JP2008001766A - Resin composition and molded article comprising the same - Google Patents
Resin composition and molded article comprising the same Download PDFInfo
- Publication number
- JP2008001766A JP2008001766A JP2006171143A JP2006171143A JP2008001766A JP 2008001766 A JP2008001766 A JP 2008001766A JP 2006171143 A JP2006171143 A JP 2006171143A JP 2006171143 A JP2006171143 A JP 2006171143A JP 2008001766 A JP2008001766 A JP 2008001766A
- Authority
- JP
- Japan
- Prior art keywords
- resin
- weight
- parts
- acid
- resin composition
- 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.)
- Granted
Links
- 239000011342 resin composition Substances 0.000 title claims abstract description 52
- 229920005989 resin Polymers 0.000 claims abstract description 160
- 239000011347 resin Substances 0.000 claims abstract description 160
- 229920000747 poly(lactic acid) Polymers 0.000 claims abstract description 68
- 239000004626 polylactic acid Substances 0.000 claims abstract description 68
- 125000003118 aryl group Chemical group 0.000 claims abstract description 53
- 239000000049 pigment Substances 0.000 claims abstract description 34
- YCKRFDGAMUMZLT-UHFFFAOYSA-N Fluorine atom Chemical compound [F] YCKRFDGAMUMZLT-UHFFFAOYSA-N 0.000 claims abstract description 17
- 239000011737 fluorine Substances 0.000 claims abstract description 17
- 229910052731 fluorine Inorganic materials 0.000 claims abstract description 17
- -1 polytetrafluoroethylene Polymers 0.000 claims description 90
- PPBRXRYQALVLMV-UHFFFAOYSA-N Styrene Chemical compound C=CC1=CC=CC=C1 PPBRXRYQALVLMV-UHFFFAOYSA-N 0.000 claims description 56
- 229920005668 polycarbonate resin Polymers 0.000 claims description 41
- 239000004431 polycarbonate resin Substances 0.000 claims description 41
- 239000003484 crystal nucleating agent Substances 0.000 claims description 27
- 238000002156 mixing Methods 0.000 claims description 24
- 229920005992 thermoplastic resin Polymers 0.000 claims description 24
- 229920001343 polytetrafluoroethylene Polymers 0.000 claims description 22
- 239000004810 polytetrafluoroethylene Substances 0.000 claims description 22
- 239000000203 mixture Substances 0.000 claims description 20
- GWEVSGVZZGPLCZ-UHFFFAOYSA-N Titan oxide Chemical compound O=[Ti]=O GWEVSGVZZGPLCZ-UHFFFAOYSA-N 0.000 claims description 15
- OGIDPMRJRNCKJF-UHFFFAOYSA-N titanium oxide Inorganic materials [Ti]=O OGIDPMRJRNCKJF-UHFFFAOYSA-N 0.000 claims description 12
- 229920001971 elastomer Polymers 0.000 claims description 10
- 239000004645 polyester resin Substances 0.000 claims description 10
- 229920000098 polyolefin Polymers 0.000 claims description 10
- 229920001225 polyester resin Polymers 0.000 claims description 8
- 239000005060 rubber Substances 0.000 claims description 8
- 239000011258 core-shell material Substances 0.000 claims description 6
- 239000002530 phenolic antioxidant Substances 0.000 claims description 4
- ISWSIDIOOBJBQZ-UHFFFAOYSA-N Phenol Chemical compound OC1=CC=CC=C1 ISWSIDIOOBJBQZ-UHFFFAOYSA-N 0.000 abstract description 20
- 239000003963 antioxidant agent Substances 0.000 abstract description 15
- 230000003078 antioxidant effect Effects 0.000 abstract description 12
- 238000013329 compounding Methods 0.000 abstract description 9
- 229920000515 polycarbonate Polymers 0.000 abstract description 9
- 239000004417 polycarbonate Substances 0.000 abstract description 9
- 239000000047 product Substances 0.000 description 43
- 239000003063 flame retardant Substances 0.000 description 40
- 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 description 24
- 229920000642 polymer Polymers 0.000 description 21
- 239000004014 plasticizer Substances 0.000 description 20
- 239000000835 fiber Substances 0.000 description 19
- OAICVXFJPJFONN-UHFFFAOYSA-N Phosphorus Chemical compound [P] OAICVXFJPJFONN-UHFFFAOYSA-N 0.000 description 18
- KAKZBPTYRLMSJV-UHFFFAOYSA-N Butadiene Chemical compound C=CC=C KAKZBPTYRLMSJV-UHFFFAOYSA-N 0.000 description 16
- PEDCQBHIVMGVHV-UHFFFAOYSA-N Glycerine Chemical compound OCC(O)CO PEDCQBHIVMGVHV-UHFFFAOYSA-N 0.000 description 16
- 238000001746 injection moulding Methods 0.000 description 16
- 238000000034 method Methods 0.000 description 15
- OKTJSMMVPCPJKN-UHFFFAOYSA-N Carbon Chemical compound [C] OKTJSMMVPCPJKN-UHFFFAOYSA-N 0.000 description 14
- 239000005977 Ethylene Substances 0.000 description 14
- 239000000945 filler Substances 0.000 description 14
- NLHHRLWOUZZQLW-UHFFFAOYSA-N Acrylonitrile Chemical compound C=CC#N NLHHRLWOUZZQLW-UHFFFAOYSA-N 0.000 description 13
- VGGSQFUCUMXWEO-UHFFFAOYSA-N Ethene Chemical compound C=C VGGSQFUCUMXWEO-UHFFFAOYSA-N 0.000 description 13
- LYCAIKOWRPUZTN-UHFFFAOYSA-N Ethylene glycol Chemical compound OCCO LYCAIKOWRPUZTN-UHFFFAOYSA-N 0.000 description 12
- 150000001875 compounds Chemical class 0.000 description 12
- 229910052698 phosphorus Inorganic materials 0.000 description 12
- 229920001577 copolymer Polymers 0.000 description 11
- ZFSLODLOARCGLH-UHFFFAOYSA-N isocyanuric acid Chemical compound OC1=NC(O)=NC(O)=N1 ZFSLODLOARCGLH-UHFFFAOYSA-N 0.000 description 11
- 229910052751 metal Chemical class 0.000 description 11
- 239000002184 metal Chemical class 0.000 description 11
- 239000011574 phosphorus Substances 0.000 description 11
- 239000004593 Epoxy Substances 0.000 description 10
- XLOMVQKBTHCTTD-UHFFFAOYSA-N Zinc monoxide Chemical compound [Zn]=O XLOMVQKBTHCTTD-UHFFFAOYSA-N 0.000 description 10
- 125000003178 carboxy group Chemical group [H]OC(*)=O 0.000 description 10
- JVTAAEKCZFNVCJ-UHFFFAOYSA-N lactic acid Chemical compound CC(O)C(O)=O JVTAAEKCZFNVCJ-UHFFFAOYSA-N 0.000 description 10
- 229910019142 PO4 Inorganic materials 0.000 description 9
- 239000004793 Polystyrene Substances 0.000 description 9
- 239000002245 particle Substances 0.000 description 9
- 239000010452 phosphate Substances 0.000 description 9
- VYPSYNLAJGMNEJ-UHFFFAOYSA-N Silicium dioxide Chemical compound O=[Si]=O VYPSYNLAJGMNEJ-UHFFFAOYSA-N 0.000 description 8
- 239000002253 acid Substances 0.000 description 8
- IISBACLAFKSPIT-UHFFFAOYSA-N bisphenol A Chemical compound C=1C=C(O)C=CC=1C(C)(C)C1=CC=C(O)C=C1 IISBACLAFKSPIT-UHFFFAOYSA-N 0.000 description 8
- 238000007334 copolymerization reaction Methods 0.000 description 8
- 230000000694 effects Effects 0.000 description 8
- 125000003700 epoxy group Chemical group 0.000 description 8
- 235000011187 glycerol Nutrition 0.000 description 8
- 239000010439 graphite Substances 0.000 description 8
- 229910002804 graphite Inorganic materials 0.000 description 8
- 239000000178 monomer Substances 0.000 description 8
- NBIIXXVUZAFLBC-UHFFFAOYSA-K phosphate Chemical compound [O-]P([O-])([O-])=O NBIIXXVUZAFLBC-UHFFFAOYSA-K 0.000 description 8
- 229920000728 polyester Polymers 0.000 description 8
- 229920002223 polystyrene Polymers 0.000 description 8
- 150000003839 salts Chemical class 0.000 description 8
- 239000002981 blocking agent Substances 0.000 description 7
- 239000006229 carbon black Substances 0.000 description 7
- 238000002844 melting Methods 0.000 description 7
- 230000008018 melting Effects 0.000 description 7
- 229910017464 nitrogen compound Inorganic materials 0.000 description 7
- 150000002830 nitrogen compounds Chemical class 0.000 description 7
- 229920000058 polyacrylate Polymers 0.000 description 7
- ARCGXLSVLAOJQL-UHFFFAOYSA-N trimellitic acid Chemical compound OC(=O)C1=CC=C(C(O)=O)C(C(O)=O)=C1 ARCGXLSVLAOJQL-UHFFFAOYSA-N 0.000 description 7
- BAPJBEWLBFYGME-UHFFFAOYSA-N Methyl acrylate Chemical compound COC(=O)C=C BAPJBEWLBFYGME-UHFFFAOYSA-N 0.000 description 6
- DNIAPMSPPWPWGF-UHFFFAOYSA-N Propylene glycol Chemical compound CC(O)CO DNIAPMSPPWPWGF-UHFFFAOYSA-N 0.000 description 6
- 229920002678 cellulose Polymers 0.000 description 6
- 239000003795 chemical substances by application Substances 0.000 description 6
- 238000000576 coating method Methods 0.000 description 6
- 230000000052 comparative effect Effects 0.000 description 6
- 239000002270 dispersing agent Substances 0.000 description 6
- QQVIHTHCMHWDBS-UHFFFAOYSA-N isophthalic acid Chemical compound OC(=O)C1=CC=CC(C(O)=O)=C1 QQVIHTHCMHWDBS-UHFFFAOYSA-N 0.000 description 6
- ZQKXQUJXLSSJCH-UHFFFAOYSA-N melamine cyanurate Chemical compound NC1=NC(N)=NC(N)=N1.O=C1NC(=O)NC(=O)N1 ZQKXQUJXLSSJCH-UHFFFAOYSA-N 0.000 description 6
- 230000003287 optical effect Effects 0.000 description 6
- 229920003229 poly(methyl methacrylate) Polymers 0.000 description 6
- 239000004926 polymethyl methacrylate Substances 0.000 description 6
- 229920001296 polysiloxane Polymers 0.000 description 6
- BFKJFAAPBSQJPD-UHFFFAOYSA-N tetrafluoroethene Chemical group FC(F)=C(F)F BFKJFAAPBSQJPD-UHFFFAOYSA-N 0.000 description 6
- UQSXHKLRYXJYBZ-UHFFFAOYSA-N Iron oxide Chemical compound [Fe]=O UQSXHKLRYXJYBZ-UHFFFAOYSA-N 0.000 description 5
- VVQNEPGJFQJSBK-UHFFFAOYSA-N Methyl methacrylate Chemical compound COC(=O)C(C)=C VVQNEPGJFQJSBK-UHFFFAOYSA-N 0.000 description 5
- 239000004809 Teflon Substances 0.000 description 5
- 229920006362 Teflon® Polymers 0.000 description 5
- 229920000122 acrylonitrile butadiene styrene Polymers 0.000 description 5
- 229910045601 alloy Inorganic materials 0.000 description 5
- 239000000956 alloy Substances 0.000 description 5
- WNROFYMDJYEPJX-UHFFFAOYSA-K aluminium hydroxide Chemical compound [OH-].[OH-].[OH-].[Al+3] WNROFYMDJYEPJX-UHFFFAOYSA-K 0.000 description 5
- 239000003086 colorant Substances 0.000 description 5
- 239000004310 lactic acid Substances 0.000 description 5
- 235000014655 lactic acid Nutrition 0.000 description 5
- 238000000465 moulding Methods 0.000 description 5
- 150000003014 phosphoric acid esters Chemical class 0.000 description 5
- 229920002050 silicone resin Polymers 0.000 description 5
- 239000000126 substance Substances 0.000 description 5
- 229910052623 talc Inorganic materials 0.000 description 5
- 239000011787 zinc oxide Substances 0.000 description 5
- VXNZUUAINFGPBY-UHFFFAOYSA-N 1-Butene Chemical compound CCC=C VXNZUUAINFGPBY-UHFFFAOYSA-N 0.000 description 4
- 239000004743 Polypropylene Substances 0.000 description 4
- 229920000297 Rayon Polymers 0.000 description 4
- KKEYFWRCBNTPAC-UHFFFAOYSA-N Terephthalic acid Chemical compound OC(=O)C1=CC=C(C(O)=O)C=C1 KKEYFWRCBNTPAC-UHFFFAOYSA-N 0.000 description 4
- 150000008065 acid anhydrides Chemical class 0.000 description 4
- WNLRTRBMVRJNCN-UHFFFAOYSA-N adipic acid Chemical compound OC(=O)CCCCC(O)=O WNLRTRBMVRJNCN-UHFFFAOYSA-N 0.000 description 4
- 125000000217 alkyl group Chemical group 0.000 description 4
- 150000001732 carboxylic acid derivatives Chemical class 0.000 description 4
- DOIRQSBPFJWKBE-UHFFFAOYSA-N dibutyl phthalate Chemical compound CCCCOC(=O)C1=CC=CC=C1C(=O)OCCCC DOIRQSBPFJWKBE-UHFFFAOYSA-N 0.000 description 4
- ZBCBWPMODOFKDW-UHFFFAOYSA-N diethanolamine Chemical compound OCCNCCO ZBCBWPMODOFKDW-UHFFFAOYSA-N 0.000 description 4
- CGPRUXZTHGTMKW-UHFFFAOYSA-N ethene;ethyl prop-2-enoate Chemical compound C=C.CCOC(=O)C=C CGPRUXZTHGTMKW-UHFFFAOYSA-N 0.000 description 4
- 229920001038 ethylene copolymer Polymers 0.000 description 4
- VOZRXNHHFUQHIL-UHFFFAOYSA-N glycidyl methacrylate Chemical group CC(=C)C(=O)OCC1CO1 VOZRXNHHFUQHIL-UHFFFAOYSA-N 0.000 description 4
- 125000002887 hydroxy group Chemical group [H]O* 0.000 description 4
- 239000012796 inorganic flame retardant Substances 0.000 description 4
- 125000002496 methyl group Chemical group [H]C([H])([H])* 0.000 description 4
- 239000011812 mixed powder Substances 0.000 description 4
- 239000003921 oil Substances 0.000 description 4
- 235000019198 oils Nutrition 0.000 description 4
- 229920001155 polypropylene Polymers 0.000 description 4
- GHMLBKRAJCXXBS-UHFFFAOYSA-N resorcinol Chemical compound OC1=CC=CC(O)=C1 GHMLBKRAJCXXBS-UHFFFAOYSA-N 0.000 description 4
- CXMXRPHRNRROMY-UHFFFAOYSA-N sebacic acid Chemical compound OC(=O)CCCCCCCCC(O)=O CXMXRPHRNRROMY-UHFFFAOYSA-N 0.000 description 4
- UQDJGEHQDNVPGU-UHFFFAOYSA-N serine phosphoethanolamine Chemical compound [NH3+]CCOP([O-])(=O)OCC([NH3+])C([O-])=O UQDJGEHQDNVPGU-UHFFFAOYSA-N 0.000 description 4
- 159000000000 sodium salts Chemical class 0.000 description 4
- 239000000454 talc Substances 0.000 description 4
- 238000012360 testing method Methods 0.000 description 4
- 229920001187 thermosetting polymer Polymers 0.000 description 4
- 150000003918 triazines Chemical class 0.000 description 4
- HIDBROSJWZYGSZ-UHFFFAOYSA-N 1-phenylpyrrole-2,5-dione Chemical compound O=C1C=CC(=O)N1C1=CC=CC=C1 HIDBROSJWZYGSZ-UHFFFAOYSA-N 0.000 description 3
- VPWNQTHUCYMVMZ-UHFFFAOYSA-N 4,4'-sulfonyldiphenol Chemical class C1=CC(O)=CC=C1S(=O)(=O)C1=CC=C(O)C=C1 VPWNQTHUCYMVMZ-UHFFFAOYSA-N 0.000 description 3
- WFDIJRYMOXRFFG-UHFFFAOYSA-N Acetic anhydride Chemical compound CC(=O)OC(C)=O WFDIJRYMOXRFFG-UHFFFAOYSA-N 0.000 description 3
- UHOVQNZJYSORNB-UHFFFAOYSA-N Benzene Chemical compound C1=CC=CC=C1 UHOVQNZJYSORNB-UHFFFAOYSA-N 0.000 description 3
- 229930185605 Bisphenol Natural products 0.000 description 3
- 229920008347 Cellulose acetate propionate Polymers 0.000 description 3
- 229920002284 Cellulose triacetate Polymers 0.000 description 3
- OFOBLEOULBTSOW-UHFFFAOYSA-N Malonic acid Chemical compound OC(=O)CC(O)=O OFOBLEOULBTSOW-UHFFFAOYSA-N 0.000 description 3
- 229920000877 Melamine resin Polymers 0.000 description 3
- MUBZPKHOEPUJKR-UHFFFAOYSA-N Oxalic acid Chemical compound OC(=O)C(O)=O MUBZPKHOEPUJKR-UHFFFAOYSA-N 0.000 description 3
- OFBQJSOFQDEBGM-UHFFFAOYSA-N Pentane Chemical compound CCCCC OFBQJSOFQDEBGM-UHFFFAOYSA-N 0.000 description 3
- 229920000388 Polyphosphate Polymers 0.000 description 3
- XSQUKJJJFZCRTK-UHFFFAOYSA-N Urea Chemical compound NC(N)=O XSQUKJJJFZCRTK-UHFFFAOYSA-N 0.000 description 3
- NNLVGZFZQQXQNW-ADJNRHBOSA-N [(2r,3r,4s,5r,6s)-4,5-diacetyloxy-3-[(2s,3r,4s,5r,6r)-3,4,5-triacetyloxy-6-(acetyloxymethyl)oxan-2-yl]oxy-6-[(2r,3r,4s,5r,6s)-4,5,6-triacetyloxy-2-(acetyloxymethyl)oxan-3-yl]oxyoxan-2-yl]methyl acetate Chemical compound O([C@@H]1O[C@@H]([C@H]([C@H](OC(C)=O)[C@H]1OC(C)=O)O[C@H]1[C@@H]([C@@H](OC(C)=O)[C@H](OC(C)=O)[C@@H](COC(C)=O)O1)OC(C)=O)COC(=O)C)[C@@H]1[C@@H](COC(C)=O)O[C@@H](OC(C)=O)[C@H](OC(C)=O)[C@H]1OC(C)=O NNLVGZFZQQXQNW-ADJNRHBOSA-N 0.000 description 3
- NIXOWILDQLNWCW-UHFFFAOYSA-N acrylic acid group Chemical group C(C=C)(=O)O NIXOWILDQLNWCW-UHFFFAOYSA-N 0.000 description 3
- BVKZGUZCCUSVTD-UHFFFAOYSA-N carbonic acid Chemical class OC(O)=O BVKZGUZCCUSVTD-UHFFFAOYSA-N 0.000 description 3
- 238000004040 coloring Methods 0.000 description 3
- 238000002485 combustion reaction Methods 0.000 description 3
- 239000012792 core layer Substances 0.000 description 3
- MTHSVFCYNBDYFN-UHFFFAOYSA-N diethylene glycol Chemical compound OCCOCCO MTHSVFCYNBDYFN-UHFFFAOYSA-N 0.000 description 3
- 239000000975 dye Substances 0.000 description 3
- 239000003822 epoxy resin Substances 0.000 description 3
- 150000002148 esters Chemical class 0.000 description 3
- 238000001125 extrusion Methods 0.000 description 3
- 239000012765 fibrous filler Substances 0.000 description 3
- 239000003365 glass fiber Substances 0.000 description 3
- 125000003055 glycidyl group Chemical group C(C1CO1)* 0.000 description 3
- 238000010559 graft polymerization reaction Methods 0.000 description 3
