- Prior art keywords
- group
- general formula
- bulky amine
- alkyl
- butyl
- Prior art date
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- Granted
Links
- 239000003063 flame retardant Substances 0.000 title claims abstract description 78
- 229920000098 polyolefin Polymers 0.000 title claims abstract description 32
- RNFJDJUURJAICM-UHFFFAOYSA-N 2,2,4,4,6,6-hexaphenoxy-1,3,5-triaza-2$l^{5},4$l^{5},6$l^{5}-triphosphacyclohexa-1,3,5-triene Chemical compound N=1P(OC=2C=CC=CC=2)(OC=2C=CC=CC=2)=NP(OC=2C=CC=CC=2)(OC=2C=CC=CC=2)=NP=1(OC=1C=CC=CC=1)OC1=CC=CC=C1 RNFJDJUURJAICM-UHFFFAOYSA-N 0.000 title claims abstract description 26
- -1 pentabromophenyl Chemical group 0.000 claims abstract description 225
- 150000001412 amines Chemical class 0.000 claims abstract description 98
- 239000000203 mixture Substances 0.000 claims abstract description 79
- 150000001875 compounds Chemical class 0.000 claims abstract description 70
- JDSHMPZPIAZGSV-UHFFFAOYSA-N melamine Chemical compound NC1=NC(N)=NC(N)=N1 JDSHMPZPIAZGSV-UHFFFAOYSA-N 0.000 claims abstract description 13
- 229910052799 carbon Inorganic materials 0.000 claims description 52
- 150000002148 esters Chemical class 0.000 claims description 46
- 239000000126 substance Substances 0.000 claims description 35
- 125000001931 aliphatic group Chemical group 0.000 claims description 30
- 125000002887 hydroxy group Chemical group [H]O* 0.000 claims description 26
- 125000000217 alkyl group Chemical group 0.000 claims description 25
- 239000004743 Polypropylene Substances 0.000 claims description 20
- 229920001155 polypropylene Polymers 0.000 claims description 20
- 229920000877 Melamine resin Polymers 0.000 claims description 12
- 229910052751 metal Inorganic materials 0.000 claims description 12
- 239000002184 metal Substances 0.000 claims description 12
- 239000004114 Ammonium polyphosphate Substances 0.000 claims description 11
- 235000019826 ammonium polyphosphate Nutrition 0.000 claims description 11
- 229920001276 ammonium polyphosphate Polymers 0.000 claims description 11
- WJTCGQSWYFHTAC-UHFFFAOYSA-N cyclooctane Chemical compound C1CCCCCCC1 WJTCGQSWYFHTAC-UHFFFAOYSA-N 0.000 claims description 10
- 239000004914 cyclooctane Substances 0.000 claims description 10
- 125000001436 propyl group Chemical group [H]C([*])([H])C([H])([H])C([H])([H])[H] 0.000 claims description 10
- 125000004432 carbon atom Chemical group C* 0.000 claims description 9
- VUNCWTMEJYMOOR-UHFFFAOYSA-N hexachlorocyclopentadiene Chemical compound ClC1=C(Cl)C(Cl)(Cl)C(Cl)=C1Cl VUNCWTMEJYMOOR-UHFFFAOYSA-N 0.000 claims description 9
- 239000000049 pigment Substances 0.000 claims description 7
- 150000005690 diesters Chemical class 0.000 claims description 6
- 230000026030 halogenation Effects 0.000 claims description 6
- 238000005658 halogenation reaction Methods 0.000 claims description 6
- RGSFGYAAUTVSQA-UHFFFAOYSA-N pentamethylene Natural products C1CCCC1 RGSFGYAAUTVSQA-UHFFFAOYSA-N 0.000 claims description 6
- 125000004817 pentamethylene group Chemical group [H]C([H])([*:2])C([H])([H])C([H])([H])C([H])([H])C([H])([H])[*:1] 0.000 claims description 6
- JOYRKODLDBILNP-UHFFFAOYSA-N Ethyl urethane Chemical compound CCOC(N)=O JOYRKODLDBILNP-UHFFFAOYSA-N 0.000 claims description 5
- 241001597008 Nomeidae Species 0.000 claims description 5
- 239000003963 antioxidant agent Substances 0.000 claims description 5
- 150000007530 organic bases Chemical class 0.000 claims description 5
- 230000003078 antioxidant effect Effects 0.000 claims description 4
- 239000002075 main ingredient Substances 0.000 claims description 4
- AVXURJPOCDRRFD-UHFFFAOYSA-N Hydroxylamine Chemical compound ON AVXURJPOCDRRFD-UHFFFAOYSA-N 0.000 claims description 3
- 239000004902 Softening Agent Substances 0.000 claims description 3
- 229940058344 antitrematodals organophosphorous compound Drugs 0.000 claims description 3
- 239000000975 dye Substances 0.000 claims description 3
- 230000009931 harmful effect Effects 0.000 claims description 3
- 229910044991 metal oxide Inorganic materials 0.000 claims description 3
- 150000004706 metal oxides Chemical class 0.000 claims description 3
- 150000002903 organophosphorus compounds Chemical class 0.000 claims description 3
- YSMRWXYRXBRSND-UHFFFAOYSA-N TOTP Chemical compound CC1=CC=CC=C1OP(=O)(OC=1C(=CC=CC=1)C)OC1=CC=CC=C1C YSMRWXYRXBRSND-UHFFFAOYSA-N 0.000 claims description 2
- 239000012752 auxiliary agent Substances 0.000 claims description 2
- 239000013008 thixotropic agent Substances 0.000 claims description 2
- 230000002152 alkylating effect Effects 0.000 claims 2
- 239000004611 light stabiliser Substances 0.000 abstract description 11
- 229920001169 thermoplastic Polymers 0.000 abstract description 11
- DYIZJUDNMOIZQO-UHFFFAOYSA-N 4,5,6,7-tetrabromo-2-[2-(4,5,6,7-tetrabromo-1,3-dioxoisoindol-2-yl)ethyl]isoindole-1,3-dione Chemical compound O=C1C(C(=C(Br)C(Br)=C2Br)Br)=C2C(=O)N1CCN1C(=O)C2=C(Br)C(Br)=C(Br)C(Br)=C2C1=O DYIZJUDNMOIZQO-UHFFFAOYSA-N 0.000 abstract description 2
- DEIGXXQKDWULML-UHFFFAOYSA-N 1,2,5,6,9,10-hexabromocyclododecane Chemical compound BrC1CCC(Br)C(Br)CCC(Br)C(Br)CCC1Br DEIGXXQKDWULML-UHFFFAOYSA-N 0.000 abstract 1
- NZUPFZNVGSWLQC-UHFFFAOYSA-N 1,3,5-tris(2,3-dibromopropyl)-1,3,5-triazinane-2,4,6-trione Chemical compound BrCC(Br)CN1C(=O)N(CC(Br)CBr)C(=O)N(CC(Br)CBr)C1=O NZUPFZNVGSWLQC-UHFFFAOYSA-N 0.000 abstract 1
- UGQQAJOWXNCOPY-UHFFFAOYSA-N dechlorane plus Chemical compound C12CCC3C(C4(Cl)Cl)(Cl)C(Cl)=C(Cl)C4(Cl)C3CCC2C2(Cl)C(Cl)=C(Cl)C1(Cl)C2(Cl)Cl UGQQAJOWXNCOPY-UHFFFAOYSA-N 0.000 abstract 1
- 229940056960 melamin Drugs 0.000 abstract 1
- 229910052757 nitrogen Inorganic materials 0.000 description 56
- 239000002585 base Substances 0.000 description 53
- 125000001997 phenyl group Chemical group [H]C1=C([H])C([H])=C(*)C([H])=C1[H] 0.000 description 39
- 150000001721 carbon Chemical group 0.000 description 35
- 229910052739 hydrogen Inorganic materials 0.000 description 35
- 239000001257 hydrogen Substances 0.000 description 34
- LFQSCWFLJHTTHZ-UHFFFAOYSA-N Ethanol Chemical compound CCO LFQSCWFLJHTTHZ-UHFFFAOYSA-N 0.000 description 21
- ISWSIDIOOBJBQZ-UHFFFAOYSA-N Phenol Chemical compound OC1=CC=CC=C1 ISWSIDIOOBJBQZ-UHFFFAOYSA-N 0.000 description 21
- 150000002431 hydrogen Chemical class 0.000 description 20
- 239000002253 acid Substances 0.000 description 19
- 239000001301 oxygen Substances 0.000 description 18
- 229910052760 oxygen Inorganic materials 0.000 description 18