- WGCNASOHLSPBMP-UHFFFAOYSA-N hydroxyacetaldehyde Natural products OCC=O WGCNASOHLSPBMP-UHFFFAOYSA-N 0.000 description 3
- 239000001023 inorganic pigment Substances 0.000 description 3
- NLYAJNPCOHFWQQ-UHFFFAOYSA-N kaolin Chemical compound O.O.O=[Al]O[Si](=O)O[Si](=O)O[Al]=O NLYAJNPCOHFWQQ-UHFFFAOYSA-N 0.000 description 3
- 229910052622 kaolinite Inorganic materials 0.000 description 3
- 238000004898 kneading Methods 0.000 description 3
- 239000010410 layer Substances 0.000 description 3
- FPYJFEHAWHCUMM-UHFFFAOYSA-N maleic anhydride Chemical compound O=C1OC(=O)C=C1 FPYJFEHAWHCUMM-UHFFFAOYSA-N 0.000 description 3
- 238000004519 manufacturing process Methods 0.000 description 3
- 239000000463 material Substances 0.000 description 3
- 230000007246 mechanism Effects 0.000 description 3
- JDSHMPZPIAZGSV-UHFFFAOYSA-N melamine Chemical compound NC1=NC(N)=NC(N)=N1 JDSHMPZPIAZGSV-UHFFFAOYSA-N 0.000 description 3
- 229910052757 nitrogen Inorganic materials 0.000 description 3
- LYRFLYHAGKPMFH-UHFFFAOYSA-N octadecanamide Chemical compound CCCCCCCCCCCCCCCCCC(N)=O LYRFLYHAGKPMFH-UHFFFAOYSA-N 0.000 description 3
- 229920000620 organic polymer Polymers 0.000 description 3
- TWNQGVIAIRXVLR-UHFFFAOYSA-N oxo(oxoalumanyloxy)alumane Chemical compound O=[Al]O[Al]=O TWNQGVIAIRXVLR-UHFFFAOYSA-N 0.000 description 3
- 238000007747 plating Methods 0.000 description 3
- 229920002239 polyacrylonitrile Polymers 0.000 description 3
- 229920001515 polyalkylene glycol Polymers 0.000 description 3
- 229920002961 polybutylene succinate Polymers 0.000 description 3
- 239000004631 polybutylene succinate Substances 0.000 description 3
- 229920000647 polyepoxide Polymers 0.000 description 3
- 229920005862 polyol Polymers 0.000 description 3
- 239000001205 polyphosphate Substances 0.000 description 3
- 235000011176 polyphosphates Nutrition 0.000 description 3
- 239000000843 powder Substances 0.000 description 3
- 229910052814 silicon oxide Inorganic materials 0.000 description 3
- 229920002545 silicone oil Polymers 0.000 description 3
- 238000006467 substitution reaction Methods 0.000 description 3
- XOLBLPGZBRYERU-UHFFFAOYSA-N tin dioxide Chemical compound O=[Sn]=O XOLBLPGZBRYERU-UHFFFAOYSA-N 0.000 description 3
- QHGNHLZPVBIIPX-UHFFFAOYSA-N tin(ii) oxide Chemical class [Sn]=O QHGNHLZPVBIIPX-UHFFFAOYSA-N 0.000 description 3
- BIKXLKXABVUSMH-UHFFFAOYSA-N trizinc;diborate Chemical compound [Zn+2].[Zn+2].[Zn+2].[O-]B([O-])[O-].[O-]B([O-])[O-] BIKXLKXABVUSMH-UHFFFAOYSA-N 0.000 description 3
- 125000000391 vinyl group Chemical group [H]C([*])=C([H])[H] 0.000 description 3
- 229920002554 vinyl polymer Polymers 0.000 description 3
- XLYOFNOQVPJJNP-UHFFFAOYSA-N water Substances O XLYOFNOQVPJJNP-UHFFFAOYSA-N 0.000 description 3
- PUPZLCDOIYMWBV-UHFFFAOYSA-N (+/-)-1,3-Butanediol Chemical compound CC(O)CCO PUPZLCDOIYMWBV-UHFFFAOYSA-N 0.000 description 2
- JYEUMXHLPRZUAT-UHFFFAOYSA-N 1,2,3-triazine Chemical group C1=CN=NN=C1 JYEUMXHLPRZUAT-UHFFFAOYSA-N 0.000 description 2
- MYRTYDVEIRVNKP-UHFFFAOYSA-N 1,2-Divinylbenzene Chemical compound C=CC1=CC=CC=C1C=C MYRTYDVEIRVNKP-UHFFFAOYSA-N 0.000 description 2
- NXQMCAOPTPLPRL-UHFFFAOYSA-N 2-(2-benzoyloxyethoxy)ethyl benzoate Chemical compound C=1C=CC=CC=1C(=O)OCCOCCOC(=O)C1=CC=CC=C1 NXQMCAOPTPLPRL-UHFFFAOYSA-N 0.000 description 2
- XAIZOTQTRJYNHC-UHFFFAOYSA-N 4-[2-(3,5-diethyl-4-hydroxyphenyl)propan-2-yl]-2,6-diethylphenol Chemical compound CCC1=C(O)C(CC)=CC(C(C)(C)C=2C=C(CC)C(O)=C(CC)C=2)=C1 XAIZOTQTRJYNHC-UHFFFAOYSA-N 0.000 description 2
- WSSSPWUEQFSQQG-UHFFFAOYSA-N 4-methyl-1-pentene Chemical compound CC(C)CC=C WSSSPWUEQFSQQG-UHFFFAOYSA-N 0.000 description 2
- OZJPLYNZGCXSJM-UHFFFAOYSA-N 5-valerolactone Chemical compound O=C1CCCCO1 OZJPLYNZGCXSJM-UHFFFAOYSA-N 0.000 description 2
- NIXOWILDQLNWCW-UHFFFAOYSA-M Acrylate Chemical compound [O-]C(=O)C=C NIXOWILDQLNWCW-UHFFFAOYSA-M 0.000 description 2
- QGZKDVFQNNGYKY-UHFFFAOYSA-N Ammonia Chemical compound N QGZKDVFQNNGYKY-UHFFFAOYSA-N 0.000 description 2
- PAYRUJLWNCNPSJ-UHFFFAOYSA-N Aniline Chemical compound NC1=CC=CC=C1 PAYRUJLWNCNPSJ-UHFFFAOYSA-N 0.000 description 2
- 229910052582 BN Inorganic materials 0.000 description 2
- PZNSFCLAULLKQX-UHFFFAOYSA-N Boron nitride Chemical compound N#B PZNSFCLAULLKQX-UHFFFAOYSA-N 0.000 description 2
- IRIAEXORFWYRCZ-UHFFFAOYSA-N Butylbenzyl phthalate Chemical compound CCCCOC(=O)C1=CC=CC=C1C(=O)OCC1=CC=CC=C1 IRIAEXORFWYRCZ-UHFFFAOYSA-N 0.000 description 2
- SOGAXMICEFXMKE-UHFFFAOYSA-N Butylmethacrylate Chemical compound CCCCOC(=O)C(C)=C SOGAXMICEFXMKE-UHFFFAOYSA-N 0.000 description 2
- 229920000623 Cellulose acetate phthalate Polymers 0.000 description 2
- 229920001747 Cellulose diacetate Polymers 0.000 description 2
- RTZKZFJDLAIYFH-UHFFFAOYSA-N Diethyl ether Chemical compound CCOCC RTZKZFJDLAIYFH-UHFFFAOYSA-N 0.000 description 2
- NIQCNGHVCWTJSM-UHFFFAOYSA-N Dimethyl phthalate Chemical compound COC(=O)C1=CC=CC=C1C(=O)OC NIQCNGHVCWTJSM-UHFFFAOYSA-N 0.000 description 2
- 241000196324 Embryophyta Species 0.000 description 2
- QUSNBJAOOMFDIB-UHFFFAOYSA-N Ethylamine Chemical compound CCN QUSNBJAOOMFDIB-UHFFFAOYSA-N 0.000 description 2
- IAYPIBMASNFSPL-UHFFFAOYSA-N Ethylene oxide Chemical compound C1CO1 IAYPIBMASNFSPL-UHFFFAOYSA-N 0.000 description 2
- PIICEJLVQHRZGT-UHFFFAOYSA-N Ethylenediamine Chemical class NCCN PIICEJLVQHRZGT-UHFFFAOYSA-N 0.000 description 2
- AEMRFAOFKBGASW-UHFFFAOYSA-N Glycolic acid Chemical compound OCC(O)=O AEMRFAOFKBGASW-UHFFFAOYSA-N 0.000 description 2
- 240000000797 Hibiscus cannabinus Species 0.000 description 2
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- 238000004381 surface treatment Methods 0.000 description 1
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- ARERIMFZYPFJAV-UHFFFAOYSA-N tetrabromodiphenyl ethers Chemical compound C1=CC(Br)=CC=C1OC1=CC=C(Br)C(Br)=C1Br ARERIMFZYPFJAV-UHFFFAOYSA-N 0.000 description 1
- LVEOKSIILWWVEO-UHFFFAOYSA-N tetradecyl 3-(3-oxo-3-tetradecoxypropyl)sulfanylpropanoate Chemical compound CCCCCCCCCCCCCCOC(=O)CCSCCC(=O)OCCCCCCCCCCCCCC LVEOKSIILWWVEO-UHFFFAOYSA-N 0.000 description 1
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- LLZRNZOLAXHGLL-UHFFFAOYSA-J titanic acid Chemical compound O[Ti](O)(O)O LLZRNZOLAXHGLL-UHFFFAOYSA-J 0.000 description 1
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- LDGFRUUNCRYSQK-UHFFFAOYSA-N triazin-4-ylmethanediamine Chemical compound NC(N)C1=CC=NN=N1 LDGFRUUNCRYSQK-UHFFFAOYSA-N 0.000 description 1
- STCOOQWBFONSKY-UHFFFAOYSA-N tributyl phosphate Chemical compound CCCCOP(=O)(OCCCC)OCCCC STCOOQWBFONSKY-UHFFFAOYSA-N 0.000 description 1
- VLCLHFYFMCKBRP-UHFFFAOYSA-N tricalcium;diborate Chemical compound [Ca+2].[Ca+2].[Ca+2].[O-]B([O-])[O-].[O-]B([O-])[O-] VLCLHFYFMCKBRP-UHFFFAOYSA-N 0.000 description 1
- MZHULIWXRDLGRR-UHFFFAOYSA-N tridecyl 3-(3-oxo-3-tridecoxypropyl)sulfanylpropanoate Chemical compound CCCCCCCCCCCCCOC(=O)CCSCCC(=O)OCCCCCCCCCCCCC MZHULIWXRDLGRR-UHFFFAOYSA-N 0.000 description 1
- WEAPVABOECTMGR-UHFFFAOYSA-N triethyl 2-acetyloxypropane-1,2,3-tricarboxylate Chemical compound CCOC(=O)CC(C(=O)OCC)(OC(C)=O)CC(=O)OCC WEAPVABOECTMGR-UHFFFAOYSA-N 0.000 description 1
- DQWPFSLDHJDLRL-UHFFFAOYSA-N triethyl phosphate Chemical compound CCOP(=O)(OCC)OCC DQWPFSLDHJDLRL-UHFFFAOYSA-N 0.000 description 1
- 125000002023 trifluoromethyl group Chemical group FC(F)(F)* 0.000 description 1
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- WVLBCYQITXONBZ-UHFFFAOYSA-N trimethyl phosphate Chemical compound COP(=O)(OC)OC WVLBCYQITXONBZ-UHFFFAOYSA-N 0.000 description 1
- XZZNDPSIHUTMOC-UHFFFAOYSA-N triphenyl phosphate Chemical compound C=1C=CC=CC=1OP(OC=1C=CC=CC=1)(=O)OC1=CC=CC=C1 XZZNDPSIHUTMOC-UHFFFAOYSA-N 0.000 description 1
- FIQMHBFVRAXMOP-UHFFFAOYSA-N triphenylphosphane oxide Chemical compound C=1C=CC=CC=1P(C=1C=CC=CC=1)(=O)C1=CC=CC=C1 FIQMHBFVRAXMOP-UHFFFAOYSA-N 0.000 description 1
- WTLBZVNBAKMVDP-UHFFFAOYSA-N tris(2-butoxyethyl) phosphate Chemical compound CCCCOCCOP(=O)(OCCOCCCC)OCCOCCCC WTLBZVNBAKMVDP-UHFFFAOYSA-N 0.000 description 1
- GTRSAMFYSUBAGN-UHFFFAOYSA-N tris(2-chloropropyl) phosphate Chemical compound CC(Cl)COP(=O)(OCC(C)Cl)OCC(C)Cl GTRSAMFYSUBAGN-UHFFFAOYSA-N 0.000 description 1
- QEEHNBQLHFJCOV-UHFFFAOYSA-N tris(2-phenylphenyl) phosphate Chemical compound C=1C=CC=C(C=2C=CC=CC=2)C=1OP(OC=1C(=CC=CC=1)C=1C=CC=CC=1)(=O)OC1=CC=CC=C1C1=CC=CC=C1 QEEHNBQLHFJCOV-UHFFFAOYSA-N 0.000 description 1
- LIPMRGQQBZJCTM-UHFFFAOYSA-N tris(2-propan-2-ylphenyl) phosphate Chemical compound CC(C)C1=CC=CC=C1OP(=O)(OC=1C(=CC=CC=1)C(C)C)OC1=CC=CC=C1C(C)C LIPMRGQQBZJCTM-UHFFFAOYSA-N 0.000 description 1
- BHYQWBKCXBXPKM-UHFFFAOYSA-N tris[3-bromo-2,2-bis(bromomethyl)propyl] phosphate Chemical compound BrCC(CBr)(CBr)COP(=O)(OCC(CBr)(CBr)CBr)OCC(CBr)(CBr)CBr BHYQWBKCXBXPKM-UHFFFAOYSA-N 0.000 description 1
- NSBGJRFJIJFMGW-UHFFFAOYSA-N trisodium;stiborate Chemical compound [Na+].[Na+].[Na+].[O-][Sb]([O-])([O-])=O NSBGJRFJIJFMGW-UHFFFAOYSA-N 0.000 description 1
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- UGZADUVQMDAIAO-UHFFFAOYSA-L zinc hydroxide Chemical compound [OH-].[OH-].[Zn+2] UGZADUVQMDAIAO-UHFFFAOYSA-L 0.000 description 1
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- BNEMLSQAJOPTGK-UHFFFAOYSA-N zinc;dioxido(oxo)tin Chemical compound [Zn+2].[O-][Sn]([O-])=O BNEMLSQAJOPTGK-UHFFFAOYSA-N 0.000 description 1
- BHTBHKFULNTCHQ-UHFFFAOYSA-H zinc;tin(4+);hexahydroxide Chemical compound [OH-].[OH-].[OH-].[OH-].[OH-].[OH-].[Zn+2].[Sn+4] BHTBHKFULNTCHQ-UHFFFAOYSA-H 0.000 description 1
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- 150000003755 zirconium compounds Chemical class 0.000 description 1
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Abstract
Description
本発明は、ポリ乳酸樹脂、芳香族ポリカーボネート樹脂、顔料、フッ素系樹脂およびヒンダードフェノール系酸化防止剤を用いた樹脂組成物であり、鮮明度光沢度の高い着色外観を持つ成形品、かつ初期の成形品に焼けスジ発生のない成形品に関するものである。 The present invention is a resin composition using a polylactic acid resin, an aromatic polycarbonate resin, a pigment, a fluorine-based resin and a hindered phenol-based antioxidant, and a molded product having a colored appearance with high sharpness and glossiness, and an initial product The present invention relates to a molded product that is free from burning streaks.
ポリ乳酸樹脂は、高い融点を持ち、また溶融成形可能であることから、実用上優れた生分解性ポリマーとして期待されている。また、将来的にはバイオ原料から作られる汎用ポリマーとしての利用も期待され、射出成形、押出成形などで種々の成形品とされる。 Polylactic acid resin is expected as a practically excellent biodegradable polymer because it has a high melting point and can be melt-molded. In addition, in the future, it is expected to be used as a general-purpose polymer made from bio raw materials, and various molded products are formed by injection molding, extrusion molding, and the like.
しかしながら、ポリ乳酸樹脂は耐衝撃性と耐熱性に劣り脆いという欠点があり、特許文献1には、ポリ乳酸樹脂のビィカット軟化点改質のため、芳香族ポリカーボネート樹脂を配合することが提案されている。しかしながら、鮮明度光沢度が低く、着色性に優れる成形品が得られ難いという課題があった。 However, polylactic acid resin has the disadvantage that it is inferior in impact resistance and heat resistance and is brittle, and Patent Document 1 proposes blending an aromatic polycarbonate resin in order to improve the big cut softening point of polylactic acid resin. Yes. However, there has been a problem that it is difficult to obtain a molded article having low sharpness and glossiness and excellent colorability.
また、ポリ乳酸樹脂の着色方法として、特許文献2には顔料と顔料分散剤としてワックス系分散剤を配合することが提案されている。しかしながら、ポリ乳酸樹脂と芳香族ポリカーボネート樹脂のポリマーブレンド物に対しては、ワックス系分散剤による顔料分散剤として効果が小さく、鮮明度光沢度が低く、着色性に優れる成形品が得られ難いという課題があり、鮮明度光沢度が高く、着色性に優れる成形品が望まれていた。 As a method for coloring a polylactic acid resin, Patent Document 2 proposes blending a wax-based dispersant as a pigment and a pigment dispersant. However, for polymer blends of polylactic acid resins and aromatic polycarbonate resins, it is less effective as a pigment dispersant with wax-based dispersants, and it is difficult to obtain molded products with low sharpness and glossiness and excellent colorability. There has been a demand for a molded article that has problems, has high definition and glossiness, and is excellent in colorability.
ここで、2種以上のポリマー同士を溶融混合することは、ポリマーブレンドまたはポリマーアロイとして広く知られている。しかしながら、2種以上のポリマー同士を溶融混合した場合の多くは、粘度、分子量や分子構造などの違いにより、個々の相に分離し、粗大分散構造を有し、得られる成形品の表面に相分離による混合ムラが見られ、成形品外観に真珠光沢、表面剥離およびフローマークの発生などを引き起こし成形品外観や着色性に影響を与える課題がある。 Here, melting and mixing two or more kinds of polymers is widely known as a polymer blend or a polymer alloy. However, in many cases when two or more polymers are melt-mixed, they are separated into individual phases due to differences in viscosity, molecular weight, molecular structure, etc., and have a coarse dispersion structure. Mixing unevenness due to separation is observed, and there is a problem that the appearance of the molded product is affected by the occurrence of pearly luster, surface peeling, flow marks, and the like.
本発明のポリ乳酸樹脂と芳香族ポリカーボネートのポリマーアロイの場合も粗大分散構造を有し、成形品外観に真珠光沢、表面剥離およびフローマークの発生が認められるため、鮮明度光沢度が低く、着色性に優れる成形品が得られ難いという課題があった。 In the case of the polymer alloy of the polylactic acid resin and aromatic polycarbonate of the present invention, it has a coarse dispersion structure, and pearly luster, surface peeling and flow mark are observed in the appearance of the molded product, so the vividness and glossiness are low, and coloring There was a problem that it was difficult to obtain a molded product having excellent properties.
このような相分離を改良する方法として、次の相溶化剤を配合することが提案されている。 As a method for improving such phase separation, blending the following compatibilizing agent has been proposed.
特許文献3には、ポリ乳酸樹脂とポリカーボネートにラジカル反応開始剤を窒素雰囲気下、溶融混合することが提案されている。しかしながら、成形品外観や着色性に関しては何ら開示されていない。 Patent Document 3 proposes melt-mixing a radical reaction initiator in a polylactic acid resin and polycarbonate under a nitrogen atmosphere. However, there is no disclosure regarding the appearance or colorability of the molded product.
また、特許文献4はポリ乳酸樹脂に難燃剤と難燃助剤としてフッ素系樹脂を配合することが提案され、さらに、芳香族ポリカーボネート樹脂と顔料を配合し得ることが開示されているが、ポリマーアロイによる成形品外観や着色性の課題と具体的手段については何ら開示されてなかった。 Patent Document 4 proposes that a polylactic acid resin is blended with a fluorine-based resin as a flame retardant and a flame retardant aid, and further discloses that an aromatic polycarbonate resin and a pigment can be blended. There was no disclosure about the problems and specific means of appearance and colorability of molded articles by alloy.
また、ポリ乳酸樹脂と芳香族ポリカーボネートの樹脂組成物を射出成形した際、初期の成形品に焼けスジが入ることが多くその改善が望まれていた。
本発明は、上述した従来技術における問題点の解決を課題として検討した結果達成されたものである。 The present invention has been achieved as a result of studying the solution of the problems in the prior art described above as an issue.
したがって、本発明の目的は、ポリ乳酸樹脂と芳香族ポリカーボネート樹脂からなる着色樹脂組成物において、鮮明度光沢度の高い着色外観を持つ成形品、かつ初期の成形品に焼けスジ発生のない成形品を提供することにある。 Accordingly, an object of the present invention is to provide a colored resin composition comprising a polylactic acid resin and an aromatic polycarbonate resin, a molded product having a colored appearance with a high definition and glossiness, and a molded product that is free from burning streaks in the initial molded product. Is to provide.
前記の課題を解決するため、本発明は次の構成からなる樹脂組成物およびそれからなる成形品が前記の課題解決に合致する優れた特性を有することを見出し、本発明に到達した。 In order to solve the above-mentioned problems, the present invention has found that a resin composition having the following constitution and a molded product comprising the resin composition have excellent characteristics that meet the above-mentioned problem-solving, and have reached the present invention.
すなわち、本発明は、
(イ)(A)ポリ乳酸樹脂80〜20重量%、(B)芳香族ポリカーボネート樹脂20〜80重量%、さらに、(A)と(B)成分の合計100重量部に対し、(C)顔料0.1〜20重量部、(D)フッ素系樹脂0.1〜10重量部および(E)ヒンダードフェノール系酸化防止剤0.01〜10重量部を配合してなる樹脂組成物、
(ロ)さらに、(C)顔料100重量部に対し、酸化チタンを1〜50重量部配合してなる(イ)に記載の樹脂組成物、
(ハ)前記(D)フッ素系樹脂がポリテトラフルオロエチレンである(イ)〜(ロ)のいずれか1項に記載の樹脂組成物、
(ニ)前記(D)フッ素系樹脂がアクリル変性ポリテトラフルオロエチレンである(イ)〜(ハ)のいずれか1項に記載の樹脂組成物、
(ホ)さらに、(A)と(B)成分の合計100重量部に対し、(A)ポリ乳酸樹脂、(B)ポリカーボネート樹脂以外の(F)熱可塑性樹脂1〜100重量部を配合してなる(イ)〜(ニ)のいずれか1項に記載の樹脂組成物、
(ヘ)前記(F)熱可塑性樹脂が、(A)(B)以外のポリエステル樹脂、スチレン系樹脂、コアシェルゴムおよびポリオレフィン系共重合体である(ホ)に記載の樹脂組成物、
(ト)さらに、(G)結晶核剤を配合してなる(イ)〜(ヘ)のいずれか1項に記載の樹脂組成物、
(チ)鮮明度光沢度が0.4以上である(イ)〜(ト)のいずれか1項に記載の樹脂組成物からなる成形品である。
That is, the present invention
(A) (A) Polylactic acid resin 80 to 20% by weight, (B) Aromatic polycarbonate resin 20 to 80% by weight, and (C) Pigment with respect to a total of 100 parts by weight of components (A) and (B) 0.1 to 20 parts by weight, (D) 0.1 to 10 parts by weight of a fluororesin, and (E) 0.01 to 10 parts by weight of a hindered phenol antioxidant,
(B) Furthermore, (C) 1-50 parts by weight of titanium oxide is blended with 100 parts by weight of pigment, and the resin composition according to (a),
(C) The resin composition according to any one of (A) to (B), wherein the (D) fluorine-based resin is polytetrafluoroethylene.
(D) The resin composition according to any one of (A) to (C), wherein the (D) fluorine-based resin is acrylic-modified polytetrafluoroethylene,
(E) Furthermore, for 100 parts by weight of the total of the components (A) and (B), (F) 1-100 parts by weight of (F) thermoplastic resin other than (A) polylactic acid resin and (B) polycarbonate resin are blended. The resin composition according to any one of (i) to (d),
(F) The resin composition according to (e), wherein the thermoplastic resin (F) is a polyester resin other than (A) or (B), a styrene resin, a core shell rubber, and a polyolefin copolymer,
(G) The resin composition according to any one of (A) to (F), further comprising (G) a crystal nucleating agent,
(H) A molded article made of the resin composition according to any one of (i) to (g) having a sharpness and glossiness of 0.4 or more.
本発明の樹脂組成物から得られる成形品は、鮮明度光沢度に優れ、かつ焼けスジ発生のない成形品であり、上記の特性を生かして、機械機構部品、電気・電子部品、建築部材、自動車部品および日用品など各種用途に有効に利用することができる。 The molded product obtained from the resin composition of the present invention is a molded product that is excellent in sharpness and gloss and does not cause burn streaks, taking advantage of the above characteristics, mechanical mechanism parts, electrical / electronic parts, building members, It can be effectively used for various applications such as automobile parts and daily necessities.
以下、本発明について詳細に説明する。 Hereinafter, the present invention will be described in detail.
本発明に用いられる(A)ポリ乳酸樹脂とは、L−乳酸及び/またはD−乳酸を主たる構成成分とするポリマーであるが、乳酸以外の他の共重合成分を含んでいてもよい。他のモノマー単位としては、エチレングリコール、ブロピレングリコール、ブタンジオール、ヘプタンジオール、ヘキサンジオール、オクタンジオール、ノナンジオ−ル、デカンジオール、1,4−シクロヘキサンジメタノ−ル、ネオペンチルグリコール、グリセリン、ペンタエリスリトール、ビスフェノ−ルA、ポリエチレングリコール、ポリプロピレングリコールおよびポリテトラメチレングリコールなどのグリコール化合物、シュウ酸、アジピン酸、セバシン酸、アゼライン酸、ドデカンジオン酸、マロン酸、グルタル酸、シクロヘキサンジカルボン酸、テレフタル酸、イソフタル酸、フタル酸、ナフタレンジカルボン酸、ビス(p−カルボキシフェニル)メタン、アントラセンジカルボン酸、4,4’−ジフェニルエーテルジカルボン酸、5−ナトリウムスルホイソフタル酸、5−テトラブチルホスホニウムイソフタル酸などのジカルボン酸、グリコール酸、ヒドロキシプロピオン酸、ヒドロキシ酪酸、ヒドロキシ吉草酸、ヒドロキシカプロン酸、ヒドロキシ安息香酸などのヒドロキシカルボン酸、およびカプロラクトン、バレロラクトン、プロピオラクトン、ウンデカラクトン、1,5−オキセパン−2−オンなどのラクトン類を挙げることができる。このような他の共重合成分は、全単量体成分に対し、0〜30モル%であることが好ましく、0〜10モル%であることが好ましい。 The (A) polylactic acid resin used in the present invention is a polymer mainly composed of L-lactic acid and / or D-lactic acid, but may contain other copolymerization components other than lactic acid. Other monomer units include ethylene glycol, propylene glycol, butanediol, heptanediol, hexanediol, octanediol, nonanediol, decanediol, 1,4-cyclohexanedimethanol, neopentyl glycol, glycerin, pentane. Glycol compounds such as erythritol, bisphenol A, polyethylene glycol, polypropylene glycol and polytetramethylene glycol, oxalic acid, adipic acid, sebacic acid, azelaic acid, dodecanedioic acid, malonic acid, glutaric acid, cyclohexanedicarboxylic acid, terephthalic acid , Isophthalic acid, phthalic acid, naphthalenedicarboxylic acid, bis (p-carboxyphenyl) methane, anthracene dicarboxylic acid, 4,4′-diphenyl ether dicarbohydrate Acids, dicarboxylic acids such as 5-sodium sulfoisophthalic acid, 5-tetrabutylphosphonium isophthalic acid, hydroxycarboxylic acids such as glycolic acid, hydroxypropionic acid, hydroxybutyric acid, hydroxyvaleric acid, hydroxycaproic acid, hydroxybenzoic acid, and caprolactone And lactones such as valerolactone, propiolactone, undecalactone, and 1,5-oxepan-2-one. Such other copolymerization component is preferably 0 to 30 mol%, and preferably 0 to 10 mol%, based on all monomer components.
本発明においては、相溶性の点から、乳酸成分の光学純度が高い(A)ポリ乳酸樹脂を用いることが好ましい。すなわち、(A)ポリ乳酸樹脂の総乳酸成分の内、L体が80%以上含まれるかあるいはD体が80%以上含まれることが好ましく、L体が90%以上含まれるかあるいはD体が90%以上含まれることが特に好ましく、L体が95%以上含まれるかあるいはD体が95%以上含まれることが更に好ましく、L体が98%以上含まれるかあるいはD体が98%以上含まれることが更に好ましい。 In the present invention, it is preferable to use a polylactic acid resin (A) in which the optical purity of the lactic acid component is high from the viewpoint of compatibility. That is, (A) Of the total lactic acid components of the polylactic acid resin, it is preferable that the L-form is contained in 80% or more, or the D-form is contained in 80% or more, and the L-form is contained in 90% or more or the D-form is contained. It is particularly preferably 90% or more, more preferably 95% or more of L isomer or 95% or more of D isomer, 98% or more of L isomer, or 98% or more of D isomer. More preferably.
また、L体が80%以上含まれるポリ乳酸とD体が80%以上含まれるポリ乳酸を併用して用いることも好ましく、L体が90%以上含まれるポリ乳酸とD体が90%以上含まれるポリ乳酸を併用して用いることがさらに好ましい。 It is also preferable to use a polylactic acid containing 80% or more of L-form and a polylactic acid containing 80% or more of D-form. It contains 90% or more of polylactic acid containing 90% or more of L-form and D-form. It is more preferable to use polylactic acid in combination.
(A)ポリ乳酸樹脂は、変性したものを用いてもよく、例えば、無水マレイン酸変性ポリ乳酸樹脂、エポキシ変性ポリ乳酸樹脂、アミン変性ポリ乳酸樹脂などを用いることにより、耐熱性だけでなく、機械特性も向上する傾向にあり好ましい。 (A) The polylactic acid resin may be modified, for example, by using maleic anhydride-modified polylactic acid resin, epoxy-modified polylactic acid resin, amine-modified polylactic acid resin, etc., not only heat resistance, The mechanical properties tend to be improved, which is preferable.
(A)ポリ乳酸樹脂の製造方法としては、公知の重合方法を用いることができ、乳酸からの直接重合法、およびラクチドを介する開環重合法などを挙げることができる。 (A) As a manufacturing method of a polylactic acid resin, a well-known polymerization method can be used, and the direct polymerization method from lactic acid, the ring-opening polymerization method via a lactide, etc. can be mentioned.
(A)ポリ乳酸樹脂の分子量や分子量分布については、実質的に成形加工が可能であれば特に制限されるものではないが、重量平均分子量としては、通常1万以上、好ましくは4万以上、さらに8万以上であることが望ましい。上限としては、成形時の流動性の点から35万以下であることが好ましい。ここでいう重量平均分子量とは、ゲルパーミテーションクロマトグラフィーで測定したポリメチルメタクリレート(PMMA)換算の分子量をいう。 (A) The molecular weight or molecular weight distribution of the polylactic acid resin is not particularly limited as long as it can be substantially molded, but the weight average molecular weight is usually 10,000 or more, preferably 40,000 or more, Furthermore, it is desirable that it is 80,000 or more. The upper limit is preferably 350,000 or less from the viewpoint of fluidity during molding. The weight average molecular weight here refers to the molecular weight in terms of polymethyl methacrylate (PMMA) measured by gel permeation chromatography.
(A)ポリ乳酸樹脂の融点については、特に制限されるものではないが、120℃以上であることが好ましく、さらに150℃以上であることが好ましい。(A)ポリ乳酸樹脂の融点は光学純度が高いほど高くなる傾向にあるため、上記融点の高いポリ乳酸樹脂は、光学純度の高いポリ乳酸樹脂を用いればよい。 (A) Although it does not restrict | limit especially about melting | fusing point of a polylactic acid resin, It is preferable that it is 120 degreeC or more, and also it is preferable that it is 150 degreeC or more. (A) Since the melting point of the polylactic acid resin tends to increase as the optical purity increases, the polylactic acid resin having a high melting point may be a polylactic acid resin having a high optical purity.
また、(A)ポリ乳酸樹脂を超えない配合量でセルロースエステルを配合しても良い。前記のセルロースエステルとは、セルロースの水酸基がエステル化剤によって封鎖されているものを言う。具体的なエステル化剤としは、塩化アセチル、塩化プロピオニルなどの酸塩基物、無水酢酸、無水ピロピオン酸、無水酪酸などの酸無水物、アミド化合物、エステル化合物などのカルボン酸化合物誘導体、およびε−カプロラクトンなどの環状エステルなどが挙げられ、具体的なセルロースエステルの種類としては、セルロースアセテート、セルロースジアセテートセルローストリアセテート、セルロースアセテートプロピオネート、セルロースアセテートブチレート、セルロースアセテートフタレートなどが挙げられ、(A)ポリ乳酸樹脂との相溶性または混和性の観点から、セルロースジアセテート、セルローストリアセテート、セルロースアセテートプロピオネート、セルロースアセテートブチレート、セルロースアセテートフタレートが好ましく、さらにはセルローストリアセテート、セルロースアセテートプロピオネートがより好ましい。 Moreover, you may mix | blend a cellulose ester with the compounding quantity which does not exceed (A) polylactic acid resin. The cellulose ester refers to one in which the hydroxyl group of cellulose is blocked with an esterifying agent. Specific esterifying agents include acid bases such as acetyl chloride and propionyl chloride, acid anhydrides such as acetic anhydride, pyropionic acid and butyric anhydride, carboxylic acid compound derivatives such as amide compounds and ester compounds, and ε- Specific examples of cellulose esters include cellulose acetate, cellulose diacetate, cellulose triacetate, cellulose acetate propionate, cellulose acetate butyrate, and cellulose acetate phthalate. ) From the viewpoint of compatibility or miscibility with polylactic acid resin, cellulose diacetate, cellulose triacetate, cellulose acetate propionate, cellulose acetate butyrate, cellulose acetate phthalate It is preferred, and cellulose triacetate, and more preferably cellulose acetate propionate.
また、セルロースにおける水酸基の置換度(セルロースエステルに置換された水酸基の平均個数)は、グルコース単位あたり0.5〜2.9であることが好ましい。また、(A)ポリ乳酸樹脂とのより良好な相溶性または混和性の観点から、置換度は1.5〜2.9であることが好ましく、また2.0〜2.8であることがより好ましい。また、上記の置換度は、アルカリ加水分解により生成したエステル化剤を高速液体クロマトグラフィーに供し定量することによって求めることができる。 Moreover, it is preferable that the substitution degree of the hydroxyl group in cellulose (average number of hydroxyl groups substituted by cellulose ester) is 0.5 to 2.9 per glucose unit. In addition, from the viewpoint of better compatibility or miscibility with (A) polylactic acid resin, the degree of substitution is preferably 1.5 to 2.9, and more preferably 2.0 to 2.8. More preferred. Moreover, said substitution degree can be calculated | required by using and esterifying the esterifying agent produced | generated by alkaline hydrolysis to a high performance liquid chromatography.
本発明における(B)芳香族ポリカーボネート樹脂とは、芳香族二価フェノール系化合物とホスゲン、または炭酸ジエステルとを反応させることにより得られる芳香族ホモまたはコポリカーボネートなどの芳香族ポリカーボネートが挙げられる。 Examples of the aromatic polycarbonate resin (B) in the present invention include aromatic polycarbonates such as aromatic homo- or copolycarbonates obtained by reacting aromatic dihydric phenol compounds with phosgene or diester carbonate.
また、前記の芳香族二価フェノール系化合物としては、2,2−ビス(4−ヒドロキシフェニル)プロパン、2,2−ビス(4−ヒドロキシ−3,5−ジメチルフェニル)プロパン、ビス(4−ヒドロキシフェニル)メタン、1,1−ビス(4−ヒドロキシフェニル)エタン、2,2−ビス(4−ヒドロキシフェニル)ブタン、2,2−ビス(4−ヒドロキシ−3,5−ジフェニル)ブタン、2,2−ビス(4−ヒドロキシ−3,5−ジエチルフェニル)プロパン、2,2−ビス(4−ヒドロキシ−3,5−ジエチルフェニル)プロパン、1,1−ビス(4−ヒドロキシフェニル)シクロヘキサン、1−フェニル−1,1−ビス(4−ヒドロキシフェニル)エタン等が使用でき、これら単独あるいは混合物として使用することができる。 Examples of the aromatic dihydric phenol compound include 2,2-bis (4-hydroxyphenyl) propane, 2,2-bis (4-hydroxy-3,5-dimethylphenyl) propane, and bis (4- Hydroxyphenyl) methane, 1,1-bis (4-hydroxyphenyl) ethane, 2,2-bis (4-hydroxyphenyl) butane, 2,2-bis (4-hydroxy-3,5-diphenyl) butane, 2 , 2-bis (4-hydroxy-3,5-diethylphenyl) propane, 2,2-bis (4-hydroxy-3,5-diethylphenyl) propane, 1,1-bis (4-hydroxyphenyl) cyclohexane, 1-phenyl-1,1-bis (4-hydroxyphenyl) ethane or the like can be used, and these can be used alone or as a mixture.
(A)ポリ乳酸樹脂と(B)芳香族ポリカーボネートの配合比率は、射出成形時の成形サイクルと熱変形温度の観点から、(A)ポリ乳酸樹脂80〜20重量%と(B)芳香族ポリカーボネート樹脂20〜80重量%が好ましく、(A)ポリ乳酸樹脂75〜25重量%と(B)芳香族ポリカーボネート樹脂25〜75重量%であることがより好ましく、(A)ポリ乳酸樹脂70〜30重量%と(B)芳香族ポリカーボネート樹脂30〜70重量%であることが特に好ましい。 The blending ratio of (A) polylactic acid resin and (B) aromatic polycarbonate is (A) polylactic acid resin 80 to 20% by weight and (B) aromatic polycarbonate from the viewpoint of the molding cycle and heat distortion temperature during injection molding. The resin is preferably 20 to 80% by weight, more preferably (A) 75 to 25% by weight of the polylactic acid resin and (B) 25 to 75% by weight of the aromatic polycarbonate resin, and (A) 70 to 30% by weight of the polylactic acid resin. % And (B) 30 to 70% by weight of the aromatic polycarbonate resin is particularly preferable.
本発明において、(A)ポリ乳酸樹脂に(B)芳香族ポリカーボネート樹脂を配合することで、(A)ポリ乳酸樹脂の射出成形時の成形サイクルと熱変形温度を改質することができ、(B)芳香族ポリカーボネート樹脂の配合量が20重量%未満では前記の改質効果が不十分であり、(B)芳香族ポリカーボネート樹脂の配合量が80重量%を超えると成形品外観に透明感が出るため好ましくない。 In the present invention, by blending the (A) polylactic acid resin with the (B) aromatic polycarbonate resin, the molding cycle and the heat distortion temperature during the injection molding of the (A) polylactic acid resin can be modified. B) When the blending amount of the aromatic polycarbonate resin is less than 20% by weight, the above-described modification effect is insufficient. When the blending amount of the (B) aromatic polycarbonate resin exceeds 80% by weight, the appearance of the molded product is transparent. Because it comes out, it is not preferable.
本発明における(C)顔料とは、水や油に溶解しない色材であり、無機顔料と有機顔料に大別され、無機顔料としては天然鉱物顔料、合成無機顔料およびセラミック顔料などが挙げられ、有機顔料としては、アゾ系顔料、多環式系顔料およびレーキ顔料などが挙げられる。好ましく用いられる顔料の具体例としては、カーボンブラック、酸化チタン、酸化鉄、弁柄、群青、紺青、焼成イエロー、酸化亜鉛、キナクリドン、フタロシアニンブルー、フタロシアニングリーンおよびアゾ系顔料などが挙げられ一種以上で用いられる。また、水や油に溶解する種々の色の染料をさらに1種以上併用配合し、種々の色に着色することも可能である。前記の(C)顔料の配合量は、(A)ポリ乳酸樹脂と(B)芳香族ポリカーボネート樹脂100重量部に対し、0.1〜20重量部、好ましくは0.2〜15重量部、より好ましくは0.3〜10重量部であり、0.1重量部未満では顔料の濃度が低すぎて所望する色に調色することが困難であり、20重量部を超すと衝撃強度や機械的性質を低下させるため好ましくない。 The (C) pigment in the present invention is a color material that does not dissolve in water or oil, and is roughly classified into inorganic pigments and organic pigments, and examples of inorganic pigments include natural mineral pigments, synthetic inorganic pigments, and ceramic pigments. Examples of organic pigments include azo pigments, polycyclic pigments, lake pigments, and the like. Specific examples of pigments that are preferably used include carbon black, titanium oxide, iron oxide, dial, ultramarine, bitumen, calcined yellow, zinc oxide, quinacridone, phthalocyanine blue, phthalocyanine green, and azo pigments. Used. In addition, it is possible to further mix one or more dyes of various colors that dissolve in water or oil and color them in various colors. The blending amount of the (C) pigment is 0.1 to 20 parts by weight, preferably 0.2 to 15 parts by weight, based on 100 parts by weight of (A) polylactic acid resin and (B) aromatic polycarbonate resin. Preferably, the amount is 0.3 to 10 parts by weight. If the amount is less than 0.1 part by weight, it is difficult to adjust the pigment color to a desired color, and if it exceeds 20 parts by weight, impact strength and mechanical strength are increased. This is not preferable because the properties are deteriorated.
また、とくに黒色や紺色など濃い色の着色は難しく、鮮明度光沢度を高くするにはカーボンブラックなどの顔料を多量に配合する必要があったが、カーボンブラック100重量部に酸化チタンを1〜50重量部配合したところ、鮮明度光沢度が大きく改善された。したがって、黒色や紺色など濃い色の調色には、鮮明度光沢度を高くするため、(C)顔料と共に酸化チタンを併用配合することが好ましく、(C)顔料100重量部に対し、1〜50重量部が好ましく、より好ましくは2〜30重量であり、1重量部未満では鮮明度光沢度の改善効果が少なく、50重量部を超すと所望する色の調色が難しくなるため好ましくない。なお、ここで用いる酸化チタンは本発明の熱可塑性樹脂および/または顔料と混合して用いても良く、酸化チタンを任意の段階で配合しても良い。 In particular, it is difficult to color dark colors such as black and amber, and it is necessary to blend a large amount of pigments such as carbon black in order to increase the sharpness and glossiness. When 50 parts by weight was blended, sharpness and glossiness were greatly improved. Therefore, in order to increase the vividness and glossiness of dark colors such as black and amber, it is preferable to combine titanium oxide together with (C) pigment, and (C) 1 to 100 parts by weight of pigment. 50 parts by weight is preferable, more preferably 2 to 30 parts by weight. If it is less than 1 part by weight, the effect of improving the sharpness and glossiness is small, and if it exceeds 50 parts by weight, the desired color toning becomes difficult, which is not preferable. In addition, the titanium oxide used here may be used by mixing with the thermoplastic resin and / or pigment of the present invention, and titanium oxide may be blended at an arbitrary stage.