- FIDRAVVQGKNYQK-UHFFFAOYSA-N 1,2,3,4-tetrahydrotriazine Chemical compound C1NNNC=C1 FIDRAVVQGKNYQK-UHFFFAOYSA-N 0.000 description 16
- UFHFLCQGNIYNRP-UHFFFAOYSA-N Hydrogen Chemical compound [H][H] UFHFLCQGNIYNRP-UHFFFAOYSA-N 0.000 description 14
- 239000000654 additive Substances 0.000 description 14
- 238000004380 ashing Methods 0.000 description 14
- LYCAIKOWRPUZTN-UHFFFAOYSA-N ethylene glycol Natural products OCCO LYCAIKOWRPUZTN-UHFFFAOYSA-N 0.000 description 14
- 239000000463 material Substances 0.000 description 14
- 125000002496 methyl group Chemical group [H]C([H])([H])* 0.000 description 14
- OFOBLEOULBTSOW-UHFFFAOYSA-N Malonic acid Chemical compound OC(=O)CC(O)=O OFOBLEOULBTSOW-UHFFFAOYSA-N 0.000 description 13
- 230000000996 additive effect Effects 0.000 description 13
- OKKJLVBELUTLKV-UHFFFAOYSA-N methanol Natural products OC OKKJLVBELUTLKV-UHFFFAOYSA-N 0.000 description 13
- 229920000642 polymer Polymers 0.000 description 13
- 239000004698 Polyethylene Substances 0.000 description 12
- QVGXLLKOCUKJST-UHFFFAOYSA-N atomic oxygen Chemical compound [O] QVGXLLKOCUKJST-UHFFFAOYSA-N 0.000 description 12
- 238000000034 method Methods 0.000 description 12
- 229960003742 phenol Drugs 0.000 description 12
- 229920000573 polyethylene Polymers 0.000 description 12
- 229920002397 thermoplastic olefin Polymers 0.000 description 12
- VGGSQFUCUMXWEO-UHFFFAOYSA-N Ethene Chemical compound C=C VGGSQFUCUMXWEO-UHFFFAOYSA-N 0.000 description 11
- 230000008859 change Effects 0.000 description 11
- KBPLFHHGFOOTCA-UHFFFAOYSA-N 1-Octanol Chemical compound CCCCCCCCO KBPLFHHGFOOTCA-UHFFFAOYSA-N 0.000 description 10
- DNIAPMSPPWPWGF-UHFFFAOYSA-N Propylene glycol Chemical compound CC(O)CO DNIAPMSPPWPWGF-UHFFFAOYSA-N 0.000 description 10
- 125000001118 alkylidene group Chemical group 0.000 description 10
- 125000001797 benzyl group Chemical group [H]C1=C([H])C([H])=C(C([H])=C1[H])C([H])([H])* 0.000 description 10
- XBDQKXXYIPTUBI-UHFFFAOYSA-N dimethylselenoniopropionate Natural products CCC(O)=O XBDQKXXYIPTUBI-UHFFFAOYSA-N 0.000 description 10
- 229940059574 pentaerithrityl Drugs 0.000 description 10
- 125000003118 aryl group Chemical group 0.000 description 9
- 125000000484 butyl group Chemical group [H]C([*])([H])C([H])([H])C([H])([H])C([H])([H])[H] 0.000 description 9
- 239000003795 chemical substances by application Substances 0.000 description 9
- 229920001577 copolymer Polymers 0.000 description 9
- ZFSLODLOARCGLH-UHFFFAOYSA-N isocyanuric acid Natural products OC1=NC(O)=NC(O)=N1 ZFSLODLOARCGLH-UHFFFAOYSA-N 0.000 description 9
- GLDOVTGHNKAZLK-UHFFFAOYSA-N octadecan-1-ol Chemical compound CCCCCCCCCCCCCCCCCCO GLDOVTGHNKAZLK-UHFFFAOYSA-N 0.000 description 9
- 239000000843 powder Substances 0.000 description 9
- 239000004594 Masterbatch (MB) Substances 0.000 description 8
- CXMXRPHRNRROMY-UHFFFAOYSA-N sebacic acid Chemical compound OC(=O)CCCCCCCCC(O)=O CXMXRPHRNRROMY-UHFFFAOYSA-N 0.000 description 8
- RKMGAJGJIURJSJ-UHFFFAOYSA-N 2,2,6,6-Tetramethylpiperidine Substances CC1(C)CCCC(C)(C)N1 RKMGAJGJIURJSJ-UHFFFAOYSA-N 0.000 description 7
- 239000005977 Ethylene Substances 0.000 description 7
- 125000003545 alkoxy group Chemical group 0.000 description 7
- 230000000052 comparative effect Effects 0.000 description 7
- 125000000113 cyclohexyl group Chemical group [H]C1([H])C([H])([H])C([H])([H])C([H])(*)C([H])([H])C1([H])[H] 0.000 description 7
- 239000004700 high-density polyethylene Substances 0.000 description 7
- 150000002430 hydrocarbons Chemical group 0.000 description 7
- 239000002530 phenolic antioxidant Substances 0.000 description 7
- 238000002360 preparation method Methods 0.000 description 7
- QQONPFPTGQHPMA-UHFFFAOYSA-N propylene Natural products CC=C QQONPFPTGQHPMA-UHFFFAOYSA-N 0.000 description 7
- 239000003381 stabilizer Substances 0.000 description 7
- 125000004079 stearyl group Chemical group [H]C([*])([H])C([H])([H])C([H])([H])C([H])([H])C([H])([H])C([H])([H])C([H])([H])C([H])([H])C([H])([H])C([H])([H])C([H])([H])C([H])([H])C([H])([H])C([H])([H])C([H])([H])C([H])([H])C([H])([H])C([H])([H])[H] 0.000 description 7
- 238000005211 surface analysis Methods 0.000 description 7
- 125000003903 2-propenyl group Chemical group [H]C([*])([H])C([H])=C([H])[H] 0.000 description 6
- PXHVJJICTQNCMI-UHFFFAOYSA-N Nickel Chemical compound [Ni] PXHVJJICTQNCMI-UHFFFAOYSA-N 0.000 description 6
- ABLZXFCXXLZCGV-UHFFFAOYSA-N Phosphorous acid Chemical compound OP(O)=O ABLZXFCXXLZCGV-UHFFFAOYSA-N 0.000 description 6
- QRUDEWIWKLJBPS-UHFFFAOYSA-N benzotriazole Chemical compound C1=CC=C2N[N][N]C2=C1 QRUDEWIWKLJBPS-UHFFFAOYSA-N 0.000 description 6
- 239000012964 benzotriazole Substances 0.000 description 6
- 125000003236 benzoyl group Chemical group [H]C1=C([H])C([H])=C(C([H])=C1[H])C(*)=O 0.000 description 6
- FQUNFJULCYSSOP-UHFFFAOYSA-N bisoctrizole Chemical compound N1=C2C=CC=CC2=NN1C1=CC(C(C)(C)CC(C)(C)C)=CC(CC=2C(=C(C=C(C=2)C(C)(C)CC(C)(C)C)N2N=C3C=CC=CC3=N2)O)=C1O FQUNFJULCYSSOP-UHFFFAOYSA-N 0.000 description 6
- 239000001055 blue pigment Substances 0.000 description 6
- ZJIPHXXDPROMEF-UHFFFAOYSA-N dihydroxyphosphanyl dihydrogen phosphite Chemical compound OP(O)OP(O)O ZJIPHXXDPROMEF-UHFFFAOYSA-N 0.000 description 6
- 125000003438 dodecyl group Chemical group [H]C([H])([H])C([H])([H])C([H])([H])C([H])([H])C([H])([H])C([H])([H])C([H])([H])C([H])([H])C([H])([H])C([H])([H])C([H])([H])C([H])([H])* 0.000 description 6
- 238000009472 formulation Methods 0.000 description 6
- NAQMVNRVTILPCV-UHFFFAOYSA-N hexane-1,6-diamine Chemical compound NCCCCCCN NAQMVNRVTILPCV-UHFFFAOYSA-N 0.000 description 6
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- TVMXDCGIABBOFY-UHFFFAOYSA-N n-Octanol Natural products CCCCCCCC TVMXDCGIABBOFY-UHFFFAOYSA-N 0.000 description 6
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- IIYFAKIEWZDVMP-UHFFFAOYSA-N tridecane Chemical compound CCCCCCCCCCCCC IIYFAKIEWZDVMP-UHFFFAOYSA-N 0.000 description 6
- SNRUBQQJIBEYMU-UHFFFAOYSA-N Dodecane Natural products CCCCCCCCCCCC SNRUBQQJIBEYMU-UHFFFAOYSA-N 0.000 description 5
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- 150000001408 amides Chemical class 0.000 description 5
- WPYMKLBDIGXBTP-UHFFFAOYSA-N benzoic acid Chemical compound OC(=O)C1=CC=CC=C1 WPYMKLBDIGXBTP-UHFFFAOYSA-N 0.000 description 5
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- 125000001495 ethyl group Chemical group [H]C([H])([H])C([H])([H])* 0.000 description 5
- 125000003055 glycidyl group Chemical group C(C1CO1)* 0.000 description 5
- 125000002347 octyl group Chemical group [H]C([*])([H])C([H])([H])C([H])([H])C([H])([H])C([H])([H])C([H])([H])C([H])([H])C([H])([H])[H] 0.000 description 5