また、前記のカーボンブラックとしては、限定されるものではないが、チャンネルブラック、ファーネスブラック、アセチレンブラック、アントラセンブラック、油煙、松煙、植物黒、動物黒および、黒鉛などが挙げられ、平均粒径20μm以下、ジブチルフタレート吸油量50〜400cm3/100gのカーボンブラックが好ましく用いられ、処理剤として酸化アルミニウム、酸化珪素、酸化亜鉛、酸化ジルコニウム、ポリオール、シランカップリング剤などで処理されていても良い。 Examples of the carbon black include, but are not limited to, channel black, furnace black, acetylene black, anthracene black, oil smoke, pine smoke, plant black, animal black, and graphite. 20μm or less, carbon black dibutyl phthalate absorption 50~400cm 3 / 100g is preferably used, aluminum oxide treatment agent, silicon oxide, zinc oxide, zirconium oxide, polyol, it may be treated with a silane coupling agent .
また、前記の酸化チタンとしては、ルチル形、あるいはアナターゼ形などの結晶形を持ち、平均粒子径20μm以下の酸化チタンが好ましく用いられ、処理剤として酸化アルミニウム、酸化珪素、酸化亜鉛、酸化ジルコニウム、ポリオール、シランカップリング剤などで処理されていても良い。また、上記のカーボンブラック、酸化チタン、および種々の色の顔料や染料は、本発明の樹脂組成物との分散性向上や製造時のハンドリング性の向上のため、種々の熱可塑性樹脂と溶融ブレンドあるいは単にブレンドした混合材料(色材マスターあるいはマスターペレット)に加工して用いても良い。また、前記の熱可塑性樹脂としては、ポリ乳酸樹脂や芳香族ポリカーボネート樹脂が好ましく、ポリ乳酸樹脂がとくに好ましく用いられ、前記のマスターあるいはマスターペレット中に含有するカーボンブラック、酸化チタン、および種々の色の顔料や染料の配合量は多いほど好ましく、少なくとも5重量%を超える配合量が好ましい。 Further, as the titanium oxide, titanium oxide having a crystal form such as rutile form or anatase form and having an average particle diameter of 20 μm or less is preferably used, and aluminum oxide, silicon oxide, zinc oxide, zirconium oxide, It may be treated with a polyol, a silane coupling agent or the like. In addition, the above-mentioned carbon black, titanium oxide, and various color pigments and dyes are melt blended with various thermoplastic resins in order to improve dispersibility with the resin composition of the present invention and to improve handling during production. Alternatively, it may be processed into a blended mixed material (coloring material master or master pellet). The thermoplastic resin is preferably a polylactic acid resin or an aromatic polycarbonate resin, particularly preferably a polylactic acid resin, and carbon black, titanium oxide, and various colors contained in the master or master pellet. The amount of the pigment or dye is preferably as large as possible, and is preferably at least 5% by weight.
本発明における(D)フッ素系樹脂とは、物質分子中にフッ素を含有する樹脂であり、具体的には、ポリテトラフルオロエチレン、ポリヘキサフルオロプロピレン、テトラフルオロエチレン/ヘキサフルオロプロピレン共重合体、テトラフルオロエチレン/パーフルオロアルキルビニルエーテル共重合体、テトラフルオロエチレン/エチレン共重合体、ヘキサフルオロプロピレン/プロピレン共重合体、ポリビニリデンフルオライド、ビニリデンフルオライド/エチレン共重合体などが挙げられるが、中でもポリテトラフルオロエチレン、テトラフルオロエチレン/パーフルオロアルキルビニルエーテル共重合体、テトラフルオロエチレン/ヘキサフルオロプロピレン共重合体、テトラフルオロエチレン/エチレン共重合体、ポリビニリデンフルオライドが好ましく、特にポリテトラフルオロエチレン、テトラフルオロエチレン/エチレン共重合体が好ましく、さらにはポリテトラフルオロエチレンが好ましく、ポリテトラフルオロエチレン粒子とアクリル系重合体とからなるアクリル変性ポリテトラフルオロエチレンも好ましく用いられる。また、ポリテトラフルオロエチレンなどのフッ素系樹脂の分子量は1万〜1000万の範囲のものが好ましく、とくに10万〜100万の範囲のものがより好ましく用いられる。前記のポリテトラフルオロエチレンの市販品としては、三井・デュポンフロロケミカル(株)製の“テフロン(登録商標)”6−J、“テフロン(登録商標)”6C−J、“テフロン(登録商標)”62−J、旭アイシーアイフロロポリマーズ(株)製の“フルオン”CD1やCD076などが市販されている。また、ポリテトラフルオロエチレン粒子と有機系重合体とからなるアクリル変成ポリテトラフルオロエチレンの市販品としては、三菱レイヨン(株)から、“メタブレン(登録商標)”Aシリーズとして市販され、“メタブレン(登録商標)”A−3000、“メタブレン(登録商標)”A−3800などが市販されている。また、ポリテトラフルオロエチレンの“テフロン(登録商標)”6−Jなどは凝集し易いため、他の樹脂組成物と共にヘンシェルミキサーなどで機械的に強く混合すると凝集により塊が生じる場合があり、混合条件によってはハンドリング性や分散性に課題がある。一方、ポリテトラフルオロエチレン粒子とアクリル系重合体とからなるポリテトラフルオロエチレン含有混合粉体は前記のハンドリング性や分散性に優れ、とくに好ましく用いられる。前記のポリテトラフルオロエチレン粒子とアクリル系重合体とからなるポリテトラフルオロエチレン含有混合粉体とは、限定されるものではないが、特開2000−226523号公報で開示されているポリテトラフルオロエチレン粒子と有機系重合体とからなるポリテトラフルオロエチレン含有混合粉体などが挙げられ、前記の有機系重合体としては芳香族ビニル系単量体、アクリル酸エステル系単量体、およびシアン化ビニル系単量体を10重量%以上含有するアクリル系重合体などであり、それらの混合物でもよく、ポリテトラフルオロエチレン含有混合粉体中のポリテトラフルオロエチレンの含有量は0.1重量%〜90重量%であることが好ましい。 The (D) fluorine-based resin in the present invention is a resin containing fluorine in a substance molecule, specifically, polytetrafluoroethylene, polyhexafluoropropylene, tetrafluoroethylene / hexafluoropropylene copolymer, Tetrafluoroethylene / perfluoroalkyl vinyl ether copolymer, tetrafluoroethylene / ethylene copolymer, hexafluoropropylene / propylene copolymer, polyvinylidene fluoride, vinylidene fluoride / ethylene copolymer, etc. Polytetrafluoroethylene, tetrafluoroethylene / perfluoroalkyl vinyl ether copolymer, tetrafluoroethylene / hexafluoropropylene copolymer, tetrafluoroethylene / ethylene copolymer, polyvinylidene Fluoride is preferred, especially polytetrafluoroethylene and tetrafluoroethylene / ethylene copolymer, more preferably polytetrafluoroethylene, and acrylic modified polytetrafluoroethylene comprising polytetrafluoroethylene particles and an acrylic polymer is also preferred. Preferably used. Further, the molecular weight of the fluorine-based resin such as polytetrafluoroethylene is preferably in the range of 10,000 to 10,000,000, and more preferably in the range of 100,000 to 1,000,000. Commercially available products of the above-mentioned polytetrafluoroethylene include “Teflon (registered trademark)” 6-J, “Teflon (registered trademark)” 6C-J, and “Teflon (registered trademark)” manufactured by Mitsui DuPont Fluorochemical Co., Ltd. “62-J,“ Full-on ”CD1 and CD076 manufactured by Asahi IC Fluoropolymers Co., Ltd. are commercially available. A commercial product of acrylic modified polytetrafluoroethylene composed of polytetrafluoroethylene particles and an organic polymer is commercially available from Mitsubishi Rayon Co., Ltd. as “Metabrene (registered trademark)” A series. (Registered trademark) “A-3000”, “metabrene (registered trademark)” A-3800, etc. are commercially available. In addition, polytetrafluoroethylene “Teflon (registered trademark)” 6-J and the like are prone to agglomerate, so if they are mechanically strongly mixed with other resin compositions using a Henschel mixer or the like, agglomeration may occur due to aggregation. There are problems in handling and dispersibility depending on conditions. On the other hand, a polytetrafluoroethylene-containing mixed powder composed of polytetrafluoroethylene particles and an acrylic polymer is excellent in handling properties and dispersibility, and is particularly preferably used. The polytetrafluoroethylene-containing mixed powder composed of the polytetrafluoroethylene particles and the acrylic polymer is not limited, but polytetrafluoroethylene disclosed in Japanese Patent Application Laid-Open No. 2000-226523. Polytetrafluoroethylene-containing mixed powder composed of particles and an organic polymer, and the like. Examples of the organic polymer include aromatic vinyl monomers, acrylate monomers, and vinyl cyanide. An acrylic polymer containing 10% by weight or more of a monomer, and a mixture thereof. The content of polytetrafluoroethylene in the polytetrafluoroethylene-containing mixed powder is 0.1 to 90% by weight. It is preferable that it is weight%.
また、(D)フッ素系樹脂の配合量は、(A)ポリ乳酸樹脂と(B)芳香族ポリカーボネート樹脂100重量部に対し、0.1〜10重量部であり、好ましくは0.2〜8重量部が好ましく、より好ましくは0.3〜6重量部が好ましく、(D)フッ素系樹脂からなる顔料分散剤の配合量が10重量部を超すと本発明の熱変形温度や流動性が低下するため好ましくない。 The blending amount of (D) fluorine-based resin is 0.1 to 10 parts by weight, preferably 0.2 to 8 parts per 100 parts by weight of (A) polylactic acid resin and (B) aromatic polycarbonate resin. Parts by weight are preferred, more preferably 0.3 to 6 parts by weight, and if the blending amount of the pigment dispersant comprising (D) a fluororesin exceeds 10 parts by weight, the heat distortion temperature and fluidity of the present invention are reduced. Therefore, it is not preferable.
本発明における(E)ヒンダードフェノール系酸化防止剤とは、(A)ポリ乳酸樹脂、(B)芳香族ポリカーボネート、(C)顔料および(D)フッ素系樹脂から得られる樹脂組成物を射出成形した際、初期の成形品に焼けスジが入る課題があり、その改善を目的に配合する酸化防止剤である。 The (E) hindered phenol antioxidant in the present invention is an injection molding of a resin composition obtained from (A) a polylactic acid resin, (B) an aromatic polycarbonate, (C) a pigment, and (D) a fluorine resin. In this case, there is a problem that burn lines are generated in the initial molded product, and the antioxidant is blended for the purpose of improvement.
本発明で使用する(E)ヒンダードフェノール系酸化防止剤の具体例としては、トリエチレングリコール−ビス[3−(3−t−ブチル−5−メチル−4−ヒドロキシフェニル)プロピオネート]、ペンタエリスリチル−テトラキス[3−(3,5−ジ−t−ブチル−4−ヒドロキシフェニル)プロピオネート]、1.6−ヘキサンジオール−ビス[3−(3,5−ジ−t−ブチル−4−ヒドロキシフェニル)プロピオネート、オクタドデシル−3−(3,5−ジ−t−ブチル−4−ヒドロキシフェニル)プロピオネート、N,N’−ヘキサメチレンビス(3,5−ジ−t−ブチル−4−ヒドロキシ−ヒドロシンナマミド、3,5−ジ−t−ブチル−4−ヒドロキシ−ベンジルフォスフォネート−ジエチルエステルおよび1,3,5−トリメチル−2,4,6−トリス(3,5−ジ−t−ブチル−4−ヒドロキシベンジル)ベンゼンなどが挙げられる。 Specific examples of the (E) hindered phenol antioxidant used in the present invention include triethylene glycol-bis [3- (3-tert-butyl-5-methyl-4-hydroxyphenyl) propionate], pentaerythris Lithyl-tetrakis [3- (3,5-di-tert-butyl-4-hydroxyphenyl) propionate], 1.6-hexanediol-bis [3- (3,5-di-tert-butyl-4-hydroxy) Phenyl) propionate, octadodecyl-3- (3,5-di-tert-butyl-4-hydroxyphenyl) propionate, N, N′-hexamethylenebis (3,5-di-tert-butyl-4-hydroxy-) Hydrocinnamamide, 3,5-di-tert-butyl-4-hydroxy-benzylphosphonate-diethyl ester and 1,3,5-trimethyl Such as Le 2,4,6-tris (3,5-di -t- butyl-4-hydroxybenzyl) benzene.
また、(E)ヒンダードフェノール系酸化防止剤の配合量は、(A)ポリ乳酸樹脂と(B)芳香族ポリカーボネート樹脂100重量部に対し、0.01〜10重量部が好ましく、0.03〜8重量部がさらに好ましく、0.01重量部未満では焼けスジ改善の効果がなく、10重量部を超すと機械的性質を低下させるため好ましくない
また、(E)ヒンダードフェノール系酸化防止剤に併用可能な安定剤としてはホスファイト系酸化防止剤、チオエーテル系酸化防止剤および光安定剤などがあり、本発明樹脂組成物の耐熱エージング性や耐光(候)性改善を目的に配合される。
Moreover, the compounding quantity of (E) hindered phenolic antioxidant is 0.01-10 weight part with respect to 100 weight part of (A) polylactic acid resin and (B) aromatic polycarbonate resin, and is 0.03. -8 parts by weight is more preferable, and if it is less than 0.01 parts by weight, there is no effect of improving the burning streak, and if it exceeds 10 parts by weight, it is not preferable because the mechanical properties are lowered. (E) Hindered phenol antioxidant As stabilizers that can be used in combination, there are phosphite-based antioxidants, thioether-based antioxidants, light stabilizers, and the like, which are blended for the purpose of improving the heat aging resistance and light resistance (weather) resistance of the resin composition of the present invention. .
前記のホスファイト系酸化防止剤としては、トリス(2,4−ジ−t−ブチルフェニル)ホスファイト、2,2−メチレンビス(4,6−ジ−t−ブチルフェニル)オクチルホスファイト、ビス(2,6−ジ−t−ブチル−4−メチルフェニル)ペンタエリスリトール−ジ−ホスファイト、テトラキス(2,4−ジ−t−ブチルフェニル)−4,4’−ビフェニレンホスホナイトなどが好ましく使用できる。前記のチオエーテル系酸化防止剤としては、ジラウリルチオジプロピオネート、ジトリデシルチオジプロピオネート、ジミリスチルチオジプロピオネート、ジステアリルチオジプロピオネート、ペンタエリスリトール−テトラキス(3−ラウリルチオプロピオネート)、ペンタエリスリトール−テトラキス(3−ドデシルチオプロピオネート)、ペンタエリスリトール−テトラキス(3−オクタデシルチオプロピオネート)、ペンタエリスリトール−テトラキス(3−ミリスチルチオプロピオネート)、ペンタエリスリトール−テトラキス(3−ステアリルチオプロピオネート)などが挙げられる。 Examples of the phosphite antioxidant include tris (2,4-di-t-butylphenyl) phosphite, 2,2-methylenebis (4,6-di-t-butylphenyl) octyl phosphite, bis ( 2,6-di-t-butyl-4-methylphenyl) pentaerythritol-di-phosphite, tetrakis (2,4-di-t-butylphenyl) -4,4′-biphenylenephosphonite can be preferably used. . Examples of the thioether-based antioxidant include dilauryl thiodipropionate, ditridecyl thiodipropionate, dimyristyl thiodipropionate, distearyl thiodipropionate, pentaerythritol tetrakis (3-lauryl thiopropionate). ), Pentaerythritol-tetrakis (3-dodecylthiopropionate), pentaerythritol-tetrakis (3-octadecylthiopropionate), pentaerythritol-tetrakis (3-myristylthiopropionate), pentaerythritol-tetrakis (3 -Stearyl thiopropionate).
前記の光安定剤としては、ベンゾフェノン系化合物、ベンゾトリアゾール系化合物、芳香族ベンゾエート系化合物、蓚酸アニリド系化合物、シアノアクリレート系化合物及びヒンダードアミン系化合物などを挙げることができる。 Examples of the light stabilizer include benzophenone compounds, benzotriazole compounds, aromatic benzoate compounds, oxalic acid anilide compounds, cyanoacrylate compounds, hindered amine compounds, and the like.
本発明における(A)ポリ乳酸樹脂、(B)芳香族ポリカーボネート樹脂以外の(F)熱可塑性樹脂とは、本発明樹脂組成物の熱変形温度あるいは耐衝撃性を改善することを目的に用いられる。 The (F) thermoplastic resin other than (A) polylactic acid resin and (B) aromatic polycarbonate resin in the present invention is used for the purpose of improving the heat distortion temperature or impact resistance of the resin composition of the present invention. .
また、(F)熱可塑性樹脂の具体例としては、(A)(B)成分以外のポリエステル樹脂、ポリスチレン樹脂やスチレン系共重合体などのスチレン系樹脂、ポリフェニレンエーテル樹脂、ポリフェニレンスルフィド樹脂、ポリメタクリル酸メチル樹脂、ポリ塩化ビニル樹脂、ポリアリレート樹脂、ポリエーテルイミド樹脂、ポリエーテルエーテルケトン、ポリイミド樹脂、ポリアミドイミド樹脂、液晶芳香族ポリエステル樹脂、ポリアセタール樹脂、ポリアミド樹脂(ナイロン6、ナイロン66、ナイロン46などのポリアミド共重合体、ポリアミドエラストマーなど)、ポリエチレン樹脂、ホモあるいはブロックポリプロピレン樹脂等のポリオレフィン系樹脂、ポリオレフィン系共重合体、アクリル系ゴム、ポリウレタン樹脂、塩素化ポリエチレン樹脂、塩素化ポリプロピレン樹脂、熱可塑性澱粉樹脂、ポリエーテルスルホン樹脂、フェノキシ樹脂、熱可塑性フェノール樹脂、ポリ−4−メチルペンテン−1樹脂、コアシェルゴムおよびポリビニルアルコール樹脂が好ましく、一種以上で用いられ、(A)(B)成分以外のポリエステル樹脂、スチレン系樹脂、コアシェルゴムおよびポリオレフィン系共重合体がとくに好ましく用いられる。 Specific examples of the thermoplastic resin (F) include polyester resins other than the components (A) and (B), styrene resins such as polystyrene resins and styrene copolymers, polyphenylene ether resins, polyphenylene sulfide resins, and polymethacrylic resins. Acid methyl resin, polyvinyl chloride resin, polyarylate resin, polyetherimide resin, polyetheretherketone, polyimide resin, polyamideimide resin, liquid crystal aromatic polyester resin, polyacetal resin, polyamide resin (nylon 6, nylon 66, nylon 46 Polyamide copolymers, polyamide elastomers, etc.), polyethylene resins, polyolefin resins such as homo or block polypropylene resins, polyolefin copolymers, acrylic rubber, polyurethane resins, chlorinated poly Tylene resin, chlorinated polypropylene resin, thermoplastic starch resin, polyethersulfone resin, phenoxy resin, thermoplastic phenol resin, poly-4-methylpentene-1 resin, core shell rubber and polyvinyl alcohol resin are preferred, and one or more are used. Polyester resins other than the components (A) and (B), styrene resins, core shell rubbers, and polyolefin copolymers are particularly preferably used.
前記のとくに好ましく用いられる(A)(B)成分以外のポリエステル樹脂としては、ポリトリメチレンテレフタレート樹脂、ポリエチレンテレフタレート樹脂、ポリブチレンテレフタレート樹脂、ポリシクロヘキサンテレフタレート樹脂、ポリエステルエラストマーなどの芳香族ポリエステル樹脂、ポリエチレンテレフタレート/サクシネート樹脂、ポリブチレンサクシネート樹脂、ポリカプロラクトン樹脂などの脂肪族ポリエステル樹脂、脂肪族芳香族ポリエステル樹脂などが挙げられ、衝撃改善効果の高いポリブチレンサクシネート樹脂がとくに好ましく用いられる。 Polyester resins other than the above-described particularly preferably used components (A) and (B) include polytrimethylene terephthalate resins, polyethylene terephthalate resins, polybutylene terephthalate resins, polycyclohexane terephthalate resins, aromatic polyester resins such as polyester elastomers, polyethylene, and the like. Examples thereof include aliphatic polyester resins such as terephthalate / succinate resin, polybutylene succinate resin, and polycaprolactone resin, and aliphatic aromatic polyester resins. Polybutylene succinate resin having a high impact improving effect is particularly preferably used.
前記のとくに好ましく用いられるスチレン系樹脂とは、スチレンあるいはαーメチルスチレンに芳香族ビニル化合物、シアン化ビニル化合物、(メタ)アクリル酸アルキルエステル、およびマレイミド系単量体から選択される一種以上の単量体を重合してなる樹脂、あるいは、ポリブタジエン、ブチレンやイソプレンなどのゴム系成分にこれら単量体をグラフト重合あるいは共重合したスチレン系樹脂、(B)芳香族ポリカーボネート樹脂にスチレンをグラフト重合あるいは共重合したスチレン系樹脂などが挙げられる(以下これらを「共重合体」と総称することがある)。上記芳香族ビニル化合物としては、ビニルトルエン、および、ジビニルベンゼンなどが挙げられ、シアン化ビニル化合物としてはアクリロニトリル、およびメタクリロニトリルなどが挙げられ、(メタ)アクリル酸アルキルエステルとしては、メタクリル酸メチル、メタクリル酸エチル、メタクリル酸n−ブチル、アクリル酸メチル、アクリル酸エチル、アクリル酸n−ブチル、およびアクリル酸ステアリルなどの(メタ)アクリル酸アルキルエステル等が挙げられ、マレイミド系単量体としては、マレイミド、N−メチルマレイミド、N−エチルマレイミド、N−フェニルマレイミド、N−シクロヘキシルマレイミド、およびその誘導体などのN−置換マレイミドなどが挙げられる。さらに、スチレン系共重合体と共重合が可能な下記の成分との共重合体も本発明に含まれる。かかる共重合が可能な成分の具体例としては、ジエン化合物、マレイン酸ジアルキルエステル、アリルアルキルエーテル、不飽和アミノ化合物、およびビニルアルキルエーテルなどが挙げられる。また、不飽和酸無水物あるいはエポキシ基含有ビニル系単量体をグラフト重合もしくは共重合されたスチレン系樹脂も本発明に含まれる。 The particularly preferably used styrenic resin is one or more kinds of styrene or α-methylstyrene selected from aromatic vinyl compounds, vinyl cyanide compounds, (meth) acrylic acid alkyl esters, and maleimide monomers. A polymer obtained by polymerizing a polymer, a styrene resin obtained by graft polymerization or copolymerization of these monomers with a rubber component such as polybutadiene, butylene or isoprene, or (B) graft polymerization or copolymerization of styrene with an aromatic polycarbonate resin. Examples thereof include polymerized styrene resins (hereinafter, these may be collectively referred to as “copolymers”). Examples of the aromatic vinyl compound include vinyl toluene and divinylbenzene, examples of the vinyl cyanide compound include acrylonitrile and methacrylonitrile, and examples of the (meth) acrylic acid alkyl ester include methyl methacrylate. (Meth) acrylic acid alkyl esters such as ethyl methacrylate, n-butyl methacrylate, methyl acrylate, ethyl acrylate, n-butyl acrylate, and stearyl acrylate. , N-substituted maleimides such as maleimide, N-methylmaleimide, N-ethylmaleimide, N-phenylmaleimide, N-cyclohexylmaleimide, and derivatives thereof. Furthermore, the copolymer with the following component which can be copolymerized with a styrene-type copolymer is also contained in this invention. Specific examples of components capable of such copolymerization include diene compounds, maleic acid dialkyl esters, allyl alkyl ethers, unsaturated amino compounds, and vinyl alkyl ethers. A styrene resin obtained by graft polymerization or copolymerization of an unsaturated acid anhydride or an epoxy group-containing vinyl monomer is also included in the present invention.
スチレン系樹脂の具体例としては、メタクリル酸メチル/アクリロニトリル/スチレン樹脂、アクリロニトリル/スチレン樹脂(AS樹脂)、スチレン/ブタジエン樹脂(SB樹脂)、アクリロニトリル/ブタジエン/スチレン樹脂(ABS樹脂)、スチレン/ブタジエン/スチレン樹脂(SBS樹脂)、スチレン/エチレン/ブチレン/スチレン樹脂(SEBS樹脂)、スチレン/イソプレン/スチレン樹脂(SIS樹脂)、アクリレート/アクリロニトリル/スチレン樹脂(AAS樹脂)、塩素化ポリエチレン/アクリロニトリル/スチレン樹脂(ACS樹脂)、アクリロニトリル/エチレン/スチレン樹脂(AES樹脂)、スチレン/Nーフェニルマレイミド樹脂、スチレン/アクリロニトリル/Nーフェニルマレイミド樹脂、メタクリル酸メチル/ブタジエン/スチレン樹脂(MBS樹脂)、メタクリル酸メチル/アクリロニトリル/ブタジエン/スチレン樹脂(MABS樹脂)、ハイインパクト−ポリスチレン樹脂(HI−PS樹脂)、ポリカーボネート−g−ポリスチレン、ポリカーボネート−g−ポリスチレン/ポリアクリロニトリル、ポリカーボネート−g−無水マレイン酸/ポリスチレン、ポリカーボネート−g−無水マレイン酸/ポリスチレン/ポリアクリロニトリル、エポキシ基含有SB樹脂、エポキシ基含有SBS樹脂、エポキシ基含有SEBS樹脂などが挙げられ、それらは二種以上の混合物として用いても良く、アクリロニトリル/ブタジエン/スチレン樹脂(ABS樹脂)、メタクリル酸メチル/ブタジエン/スチレン樹脂(MBS樹脂)およびメタクリル酸メチル/アクリロニトリル/ブタジエン/スチレン樹脂(MABS樹脂)が好ましく用いられる。なお、前記のスチレン系樹脂の中でブタジエンなどのゴム成分が多く共重合された場合あるいはエポキシ基を含有する場合は、とくに衝撃強度を向上する効果が期待できる(/は共重合、−g−はグラフトを示す)。 Specific examples of the styrene resin include methyl methacrylate / acrylonitrile / styrene resin, acrylonitrile / styrene resin (AS resin), styrene / butadiene resin (SB resin), acrylonitrile / butadiene / styrene resin (ABS resin), styrene / butadiene. / Styrene resin (SBS resin), styrene / ethylene / butylene / styrene resin (SEBS resin), styrene / isoprene / styrene resin (SIS resin), acrylate / acrylonitrile / styrene resin (AAS resin), chlorinated polyethylene / acrylonitrile / styrene Resin (ACS resin), acrylonitrile / ethylene / styrene resin (AES resin), styrene / N-phenylmaleimide resin, styrene / acrylonitrile / N-phenylmaleimide resin, Methyl lurate / butadiene / styrene resin (MBS resin), methyl methacrylate / acrylonitrile / butadiene / styrene resin (MABS resin), high impact-polystyrene resin (HI-PS resin), polycarbonate-g-polystyrene, polycarbonate-g- Polystyrene / polyacrylonitrile, polycarbonate-g-maleic anhydride / polystyrene, polycarbonate-g-maleic anhydride / polystyrene / polyacrylonitrile, epoxy group-containing SB resin, epoxy group-containing SBS resin, epoxy group-containing SEBS resin, etc. They may be used as a mixture of two or more, such as acrylonitrile / butadiene / styrene resin (ABS resin), methyl methacrylate / butadiene / styrene resin (MBS resin) and Methyl acrylic acid / acrylonitrile / butadiene / styrene resin (MABS resin) is preferably used. In addition, when many rubber components, such as butadiene, are copolymerized in the said styrene-type resin, or when an epoxy group is contained, the effect which improves especially impact strength can be anticipated (/ is copolymerization, -g- Indicates a graft).
前記のとくに好ましく用いられるコアシェルゴムとは、最外層のシェル層と2層以上の内層のコア層からなる多層構造体であり、例えばコア層がジメチルシロキサン/アクリル酸ブチル重合体などの軟質系の樹脂で最外層がスチレン系共重合体、ポリメタクリル酸メチルなどの熱可塑性樹脂さらには、いずれかの層がメタクリル酸グリシジルや酸無水物などで変性されている多層構造体である。また、多層構造体の粒子径については、特に限定されるものではないが、0.01μm以上、1000μm以下であることが好ましく、さらに、0.02μm以上、100μm以下であることがより好ましく、特に0.05μm以上、10μm以下であることが最も好ましい。また、多層構造体において、コアとシェルの重量比は、特に限定されるものではないが、多層構造体に対して、コア層が10重量部以上、90重量部以下であることが好ましく、さらに、30重量部以上、80重量部以下であることがより好ましい。 The particularly preferably used core-shell rubber is a multilayer structure comprising an outermost shell layer and two or more inner core layers. For example, the core layer is made of a soft material such as dimethylsiloxane / butyl acrylate polymer. It is a multilayer structure in which the outermost layer is a resin, a styrene copolymer, a thermoplastic resin such as polymethyl methacrylate, and any one layer is modified with glycidyl methacrylate or acid anhydride. The particle diameter of the multilayer structure is not particularly limited, but is preferably 0.01 μm or more and 1000 μm or less, more preferably 0.02 μm or more and 100 μm or less, and particularly Most preferably, it is 0.05 μm or more and 10 μm or less. In the multilayer structure, the weight ratio of the core and the shell is not particularly limited, but the core layer is preferably 10 parts by weight or more and 90 parts by weight or less with respect to the multilayer structure. 30 parts by weight or more and 80 parts by weight or less is more preferable.
また、多層構造体としては、前記した条件を満たす市販品を用いてもよく、また公知の方法により作製して用いることもできる。 Moreover, as a multilayer structure, the commercial item which satisfy | fills above-described conditions may be used, and it can also produce and use by a well-known method.
また、多層構造体の市販品としては、例えば、三菱レイヨン社製”メタブレン”、鐘淵化学工業社製”カネエース”、呉羽化学工業社製”パラロイド”、ロームアンドハース社製”アクリロイド”、武田薬品工業社製”スタフィロイド”およびクラレ社製”パラペットSA”などが挙げられる。 Commercially available multilayer structures include, for example, “Metablene” manufactured by Mitsubishi Rayon Co., “Kane Ace” manufactured by Kaneka Chemical Industry Co., “Paraloid” manufactured by Kureha Chemical Industry Co., Ltd., “Acryloid” manufactured by Rohm and Haas Co., Ltd., Takeda Examples thereof include “STAPHYLOID” manufactured by Yakuhin Kogyo Co., Ltd. and “Parapet SA” manufactured by Kuraray Co., Ltd.
前記の好ましく用いられるポリオレフィン系共重合体とは、エチレンユニットを含有するポリオレフィン系共重合体であり、エチレン/アクリル酸メチル、エチレン/メタクリル酸メチル、エチレン/プロピレン、エチレン/ブテン−1およびエチレン/酢酸ビニルなどが挙げられる。とくに、前記のポリオレフィン系共重合体にグリシジル基、エポキシ基、酸無水物基の一種がグラフトあるいは共重合されたポリオレフィン系共重合体が好ましく用いられる。前記の具体例としては、エチレン/グリシジルメタクリレート、エチレン/アクリル酸メチル/グリシシルメタクリレート、エチレン/無水マレイン酸、エチレン/プロピレン/無水マレイン酸、エチレン/ブテン−1/無水マレイン酸、エチレン/エチルアクリレート−g−ポリスチレン、エチレン/グリシシルメタクリレート−g−ポリスチレン、エチレン/グリシシルメタクリレート−g−ポリメタクリル酸メチル、エチレン/エチルアクリート無水マレイン酸−g−ポリメタクリル酸メチル、エチレン/グリシシルメタクリレート−g−ポリスチレン/ポリアクリロニトリル、およびエチレン/エチルアクリレート/無水マレイン酸−g−ポリスチレンなどが挙げられ、本発明の性能を維持しながらさらに耐衝撃性に優れる樹脂組成物が得られる(/は共重合、−g−はグラフトを示す)。 The polyolefin copolymer preferably used is a polyolefin copolymer containing an ethylene unit, and includes ethylene / methyl acrylate, ethylene / methyl methacrylate, ethylene / propylene, ethylene / butene-1 and ethylene / Examples include vinyl acetate. In particular, a polyolefin copolymer obtained by grafting or copolymerizing one type of glycidyl group, epoxy group, and acid anhydride group to the polyolefin copolymer is preferably used. Specific examples include ethylene / glycidyl methacrylate, ethylene / methyl acrylate / glycidyl methacrylate, ethylene / maleic anhydride, ethylene / propylene / maleic anhydride, ethylene / butene-1 / maleic anhydride, ethylene / ethyl acrylate. -G-polystyrene, ethylene / glycidyl methacrylate-g-polystyrene, ethylene / glycisyl methacrylate-g-polymethyl methacrylate, ethylene / ethyl acrylate maleic anhydride-g-polymethyl methacrylate, ethylene / glycisyl methacrylate-g -Polystyrene / polyacrylonitrile, ethylene / ethyl acrylate / maleic anhydride-g-polystyrene, etc., and a resin composition having excellent impact resistance while maintaining the performance of the present invention Is obtained (/ copolymerization,-g-denotes a graft).
また、前記のポリオレフィン系共重合体にグリシジル基、エポキシ基、酸無水物基の一種がグラフトあるいは共重合されたポリオレフィン系共重合体は公知の方法により作製して用いても良く、市販品の住友化学(株)製“ボンドファースト”や三井石油化学(株)製“アドマー”や“N−タフマー”、日本油脂(株)製”モディパー”などを用いても良い。 In addition, a polyolefin copolymer obtained by grafting or copolymerizing one type of glycidyl group, epoxy group, and acid anhydride group to the above-mentioned polyolefin copolymer may be prepared and used by a known method. “Bond First” manufactured by Sumitomo Chemical Co., Ltd., “Admer” or “N-Tuffmer” manufactured by Mitsui Petrochemical Co., Ltd., “Modiper” manufactured by Nippon Oil & Fats Co., Ltd. may be used.
また、(A)ポリ乳酸樹脂、(B)芳香族ポリカーボネート樹脂以外の(F)熱可塑性樹脂は1種で用いても2種以上併用して用いても良く、配合量は(A)ポリ乳酸樹脂と(B)芳香族ポリカーボネート樹脂100重量部に対し、1〜100重量部であり、好ましくは2〜90重量部、さらに好ましくは3〜80重量部、最も好ましくは4〜70重量部であり、1重量部未満の場合は耐熱性や衝撃強度などを改良する効果が小さく、100重量部を超える場合は植物由来の(A)ポリ乳酸樹脂成分割合が極端に少なくなるため、地球環境保全の見地から好ましくない。 In addition, (A) polylactic acid resin and (B) thermoplastic resin other than aromatic polycarbonate resin may be used alone or in combination of two or more. The blending amount is (A) polylactic acid. 1 to 100 parts by weight, preferably 2 to 90 parts by weight, more preferably 3 to 80 parts by weight, and most preferably 4 to 70 parts by weight with respect to 100 parts by weight of the resin and (B) aromatic polycarbonate resin When the amount is less than 1 part by weight, the effect of improving the heat resistance and impact strength is small, and when it exceeds 100 parts by weight, the proportion of the plant-derived (A) polylactic acid resin component is extremely reduced. It is not preferable from the viewpoint.
本発明の(G)結晶核剤とは、一般にポリマーの結晶核剤として用いられるものを特に制限なく用いることができ、無機系結晶核剤および有機系結晶核剤のいずれをも使用することができ、耐熱性が向上するという観点から、(G)結晶核剤を含有することが好ましい。 As the (G) crystal nucleating agent of the present invention, those generally used as polymer crystal nucleating agents can be used without particular limitation, and both inorganic crystal nucleating agents and organic crystal nucleating agents can be used. In view of improving heat resistance, it is preferable to contain (G) a crystal nucleating agent.
無機系結晶核剤の具体例としては、タルク、カオリナイト、モンモリロナイト、マイカ、合成マイカ、クレー、ゼオライト、シリカ、グラファイト、酸化亜鉛、酸化マグネシウム、酸化カルシウム、硫化カルシウム、窒化ホウ素、炭酸マグネシウム、炭酸カルシウム、硫酸バリウム、酸化アルミニウム、酸化ネオジウムおよびフェニルホスホネートの金属塩などが挙げられ、耐熱性を向上させる効果が大きいという観点から、タルク、カオリナイト、モンモリロナイトおよび合成マイカが好ましく、とくにタルク、カオリナイトが好ましく用いられる。これらは単独ないし2種以上を用いることができ、これらの無機系結晶核剤は、組成物中での分散性を高めるために、有機物で修飾されていることが好ましい。 Specific examples of inorganic crystal nucleating agents include talc, kaolinite, montmorillonite, mica, synthetic mica, clay, zeolite, silica, graphite, zinc oxide, magnesium oxide, calcium oxide, calcium sulfide, boron nitride, magnesium carbonate, carbonic acid. Examples include calcium, barium sulfate, aluminum oxide, neodymium oxide, and metal salts of phenylphosphonate, and talc, kaolinite, montmorillonite, and synthetic mica are preferred from the viewpoint of having a large effect of improving heat resistance, and particularly talc, kaolinite. Is preferably used. These may be used alone or in combination of two or more. These inorganic crystal nucleating agents are preferably modified with an organic substance in order to enhance dispersibility in the composition.
無機系結晶核剤の配合量は、(A)ポリ乳酸樹脂と(B)芳香族ポリカーボネート樹脂100重量部に対し、0.01〜70重量部が好ましく、0.05〜50重量部がより好ましく、0.1〜30重量部がさらに好ましい。 The compounding amount of the inorganic crystal nucleating agent is preferably 0.01 to 70 parts by weight, more preferably 0.05 to 50 parts by weight with respect to 100 parts by weight of (A) polylactic acid resin and (B) aromatic polycarbonate resin. 0.1 to 30 parts by weight is more preferable.
また、有機系結晶核剤の具体例としては、安息香酸ナトリウム、安息香酸カリウム、安息香酸リチウム、安息香酸カルシウム、安息香酸マグネシウム、安息香酸バリウム、テレフタル酸リチウム、テレフタル酸ナトリウム、テレフタル酸カリウム、シュウ酸カルシウム、ラウリン酸ナトリウム、ラウリン酸カリウム、ミリスチン酸ナトリウム、ミリスチン酸カリウム、ミリスチン酸カルシウム、オクタコサン酸ナトリウム、オクタコサン酸カルシウム、ステアリン酸ナトリウム、ステアリン酸カリウム、ステアリン酸リチウム、ステアリン酸カルシウム、ステアリン酸マグネシウム、ステアリン酸バリウム、モンタン酸ナトリウム、モンタン酸カルシウム、トルイル酸ナトリウム、サリチル酸ナトリウム、サリチル酸カリウム、サリチル酸亜鉛、アルミニウムジベンゾエート、カリウムジベンゾエート、リチウムジベンゾエート、ナトリウムβ−ナフタレート、ナトリウムシクロヘキサンカルボキシレートなどの有機カルボン酸金属塩、p−トルエンスルホン酸ナトリウム、スルホイソフタル酸ナトリウムなどの有機スルホン酸塩、ステアリン酸アミド、エチレンビスラウリン酸アミド、パルチミン酸アミド、ヒドロキシステアリン酸アミド、エルカ酸アミド、トリメシン酸トリス(t−ブチルアミド)などのカルボン酸アミド、低密度ポリエチレン、高密度ポリエチレン、ポリプロピレン、ポリイソプロピレン、ポリブテン、ポリ−4−メチルペンテン、ポリ−3−メチルブテン−1、ポリビニルシクロアルカン、ポリビニルトリアルキルシラン、高融点ポリ乳酸などのポリマー、エチレン−アクリル酸またはメタクリル酸コポリマーのナトリウム塩、スチレン−無水マレイン酸コポリマーのナトリウム塩などのカルボキシル基を有する重合体のナトリウム塩またはカリウム塩(いわゆるアイオノマー)、ベンジリデンソルビトールおよびその誘導体および2,2−メチルビス(4,6−ジ−t−ブチルフェニル)ナトリウムなどが挙げられ、耐熱性を向上させる効果が大きいという観点からは、有機カルボン酸金属塩およびカルボン酸アミドが好ましい。これらは単独ないし2種以上用いることができる。 Specific examples of organic crystal nucleating agents include sodium benzoate, potassium benzoate, lithium benzoate, calcium benzoate, magnesium benzoate, barium benzoate, lithium terephthalate, sodium terephthalate, potassium terephthalate, Calcium oxide, sodium laurate, potassium laurate, sodium myristate, potassium myristate, calcium myristate, sodium octacosanoate, calcium octacosanoate, sodium stearate, potassium stearate, lithium stearate, calcium stearate, magnesium stearate, Barium stearate, sodium montanate, calcium montanate, sodium toluate, sodium salicylate, potassium salicylate, salicylic acid , Metal salts of organic carboxylic acids such as aluminum dibenzoate, potassium dibenzoate, lithium dibenzoate, sodium β-naphthalate, sodium cyclohexanecarboxylate, organic sulfonates such as sodium p-toluenesulfonate, sodium sulfoisophthalate, stearic acid Amide, ethylenebislauric acid amide, palmitic acid amide, hydroxystearic acid amide, erucic acid amide, carboxylic acid amides such as trimesic acid tris (t-butylamide), low density polyethylene, high density polyethylene, polypropylene, polyisopropylene, polybutene Polymers such as poly-4-methylpentene, poly-3-methylbutene-1, polyvinylcycloalkane, polyvinyltrialkylsilane, and high melting point polylactic acid, Sodium salt or potassium salt of a polymer having a carboxyl group such as sodium salt of ethylene-acrylic acid or methacrylic acid copolymer, sodium salt of styrene-maleic anhydride copolymer (so-called ionomer), benzylidene sorbitol and its derivatives and 2,2- Examples thereof include methylbis (4,6-di-t-butylphenyl) sodium, and from the viewpoint that the effect of improving heat resistance is great, organic carboxylic acid metal salts and carboxylic acid amides are preferred. These may be used alone or in combination of two or more.
有機系結晶核剤の配合量は、(A)ポリ乳酸樹脂と(B)芳香族ポリカーボネート樹脂100重量部に対し、0.01〜20重量部が好ましく、0.05〜10重量部がより好ましく、0.1〜5重量部がさらに好ましい。 The compounding amount of the organic crystal nucleating agent is preferably 0.01 to 20 parts by weight, more preferably 0.05 to 10 parts by weight with respect to 100 parts by weight of (A) polylactic acid resin and (B) aromatic polycarbonate resin. 0.1 to 5 parts by weight is more preferable.