- 125000005447 octyloxy group Chemical group [H]C([H])([H])C([H])([H])C([H])([H])C([H])([H])C([H])([H])C([H])([H])C([H])([H])C([H])([H])O* 0.000 description 5
- 125000002924 primary amino group Chemical group [H]N([H])* 0.000 description 5
- 235000019260 propionic acid Nutrition 0.000 description 5
- IUVKMZGDUIUOCP-BTNSXGMBSA-N quinbolone Chemical compound O([C@H]1CC[C@H]2[C@H]3[C@@H]([C@]4(C=CC(=O)C=C4CC3)C)CC[C@@]21C)C1=CCCC1 IUVKMZGDUIUOCP-BTNSXGMBSA-N 0.000 description 5
- 125000001424 substituent group Chemical group 0.000 description 5
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- WJFKNYWRSNBZNX-UHFFFAOYSA-N 10H-phenothiazine Chemical compound C1=CC=C2NC3=CC=CC=C3SC2=C1 WJFKNYWRSNBZNX-UHFFFAOYSA-N 0.000 description 4
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- DWDAZFJBSZTCCM-UHFFFAOYSA-N [O]C1CCCCC1 Chemical compound [O]C1CCCCC1 DWDAZFJBSZTCCM-UHFFFAOYSA-N 0.000 description 4
- 238000010521 absorption reaction Methods 0.000 description 4
- 235000006708 antioxidants Nutrition 0.000 description 4
- 150000001732 carboxylic acid derivatives Chemical class 0.000 description 4
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- 125000002704 decyl group Chemical group [H]C([H])([H])C([H])([H])C([H])([H])C([H])([H])C([H])([H])C([H])([H])C([H])([H])C([H])([H])C([H])([H])C([H])([H])* 0.000 description 4
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- 125000004185 ester group Chemical group 0.000 description 4
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- HTSVYUUXJSMGQC-UHFFFAOYSA-N 2-chloro-1,3,5-triazine Chemical class ClC1=NC=NC=N1 HTSVYUUXJSMGQC-UHFFFAOYSA-N 0.000 description 3
- BKZXZGWHTRCFPX-UHFFFAOYSA-N 2-tert-butyl-6-methylphenol Chemical compound CC1=CC=CC(C(C)(C)C)=C1O BKZXZGWHTRCFPX-UHFFFAOYSA-N 0.000 description 3
- ACZGCWSMSTYWDQ-UHFFFAOYSA-N 3h-1-benzofuran-2-one Chemical class C1=CC=C2OC(=O)CC2=C1 ACZGCWSMSTYWDQ-UHFFFAOYSA-N 0.000 description 3
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- 239000001273 butane Substances 0.000 description 3
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- XJDNKRIXUMDJCW-UHFFFAOYSA-J titanium tetrachloride Chemical compound Cl[Ti](Cl)(Cl)Cl XJDNKRIXUMDJCW-UHFFFAOYSA-J 0.000 description 1
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- C08K3/32—Phosphorus-containing compounds
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Abstract
稳定化的热塑性聚合物,尤其聚烯烃组合物,它们包括选自下面这些的阻燃剂:b1)蜜胺型阻燃剂,或此类化合物中的一种,b2)双-(六氯环戊二烯基并)环辛烷,b3)三-(2,3-二溴丙基)-异氰脲酸酯,b4)亚乙基-双-四溴邻苯二甲酰亚胺;b5)1,2,5,6,9,10-六溴环十二烷,b6)乙烷-1,2-双(五溴苯基);和c)烃氧基胺或羟基烃氧基胺类型的位阻胺光稳定剂和任选的其它组分,兼备最佳的户外耐候稳定性和良好的阻燃性质。
Description
本案是优先权申请日为2000年12月12日、中国专利申请号为01143159.5、发明名称为“改进耐候性的阻燃聚烯烃”的申请的分案申请。
技术领域
本发明涉及被稳定化后可抵抗光、氧和热的损害作用和含有某些阻燃剂的热塑性有机聚合物,尤其聚烯烃如热塑性聚烯烃(TPO),它含有烃氧基胺或羟基烃氧基胺类型的位阻胺和任选的其它稳定剂,涉及这些阻燃剂和位阻胺类赋予光稳定化性能和阻燃性能的用途,和涉及改进热塑性有机聚合物的光稳定性和阻燃性的相应方法。
背景技术
美国专利5,393,812描述了通过添加卤化烃基磷酸酯或膦酸酯阻燃剂赋予阻燃性和用烷氧基胺官能化位阻胺加以稳定化而具备耐候性的聚烯烃组合物。EP-A-792911提出了烷氧基胺官能化位阻胺用于改进聚烯烃的阻燃性质的用途。烷氧基胺官能化位阻胺单独作为阻燃剂的活性已公开在WO99/00450中。
但仍然需要改进阻燃性聚合物组合物,以获得良好的耐候稳定性。
发明内容
现在已经发现,当某些位阻胺稳定剂与特定的阻燃剂并用时,抵抗紫外线和耐候的最佳稳定化和良好的阻燃性质,尤其对于户外应用,都能够体现于热塑性聚合物,尤其聚烯烃,聚烯烃共聚物或它们的混合物如冲击改性聚烯烃或热塑性聚烯烃(TPO)中。因此,本发明涉及选自以下的阻燃剂:
b1)蜜胺型阻燃剂和/或聚磷酸铵,
b2)双-(六氯环戊二烯基并)环辛烷,
b3)三-(2,3-二溴丙基)-异氰脲酸酯,
b4)亚乙基-双-四溴邻苯二甲酰亚胺,
b5)1,2,5,6,9,10-六溴环十二烷,
b6)乙烷-1,2-双(五溴苯基);
和
c)烃氧基胺或羟基烃氧基胺类型的位阻胺光稳定剂的联合使用,以同时赋予热塑性聚合物(a)耐候稳定性和阻燃性,
前提条件是,如果位阻胺属于羟基烃氧基类型,则该阻燃剂不是(b4)。
组分(c)的烃氧基胺或羟基烃氧基胺类型的位阻胺光稳定剂体现特征于它的在氨基氮原子上的取代基E1-O-(参见下式),其中E1优选是在烃氧基胺类型的位阻胺中的C1-C18烷基,C5-C12环烷基或C7-C15芳烷基;和E1优选是在羟基烃氧基胺类型的位阻胺中的C1-C18烷基,C5-C12环烷基或C7-C15芳烷基,其中每一个在脂族部分中被1-3个OH基团取代。含有反应活性OH基团的后一类型的化合物也能够以它的反应产物形式使用。
组分c的烃氧基胺或羟基烃氧基胺类型的该位阻胺光稳定剂通常是含有下式的基团的化合物
其中G1和G2独立地是具有1-4个碳原子的烷基或一起是五亚甲基,和
E1是C1-C18烷基,C5-C12环烷基或C7-C15芳烷基;或E1是在脂族部分中被1-3个OH基团取代的C1-C18烷基,C5-C12环烷基或C7-C15芳烷基;或是它们的反应产物。优选的是符合下式的环状位阻胺
其中
G1,G2和E1如以上所定义;
T是为了完成通式I以便与位阻胺氮原子和被G1和G2取代的两个季碳原子一起形成5元-或6元脂族环结构尤其哌啶环所需要的二价有机基;
或是由二烷基酯或异氰酸酯与其中E1含有1个OH基团和T是-CH2-CH(OH)-CH2-的通式(I)的化合物反应所形成的低聚或高聚位阻胺分子;
或是其中E1含有1个OH基团和T是-CH2-CH(OH)-CH2-的通式(I)的简单二酯或脲烷衍生物.
一般而言,所用组分c的化合物的有效稳定量是0.01-10wt%,优选0.05-5wt%,尤其0.1-2wt%的组分(c)的稳定剂,基于聚合物组分(a)。
本发明的组分(c)的位阻胺类已知为光稳定剂(US-5004770;US-5096950;US-5204473;US-5096950;US-5300544;US-6117995;US-6271377)。
组分(b)的阻燃剂的是可商购的化合物。最优选的是三-(2,3-二溴丙基)-异氰脲酸酯(b3)。
无卤素的阻燃剂b1通常以相当于聚合物(a)的1-约50wt%,优选相当于聚合物(a)的5-50wt%的量使用。b1∶c最优选是在20∶1到250∶1范围内。
卤化阻燃剂b2,b3,b4,b5和/或b6通常是以相当于聚合物(a)的0.5-40wt%的总量,更优选相当于聚合物(a)的3-40wt%,最优选5-35wt%的总量使用。
在本发明组合物中阻燃剂(b)的最优选量:
对于b1)蜜胺型阻燃剂和/或聚磷酸铵,是20-50%;
对于b2)双-(六氯环戊二烯基并)环辛烷,是5-20%;
对于b3)三-(2,3-二溴丙基)-异氰脲酸酯,是2-10%;
对于b4)亚乙基-双-四溴邻苯二甲酰亚胺,是10-40%;
对于b5)1,2,5,6,9,10-六溴环十二烷,是2-20%;
对于b6)乙烷-1,2-双(五溴苯基),是2-20%;
各量表示重量百分数,基于聚合物(a)的重量。
在本发明的上下文中也十分重要的是使用阻燃剂三(3-溴-2,2-(溴甲基)丙基)磷酸酯(b7;见下文),它最优选以基于聚合物(a)重量的2-20wt%,尤其2-10wt%的量使用。
卤化阻燃剂b2,b3,b4,b5,b6或b7∶c的比率最优选是在5∶1到100∶1范围内。
理想地,卤化阻燃剂如b2,b3,b4,b5,b6和/或b7可以与合适的协合剂如锑化合物(常常是Sb2O3)相结合使用,它通常以相当于聚合物(a)的0.5-20wt%的量添加。
组分a常常选自下列热塑性聚合物:
1、单烯烃和二烯烃的聚合物,例如聚丙烯,聚异丁烯,聚丁烯-1,聚-4-甲基戊烯-1,聚异戊二烯或聚丁二烯,以及环状烯烃如环戊烯或降冰片烯的聚合物,聚乙烯(任选地加以交联),例如高密度聚乙烯(HDPE),高密度和高分子量聚乙烯(HDPE-HMW),高密度和超高分子量聚乙烯(HDPE-UHMW),中等密度聚乙烯(MDPE),低密度聚乙烯(LDPE),线性低密度聚乙烯(LLDPE),(VLDPE)和(ULDPE)。
聚烯烃,即在前面的段落中例举的单烯烃的聚合物,优选聚乙烯和聚丙烯,能够通过不同的方法,和优选通过下面的方法来制备:
a)自由基聚合反应(一般在高压和升高的温度下)。
b)使用一般含有元素周期表的IVb,Vb,VIb或VIII族的一种或一种以上金属的催化剂的催化聚合反应。这些金属通常具有一个或一个以上的配位体,典型的是π键或σ键配位的氧化物,卤化物,醇化物,酯类,醚类,胺类,烷基类,链烯基类和/或芳基类。这些金属配合物可以是游离形式或被固定在基体上,典型地在活化氯化镁、氯化钛(III)、氧化铝或氧化硅上。这些催化剂可以溶于或不溶于聚合反应介质中。这些催化剂本身可用于聚合反应或另外使用活化剂,典型的是金属烷基化物,金属氢化物,金属烷基卤化物,金属烷基氧化物或金属烷基噁烷(alkyloxanes),这些金属是元素周期表的Ia,IIa和/或IIIa族的元素。活化剂可以方便地另外用酯,醚,胺或甲硅烷基醚基团改性。这些催化剂体系通常被命名为Phillips,Standard OilIndiana,Ziegler(-Natta),TNZ(Dupont),金属茂或单位点催化剂(SSC)。
2、在以上1)项提到的聚合物的混合物,例如聚丙烯与聚异丁烯的混合物,聚丙烯与聚乙烯的混合物(例如PP/HDPE,PP/LDPE)和不同类型的聚乙烯的混合物(例如LDPE/HDPE)。
3、单烯烃和二烯烃的共聚物,或单烯烃和二烯烃与其它乙烯基单体的共聚物,例如乙烯/丙烯共聚物,线性低密度聚乙烯(LLDPE)和它与低密度聚乙烯(LDPE)的混合物,丙烯/丁烯-1共聚物,丙烯/异丁烯共聚物,乙烯/丁烯-1共聚物,乙烯/己烯共聚物,乙烯/甲基戊烯共聚物,乙烯/庚烯共聚物,乙烯/辛烯共聚物,丙烯/丁二烯共聚物,异丁烯/异戊二烯共聚物,乙烯/丙烯酸烷基酯共聚物,乙烯/甲基丙烯酸烷基酯共聚物,乙烯/乙酸乙烯酯共聚物和它们与一氧化碳的共聚物或乙烯/丙烯酸共聚物和它们的盐类(离聚物类)以及乙烯与丙烯和二烯烃如己二烯、二聚环戊二烯或亚乙基一降冰片烯的三元共聚物;和此类共聚物相互之间的混合物和与以上1)项中提到的聚合物的混合物,例如聚丙烯/乙烯-丙烯共聚物,LDPE/乙烯-乙酸乙烯酯共聚物(EVA),LDPE/乙烯-丙烯酸共聚物(EAA),LLDPE/EVA,LLDPE/EAA和交替或无规聚亚烷基/一氧化碳共聚物和它们与其它聚合物如聚酰胺的混合物。
44.上述聚合物的共混物(聚合物的混合物),例如PP/EPDM。
在下文中,该术语聚烯烃将用于表示纯聚烯烃均聚物以及它的共聚物和共混物。
优选地,该聚烯烃或热塑性烯烃或聚烯烃(TPO)是在这些组合物中存在的唯一有机聚合物;它主要是聚乙烯(PE)或聚丙烯(PP),尤其是LDPE,LLDPE或PP,或PP和PE的共聚物。
尤其优选作为组分(a)的是已知为热塑性(聚)烯烃(TPO)的聚合物,例如含有冲击改性剂或弹性体组分如EPR等的聚丙烯或聚乙烯,或非均相共聚物(参见例如W.Neissl等人,Kunststoffe 83,No.8,1993)。
其中本发明化合物是有效的聚合物组合物的例子包括:因卤化阻燃剂的分解产生的酸性残基使不具有N-OR基团的位阻胺减活的阻燃性聚烯烃,来***虫剂的酸性残基干扰“正常”位阻胺稳定剂的活性的屋顶薄膜、棚膜和农用地膜,以及热塑性聚烯烃,其中颜料与碱性位阻胺稳定剂的相互作用干扰对该基材表面的涂漆。
优选地,本组分c的化合物是含有通式(II)和/或(III)的基团的环状位阻胺:
其中G是氢或甲基,和G1和G2彼此独立地是氢,甲基或一起是取代基=O。
本组分c的位阻胺的例子是下面在类型(a’)至(m’)名义下描述的化合物。
(a’)下式(1a)的化合物:
其中n1是1-4中的数,G和G1彼此独立地是氢或甲基,
G11是O,羟基,C1-C18烷氧基,C5-C12环烷氧基,C7-C15苯基烷氧基;或G11是在各自的脂族部分中被1-3个OH基团取代的C1-C18烷氧基,C5-C12环烷氧基或C7-C15苯基烷氧基;G11优选是C1-C12烷氧基或环己基氧基或C2-C8羟基烷氧基,尤其辛氧基,环己基氧基或2-羟基-2-甲基丙氧基,并且如果n1是1,则G12是氢,不被或被一个或多个氧原子***的C1-C18烷基,COO和/或CONH基团,或者是氰基乙基,苯甲酰基,缩水甘油基,脂肪族、环脂族、芳脂族、不饱和的或芳族羧酸、氨基甲酸或含磷的酸的一价基团或一价甲硅烷基,优选具有2-18个碳原子的脂族羧酸、具有7-15个碳原子的环脂族羧酸或具有3-5个碳原子的α,β-不饱和羧酸或具有7-15个碳原子的芳族羧酸的基团,其中各羧酸能够在脂族、环脂族或芳族结构部分中被1-3个-COOZ12基团取代,其中Z12是H,C1-C20烷基,C3-C12链烯基,C5-C7环烷基,苯基或苄基,
如果n1是2,则G12是C2-C12亚烷基,C4-C12亚链烯基,亚二甲苯基,脂肪族、环脂族、芳脂族或芳族二羧酸、二氨基甲酸或含磷的酸的二价基团或二价甲硅烷基;优选是具有2-36个碳原子的脂族二羧酸,或具有8-14个碳原子的环脂族或芳族二羧酸或具有8-14个碳原子的脂肪族,环脂族或芳族二氨基甲酸的二价基团,其中各二羧酸可以在该脂肪族,环脂族或芳族结构部分中被一个或两个COOZ12基团取代,
如果n1是3,则G12是脂肪族,环脂族或芳族三羧酸的三价基团,它可以在芳族三(氨基甲酸)或含磷的酸的脂肪族,环脂族或芳族结构部分中被COOZ12取代,或是三价甲硅烷基,优选的基团包括苯三甲酸的次氮基三乙酸的三乙酰基,
以及如果n1是4,则G12是脂肪族,环脂族或芳族四羧酸的四价基团。
以上提及的羧酸基团在每一种情况下是指通式(-CO)xR的基团,其中x与以上对于n1的定义相同,和R的含意来源于以上给出的定义。
具有至多20个碳原子烷基是,例如,甲基,乙基,正-丙基,正丁基,仲丁基,叔丁基,正己基,正辛基,2-乙基己基,正壬基,正癸基,正十一烷基,正十二烷基,正十三烷基,正十四烷基,正十六烷基或正十八烷基。
C1-C18烷氧基G11是,例如,甲氧基,乙氧基,丙氧基,异丙氧基,丁氧基,异丁氧基,戊氧基,异戊氧基,己氧基,庚氧基,辛氧基,癸氧基,十二烷氧基,十四烷氧基,十六烷氧基和十八烷氧基。C6-C12烷氧基,特别庚氧基和辛氧基,是优选的。
C5-C12环烷氧基G11是,例如,环戊氧基,环己氧基,环庚氧基,环辛氧基,环癸氧基和环十二烷氧基。C5-C8环烷氧基,特别环戊氧基和环己氧基,是优选的。
C7-C9苯基烷氧基是,例如,苄氧基。
作为在脂族部分中被1-3个OH基团取代的C1-C18烷氧基,C5-C12环烷氧基或C7-C15苯基烷氧基的G11是通过优选从下述醇中抽走碳键接的氢原子所形成的基团:2-甲基-2-丙醇(叔丁醇),2-丙醇,2,2-二甲基-1-丙醇,2-甲基-2-丁醇,乙醇,1-丙醇,1-丁醇,1-戊醇,1-己醇,1-壬醇,1-癸醇,1-十二烷醇,1-十八烷醇,2-丁醇,2-戊醇,2-乙基-1-己醇,环己醇,环辛醇,烯丙基醇,苯乙醇或1-苯基-1-乙醇;1,2-乙二醇,1,2-丙二醇,1,3-丙二醇,12-丁二醇,1,3-丁二醇,1,4-丁二醇,2,2-二甲基-1,3-丙二醇,1,2-环己二醇,1,3-环己二醇或1,4-环己二醇;甘油,1,1,1-三(羟甲基)甲烷,2-乙基-2-(羟甲基)-1,3-丙二醇,1,2,4-丁三醇或1,2,6-己烷三醇。
更优选地,G11是从2-甲基-2-丙醇或环己醇,1,4-丁二醇,2,2-二甲基-1,3-丙二醇,1,2-环己二醇,1,3-环己二醇或1,4-环己二醇形成的。最优选的羟基取代G11是2-羟基-2-甲基丙氧基。
几个G12基团的例子在下面给出。
如果G12是羧酸的一价基团,则它例如是乙酰基,己酰基,硬脂酰基,丙烯酰基,甲基丙烯酰基,苯甲酰基或β-(3,5-二-叔丁基-4-羟苯基)丙酰基。
如果G12是一价甲硅烷基,则它例如是下式的基团
-(CjH2j)-Si(Z’)2Z″,
其中j是是2-5范围内的整数,Z’和Z″彼此独立地是C1-C4烷基或C1-C4烷氧基。
如果G12是二羧酸的二价基团,则它例如是丙二酰基,琥珀酰基,戊二酰基,己二酰基,辛二酰基,癸二酰基,顺丁烯二酰基,衣康酰基,邻苯二甲酰基,二丁基丙二酰基,二苄基丙二酰基,丁基(3,5-二-叔丁基-4-羟基苄基)丙二酰基或双环庚烯二甲酰基或下式的基团
如果G12是三羧酸的三价基团,则它是例如1,2,4-苯三酰基,柠檬酰基或次氮基三乙酰基。
如果G12是四羧酸的四价基团,它是例如丁烷-1,2,3,4-四羧酸或苯均四酸的四价基团。
如果G12是二氨基甲酸的二价基团,则它是例如六亚甲基二氨基甲酰基或2,4-亚甲苯基二氨基甲酰基。
优选的是满足以下条件的通式(1a)的化合物:其中G和G1是氢,G11是氢或甲基,n1是2和G12是具有4-12个碳原子的脂族二羧酸的二酰基。
(b’)以下通式(1b)的化合物:
其中n2是数字1,2或3,G、G1和G11如在(a’)项中所定义,G13是氢,C1-C12烷基,C2-C5羟基烷基,C5-C7环烷基,C7-C8芳烷基,C1-C18链烷酰基,C3-C5链烯酰基,苯甲酰基或下式的基团
和如果n2是1,则G14是氢,C1-C18烷基,C3-C8链烯基,C5-C7环烷基,被羟基、氰基、烷氧基羰基或脲基取代的C1-C4烷基,或结构式-CONH-Z的基团,或G14是缩水甘油基,结构式-CH2-CH(OH)-Z或结构式-CONH-Z的基团,其中Z是氢、甲基或苯基或CH2-OZ14,而Z14是氢或C1-C18烷基;
如果n2是2,则G14是C2-C12亚烷基,C6-C12亚芳基,亚二甲苯基,-CH2-CH(OH)-CH2基团或-CH2-CH(OH)-CH2-O-D-O-基团,其中D是C2-C10亚烷基,C6-C16亚芳基,C6-C12亚环烷基,或,只要G13不是烷酰基、链烯酰基或苯甲酰基,那么G14能够另外是1-氧代-C2-C12亚烷基,脂肪族、环脂族或芳族二羧酸或二氨基甲酸的二价基团或另外是基团-CO-,
如果n2是3,则G14是基团
或,如果n2是1,则G13和G14一起能够是脂肪族,环脂族或芳族1,2-或1,3-二羧酸的二价基团。
对于基团G13,G14和D的一些例子在下面给出。
任何烷基取代基与以上对于(a’)的定义相同。
任何C5-C7环烷基取代基尤其是环己基。
C7-C8芳烷基G13特别是苯乙基或尤其苄基。
C2-C5羟基烷基G13尤其是2-羟乙基或2-羟丙基。
C1-C18链烷酰基G13例如是甲酰基,乙酰基,丙酰基,丁酰基,辛酰基,十二烷酰基,十六酰基,十八酰基,但优选是乙酰基,以及C3-C5链烯酰基G13,特别是丙烯酰基。
C2-C8链烯基G14是,例如,烯丙基,甲代烯丙基,2-丁烯基,2-戊烯基,2-己烯基或2-辛烯基。
作为羟基-,氰基-,烷氧基羰基-或脲基-取代的C1-C4烷基的G14能够是,例如,2-羟乙基,2-羟丙基,2-氰基乙基,甲氧基羰基甲基,2-乙氧基羰基乙基,2-氨基羰基丙基或2-(二甲基氨基羰基)乙基。
任何C2-C12亚烷基基团是,例如,亚乙基,亚丙基,2,2-二甲基亚丙基,四亚甲基,六亚甲基,八亚甲基,十亚甲基或十二亚甲基。
任何C6-C15亚芳基取代基是,例如,邻-,间-或对-亚苯基,1,4-亚萘基或4,4’-二亚苯基。
C6-C12亚环烷基特别是亚环己基。
作为1-氧代-C2-C12亚烷基的G14优选是以下基团
(c’)下式(1c)的化合物
其中n3是数字1或2,G、G1和G11与以上在(a’)项中的定义相同,以及如果n3是1,则G15和G’15独立地是C1-C12烷基,C2-C12链烯基,C7-C12芳烷基,或G15也是氢,或G15和G’15一起是C2-C8亚烷基,C5-C15亚链烯基,C2-C8羟基亚烷基或C4-C22酰氧基亚烷基,以及如果n3是2,则G15和G’15一起是(-CH2)2C(CH2-)2基团。
C2-C8亚烷基或C2-C8羟基亚烷基G15和G’15是,例如,亚乙基,1-甲基亚乙基,亚丙基,2-乙基亚丙基或2-乙基-2-羟基甲基亚丙基。
C4-C22酰氧基亚烷基G15和G’15是,例如,2-乙基-2-乙酰氧基甲基亚丙基。
(d’)结构式(1d-1),(1d-2)或(1d-3)的化合物,
其中n4是数字1或2,G、G1和G11与以上(a’)项中定义相同,G16是氢,C1-C12烷基,烯丙基,苄基,缩水甘油基或C2-C6烷氧基烷基,并且如果n4是1,则G17是氢,C1-C12烷基,C3-C5链烯基,C7-C9芳烷基,C5-C7环烷基,C2-C4羟基烷基,C2-C6烷氧基烷基,C6-C10芳基,缩水甘油基或结构式-(CH2)p-COO-Q或-(CH2)p-O-CO-Q的基团,其中p是1或2,和Q是C1-C4烷基或苯基,和
如果n4是2,则G17是C2-C12亚烷基,C4-C12亚链烯基,C6-C12亚芳基,通式-CH2-CH(OH)-CH2-O-D’-O-CH2-CH(OH)-CH2-的基团,其中D’是C2-C10亚烷基,C6-C15亚芳基或C6-C12亚环烷基,或通式-CH2CH(OD″)CH2-(OCH2-CH(OD″)CH2)2-的基团,其中D″是氢,C1-C18烷基,烯丙基,苄基,C2-C12链烷酰基或苯甲酰基,T1和T2彼此独立地是氢,C1-C18烷基或未被取代的或卤素-或C1-C4烷基取代的C6-C10芳基或C7-C9芳烷基,或
T1和T2与键接它们的该碳原子一起形成C5-C14环烷烃环。
任何C1-C12烷基取代基是,例如,甲基,乙基,正-丙基,正丁基,仲丁基,叔丁基,正己基,正辛基,2-乙基己基,正壬基,正癸基,正十一烷基或正十二烷基。
任何C1-C18烷基取代基能够是,例如,该上述的基团和另外,例如,正十三烷基,正十四烷基,正十六烷基或正十八烷基。
任何C2-C6烷氧基烷基取代基是,例如,甲氧基甲基,乙氧基甲基,丙氧基甲基,叔丁氧基甲基,乙氧基乙基,乙氧基丙基,正丁氧基乙基,叔丁氧基乙基,异丙氧基乙基或丙氧基丙基。
C3-C5链烯基G17是,例如,1-丙烯基,烯丙基,甲代烯丙基,2-丁烯基或2-戊烯基。
C7-C9芳烷基G17,T1和T2特别是苯乙基或尤其苄基。如果T1和T2与该碳原子一起形成环烷烃环,它能够是例如环戊烷,环己烷,环辛烷或环十二烷烃环。
C2-C4羟基烷基G17是,例如,2-羟乙基,2-羟丙基,2-羟丁基或4-羟丁基。
C6-C10芳基G17,T1和T2特别是苯基或α-或β-萘基,它是未被取代的或被卤素或C1-C4烷基取代。
C2-C12亚烷基G17是,例如,亚乙基,亚丙基,2,2-二甲基亚丙基,四亚甲基,六亚甲基,八亚甲基,十亚甲基或十二亚甲基。
C4-C12亚链烯基G17特别是2-亚丁烯基,2-亚戊烯基或3-亚己烯基。
C6-C12亚芳基G17是,例如,邻-,间-或对-亚苯基,1,4-亚萘基或4,4’-二亚苯基。
C2-C12链烷酰基D″是,例如,丙酰基,丁酰基,辛酰基,十二烷酰基,但优选乙酰基。
C2-C10亚烷基,C6-C15亚芳基或C6-C12亚环烷基D’具有例如在(b’)名义下给出的含意中的一个。
(e’)结构式(1e)的化合物
其中n5是数字1或2,以及G18是下式的基团
或
其中G和G11与(a’)中定义相同,并且G1和G2是氢,甲基或一起是取代基=O,
E是-O-或-ND″’-
A是C2-C6亚烷基或-(CH2)3-O-和
x1是数字0或1,
D″’是氢,C1-C12烷基,C2-C12亚烷基-N(DV)2,C2-C5羟基烷基或C5-C7环烷基,其中DV独立地是氢或丁基,
G19等同于G18或是基团-N(G21)(G22),-OG23,-N(H)(CH2OG23)或-N(CH2OG23)2中一个,
如果n5=1,则G20等同于G18或G19和,如果n5=2,则是-E-DIV-E-基团,其中DIV是C2-C8亚烷基或被1或2个-NG21-基团***的C2-C8亚烷基,
G21是氢,C1-C12烷基,环己基,苄基或C1-C4-羟烷基或下式的基团
或
G22是C1-C12烷基,环己基,苄基或C1-C4羟基烷基,和
G23是氢,C1-C12烷基或苯基,或G21和G22一起是C4-C5亚烷基或C4-C5氧杂亚烷基,例如-CH2CH2-O-CH2CH2-,或通式-CH2CH2-N(G11)-CH2CH2-的基团。
在通式(1e)中几个变量的一些例子在下面给出。
任何C1-C12烷基取代基是,例如,甲基,乙基,正-丙基,正丁基,仲丁基,叔丁基,正己基,正辛基,2-乙基己基,正壬基,正癸基,正十一烷基或正十二烷基。
任何羟烷基取代基是,例如,2-羟乙基,2-羟丙基,3-羟丙基,2-羟丁基或4-羟丁基。
任何C5-C7环烷基取代基是,例如,环戊基,环己基或环庚基。环己基是优选的。
C2-C6亚烷基A是,例如,亚乙基,亚丙基,2,2-二甲基亚丙基,四亚甲基或六亚甲基。
如果G21和G22一起是C4-C5亚烷基或氧杂亚烷基,则它们是例如四亚甲基,五亚甲基或3-氧杂五亚甲基。
(f’)下式(1f)的化合物
其中G11与(a’)中定义相同。
(g’)低聚或聚合物,它们的重复结构单元含有2,2,6,6-四烷基哌啶基,特别是含有此类基团的聚酯,聚醚,聚酰胺,聚胺,聚氨酯类,聚脲类,聚氨基三嗪,聚(甲基)丙烯酸酯,聚(甲基)丙烯酰胺和它们的共聚物。
来自这一类型的2,2,6,6-聚烷基哌啶化合物的例子是以下结构式的化合物。m1到m14是从2到大约200,优选2到100,例如2到50,2到40,3到40或4到10的数。
在下面所列的低聚物或聚合物化合物中使自由价饱和的端基的含意将取决于用于制备该化合物的方法。在该化合物的合成之后,端基也能够另外加以改性。
聚合物化合物的例子是:
1)结构式(1g)的化合物
其中G24,G25,G26,G27和G28彼此独立地是直接的键或C1-C10亚烷基,G11与(a’)中定义相同和m17是从1到50的数。
在结构式(1g)的化合物中,键接于>C=O基团的端基能够是例如:
和键接于氧的端基能够是例如
2)下式(2g)的化合物
其中指数m18是在1到15范围内;
R12是C2-C12亚烷基,C4-C12亚链烯基,C5-C7亚环烷基,C5-C7亚环烷基-二(C1-C4亚烷基),C1-C4亚烷基二(C5-C7亚环烷基),亚苯基二(C1-C4亚烷基)或被1,4-哌嗪二基、-O-或>N-X1***的C4-C12亚烷基,而X1是C1-C12酰基或(C1-C12烷氧基)羰基或具有以下给出的R14的意义中的一个,但氢除外;或R12通式(2g’)或(2g″)的基团;
X2是C1-C18烷基,未被取代或被1、2或3个C1-C4烷基取代的C5-C12环烷基;未被取代或被1、2或3个C1-C4烷基或C1-C4烷氧基取代的苯基;在苯基上未被取代或被1、2或3个C1-C4烷基取代的C7-C9苯基烷基;和