本発明においては、耐熱性が向上するという観点から、さらに結晶核剤以外の充填剤を含有することが好ましい。本発明で用いる結晶核剤以外の充填剤としては、通常熱可塑性樹脂の強化に用いられる繊維状、板状、粒状、粉末状のものを用いることができる。具体的には、ガラス繊維、アスベスト繊維、炭素繊維、グラファイト繊維、金属繊維、チタン酸カリウムウイスカー、ホウ酸アルミニウムウイスカー、マグネシウム系ウイスカー、珪素系ウイスカー、ワラストナイト、セピオライト、アスベスト、スラグ繊維、ゾノライト、エレスタダイト、石膏繊維、シリカ繊維、シリカ・アルミナ繊維、ジルコニア繊維、窒化ホウ素繊維、窒化硅素繊維及びホウ素繊維などの無機繊維状充填剤、ポリエステル繊維、ナイロン繊維、アクリル繊維、再生セルロース繊維、アセテート繊維、ケナフ、ラミー、木綿、ジュート、麻、サイザル、亜麻、リネン、絹、マニラ麻、さとうきび、木材パルプ、紙屑、古紙及びウールなどの有機繊維状充填剤、ガラスフレーク、グラファイト、金属箔、セラミックビーズ、セリサイト、ベントナイト、ドロマイト、微粉珪酸、長石粉、チタン酸カリウム、シラスバルーン、珪酸アルミニウム、酸化珪素、石膏、ノバキュライト、ドーソナイトおよび白土などなどの板状や粒状の充填剤が挙げられる。これらの充填剤の中では、無機繊維状充填剤が好ましく、特にガラス繊維、ワラストナイトが好ましい。また、有機繊維状充填剤の使用も好ましく、脂肪族ポリエステル樹脂の生分解性を生かすという観点から、天然繊維や再生繊維がさらに好ましく、とくにケナフが好ましい。また、配合に供する繊維状充填剤のアスペクト比(平均繊維長/平均繊維径)は5以上であることが好ましく、10以上であることがさらに好ましく、20以上であることがさらに好ましい。 In this invention, it is preferable to contain fillers other than a crystal nucleating agent from a viewpoint that heat resistance improves. As fillers other than the crystal nucleating agent used in the present invention, fibers, plates, granules, and powders that are usually used for reinforcing thermoplastic resins can be used. Specifically, glass fiber, asbestos fiber, carbon fiber, graphite fiber, metal fiber, potassium titanate whisker, aluminum borate whisker, magnesium whisker, silicon whisker, wollastonite, sepiolite, asbestos, slag fiber, zonolite , Elastadite, gypsum fiber, silica fiber, silica-alumina fiber, zirconia fiber, boron nitride fiber, silicon nitride fiber and boron fiber, etc., inorganic fiber filler, polyester fiber, nylon fiber, acrylic fiber, regenerated cellulose fiber, acetate fiber Organic fiber fillers such as kenaf, ramie, cotton, jute, hemp, sisal, flax, linen, silk, manila hemp, sugar cane, wood pulp, paper waste, waste paper and wool, glass flakes, graphite, metal foil, ceramic beads Sericite, bentonite, dolomite, fine silicic acid, feldspar powder, potassium titanate, shirasu balloon, aluminum silicate, silicon oxide, gypsum, novaculite, include plate-like or particulate filler, such as such as dawsonite and white clay. Among these fillers, inorganic fibrous fillers are preferable, and glass fibers and wollastonite are particularly preferable. In addition, use of an organic fibrous filler is also preferable, and natural fibers and regenerated fibers are more preferable from the viewpoint of taking advantage of the biodegradability of the aliphatic polyester resin, and kenaf is particularly preferable. Further, the aspect ratio (average fiber length / average fiber diameter) of the fibrous filler used for blending is preferably 5 or more, more preferably 10 or more, and further preferably 20 or more.
上記の充填剤は、エチレン/酢酸ビニル共重合体などの熱可塑性樹脂や、エポキシ樹脂などの熱硬化性樹脂で被覆または集束処理されていてもよく、アミノシランやエポキシシランなどのカップリング剤などで処理されていてもよい。 The filler may be coated or focused with a thermoplastic resin such as an ethylene / vinyl acetate copolymer or a thermosetting resin such as an epoxy resin, or may be a coupling agent such as aminosilane or epoxysilane. It may be processed.
結晶核剤以外の充填剤の配合量は、(A)ポリ乳酸樹脂と(B)芳香族ポリカーボネート樹脂100重量部に対し、0.1〜200重量部が好ましく、0.5〜100重量部がさらに好ましい。 The blending amount of the filler other than the crystal nucleating agent is preferably 0.1 to 200 parts by weight, and 0.5 to 100 parts by weight with respect to 100 parts by weight of the (A) polylactic acid resin and (B) the aromatic polycarbonate resin. Further preferred.
本発明の樹脂組成物に難燃性を付与する目的で次の難燃剤を配合することができる。配合し得る難燃剤の具体的例としては、臭素系難燃剤、リン系難燃剤、窒素化合物系難燃剤、シリコーン系難燃剤、およびその他の無機系難燃剤などが挙げられ、これら少なくとも一種以上を選択して用いることができる。 The following flame retardants can be blended for the purpose of imparting flame retardancy to the resin composition of the present invention. Specific examples of flame retardants that can be blended include brominated flame retardants, phosphorus flame retardants, nitrogen compound flame retardants, silicone flame retardants, and other inorganic flame retardants. It can be selected and used.
前記の臭素系難燃剤の具体例としては、デカブロモジフェニルオキサイド、オクタブロモジフェニルオキサイド、テトラブロモジフェニルオキサイド、テトラブロモ無水フタル酸、ヘキサブロモシクロドデカン、ビス(2,4,6−トリブロモフェノキシ)エタン、エチレンビステトラブロモフタルイミド、ヘキサブロモベンゼン、1,1−スルホニル[3,5−ジブロモ−4−(2,3−ジブロモプロポキシ)]ベンゼン、ポリジブロモフェニレンオキサイド、テトラブロムビスフェノール−S、トリス(2,3−ジブロモプロピル−1)イソシアヌレート、トリブロモフェノール、トリブロモフェニルアリルエーテル、トリブロモネオペンチルアルコール、ブロム化ポリスチレン、ブロム化ポリエチレン、テトラブロムビスフェノール−A、テトラブロムビスフェノール−A誘導体、テトラブロムビスフェノール−A−エポキシオリゴマーまたはポリマー、テトラブロムビスフェノール−A−カーボネートオリゴマーまたはポリマー、ブロム化フェノールノボラックエポキシなどのブロム化エポキシ樹脂、テトラブロムビスフェノール−A−ビス(2−ヒドロキシジエチルエーテル)、テトラブロムビスフェノール−A−ビス(2,3−ジブロモプロピルエーテル)、テトラブロムビスフェノール−A−ビス(アリルエーテル)、テトラブロモシクロオクタン、エチレンビスペンタブロモジフェニル、トリス(トリブロモネオペンチル)ホスフェート、ポリ(ペンタブロモベンジルポリアクリレート)、オクタブロモトリメチルフェニルインダン、ジブロモネオペンチルグリコール、ペンタブロモベンジルポリアクリレート、ジブロモクレジルグリシジルエーテル、N,N’−エチレン−ビス−テトラブロモフタルイミドなどが挙げられる。なかでも、テトラブロムビスフェノール−A−エポキシオリゴマー、テトラブロムビスフェノール−A−カーボネートオリゴマー、ブロム化エポキシ樹脂が好ましい。 Specific examples of the brominated flame retardant include decabromodiphenyl oxide, octabromodiphenyl oxide, tetrabromodiphenyl oxide, tetrabromophthalic anhydride, hexabromocyclododecane, bis (2,4,6-tribromophenoxy) ethane. , Ethylenebistetrabromophthalimide, hexabromobenzene, 1,1-sulfonyl [3,5-dibromo-4- (2,3-dibromopropoxy)] benzene, polydibromophenylene oxide, tetrabromobisphenol-S, tris (2 , 3-Dibromopropyl-1) isocyanurate, tribromophenol, tribromophenyl allyl ether, tribromoneopentyl alcohol, brominated polystyrene, brominated polyethylene, tetrabromobisphenol- , Tetrabromobisphenol-A derivatives, tetrabromobisphenol-A-epoxy oligomers or polymers, tetrabromobisphenol-A-carbonate oligomers or polymers, brominated epoxy resins such as brominated phenol novolac epoxy, tetrabromobisphenol-A-bis ( 2-hydroxydiethyl ether), tetrabromobisphenol-A-bis (2,3-dibromopropyl ether), tetrabromobisphenol-A-bis (allyl ether), tetrabromocyclooctane, ethylenebispentabromodiphenyl, tris (tri Bromoneopentyl) phosphate, poly (pentabromobenzylpolyacrylate), octabromotrimethylphenylindane, dibromoneopentylglyco Le, pentabromobenzyl polyacrylate, dibromo cresyl glycidyl ether, N, N'ethylene - bis - such as tetrabromo phthalic imide. Of these, tetrabromobisphenol-A-epoxy oligomer, tetrabromobisphenol-A-carbonate oligomer, and brominated epoxy resin are preferable.
前記のリン系難燃剤は特に限定されることはなく、通常一般に用いられるリン系難燃剤を用いることができ、代表的にはリン酸エステル、ポリリン酸塩などの有機リン系化合物や、赤リンが挙げられる。 The phosphorus-based flame retardant is not particularly limited, and generally used phosphorus-based flame retardants can be used. Typically, organic phosphorus compounds such as phosphate esters and polyphosphates, red phosphorus, Is mentioned.
前記の有機リン系化合物におけるリン酸エステルの具体例としては、トリメチルホスフェート、トリエチルホスフェート、トリブチルホスフェート、トリ(2−エチルヘキシル)ホスフェート、トリブトキシエチルホスフェート、トリフェニルホスフェート、トリクレジルホスフェート、トリキシレニルホスフェート、トリス(イソプロピルフェニル)ホスフェート、トリス(フェニルフェニル)ホスフェート、トリナフチルホスフェート、クレジルジフェニルホスフェート、キシレニルジフェニルホスフェート、ジフェニル(2−エチルヘキシル)ホスフェート、ジ(イソプロピルフェニル)フェニルホスフェート、モノイソデシルホスフェート、2−アクリロイルオキシエチルアシッドホスフェート、2−メタクリロイルオキシエチルアシッドホスフェート、ジフェニル−2−アクリロイルオキシエチルホスフェート、ジフェニル−2−メタクリロイルオキシエチルホスフェート、メラミンホスフェート、ジメラミンホスフェート、メラミンピロホスフェート、トリフェニルホスフィンオキサイド、トリクレジルホスフィンオキサイド、メタンホスホン酸ジフェニル、フェニルホスホン酸ジエチル、レゾルシノールポリフェニルホスフェート、レゾルシノールポリ(ジ−2,6−キシリル)ホスフェート、ビスフェノールAポリクレジルホスフェート、ハイドロキノンポリ(2,6−キシリル)ホスフェートならびにこれらの縮合物などの縮合リン酸エステルを挙げることができる。市販の縮合リン酸エステルとしては、例えば大八化学社製PX−200、PX−201、PX−202、CR−733S、CR−741、CR747、旭電化製FP−600、FP−700などを挙げることができる。 Specific examples of the phosphoric acid ester in the organophosphorus compound include trimethyl phosphate, triethyl phosphate, tributyl phosphate, tri (2-ethylhexyl) phosphate, tributoxyethyl phosphate, triphenyl phosphate, tricresyl phosphate, trixylenyl. Phosphate, tris (isopropylphenyl) phosphate, tris (phenylphenyl) phosphate, trinaphthyl phosphate, cresyl diphenyl phosphate, xylenyl diphenyl phosphate, diphenyl (2-ethylhexyl) phosphate, di (isopropylphenyl) phenyl phosphate, monoisodecyl Phosphate, 2-acryloyloxyethyl acid phosphate, 2-methacryloyloxyethyl acetate Phosphate, diphenyl-2-acryloyloxyethyl phosphate, diphenyl-2-methacryloyloxyethyl phosphate, melamine phosphate, dimelamine phosphate, melamine pyrophosphate, triphenylphosphine oxide, tricresylphosphine oxide, diphenyl methanephosphonate, phenylphosphonic acid Examples include condensed phosphate esters such as diethyl, resorcinol polyphenyl phosphate, resorcinol poly (di-2,6-xylyl) phosphate, bisphenol A polycresyl phosphate, hydroquinone poly (2,6-xylyl) phosphate, and condensates thereof. be able to. Examples of commercially available condensed phosphate esters include PX-200, PX-201, PX-202, CR-733S, CR-741, CR747 manufactured by Daihachi Chemical Co., Ltd., FP-600, FP-700 manufactured by Asahi Denka. be able to.
また、リン酸、ポリリン酸と周期律表IA族〜IVB族の金属、アンモニア、脂肪族アミン、芳香族アミンとの塩からなるリン酸塩、ポリリン酸塩を挙げることもできる。ポリリン酸塩の代表的な金属塩として、リチウム塩、ナトリウム塩、カルシウム塩、バリウム塩、鉄(II)塩、鉄(III)塩、アルミニウム塩など、脂肪族アミン塩としてメチルアミン塩、エチルアミン塩、ジエチルアミン塩、トリエチルアミン塩、エチレンジアミン塩、ピペラジン塩などがあり、芳香族アミン塩としてはピリジン塩、トリアジン塩、メラミン塩、アンモニウム塩などが挙げられる。 Moreover, the phosphate and polyphosphate which consist of a salt with phosphoric acid, polyphosphoric acid, a metal of group IA-IVB of the periodic table, ammonia, an aliphatic amine, and an aromatic amine can also be mentioned. Typical metal salts of polyphosphate include lithium salt, sodium salt, calcium salt, barium salt, iron (II) salt, iron (III) salt, aluminum salt, etc., aliphatic amine salt such as methylamine salt, ethylamine salt , Diethylamine salt, triethylamine salt, ethylenediamine salt, piperazine salt and the like, and aromatic amine salt includes pyridine salt, triazine salt, melamine salt, ammonium salt and the like.
また、上記の他、トリスクロロエチルホスフェート、トリスジクロロプロピルホスフェート、トリス(β−クロロプロピル)ホスフェート)などの含ハロゲンリン酸エステル、また、リン原子と窒素原子が二重結合で結ばれた構造を有するホスファゼン化合物、リン酸エステルアミドを挙げることができる。 In addition to the above, halogen-containing phosphate esters such as trischloroethyl phosphate, trisdichloropropyl phosphate, tris (β-chloropropyl) phosphate), and a structure in which a phosphorus atom and a nitrogen atom are connected by a double bond. Examples thereof include phosphazene compounds and phosphoric ester amides.
また、赤リンとしては、未処理の赤リンのみでなく、熱硬化性樹脂被膜、金属水酸化物被膜、金属メッキ被膜から成る群より選ばれる1種以上の化合物被膜により処理された赤リンを好ましく使用することができる。熱硬化性樹脂被膜の熱硬化性樹脂としては、赤リンを被膜できる樹脂であれば特に制限はなく、例えば、フェノール−ホルマリン系樹脂、尿素−ホルマリン系樹脂、メラミン−ホルマリン系樹脂、アルキッド系樹脂などが挙げられる。金属水酸化物被膜の金属水酸化物としては、赤リンを被膜できるものであれば特に制限はなく、例えば、水酸化アルミニウム、水酸化マグネシウム、水酸化亜鉛、水酸化チタンなどを挙げることができる。金属メッキ被膜の金属としては、赤リンを被膜できるものであれば特に制限はなく、Fe、Ni、Co、Cu、Zn、Mn、Ti、Zr、Alまたはこれらの合金などが挙げられる。さらに、これらの被膜は2種以上組み合わせて、あるいは2種以上に積層されていてもよい。 Further, as red phosphorus, not only untreated red phosphorus but also red phosphorus treated with one or more compound films selected from the group consisting of thermosetting resin coatings, metal hydroxide coatings, and metal plating coatings. It can be preferably used. The thermosetting resin of the thermosetting resin film is not particularly limited as long as it is a resin capable of coating red phosphorus. For example, phenol-formalin resin, urea-formalin resin, melamine-formalin resin, alkyd resin Etc. The metal hydroxide coating is not particularly limited as long as it can coat red phosphorus, and examples thereof include aluminum hydroxide, magnesium hydroxide, zinc hydroxide, and titanium hydroxide. . The metal of the metal plating film is not particularly limited as long as it can coat red phosphorus, and examples thereof include Fe, Ni, Co, Cu, Zn, Mn, Ti, Zr, Al, and alloys thereof. Furthermore, these coatings may be laminated in combination of two or more or in combination of two or more.
前記の窒素化合物系難燃剤としては、脂肪族アミン化合物、芳香族アミン化合物、含窒素複素環化合物、シアン化合物、脂肪族アミド、芳香族アミド、尿素、チオ尿素などを挙げることができる。なお、上記リン系難燃剤で例示したようなポリリン酸アンモニウムなど含窒素リン系難燃剤はここでいう窒素化合物系難燃剤には含まない。脂肪族アミンとしては、エチルアミン、ブチルアミン、ジエチルアミン、エチレンジアミン、ブチレンジアミン、トリエチレンテトラミン、1,2−ジアミノシクロヘキサン、1,2−ジアミノシクロオクタンなどを挙げることができる。芳香族アミンとしては、アニリン、フェニレンジアミンなどを挙げることができる。含窒素複素環化合物としては、尿酸、アデニン、グアニン、2,6−ジアミノプリン、2,4,6−トリアミノピリジン、トリアジン化合物などを挙げることができる。シアン化合物としては、ジシアンジアミドなどを挙げることができる。脂肪族アミドとしては、N,N−ジメチルアセトアミドなどを挙げることができる。芳香族アミドとしては、N,N−ジフェニルアセトアミドなどを挙げることができる。 Examples of the nitrogen compound-based flame retardant include aliphatic amine compounds, aromatic amine compounds, nitrogen-containing heterocyclic compounds, cyanide compounds, aliphatic amides, aromatic amides, urea, thiourea and the like. In addition, nitrogen-containing phosphorus flame retardants such as ammonium polyphosphate as exemplified in the above phosphorus flame retardant are not included in the nitrogen compound flame retardant referred to herein. Examples of the aliphatic amine include ethylamine, butylamine, diethylamine, ethylenediamine, butylenediamine, triethylenetetramine, 1,2-diaminocyclohexane, 1,2-diaminocyclooctane and the like. Examples of the aromatic amine include aniline and phenylenediamine. Examples of nitrogen-containing heterocyclic compounds include uric acid, adenine, guanine, 2,6-diaminopurine, 2,4,6-triaminopyridine, and triazine compounds. Examples of the cyan compound include dicyandiamide. Examples of the aliphatic amide include N, N-dimethylacetamide. Examples of aromatic amides include N, N-diphenylacetamide.
上記において例示したトリアジン化合物は、トリアジン骨格を有する含窒素複素環化合物であり、トリアジン、メラミン、ベンゾグアナミン、メチルグアナミン、シアヌル酸、メラミンシアヌレート、メラミンイソシアヌレート、トリメチルトリアジン、トリフェニルトリアジン、アメリン、アメリド、チオシアヌル酸、ジアミノメルカプトトリアジン、ジアミノメチルトリアジン、ジアミノフェニルトリアジン、ジアミノイソプロポキシトリアジンなどを挙げることができる。 The triazine compounds exemplified above are nitrogen-containing heterocyclic compounds having a triazine skeleton, and are triazine, melamine, benzoguanamine, methylguanamine, cyanuric acid, melamine cyanurate, melamine isocyanurate, trimethyltriazine, triphenyltriazine, amelin, and amelide. And thiocyanuric acid, diaminomercaptotriazine, diaminomethyltriazine, diaminophenyltriazine, diaminoisopropoxytriazine and the like.
メラミンシアヌレートまたはメラミンイソシアヌレートとしては、シアヌール酸またはイソシアヌール酸とトリアジン化合物との付加物が好ましく、通常は1対1(モル比)、場合により1対2(モル比)の組成を有する付加物を挙げることができる。また、公知の方法で製造されるが、例えば、メラミンとシアヌール酸またはイソシアヌール酸の混合物を水スラリーとし、良く混合して両者の塩を微粒子状に形成させた後、このスラリーを濾過、乾燥後に一般には粉末状で得られる。また、上記の塩は完全に純粋である必要は無く、多少未反応のメラミンないしシアヌール酸、イソシアヌール酸が残存していても良い。また、樹脂に配合される前の平均粒径は、成形品の難燃性、機械的強度、表面性の点から100〜0.01μmが好ましく、更に好ましくは80〜1μmである。 As melamine cyanurate or melamine isocyanurate, an addition product of cyanuric acid or isocyanuric acid and a triazine compound is preferable, usually an addition having a composition of 1 to 1 (molar ratio) and optionally 1 to 2 (molar ratio). You can list things. Although it is produced by a known method, for example, a mixture of melamine and cyanuric acid or isocyanuric acid is made into a water slurry and mixed well to form both salts into fine particles, and then the slurry is filtered and dried. Later it is generally obtained in powder form. The salt does not need to be completely pure, and some unreacted melamine, cyanuric acid or isocyanuric acid may remain. Moreover, the average particle diameter before blending with the resin is preferably 100 to 0.01 μm, more preferably 80 to 1 μm from the viewpoint of flame retardancy, mechanical strength, and surface property of the molded product.
窒素化合物系難燃剤の中では、含窒素複素環化合物が好ましく、中でもトリアジン化合物が好ましく、さらにメラミンシアヌレートが好ましい。 Of the nitrogen compound-based flame retardants, nitrogen-containing heterocyclic compounds are preferable, among which triazine compounds are preferable, and melamine cyanurate is more preferable.
また、上記窒素化合物系難燃剤の分散性が悪い場合には、トリス(β−ヒドロキシエチル)イソシアヌレートなどの分散剤やポリビニルアルコール、金属酸化物などの公知の表面処理剤などを併用してもよい。 When the dispersibility of the nitrogen compound flame retardant is poor, a dispersant such as tris (β-hydroxyethyl) isocyanurate or a known surface treatment agent such as polyvinyl alcohol or metal oxide may be used in combination. Good.