该基团X3彼此独立地是C2-C12亚烷基;
该基团A彼此独立地是-OR13,-N(R14)(R15)或通式(2g″’)的基团;
R13,R14和R15,它们可以相同或不同,是氢,C1-C18烷基,未取代或被1、2或3个C1-C4烷基取代的C5-C12环烷基;C3-C18链烯基,未取代或被1、2或3个C1-C4烷基或C1-C4烷氧基取代的苯基;未取代或在苯基上被1、2或3个C1-C4烷基取代的C7-C9苯基烷基;四氢化糠基或在2、3或4位上被-OH、C1-C8烷氧基、二(C1-C4烷基)氨基或下式(2gIV)的基团取代的C2-C4烷基;
而Y是-O-,-CH2-,-CH2CH2-或>N-CH3,
或-N(R14)(R15)另外是通式(2gIV)的基团;
X是-O-或>N-R16;
R16是氢,C1-C18烷基,C3-C16链烯基,未取代或被1、2或3个C1-C4烷基取代的C5-C12环烷基;未取代或在苯基上被1、2或3个C1-C4烷基取代的C7-C9苯基烷基;四氢化糠基,通式(2gV)的基团,
或在2、3或4位上被-OH取代的C2-C4烷基,C1-C8烷氧基,二(C1-C4烷基)氨基或通式(2gIV)的基团;
R11具有对于R16所给出的定义中的一个;和
该基团B彼此独立地具有对于A给出的定义中的一个。
3)下式(3g)的化合物
其中G11与(a’)中定义相同,G29和G32彼此独立地是直接的键或-N(X1)-CO-X2-CO-N(X3)-基团,其中X1和X3彼此独立地是氢,C1-C8烷基,C5-C13环烷基,苯基,C7-C9苯基烷基或下式的基团
和X2是直接的键或C1-C4亚烷基,G30、G31、G34和G35彼此独立地是氢,C1-C30烷基,C5-C12环烷基或苯基,G33是氢,C1-C30烷基,C5-C12环烷基,C7-C9苯基烷基,苯基或通式(3g)的基团,并且m19是1到50的数。
在通式(3g)的化合物中,键接于2,5-二氧代吡咯烷环的端基能够是例如氢,和键接于-C(G34)(G35)-基团的端基能够是例如:
4)可通过由通式(4g)的聚胺与氰尿酰氯反应所获得的中间产物进一步与通式(4g’)的化合物进行反应获得的产物:
其中m’20,m″20和m″’20彼此独立地是2-12的数,
G36是氢,C1-C12烷基,C5-C12环烷基,苯基或C7-C9苯基烷基,和
G11与(a’)中定义相同。
一般而言,上面的反应产物能够以例如下面3个结构式的化合物为代表。它也能够是这三种化合物的混合物形式:
5)下式(5g)的化合物
其中G11与(a’)中定义相同,G37是C1-C10烷基,C5-C12环烷基,C1-C4烷基取代的C5-C12环烷基,苯基或C1-C10烷基取代的苯基,G38是C3-C10亚烷基和m21是1到50的数。
在通式(5g)的化合物中,键接于硅原子上的端基能够是例如,(G37)3Si-O-,和键接于氧的端基能够是例如,-Si(G37)3。
通式(5g)的化合物也能够是环状化合物形式,如果m21是3到10的数的话,即在结构式中示出的自由价形成了直接的键。
6)下式(6g)的化合物
其中E是在(e’)中定义的-O-或-ND″’-,T3是亚乙基或1,2-亚丙基,是从α-烯烃与烷基丙烯酸酯或甲基丙烯酸酯的共聚物,优选乙烯和丙烯酸乙酯的共聚物衍生的重复结构单元,和其中k是2到100。
7)下式的(7g)的化合物
其中m是1-1 00;
G50是具有1-18个碳原子的直链或支链亚烷基,具有5-8个碳原子的亚环烷基,具有5-8个碳原子的亚环链烯基,具有3-18个碳原子的亚链烯基,被苯基或进一步被1个或2个具有1-4个碳原子的烷基取代的苯基所取代的具有1-4碳原子的直链或支链亚烷基,限制条件是,在通式(7g)中连续的位阻胺结构部分能够以头-头或头-尾方式取向;
T4是氢或
G55是具有1-18个碳原子的直链或支链亚烷基,具有5-8个碳原子的亚环烷基或亚环链烯基,亚苯基或具有2-18个碳原子的-NH-亚烷基-NH-,包括5-氨基-1-氨甲基-1,3,3-三甲基环己烷和-NH-亚二甲苯基-NH-;
T5是C1-C4烷基;
或
在以上所示的低聚物和聚合物化合物中,烷基的例子是甲基,乙基,丙基,异丙基,正丁基,仲丁基,异丁基,叔丁基,2-乙基丁基,正戊基,异戊基,1-甲基戊基,1,3-二甲基丁基,正己基,1-甲基己基,正庚基,异庚基,1,1,3,3-四甲基丁基,1-甲基庚基,3-甲基庚基,正辛基,2-乙基-己基,1,1,3-三甲基己基,1,1,3,3-四甲基戊基,壬基,癸基,十一烷基,1-甲基十一烷基,十二烷基,1,1,3,3,5,5-六甲基己基,十三烷基,十四烷基,十五烷基,十六烷基,十七烷基,十八烷基,二十烷基和二十二烷基;
环烷基的例子是环戊基,环己基,环庚基和环辛基;C7-C9苯基烷基的例子是苄基;和
亚烷基的例子是亚乙基,亚丙基,三亚甲基,四亚甲基,五亚甲基,2,2-二甲基三亚甲基,六亚甲基,三甲基六亚甲基,八亚甲基和十亚甲基。
(h’)下式(1h)的化合物
其中n6是数字1或2,G和G11与(a’)中定义相同,以及G14与(b’)中定义相同,但是G14不能是-CONH-Z和-CH2-CH(OH)-CH2-O-D-O-。
(i’)下式(1i)的化合物
其中该基团G39彼此独立地是通式(1i-1)的基团:
其中G40是C1-C12烷基或C5-C12环烷基,G41是C2-C12亚烷基和G42与以上G11的定义相同。
烷基例如是C1-C4烷基,特别是甲基,乙基,丙基或丁基。
环烷基优选是环己基。
亚烷基例如是亚乙基,亚丙基,三亚甲基,四亚甲基,五亚甲基,2,2-二甲基三亚甲基或六亚甲基。
链烯基优选是烯丙基。
苯基烷基优选是苄基。
酰基优选是乙酰基。
(j’)下式(1j)的化合物
其中G,G11如以上所定义和
当n7是1时,T7是氢,C1-C12烷基,C3-C5链烯基,C7-C9芳烷基,C5-C7环烷基,C2-C4羟基烷基,C2-C6烷氧基烷基,C6-C10芳基,缩水甘油基,通式-(CH2)t-COO-Q或通式-(CH2)t-O-CO-Q的基团,其中t是1或2,和Q是C1-C4烷基或苯基;或
当n7是2时,T7是C2-C12亚烷基,C6-C12亚芳基,基团-CH2CH(OH)-CH2-O-X-O-CH2-CH(OH)-CH2-,其中X是C2-C10亚烷基,C6-C15亚芳基或C6-C12亚环烷基,或基团-CH2CH(OZ’)CH2-(OCH2-CH(OZ’)CH2)2-,其中Z’是氢,C1-C18烷基,烯丙基,苄基,C2-C12链烷酰基或苯甲酰基。
(k’)下式(1k)的化合物
其中G,G11如以上所定义。
(I’)下式(1l)的化合物
其中G,G11如以上所定义。
(m’)下式(1m)的化合物
其中G如以上所定义,n8是1,2或3,
如果n8是1,则G51是-G50-O-CO-G56;G52是-O-CO-G56;和G53是氢;其中G56具有1-18个碳原子的烷基或-NH-烷基或具有5-8个碳原子的-NH-环烷基;
如果n8是2,G51是具有1-18个碳原子的亚烷基,具有3-18个碳原子的羟基亚烷基,具有5-8个碳原子的亚环烷基,具有5-8个碳原子的亚环链烯基或羟基亚环烷基,具有3-18个碳原子的亚链烯基,或具有1-4个碳原子的直链或支链亚烷基或具有2-4个碳原子的羟基亚烷基,它们两者被苯基或被进一步被1个或2个具有1-4个碳原子的烷基取代的苯基所取代;或G51是脂肪族,环脂族,芳脂族或芳族二羧酸或二氨基甲酸的二价酰基,优选具有2-18个碳原子的脂族二羧酸,具有8-14个碳原子的环脂族或芳族二羧酸的酰基,
如果n6是3,G51是具有1-18个碳原子的链烷烃三基,具有3-18个碳原子的羟基链烷烃三基,具有5-8个碳原子的环烷烃三基,具有5-8个碳原子的环链烯烃三基,具有3-8个碳原子的链烯烃三基,被苯基或被进一步被1个或2个具有1-4个碳原子的烷基取代的苯基所取代的具有1-4个碳原子的直链或支链链烷烃三基;
如果n6是2或3,
G52是-O-G12;-N(G13)G14;-O-G15;-COO-T7;或下式的基团
和
G53是氢,或如果G52是-O-G15,则G53是O-G’15;或G52和G53一起是=O;或下式的基团
其中,如果n1是1,则G11和G12与(a’)中定义相同;如果n2是1,则G13和G14与(b’)中定义相同;如果n3是1,则G15和G’15与(c’)中定义相同;G18,G19,A,E,DIV,x1与(e’)中定义相同;如果n7是1,则T7与(j’)中定义相同;
如果n1是2,则G54与(a’)的G12定义相同;如果n2是2,则G55与(b’)的G14定义相同;如果n7是2,则G56与(j’)的T7定义相同。
特别在技术上重要的是羟基烃氧基胺类型的位阻胺光稳定剂,其中E1优选是C1-C18烷基,C5-C12环烷基或C7-C15芳烷基,它们当中的每一个在脂肪族部分中被1-3个OH基团,尤其被1个OH基团取代。
因此,本发明还涉及被稳定化后可抵抗光和风化的有害影响的阻燃性组合物,它包括
a)聚烯烃,和
b)选自以下的阻燃剂
b1)蜜胺型阻燃剂和/或聚磷酸铵,
b2)双-(六氯环戊二烯基并)环辛烷,
b3)三-(2,3-二溴丙基)-异氰脲酸酯,
b4)亚乙基-双-四溴邻苯二甲酰亚胺;
和
c)羟基烃氧基胺类型的位阻胺光稳定剂。
此外,本发明涉及赋予热塑性聚合物以光稳定性和阻燃性的方法,该方法包括向该聚合物中加入阻燃剂三-(2,3-二溴丙基)-异氰脲酸酯和烃氧基胺或羟基烃氧基胺类型的位阻胺光稳定剂的结合物。包括以下组分的阻燃性和光稳定的组合物:
a)聚烯烃,
b)作为阻燃剂的三-(2,3-二溴丙基)-异氰脲酸酯和
c)烃氧基胺或羟基烃氧基胺类型的位阻胺光稳定剂是本发明的另一优选的主题。
在该新型方法和新型组合物中优选的组分a和c和它们的量是如以上所述。
本发明的组分b和c以及任选的其它组分可通过传统技术,在该组合物制造成型制品之前的任何方便阶段中,容易地引入到聚合物中。例如,该添加剂可与干燥粉形式的聚合物混合,或添加剂的悬浮液或乳液可以与聚合物的溶液,悬浮液,或乳液混合。该添加剂可单独或彼此混合后加入到组分(a)中。如果需要,各组分能够在被引入到需要稳定的材料中之前相互以熔体形式混合(熔融掺混)。组分b和/或c和任选的其它添加剂可以,例如在模塑之前或之后引入,或也可通过将溶解或分散的稳定剂混合物施加到需要稳定的材料中来引入,随后有或没有溶剂的蒸发。组分b和/或c的添加剂以及其它添加剂也能够以母料形式加入到需要稳定的材料中,该母料含有例如大约2.5wt%到大约25wt%的浓度的这些组分;在此类操作中,该聚合物能够以粉末、粒料、溶液、悬浮液的形式或胶乳形式使用。
该引入能够在成形操作之前或过程中进行,或通过将已溶解或分散的化合物施加到聚合物,有或没有随后的溶剂的蒸发来进行。对于弹性体,这些也能够作为胶乳被稳定。将本发明的稳定剂引入到聚合物的另一种可能性是在相应单体的聚合反应之前、过程中或直接在该反应之后添加它们。对于在聚合反应之前或过程中的添加,本发明的稳定剂也能够用作聚合物的链长的调节剂(链终止剂)。
本发明的组分b和c能够审慎地由下列方法引入:
-作为乳液或分散体(例如加入到胶乳或乳液聚合物中),
-在附加组分或聚合物混合物的混合过程中作为干燥混合物加入,
-直接引入到加工装置(例如挤出机,密闭式混合机等)中,
-作为溶液或熔体。
本发明的组分b和c的添加剂组合可用于许多应用,尤其户外应用,包括下面这些:
热塑性烯烃(TPO),例如可涂漆的热塑性聚烯烃
聚丙烯模塑制品
聚乙烯薄膜
具有溴化阻燃剂的模塑聚丙烯
具有溴化阻燃剂的模塑热塑性聚烯烃
有溴化阻燃剂的聚乙烯薄膜
有助稳定剂的热塑性弹性体
油脂填充的电线和电缆绝缘体
在塑料基材上的涂料
聚烯烃罐或含有化学药品的容器
有防雾剂的聚烯烃薄膜
有IR生热填料如水滑石例如DHT4A的聚烯烃薄膜
有抗静电剂的聚烯烃薄膜
阻燃性的模塑聚丙烯制品
阻燃性的模塑加工的热塑性聚烯烃
阻燃性聚乙烯薄膜
用于层压到塑料基材上的预形成膜
电子器件
储运用的容器,盒子,箱
汽车应用例如仪表板,垫板
家具例如运动场座位,公共场合的座位
屋顶薄板
屋顶膜
地板材料
衬材
异型材,尤其窗和门异型材
地膜。
含有这里所述的稳定剂的材料能够用于生产模制品,挤出制品,转模塑制品,注射模制品,吹塑模制品,单-和多层薄膜,挤塑型材,表面涂层等等。
本发明的稳定化组合物还可任选含有各种常规的添加剂,其量优选是组分(a)的0.01-10wt%,更优选大约0.025-大约2wt%,和尤其约0.1-大约1wt%,如下面列出的材料或这些材料的混合物。
1、抗氧化剂
1.1、
烷基化一元酚类,例如,2,6-二叔丁基-4-甲基苯酚,2-叔丁基-4,6-二甲基苯酚,2,6-二叔丁基-4-乙基苯酚,2,6-二叔丁基-4-正丁基苯酚,2,6-二叔丁基-4-异丁基苯酚,2,6-二环戊基-4-甲基苯酚,2-(α-甲基环己基)-4,6-二甲基苯酚,2,6-双十八烷基-4-甲基苯酚,2,4,6-三环己基苯酚,2,6-二叔丁基-4-甲氧基甲基苯酚;壬基苯酚类,它是线性的或在支链上支化,例如2,6-二壬基-4-甲基苯酚,2,4-二甲基-6-(1′-甲基十一烷-1′-基)苯酚,2,4-二甲基-6-(1′-甲基十七烷-1′-基)苯酚,2,4-二甲基-6-(1′-甲基十三烷-1′-基)苯酚;以及它们的混合物。
1.2、烷基硫代甲基酚类,例如2,4-二-辛基硫代甲基-6-叔丁基苯酚,2,4-二辛基硫代甲基-6-甲基苯酚,2,4-二辛基硫代甲基-6-乙基苯酚,2,6-双十二烷基硫代甲基-4-壬基苯酚。
1.3、氢醌类或烷基化氢醌类,例如,2,6-二叔丁基-4-甲氧基苯酚,2,5-二叔丁基氢醌,2,5-二叔戊基氢醌,2,6-二苯基-4-十八烷氧基苯酚,2,6-二叔丁基氢醌,2,5-二叔丁基-4-羟基苯甲醚,3,5-二叔丁基-4-羟基苯甲醚,硬脂酸3,5-二叔丁基-4-羟基苯基酯,己二酸双(3,5-二叔丁基-4-羟基苯基)酯。
1.4、生育酚,例如α-生育酚,β-生育酚,γ-生育酚,δ-生育酚和它们的混合物(维生素E)。
1.5、羟基化硫代二苯基醚类,例如,2,2′-硫代双(6-叔丁基-4-甲基苯酚),2,2′-硫代双(4-辛基苯酚),4,4′-硫代双(6-叔丁基-3-甲基苯酚),4,4′-硫代双(6-叔丁基-2-甲基苯酚),4,4′-硫代双(3,6-二仲戊基苯酚),4,4’-双(2,6-二甲基-4-羟基苯基)二硫醚。
1.6、亚烷基双酚类,例如,2,2′-亚甲基双(6-叔丁基-4-甲基苯酚),2,2′-亚甲基双(6-叔丁基-4-乙基苯酚),2,2′-亚甲基双[4-甲基-6-(α-甲基环己基)苯酚],2,2′-亚甲基双(4-甲基-6-环己基苯酚),2,2′-亚甲基双(6-壬基-4-甲基苯酚),2,2′-亚甲基双(4,6-二叔丁基苯酚),2,2′-亚乙基双(4,6-二叔丁基苯酚),2,2′-亚乙基双(6-叔丁基-4-异丁基苯酚),2,2′-亚甲基双[6-(α-甲基苄基)-4-壬基苯酚],2,2′-亚甲基双[6-(α,α-二甲基苄基)-4-壬基苯酚],4,4′-亚甲基双(2,6-二叔丁基苯酚),4,4′-亚甲基双(6-叔丁基-2-甲基苯酚),1,1′-双(5-叔丁基-4-羟基-2-甲基苯基)丁烷,2,6-双(3-叔丁基-5-甲基-2-羟基苄基)-4-甲基苯酚,1,1,3-三(5-叔丁基-4-羟基-2-甲基苯基)丁烷,1,1-双(5-叔丁基-4-羟基-2-甲基苯基)-3-正十二烷基巯基丁烷,双[3,3-双(3′-叔丁基-4′-羟基苯基)丁酸]乙二醇酯,双(3-叔丁基-4-羟基-5-甲基-苯基)二环戊二烯,对苯二甲酸双[2-(3′-叔丁基-2′-羟基-5 ′-甲基苄基)-6-叔丁基-4-甲基苯基]酯,1,1-双-(3,5-二甲基-2-羟基苯基)丁烷,2,2-双-(3,5-二叔丁基-4-羟基苯基)丙烷,2,2-双-(5-叔丁基-4-羟基-2-甲基苯基)-4-正十二烷基巯基丁烷,1,1,5,5-四-(5-叔丁基-4-羟基-2-甲基苯基)戊烷。
1.7.0-,N-和S-苄基化合物类,例如3,5,3′,5′-四叔丁基-4,4′-二羟基二苄基醚,4-羟基-3,5-二甲基苄基巯基乙酸十八烷基酯,4-羟基-3,5-二叔丁基苄基巯基乙酸十三烷基酯,三(3,5-二叔丁基-4-羟基苄基)胺,二硫代对苯二甲酸双(4-叔丁基-3-羟基-2,6-二甲基苄基)酯,双(3,5-二叔丁基-4-羟基-苄基)硫醚,3,5-二叔丁基-4-羟基苄基巯基乙酸异辛基酯。
1.8、羟苄基化丙二酸酯类,例如,2,2-双-(3,5-二叔丁基-2-羟基苄基)丙二酸二(十八烷基)酯,2-(3-叔丁基-4-羟基-5-甲基苄基)丙二酸二(十八烷基)酯,2,2-双(3,5-二叔丁基-4-羟基苄基)丙二酸二(十二烷基巯基乙基)酯,2,2-双(3,5-二叔丁基-4-羟基苄基)丙二酸双[4-(1,1,3,3-四甲基丁基)苯基]酯。
1.9、芳族羟苄基化合物类,例如1,3,5-三(3,5-二叔丁基-4-羟基苄基)-2,4,6-三甲基苯,1,4-双(3,5-二叔丁基-4-羟基苄基)-2,3,5,6-四甲基苯,2,4,6-三(3,5-二叔丁基-4-羟基苄基)苯酚。
1.10、三嗪化合物类,例如2,4-双(辛基巯基)-6-(3,5-二叔丁基-4-羟基苯胺基)-1,3,5-三嗪,2-辛基巯基-4,6-双(3,5-二叔丁基-4-羟基苯胺基)-1,3,5-三嗪,2-辛基巯基-4,6-双(3,5-二叔丁基-4-羟基苯氧基)-1,3,5-三嗪,2,4,6-三(3,5-二叔丁基-4-羟基苯氧基)-1,2,3-三嗪,1,3,5-三(3,5-二叔丁基-4-羟基苄基)异氰脲酸酯,1,3,5-三(4-叔丁基-3-羟基-2,6-二甲基苄基)-异氰脲酸酯,2,4,6-三(3,5-二叔丁基-4-羟基苯基乙基)-1,3,5-三嗪,1,3,5-三(3,5-二叔丁基-4-羟基苯基丙酰基)-六氢-1,3,5-三嗪,1,3,5-三(3,5-二环己基-4-羟基苄基)异氰脲酸酯。
1.11、苄基膦酸酯类,例如2,5-二叔丁基-4-羟基苄基膦酸二甲酯,3,5-二叔丁基-4-羟基苄基膦酸二乙酯,3,5-二叔丁基-4-羟基苄基膦酸二(十八烷基)酯,5-叔丁基-4-羟基-3-甲基苄基膦酸二(十八烷基)酯,3,5-二叔丁基-4-羟基苄基膦酸的单乙酯的钙盐。
1.12、酰基氨基酚类,例如4-羟基月桂酰苯胺,4-羟基硬脂酰苯胺,N-(3,5-二叔丁基-4-羟基苯基)氨基甲酸辛酯。
1.13、β-(3,5-二叔丁基-4-羟基苯基)丙酸的酯类,构成酯基的是单羟基或多羟基醇类,例如甲醇,乙醇,正辛醇,异辛醇,十八烷醇,1,6-己二醇,1,9-壬二醇,乙二醇,1,2-丙二醇,新戊二醇,硫代二甘醇,二甘醇,三甘醇,季戊四醇,异氰脲酸三(羟基乙基)酯,N,N′-双(羟乙基)草酰胺,3-硫代十一烷醇,3-硫代十五烷醇,三甲基己二醇,三羟甲基丙烷,4-羟甲基-1-磷杂-2,6,7-三氧杂双环[2.2.2]辛烷。
1.14、β-(5-叔丁基-4-羟基-3-甲基苯基)丙酸的酯类,构成酯基的是单羟基或多羟基醇类,例如甲醇,乙醇,正辛醇,异辛醇,十八烷醇,1,6-己二醇,1,9-壬二醇,乙二醇,1,2-丙二醇,新戊二醇,硫代二甘醇,二甘醇,三甘醇,季戊四醇,异氰脲酸三(羟基乙基)酯,N,N′-双(羟乙基)草酰胺,3-硫代十一烷醇,3-硫代十五烷醇,三甲基己二醇,三羟甲基丙烷,4-羟甲基-1-磷杂-2,6,7-三氧杂双环[2.2.2]辛烷;3,9-双[2-{3-(3-叔丁基-4-羟基-5-甲基苯基)丙酰氧基}-1,1-二甲基乙基]-2,4,8,10-四氧杂螺[5.5]十一烷。
1.15、β-(3,5-二环己基-4-羟基苯基)丙酸的酯类,构成酯基的是单羟基或多羟基醇类,例如甲醇,乙醇,辛醇,十八烷醇,1,6-己二醇,1,9-壬二醇,乙二醇,1,2-丙二醇,新戊二醇,硫代二甘醇,二甘醇,三甘醇,季戊四醇,异氰脲酸三(羟基乙基)酯,N,N′-双(羟乙基)草酰胺,3-硫代十一烷醇,3-硫代十五烷醇,三甲基己二醇,三羟甲基丙烷,4-羟甲基-1-磷杂-2,6,7-三氧杂双环[2.2.2]辛烷。
1.16、3,5-二叔丁基-4-羟基苯基乙酸的酯类,构成酯基的是单羟基或多羟基醇类,例如甲醇,乙醇,辛醇,十八烷醇,1,6-己二醇,1,9-壬二醇,乙二醇,1,2-丙二醇,新戊二醇,硫代二甘醇,二甘醇,三甘醇,季戊四醇,异氰脲酸三(羟基乙基)酯,N,N′-双(羟乙基)草酰胺,3-硫代十一烷醇,3-硫代十五烷醇,三甲基己二醇,三羟甲基丙烷,4-羟甲基-1-磷杂-2,6,7-三氧杂双环[2.2.2]辛烷。
1.17、β-(3,5-二叔丁基-4-羟基苯基)丙酸的酰胺类,例如N,N′-双(3,5-二叔丁基-4-羟基苯基丙酰基)六亚甲基二胺,N,N′-双(3,5-二叔丁基-4-羟基苯基丙酰基)三亚甲基二胺,N,N′-双(3,5-二叔丁基-4-羟基苯基丙酰基)肼,N,N’-双[2-(3-[3,5-二叔丁基-4-羟基苯基]丙酰氧基)乙基]草酰胺(NaugardXL-1,由Uniroyal提供)。
1.18、抗坏血酸(维生素C)
1.19、胺类抗氧化剂,例如N,N′-二异丙基-对-亚苯基二胺,N,N′-二仲丁基-对-亚苯基二胺,N,N′-双(1,4-二甲基戊基)-对-亚苯基二胺,N,N′-双(1-乙基-3-甲基戊基)-对-亚苯基二胺,N,N’-双(1-甲基庚基)-对亚苯基二胺,N,N’-二环己基-对亚苯基二胺,N,N′-二苯基-对-亚苯基二胺,N,N′-双(2-萘基)-对-亚苯基二胺,N-异丙基-N′-苯基-对-亚苯基二胺,N-(1,3-二甲基丁基)-N′-苯基-对-亚苯基二胺,N-(1-甲基庚基)-N′-苯基-对-亚苯基二胺,N-环己基-N′-苯基-对-亚苯基二胺,4-(对甲苯氨磺酰基)二苯胺,N,N′-二甲基-N,N′-二仲丁基-对亚苯基二胺,二苯胺,N-烯丙基二苯胺,4-异丙氧基-二苯胺,N-苯基-1-萘基胺,N-(4-叔辛基苯基)-1-萘基胺,N-苯基-2-萘基胺,辛基化二苯胺(例如p,p′-二叔辛基二苯胺),4-正丁基氨基苯酚,4-丁酰氨基苯酚,4-壬酰氨基苯酚,4-十二酰氨基苯酚,4-十八酰氨基苯酚,双(4-甲氧基苯基)胺,2,6-二叔丁基-4-二甲氨基甲基苯酚,2,4′-二氨基二苯基甲烷,4,4′-二氨基二苯基甲烷,N,N,N′,N′-四甲基-4,4′-二氨基二苯基甲烷,1,2-双[(2-甲基苯基)氨基]乙烷,1,2-双(苯基氨基)丙烷,(邻甲苯基)双胍,双[4-(1′,3′-二甲基丁基)苯基]胺,叔辛基化N-苯基-1-萘基胺,单和二烷基化叔丁基/叔辛基二苯基胺类的混合物,单和二烷基化壬基二苯基胺类的混合物,单和二烷基化十二烷基二苯基胺类的混合物,单和二烷基化异丙基/异己基二苯基胺类的混合物,单和二烷基化叔丁基二苯基胺类的混合物,2,3-二氢-3,3-二甲基-4H-1,4-苯并噻嗪,吩噻嗪,单和二烷基化叔丁基/叔辛基吩噻嗪的混合物,单和二烷基化叔辛基吩噻嗪的混合物,N-烯丙基吩噻嗪,N,N,N′,N′-四苯基-1,4-二氨基丁-2-烯,N,N-双(2,2,6,6-四甲基-哌啶-4-基-六亚甲基二胺,双(2,2,6,6-四甲基-哌啶-4-基)癸二酸酯,2,2,6,6-四甲基哌啶-4-酮,2,2,6,6-四甲基哌啶-4-醇。
2.UV吸收剂和光稳定剂
2.1、
2-(2′-羟基苯基)苯并***类,例如2-(2′-羟基-5′-甲基苯基)苯并***,2-(3′,5′-二叔丁基-2′-羟基苯基)苯并***,2-(5′-叔丁基-2′-羟基苯基)苯并***,2-(2′-羟基)-5′-(1,1,3,3-四甲基丁基)苯基)苯并***,2-(3′,5′-二叔丁基-2 ′-羟基苯基)-5-氯-苯并***,2-(3′-叔丁基-2′-羟基-5′-甲基苯基)-5-氯-苯并***,2-(3′-仲丁基-5′-叔丁基-2′-羟基苯基)苯并***,2-(2′-羟基-4′-辛氧基苯基)苯并***,2-(3′,5′-二叔戊基-2′-羟基苯基)苯并***,2-(3′,5′-双-(α,α-二甲基苄基)-2′-羟基苯基)苯并***,2-(3′-叔丁基-2′-羟基-5′-(2-辛氧基羰基乙基)苯基)-5-氯-苯并***,2-(3′-叔丁基-5′-[2-(2-乙基己氧基)-羰基乙基]-2′-羟基苯基)-5-氯-苯并***,2-(3′-叔丁基-2′-羟基-5′-(2-甲氧基羰基乙基)苯基)-5-氯-苯并***,2-(3′-叔丁基-2′-羟基-5′-(2-甲氧基羰基乙基)苯基)苯并***,2-(3′-叔丁基-2′-羟基-5′-(2-辛氧基羰基乙基)苯基)苯并***,2-(3′-叔丁基-5′-[2-(2-乙基己氧基)羰基乙基]-2′-羟基苯基)苯并***,2-(3′-十二烷基-2′-羟基-5′-甲基苯基)苯并***,和2-(3′-叔丁基-2′-羟基-5′-(2-异辛氧基羰基乙基)苯基苯并***的混合物,2,2′-亚甲基-双[4-(1,1,3,3-四甲基丁基)-6-苯并***-2-基苯酚];2-[3′-叔丁基-5′-(2-甲氧基羰基乙基)-2′-羟基苯基]-2H-苯并***与聚乙二醇300的酯基转移产物;[R-CH2CH2-COO-CH2CH2-]2-其中R=3′-叔丁基-4′-羟基-5′-2H-苯并***-2-基苯基,2-[2’-羟基-3’-(α,α-二甲基苄基)-5’-(1,1,3,3-四甲基丁基)苯基]苯并***;2-[2’-羟基-3’-(1,1,3,3-四甲基丁基)-5’-(α,α-二甲基苄基)苯基]苯并***。
2.2、2-羟基二苯甲酮类,例如4-羟基,4-甲氧基,4-辛氧基,4-癸氧基,4-十二烷氧基,4-苄氧基,4,2′,4′-三羟基和2′-羟基-4,4′-二甲氧基衍生物。
2.3、取代的和未取代的苯甲酸的酯类,例如水杨酸4-叔丁基-苯基酯,水杨酸苯酯,水杨酸辛基苯酯,二苯甲酰基间苯二酚,双(4-叔丁基苯甲酰基)间苯二酚,苯甲酰基间苯二酚,3,5-二叔丁基-4-羟基苯甲酸2,4-二叔丁基苯基酯,3,5-二叔丁基-4-羟基苯甲酸十六烷基酯,3,5-二叔丁基-4-羟基苯甲酸十八烷基酯,3,5-二叔丁基-4-羟基苯甲酸2-甲基-4,6-二叔丁基苯基酯。
2.4、丙烯酸酯类,例如α-氰基-β,β-二苯基丙烯酸乙酯,α-氰基-β,β-二苯基丙烯酸异辛酯,α-甲酯基肉桂酸甲酯,α-氰基-β-甲基-对甲氧基肉桂酸甲酯,α-氰基-β-甲基-对甲氧基肉桂酸丁酯,α-甲酯基-对甲氧基肉桂酸甲酯和N-(β-甲酯基-β-氰基乙烯基)-2-甲基二氢吲哚。
2.5、镍化合物类,例如2,2′-硫代-双-[4-(1,1,3,3-四甲基-丁基)苯酚]的镍配合物,如1∶1或1∶2配合比,有或没有附加的配位体如正丁基胺,三乙醇胺或N-环己基二乙醇胺,二丁基二硫代氨基甲酸镍,4-羟基-3,5-二叔丁基苄基膦酸的单烷基酯(例如甲酯或乙酯)类的镍盐,酮肟例如2-羟基-4-甲基苯基十一烷基酮肟的镍配合物类,1-苯基-4-月桂酰基-5-羟基吡唑的镍配合物,有或没有附加的配位体。
2.6、普通的空间位阻胺,例如癸二酸双(2,2,6,6-四甲基-4-哌啶基)酯,琥珀酸双(2,2,6,6-四甲基-4-哌啶基)酯,癸二酸双(1,2,2,6,6-五甲基-4-哌啶基)酯,双(1,2,2,6,6-五甲基-4-哌啶基)正丁基-3,5-二叔丁基-4-羟基苄基丙二酸酯,1-(2-羟乙基)-2,2,6,6-四甲基-4-羟基哌啶和琥珀酸的缩合物,N,N′-双(2,2,6,6-四甲基-4-哌啶基)六亚甲基二胺和4-叔辛基氨基-2,6-二氯-1,3,5-三嗪的线性或环状缩合物,次氮基三乙酸三(2,2,6,6-四甲基-4-哌啶基)酯,1,2,3,4-丁烷四羧酸四(2,2,6,6-四甲基-4-哌啶基)酯,1,1′-(1,2-亚乙基)双(3,3,5,5-四甲基哌嗪酮),4-苯甲酰基-2,2,6,6-四甲基哌啶,4-硬脂酰氧基-2,2,6,6-四甲基哌啶,2-正丁基-2-(2-羟基-3,5-二叔丁基苄基)丙二酸双(1,2,2,6,6-五甲基哌啶基)酯,3-正辛基-7,7,9,9-四甲基-1,3,8-三氮杂螺[4.5]癸烷-2,4-二酮,N,N′-双-(2,2,6,6-四甲基-4-哌啶基)六亚甲基二胺和4-吗啉代-2,6-二氯-1,3,5-三嗪的线性或环状缩合物,2-氯-4,6-双(4-正丁基氨基-2,2,6,6-四甲基哌啶基)-1,3,5-三嗪和1,2-双(3-氨基丙基氨基)乙烷的缩合物,2-氯-4,6-二(4-正丁基氨基-1,2,2,6,6-五甲基哌啶基)-1,3,5-三嗪和1,2-双(3-氨基丙基氨基)乙烷的缩合物,8-乙酰基-3-十二烷基-7,7,9,9-四甲基-1,3,8-三氮杂螺[4.5]癸烷-2,4-二酮,3-十二烷基-1-(2,2,6,6-四甲基-4-哌啶基)吡咯烷-2,5-二酮,3-十二烷基-1-(1,2,2,6,6-五甲基-4-哌啶基)吡咯烷-2,5-二酮,5-(2-乙基己酰基)-氧基甲基-3,3,5-三甲基-2-吗啉酮,1,3,5-三(N-环己基-N-(2,2,6,6-四甲基哌嗪-3-酮-4-基)氨基)-s-三嗪,1,3,5-三(N-环己基-N-(1,2,2,6,6-五甲基哌嗪-3-酮-4-基)氨基)-s-三嗪,4-十六烷氧基-和4-硬脂酰氧基-2,2,6,6-四甲基哌啶的混合物,N,N′-双(2,2,6,6-四甲基-4-哌啶基)六亚甲基二胺和4-环己基氨基-2,6-二氯-1,3,5-三嗪的缩合物,1,2-双(3-氨基-丙基氨基)乙烷和2,4,6-三氯-1,3,5-三嗪的缩合物,以及4-丁基氨基-2,2,6,6-四甲基哌啶(CAS登记号[136504-96-6]);1,6-己烷二胺和2,4,6-三氯-1,3,5-三嗪以及N,N-二丁基胺和4-丁基氨基-2,2,6,6-四甲基哌啶(CAS登记号[192268-64-7]);N-(2,2,6,6-四甲基-4-哌啶基)正十二烷基琥珀酰亚胺,N-(1,2,2,6,6-五甲基-4-哌啶基)正十二烷基琥珀酰亚胺,2-十一烷基-7,7,9,9-四甲基-1-氧杂-3,8-二氮杂-4-氧代-螺[4.5]癸烷,7,7,9,9-四甲基-2-环十一烷基-1-氧杂-3,8-二氮杂-4-氧代螺[4.5]癸烷和表氯醇的反应产物,1,1-双(1,2,2,6,6-五甲基-4-哌啶基氧基羰基)-2-(4-甲氧基苯基)乙烯,N,N’-双甲酰基-N,N’-双(2,2,6,6-四甲基-4-哌啶基)六亚甲基二胺,4-甲氧基-亚甲基-丙二酸与1,2,2,6,6-五甲基-4-羟基哌啶的二酯,聚[甲基丙基-3-氧基-4-(2,2,6,6-四甲基-4-哌啶基)]硅氧烷,马来酸酐-α-烯烃共聚物与2,2,6,6-四甲基-4-氨基哌啶或1,2,2,6,6-五甲基-4-氨基哌啶的反应产物。