本発明で用いられるシリコーン系難燃剤としては、シリコーン樹脂、シリコーンオイルを挙げることができる。前記シリコーン樹脂は、SiO2、RSiO3/2、R2SiO、R3SiO1/2の構造単位を組み合わせてできる三次元網状構造を有する樹脂などを挙げることができる。ここで、Rはメチル基、エチル基、プロピル基等のアルキル基、または、フェニル基、ベンジル基等の芳香族基、または上記置換基にビニル基を含有した置換基を示す。前記シリコーンオイルは、ポリジメチルシロキサン、およびポリジメチルシロキサンの側鎖あるいは末端の少なくとも1つのメチル基が、水素元素、アルキル基、シクロヘキシル基、フェニル基、ベンジル基、アミノ基、エポキシ基、ポリエーテル基、カルボキシル基、メルカプト基、クロロアルキル基、アルキル高級アルコールエステル基、アルコール基、アラルキル基、ビニル基、またはトリフロロメチル基の選ばれる少なくとも1つの基により変性された変性ポリシロキサン、またはこれらの混合物を挙げることができ、(B)芳香族ポリカーボネート樹脂にシリコーン系樹脂を共重合させた樹脂を用いても良い。 Examples of the silicone-based flame retardant used in the present invention include silicone resins and silicone oils. Examples of the silicone resin include resins having a three-dimensional network structure formed by combining structural units of SiO 2 , RSiO 3/2 , R 2 SiO, and R 3 SiO 1/2 . Here, R represents an alkyl group such as a methyl group, an ethyl group or a propyl group, an aromatic group such as a phenyl group or a benzyl group, or a substituent containing a vinyl group in the above substituent. In the silicone oil, polydimethylsiloxane, and at least one methyl group in the side chain or terminal of polydimethylsiloxane is a hydrogen element, an alkyl group, a cyclohexyl group, a phenyl group, a benzyl group, an amino group, an epoxy group, or a polyether group. , A modified polysiloxane modified with at least one group selected from a carboxyl group, a mercapto group, a chloroalkyl group, an alkyl higher alcohol ester group, an alcohol group, an aralkyl group, a vinyl group, or a trifluoromethyl group, or a mixture thereof (B) A resin obtained by copolymerizing an aromatic polycarbonate resin with a silicone resin may be used.
前記のその他の無機系難燃剤としては、水酸化マグネシウム、水酸化アルミニウム、三酸化アンチモン、五酸化アンチモン、アンチモン酸ソーダ、ヒドロキシスズ酸亜鉛、スズ酸亜鉛、メタスズ酸、酸化スズ、酸化スズ塩、硫酸亜鉛、酸化亜鉛、酸化第一鉄、酸化第二鉄、酸化第一錫、酸化第二スズ、ホウ酸亜鉛、ホウ酸カルシウム、ホウ酸アンモニウム、オクタモリブデン酸アンモニウム、タングステン酸の金属塩、タングステンとメタロイドとの複合酸化物酸、スルファミン酸アンモニウム、臭化アンモニウム、ジルコニウム系化合物、グアニジン系化合物、黒鉛、膨潤性黒鉛などを挙げることができる。中でも、水酸化アルミニウム、ホウ酸亜鉛、膨潤性黒鉛が好ましい。 Examples of the other inorganic flame retardant include magnesium hydroxide, aluminum hydroxide, antimony trioxide, antimony pentoxide, sodium antimonate, zinc hydroxystannate, zinc stannate, metastannic acid, tin oxide, tin oxide salt, Zinc sulfate, zinc oxide, ferrous oxide, ferric oxide, stannous oxide, stannic oxide, zinc borate, calcium borate, ammonium borate, ammonium octamolybdate, metal salt of tungstic acid, tungsten And oxides of metal oxide and metalloid, ammonium sulfamate, ammonium bromide, zirconium compounds, guanidine compounds, graphite, swellable graphite, and the like. Of these, aluminum hydroxide, zinc borate, and swellable graphite are preferable.
前記の難燃剤は、1種で用いても、2種以上併用して用いてもかまわない。なお、水酸化アルミニウムを用いる場合は、(A)ポリ乳酸樹脂と(B)芳香族ポリカーボネート樹脂を予め混練し、混練温度210℃以下で溶融混合して用いることが好ましい。 The above flame retardants may be used alone or in combination of two or more. In addition, when using aluminum hydroxide, it is preferable to knead | mix previously (A) polylactic acid resin and (B) aromatic polycarbonate resin, and to melt-mix and use it at the kneading | mixing temperature of 210 degrees C or less.
前記の難燃剤の量は、(A)ポリ乳酸樹脂と(B)芳香族ポリカーボネート樹脂の合計量100重量部に対し、0.5〜100重量部であり、さらには1〜80重量部が好ましい。 The amount of the flame retardant is 0.5 to 100 parts by weight, more preferably 1 to 80 parts by weight with respect to 100 parts by weight of the total amount of (A) polylactic acid resin and (B) aromatic polycarbonate resin. .
前記の難燃剤の中では、ハロゲンを全く含有しないリン系難燃剤、窒素化合物系難燃剤、シリコーン系難燃剤およびその他の無機系難燃剤から選択される少なくとも1種または2種以上を組み合わせて用いることが好ましい。上記において難燃剤を2種以上併用する場合、リン系難燃剤と他の難燃剤を併用することが好ましい。リン系難燃剤と併用する窒素化合物系難燃剤としては、含窒素複素環化合物が好ましく、中でもトリアジン化合物が好ましく、さらにメラミンシアヌレートが好ましい。また、リン系難燃剤と併用するシリコーン系難燃剤としては、シリコーン樹脂、シリコーン樹脂を共重合した(B)芳香族ポリカーボネート樹脂が好ましい。また、リン系難燃剤と併用するその他の無機系難燃剤としては、水酸化アルミニウム、ホウ酸亜鉛および膨潤性黒鉛が好ましい。また、リン系難燃剤との配合比率は任意の量を組み合わせることができ、とくに難燃剤100重量%中のリン系難燃剤の量は1重量%以上であることが好ましく、2〜98重量%であることがより好ましい。 Among the above-mentioned flame retardants, at least one selected from phosphorous flame retardants containing no halogen, nitrogen compound flame retardants, silicone flame retardants and other inorganic flame retardants is used in combination. It is preferable. In the above, when two or more flame retardants are used in combination, it is preferable to use a phosphorus-based flame retardant together with another flame retardant. The nitrogen compound-based flame retardant used in combination with the phosphorus-based flame retardant is preferably a nitrogen-containing heterocyclic compound, more preferably a triazine compound, and further preferably melamine cyanurate. Moreover, as a silicone type flame retardant used together with a phosphorus type flame retardant, (B) aromatic polycarbonate resin which copolymerized silicone resin and silicone resin is preferable. Moreover, as other inorganic flame retardants used in combination with phosphorus flame retardants, aluminum hydroxide, zinc borate and swellable graphite are preferable. Further, the blending ratio with the phosphorus-based flame retardant can be combined in any amount, and the amount of the phosphorus-based flame retardant in 100% by weight of the flame retardant is particularly preferably 1% by weight or more, and 2 to 98% by weight. It is more preferable that
本発明においては、耐熱性が向上するという観点から、さらに可塑剤を含有することが好ましい。本発明で使用する可塑剤としては、一般にポリマーの可塑剤として用いられるものを特に制限なく用いることができ、例えばポリエステル系可塑剤、グリセリン系可塑剤、多価カルボン酸エステル系可塑剤、ポリアルキレングリコール系可塑剤及びエポキシ系可塑剤などを挙げることができる。 In the present invention, it is preferable to further contain a plasticizer from the viewpoint of improving heat resistance. As the plasticizer used in the present invention, those generally used as polymer plasticizers can be used without particular limitation. For example, polyester plasticizer, glycerin plasticizer, polyvalent carboxylic ester plasticizer, polyalkylene Examples include glycol plasticizers and epoxy plasticizers.
ポリエステル系可塑剤の具体例としては、アジピン酸、セバチン酸、テレフタル酸、イソフタル酸、ナフタレンジカルボン酸、ジフェニルジカルボン酸などの酸成分と、プロピレングリコール、1,3−ブタンジオール、1,4−ブタンジオール、1,6−ヘキサンジオール、エチレングリコール、ジエチレングリコールなどのジオール成分からなるポリエステルやポリカプロラクトンなどのヒドロキシカルボン酸からなるポリエステルなどを挙げることができる。これらのポリエステルは単官能カルボン酸もしくは単官能アルコールで末端封鎖されていてもよく、またエポキシ化合物などで末端封鎖されていてもよい。 Specific examples of the polyester plasticizer include acid components such as adipic acid, sebacic acid, terephthalic acid, isophthalic acid, naphthalenedicarboxylic acid, diphenyldicarboxylic acid, propylene glycol, 1,3-butanediol, 1,4-butane. Examples thereof include polyesters composed of diol components such as diol, 1,6-hexanediol, ethylene glycol and diethylene glycol, and polyesters composed of hydroxycarboxylic acid such as polycaprolactone. These polyesters may be end-capped with a monofunctional carboxylic acid or monofunctional alcohol, or may be end-capped with an epoxy compound or the like.
グリセリン系可塑剤の具体例としては、グリセリンモノアセトモノラウレート、グリセリンジアセトモノラウレート、グリセリンモノアセトモノステアレート、グリセリンジアセトモノオレートおよびグリセリンモノアセトモノモンタネートなどを挙げることができる。 Specific examples of the glycerin plasticizer include glycerin monoacetomonolaurate, glycerin diacetomonolaurate, glycerin monoacetomonostearate, glycerin diacetomonooleate, and glycerin monoacetomonomontanate.
多価カルボン酸系可塑剤の具体例としては、フタル酸ジメチル、フタル酸ジエチル、フタル酸ジブチル、フタル酸ジオクチル、フタル酸ジヘプチル、フタル酸ジベンジル、フタル酸ブチルベンジルなどのフタル酸エステル、トリメリット酸トリブチル、トリメリット酸トリオクチル、トリメリット酸トリヘキシルなどのトリメリット酸エステル、アジピン酸ジイソデシル、アジピン酸n−オクチル−n−デシルアジピン酸エステルなどのセバシン酸エステル、アセチルクエン酸トリエチル、アセチルクエン酸トリブチルなどのクエン酸エステル、アゼライン酸ジ−2−エチルヘキシルなどのアゼライン酸エステル、セバシン酸ジブチル、およびセバシン酸ジ−2−エチルヘキシルなどのセバシン酸エステルなどを挙げることができる。 Specific examples of polycarboxylic acid plasticizers include phthalates such as dimethyl phthalate, diethyl phthalate, dibutyl phthalate, dioctyl phthalate, diheptyl phthalate, dibenzyl phthalate, butyl benzyl phthalate, and trimellitic acid. Trimellitic acid esters such as tributyl, trioctyl trimellitic acid, trihexyl trimellitic acid, sebacic acid esters such as diisodecyl adipate, n-octyl-n-decyl adipate adipate, triethyl acetylcitrate, tributyl acetylcitrate, etc. Citrate esters, azelaic acid esters such as di-2-ethylhexyl azelate, sebacic acid esters such as dibutyl sebacate, and di-2-ethylhexyl sebacate.
ポリアルキレングリコール系可塑剤の具体例としては、ポリエチレングリコール、ポリプロピレングリコール、ポリ(エチレンオキサイド・プロピレンオキサイド)ブロック及び/またはランダム共重合体、ポリテトラメチレングリコール、ビスフェノール類のエチレンオキシド付加重合体、ビスフェノール類のプロピレンオキシド付加重合体、ビスフェノール類のテトラヒドロフラン付加重合体などのポリアルキレングリコールあるいはその末端エポキシ変性化合物、末端エステル変性化合物および末端エーテル変性化合物などの末端封鎖化合物などを挙げることができる。 Specific examples of the polyalkylene glycol plasticizer include polyethylene glycol, polypropylene glycol, poly (ethylene oxide / propylene oxide) block and / or random copolymer, polytetramethylene glycol, ethylene oxide addition polymer of bisphenols, bisphenols Polyalkylene glycols such as propylene oxide addition polymers, tetrahydrofuran addition polymers of bisphenols, or end-capped compounds such as terminal epoxy-modified compounds, terminal ester-modified compounds, and terminal ether-modified compounds.
エポキシ系可塑剤とは、一般にはエポキシステアリン酸アルキルと大豆油とからなるエポキシトリグリセリドなどを指すが、その他にも、主にビスフェノールAとエピクロロヒドリンを原料とするような、いわゆるエポキシ樹脂も使用することができる。 The epoxy plasticizer generally refers to an epoxy triglyceride composed of an alkyl epoxy stearate and soybean oil, but there are also so-called epoxy resins mainly made of bisphenol A and epichlorohydrin. Can be used.
その他の可塑剤の具体例としては、ネオペンチルグリコールジベンゾエート、ジエチレングリコールジベンゾエート、トリエチレングリコールジ−2−エチルブチレートなどの脂肪族ポリオールの安息香酸エステル、ステアリン酸アミドなどの脂肪酸アミド、オレイン酸ブチルなどの脂肪族カルボン酸エステル、アセチルリシノール酸メチル、アセチルリシノール酸ブチルなどのオキシ酸エステル、ペンタエリスリトール、各種ソルビトール、ポリアクリル酸エステル、シリコーンオイルおよびパラフィン類などを挙げることができる。 Specific examples of other plasticizers include benzoic acid esters of aliphatic polyols such as neopentyl glycol dibenzoate, diethylene glycol dibenzoate, triethylene glycol di-2-ethylbutyrate, fatty acid amides such as stearamide, oleic acid Examples thereof include aliphatic carboxylic acid esters such as butyl, oxyacid esters such as methyl acetylricinoleate and butyl acetylricinoleate, pentaerythritol, various sorbitols, polyacrylic acid esters, silicone oils, and paraffins.
本発明で使用する可塑剤としては、上記に例示したものの中でも、特にポリエステル系可塑剤及びポリアルキレングリコール系可塑剤から選択した少なくとも1種が好ましい。本発明に使用する可塑剤は、単独ないし2種以上用いることができる。 Among the plasticizers used in the present invention, at least one selected from polyester plasticizers and polyalkylene glycol plasticizers is particularly preferable. The plasticizer used in the present invention may be used alone or in combination of two or more.
また、可塑剤の配合量は、(A)ポリ乳酸樹脂と(B)芳香族ポリカーボネート樹脂100重量部に対し、0.01〜30重量部の範囲が好ましく、0.1〜20重量部の範囲がより好ましく、0.5〜10重量部の範囲がさらに好ましい。 Moreover, the compounding quantity of a plasticizer has the preferable range of 0.01-30 weight part with respect to 100 weight part of (A) polylactic acid resin and (B) aromatic polycarbonate resin, The range of 0.1-20 weight part Is more preferable, and the range of 0.5 to 10 parts by weight is even more preferable.
本発明においては、結晶核剤と可塑剤を各々単独で用いてもよいが、両者を併用して用いることが好ましい。 In the present invention, each of the crystal nucleating agent and the plasticizer may be used alone, but it is preferable to use both in combination.
本発明においては、加水分解抑制により耐熱性、耐久性が向上するという観点から、さらにカルボキシル基反応性末端封鎖剤を含有することが好ましい。 In the present invention, it is preferable to further contain a carboxyl group-reactive end-blocking agent from the viewpoint of improving heat resistance and durability by inhibiting hydrolysis.
本発明で使用するカルボキシル基反応性末端封鎖剤としては、ポリマーのカルボキシル末端基を封鎖することのできる化合物であれば特に制限はなく、ポリマーのカルボキシル末端の封鎖剤として用いられているものを用いることができる。本発明においてかかるカルボキシル基反応性末端封鎖剤は、(A)ポリ乳酸樹脂や(B)芳香族ポリカーボネート樹脂の末端を封鎖するのみではなく、天然由来の有機充填剤の熱分解や加水分解などで生成する乳酸やギ酸などの酸性低分子化合物のカルボキシル基も封鎖することができる。また、上記末端封鎖剤は、熱分解により酸性低分子化合物が生成する水酸基末端も封鎖できる化合物であることがさらに好ましい。 The carboxyl group-reactive end-blocking agent used in the present invention is not particularly limited as long as it is a compound that can block the carboxyl end group of the polymer, and those used as the carboxyl-terminal blocking agent of the polymer are used. be able to. In the present invention, the carboxyl group-reactive end-blocking agent not only blocks the end of (A) polylactic acid resin or (B) aromatic polycarbonate resin, but also thermally decomposes or hydrolyzes naturally-derived organic fillers. The carboxyl group of acidic low molecular weight compounds such as lactic acid and formic acid produced can also be blocked. Further, the end-capping agent is more preferably a compound that can also block the hydroxyl end where an acidic low molecular weight compound is generated by thermal decomposition.
このようなカルボキシル基反応性末端封鎖剤としては、エポキシ化合物、オキサゾリン化合物、オキサジン化合物、カルボジイミド化合物、カルボジイミド変性イソシアネート化合物から選ばれる少なくとも1種の化合物を使用することが好ましく、なかでもエポキシ化合物および/またはカルボジイミド化合物、エポキシ化合物および/またはカルボジイミド変性イソシアネート化合物が好ましい。 As such a carboxyl group-reactive end-blocking agent, it is preferable to use at least one compound selected from an epoxy compound, an oxazoline compound, an oxazine compound, a carbodiimide compound, and a carbodiimide-modified isocyanate compound. Or a carbodiimide compound, an epoxy compound and / or a carbodiimide-modified isocyanate compound are preferred.
カルボキシル基反応性末端封鎖剤の配合量は、(A)ポリ乳酸樹脂と(B)芳香族ポリカーボネート樹脂100重量部に対し、0.01〜10重量部の範囲が好ましく、0.05〜5重量部の範囲がより好ましい。
カルボキシル基反応性末端封鎖剤の添加時期は、特に限定されないが、耐熱性を向上するだけでなく、機械特性や耐久性を向上できるという点で、(A)ポリ乳酸樹脂と(B)芳香族ポリカーボネート樹脂予め溶融混練した後、天然由来の有機充填剤と混練することが好ましい。
The blending amount of the carboxyl group-reactive end-blocking agent is preferably in the range of 0.01 to 10 parts by weight, and 0.05 to 5 parts by weight with respect to 100 parts by weight of (A) polylactic acid resin and (B) aromatic polycarbonate resin. A range of parts is more preferred.
The addition time of the carboxyl group-reactive end-blocking agent is not particularly limited, but (A) polylactic acid resin and (B) aromatic in that not only heat resistance can be improved but also mechanical properties and durability can be improved. It is preferable to knead with a natural organic filler after melt-kneading the polycarbonate resin in advance.
本発明において、本発明の目的を損なわない範囲で公知の滑剤、離型剤、帯電防止剤、発泡剤などを添加することができ、これらの添加剤は、本発明の樹脂組成物を製造する任意の段階で配合することが可能であり、例えば、少なくとも(A)ポリ乳酸樹脂と(B)芳香族ポリカーボネート樹脂を配合する際に同時に添加する方法や、本発明の樹脂組成物を溶融混練した後に添加する方法が挙げられる。
ができる。
In the present invention, known lubricants, mold release agents, antistatic agents, foaming agents and the like can be added as long as the object of the present invention is not impaired, and these additives produce the resin composition of the present invention. For example, at least (A) a polylactic acid resin and (B) an aromatic polycarbonate resin can be added at the same time, or the resin composition of the present invention is melt-kneaded. The method of adding later is mentioned.
Can do.
本発明における鮮明度光沢度とは、着色成形品の成形品外観を評価する指標であり、着色プレート(成形品)を財団法人日本色彩研究所製<PGD>携帯用鮮明度光沢度計を用いて測定した。前記の鮮明度光沢度の測定値は、2.0〜0.1までの数字であり、数字が大きいほど優れ、0.1に達しない鮮明度光沢度の成形品は鮮明度光沢度が非常に劣る成形品であり、鮮明度光沢度は0.3以上が好ましく、0.5以上がさらに好ましい。
また、鮮明度光沢度の値は、成形に用いた金型の表面仕上げによっても左右されることから、金型の表面仕上げに優れる金型を用いる必要があり、鮮明度光沢度に優れるABS樹脂などの熱可塑性樹脂の鮮明度光沢度を測定した値が1.5以上を示す金型が好ましく、1.5未満では測定される数値範囲が狭くなり好ましくない。
The sharpness and glossiness in the present invention is an index for evaluating the appearance of a colored molded product, and the colored plate (molded product) is a <PGD> portable sharpness glossiness meter manufactured by Nippon Color Research Institute. Measured. The measurement value of the above-mentioned sharpness and glossiness is a number from 2.0 to 0.1. The larger the number, the better. The molded product with the sharpness and glossiness that does not reach 0.1 is very sharp. The sharpness and glossiness are preferably 0.3 or more, and more preferably 0.5 or more.
Moreover, since the value of the sharpness and glossiness depends on the surface finish of the mold used for molding, it is necessary to use a mold that is excellent in the surface finish of the mold, and the ABS resin that is excellent in the sharpness and glossiness. A mold in which the value obtained by measuring the sharpness and glossiness of a thermoplastic resin such as 1.5 is not less than 1.5 is preferable.