2.7、草酰胺类,例如4,4′-二辛氧基N,N′-草酰二苯胺,2,2′-二乙氧基N,N’-草酰二苯胺,2,2′-二辛氧基-5,5’-二叔丁氧基N,N’-草酰二苯胺(2,2’-dioctyloxy-5,5’-di-tert-butoxanilide),2,2’-二(十二烷氧基)-5,5’-二叔丁氧基N,N’-草酰二苯胺,2-乙氧基-2′-乙基N,N’-草酰二苯胺,N,N′-双(3-二甲氨基丙基)草酰胺,2-乙氧基-5-叔丁基-2′-乙氧基N,N’-草酰二苯胺和它与2-乙氧基-2′-乙基-5,4′-二叔丁氧基N,N’-草酰二苯胺的混合物以及邻-和对-甲氧基双取代的N,N’-草酰二苯胺类的混合物和邻-和对-乙氧基-二取代的N,N’草酰二苯胺类的混合物。
2.8、2-(2-羟基苯基)-1,3,5-三嗪类,例如2,4,6-三(2-羟基-4-辛氧基苯基)-1,3,5-三嗪,2-(2-羟基-4-辛氧基苯基)-4,6-双(2,4-二甲基苯基)-1,3,5-三嗪,2-(2,4-二羟基苯基)-4,6-双(2,4-二甲基苯基)-1,3,5-三嗪,2,4-双(2-羟基-4-丙氧基苯基)-6-(2,4-二甲基苯基)-1,3,5-三嗪,2-(2-羟基-4-辛氧基苯基)-4,6-双(4-甲基苯基)-1,3,5-三嗪,2-(2-羟基-4-十二烷氧基苯基)-4,6-双(2,4-二甲基苯基)-1,3,5-三嗪,2-(2-羟基-4-十三烷氧基苯基)-4,6-双(2,4-二甲基苯基)-1,3,5-三嗪,2-[2-羟基-4-(2-羟基-3-丁氧基-丙氧基)苯基]-4,6-双(2,4-二甲基)-1,3,5-三嗪,2-[2-羟基-4-(2-羟基-3-辛氧基-丙氧基)苯基]-4,6-双(2,4-二甲基)-1,3,5-三嗪,2-[4-(十二烷氧基/十三烷氧基-2-羟基丙氧基)-2-羟基-苯基]-4,6-双(2,4-二甲基苯基)-1,3,5-三嗪,2-[2-羟基-4-(2-羟基-3-十二烷氧基-丙氧基)苯基]-4,6-双(2,4-二甲基苯基)-1,3,5-三嗪,2-(2-羟基-4-己氧基)苯基-4,6-二苯基-1,3,5-三嗪,2-(2-羟基-4-甲氧基苯基)-4,6-二苯基-1,3,5-三嗪,2,4,6-三[2-羟基-4-(3-丁氧基-2-羟基-丙氧基)苯基]-1,3,5-三嗪,2-(2-羟基苯基)-4-(4-甲氧基苯基)-6-苯基-1,3,5-三嗪,2{2-羟基-4-[3-(2-乙基己基-1-氧基)-2-羟基丙氧基]苯基}-4,6-双(2,4-二甲基苯基)-1,3,5-三嗪。
3.金属减活剂类,例如N,N′-二苯基草酰胺,N-水杨醛-N′-水杨酰基肼,N,N′-双(水杨酰基)肼,N,N′-双(3,5-二叔丁基-4-羟基苯基丙酰基)肼,3-水杨酰基氨基-1,2,4-***,双(亚苄基)草酰二肼,N,N’-草酰二苯胺,间苯二甲酰二肼,癸二酰双(苯基肼),N,N′-二乙酰基己二酰二肼,N,N′-双(水杨酰基)草酰二肼,N,N′-双(水杨酰基)硫代丙酰基二肼。
4.亚磷酸酯类和亚膦酸酯类,例如亚磷酸三苯酯,亚磷酸二苯基烷基酯,亚磷酸苯基二烷基酯,亚磷酸三(壬基苯基)酯,亚磷酸三月桂基酯,亚磷酸三(十八烷基)酯,二亚磷酸二硬脂基季戊四醇酯,亚磷酸三(2,4-二叔丁基苯基)酯,二亚磷酸二异癸基季戊四醇酯,二亚磷酸双(2,4-二叔丁基苯基)季戊四醇酯,二亚磷酸双(2,4-二枯基苯基)季戊四醇酯,二亚磷酸双(2,6-二叔丁基-4-甲基苯基)-季戊四醇酯,二亚磷酸二异癸基氧基季戊四醇酯,二亚磷酸双(2,4-二叔丁基-6-甲基苯基)季戊四醇酯,二亚磷酸双(2,4,6-三叔丁基苯基)季戊四醇酯,三亚磷酸三硬脂基山梨糖醇酯,二膦酸四(2,4-二叔丁基苯基)4,4′-亚联苯基酯,6-异辛氧基-2,4,8,10-四叔丁基-12H-二苯并[d,g]-1,3,2-dioxaphosphocin,亚磷酸双(2,4-二叔丁基-6-甲基苯基)甲基酯,亚磷酸双(2,4-二叔丁基-6-甲基苯基)乙基酯,6-氟-2,4,8,10-四叔丁基-12-甲基-二苯并[d,g]-1,3,2-dioxaphosphocin,2,2′,2″-次氮基[三乙基三(3,3’,5,5’-四叔丁基-1,1’-二苯基-2,2’-二基)亚磷酸酯],亚磷酸2-乙基己基(3,3’,5,5’-四叔丁基-1,1’-二苯基-2,2’-二基)酯,5-丁基-5-乙基-2-(2,4,6-三叔丁基苯氧基)-1,3,2-dioxaphophirane。
下面的亚磷酸酯是尤其优选的:
亚磷酸三(2,4-二叔丁基苯基)酯(Irgafos168,Ciba-Geigy),亚磷酸三(壬基苯基)酯,
5.羟基胺类,例如N,N-二苄基羟基胺,N,N-二乙基羟基胺,N,N-二辛基羟基胺,N,N-二月桂基羟基胺,N,N-二(十四烷基)羟基胺,N,N-二(十六烷基)羟基胺,N,N-二(十八烷基)羟基胺,N-十六烷基-N-十八烷基羟基胺,N-十七烷基-N-十八烷基羟基胺,从氢化牛胺得到的N,N-二烷基羟基胺。
6.硝酮类,例如N-苄基-α-苯基-硝酮,N-乙基-α-甲基-硝酮,N-辛基-α-庚基-硝酮,N-月桂基-α-十一烷基-硝酮,N-十四烷基-α-十三烷基-硝酮,N-十六烷基-α-十五烷基-硝酮,N-十八烷基-α-十七烷基-硝酮,N-十六烷基-α-十七烷基-硝酮,N-十八烷基-α-十五烷基-硝酮,N-十七烷基-α-十七烷基-硝酮,N-十八烷基-α-十六烷基-硝酮,从氢化牛胺衍生而来的N,N-二烷基羟基胺获得的硝酮。
7.硫代协合剂,例如硫代二丙酸二月桂基酯或硫代二丙酸二硬脂基酯。
8.过氧化物清除剂,例如β-硫代二丙酸的酯类,例如月桂基、硬脂基、十四烷基或十三烷基酯类,巯基苯并咪唑或2-巯基苯并咪唑的锌盐,二丁基二硫代氨基甲酸锌,二(十八烷基)二硫醚,四(β-十二烷基巯基)丙酸季戊四醇酯。
9.聚酰胺稳定剂,例如铜盐与碘化物和/或磷化合物的混合物,和二价锰的盐。
10.碱性助稳定剂,例如三聚氰胺,聚乙烯基吡咯烷酮,双氰胺,三烯丙基氰脲酸酯,脲衍生物,肼衍生物,胺类,聚酰胺类,聚氨酯类,高级脂肪酸的碱金属盐和碱土金属盐,例如硬脂酸钙,硬脂酸锌,二十二烷酸镁,硬脂酸镁,蓖麻酸钠和棕榈酸钾,邻苯二酚锑或邻苯二酚锌。
11.成核剂类,例如,无机物质,如滑石,金属氧化物类如二氧化钛或氧化镁,优选碱土金属的磷酸盐、碳酸盐或硫酸盐;有机化合物如单或多羧酸类和它们的盐类,例如4-叔丁基苯甲酸,己二酸,二苯基乙酸,琥珀酸钠或苯甲酸钠;聚合化合物如离子共聚物(“离聚物”)。尤其优选的是1,3:2,4-双(3’,4’-二甲基苄叉基)山梨糖醇,1,3:2,4-二(对甲基二苄叉基)山梨糖醇,和1,3:2,4-二(苄叉基)山梨糖醇。
12.填料和增强剂,例如碳酸钙,硅酸盐,玻璃纤维,玻璃珠,石棉,滑石,高岭土,云母,硫酸钡,金属氧化物和氢氧化物,炭黑,石墨,木粉和其它天然产物的粉末或纤维,合成纤维。
13.其它添加剂,例如增塑剂,润滑剂,乳化剂,颜料,流变添加剂,催化剂,流动控制剂,荧光增白剂,阻燃剂,抗静电剂和发泡剂。
14.苯并呋喃酮类和二氢吲哚酮类,例如在US 4,325,863,US 4338244,US 5,175,312,US 5,216,052,US 5,252,643,DE-A-4,316,611,DE-A-4,316,622,DE-A-4,316,876;EP-A-0589839或EP-A-0591102中公开的那些,或3-[4-(2-乙酰氧基乙氧基)苯基]-5,7-二叔丁基-苯并呋喃-2-酮,5,7-二叔丁基-3-[4-(2-硬脂酰氧基乙氧基)苯基]苯并呋喃-2-酮,3,3′-双[5,7-二叔丁基-3-(4-[2-羟基乙氧基]苯基)苯并呋喃-2-酮],5,7-二叔丁基-3-(4-乙氧基苯基)苯并呋喃-2-酮,3-(4-乙酰氧基-3,5-二甲基苯基)-5,7-二叔丁基-苯并呋喃-2-酮,3-(3,5-二甲基-4-新戊酰氧基苯基)-5,7-一叔丁基-苯并呋喃-2-酮,3-(3,4-二甲基苯基)-5,7-二叔丁基-苯并呋喃-2-酮,3-(2,3-二甲基苯基)-5,7-二叔丁基-苯并呋喃-2-酮。
15.胺氧化物,例如在US专利5,844,029和5,880,191中的公开的胺氧化物衍生物;二癸基甲基胺氧化物,三癸基胺氧化物,三(十二烷基)胺氧化物和三(十六烷基)胺氧化物。US专利5,844,029和5,880,191公开了饱和烃胺氧化物用于稳定热塑性树脂的用途。它公开了热塑性组合物进一步含有选自酚类抗氧化剂、位阻胺光稳定剂、紫外线吸收剂、有机磷化合物、脂肪酸的碱金属盐和协合剂的稳定剂或稳定剂混合物。但是,胺氧化物与其它稳定剂的共同使用来稳定聚烯烃则没有列举。
进一步优选的组合物包括,除组分(b)和(c)外的其它添加剂,尤其酚类抗氧剂,光稳定剂或加工稳定剂。
特别优选的添加剂是酚类抗氧剂(所列目录中的1项),其它位阻胺(所列目录的2.6项),苯并***和/或邻-羟基苯基三嗪类型的光稳定剂(所列目录的2.1和2.8项),亚磷酸酯和亚膦酸酯(所列目录的4项)和过氧化物破坏性化合物(所列目录的5.项)。
也特别优选的附加添加剂(稳定剂)是苯并呋喃-2-酮,例如在US-A-4,325,863,US-A-4,338,244和US-A-5,175,312中描述的那些。
本发明组合物可另外包含选自s-三嗪,N,N’-草酰二苯胺,羟基二苯甲酮,苯甲酸盐和a-氰基丙烯酸酯的另一种UV吸收剂。特别地,本发明组合物可另外包含有效稳定量的至少一种其它2-羟苯基-2H-苯并***;另一种三芳基-s-三嗪;或位阻胺或它们的混合物。优选的是选自以下的附加组分:颜料,染料,增塑剂,抗氧化剂,触变剂,流平助剂,碱性助稳定剂,其它光稳定剂象UV吸收剂和位阻胺,金属减活剂,金属氧化物,有机磷化合物,羟胺,和它们的混合物,尤其是颜料,酚类抗氧剂,硬脂酸钙,硬脂酸锌,2-(2’-羟苯基)苯并***和2-(2-羟苯基)-1,3,5-三嗪类型的UV吸收剂,和位阻胺。
本发明的众多发现中的一个是:在光稳定性和阻燃性两方面的尤其改进的性能都可以获得,如果热塑性聚合物除了含有阻燃剂之外还含有高分子量的普通位阻胺和羟基烃氧基胺类型的低分子量位阻胺的结合物的话。因此,本发明还涉及被稳定化后以抵抗光和风化的有害作用的阻燃性组合物,它包括:
A)热塑性聚合物,
B)选自聚磷酸铵,卤化和/或蜜胺型阻燃剂的阻燃剂,和
C)位阻胺光稳定剂类的结合物,它包括
C1)羟基烃氧基胺类型的低分子量位阻胺,和
C2)普通的高分子量位阻胺。
在这些组合物中的优选聚合物(A)最初所解释的(a)。
可在本发明的组合物中用作组分(B)的卤化阻燃剂可以选自有机芳族卤代化合物,如卤代的苯类,联苯类,酚类,它们的醚类或酯类,双酚类,二苯基醚类,芳族羧酸或多元酸,它们的酸酐、酰胺或酰亚胺;有机环脂族或聚环脂族卤代化合物;以及有机的脂肪族的卤代化合物如卤化链烷烃,低聚物或聚合物,烷基磷酸酯或烷基异氰脲酸酯。这些组分中的许多是现有技术中已知的,参见例如US专利4,579,906(3栏,30-41行),5,393,812;也参见<塑料添加剂手册>,H.Zweifel编辑,第五版,Hanser Publ.,Munich 2001,681-698页。
该卤化的阻燃例如可以是氯化或溴化的化合物,例如选自下列化合物:
氯代烷基磷酸酯(ANTIBLAZEAB-100,Albright & Wilson;FYROLFR-2,Akzo Nobel),
多溴化二苯基醚(DE-60F,Great Lakes Corp.),
十溴二苯基醚(DBDPO;SAYTEX102E),
三(3-溴-2,2-双(溴甲基)丙基]磷酸酯(PB370,FMC Corp.),
双酚A的双(2,3-二溴丙基醚)(PE68),
溴化的环氧树脂,
亚乙基-双(四溴邻苯二甲酰亚胺)(SAYTEXBT-93),
双(六氯环戊二烯基并)环辛烷(DECLORANE PLUS),
氯化石蜡,
1,2-双(三溴苯氧基)乙烷(FF680),
四溴双酚A(SAYTEX RB100),
亚乙基双-(二溴降冰片烷二羧酰亚胺)(SAYTEXBN-451),
双-(六氯环戊二烯基并)环辛烷,
三(2,3-二溴丙基)-异氰脲酸酯,
亚乙基-双-四溴邻苯二甲酰亚胺。
优选作为组分(B)的是溴化阻燃剂。
在本发明的组合物中最优选的阻燃剂(B)是
B1)蜜胺型阻燃剂和/或聚磷酸铵,
B2)双-(六氯环戊二烯基并)环辛烷,
B3)三(2,3-二溴丙基)-异氰脲酸酯,
B4)亚乙基-双-四溴邻苯二甲酰亚胺,
B5)1,2,5,6,9,10-六溴环十二烷,
B6)乙烷-1,2-双(五溴苯基),
B7)三(3-溴-2,2-(溴甲基)丙基)磷酸酯。
在本发明组合物中尤其优选的阻燃剂(B)是最初对于组分(b)所解释的那些。
阻燃剂(B)的含量常常是聚合物基材(A)的0.5-50wt%;对于最优选的阻燃剂(B)而言的更优选剂量是最初对于组分(b)所解释的。
在这些组合物中(B)∶(C)的比率优选是在20∶1-250∶1范围内。
在这些组合物中(C1)∶(C2)比率常常是在1∶5-5∶1范围内。对于聚合物基材(A)是聚烯烃的情况,低分子量组分(C1)优选是以与(C2)大约相同或比它更大的量使用,例如40-95重量份的(C1),基于100重量份的由(C1)和(C2)组成的组分(C)。
在具有主要组分聚乙烯的聚烯烃中,低分子量部分(C1)的量常常是组分(C)的总量的大约一半,例如相当于全部组分(C)的40-约70wt%,更特别地45-约55wt%。
在具有主要组分聚丙烯的聚烯烃中,低分子量部分(C1)的量常常是组分(C)的总量的一半以上,例如相当于全部组分(C)的50-约90wt%,更特别地60-约85wt%。
在聚烯烃的情况下,该低分子量组分(C1)也可以是烃氧基胺类型。因此,本发明的另一目的涉及一种组合物,它包括
A)聚烯烃,
B)选自聚磷酸铵,卤化和/或蜜胺型阻燃剂的阻燃剂,和
C)位阻胺光稳定剂类的结合物,它包括,基于100重量份的全部组分(C):
C1)40-95wt%的烃氧基胺类型的低分子量位阻胺,和
C2)5-60重量份的普通高分子量位阻胺。
羟基烃氧基胺类型或如果合适的话,烃氧基胺类型(C1)的低分子量位阻胺通常具有200-1000g/mol,尤其300-800g/mol的分子量范围。它可以是一种化合物或多种化合物的混合物,每一种满足该分子量条件。尤其优选的是,例如:
1-环己基氧基-2,2,6,6-四甲基-4-十八烷基氨基哌啶;
癸二酸双(1-辛氧基-2,2,6,6-四甲基哌啶-4-基)酯;
己二酸双(1-环己基氧基-2,2,6,6-四甲基哌啶-4-基)酯;
1-(2-羟基-2-甲基丙氧基)-4-十八烷酰氧基-2,2,6,6-四甲基哌啶。
该高分子量位阻胺(C2)是属于含有2,2,6,6-四甲基-4-哌啶基结构部分的普通类型,它的氮原子是未取代的(仲位阻胺)或被烷基、尤其被甲基取代(烷氧基化叔位阻胺)或是聚合物骨架的一部分(聚合的叔位阻胺)。它通常具有1200到10000g/mol,尤其1500到5000g/mol的分子量。用于本发明组合物中的此类化合物的例子能够在以上2.6项列出的那些中找到,例如以下化合物:
高分子量的仲位阻胺的例子
其中n主要在3-5范围内。
高分子量的甲基化的叔位阻胺的例子
其中n如以上所定义;
R-NH-(CH2)3-N(R)-(CH2)2-N(R)-(CH2)3-NH-R,其中R是
(CAS-No.106990-43-6).
具有高分子量的聚合的叔位阻胺的例子
(Mn:>2500;CAS-No.65447-77-0)。
尤其优选的组分(C2)的化合物是含有2,2,6,6-四甲基-4-哌啶基结构部分的那些,它的氮原子是未被取代的或是烷基、尤其甲基取代的。尤其优选的组分(C2)的化合物也含有三嗪结构部分作为结构骨架。
通常,组分(C)的含量是0.01-10wt%,优选0.05-5wt%,尤其0.1-3wt%,基于聚合物组分(A)。该重量比(C1)∶(C2)优选是1∶10到10∶1;最优选1∶1到10∶1。
任选用于本发明的这些组合物中的其它组分,和使用它们的方法是最初所解释的。
下面的实施例仅仅是为了说明目的,但不认为以任何方式限制本发明。室温代表在20-25℃范围内的温度。百分比是按重量计,除非另有说明。
具体实施方式
简写:
v 体积份数
w 重量份数
1HNMR 1H的核磁共振谱(NMR)
m/z质谱分析(原子单位)
amu 分子量g/mol(=原子单位)
Mn数均分子量(通常由GPC测定)
PP 聚丙烯
PE 聚乙烯
PE-LD 低密度聚乙烯(LDPE)
用于该实施例中的
烃氧基胺或羟基烃氧基胺类型的位阻胺(本发明组分c)是以下化合物
在US6,271,377的实施例73中公开;
c2:具有下式的主要组分的那些化合物的混合物
R1NH-CH2CH2CH2NR2CH2CH2NR3CH2CH2CH2NHR4
其中R1,R2,R3和R4中3个是下式的残基
和R1,R2,R3和R4中一个是氢
(c2,公开在US-5844026的实施例3中)
(US-6117995的实施例2)。
在实施例中使用的
其它稳定剂是下式的化合物
A:R-NH-(CH2)3-N(R)-(CH2)2-N(R)-(CH2)3-NH-R(CAS登记号106990-43-6)
其中R是基团
B:聚[[6-[(1,1,3,3-四甲基丁基)氨基]-1,3,5-三嗪-2,4-二基][[(2,2,6,6-四甲基-4-哌啶基)亚氨基]六亚甲基[(2,2,6,6-四甲基-4-哌啶基)亚氨基](CAS-No.70624-18-9)
C:癸二酸双(2,2,6,6-四甲基哌啶-4-基)酯(CAS-No.52829-07-9)
D:具有下式的低聚物(CAS-No.65447-77-0):
化合物c2,c3和A-G是可以从Ciba Specialty Chemicals商购的商品稳定剂。
实施例1
样品制备:聚合物粉末和稳定剂进行预混合(Henschel混合器,800rpm,室温),颜料粉和阻燃剂作为在PP中的浓缩物被添加,和在鼓式混合机中均化。通过挤出(Collin双螺杆挤出机,最高200℃,100rpm)实现进一步均化和造粒。
随后,利用装有相应喷嘴(样品尺寸2mm厚度,10cm宽度)的单螺杆挤出机(最高200℃,70rpm)将该混合物加工成平膜。
耐候性:冲切的样品进行加速风化(AtlasWOM Ci65,0.35W/m2(在340nm),102分干燥,18分喷水,63℃黑板温度。按照下列方式分析在表面上的风化效果:
肉眼检查灰化(灰化表示在表面上的分解)。
光泽:Minolta;表面的降解会降低偏振光的反射(如在DIN67530中所定义的60°光泽)。
ΔE:变色(根据DIN6174)。
配方:
84重量份的聚丙烯-乙烯共聚物(NovolenPPG 1022),
15重量份的含有51wt%的亚乙基-双四溴邻苯二甲酰亚胺(b4)和17wt%Sb2O3的PE型阻燃剂母料,
1重量份的TiO2和
0.2重量份的蓝色颜料(Cromophtal蓝4GNP),
和在下表中示出的稳定剂(量是以总配制料的wt%给出)。
结果显示在下表中。
表:在2000h的耐候性试验之后的表面分析
Exp.# | 稳定剂 | 观察评价 | 光泽 | ΔE |
a* | 无 | 灰化 | 3 | 5.9 |
b | 0.3%c10.1%B0.2%F | 没有改变 | 53 | 1.5 |
c* | 0.3%C0.1%B0.2%F | 灰化 | 8 | 4.6 |
d | 0.3%c10.1%B0.2%E | 没有改变 | 51 | 2.8 |
e* | 0.3%C0.1%B0.2%E | 灰化 | 8 | 5.9 |
*对比实施例
含有本发明的阻燃剂和位阻胺的结合物的样品没有显示灰化,比其中本发明组分c被另一种位阻胺代替的样品显示出更好的光泽和明显低的变色。
实施例2
制备样品和按照在实施例1中所述进行加速风化试验。
配方
89重量份的聚丙烯-乙烯共聚物(NovolenPPG 1022),
10重量份的含有30wt%的三(2,3-二溴丙基)-异氰脲酸酯(b3)和15%Sb2O3的PE型阻燃剂母料,
1重量份的TiO2和
0.2重量份的蓝色颜料(Cromophtal蓝4GNP),
和在下表中示出的稳定剂(量是以总配制料的wt%给出)。结果显示在下表中。
表:在2000h的风化试验之后的表面分析
Exp.# | 稳定剂 | 观察评价 | 光泽 | ΔE |
a* | 无 | 灰化 | 8 | 7.5 |
b | 0.3%c10.1%B0.2%F | 没有改变 | 58 | 1.7 |
c* | 0.3%C0.1%B0.2%F | 灰化 | 12 | 6.4 |
d | 0.3%c30.1%B0.2%E | 没有改变 | 57 | 3 |
e | 0.3%c10.1%B0.2%E | 没有改变 | 63 | 2.3 |
f* | 0.3%C0.1%B0.2%E | 灰化 | 14 | 7.1 |
*对比实施例
用同样量的c2或c4代替在以上实施例中的化合物c3也获得了优异的性能。
实施例3
样品制备:聚合物粉料,阻燃剂和稳定剂进行预混合(Henschel混合器,800rpm,室温),颜料作为在PE-LD中的浓缩物被添加进去,然后在鼓式混合机中均化。通过挤出(Berstorff双螺杆挤出机,最高200℃,100rpm)实现进一步均化和造粒。
通过在最高200℃的增塑温度和50℃的成形温度下压塑(Engel)获得试样(44×68×2mm)。与实施例1中一样进行样品的加速风化和评估。
配方:
73重量份的聚丙烯-乙烯共聚物(Appryl3060),
25重量份的蜜胺多磷酸盐(阻燃剂b1,MelapurP46),
2重量份的蓝色颜料母料(在PE-LD中的10%Cromophtal蓝4GNP),0.15重量份的商购酚类抗氧剂(亚磷酸三(2,4-二叔丁基苯基)酯和四[3-(3,5-二叔丁基-4-羟苯基)丙酸]季戊四醇酯的1∶1混合物,可从Ciba Specialty Chemicals获得,)
和在下表中示出的稳定剂(量是以总配制料的wt%给出)。结果显示在下表中。
表:在1000h的风化试验之后的表面分析
Exp.# | 稳定剂 | 观察评价 | 光泽 | ΔE |
a* | 0.2%A0.2%D | 灰化 | 5 | 23.9 |
b | 0.133%A0.266%c1 | 未改变 | 19 | 3.9 |
*对比实施例
实施例4
与实施例3中一样进行样品制备,样品的加速风化和评估。
配方:
82重量份的聚丙烯-乙烯共聚物(Appryl3060),
12重量份的双-(六氯环戊二烯基并)环辛烷(阻燃剂b2,DechloranPlus),
4重量份的Sb2O3
2重量份的蓝色颜料母料(在PE-LD中10%Cromophtal蓝4GNP),
0.15重量份的商购酚类抗氧剂(亚磷酸三(2,4-二叔丁基苯基)酯和四[3-(3,5-二叔丁基-4-羟苯基)丙酸]季戊四醇酯的1∶1混合物,可从Ciba Specialty Chemicals获得)
和在下表中示出的稳定剂(量是以总配制料的wt%给出)。结果显示在下表中。
表:在1000h的风化之后的表面分析
Exp.# | 稳定剂 | 观察评价 | 光泽 | ΔE |
a* | 0.2%B0.2%C | 灰化 | 7 | 5.1 |
b | 0.2%A0.2%c1 | 未变化 | 35 | 0.7 |
*对比实施例
实施例5
与实施例3中一样进行样品制备,样品的加速风化和评估。配方与实施例3的配方相同,所不同的是蜜胺型多磷酸盐阻燃剂被同样量的聚磷酸铵代替(阻燃剂b1;ExolithAP752)。结果显示在下表中。
表:在1500h的风化之后的表面分析
Exp.# | 稳定剂 | 观察评价 | 光泽 | ΔE |
a* | 0.2%A0.2%D | 灰化 | 5 | 21.4 |
b | 0.2%A0.2%c1 | 未变化 | 28 | 3.1 |
*对比实施例
实施例6
与实施例3中一样进行样品制备,样品的加速风化和评估。
配方
92重量份的聚丙烯-乙烯共聚物(Appryl3060),
4重量份的磷酸三(3-溴-2,2-(溴甲基)丙基)酯,(阻燃剂,FR372,DeadSee Bromine),
2重量份的Sb2O3,
2重量份的蓝色颜料母料(在PE-LD中的10%Cromophtal蓝4GNP),0.15重量份的商购酚类抗氧剂(亚磷酸三(2,4-二叔丁基苯基)酯和四[3-(3,5-二叔丁基-4-羟苯基)丙酸]季戊四醇酯的1∶1混合物,可从Ciba Specialty Chemicals获得)和在下表中示出的稳定剂(量是以总配制料的wt%给出)。结果显示在下列表中。
表:在1500h的风化之后表面分析
Exp.# | 稳定剂 | 观察评价 | 光泽 | ΔE |
a* | 0.2%B0.2%C | 灰化 | 6 | 7.6 |
b | 0.2%A0.2%c1 | 未变化 | 56 | 0.4 |
c | 0.4%c1 | 未变化 | 56 | 0.3 |
*对比实施例
实施例7
与实施例3中一样进行样品制备,样品的加速风化和评估。
配方
88重量份的聚丙烯-乙烯共聚物(Appryl3060),
8重量份的乙烷-1,2-双(五溴苯基)(阻燃剂b6,Saytex8010),4重量份的Sb2O3
2重量份的蓝色颜料母料(在PE-LD中的10%Cromophtal蓝4GNP)0.15重量份的商购酚类抗氧剂(亚磷酸三(2,4-二叔丁基苯基)酯和四[3-(3,5-二叔丁基-4-羟苯基)丙酸]季戊四醇酯的1∶1混合物,可从Ciba Specialty Chemicals获得),
和在下表中示出的稳定剂(量是以总配制料的wt%给出)。结果显示在下列表中。
表:在750h的风化之后的表面分析
Exp.# | 稳定剂 | 观察评价 | 光泽 | ΔE |
a* | 0.2%B0.2%C0.1%G | 灰化 | 10 | 6.5 |
b | 0.13%A0.27%c10.1%G | 未变化 | 38 | 5.3 |
*对比实施例
Claims (7)
1.阻燃性和光稳定的组合物,包括
a)聚烯烃,
b)以组分a)重量计为0.5到50wt%的阻燃剂三-(2,3-二溴丙基)-异氰脲酸酯,和
c)以组分a)重量计为0.01到10wt%的环状位阻胺,其符合以下通式:
其中
G1和G2独立地是具有1-4个碳原子的烷基或一起是五亚甲基,和
E1是C1-C18烷基、C5-C12环烷基或C7-C15芳烷基;或E1是C1-C18烷基、C5-C12环烷基或C7-C15芳烷基,它们当中的每个都在脂族部分中被1-3个OH基团取代;
T是需要来完成通式(I)以便与该位阻胺氮原子和被G1和G2取代的两个季碳原子一起形成5员-或6员脂族环结构的二价有机基;
或是由二烷基酯或异氰酸酯与其中E1含有1个OH基团和T是-CH2-CH(OH)-CH2-的通式(I)的化合物反应所形成的低聚或高聚位阻胺分子;
或是其中E1含有1个OH基团和T是-CH2-CH(OH)-CH2-的通式(I)的简单二酯或脲烷衍生物。
2.阻燃性和光稳定的组合物包括
a)聚烯烃,
b)以组分a)重量计为0.5到50wt%的选自以下的阻燃剂:
b1)蜜胺型阻燃剂和/或聚磷酸铵,
b2)双-(六氯环戊二烯基并)环辛烷,
b3)三-(2,3-二溴丙基)-异氰脲酸酯,
b5)1,2,5,6,9,10-H-六溴环十二烷,和
b6)乙烷-1,2-双(五溴苯基);
c)以组分a)重量计为0.01到10wt%的环状位阻胺,其符合以下通式:
其中
G1和G2独立地是具有1-4个碳原子的烷基或一起是五亚甲基,
和
E1是C1-C18烷基,C5-C12环烷基或C7-C15芳烷基,它们当中的每一个在脂族部分中被1-3个OH基团取代;
T是需要来完成通式(I)以便与位阻胺氮原子和被G1和G2取代的两个季碳原子一起形成5员-或6员脂族环结构的二价有机基;
或是由二烷基酯或异氰酸酯与其中E1含有1个OH基团和T是-CH2-CH(OH)-CH2-的通式(I)的化合物反应所形成的低聚或高聚位阻胺分子;
或是其中E1含有1个OH基团和T是-CH2-CH(OH)-CH2-的通式(I)的简单二酯或脲烷衍生物。
3.被稳定化后以抵抗光和风化的有害影响的阻燃性组合物,它包括
a)聚烯烃,
b)以组分a)重量计为0.5到50wt%的选自聚磷酸铵、卤化和蜜胺型阻燃剂中至少一种的阻燃剂,和
c)以组分a)重量计为0.01到10wt%的环状位阻胺的结合物,包括
c1)低分子量的环状位阻胺,其符合以下通式:
其中
G1和G2独立地是具有1-4个碳原子的烷基或一起是五亚甲基,
和
E1是C1-C18烷基,C5-C12环烷基或C7-C15芳烷基,它们当中的每一个在脂族部分中被1-3个OH基团取代;
T是需要来完成通式(I)以便与位阻胺氮原子和被G1和G2取代的两个季碳原子一起形成5员-或6员脂族环结构的二价有机基;
或是由二烷基酯或异氰酸酯与其中E1含有1个OH基团和T是-CH2-CH(OH)-CH2-的通式(I)的化合物反应所形成的低聚或高聚位阻胺分子;
或是其中E1含有1个OH基团和T是-CH2-CH(OH)-CH2-的通式(I)的简单二酯或脲烷衍生物;
c2)高分子量仲或烷基化的或聚合的叔位阻胺。
4.被稳定化后以抵抗光和风化的有害影响的阻燃性组合物,它包括
a)聚烯烃,
b)以组分a)重量计为0.5到50wt%的选自聚磷酸铵、卤化和蜜胺型阻燃剂中至少一种的阻燃剂,和
c)以组分a)重量计为0.01到10wt%的位阻胺,包括,基于100重量份的全部组分(c):
c1)40-95重量份的低分子量环状位阻胺,其符合以下通式:
其中
G1和G2独立地是具有1-4个碳原子的烷基或一起是五亚甲基,
和
E1是C1-C18烷基,C5-C12环烷基或C7-C15芳烷基,它们当中的每一个在脂族部分中被1-3个OH基团取代;
T是需要来完成通式(I)以便与位阻胺氮原子和被G1和G2取代的两个季碳原子一起形成5员-或6员脂族环结构的二价有机基;
或是由二烷基酯或异氰酸酯与其中E1含有1个OH基团和T是-CH2-CH(OH)-CH2-的通式(I)的化合物反应所形成的低聚或高聚位阻胺分子;
或是其中E1含有1个OH基团和T是-CH2-CH(OH)-CH2-的通式(I)的简单二酯或脲烷衍生物,和
c2)5-60重量份的高分子量仲或烷基化的或聚合的叔位阻胺;
前提条件是,当聚烯烃(a)为具有聚丙烯为主要组分的聚烯烃时,基于组分(c)的总量,所述低分子量位阻胺(c1)为60-85重量份,和高分子量位阻胺(c2)为15-40重量份。
5.根据权利要求3或4的组合物,其中组分(b)选自
b1)蜜胺型阻燃剂和/或聚磷酸铵,
b2)双-(六氯环戊二烯基并)环辛烷,
b3)三-(2,3-二溴丙基)-异氰脲酸酯,
b4)亚乙基-双-四溴邻苯二甲酰亚胺,
b5)1,2,5,6,9,10-H-六溴环十二烷,
b6)乙烷-1,2-双(五溴苯基);
b7)磷酸三(3-溴-2,2-(溴甲基)丙基)酯。
6.根据权利要求3或4的组合物,其中低分子量的环状位阻胺(c1)具有200-1000g/mol的分子量,和该高分子量位阻胺(c2)具有1200-10000g/mol的分子量。
7.根据权利要求1-4中任何一项的组合物,其中还包括选自以下一种或多种的其它组分:颜料、染料、增塑剂、抗氧化剂、触变剂、流平助剂、碱性助稳定剂、其它光稳定剂、金属减活剂、金属氧化物、有机磷化合物、羟胺和它们的混合物。
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Cited By (3)
Publication number | Priority date | Publication date | Assignee | Title |
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CN100365051C (zh) * | 2006-11-24 | 2008-01-30 | 北京理工大学 | 一种增强增韧阻燃聚烯烃树脂组合物及其制备方法 |
CN112204098A (zh) * | 2018-04-27 | 2021-01-08 | 陶氏环球技术有限责任公司 | 磷酸盐增强的耐热乙烯/α-烯烃互聚物组合物 |
CN112204098B (zh) * | 2018-04-27 | 2023-11-14 | 陶氏环球技术有限责任公司 | 磷酸盐增强的耐热乙烯/α-烯烃互聚物组合物 |
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