本発明の樹脂組成物の製造方法については特に限定されるものではないが、例えば(A)ポリ乳酸樹脂、(B)芳香族ポリカーボネート樹脂、(C)顔料および(D)フッ素系樹脂、必要に応じて(E)ヒンダードフェノール系酸化防止剤、(A)(B)成分以外の(F)熱可塑性樹脂、(G)結晶核剤さらに必要に応じて結晶核剤以外の充填剤、難燃剤、その他の添加剤を予めブレンドした後、(A)ポリ乳酸樹脂の融点以上において、1軸または2軸押出機を用いて均一に溶融混練する方法される。 Although it does not specifically limit about the manufacturing method of the resin composition of this invention, For example, (A) polylactic acid resin, (B) aromatic polycarbonate resin, (C) pigment, and (D) fluorine resin, as needed According to (E) hindered phenolic antioxidant, (A) (B) component other than (F) thermoplastic resin, (G) crystal nucleating agent, if necessary, filler other than crystal nucleating agent, flame retardant Then, after other additives are blended in advance, (A) at a melting point or higher of the polylactic acid resin, the mixture is uniformly melt kneaded using a single screw or twin screw extruder.
本発明の樹脂組成物は、独特の特性を持つ組成物であり、押出成形、射出成形、ブロー成形、および未延伸糸、延伸糸、超延伸糸など各種繊維への紡糸などの方法によって、各種製品形状に加工し利用することができ、とくに機械機構部品、電気・電子部品、自動車部品、光学機器、建築部材および日用品など各種用途の成形品として利用することができ、特に機械機構部品、電気・電子部品、自動車部品の成形品として好ましく用いられ、塗装やメッキなどの表面加工を施して用いても良い。 The resin composition of the present invention is a composition having unique characteristics, and various methods are employed by methods such as extrusion molding, injection molding, blow molding, and spinning into various fibers such as undrawn yarn, drawn yarn, and superdrawn yarn. It can be processed into product shapes and used, especially as mechanical parts, electrical / electronic parts, automobile parts, optical equipment, building components and daily products, especially mechanical parts, electrical parts -It is preferably used as a molded product of electronic parts and automobile parts, and may be used after being subjected to surface treatment such as painting or plating.
上記の押出成形により得られる押出成形品としては、フイルム、インフレフィルム、シート、チューブおよび丸棒など各種形状の棒などの押出成形品が挙げられ、延伸されて使用することもでき、機械機構部品、電気・電子部品、自動車部品、光学機器、建築部材および日用品などの各種用途の成形品にさらに加工されて、利用することができる。また、射出成形により得られる射出成形品の機械機構部品としては、洗浄用治具、オイルレス軸受、船尾軸受、水中軸受、などの各種軸受、モーター部品、ライター、タイプライターなどを挙げることができ、射出成形品の電機・電子部品としては、電気機器の筐体、OA機器の筐体、各種カバー、各種ギヤー、各種ケース、コネクター、ソケット、充電台、、コンセントカバー、VTR部品、テレビ部品、オフィスコンピューター関連部品、卓上電話関連部品、ファクシミリ関連部品、複写機関連部品などの一部分以上を構成する成形品を挙げることができ、射出成形品の自動車部品としては、精密機械関連部品、ワイパーモーター関係部品、各種スィッチ部品、各種リレー部品、ランプソケット、ランプハウジング、各種ケースなどの一部分以上を構成する成形品を挙げることができ、光学機器としては、顕微鏡、双眼鏡、カメラ、時計などの一部分以上を構成する成形品を挙げることができる。また、ブロー成形品としては、ジャバラ、ブーツ、ボトルおよび異径管・筒類として必要な形状に成形加工され、機械機構部品、電気・電子部品、自動車部品、光学機器、建築部材および日用品などの成形品として各種用途に利用することができる。 Examples of the extrusion-molded product obtained by the above-described extrusion molding include extrusion-molded products such as films, inflation films, sheets, tubes and round bars, and can be used after being stretched. Further, it can be further processed into a molded product for various uses such as electric / electronic parts, automobile parts, optical equipment, building materials and daily necessities. In addition, examples of the mechanical mechanism parts of injection molded products obtained by injection molding include various types of bearings such as cleaning jigs, oilless bearings, stern bearings, underwater bearings, motor parts, lighters, typewriters, etc. The electrical and electronic parts of injection molded products include: electrical equipment casings, OA equipment casings, various covers, various gears, various cases, connectors, sockets, charging stands, outlet covers, VTR parts, TV parts, It can include molded parts that make up part of office computer-related parts, desk phone-related parts, facsimile-related parts, copying machine-related parts, etc. The automobile parts of injection-molded parts include precision machine-related parts, wiper motor-related parts. Parts, various switch parts, various relay parts, lamp sockets, lamp housings, various cases, etc. Mention may be made of molded article constituting the above minute, the optics include a molded article constituting a microscope, binoculars, camera, or a portion of such clock. In addition, blow molded products are molded into the necessary shape as bellows, boots, bottles, and different diameter pipes / cylinders, such as mechanical mechanism parts, electrical / electronic parts, automobile parts, optical equipment, building components, and daily necessities. It can be used for various purposes as a molded product.
以下に、実施例によって本発明を更に詳細に説明するが、これらは本発明を限定するものではない。 The present invention will be described in more detail below by way of examples, but these examples do not limit the present invention.
[実施例1〜18、比較例1〜8]
D体の含有量が1.2%であり、PMMA換算の重量平均分子量が16万である(A)ポリL乳酸樹脂、下記に示す芳香族ポリカーボネート樹脂、顔料、フッ素系樹脂、ヒンダードフェノール系酸化防止剤、(A)(B)以外の熱可塑性樹脂、結晶核剤および結晶核剤以外の充填剤や各種難燃剤を、それぞれ表1〜表3に示した割合で混合し、30mm径の2軸押出機により、シリンダー温度250℃、回転数150rpmの条件で溶融混練を行い、ダイスからストランド状に溶融ガットを引き、冷却バスで水冷し、ストランドカッターでペレット化した樹脂組成物を得た。
[Examples 1 to 18, Comparative Examples 1 to 8]
(A) poly-L lactic acid resin, aromatic polycarbonate resin shown below, pigment, fluorine-based resin, hindered phenol type Antioxidants, thermoplastic resins other than (A) and (B), fillers other than crystal nucleating agents and crystal nucleating agents and various flame retardants are mixed in the proportions shown in Tables 1 to 3, respectively, Using a twin-screw extruder, melt kneading was performed under conditions of a cylinder temperature of 250 ° C. and a rotation speed of 150 rpm, a molten gut was drawn from the die in a strand shape, water-cooled with a cooling bath, and a resin composition pelletized with a strand cutter was obtained. .
なお、表1〜表3における(B)芳香族ポリカーボネート樹脂、(C)顔料、(D)フッ素系樹脂、(E)ヒンダードフェノール系酸化防止剤、(F)(A)(B)以外の熱可塑性樹脂、(G)結晶核剤、結晶核剤以外の充填剤および難燃剤の符号は、次の内容を示すものである。なお、(C)〜(G)、結晶核剤以外の充填剤および難燃剤の配合量は、(A)ポリ乳酸樹脂と(B)芳香族ポリカーボネート樹脂の合計100重量部に対する配合量である。
(B)芳香族ポリカーボネート樹脂(出光石油化学工業(株)製“タフロン”A−1900)
(C)顔料:C−1カーボンブラック(デグサジャパン(株)製、ファーネスブラック、“Printex”35)
(C)顔料:C−2酸化チタン(石原産業(株)製ルチル型酸化チタン、R−620)
(D)フッ素系樹脂:D−1テトラフルオロエチレン(三井・デュポンフロロケミカル(株)製“テフロン(登録商標)”6−J)。
(D)フッ素系樹脂:D−2アクリル変性テトラフルオロエチレン(三菱レイヨン(株)製“メタブレン(登録商標)”A−3800)。
(E)ヒンダードフェノール系酸化防止剤:E−1ペンタエリスリチル−テトラキス{3−(3,5−t−ブチル−4−ヒドロキシフェニル)プロピオネート}(日本チバガイギー(株)製“イルガノックス”1010
(F)(A)(B)以外の熱可塑性樹脂:F−1ABS樹脂(スチレン/アクリロニトリル/ブタジエン/スチレン)(東レ(株)製“トヨラック”T−100)。
(F)(A)(B)以外の熱可塑性樹脂:F−2ポリプロピレン(ブロックタイプ)((株)プライムポリマー製J715M)。
(F)(A)(B)以外の熱可塑性樹脂:F−3ポリブチレンサクシネート樹脂(昭和高分子製“ビオノーレ”1001)。
(F)(A)(B)以外の熱可塑性樹脂:F−4シリコーン・アクリル複合コアシェルゴム(三菱レイヨン(株)製“メタブレン”SX−005)。
(F)(A)(B)以外の熱可塑性樹脂:F−5ポリ(エチレン/アクリル酸エチル/無水マレイン酸)−g−ポリメタクリル酸メチル(日本油脂(株)製“モディパー”A−8200)。
(F)(A)(B)以外の熱可塑性樹脂:F−6エチレン/グリシジルメタクリレート(住友化学工業(株)製“ボンドファースト”E)。
(G)無機結晶核剤:G−1タルク(日本タルク(株)製“P−6”、平均粒径約4μm)。
結晶核剤以外の充填剤:チョップドストランドのガラス繊維(日東紡績(株)製CS−3J948)(GFと略する)。
難燃剤:縮合リン酸エステル(大八化学工業(株)製“PX−200”)(PX−200と略する)。
In Tables 1 to 3, other than (B) aromatic polycarbonate resin, (C) pigment, (D) fluorine resin, (E) hindered phenol antioxidant, (F) (A) (B) The symbols of the thermoplastic resin, (G) crystal nucleating agent, fillers other than the crystal nucleating agent, and flame retardant indicate the following contents. In addition, the compounding quantity of fillers other than (C)-(G) and a crystal nucleating agent, and a flame retardant is a compounding quantity with respect to a total of 100 weight part of (A) polylactic acid resin and (B) aromatic polycarbonate resin.
(B) Aromatic polycarbonate resin (“Taflon” A-1900 manufactured by Idemitsu Petrochemical Co., Ltd.)
(C) Pigment: C-1 carbon black (manufactured by Degussa Japan Co., Ltd., furnace black, “Printex” 35)
(C) Pigment: C-2 titanium oxide (Ishihara Sangyo Co., Ltd. rutile titanium oxide, R-620)
(D) Fluorine-based resin: D-1 tetrafluoroethylene (“Teflon (registered trademark)” 6-J manufactured by Mitsui DuPont Fluorochemical Co., Ltd.).
(D) Fluorine-based resin: D-2 acrylic-modified tetrafluoroethylene (Mitsubrene (registered trademark) A-3800 manufactured by Mitsubishi Rayon Co., Ltd.).
(E) Hindered phenol antioxidant: E-1 pentaerythrityl-tetrakis {3- (3,5-t-butyl-4-hydroxyphenyl) propionate} ("Irganox" 1010 manufactured by Ciba Geigy Japan, Inc.)
(F) Thermoplastic resins other than (A) and (B): F-1 ABS resin (styrene / acrylonitrile / butadiene / styrene) (“Toyolac” T-100, manufactured by Toray Industries, Inc.).
(F) Thermoplastic resins other than (A) and (B): F-2 polypropylene (block type) (J715M manufactured by Prime Polymer Co., Ltd.).
(F) Thermoplastic resins other than (A) and (B): F-3 polybutylene succinate resin (“Bionore” 1001 manufactured by Showa Polymer Co., Ltd.).
(F) Thermoplastic resins other than (A) and (B): F-4 silicone / acrylic composite core-shell rubber ("METABRENE" SX-005 manufactured by Mitsubishi Rayon Co., Ltd.).
(F) Thermoplastic resins other than (A) and (B): F-5 poly (ethylene / ethyl acrylate / maleic anhydride) -g-polymethyl methacrylate (“Modiper” A-8200 manufactured by NOF Corporation) ).
(F) Thermoplastic resins other than (A) and (B): F-6 ethylene / glycidyl methacrylate (“Bond First” E manufactured by Sumitomo Chemical Co., Ltd.).
(G) Inorganic crystal nucleating agent: G-1 talc (“P-6” manufactured by Nippon Talc Co., Ltd., average particle diameter of about 4 μm).
Filler other than crystal nucleating agent: Glass fiber of chopped strand (CS-3J948 manufactured by Nitto Boseki Co., Ltd.) (abbreviated as GF).
Flame retardant: condensed phosphate ester (“PX-200” manufactured by Daihachi Chemical Industry Co., Ltd.) (abbreviated as PX-200).
また、得られた樹脂組成物について、東芝機械(株)製IS55EPN射出成形機を用い、シリンダー温度250℃、金型温度80℃の条件で射出成形を行い、3mm厚み80mm×120mm角板を得、下記の(1)〜(2)の方法で成形品表面の鮮明度光沢度と初期の成形品に焼けスジ発生について評価した。また、物性と難燃性については、(3)〜(5)の方法で評価した。 In addition, the obtained resin composition was subjected to injection molding under the conditions of a cylinder temperature of 250 ° C. and a mold temperature of 80 ° C. using an IS55EPN injection molding machine manufactured by Toshiba Machine Co., Ltd. to obtain a 3 mm thick 80 mm × 120 mm square plate. Then, the following methods (1) to (2) were used to evaluate the sharpness and glossiness of the surface of the molded product and the occurrence of burning streaks on the initial molded product. Moreover, about the physical property and the flame retardance, it evaluated by the method of (3)-(5).
(1)鮮明度光沢度
財団法人日本色彩研究所製<PGD>携帯用鮮明度光沢度計を用い、成形品の鮮明度光沢度を測定した。なお、鮮明度光沢度の値は、2.0〜0.1までの数字であり、数字が大きいほど優れ、0.1に達しない鮮明度光沢度の成形品は規格外とした。
(1) Sharpness and glossiness The sharpness and glossiness of the molded product were measured using <PGD> portable sharpness and glossiness meter manufactured by Nippon Color Research Institute. The value of the sharpness and glossiness is a number from 2.0 to 0.1. The larger the number, the better, and the molded product with the sharpness and glossiness that does not reach 0.1 is out of specification.
なお、鮮明度光沢度の値は、使用した金型の表面仕上げによっても左右されることから、金型の表面仕上げを見るため、汎用樹脂の中で鮮明度光沢度に優れるABS樹脂(東レ(株)製“トヨラック”T−100黒色)を同じ成形条件で成形し、鮮明度光沢度を測定したところ1.5を示した。 In addition, since the value of the sharpness and glossiness depends on the surface finish of the mold used, ABS resin (Toray (excellent) in general-purpose resin has excellent sharpness and glossiness in order to see the surface finish of the mold. Co., Ltd. “Toyolac” T-100 Black) was molded under the same molding conditions, and the sharpness and glossiness were measured to show 1.5.
(2)初期の成形品の焼けスジ評価
樹脂組成物を射出成形機内に15分間滞留させ、その後の射出成形により角板を得た。さらに、射出成形機内の樹脂組成物をパージ(排出)後、樹脂組成物を射出成形機内に再び15分間滞留させ、その後の射出成形により角板を得た。この操作をさらに3回繰り返して合計5個の角板を得た。前記の5個の角板の成形品表面を目視観察し、2個以上の角板に焼けスジが認められた角板を×と判定、1個の角板に焼けスジが認められた角板を△と判定、5個の角板に焼けスジが観察されない角板を○と判定した。
(2) Evaluation of Burn Streaks of Initial Molded Product The resin composition was allowed to stay in the injection molding machine for 15 minutes, and a square plate was obtained by subsequent injection molding. Furthermore, after purging (discharging) the resin composition in the injection molding machine, the resin composition was again retained in the injection molding machine for 15 minutes, and a square plate was obtained by subsequent injection molding. This operation was further repeated 3 times to obtain a total of 5 square plates. By visually observing the surface of the molded product of the five square plates, a square plate in which two or more square plates were found to be burned was judged as x, and a square plate in which one piece was burned was found. Was determined to be Δ, and a square plate in which no burning streaks were observed on five square plates was determined to be ◯.
(3)熱変形温度
射出成形により作製した3mm厚みの試験片を用い、ASTM法D648に従い、0.46MPaの荷重条件で熱変形試験を行った。
(3) Thermal deformation temperature A thermal deformation test was performed under a load condition of 0.46 MPa according to ASTM method D648 using a 3 mm-thick test piece produced by injection molding.
(4)衝撃強度
射出成形により作製した3mm厚みの衝撃試験片を用い、ASTM法D256に従い、アイゾット衝撃試験(ノッチ無し)を測定した。
(4) Impact strength An Izod impact test (no notch) was measured according to ASTM method D256 using a 3 mm-thick impact test piece produced by injection molding.
(5)難燃性
射出成形により作製した1.6mm厚みの127mm×12.7mmの燃焼試験片を用いて、アメリカUL規格サブジェクト94(UL94)の垂直燃焼試験法に準拠して燃焼試験を行い、難燃性を評価し、その評価ランクは難燃性が優れる順にV−0、V−1、V−2で示され、前記のランクに該当しなかった物は規格外とした。
(5) Flame retardance Using a 1.6mm-thickness 127mm x 12.7mm combustion test piece produced by injection molding, a combustion test is conducted in accordance with the vertical combustion test method of the US UL standard subject 94 (UL94). The flame retardancy was evaluated, and the evaluation ranks were indicated by V-0, V-1, and V-2 in the order of excellent flame retardancy, and those that did not fall within the above rank were out of specification.
これらの結果を表1〜表3に併せて示す。 These results are also shown in Tables 1 to 3.
表1の実施例1〜8から、本発明の(A)〜(E)成分を配合した樹脂組成物は、鮮明度光沢度、焼けスジ、熱変形温度、衝撃強度に優れる樹脂組成物からなる成形品と言える。 From Examples 1 to 8 in Table 1, the resin composition containing the components (A) to (E) of the present invention consists of a resin composition excellent in sharpness, glossiness, burnt lines, heat distortion temperature, and impact strength. It can be said to be a molded product.
表2の比較例1から、(D)フッ素系樹脂と(E)ヒンダードフェノール系酸化防止剤を配合しない樹脂組成物は、鮮明度光沢度に劣り、かつ焼けスジが発生して不良品が発生する樹脂組成物であった。また、比較例2〜3から、(D)成分あるいは(E)成分のいずれかを配合しない組成物は、鮮明度光沢度に劣るか、もしくは焼けスジが発生して不良品が発生する樹脂組成物のいずれかであった。
表2の比較例4から、本発明範囲より多量の(A)ポリ乳酸樹脂の配合比率においては、鮮明度光沢度と物性に劣る樹脂組成物であった。また、比較例5から、本発明範囲より多量の(B)芳香族ポリカーボネート樹脂の配合比率においては、鮮明度光沢度に劣ることと、部分的に透明な部分が存在する樹脂組成物であった。
From Comparative Example 1 in Table 2, the resin composition not containing (D) a fluororesin and (E) a hindered phenolic antioxidant is inferior in sharpness and glossiness, and has burned streaks and defective products. It was a generated resin composition. Further, from Comparative Examples 2 to 3, the composition not containing any of the component (D) or the component (E) is inferior in the glossiness of the sharpness, or a resin composition in which a burnt streak occurs and a defective product is generated. It was one of the things.
From the comparative example 4 of Table 2, it was a resin composition inferior to a glossiness of a sharpness and a physical property in the compounding ratio of (A) polylactic acid resin more than the range of this invention. Further, from Comparative Example 5, the blending ratio of the aromatic polycarbonate resin (B) in a larger amount than the range of the present invention was a resin composition having inferior sharpness and glossiness and partially transparent portions. .
表2の比較例6〜8から、(C)顔料、(D)フッ素系樹脂および(E)ヒンダードフェノール系酸化防止剤のいずれかが本発明範囲より多量に配合された場合は、鮮明度光沢度と衝撃強度に劣る樹脂組成物であった。 From Comparative Examples 6 to 8 in Table 2, when any of (C) pigment, (D) fluororesin and (E) hindered phenol antioxidant is blended in a larger amount than the range of the present invention, the sharpness The resin composition was inferior in gloss and impact strength.
表3の実施例9から、さらに(G)結晶核剤を配合した樹脂組成物は、本発明の性能を維持しながら、熱変形温度に優れると言える。また、実施例10から、結晶核剤以外の充填剤のGFを配合した樹脂組成物は、とくに熱変形温度に優れるものの、鮮明度光沢度の低下が認められた。また、実施例11〜16から、さらに(F)(A)(B)以外の熱可塑性樹脂を配合した樹脂組成物は、本発明の性能を維持しながら、熱変形温度もしくは衝撃強度に優れると言える。また、実施例17〜18から、さらに難燃剤を配合した樹脂組成物は、本発明の性能を維持しながら、難燃性が付与された成形品と言える。 From Example 9 of Table 3, it can be said that the resin composition which further mix | blended (G) crystal nucleating agent is excellent in heat-deformation temperature, maintaining the performance of this invention. Further, from Example 10, the resin composition containing the filler GF other than the crystal nucleating agent was particularly excellent in heat distortion temperature, but a decrease in sharpness and glossiness was recognized. Moreover, from Examples 11-16, the resin composition which mix | blended thermoplastic resins other than (F) (A) (B) is excellent in heat-deformation temperature or impact strength, maintaining the performance of this invention. I can say that. Moreover, it can be said from Examples 17-18 that the resin composition which mix | blended the flame retardant further is a molded article to which the flame retardance was provided, maintaining the performance of this invention.
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